2026-05-13T06:50:37Z https://archive.materialscloud.org/oai2d

oai:materialscloud.org:k45dq-ebf35 2026-01-26T11:11:41Z openaire_data community-mcarchive

Cignarella, Chiara Bastonero, Lorenzo Monacelli, Lorenzo Marzari, Nicola Cignarella, Chiara Bastonero, Lorenzo Monacelli, Lorenzo Marzari, Nicola 2025-09-29 Ultrathin nanowires could play a central role in next-generation downscaled electronics. Here, we explore some of the most promising candidates identified from previous high-throughput screening: CuC2, TaSe3, and AuSe2, to gain insight into the thermodynamic and anharmonic behaviors of nanowires that could be exfoliated from weakly-bonded three-dimensional materials. We analyze thermal stability, linear thermal expansion, and anharmonic heat capacity using the stochastic self-consistent harmonic approximation. Notably, our work unveils exotic features common among all the 1D wires: a colossal record negative thermal expansion and very large deviations from the Dulong-Petit law due to strong anharmonicity. application/zip text/plain https://doi.org/10.24435/materialscloud:fj-20 oai:materialscloud.org:k45dq-ebf35 mcid:2025.149 eng Materials Cloud https://doi.org/10.48550/arXiv.2508.07971 https://doi.org/10.1021/acs.nanolett.5c04282 https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:t7-14 info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode one-dimensional materials SSCHA anharmonicity negative thermal expansion heat capacity density-functional-theory Extreme anharmonicity and thermal contraction of 1D wires info:eu-repo/semantics/other

oai:materialscloud.org:avdyj-b2m14 2026-03-06T15:32:32Z openaire_data community-mcarchive

Royo, Miquel Royo, Miquel Stengel, Massimiliano 2026-02-03 Noncollinear magnets are notoriously difficult to describe within first-principles approaches based on density-functional theory (DFT) because of the presence of low-lying spin excitations. At the level of ground-state calculations, several methods exist to constrain the magnetic moments to a predetermined configuration, and thereby accelerate convergence towards self-consistency. Their use in a perturbative context, however, remains very limited. Here we present a general methodological framework to achieve parametric control over the local spin moments at the linear-response level. Our strategy builds on the concept of Legendre transform to switch between various flavors of magnetic functionals, and to relate their second derivatives via simple linear-algebra operations. Thereby, we can address an arbitrary response function at the time-dependent DFT level of theory with optimal accuracy and minimal computational effort. In the low frequency limit, we identify the leading correction to the existing adiabatic formulation of the problem [S. Ren , Phys. Rev. X 14, 011041 (2024)], consisting in a renormalization of the phonon and magnon masses due to electron inertia. As a demonstration, we apply our methodology to the THz optical response of bulk CrI3 and Cr2O3, where we identify contributions from hybrid (electro)magnons with mixed spin-lattice character.  This dataset contains the input and output files used to produce the results presented in sections V and VI of the manuscript.   application/gzip text/plain https://doi.org/10.24435/materialscloud:1n-wg oai:materialscloud.org:avdyj-b2m14 mcid:2026.33 eng Materials Cloud https://doi.org/10.1103/c68v-8tkb https://doi.org/10.48550/arXiv.2501.10188 https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:38-0h info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode Magnetic insulators Nonadiabatic regime Density-functional perturbation theory Magnon-phonon coupling Dynamical response of noncollinear spin systems at constrained magnetic moments info:eu-repo/semantics/other

oai:materialscloud.org:0n7bp-3dg82 2025-07-18T08:25:50Z openaire_data community-mcarchive

Lustemberg, Pablo G. Ganduglia-Pirovano, M. Verónica Rodríguez, José A. Fernández Villanueva, Estefanía Ramírez, Pedro J. Lustemberg, Pablo G. Pérez, Rubén Ganduglia-Pirovano, M. Verónica Rodríguez, José A. 2025-07-18 The direct conversion of methane-to-methanol remains a critical challenge in methane valorization. In this study, we unveil the crucial role of PdAu/CeO2 catalysts in enabling selective methane transformation under mild conditions, using only water as the sole oxidant. Through a combination of experimental techniques, including XPS and catalytic testing, alongside density functional theory (DFT) calculations, we demonstrate that a Pd0.3Au0.7/CeO2 catalyst, which predominantly exposes isolated Pd atoms, achieves remarkable methanol selectivity (&sim;80%) at 500 K with a 1:1 methaneto-water ratio. While Pd/CeO2 efficiently activates methane, its tendency for overreaction leads to complete methanol decomposition, thereby limiting selectivity. Alloying Pd withAu on ceria mitigates this over-reactivity, preventing methanol degradation while maintaining sufficient catalytic activity. The PdAu/CeO2 composite exhibits a synergistic effect: Pd in contact with the ceria support facilitates methane activation and water dissociation, while Au fine-tunes reactivity to promote methanol formation. DFT calculations confirm that isolated Pd sites at the PdAu/CeO2 interface play a key role in balancing activity and selectivity. This work underscores the importance of alloy/oxide interfaces in controlling selective methane conversion with water and offers valuable insights for designing highly efficient catalysts for methanol synthesis. application/gzip text/markdown text/plain https://doi.org/10.24435/materialscloud:nc-b8 oai:materialscloud.org:0n7bp-3dg82 mcid:2025.111 eng Materials Cloud https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:4y-bf info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode Computational chemistry Heterogeneous catalysis Methane to methanol CH4 CH3OH Gold Palladium CeO2 ceria Alloy Bimetallic Nanoparticle DFT GOFEE Engineering PdAu/CeO2 alloy/oxide interfaces for selective methane-to-methanol conversion with water info:eu-repo/semantics/other

oai:materialscloud.org:8dhnc-d7064 2026-02-26T16:36:06Z openaire_data community-mcarchive

Enrico, Di Lucente Flaviano José, dos Santos Enrico, Di Lucente Flaviano José, dos Santos Nicola, Marzari 2026-02-03 Skutterudites are promising materials for thermoelectric and spintronics applications. Here we explore spin fluctuations in the FeSb3 skutterudite and their effect on its electronic structure using Hubbard-corrected density-functional theory calculations. We identify multiple magnetic and charge-disproportionated configurations, with an antiferromagnetic metallic ground state. Paramagnetic fluctuations modeled through a special quasirandom spin structure open a 61 meV gap, consistent with experiments. This state features non-degenerate spin channels and band-avoided crossings, hinting at a potential altermagnetic transition with topological features. Mapping the electronic structure to a Heisenberg Hamiltonian fails to explain the low Néel temperature (10 K), highlighting the role of magnetic exchange frustration and the need for more in-depth experimental investigations. This dataset contains first-principles calculations supporting the study “Spin fluctuations steer the electronic behavior in the FeSb₃ skutterudite”. It includes linear-response Hubbard parameters, phonon dispersions, electronic band structures, special quasirandom structures modeling of paramagnetism, and magnetic exchange interactions for FeSb₃. The data document how spin fluctuations stabilize the structure, open a small electronic gap, and strongly affect magnetic energetics. application/zip text/plain https://doi.org/10.24435/materialscloud:34-sg oai:materialscloud.org:8dhnc-d7064 mcid:2026.34 eng Materials Cloud https://doi.org/10.1103/lyy4-cmf6 https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:wg-as info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode magnetism condensed matter physics first-principles simulations special quasi random structures paramagnetism spin fluctuations Heisenberg model Spin fluctuations steer the electronic behavior in the FeSb3 skutterudite info:eu-repo/semantics/other

oai:materialscloud.org:z7tes-s0y64 2026-03-16T20:18:36Z openaire_data community-mcarchive

Haxhijaj, Adonis Haxhijaj, Adonis Riemelmoser, Stefan Pasquarello, Alfredo 2026-02-20 The strongly constrained and appropriately normed (SCAN) meta-GGA functional is a milestone achievement of electronic structure theory. Recently, a revised and restored form (r²SCAN) has been suggested as a replacement for SCAN in high-throughput applications. Here, we assess the accuracy and reliability of the r²SCAN meta-GGA functional for the group IV elemental solids carbon (C), silicon (Si), germanium (Ge), and tin (Sn). We show that the r²SCAN functional agrees closely with its parent functional SCAN for elastic constants, bulk moduli, and phonon dispersions, but the numerical stability of r²SCAN is superior. Both meta-GGA functionals outperform standard GGA (Perdew-Burke-Ernzerhof) in terms of accuracy and approach the level of common hybrid functionals (Heyd-Scuseria-Ernzerhof). However, we find that r²SCAN performs much worse than SCAN for the α ↔ β phase transition of both Ge and Sn, yielding larger phase energy differences and transition pressures. Here we make available the raw phonon dispersion data and VASP input files for an example phonon calculation. application/x-xz application/x-xz text/plain https://doi.org/10.24435/materialscloud:dp-1f oai:materialscloud.org:z7tes-s0y64 mcid:2026.44 eng Materials Cloud https://doi.org/10.1103/znkf-3g37 https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:41-8x info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode DFT phonons VASP Lattice dynamics and structural phase stability of group IV elemental solids with the r²SCAN functional info:eu-repo/semantics/other

oai:materialscloud.org:871 2021-05-31T22:01:18Z openaire_data community-mcarchive

El Darai, Théo Cousin, Samuel Stern, Quentin Ceillier, Morgan Kempf, James Eshchenko, Dmitry Melzi, Roberto Schnell, Marc Gremillard, Laurent Bornet, Aurélien Milani, Jonas Vuichoud, Basile Cala, Olivier Montarnal, Damien Jannin, Sami El Darai, Théo Cousin, Samuel Stern, Quentin Ceillier, Morgan Kempf, James Eshchenko, Dmitry Melzi, Roberto Schnell, Marc Gremillard, Laurent Bornet, Aurélien Milani, Jonas Vuichoud, Basile Cala, Olivier Montarnal, Damien Jannin, Sami 2021-05-31 Hyperpolarization by dissolution dynamic nuclear polarization (dDNP) has enabled promising applications in spectroscopy and imaging, but remains poorly widespread due to experimental complexity. Broad democratization of dDNP would require remote preparation and distribution of hyperpolarized samples from dedicated facilities. We describe here new hyperpolarizing polymers (HYPOPs) that can generate radical- and contaminant-free hyperpolarized samples within minutes with lifetimes exceeding hours in the solid state. HYPOPs feature tunable macroporous porosity, with porous volumes up to 80% and concentration of nitroxide radicals grafted in the bulk matrix up to 285 μmol g-1. Analytes can be efficiently impregnated as aqueous/alcoholic solutions and hyperpolarized up to P(13C) =25% within 8 min, through the combination of 1H spin diffusion and 1H →13C cross polarization. Solutions of 13C-analytes of biological interest hyperpolarized in HYPOPs display a very long solid-state 13C relaxation times of 5.7 h at 3.8 K, thus prefiguring transportation over long distances. application/zip application/zip application/zip application/zip application/zip application/zip text/markdown https://doi.org/10.24435/materialscloud:kv-6q oai:materialscloud.org:871 mcid:2021.79 eng Materials Cloud https://doi.org/10.21203/rs.3.rs-123790/v1 https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:27-8f info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode DNP porous polymers hyperpolarization Experimental Porous functionalized polymers enable generating and transporting hyperpolarized mixtures of metabolites info:eu-repo/semantics/other

oai:materialscloud.org:16jd7-0zz18 2025-10-30T16:04:20Z openaire_data community-mcarchive

Li, Wen Shi, Junjie Tangpakonsab, Parinya Lewis Zhang, Bin Haunold, Thomas Genest, Alexander Yigit, Nevzat Atzl, Leonard Kokkonen, Esko Qin, Yong Rupprechter, Günther 2025-10-30 The direct conversion of methane to methanol (DCMM) under continuous flow and atmospheric pressure offers notable environmental benefits and industrial promise, but remains a long-standing challenge due to the difficulty of activating CH4 while avoiding over-oxidation of methanol. Here, we demonstrate that pure ceria (CeO2), without any metal promoters, enables gas-phase DCMM with up to 80 % selectivity at 300–350 °C, upon optimization of the H2O/O2 ratio. At 550 °C, methanol and formaldehyde are formed at rates of 24 and 36 μmol g-1 h-1, respectively-both dropping below 1 μmol g-1 h-1 in the absence of O2. Ex situ transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy confirm that CeO2 maintains structural integrity and resists carbon deposition during reaction. Combining kinetic studies, steady-state in-situ diffuse reflectance infrared Fourier transform spectroscopy (in-situ DRIFTS), and density functional theory (DFT) reveals that hydroxyl groups (OH), generated from water dissociation, play a multifaceted role: they facilitate C–H bond activation, promote methoxy formation, and enhance methanol desorption. In-situ ambient-pressure X-ray photoelectron spectroscopy (AP-XPS) directly reveals the evolution of surface intermediates and shows that co-feeding O2 and H2O suppresses CH3O and CHx accumulation while boosting methanol yield—indicating a rapid intermediate turnover as key to sustained activity. AP-XPS O 1s spectra further highlight that O2 promotes H2O dissociation, regenerating reactive OH groups and maintaining performance at elevated temperature. These findings offer molecular-level insights into how water and oxygen cooperatively tune reactivity, enabling efficient methane-to-methanol conversion on a metal-free oxide catalyst. application/zip application/zip text/plain https://doi.org/10.24435/materialscloud:wn-rx oai:materialscloud.org:16jd7-0zz18 mcid:2025.171 eng Materials Cloud https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:3v-by info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode CeO2 methane to methanol In-situ AP-XPS In-situ DRIFTS reaction mechanism DFT Synergy of oxygen and water in ceria-catalyzed direct conversion of methane to methanol under continuous flow info:eu-repo/semantics/other

oai:materialscloud.org:sy3yy-qj193 2025-12-05T14:54:17Z openaire_data community-mcarchive

Pignedoli, Carlo A. Di Giovannantonio, Marco Kinikar, Amogh Xu, Xiushang Onishi, Takatsugu Ortega-Guerrero, Andres Widmer, Roland Zema, Nicola Hogan, Conor Camilli, Luca Persichetti, Luca Pignedoli, Carlo A. Fasel, Roman Narita, Akimitsu Di Giovannantonio, Marco 2025-12-05 Recent advances in nanomaterials have pushed the boundaries of nanoscale fabrication to the limit of single atoms, particularly in heterogeneous catalysis. Single atom catalysts, comprising minute amounts of transition metals dispersed on inert substrates, have emerged as prominent materials in this domain. However, overcoming the tendency of these single atoms to cluster beyond cryogenic temperatures and precisely arranging them on surfaces with desired local environments pose significant challenges. Employing organic templates for orchestrating and modulating the activity of single atoms holds promise. In recent work, we introduce a novel single-atom platform wherein atoms are firmly anchored to specific coordination sites distributed along carbon-based polymers, synthesised via on-surface synthesis. These platforms exhibit atomic-level structural precision and stability, even at elevated temperatures. The asymmetry in the structure and electronic states at the active sites anticipates the enhanced reactivity of these precisely defined reactive centers. Upon exposure to CO and CO2 gases at low temperatures, the platform demonstrates excellent trapping and conversion capabilities. Fine-tuning the structure and properties of the coordination sites offers unparalleled flexibility in tailoring functionalities, thus opening avenues for previously untapped potential in catalytic applications. This record contains data that support the results presented in the published work. text/plain application/gzip application/octet-stream https://doi.org/10.24435/materialscloud:yp-bp oai:materialscloud.org:sy3yy-qj193 mcid:2025.190 eng Materials Cloud https://doi.org/10.48550/arXiv.2409.13560 https://doi.org/10.1038/s41467-025-66171-3 https://renkulab.io/p/aiida/materials-cloud-archive/sessions/01JZAQ1T34GEE1S98BV1300FXY/start?archive_url=https://archive.materialscloud.org/api/records/sy3yy-qj193/files/calculations.aiida/content https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:gt-3s info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode MARVEL/P4 single atom catalyst DFT on surface synthesis SPM CSCS asymmetric active sites On-surface synthesis of tailored organic platforms for single metal atoms info:eu-repo/semantics/other

oai:materialscloud.org:1475 2022-09-20T14:55:34Z openaire_data community-mcarchive

Hamada, Ikutaro Abidin, Azim Fitri Zainul Hamada, Ikutaro 2022-09-20 It has been well established that nitrogen coordinated transition metal, TM-N4-C (TM=Fe and Co) moieties, are responsible for the higher catalytic activity for the electrochemical oxygen reduction reaction. However, the results obtained using density functional theory calculations vary from one to another, which can lead to controversy. Herein, we assess the accuracy of the theoretical approach using different class of exchange-correlation functionals, i.e., Perdew-Burke-Ernzerhof (PBE) and revised PBE (RPBE), those with the Grimme's semiempirical dispersion correction (PBE+D3 and RPBE+D3), and the Bayesian error estimate functional with the nonlocal correlation (BEEF-vdW) on the reaction energies of oxygen reduction reaction on TM-N4 moieties in graphene and those with OH-termination. We found that the predicted overpotentials using RPBE+D3 are comparable and consistent with those using BEEF-vdW. Our finding indicates that a proper choice of the exchange-correlation functional is crucial to a precise description of the catalytic activity of this system. text/plain application/gzip text/markdown https://doi.org/10.24435/materialscloud:hv-yd oai:materialscloud.org:1475 mcid:2022.117 eng Materials Cloud https://doi.org/10.1016/j.susc.2022.122144 https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:7n-jz info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode Density functional theory Single atom catalyst oxygen reduction reaction exchange-correlation functional Comparative density functional theory study for predicting oxygen reduction activity of single-atom catalyst info:eu-repo/semantics/other

oai:materialscloud.org:kek59-ah283 2025-11-18T15:36:12Z openaire_data community-mcarchive

Di Giovannantonio, Marco Pignedoli, Carlo A. Karbasiyoun, Moheb Di Giovannantonio, Marco Biswas, Kalyan Écija, David Blacque, Olivier Catarina, Gonçalo Krane, Nils Pignedoli, Carlo A. Ruffieux, Pascal Urgel, José I. Fasel, Roman Juríček, Michal 2025-11-18 Recent advances in the synthesis of graphene fragments that possess unpaired π-electrons and display high-spin ground states have unlocked possibilities to explore exotic physical phenomena related to magnetism. The high degree of spin-delocalisation makes these non-metal-based systems ideal building blocks for the construction of chains and lattices with strongly correlated magnetic ground states, which is the main requisite for measurement-based quantum computation.In a recent publication, we demonstrate the magnetic bistability of a diradical nanographene that allows direct spin manipulation at the single-molecule level. To this end, we made use of solution-phase synthesis and tip-induced activation on a metallic surface to construct a helical non-Kekulé hydrocarbon spin switch, with a reversible transformation between a magnetic ground state and a non-magnetic one via intramolecular bond formation/breaking. The switching process was monitored by scanning tunneling spectroscopy measurements, illustrating that this, and related systems, hold potential as spin-switch units for direct manipulation of magnetism and quantum information in entangled spin systems. This record contains data that support the results discussed in the publication. text/plain application/gzip application/octet-stream https://doi.org/10.24435/materialscloud:ae-s0 oai:materialscloud.org:kek59-ah283 mcid:2025.180 eng Materials Cloud https://doi.org/10.26434/chemrxiv-2024-0206s https://renkulab.io/p/aiida/materials-cloud-archive/sessions/01JZAQ1T34GEE1S98BV1300FXY/start?archive_url=https://archive.materialscloud.org/api/records/kek59-ah283/files/calculations.aiida/content https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:qe-99 info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode SNSF MARVEL/P4 Scanning probe microscopy hydrocarbons ab initio simulations magnetic nanocarbons Controlled magnetic bistability of a helical non-Kekulé hydrocarbon on a Au(111) surface info:eu-repo/semantics/other .eJwdzN1ugjAYANB3-a7JQj9EV-4ms0SSLf6W0hvT0YqkZRgKEWN89y2eBzgP8MZoSMK3-B1pNAsRKZLFIooCuKraQIIB2Jvqaw_JA1ozKK0GtenNuZkggU41J13BMwBf9Z1zp-Y_A5a5scSJyIyfS6SjzvhMM0p04eynYESKPN4Wsd21PCyxXrLW3w_HofxC6o5ifa9ajxXKab_KO85WHy_pemMvUiiRzwvnpGYs1fya_liSF7_f44HzJTz_ACsDQgU.agQfPg.7BRVvXiC9P_Er9eFLYNae2cJf8Y