[en] Raman spectroscopy is an advantageous method for studying the local structure of materials, but the interpretation of measured spectra is complicated by the presence of oblique phonons in polycrystals of polar materials. Whilst group theory considerations and standard ab initio calculations are helpful, they are often valid only for single crystals. In this paper, we introduce a method for computing Raman spectra of polycrystalline materials from first principles. We start from the standard approach based on the (Placzek) rotation invariants of the Raman tensors and extend it to include the effect of the coupling between the lattice vibrations and the induced electric field, and the electro-optic contribution, relevant for polar materials like ferroelectrics. As exemplified by applying the method to rhombohedral BaTiO3, AlN, and LiNbO3, such an extension brings the simulated Raman spectrum to a much better correspondence with the experimental one. Additional advantages of the method are that it is general, permits automation, and thus can be used in high-throughput fashion.
Research center :
Q-MAT
Disciplines :
Physics
Author, co-author :
Popov, Maxim N.; Materials Center Leoben (MCL) Forschung GmbH
Spitaler, Jürgen; Materials Center Leoben (MCL) Forschung GmbH
Veerapandiyan, Vignaswaran K.; Materials Center Leoben (MCL) Forschung GmbH
Bousquet, Eric ; Université de Liège - ULiège > Département de physique > Physique théorique des matériaux
Hlinka, Jiri; Academy of Sciences of the Czech Republic, > Institute of Physics
Deluca, Marco; Materials Center Leoben (MCL) Forschung GmbH
Language :
English
Title :
Raman spectra of fine-grained materials from first principles
Publication date :
2020
Journal title :
npj Computational Materials
eISSN :
2057-3960
Publisher :
Nature Publishing Group, United Kingdom
Volume :
6
Pages :
121
Peer reviewed :
Peer Reviewed verified by ORBi
Tags :
Tier-1 supercomputer CÉCI : Consortium des Équipements de Calcul Intensif
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