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:90-36 [version v1]

Publication date: Jul 27, 2023

How to cite this record

Lorenzo Bastonero, Nicola Marzari, Automated all-functionals infrared and Raman spectra, Materials Cloud Archive 2023.118 (2023), https://doi.org/10.24435/materialscloud:90-36

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
vibroscopy-linbo3.aiida MD5md5:5a8fb84c9eb7bd8bae97d3445f1aacfe Open this AiiDA archive on renkulab.io (https://renkulab.io/)	1.2 GiB	AiiDA database containing the full provenance of tests, relaxation and vibrational spectra calculations of LiNbO₃ using 7 different functionals.
README.md MD5md5:9b7b006887baa75a9eebc66ca66be512	1.8 KiB	Instructions

License

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Metadata, except for email addresses, are licensed under the Creative Commons Attribution Share-Alike 4.0 International license.

External references

Keywords

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