Lorenzo Bastonero^1*, Nicola Marzari^1,2,3*

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

Description

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.

Materials Cloud sections using this data

Files

File name	Size	Description
README.md MD5md5:e9c4327d8b731b4aa61a546f47ae7322	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.
archive.aiida MD5md5:a4ad55a9f4749d08cca7079e53b9ba93 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.
scripts.tar.gz MD5md5:933fe9973a31dbc34a9e54f890c2f45b	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.

License

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External references

Keywords

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