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Automated all-functionals infrared and Raman spectra

Lorenzo Bastonero1*, Nicola Marzari1,2,3*

1 U Bremen Excellence Chair, Bremen Center for Computational Materials Science, and MAPEX Center for Materials and Processes, University of Bremen, D-28359 Bremen, Germany

2 Theory and Simulation of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

3 Laboratory for Materials Simulations, Paul Scherrer Institut, 5232 Villigen PSI, Switzerland

* Corresponding authors emails: lbastone@uni-bremen.de, marzari@uni-bremen.de
DOI10.24435/materialscloud:pr-s2 [version v2]

Publication date: Mar 22, 2024

How to cite this record

Lorenzo Bastonero, Nicola Marzari, Automated all-functionals infrared and Raman spectra, Materials Cloud Archive 2024.49 (2024), https://doi.org/10.24435/materialscloud:pr-s2


Infrared and Raman spectroscopies are ubiquitous techniques employed in many experimental laboratories, thanks to their fast and non-destructive nature able to capture materials' features as spectroscopic fingerprints. Nevertheless, these measurements frequently need theoretical support in order to unambiguously decipher and assign complex spectra. Linear-response theory provides an effective way to obtain the higher-order derivatives needed, but its applicability to modern exchange-correlation functionals remains limited. Here, we devise an automated, open-source, user-friendly approach based on ground-state density-functional theory and the electric enthalpy functional to allow seamless calculations of first-principles infrared and Raman spectra. By employing a finite-displacement and finite-field approach, we allow for the use of any functional, as well as an efficient treatment of large low-symmetry structures. Additionally, we propose a simple scheme for efficiently sampling the Brillouin zone with different electric fields. To demonstrate the capabilities of our approach, we provide illustrations using the ferroelectric LiNbO₃ crystal as a paradigmatic example. We predict infrared and Raman spectra using various (semi)local, Hubbard corrected, and hybrid functionals. Our results also show how PBE0 and extended Hubbard functionals yield in this case the best match in term of peak positions and intensities, respectively.

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File name Size Description
4.0 KiB Instructions on how to use the data of this repository to reproduce results, figures, and tables of the related manuscript and its Supplementary Information.
Open this AiiDA archive on renkulab.io (https://renkulab.io/)
369.3 MiB AiiDA database containing the full provenance of tests, relaxation and vibrational spectra calculations of LiNbO₃ using 7 different functionals. It also contains the benchmark calculations on AlAs studied in the Supplementary Information.
461.9 KiB Python and bash scripts, along with jupyter notebooks, used to submit the AiiDA calculations, and to reproduce figures and tables of both the main manuscript and the Supplementary Information.


Files and data are licensed under the terms of the following license: Creative Commons Attribution 4.0 International.
Metadata, except for email addresses, are licensed under the Creative Commons Attribution Share-Alike 4.0 International license.

External references

Journal reference (Paper in which the method is described and the data is discussed.)


vibrational properties raman infrared automated aiida phonons ab initio density-functional theory

Version history:

2024.49 (version v2) [This version] Mar 22, 2024 DOI10.24435/materialscloud:pr-s2
2023.118 (version v1) Jul 27, 2023 DOI10.24435/materialscloud:90-36