Ronaldo Giro, Hsianghan Hsu, Akihiro Kishimoto, Rodrigo F. Neumann, Binquan Luan, Seiji Takeda, Lisa Hamada, Mathias B. Steiner

- Data sets and scripts for computational discovery of polymer membranes for carbon dioxide separation. The training data set with 1,169 homo-polymers provides carbon dioxide permeability, glass transition temperature and half decomposition temperature for each listed material. The output data set contains 784 optimized homo-polymer candidates generated by Inverse Design and Machine Learning techniques. The Jupyter notebook enables the use of the Polymer Property Prediction Engine as a service for generating the properties provided in the training data set.

Latest version: v4

Publication date: May 18, 2022

Ademir Ferreira da Silva, Ricardo Luis Ohta, Jaione Tirapu Azpiroz, Matheus Esteves Fereira, Daniel Vitor Marçal, André Botelho, Tulio Coppola, Allysson Flavio Melo de Oliveira, Murilo Bettarello, Lauren Schneider, Rodrigo Vilaça, Noorunisha Abdool, Pedro Augusto Malanga, Vanderlei Junior, Wellington Furlaneti, Mathias Steiner

- For optimizing production yield while limiting negative environmental impact, sustainable agriculture benefits greatly from real-time, on-the-spot analysis of soil at low cost. Colorimetric paper sensors are ideal candidates for cheap and rapid chemical spot testing. However, their field application requires previously unattained paper sensor reliability and automated readout and analysis by means of integrated mobile communication, artificial intelligence, and cloud computing technologies. Here, we report such a mobile chemical analysis system based on colorimetric paper sensors that operates under tropical field conditions. By mapping topsoil pH in a field with an area of 9 hectares, we have benchmarked the mobile system against precision agriculture standards following a protocol with reference analysis of compound soil samples. As compared with routine lab analysis, our mobile soil analysis system has correctly classified soil pH in 97.8% of cases (132 out of 135 tests) while ...

Latest version: v1

Publication date: May 13, 2022

Ruchika Mahajan, Arti Kashyap, Iurii Timrov

- We present a first-principles investigation of the structural, electronic, and magnetic properties of the pristine and Fe-doped α-MnO₂ using density-functional theory with extended Hubbard functionals. The onsite U and intersite V Hubbard parameters are determined from first principles and self-consistently using density-functional perturbation theory in the basis of Löwdin-orthogonalized atomic orbitals. Among the ferromagnetic and four types of antiferromagnetic (AFM) orderings for the pristine α-MnO₂ we find the C2-AFM spin configuration to be the most energetically favorable, in agreement with the experimentally observed AFM state. The computed lattice parameters, magnetic moments, and band gaps are overall in good agreement with the experimental ones when both the onsite and intersite Hubbard corrections are included. For the Fe-doped α-MnO₂ two types of doping are considered: Fe insertion in the 2 × 2 tunnels and partial substitution of Fe for Mn. The calculated formation ...

Latest version: v1

Publication date: May 12, 2022

Michelle Ernst, Tomasz Poręba, Lars Gnägi, Ganna Gryn'ova

- Molecular docking has traditionally mostly been employed in the field of protein-ligand binding. In the publication associated with this data, we extend this method, in combination with DFT-level geometry optimizations, to locate guest molecules inside the pores of metal-organic frameworks. Additional information on the adsorption strength in the studied host-guest systems emerges from the computed interaction energies. This record contains inputs and outputs of the molecular docking and the DFT computations.

Latest version: v1

Publication date: May 10, 2022

Xiangyu Chen, William Shao, Nam Le, Paulette Clancy

- Atomic-scale simulations of reactive processes have been stymied by two factors: the general lack of a suitable semi-empirical force field on the one hand, and the impractically large computational burden of using ab initio molecular dynamics on the other. In this paper, we use an “on-the-fly” active learning technique to develop a non-parameterized force field that, in essence, exhibits the accuracy of density functional theory and the speed of a classical molecular dynamics simulation. We developed a force field suitable to capture the crystallization of gallium nitride (GaN) using a novel additive manufacturing route and a combination of liquid Ga and ammonia gas precursors to grow GaN thin films. We show that this machine learning model is capable of producing a transferable force field that can model all three phases, solid, liquid and gas, involved in this additive manufacturing process. We verified our computational results against a range of experimental measurements and ...

Latest version: v1

Publication date: May 09, 2022

Yanan Zhu, Sergi Vela, Hong Meng, Clémence Corminboeuf, Maria Fumanal

- Hot exciton materials have the potential to improve the quantum efficiency of organic light-emitting diodes (OLEDs) by promoting high Reversed InterSystem Crossing (hRISC) between a high-lying triplet (Tn, n≥2) and a radiative singlet (Sm). In recent years, donor–acceptor-donor (D-A-D) molecular systems have shown great promise in its ability to enhance the hRISC process under certain conditions. However, strategies to find appropriate D-A-D combinations beyond trial-and-error are still elusive. This work exposes the limited applicability of the current fragment-based design rules and proposes high-throughput screening as the optimal route to find promising candidates that fulfill the energy criteria for hot exciton materials. The strategy consists of first establishing the thresholds for large triplet-triplet splitting and small singlet-triplet gap, then filtering combinations through rate comparison of competitive crossing pathways, and finally confirming hRISC with spin-orbital ...

Latest version: v1

Publication date: May 06, 2022

Sarah Alamdari, Jim Pfaendtner

- One proposed mechanism of implant fouling is attributed to the nonspecific adsorption of non-collagenous bone matrix proteins (NCPs) onto a newly implanted interface. With the goal of capturing the fundamental mechanistic and thermodynamic forces that govern changes in these NCP recognition domains as a function of γ-carboxyglutamic acid (Gla) post-translational modification and surface chemistry, we probe the adsorption process of the most commonly occurring NCP, osteocalcin, onto a mineral and metal oxide surface. Here, we apply two enhanced sampling methods to independently probe the effects of post-translational modification and peptide structure on adsorption. First, well-tempered metadynamics was used to capture the binding of acetyl and N-methylamide capped glutamic acid and Gla single amino acids onto crystalline hydroxyapatite and titania model surfaces at physiological pH. Following this, parallel tempering metadynamics in the well-tempered ensemble (PTMetaD-WTE) was ...

Latest version: v2

Publication date: Apr 27, 2022

Sergi Vela, Ruben Laplaza, Yuri Cho, Clemence Corminboeuf

- The creation and maintenance of crystallographic data repositories is one of the greatest data-related achievements in chemistry. Platforms such as the Cambridge Structural Database host what is likely the most diverse collection of synthesizable molecules. If properly mined, they could be the basis for the large-scale exploration of new regions of the chemical space using quantum chemistry (QC). However, it is currently challenging to retrieve all the necessary information for QC based exclusively on the available structural data, especially for transition metal complexes. To solve this shortcoming, we present cell2mol, a software that interprets crystallographic data and retrieves the connectivity and total charge of molecules, including the oxidation state (OS) of metal atoms. We prove that cell2mol outperforms other popular methods at assigning the metal OS, while offering a much more comprehensive interpretation of the unit cell, and we make publicly available reliable ...

Latest version: v1

Publication date: Apr 25, 2022

Ted Hullar, Theo Tran, Zekun Chen, Fernanda C. Bononi, Oliver Palmer, Davide Donadio, Cort Anastasio

- Photochemical reactions of contaminants in snow and ice can be important sources and sinks for various organic and inorganic compounds. Snow contaminants can be found in the bulk ice matrix, in internal liquid-like regions (LLRs), or in quasi-liquid layers (QLLs) at the air-ice interface, where they can readily exchange with the firn air. Some studies have reported that direct photochemical reactions occur faster in LLRs and QLLs than in aqueous solution, while others have found similar rates. Here, we measure the photodegradation rate constants of the three dimethoxybenzene isomers under varying experimental conditions, including in aqueous solution, in LLRs, and at the air-ice interface of nature-identical snow. Relative to aqueous solution, we find modest photodegradation enhancements (3- and 6-fold) in LLRs for two of the isomers, and larger enhancements (15- to 30-fold) at the air-ice interface for all three isomers. We use computational modeling to assess the impact of light ...

Latest version: v1

Publication date: Apr 20, 2022

Seyed Mohamad Moosavi, Balázs Álmos Novotny, Daniele Ongari, Elias Moubarak, Mehrdad Asgari, Özge Kadioglu, Charithea Charalambous, Andres Ortega-Guerrero, Amir H. Farmahini, Lev Sarkisov, Susana Garcia, Frank Noé, Berend Smit

- The heat capacity of a material is a fundamental property that is of significant practical importance. For example, in a carbon capture process, the heat required to regenerate a solid sorbent is directly related to the heat capacity of the material. However, for most materials suitable for carbon capture applications the heat capacity is not known, and thus the standard procedure is to assume the same value for all materials. In this work, we developed a machine-learning approach to accurately predict the heat capacity of these materials, i.e., zeolites, metal-organic frameworks, and covalent-organic frameworks. The accuracy of our prediction is confirmed with novel experimental data. Finally, for a temperature swing adsorption process that captures carbon from the flue gas of a coal-fired power plant, we show that for some materials the energy requirement is reduced by as much as a factor of two using the correct heat capacity.

Latest version: v1

Publication date: Apr 13, 2022

Behnood Dianat, Francesco Tavanti, Andrea Padovani, Luca Larcher, Arrigo Calzolari

- The characterization of the atomic structure of disordered systems, such as amorphous, glasses and (bio)molecule in solution, is a fundamental step for most theoretical investigations. The properties of short- and medium-range local order structures are responsible for the electronic, optical and transport properties of these systems. Here, we present the BELLO open source code, a post-processing script-tool created for the automatic analysis and extraction of structural characteristics of disordered and amorphous systems. BELLO is agnostic to the code that generated single configurations or trajectories, it provides an intuitive access through a graphical user interface (GUI), and it requires minimal computational resources. Its capabilities include the calculation of the order parameter , the folded structure identification, and statistical analysis tools such as atomic coordination number and pair/angle-distribution functions. The working principles of the code are described ...

Latest version: v1

Publication date: Apr 13, 2022

Maryam Sajedi, Maxim Krivenkov, Dmitry Marchenko, Jaime Sánchez-Barriga, Anoop K. Chandran, Andrei Varykhalov, Emile D. L. Rienks, Irene Aguilera, Stefan Blügel, Oliver Rader

- The formation of large polarons has been proposed as reason for the high defect tolerance, low mobility, low charge carrier trapping and low nonradiative recombination rates of lead halide perovskites. Recently, direct evidence for large-polaron formation has been reported from a 50% effective mass enhancement in angle-resolved photoemission of CsPbBr₃ over theory for the orthorhombic structure. We present in-depth band dispersion measurements of CsPbBr₃ and GW calculations which lead to almost identical effective masses at the valence band maximum of 0.203+/-0.016 m₀ in experiment and 0.217 m₀ in orthorhombic theory. We argue that the effective mass can be explained solely on the basis of electron-electron correlation and large polaron formation cannot be concluded from photoemission data.

Latest version: v1

Publication date: Apr 11, 2022

Pushkar Ghanekar, Siddharth Deshpande, Jeffrey Greeley

- Heterogeneous catalytic reactions are influenced by a subtle interplay of atomic-scale factors, ranging from the catalysts’ local morphology to the presence of high adsorbate coverages. Describing such phenomena via computational models requires generation and analysis of a large space of surface atomic configurations. To address this challenge, we present the Adsorbate Chemical Environment-based Graph Convolution Neural Network (ACE-GCN), a screening workflow that can account for atomistic configurations comprising diverse adsorbates, binding locations, coordination environments, and substrate morphologies. Using this workflow, we develop catalyst surface models for two illustrative systems: (i) NO adsorbed on a Pt3Sn(111) alloy surface, of interest for nitrate electroreduction processes, where high adsorbate coverages combine with the low symmetry of the alloy substrate to produce a large configurational space, and (ii) OH* adsorbed on a stepped Pt(221) facet, of relevance to ...

Latest version: v1

Publication date: Apr 11, 2022

Noah Hoffmann, Tiago F. T. Cerqueira, Jonathan Schmidt, Miguel A. L. Marques

- We present a comprehensive theoretical study of conventional superconductivity in cubic antiperovskites materials with composition XYZ₃ where X and Z are metals and Y is H, B, C, N, O, and P. Our starting point are electron-phonon calculations for 384 materials performed with density-functional perturbation theory. While 40% of the materials were dynamically unstable as they exhibited imaginary frequencies, we discovered 16 compounds with Tc higher than 5 K including antiperovskites with Y=H, N, C and O. We used these results to train interpretable machine learning models to understand and further explore this family of compounds. This lead us to predict a further 44 materials with superconducting transition temperatures above 5 K, reaching a maximum of 17.8 K for PtHBe₃. Furthermore, the models give us an understanding of the mechanism of superconductivity in anti-perovskites and highlight the importance of the density of states at the Fermi level and of the mass of the Y-atom ...

Latest version: v1

Publication date: Apr 06, 2022

Eleftherios Andritsos, Kevin Rossi

- Li–S batteries are a promising alternative to Li-ion batteries, offering large energy storage capacity and wide operating temperature range. However, their performance is heavily affected by the Li-polysulphide (LiPS) shuttling. Computational screening of LiPS adsorption on single-atom catalyst (SAC) substrates is of great aid to the design of Li–S batteries which are robust against the LiPS shuttling from the cathode to the anode and the electrolyte. To facilitate this process, we develop a machine learning (ML) protocol to accelerate the systematic mapping of dominant local energy minima found with calculations based on the density functional theory (DFT), and, in turn, fast screening of LiPS adsorption properties on SACs. We first validate the approach by probing the potential energy surface for LiPS adsorbed on graphene decorated with a Fe–N4–C SAC. We identify minima whose binding energies are better or on par with the one previously reported in the literature. We then move ...

Latest version: v2

Publication date: Apr 05, 2022

Xiao-Xiang Chen, Jia-Tong Li, Yu-Hui Fang, Xin-Yu Deng, Xue-Qing Wang, Guangchao Liu, Yunfei Wang, Xiaodan Gu, Shang-Da Jiang, Ting Lei

- Organic semiconductors with high-spin ground states are fascinating because they could enable fundamental understanding on the spin-related phenomenon in light element and provide opportunities for organic magnetic and quantum materials. Although high-spin ground states have been observed in some quinoidal type small molecules or doped organic semiconductors, semiconducting polymers with high-spin at their neutral ground state are rarely reported. Here we report three high-mobility semiconducting polymers with different spin ground states. We show that polymer building blocks with small singlet-triplet energy gap (ΔES-T) could enable small ΔES-T gap and increase the diradical character in copolymers. We demonstrate that the electronic structure, spin density, and solid-state interchain interactions in the high-spin polymers are crucial for their ground states. Polymers with a triplet ground state (S = 1) could exhibit doublet (S = 1/2) behavior due to different spin distributions ...

Latest version: v1

Publication date: Apr 01, 2022

Simon Batzner, Albert Musaelian, Lixin Sun, Mario Geiger, Jonathan P. Mailoa, Mordechai Kornbluth, Nicola Molinari, Tess E. Smidt, Boris Kozinsky

- This work presents Neural Equivariant Interatomic Potentials (NequIP), an E(3)-equivariant neural network approach for learning interatomic potentials from ab-initio calculations for molecular dynamics simulations. While most contemporary symmetry-aware models use invariant convolutions and only act on scalars, NequIP employs E(3)-equivariant convolutions for interactions of geometric tensors, resulting in a more information-rich and faithful representation of atomic environments. The method achieves state-of-the-art accuracy on a challenging and diverse set of molecules and materials while exhibiting remarkable data efficiency. NequIP outperforms existing models with up to three orders of magnitude fewer training data, challenging the widely held belief that deep neural networks require massive training sets. The high data efficiency of the method allows for the construction of accurate potentials using high-order quantum chemical level of theory as reference and enables ...

Latest version: v1

Publication date: Mar 30, 2022

Jigyasa Nigam, Sergey Pozdnyakov, Guillaume Fraux, Michele Ceriotti

- Data-driven schemes that associate molecular and crystal structures with their microscopic properties share the need for a concise, effective description of the arrangement of their atomic constituents. Many types of models rely on descriptions of atom-centered environments, that are associated with an atomic property or with an atomic contribution to an extensive macroscopic quantity. Frameworks in this class can be understood in terms of atom-centered density correlations (ACDC), that are used as a basis for a body-ordered, symmetry-adapted expansion of the targets. Several other schemes, that gather information on the relationship between neighboring atoms using "message-passing" ideas, cannot be directly mapped to correlations centered around a single atom. We generalize the ACDC framework to include multi-centered information, generating representations that provide a complete linear basis to regress symmetric functions of atomic coordinates, and provides a coherent ...

Latest version: v1

Publication date: Mar 24, 2022

Maria Fumanal, Clemence Corminboeuf

- Singlet fission (SF) is a two-step process in which a singlet splits into two triplets throughout the so-called correlated triplet-pair (1TT) state. Intramolecular SF (iSF) materials in particular, have attracted growing interest as they can be easily implemented in single junction solar cells and boost their power conversion efficiency. Still, the potential of iSF materials such as polymers and oligomers for photovoltaic applications has been partially hindered by their ability to go beyond the 1TT intermediate and generate free triplets, which mechanism remains poorly understood. In this work, the main aspects governing the 1TT dissociation in donor-acceptor copolymers and the key features that optimize this process are exposed. First, we show that both thermodynamics and kinetics play a crucial role in the intramolecular triplet-pair separation and second, we uncover the inherent flexibility of the donor unit as the fundamental ingredient to optimize them simultaneously. ...

Latest version: v1

Publication date: Mar 23, 2022

Veronika Jurásková, Frédéric Célerse, Rubén Laplaza, Clémence Corminboeuf

- Non-covalent bonding patterns are commonly harvested as a design principle in the field of catalysis, supramolecular chemistry, and functional materials to name a few. Yet, their computational description generally neglects finite temperature and environment effects, which promote competing interactions and alter their static gas-phase properties. Recently, neural network potentials (NNPs) trained on Density Functional Theory (DFT) data have become increasingly popular to simulate molecular phenomena in condensed phase with an accuracy comparable to ab initio methods. To date, most applications have centered on solid-state materials or fairly simple molecules made of a limited number of elements. Herein, we focus on the persistence and strength of chalcogen bonds involving benzotelluradiazole in condensed phase. While the tellurium-containing heteroaromatic molecules are known to exhibit pronounced interactions with anions and lone pairs of different atoms, the relevance of ...

Latest version: v1

Publication date: Mar 16, 2022

Olivia P. Pfeiffer, Haihao Liu, Luca Montanelli, Marat I. Latypov, Fatih G. Sen, Vishwanath Hegadekatte, Elsa A. Olivetti, Eric R. Homer

- Researchers continue to explore and develop aluminum alloys with new compositions and improved performance characteristics. An understanding of the current design space can help accelerate the discovery of new alloys. We present two datasets: 1) chemical composition, and 2) mechanical properties for predominantly wrought aluminum alloys. The first dataset contains 14,884 entries on aluminum alloy compositions extracted from academic literature and US patents using text processing techniques, including 550 wrought aluminum alloys which are already registered with the Aluminum Association. The second dataset contains 1,278 entries on mechanical properties for aluminum alloys, where each entry is associated with a particular wrought series designation, extracted from tables in academic literature.

Latest version: v3

Publication date: Mar 16, 2022

Jing Yang, Stefano Falletta, Alfredo Pasquarello

- We present an efficient procedure for constructing nonempirical hybrid functionals to accurately predict band gaps of extended systems. We determine mixing parameters by enforcing the generalized Koopmans’ condition on localized electron states, which are achieved by inserting an optimized potential probe. Application of this scheme to a large set of materials yields band gaps with a mean error of 0.30 eV with respect to experiment. Next, we consider a perturbative one-shot approach in which the single- particle eigenvalues are calculated with the wave functions obtained at the semilocal level. In this way, the computational cost is reduced by ∼85% without loss of accuracy. The scheme is found to be robust upon consideration of different defect species and functional forms.

Latest version: v1

Publication date: Mar 15, 2022

Daniel Marchand, W.A. Curtin

- Most metallurgical properties, e.g., dislocation propagation, precipitate formation, can only be fully understood atomistically but most phenomena and quantities of interest cannot be measured experimentally. Accurate simulation methods are essential but first-principles density functional theory (DFT) is prohibitively expensive while empirical interatomic potentials are rarely sufficiently accurate for alloys. Machine learning (ML) is emerging as an approach to create computationally-efficient atomistic potentials achieving near-DFT accuracy. Building on recent work on binary Al-Cu and ternary Al-Mg-Si, here a family of neural network potentials (NNPs) for Al alloys of Al-Cu-Mg and Al-Cu-Mg-Zn is developed and assessed using the Behler-Parinello formulation. Training of the potentials uses a robust set of metallurgically-relevant structures including intermetallic phases, stacking faults, solute/solute and solute/stacking fault interactions, solute clusters, and ...

Latest version: v2

Publication date: Mar 14, 2022

Sebastiaan Huber, Marnik Bercx, Nicolas Hörmann, Martin Uhrin, Giovanni Pizzi, Nicola Marzari

- The Materials Cloud three-dimensional database is a curated set of relaxed three-dimensional crystal structures based on raw CIF data taken from the external experimental databases MPDS, COD and ICSD. The raw CIF data have been imported, cleaned and parsed into a crystal structure; their ground-state has been computed using the SIRIUS-enabled pw.x code of the Quantum ESPRESSO distribution, and tight tolerance criteria for the calculations using the SSSP protocols. This entire procedure is encoded into an AiiDA workflow which automates the process while keeping full data provenance. Here, since the original source data of the ICSD and MPDS databases are copyrighted, only the provenance of the final SCF calculation on the relaxed structures can be made publicly available. The MC3D ID numbers come from a list of unique "parent" stoichiometric structures that has been created and curated from a collection of these experimental databases. Once a parent structure has been optimized ...

Latest version: v1

Publication date: Mar 12, 2022

Henglu Xu, Raffaela Cabriolu, Berend Smit

- If one carries out a molecular simulation of N particles using periodic boundary conditions, linear momentum is conserved and hence the number of degrees of freedom is set to 3N-3. In most programs, this number of degrees of freedom is the default setting. However, if one carries out a molecular simulation in an external field, one needs to ensure that degrees of freedom are changed from this default setting to 3N, as in an external field the velocity of the center of mass can change. Using the correct degrees of freedom is important in calculating the temperature and in some algorithms to simulate at constant temperature. For sufficiently large systems, the difference between 3N and 3N-3 is negligible in the way. However, there are systems in which the comparison with experimental data requires molecular dynamics simulations of a small number of particles. In this work, we illustrate the effect of an incorrect setting of degrees of freedom in molecular dynamic simulations ...

Latest version: v2

Publication date: Mar 09, 2022

Pietro Bonfà, Jonathan Frassineti, John M. Wilkinson, Giacomo Prando, Muhammad M. Isah, Chennan Wang, Tiziana Spina, Boby Joseph, Vesna F. Mitrović, Roberto De Renzi, Stephen J. Blundell, Samuele Sanna

- We report on the first example of quantum coherence between the spins of muons and quadrupolar nuclei. We observe this effect in vanadium intermetallic compounds which adopt the A15 crystal structure, and whose members include all technologically dominant superconductors. The entangled states are extremely sensitive to the local structural and electronic environments through the electric field gradient at the quadrupolar nuclei. This case-study demonstrates that positive muons can be used as a quantum sensing tool to probe also structural and charge related phenomena in materials, even in the absence of magnetic order. The data here contained can be used to reproduce all results and graphs shown in the article.

Latest version: v1

Publication date: Mar 08, 2022

Haiyuan Wang, Alexey Tal, Thomas Bischoff, Patrick Gono, Alfredo Pasquarello

- We develop a computationally efficient scheme to accurately determine finite-temperature band gaps. We here focus on materials belonging to the class ABX3 (A = Rb, Cs; B = Ge, Sn, Pb; and X = F, Cl, Br, I), which includes halide perovskites. First, an initial estimate of the band gap is provided for the ideal crystalline structure through the use of a range-separated hybrid functional, in which the parameters are determined nonempirically from the electron density and the high-frequency dielectric constant. Next, we consider two kinds of band-gap corrections to account for spin-orbit coupling and thermal vibrations including zero-point motions. In particular, the latter effect is accounted for through the special displacement method, which consists in using a single distorted configuration obtained from the vibrational frequencies and eigenmodes, thereby avoiding lengthy molecular dynamics. The sequential consideration of both corrections systematically improves the band gaps, ...

Latest version: v1

Publication date: Mar 04, 2022

Claudio Zeni, Andrea Anelli, Aldo Glielmo, Kevin Rossi

- We show that, contrary to popular assumptions, predictions from machine learning potentials built upon high-dimensional atom-density representations almost exclusively occur in regions of the representation space which lie outside the convex hull defined by the training set points. We then propose a perspective to rationalise the domain of robust extrapolation and accurate prediction of atomistic machine learning potentials in terms of the probability density induced by training points in the representation space. The data here contained can be used to reproduce all results and graphs shown in the article. We also include the trajectory files for the Au13 dataset we generate by running molecular dynamics simulations of an Au nanoparticle containing 13 atoms at temperatures of 50K, 100K, 200K, 300K, and 400K. Details regarding the generation of such dataset can be found in the supplementary information file for the article.

Latest version: v1

Publication date: Mar 03, 2022

Simone Gallarati, Raimon Fabregat, Veronika Juraskova, Theo Jaffrelot Inizan, Clemence Corminboeuf

- A highly appealing strategy to modulate a catalyst's activity and/or selectivity in a dynamic and non-invasive way is to incorporate a photoresponsive unit into a catalytically competent molecule. However, the description of the photoinduced conformational or structural changes that alter the catalyst's intrinsic reactivity is often reduced to a handful of intuitive static representations, which can struggle to capture the complexity of flexible organocatalysts. Here, we show how a comprehensive exploration of the free energy landscape of N-alkylated azobenzene-tethered piperidine catalysts is essential to unravel the conformational characteristics of each configurational state and explain the experimentally observed reactivity trends. Mapping the catalysts’ conformational space highlights the existence of false ON or OFF states that lower their switching ability. Our findings expose the challenges associated with the realisation of reversible steric shielding for the photocontrol ...

Latest version: v1

Publication date: Feb 24, 2022

Michele Kotiuga, Samed Halilov, Boris Kozinsky, Marco Fornari, Nicola Marzari, Giovanni Pizzi

- This work details how to determine structural prototypes for the cubic perovskite structure that are used to study the B-site displacements in the cubic, paraelectric phase. Car-Parrinello MD simulations of cubic barium titanate (BaTiO3) show the titanium displacements from the undistorted cubic structure. Using a systematic symmetry analysis we construct microscopic templates, i.e. representative structural models in the form of supercells that satisfy a desired point symmetry but are built from the combination of lower-symmetry primitive cells. Density functional theory calculations, using the microscopic templates as starting structures for a relaxation, are carried out to find structural prototypes of BaTiO3 with local polar distortions but with cubic point symmetry. The stability of these structures is studied as a function of volume and with respect to the zone-boundary phonons of pristine cubic BaTiO3. The stable distortions patterns for BaTiO3 are investigated for other titanates and for a handful of niobates and zirconates.

Latest version: v2

Publication date: Feb 22, 2022

Johannes M. Meusburger, Karen A. Hudson-Edwards, Chiu C. Tang, Eamonn T. Connolly, Rich A. Crane, A. Dominic Fortes

- Rozenite (FeSO₄·4H₂O) is a candidate mineral component of the polyhydrated sulfate deposits on the surface and in the subsurface of Mars. In order to better understand its behavior at temperature conditions prevailing on the martian surface and aid its identification in ongoing and future Rover missions we have carried out a combined experimental and computational study of the mineral’s structure and properties. We collected neutron powder diffraction data at temperatures ranging from 21 – 290 K, room temperature synchrotron X-ray data and Raman spectra. Moreover, first-principles calculations of the vibrational properties of rozenite were carried out to aid the interpretation of the Raman spectrum. In this work, we demonstrated how combining Raman spectroscopy and X-ray diffraction of the same sample material sealed inside a capillary with complementary first principles calculations yields accurate reference Raman spectra. This workflow enables the construction of a reliable ...

Latest version: v1

Publication date: Feb 18, 2022

Azim Fitri Ainul Abidin, Ikutaro Hamada

- We have studied the interaction of water and graphene doped with nitrogen in different configurations, namely, graphitic and pyridinic nitrogen, by means of the van der Waals density functional. We found that the local nitrogen configuration plays a key role in determining the stable water configuration, while the dispersion force is responsible for the water adsorption. With the graphitic nitrogen, water prefers to orient with its oxygen toward the surface, whereas for the pyridinic nitrogen it prefers to orient with its hydrogens toward the surface, because nitrogen is positively and negatively charged for the former and the latter, respectively. Our results have great implications for the modeling of the interface between water and nitrogen-doped graphitic systems.

Latest version: v1

Publication date: Feb 18, 2022

QuanSheng Wu, Jianpeng Liu, Yifei Guan, Oleg V. Yazyev

- We propose Landau levels as a probe for the topological character of electronic bands in two-dimensional moiré superlattices. We consider two configurations of twisted double bilayer graphene (TDBG) that have very similar band structures, but show different valley Chern numbers of the flat bands. These differences between the AB-AB and AB-BA configurations of TDBG clearly manifest as different Landau level sequences in the Hofstadter butterfly spectra calculated using the tight-binding model. The Landau level sequences are explained from the point of view of the distribution of orbital magnetization in momentum space that is governed by the rotational C2 and time-reversal T symmetries. Our results can be readily extended to other twisted graphene multilayers and h-BN/graphene heterostructures thus establishing the Hofstadter butterfly spectra as a powerful tool for detecting the nontrivial valley band topology.

Latest version: v1

Publication date: Feb 17, 2022

Roman Kováčik, Phivos Mavropoulos, Stefan Blügel

- The JuHemd (Jülich-Heusler-magnetic-database) is a collection of the magnetic phase transition types and transition temperatures (Tc) for experimentally documented Heusler and Heusler-like materials, as found by density functional calculations augmented by the Monte Carlo method, and as reported by experiment in the literature. The database contains results on 400 compounds, many of them with different setups of the chemical order/disorder, totaling 776 systems. The ground state electronic structure was obtained by density functional theory calculations with the JuKKR code. Two exchange-correlation functionals were employed: the local density approximation (LDA) and the generalized gradient approximation (GGA). The chemical disorder was treated within the coherent-potential approximation. For 306 materials (627 systems) with sizable magnetization, the Heisenberg exchange parameters were evaluated using the method of infinitesimal rotations and the Tc was determined by our in-house ...

Latest version: v1

Publication date: Feb 17, 2022

Lorenzo Monacelli, Michele Casula, Kosuke Nakano, Sandro Sorella, Francesco Mauri

- The interplay between electron correlation and nuclear quantum effects makes our understanding of elemental hydrogen a formidable challenge. Here, we present the phase diagram of hydrogen and deuterium at low temperatures and high-pressure (P > 300 GPa) by accounting for highly accurate electronic and nuclear enthalpies. We evaluated internal electronic energies by diffusion quantum Monte Carlo, while nuclear quantum motion and anharmonicity have been included by the stochastic self-consistent harmonic approximation. Our results show that the long-sought atomic metallic hydrogen, predicted to host room-temperature superconductivity, forms at 577±10 GPa (640±14 GPa in deuterium). Indeed, anharmonicity pushes the stability of this phase towards pressures much larger than previous theoretical estimates or attained experimental values. Before atomization, molecular hydrogen transforms from a metallic phase III to another metallic structure that is still molecular (phase VI) at 422±40 ...

Latest version: v1

Publication date: Feb 16, 2022

Junzhang Ma, Simin Nie, Xin Gui, Muntaser Naamneh, Jasmin Jandke, Chuanying Xi, Jinglei Zhang, Tian Shang, Yimin Xiong, Itzik Kapon, Neeraj Kumar, Yeong Soh, Daniel Gosálbez-Martínez, Oleg V. Yazyev, Wenhui Fan, Hannes Hübener, Umberto De Giovannini, Nicholas Clark Plumb, Milan Radovic, Michael Andreas Sentef, Weiwei Xie, Zhijun Wang, Christopher Mudry, Markus Müller, Ming Shi

- Charge neutrality and their expected itinerant nature makes excitons potential transmitters of information. However, exciton mobility remains inaccessible to traditional optical experiments that only create and detect excitons with negligible momentum. Here, using angle-resolved photoemission spectroscopy, we detect dispersing excitons in quasi-one-dimensional metallic trichalcogenide, TaSe₃. The low density of conduction electrons and low dimensionality in TaSe₃ combined with a polaronic renormalization of the conduction band and the poorly screened interaction between these polarons and photo-induced valence holes leads to various excitonic bound states that we interpret as intrachain and interchain excitons, and possibly trions. The thresholds for the formation of a photo-hole together with an exciton appear as side valence bands with dispersions nearly parallel to the main valence band, but shifted to lower excitation energies. The energy separation between side and main ...

Latest version: v1

Publication date: Feb 11, 2022

Jānis Užulis, Andris Gulans

- We present a numerical tool for solving the non-relativistic Kohn-Sham problem for spherically-symmetric atoms. It treats the Schrödinger equation as an integral equation relying heavily on convolutions. The solver supports different types of exchange-correlation functionals including screened and long-range corrected hybrids. We implement a new method for treating range separation based on the complementary error function kernel. The present tool is applied in spin-restricted non-relativistic total energy calculations of atoms. A comparison with ultra-precise reference data[Cinal, JOMC 58, 1571 (2020)] shows a 14-digit agreement for Hartree-Fock results. We provide further benchmark data obtained with 5 different exchange-correlation functionals: VWN5 (the local-density approximation), PBE (the generalized gradient approximation), PBE0 and B3LYP (hybrids with a Fock exchange) and LC-BLYP (hybrid with a long-range corrected exchange).

Latest version: v1

Publication date: Feb 11, 2022

Jes Larsen, Kostiantyn Sopiha, Clas Persson, Charlotte Platzer-Björkman, Marika Edoff

- The chalcopyrite Cu(In,Ga)S2 has gained renewed interest in recent years due to its potential application in tandem solar cells. In this contribution, a combined theoretical and experimental approach is applied to investigate stable and metastable phases forming in sputtered CuInS2 (CIS) thin films. Ab initio calculations are performed to obtain formation energies, X-ray diffraction patterns, and Raman spectra of various CIS polytypes and related compounds. Multiple low-energy CIS structures with zinc-blende and wurtzite-derived lattices are identified and their XRD/Raman patterns are shown to contain many overlapping features, which could lead to misidentification unless the techniques are duly combined and analyzed. The results are verified against experimental XRD/Raman spectra measured on a series of CIS films with different compositions and treated at different temperatures, revealing the formation of several CIS polymorphs and secondary phases. The characteristic features ...

Latest version: v1

Publication date: Feb 08, 2022

Chiara Ricca, Ulrich Aschauer

- Photochemical reactions on semiconductors are anisotropic, since they occur with different rates on surfaces of different orientation. Understanding the origin of this anisotropy is crucial to engineering more efficient photocatalysts. In this work, we use hybrid density functional theory (DFT) to identify the surfaces associated with the largest number of photo-generated carriers in different semiconductors. For each material we create a spherical heat map of the probability of optical transitions at different wave vectors. These maps allow to identify the directions associated with the majority of the photo-generated carriers and can thus be used to make predictions about the most reactive surfaces for photochemical applications. Results indicate that it is generally possible to correlate the heat maps with the anisotropy of the bands observed in conventional band-structure plots, as previously suggested. However, we also demonstrate that conventional bands-structure plots do ...

Latest version: v1

Publication date: Feb 07, 2022

Federico Grasselli

- The effects of the finite size of the simulation box in equilibrium molecular dynamics simulations are investigated for prototypical superionic conductors of different types, namely the fluorite-structure materials PbF2, CaF2, and UO2 (type II), and the alpha phase of AgI (type I). Largely validated empirical force-fields are employed to run ns-long simulations and extract general trends for several properties, at increasing size and in a wide temperature range. This work shows that, for the considered type-II superionic conductors, the diffusivity dramatically depend on the system size and that the superionic regime is shifted to larger temperatures in smaller cells. Furthermore, only simulations of several hundred atoms are able to capture the experimentally-observed, characteristic change in the activation energy of the diffusion process, occurring at the order-disorder transition to the superionic regime. Finite-size effects on ion diffusion are instead much weaker in ...

Latest version: v1

Publication date: Feb 04, 2022

David Kleiven, Jaakko Akola, Andrew Peterson, Tejs Vegge, Jin Hyun Chang

- Cluster expansion (CE) has gained an increasing level of popularity in recent years, and many strategies have been proposed for training and fitting the CE models to first-principles calculation results. The paper reports a new strategy for constructing a training set based on their relevance in Monte Carlo sampling for statistical analysis and reduction of the expected error. We call the new strategy a "bootstrapping uncertainty structure selection" (BUSS) scheme and compared its performance against a popular scheme where one uses a combination of random structure and ground-state search (referred to as RGS). The provided dataset contains the training sets generated using BUSS and RGS for constructing a CE model for disordered Cu2ZnSnS4 material. The files are in the format of the Atomic Simulation Environment (ASE) database (please refer to ASE documentation for more information https://wiki.fysik.dtu.dk/ase/index.html). Each `.db` file contains 100 DFT calculations, which were ...

Latest version: v1

Publication date: Feb 03, 2022

Arrigo Calzolari, Alessandra Catellani

- The paper reports on a theoretical description of work function of TiN, which is one of the most used materials for the realization of electrodes and gates in CMOS devices. Indeed, although the work function is a fundamental quantity in quantum mechanics and also in device physics, as it allows the understanding of band alignment at heterostructures and gap states formation at the metal/semiconductor interface, the role of defects and contaminants is rarely taken into account. Here, by using first principles simulations, we present an extensive study of the work function dependence on nitrogen vacancies and surface oxidation for different TiN surface orientations. The results complement and explain a number of existent experimental data, and provide a useful tool to tailoring transport properties of TiN electrodes in device simulations.

Latest version: v1

Publication date: Feb 01, 2022

Joonyeob Jeon, Gil Ho Yoon, Tejs Vegge, Jin Hyun Chang

- Despite the high promise of Li-metal-based batteries, its commercialization has been hampered due to the formation of dendrites that lead to mechanical instability, energy loss and eventual internal short circuits. The provided dataset consists of the phase-field simulation results for investigating the effect of applied overpotential and operating temperature on dendrite growth. These data are used for elucidating the correlation of overpotential and temperature with the surface modulation during electrodeposition. The simulation cell consists of a Li metal anode and 1M LiPF6 in EC:DMC (1:1), and the electrodeposition process was simulated under the applied overpotential ranging from 0.30 V to 0.44 V with a 0.02 V increment at temperatures from 268 K and 333 K with a 5 K increment. The data contains order parameter, chemical potential and overpotential. The supplied Python script can compute the surface tortuosity, average and maximum Li heights and dendrite height at a given temperature, overpotential and time step.

Latest version: v1

Publication date: Feb 01, 2022

Nakib Protik, Chunhua Li, Miguel Prudena, David Broido, Pablo Ordejon

- elphbolt is a modern Fortran (2018 standard) code for efficiently solving the coupled electron-phonon Boltzmann transport equations from first principles. Using results from density functional and density functional perturbation theory as inputs, it can calculate the effect of the non-equilibrium phonons on the electronic transport (phonon drag) and non-equilibrium electrons on the phononic transport (electron drag) in a fully self-consistent manner and obeying the constraints mandated by thermodynamics. It can calculate the lattice, charge, and thermoelectric transport coefficients for the temperature gradient and electric fields, and the effect of the mutual electron-phonon drag on these transport properties. The code fully exploits the symmetries of the crystal and the transport-active window to allow the sampling of extremely fine electron and phonon wave vector meshes required for accurately capturing the drag phenomena. The coarray feature of modern Fortran, which offers ...

Latest version: v1

Publication date: Feb 01, 2022

Haoyue Guo, Nongnuch Artrith

- This database contains computationally generated atomic structures of glass-ceramics lithium thiophosphates (gc-LPS) with the general composition (Li2S)x(P2S5)1-x in the XCrySDen structure format (XSF). Total energies and interatomic forces from density-functional theory (DFT) calculations are included as additional meta information. The extended XSF format is compatible with the atomic energy network (ænet) package for artificial neural network (ANN) potential construction and application. The DFT calculations used projector-augmented-wave (PAW) pseudopotentials and the Perdew−Burke−Ernzerhof (PBE) exchange-correlation functional as implemented in the Vienna Ab Initio Simulation Package (VASP) and a kinetic energy cutoff of 520 eV. The first Brillouin zone was sampled using VASP’s fully automatic k-point scheme with a length parameter Rk = 25Å. The gc-LPS structures were generated using a combination of different sampling methods. Initial amorphous structure models were generated ...

Latest version: v1

Publication date: Feb 01, 2022

Sebastian Feldmann, Michael Schmiedt, Julian Schlosser, Wolfgang Rimkus, Tobias Stempfle

- In industrial metal forming processes, the generation of datasets for inline and optical quality assessment is expensive and time-consuming. Within the research project SimKI, conventional metal forming plants were digitalized under use of perception-based sensors in combination with a completely redesigned forming tool. The integration of optical quality observation methods connected with a retrofitting approach of the press tool provides the opportunity to generate an information-feedback loop that predicts part defects prior to their occurrence. The SimKI-method additionally combines conventional statistical measurement methods with AI-based defect detection algorithms that are trained by a) generic datasets of a finite-element simulation, b) real component images of a 3D imaging device, and c) a combination of both. The generated datasets are used to accelerate the training of a DNN-based algorithm in order to identify the position and deviation from the agreed quality. The ...

Latest version: v1

Publication date: Jan 31, 2022

Tommaso Chiarotti, Nicola Marzari, Andrea Ferretti

- Dynamical potentials appear in many advanced electronic-structure methods, including self-energies from many-body perturbation theory, dynamical mean-field theory, electronic-transport formulations, and many embedding approaches. Here, we propose a novel treatment for the frequency dependence, introducing an algorithmic inversion method that can be applied to dynamical potentials expanded as sum-over-poles. This approach allows for an exact solution of Dyson-like equations at all frequencies via a mapping to a matrix diagonalization, and provides simultaneously frequency-dependent (spectral) and frequency-integrated (thermodynamic) properties of the Dyson-inverted propagators. The transformation to a sum-over-poles is performed introducing n-th order generalized Lorentzians as an improved basis set to represent the spectral function of a propagator. Numerical results for the homogeneous electron gas at the G0W0 level are provided to argue for the accuracy and efficiency of such ...

Latest version: v2

Publication date: Jan 28, 2022

Amogh Kinikar, Marco Di Giovannantonio, José I. Urgel, Kristjan Eimre, Zijie Qiu, Yanwei Gu, Enquan Jin, Akimitsu Narita, Xiao-Ye Wang, Klaus Müllen, Pascal Ruffieux, Carlo Antonio Pignedoli, Roman Fasel

- In this record we provide the data to support our recent finding on surface catalyzed cycloaromatization. Immobilization of organic building blocks on metal surfaces and their coupling via thermally induced C-C bond formations are developing as an important addition to the toolbox of organic and polymer synthesis. Additional advantages of this technique are the in situ monitoring of the reaction by scanning probe methods and the accessibility of insoluble and reactive carbon nanostructures. The diversity of conceivable products, however, sensitively depends on the number of available on-surface reactions. In the manuscript where the results are discussed, we introduce an unprecedented example, the intermolecular oxidative coupling of isopropyl substituents of arenes. With a new phenylene ring being formed, this [3+3] dimerization can be regarded as a formal cycloaromatization. The synthetic value of this novel reaction is proven by the synthesis of polyarylenes and ...

Latest version: v1

Publication date: Jan 25, 2022

Shiyi Chen, Xuesong Fan, Weidong Li, Baldur Steingrimsson, Peter Liaw

- Fatigue failure of metallic structures is of great concern to industrial applications. A material will not be able to practically useful if it is prone to fatigue failure. To take the advantage of lately emerged high entropy alloys (HEAs) for designing novel fatigue-resistant alloys, we compiled a fatigue database of HEAs from the literature reported till the yearend of 2021. The database is subdivided into three categories, i.e., low-cycle fatigue (LCF), high-cycle fatigue (HCF), and fatigue crack growth rate (FCGR), which contains 15, 23, and 28 distinct data records, respectively. Each data record in any of three categories is characteristic of a summary, which is comprised of alloy composition, key fatigue properties, and additional information influential to or interrelated with fatigue (e.g., material processing history, phase constitution, grain size, uniaxial tensile properties, and fatigue testing conditions), and an individual dataset, which makes up the original fatigue testing curve.

Latest version: v1

Publication date: Jan 24, 2022

Yi Hu, William Curtin

- Strengthening by needle-shaped β′′ precipitates is critical in Al–Mg–Si alloys. Here, the strengthening is studied computationally at the peak-aged condition where precipitate shearing and Orowan looping are usually considered to have equal strengths. Pseudo-random precipitate microstructures are constructed based on experimental precipitate dimensions and volume fractions at peak aging. A Discrete Dislocation Dynamics method is then adapted to compute the Critical Resolved Shear Stress (CRSS) for Orowan looping of dislocations moving through the non-shearable precipitate field. The CRSS for Orowan looping is determined by a typical in-situ precipitate spacing that is smaller than the average spacing and by the dislocation core energy within a radius of ≈5b, a factor rarely considered. The matrix misfit stresses, volume fraction, and precipitate shape have small effects on the CRSS. With microstructure and property details introduced as faithfully as possible, the CRSS for Orowan ...

Latest version: v1

Publication date: Jan 21, 2022

Ruben Laplaza, Simone Gallarati, Clemence Corminboeuf

- We present the NaviCatGA package, a versatile genetic algorithm capable of optimizing molecular catalyst structures using well-suited fitness functions to achieve a set of targeted properties. The flexibility and generality of this tool are demonstrated with two examples: i) Ligand optimization and exploration for Ni-catalyzed aryl-ether cleavage manipulating SMILES and using a fitness function derived from molecular volcano plots, ii) multiobjective (i.e., activity/selectivity) optimization of bipyridine N.N'-dioxide Lewis basic organocatalysts for the asymmetric propargylation of benzaldehyde from 3D molecular fragments. We show that evolutionary optimization, enabled by NaviCatGA, is an efficient way of accelerating catalyst discovery that bypasses combinatorial scaling issues and incorporates compelling chemical constraints.

Latest version: v1

Publication date: Jan 21, 2022

Varun Venoor, Jo Ann Ratto, David Kazmer, Margaret Sobkowicz

- Melt post-condensation, thermal, and thermo-oxidative degradation of a cyclo-aliphatic polyamide were studied through time-resolved rheometry (TRR). The implemented TRR elucidates structural changes occurring during two concurrent phenomena, namely melt post-condensation and thermal/thermo-oxidative degradation, during the time sweep in a parallel plate rheometer. TRR measurements were conducted on neat polyamide under nitrogen (inert/non-oxidative) and air (oxidative) environment at 3 % strain amplitude and a range of frequencies between 0.1 and 100 rad/sec for two hours. At temperatures of 260, 270, and 275 °C, a dual-stage time-dependent growth in viscoelastic properties was observed under an oxidative environment. Thermo-oxidative degradation of polyamide melt 270 °C was shown to occur from the exposed sample edge, continuing inwards, effectively reducing the radius of the unoxidized polymer melt by 6.4 %. A modeling approach using MATLAB is presented to interpret and ...

Latest version: v1

Publication date: Jan 18, 2022

Francesco Tavanti, Behnood Dianat, Alessandra Catellani, Arrigo Calzolari

- In the upcoming process to overcome the limitations of the standard von Neumann architecture, synaptic electronics is gaining a primary role for the development of in-memory computing. In this field, Ge-based compounds have been proposed as switching materials for nonvolatile memory devices and for selectors. By employing the classical molecular dynamics, we study the structural features of both the liquid states at 1500 K and the amorphous phase at 300 K of Ge-rich and Se-rich chalcogenides binary Ge_x Se_1–x systems in the range 0.4 ≤ x ≤ 0.6. The simulations rely on a model of interatomic potentials where ions interact through steric repulsion, as well as Coulomb and charge–dipole interactions given by the large electronic polarizability of Se ions. Our results indicate the formation of temperature-dependent hierarchical structures with short-range local orders and medium-range structures, which vary with the Ge content. Our work demonstrates that nanosecond-long simulations, ...

Latest version: v1

Publication date: Jan 18, 2022

Moloud Kaviani, Ulrich Aschauer

- Complex oxide functionality, such as ferroelectricity, magnetism or superconductivity is often achieved in epitaxial thin-film geometries. Oxygen vacancies tend to be the dominant type of defect in these materials but a fundamental understanding of their stability and electronic structure has so far mostly been established in the bulk or strained bulk, neglecting interfaces and surfaces present in a thin-film geometry. We investigate here, via density functional theory calculations, oxygen vacancies in the model system of a SrMnO3 (SMO) thin film grown on a SrTiO3 (STO) (001) substrate. Structural and electronic differences compared to bulk SMO result mainly from undercoordination at the film surface. The changed crystal field leads to a depletion of subsurface valence-band states and transfer of this charge to surface Mn atoms, both of which strongly affect the defect chemistry in the film. The result is a strong preference of oxygen vacancies in the surface region compared to ...

Latest version: v1

Publication date: Jan 18, 2022

Francesco Petocchi, Viktor Christiansson, Philipp Werner

- The reliable ab-initio description of strongly correlated materials is a long-sought capability in condensed matter physics. The GW+EDMFT method is a promising scheme, which provides a self-consistent description of correlations and screening, and does not require user-provided parameters. In order to test the reliability of this approach we apply it to the experimentally well characterized perovskite compound Ca₂RuO₄, in which a temperature-dependent structural deformation drives a paramagnetic metal-insulator transition. Our results demonstrate that the nonlocal polarization and self-energy components introduced by GW are essential for setting the correct balance between interactions and bandwidths, and that the GW+EDMFT scheme produces remarkably accurate predictions of the electronic properties of this strongly correlated material.

Latest version: v1

Publication date: Jan 17, 2022

Benjamin K. Chang, Jin-Jian Zhou, Nien-En Lee, Marco Bernardi

- Predicting the electrical properties of organic molecular crystals (OMCs) is challenging due to their complex crystal structures and electron-phonon (e-ph) interactions. Charge transport in OMCs is conventionally categorized into two limiting regimes – band transport, characterized by weak e-ph interactions, and charge hopping due to localized polarons formed by strong e-ph interactions. However, between these two limiting cases there is a less well understood intermediate regime where polarons are present but transport does not occur via hopping. Here we show a many-body first-principles approach that can accurately predict the carrier mobility in OMCs in the intermediate regime and shed light on its microscopic origin. Our approach combines a finite-temperature cumulant method to describe strong e-ph interactions with Green-Kubo transport calculations. We apply this parameter-free framework to naphthalene crystal, demonstrating electron mobility predictions within a factor of ...

Latest version: v2

Publication date: Jan 12, 2022

Paolo Pegolo, Stefano Baroni, Federico Grasselli

- Despite governing heat management in any realistic device, the microscopic mechanisms of heat transport in all-solid-state electrolytes are poorly known: existing calculations, all based on simplistic semi-empirical models, are unreliable for superionic conductors and largely overestimate their thermal conductivity. In this work, we deploy a combination of state-of-the-art methods to calculate the thermal conductivity of a prototypical Li-ion conductor, the Li₃ClO antiperovskite. By leveraging ab initio, machine learning, and forcefield descriptions of interatomic forces, we are able to reveal the massive role of anharmonic interactions and diffusive defects on the thermal conductivity and its temperature dependence, and to eventually embed their effects into a simple rationale which is likely applicable to a wide class of ionic conductors. In this record, we provide data and scripts to generate the plots supporting our findings. We also provide the machine learning model and the dataset to train it.

Latest version: v1

Publication date: Jan 11, 2022

Kristjan Eimre, José I. Urgel, Hironobu Hayashi, Marco Di Giovannantonio, Pascal Ruffieux, Shizuka Sato, Satoru Otomo, Yee Seng Chan, Naoki Aratani, Daniele Passerone, Oliver Gröning, Hiroko Yamada, Roman Fasel, Carlo Antonio Pignedoli

- In this record, we provide the data supporting our recent results on the synthesis of nitrogen-substituted undecacene analogs. Heteroatom substitution in acenes allows to tailor their remarkable electronic properties, expected to include spin-polarization and magnetism for larger members of the acene family. Here, we present a strategy for the on-surface synthesis of three undecacene analogs substituted with four nitrogen atoms on an Au(111) substrate, by employing specifically designed diethano-bridged precursors. A similarly designed precursor is used to synthesize the pristine undecacene molecule. In the publication where the results are discussed, the experimental features of scanning probe microscopy are compared with ab initio simulations, to demonstrate that the ground state of the synthesized tetraazaundecacene has considerable open-shell character on Au(111). Additionally, we demonstrate that electronegative nitrogen atoms induce a considerable shift in energy level ...

Latest version: v1

Publication date: Jan 11, 2022

Wenhui Fan, Simin Nie, Cuixiang Wang, Binbin Fu, Changjiang Yi, Shunye Gao, Zhicheng Rao, Dayu Yan, Junzhang Ma, Ming Shi, Yaobo Huang, Youguo Shi, Zhijun Wang, Tian Qian, Hong Ding

- Topological crystalline insulators (TCIs) are insulating electronic states with nontrivial topology protected by crystalline symmetries. Recently, theory has proposed new classes of TCIs protected by rotation symmetries Ĉ_n, which have surface rotation anomaly evading the fermion doubling theorem, i.e., n instead of 2n Dirac cones on the surface preserving the rotation symmetry. Here, we report the first realization of the Ĉ_2 rotation anomaly in a binary compound SrPb. Our first-principles calculations reveal two massless Dirac fermions protected by the combination of time-reversal symmetry T̂ and Ĉ_2y on the (010) surface. Using angle-resolved photoemission spectroscopy, we identify two Dirac surface states inside the bulk band gap of SrPb, confirming the Ĉ_2 rotation anomaly in the new classes of TCIs. The findings enrich the classification of topological phases, which pave the way for exploring exotic behavior of the new classes of TCIs.

Latest version: v1

Publication date: Dec 24, 2021

Daniel Marchand, Curtin William

- AiiDA calculations for the publication Giant hardening response in AlMgZn(Cu) alloys. This study presents a thermomechanical processing concept which is capable of exploiting the full indus- trial application potential of recently introduced AlMgZn(Cu) alloys. The beneficial linkage of alloy design and processing allows not only to satisfy the long-standing trade-off between high mechanical strength in use and good formability during processing but also addresses the need for economically feasible processing times. After an only 3-hour short pre-aging treatment at 100 °C, the two investigated alloys, based on commercial EN AW-5182 and modified with additions of Zn and Zn + Cu respectively, show high formability due to increased work-hardening. Then, these alloys exhibit a giant hardening response of up to 184 MPa to reach a yield strength of 410 MPa after a 20-minute short final heat treatment at 185 °C, i.e. paint-baking. This rapid hardening response strongly depends on the ...

Latest version: v1

Publication date: Dec 21, 2021

Giulio Imbalzano, Michele Ceriotti

- Materials composed of elements from the third and fifth columns of the periodic table display a very rich behavior, with the phase diagram usually containing a metallic liquid phase and a polar semiconducting solid. As a consequence, it is very hard to achieve transferable empirical models of interactions between the atoms that can reliably predict their behavior across the temperature and composition range that is relevant to the study of the synthesis and properties of III/V nanostructures and devices. We present a machine-learning potential trained on density functional theory reference data that provides a general-purpose model for the Ga/As system. We provide a series of stringent tests that showcase the accuracy of the potential, and its applicability across the whole binary phase space, computing with ab initio accuracy a large number of finite-temperature properties as well as the location of phase boundaries. We also show how a committee model can be used to reliably ...

Latest version: v2

Publication date: Dec 20, 2021

Benjamin A. Helfrecht, Rose K. Cersonsky, Guillaume Fraux, Michele Ceriotti

- Data analyses based on linear methods constitute the simplest, most robust, and transparent approaches to the automatic processing of large amounts of data for building supervised or unsupervised machine learning models. Principal covariates regression (PCovR) is an underappreciated method that interpolates between principal component analysis and linear regression, and can be used to conveniently reveal structure-property relations in terms of simple-to-interpret, low-dimensional maps. Here we introduce a kernelized version of PCovR and a sparsified extension, and demonstrate the performance of this approach in revealing and predicting structure-property relations in chemistry and materials science, showing a variety of examples including elemental carbon, porous silicate frameworks, organic molecules, amino acid conformers, and molecular materials.

Latest version: v2

Publication date: Dec 20, 2021

Gabriel M. Nascimento, Elton Ogoshi, Adalberto Fazzio, Carlos Mera Acosta, Gustavo M. Dalpian

- The development of spintronic devices demands the existence of materials with some kind of spin splitting (SS). In this work, we have built a database of ab initio calculated SS in 2D materials. More than that, we propose a workflow for materials design integrating an inverse design approach and a Bayesian inference optimization. We use the prediction of SS prototypes for spintronic applications as an illustrative example of the proposed workflow. The prediction process starts with the establishment of the design principles (the physical mechanism behind the target properties), that are used as filters for materials screening, and followed by density functional theory (DFT) calculations. Applying this process to the C2DB database, we identify and classify 315 2D materials according to SS type at the valence and/or conduction bands. The Bayesian optimization captures trends that are used for the rationalized design of 2D materials with the ideal conditions of band gap and SS for ...

Latest version: v1

Publication date: Dec 17, 2021

Gary Ferkinghoff, Leanna Müller, Umesh Kumar, Götz S. Uhrig, Benedikt Fauseweh

- Stable bound quantum states are ubiquitous in nature. Mostly, they result from the interaction of only pairs of particles, so called two-body interactions, even when large complex many-particle structures are formed. We show that three-particle bound states occur in a generic, experimentally accessible solid state system: antiferromagnetic spin ladders, related to high-temperature superconductors. Strikingly, this binding is induced by genuine three-particle interactions; without them there is no bound state. We compute the dynamic exchange structure factor required for the experimental detection of the predicted state by resonant inelastic x-ray scattering for realistic material parameters. Our work enables us to quantify these elusive interactions and unambiguously establishes their effect on the dynamics of the quantum many-particle state. The data provided here contains the Green function and the weights of the dynamic exchange structure factor and the corresponding Lanczos coefficients.

Latest version: v1

Publication date: Dec 17, 2021

Jonathan Schmidt, Love Pettersson, Claudio Verdozzi, Silvana Botti, Miguel Marques

- Graph neural networks have enjoyed great success in the prediction of material properties for both molecules and crystals. These networks typically use the atomic positions (usually expanded in a Gaussian basis) and the atomic species as input. Unfortunately, this information is in general not available when predicting new materials, for which the precise geometrical information is unknown. In this work, we circumvent this problem by predicting the thermodynamic stability of crystal structures without using the knowledge of the precise bond distances. We replace this information with embeddings of graph distances, allowing our networks to be used directly in high-throughput studies based on both composition and crystal structure prototype. Using these embeddings, we combine the newest developments in graph neural networks and apply them to the prediction of the distances to the convex hull. To train these networks, we curate a dataset of over 2 million density-functional ...

Latest version: v2

Publication date: Dec 16, 2021

Alberto Fabrizio, Ksenia R. Briling, Clemence Corminboeuf

- Physics-inspired molecular representations are the cornerstone of similarity-based learning applied to solve chemical problems. Despite their conceptual and mathematical diversity, this class of descriptors shares a common underlying philosophy: they all rely on the molecular information that determines the form of the electronic Schrödinger equation. Existing representations take the most varied forms, from non-linear functions of atom types and positions to atom densities and potential, up to complex quantum chemical objects directly injected into the ML architecture. In this work, we present the Spectrum of Approximated Hamiltonian Matrices (SPAᴴM) as an alternative pathway to construct quantum machine learning representations through leveraging the foundation of the electronic Schrödinger equation itself: the electronic Hamiltonian. As the Hamiltonian encodes all quantum chemical information at once, SPAᴴM representations not only distinguish different molecules and ...

Latest version: v1

Publication date: Dec 15, 2021

Michele Simoncelli, Nicola Marzari, Francesco Mauri

- Two different heat-transport mechanisms are discussed in solids: in crystals, heat carriers propagate and scatter like particles, as described by Peierls' formulation of Boltzmann transport equation for phonon wavepackets; in glasses, instead, carriers behave wave-like, diffusing via a Zener-like tunneling between quasi-degenerate vibrational eigenstates, as described by the Allen-Feldman equation. Recently, it has been shown that these two conduction mechanisms emerge as limiting cases from a unified transport equation, which describes on an equal footing solids ranging from crystals to glasses; moreover, in materials with intermediate characteristics the two conduction mechanisms coexist, and it is crucial to account for both. Here, we discuss the theoretical foundations of such transport equation as is derived from the Wigner phase-space formulation of quantum mechanics, elucidating how the interplay between disorder, anharmonicity, and the quantum Bose-Einstein statistics of ...

Latest version: v1

Publication date: Dec 15, 2021

Aleksandra Nelson, Titus Neupert, Tomáš Bzdušek, Aris Alexandradinata

- Being Wannierizable is not the end of the story for topological insulators. We introduce a family of topological insulators that would be considered trivial in the paradigm set by the tenfold way, topological quantum chemistry, and the method of symmetry-based indicators. Despite having a symmetric, exponentially localized Wannier representation, each Wannier function cannot be completely localized to a single primitive unit cell in the bulk. Such multicellular topology is shown to be neither stable nor fragile, but delicate; i.e., the topology can be nullified by adding trivial bands to either valence or conduction band.

Latest version: v1

Publication date: Dec 13, 2021

Behnam Parsaeifard, Daniele Tomerini, Deb Sankar De, Stefan Goedecker

- Fingerprint distances, which measure the similarity of atomic environments, are commonly calculated from atomic environment fingerprint vectors. In this work, we present the simplex method that can perform the inverse operation, i.e., calculating fingerprint vectors from fingerprint distances. The fingerprint vectors found in this way point to the corners of a simplex. For a large dataset of fingerprints, we can find a particular largest simplex, whose dimension gives the effective dimension of the fingerprint vector space. We show that the corners of this simplex correspond to landmark environments that can be used in a fully automatic way to analyze structures. In this way, we can, for instance, detect atoms in grain boundaries or on edges of carbon flakes without any human input about the expected environment. By projecting fingerprints on the largest simplex, we can also obtain fingerprint vectors that are considerably shorter than the original ones but whose information content is not significantly reduced.

Latest version: v1

Publication date: Dec 13, 2021

Jigyasa Nigam, Michael J. Willatt, Michele Ceriotti

- The application of machine learning to the modeling of materials and molecules has proven to be extremely successful in accelerating the understanding, design, and characterization of materials. A major factor in this success has been the development of representations of atomic structures that reflect physics-based symmetries of the underlying interactions. Most of the descriptions of atomic properties or even global observables rely on decompositions into atomic contributions that are subsequently learnt in an atom-centered framework. However, many quantities associated with quantum mechanical calculations, such as the single-particle Hamiltonian matrices written in an atomic-orbital basis, are associated with multiple atom-centers. Following the introduction of equivariant N-center structural descriptors, in the reference below, that generalize the very successful atom-centered density correlation features to the problem of learning properties indexed by N atoms, we present ...

Latest version: v1

Publication date: Dec 09, 2021

Frederick Stein, Jürg Hutter

- Due to their high accuracy, Double-Hybrid Density functionals emerged to important methods for molecular electronic-structure calculations. The high computational costs of double-hybrid calculations in condensed phase and the lack of efficient gradient implementations thereof inhibit a wide applicability for periodic systems. We present an implementation of gradients for Double-Hybrid functional theory into CP2K. The Auxiliary Density Matrix Method (ADMM) reduces the overhead from the Hartree-Fock calculations providing an efficient and accurate methodology to tackle condensed phase systems. First applications to water containing systems of different densities and molecular crystals pave the way for advanced studies. We present large benchmark systems to discuss the efficiency of our methodology on modern super computing hardware.

Latest version: v1

Publication date: Dec 09, 2021

Sara Fiore, Mathieu Luisier, Fabian Ducry, Cedric Klinkert, Jonathan Backman

- An ab initio study of the coupled electrons and phonon transport properties of MoS2-hBN devices. A comparison of the device characteristics when hBN is treated as a perfectly insulating, non vibrating layer and one where it is included in the DFT together with MoS2.

Latest version: v1

Publication date: Dec 08, 2021

Sijin Ren, Eric Fonseca, William Perry, Hai-Ping Cheng, Xiao-Guang Zhang, Richard Hennig

- This record contains data structures used in the manuscript titled Ligand optimization of exchange interaction in Co(II) dimer single molecule magnet by machine learning. Designing single-molecule magnets (SMMs) for potential applications in quantum computing and high-density data storage requires tuning their magnetic properties, especially the strength of the magnetic interaction. These properties can be characterized by first-principles calculation based on density functional theory (DFT). In this work, we study the experimentally synthesized Co(II) dimer SMM with the goal to control the exchange energy between the Co atoms through tuning of the capping ligands. The experimentally synthesized Co(II) dimer molecule has a very small exchange energy (< 1meV). We assemble a DFT dataset of 1081 ligand-substitutions for the Co(II) dimer. The ligand exchange provides a broad range of exchange energies from +50 meV to -200 meV, with 80% of the ligands yielding a small exchange ...

Latest version: v1

Publication date: Dec 07, 2021

Rahul Bhowmik, Sangwook Sihn, Ruth Pachter, Jonathan Vernon

- We have developed a polymer descriptor data set from the existing data. The data set has 188 descriptors which describe polymer atomic and molecular behavior. The descriptors are mapped to the specific heat of polymers using supervised and unsupervised machine learning approaches. The mapping helps predict the specific heat of polymers at room temperature. The descriptor data set is useful in synthesizing novel polymers with desired heat capacities.

Latest version: v2

Publication date: Dec 06, 2021

Sara Fiore, Mathieu Luisier

- An advanced modeling approach is presented to shed light on the thermal transport properties of van der Waals materials (vdWMs) composed of single-layer transition metal dichalcogenides (TMDs) stacked on top of each other with a total or partial overlap only in the middle region. It relies on the calculation of dynamical matrices from first principles and on their usage in a phonon quantum transport simulator. We observe that vibrations are transferred microscopically from one layer to the other along the overlap region which acts as a filter selecting out the states that can pass through it. Our work emphasizes the possibility of engineering heat flows at the nanoscale by carefully selecting the TMD monolayers that compose vdWMs.

Latest version: v2

Publication date: Dec 06, 2021

Edoardo Martino, Carsten Putzke, Markus König, Philip J. W. Moll, Helmuth Berger, David LeBoeuf, Maxime Leroux, Cyril Proust, Ana Akrap, Holm Kirmse, Christophe Koch, ShengNan Zhang, QuanSheng Wu, Oleg V. Yazyev, László Forró, Konstantin Semeniuk

- Crystalline defects can modify quantum interactions in solids, causing unintuitive, even favourable, properties such as quantum Hall effect or superconducting vortex pinning. Here we present another example of this notion—an unexpected unidirectional Kondo scattering in single crystals of 2H-NbS2. This manifests as a pronounced low-temperature enhancement in the out-of-plane resistivity and thermopower below 40 K, hidden for the in-plane charge transport. The anomaly can be suppressed by the c-axis-oriented magnetic field, but is unaffected by field applied along the planes. The magnetic moments originate from layers of 1T-NbS2, which inevitably form during the growth, undergoing a charge-density-wave reconstruction with each superlattice cell (David-star-shaped cluster of Nb atoms) hosting a localized spin. Our results demonstrate the unique and highly anisotropic response of a spontaneously formed Kondo-lattice heterostructure, intercalated in a layered conductor.

Latest version: v1

Publication date: Dec 06, 2021

Shoya Sakamoto, Masahito Tsujikawa, Masafumi Shirai, Kenta Amemiya, Shinji Miwa

- The Fe(CoB)/MgO interface is vital to spintronics as it exhibits the tunneling magnetoresistance (TMR) effect and interfacial perpendicular magnetic anisotropy (PMA) simultaneously. To further enhance TMR and PMA for the development of high-density magnetoresistive random access memory, it is essential to clarify the behavior of Fe atoms interfaced with MgO. This study reveals that the spin and orbital magnetic moments of Fe are enhanced at the Fe/MgO interface. The enhancement in the orbital magnetic moment is much more significant than that predicted by the standard density functional theory. Theoretical calculations based on the orbital polarization correction reproduce this enhancement, the origin of which is attributed to the electron-electron correlation resulting from electron localization at the Fe/MgO interface. The present findings highlight the importance of electro--electron correlation at ferromagnet/oxide interfaces, which has often been disregarded in spintronics, and provide a new perspective in materials design.

Latest version: v1

Publication date: Dec 06, 2021

Pablo M. Piaggi, Roberto Car

- We study the phase equilibrium between liquid water and ice Ih modeled by the TIP4P/Ice interatomic potential using enhanced sampling molecular dynamics simulations. Our approach is based on the calculation of ice Ih-liquid free energy differences from simulations that visit reversibly both phases. The reversible interconversion is achieved by introducing a static bias potential as a function of an order parameter. The order parameter was tailored to crystallize the hexagonal diamond structure of oxygen in ice Ih. We analyze the effect of the system size on the ice Ih-liquid free energy differences, and we obtain a melting temperature of 270 K in the thermodynamic limit. This result is in agreement with estimates from thermodynamic integration (272 K) and coexistence simulations (270 K). Since the order parameter does not include information about the coordinates of the protons, the spontaneously formed solid configurations contain proton disorder as expected for ice Ih.

Latest version: v1

Publication date: Dec 06, 2021

Michele Pizzochero, Kristiāns Čerņevičs, Gabriela Borin Barin, Shiyong Wang, Pascal Ruffieux, Roman Fasel, Oleg V. Yazyev

- On-surface synthesis has recently emerged as an effective route towards the atomically precise fabrication of graphene nanoribbons (GNRs) of controlled topologies and widths. However, whether and to what degree structural disorder occurs in the resulting samples is a crucial issue for prospective applications that remains to be explored. Here, we experimentally visualize ubiquitous missing benzene rings at the edges of 9-atom wide armchair nanoribbons that form upon cleavage of phenyl groups in the precursor molecules. These defects are referred to as ‘bite’ defects. First, we address their density and spatial distribution on the basis of scanning tunnelling microscopy and find that they exhibit a strong tendency to aggregate. Next, we explore their effect on the quantum charge transport from first-principles calculations, revealing that such imperfections substantially disrupt the conduction properties at the band edges. Finally, we generalize our theoretical findings to wider ...

Latest version: v1

Publication date: Dec 03, 2021

Davide Campi, Simran Kumari, Nicola Marzari

- Two-dimensional superconductors attract great interest both for their fundamental physics and for their potential applications, especially in the rapidly growing field of quantum computing. In this, we predict a remarkably high superconducting critical temperature of 21 K in the easily exfoliable, topologically nontrivial 2D semimetal W2N3. Furthermore we study how strain and doping can affect its superconducting properties.

Latest version: v1

Publication date: Dec 03, 2021

Yang Xu, Lakshmi Das, Junzhang Ma, Changjiang Yi, Simin Nie, Youguo Shi, Apoorv Tiwari, Stepan Tsirkin, Titus Neupert, Maria Medarde, Ming Shi, Johan Chang, Tian Shang

- As exemplified by the growing interest in the quantum anomalous Hall effect, the research on topology as an organizing principle of quantum matter is greatly enriched from the interplay with magnetism. In this vein, we present a combined electrical and thermoelectrical transport study on the magnetic Weyl semimetal EuCd₂As₂. Unconventional contribution to the anomalous Hall and anomalous Nernst effects were observed both above and below the magnetic transition temperature of EuCd₂As₂, indicating the existence of significant Berry curvature. EuCd₂As₂ represents a rare case in which this unconventional transverse transport emerges both above and below the magnetic transition temperature in the same material. The transport properties evolve with temperature and field in the antiferromagnetic phase in a different manner than in the paramagnetic phase, suggesting different mechanisms to their origin. Our results indicate EuCd₂As₂ is a fertile playground for investigating the interplay ...

Latest version: v1

Publication date: Dec 02, 2021

Zsuzsanna Koczor-Benda, Philippe Roelli, Christophe Galland, Edina Rosta

- We present Molecular Vibration Explorer, a freely accessible online database and interactive tool for exploring vibrational spectra and tensorial light-vibration coupling strength of a large collection of thiolated molecules. The `Gold' version of the database gathers the results from density functional theory calculations on 2'800 commercially available thiol compounds linked to a gold atom, with the main motivation to screen the best molecules for THz and mid-infrared to visible upconversion. Additionally, the `Thiol' version of the database contains results for 1'900 unbound thiolated compounds.They both provide access to a comprehensive set of computed spectroscopic parameters for all vibrational modes of all molecules in the database. Infrared absorption, Raman scattering and vibrational sum- and difference frequency generation cross sections can be simultaneously investigated by the user. Molecules can be screened for various parameters in custom frequency ranges, such as ...

Latest version: v1

Publication date: Dec 01, 2021

J. Terence Blaskovits, Maria Fumanal, Sergi Vela, Yuri Cho, Clémence Corminboeuf

- Singlet fission (SF) is a promising multiexciton-generating process. Its demanding energy splitting criterion - that the S1 energy must be at least twice that of T1 - has limited the range of materials capable of SF. We propose heteroatom oxidation as a robust strategy to achieve sufficient S1/T1 splitting, and demonstrate the potential of this approach for intramolecular SF.

Latest version: v1

Publication date: Dec 01, 2021

Philipp Rüßmann, Jordi Ribas Sobreviela, Moritz Sallermann, Markus Hoffmann, Florian Rhiem, Stefan Blügel

- Landau-Lifshitz-Gilbert (LLG) spin-dynamics calculations based on the extended Heisenberg Hamiltonian is an important tool in computational materials science involving magnetic materials. LLG simulations allow to bridge the gap from expensive quantum mechanical calculations with small unit cells to large supercells where the collective behavior of millions of spins can be studied. In this work we present the AiiDA-Spirit plugin that connects the spin-dynamics code Spirit to the AiiDA framework. AiiDA provides a Python interface that facilitates performing high-throughput calculations while automatically augmenting the calculations with metadata describing the data provenance between calculations in a directed acyclic graph. The AiiDA-Spirit interface thus provides an easy way for high-throughput spin-dynamics calculations. The interface to the AiiDA infrastructure furthermore has the advantage that input parameters for the extended Heisenberg model can be extracted from ...

Latest version: v1

Publication date: Dec 01, 2021

Prashant P. Shinde, Jia Liu, Thomas Dienel, Oliver Gröning, Tim Dumslaff, Markus Mühlinghaus, Akimitsu Narita, Klaus Müllen, Carlo A. Pignedoli, Roman Fasel, Pascal Ruffieux, Daniele Passerone

- A recently developed bottom-up synthesis strategy enables the fabrication of graphene nanoribbons with well-defined width and non-trivial edge structures from dedicated molecular precursors. Here we discuss the synthesis and properties of zigzag nanoribbons (ZGNRs) modified with periodic cove-cape-cove units along their edges. Contrary to pristine ZGNRs, which show antiferromagnetic correlation of their edge states, the edge-modified ZGNRs exhibit a finite single particle band gap without localized edge states. We report the on-surface synthesis of such edge-modified ZGNRs and discuss tunneling conductance dI/dV spectra and dI/dV spatial maps that reveal a noticeable localization of electronic states at the cape units and the opening of a band gap without presence of edge states of magnetic origin. A thorough ab initio investigation of the electronic structure identifies the conditions under which antiferromagnetically coupled, edge-localized states reappear in the electronic ...

Latest version: v1

Publication date: Dec 01, 2021

Joseph R. Nelson, Richard J. Needs, Chris J. Pickard

- Computational searches for new materials are naturally turning from binary systems, to ternary and other multicomponent systems, and beyond. Here, we select the industrially-relevant metals Ti and Al and report the results of an extensive structure prediction study on the ternary titanium-carbon-oxygen (Ti-C-O) and aluminium-carbon-oxygen (Al-C-O) systems. We map out for the first time the full phase stability of Ti-C-O and Al-C-O compounds using first-principles calculations, through simple, effcient and highly parallel random structure searching in conjunction with techniques based on complex network theory. This record contains the crystal structures used to generate our ternary convex hulls for these systems. We provide input files for the CASTEP density-functional theory code, crystallographic '.res' files of the relaxed structures, and CASTEP output files showing atomic positions and forces calculated during relaxation.

Latest version: v1

Publication date: Nov 30, 2021

Vitali Nesterov, Mario Wieser, Volker Roth

- With the recent advances in machine learning for quantum chemistry, it is now possible to predict the chemical properties of compounds and to generate novel molecules. Existing generative models mostly use a string- or graph-based representation, but the precise three-dimensional coordinates of the atoms are usually not encoded. First attempts in this direction have been proposed, where autoregressive or GAN-based models generate atom coordinates. Those either lack a latent space in the autoregressive setting, such that a smooth exploration of the compound space is not possible, or cannot generalize to varying chemical compositions. We propose a new approach to efficiently generate molecular structures that are not restricted to a fixed size or composition. Our model is based on the variational autoencoder which learns a translation-, rotation-, and permutation-invariant low-dimensional representation of molecules. Our experiments yield a mean reconstruction error below 0.05 ...

Latest version: v1

Publication date: Nov 28, 2021

Aik Rui Tan, Shingo Urata, Masatsugu Yamada, Rafael Gómez-Bombarelli

- Understanding the structure of glassy materials represents a tremendous challenge for both experiments and computations. Despite decades of scientific research, for instance, the structural origin of the density anomaly in silica glasses is still not well understood. Atomistic simulations based on molecular dynamics (MD) produce atomically resolved structure, but extracting insights about the role of disorder in the density anomaly is challenging. Here, we propose to quantify the topological differences between structural arrangements from MD trajectories using a graph-theoretical approach, such that structural differences in silica glasses that exhibit density anomaly can be captured. To balance the accuracy and speed of the MD simulations, we utilized force matching potentials to generate the silica glass structures. This approach involves casting all-atom glass configurations as networks, and subsequently applying a graph-similarity metric (D-measure). Calculated D-measure ...

Latest version: v1

Publication date: Nov 25, 2021

Venkat Kapil, Edgar Engel, Mariana Rossi, Michele Ceriotti

- Quantitative evaluation of the thermodynamic properties of materials—most notably their stability, as measured by the free energy—must take into account the role of thermal and zero-point energy fluctuations. While these effects can easily be estimated within a harmonic approximation, corrections arising from the anharmonic nature of the interatomic potential are often crucial and require computationally costly path integral simulations to obtain results that are essentially exact for a given potential. Consequently, different approximate frameworks for computing affordable estimates of the anharmonic free energies have been developed over the years. Understanding which of the approximations involved are justified for a given system, and therefore choosing the most suitable method, is complicated by the lack of comparative benchmarks. To facilitate this choice we assess the accuracy and efficiency of some of the most commonly used approximate methods: the independent mode ...

Latest version: v2

Publication date: Nov 23, 2021

Venkat Kapil, David Wilkins, Jinggang Lan, Michele Ceriotti

- The properties of molecules and materials containing light nuclei are affected by their quantum mechanical nature. Accurate modeling of these quantum nuclear effects requires computationally demanding path integral techniques. Considerable success has been achieved in reducing the cost of such simulations by using generalized Langevin dynamics to induce frequency-dependent fluctuations. Path integral generalized Langevin equation methods, however, have this far been limited to the study of static, thermodynamic properties due to the large perturbation to the system’s dynamics induced by the aggressive thermostatting. Here, we introduce a post-processing scheme, based on analytical estimates of the dynamical perturbation induced by the generalized Langevin dynamics, which makes it possible to recover meaningful time correlation properties from a thermostatted trajectory. We show that this approach yields spectroscopic observables for model and realistic systems that have an ...

Latest version: v2

Publication date: Nov 23, 2021

Riccardo De Gennaro, Nicola Colonna, Edward Linscott, Nicola Marzari

- Koopmans-compliant functionals provide a novel orbital-density-dependent framework for an accurate evaluation of spectral properties; they are obtained by imposing a generalized piecewise-linearity condition on the total energy of the system with respect to the occupation of any orbital. In crystalline materials, due to the orbital-density-dependent nature of the functionals, minimization of the total energy to a ground state provides a set of minimizing variational orbitals that are localized, and thus break the periodicity of the underlying lattice. Despite this, we show that Bloch symmetry can be preserved and it is possible to describe the electronic states with a band-structure picture, thanks to the Wannier-like character of the variational orbitals. We also present a method to unfold and interpolate the electronic bands from supercell (Gamma-point) calculations, which enables us to calculate full band structures with Koopmans-compliant functionals. The results obtained for ...

Latest version: v1

Publication date: Nov 19, 2021

Nataliya Lopanitsyna, Chiheb Ben Mahmoud, Michele Ceriotti

- Atomistic simulations provide insights into structure-property relations on an atomic size and length scale that are complementary to the macroscopic observables that can be obtained from experiments. Quantitative predictions, however, are usually hindered by the need to strike a balance between the accuracy of the calculation of the interatomic potential and the modelling of realistic thermodynamic conditions. Machine-learning techniques make it possible to efficiently approximate the outcome of accurate electronic-structure calculations that can, therefore, be combined with extensive thermodynamic sampling. We take elemental nickel as a prototypical material, whose alloys have applications from cryogenic temperatures up to close to their melting point and use it to demonstrate how a combination of machine-learning models of electronic properties and statistical sampling methods makes it possible to compute accurate finite-temperature properties at an affordable cost. We ...

Latest version: v1

Publication date: Nov 16, 2021

Giorgio Domenichini, Guido Falk von Rudorff, Otto Anatole von Lilienfeld

- This Dataset contains Supplementary information to the article "Effects of perturbation order and basis set on alchemical predictions" by Giorgio Domenichini, Guido Falk von Rudorff and O. Anatole von Lilienfeld. Our numerical analysis of potential energy estimates, and resulting binding curves, is based on CCSD reference results, and is limited to all neutral diatomics with 14 electrons (AlH ... N2). From those data can be predicted binding energy, equilibrium distance, and vibrational frequencies of neighboring out-of-sample diatomics with near CCSD quality using perturbations up to 5th order. The data stored as Comma Separated Value files (.csv) contain all the predictions within the 14 electron diatomics series, those are referred to the sections IIIA-IIIE of the article. To every file corresponds one of the eight basis sets used. The data are stored using consistently atomic units: Bohrs for length, electrons for charge and Hartrees for energy. For a better visualization ...

Latest version: v1

Publication date: Nov 16, 2021

Jaime Souto-Casares, Nicola A. Spaldin, Claude Ederer

- We address the long-standing question of the nature of oxygen vacancies in strontium titanate, using a combination of density functional theory and dynamical mean-field theory (DFT+DMFT) to investigate in particular the effect of vacancy-site correlations on the electronic properties. Our approach uses a minimal low-energy electronic subspace including the Ti-t2g orbitals plus an additional vacancy-centered Wannier function, and it provides an intuitive and physically transparent framework to study the effect of the local electron-electron interactions on the excess charge introduced by the oxygen vacancies. We estimate the strength of the screened interaction parameters using the constrained random phase approximation, and we find a sizable Hubbard U parameter for the vacancy orbital. Our main finding, which reconciles previous experimental and computational results, is that the ground state is either a state with double occupation of the localized defect state or a state with a ...

Latest version: v1

Publication date: Nov 09, 2021

Vladimir Fel'k, Sergey Komogortsev

- Ferromagnetic resonance fields in a microtube with the various ratio of the inner and outer diameter of the tube β were studied using micromagnetic simulation. For β < 0.15 the resonance field agrees with the prediction of the Kittel equation for an infinite ferromagnetic cylinder for both parallel and perpendicular orientation of the applied field to its axis. For β > 0.15 the resonance field increases from the resonance field of the infinite cylinder and approaches the level of the film magnetized along the plane. This behavior was at odds both with the prediction that can be made using analytically calculated demagnetizing factor in ferromagnetic tube, and with the prediction that use the empirical dependence of the demagnetizing field on β, established from the magnetization curves. For β > 0.15 and transverse applied field a number of resonance peaks were observed.

Latest version: v2

Publication date: Nov 05, 2021

Pedram Tavadze, Reese Boucher, Guillermo Avendaño-Franco, Keenan X. Kocan, Sobhit Singh, Viviana Dovale-Farelo, Wilfredo Ibarra-Hernández, Matthew B Johnson, David S. Mebane, Aldo H Romero

- Density-functional theory is widely used to predict the physical properties of materials. However, it usually fails for strongly correlated materials. A popular solution is to use the Hubbard corrections to treat strongly correlated electronic states. Unfortunately, the exact values of the Hubbard U and J parameters are initially unknown, and they can vary from one material to another. In this semi-empirical study, we explore the U and J parameter space of a group of iron-based compounds to simultaneously improve the prediction of physical properties (volume, magnetic moment, and bandgap). We used a Bayesian calibration assisted by Markov chain Monte Carlo sampling for three different exchange-correlation functionals (LDA, PBE, and PBEsol). We found that LDA requires the largest U correction. PBE has the smallest standard deviation and its U and J parameters are the most transferable to other iron-based compounds. Lastly, PBE predicts lattice parameters reasonably well without the Hubbard correction.

Latest version: v1

Publication date: Nov 03, 2021

Michele Pizzochero, Gabriela Borin Barin, Kristiāns Čerņevičs, Shiyong Wang, Pascal Ruffieux, Roman Fasel, Oleg V. Yazyev

- We unveil the nature of the structural disorder in bottom-up zigzag graphene nanoribbons along with its effect on the magnetism and electronic transport on the basis of scanning probe microscopies and first-principles calculations. We find that edge-missing m-xylene units emerging during the cyclodehydrogenation step of the on-surface synthesis are the most common point defects. These “bite” defects act as spin-1 paramagnetic centers, severely disrupt the conductance spectrum around the band extrema, and give rise to spin-polarized charge transport. We further show that the electronic conductance across graphene nanoribbons is more sensitive to “bite” defects forming at the zigzag edges than at the armchair ones. Our work establishes a comprehensive understanding of the low-energy electronic properties of disordered bottom-up graphene nanoribbons.

Latest version: v1

Publication date: Nov 03, 2021

Gilles Buchs, Magdalena Marganska, Jhon W. González, Kristjan Eimre, Carlo A. Pignedoli, Daniele Passerone, Andres Ayuela, Oliver Gröning, Dario Bercioux

- In this record we provide data to support our recent findings related to carbon nanotube based quantum dots for tunable terahertz detection. Generating and detecting radiation in the technologically relevant range of the so-called terahertz gap (0.1–10 THz) is challenging because of a lack of efficient sources and detectors. Quantum dots in carbon nanotubes have shown great potential to build sensitive terahertz detectors, usually based on photon-assisted tunneling. A recently reported mechanism combining resonant quantum dot transitions and tunneling barrier asymmetries results in a narrow linewidth photocurrent response with a large signal-to-noise ratio under weak THz radiation. That device was sensitive to one frequency, corresponding to transitions between equidistant quantized states. In this work we show, using numerical simulations together with scanning tunneling spectroscopy studies of a defect-induced metallic zigzag single-walled carbon nanotube quantum dot, that ...

Latest version: v1

Publication date: Nov 02, 2021

Youseung Lee, Tarun Agarwal, Mathieu Luisier

- We present an ab initio modeling framework to simulate Majorana transport in 2D semiconducting materials, paving the way for topological qubits based on 2D nanoribbons. By combining density-functional-theory and quantum transport calculations, we show that the signature of Majorana bound states (MBSs) can be found in 2D material systems as zero-energy modes with peaks in the local density-of-states. The influence of spin-orbit coupling and external magnetic fields on Majorana transport is studied for two relevant 2D materials, WSe2 and PbI2. To illustrate the capabilities of the proposed ab initio platform, a device structure capable of hosting MBSs is created from a PbI2 nanoribbon and carefully investigated. These results are compared to InSb nanowires and used to provide design guidelines for 2D topological qubits.

Latest version: v1

Publication date: Oct 31, 2021

Maximilian E. Merkel, Claude Ederer

- We explore the transition to a charge-disproportionated insulating phase in a five-orbital cubic tight-binding model applicable to transition-metal perovskites with a formal d^4 occupation of the transition-metal cation, such as ferrates or manganites. We use dynamical mean-field theory to obtain the phase diagram as a function of the average local Coulomb repulsion U and the Hund's coupling J. The main structure of the phase diagram follows from the zero band-width (atomic) limit and represents the competition between high-spin and low-spin homogeneous and an inhomogeneous charge-disproportionated state. This results in two distinct insulating phases: the standard homogeneous Mott insulator and the inhomogeneous charge-disproportionated insulator, recently also termed Hund's insulator. We characterize the unconventional nature of this Hund's insulating state. Our results are consistent with previous studies of two- and three-orbital models applicable to isolated t2g and eg ...

Latest version: v1

Publication date: Oct 29, 2021

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