Resonant Raman spectroscopies beyond density-functional theory

DOI

<p>Resonant Raman spectroscopy probes, in a single measurement, how electrons and phonons couple in a material. While density-functional theory (DFT) typically reproduces well phonon frequencies, resonant Raman intensities hinge on electron-phonon matrix elements and electronic transitions that are far more sensitive to the underlying exchange-correlation approximation, yet accessible so far only for a handful of semilocal functionals. Here, we introduce a general finite-difference framework that computes resonant Raman tensors for any electronic-structure method able to deliver forces, eigenvalues, and wavefunctions. Applying it to graphene and monolayer MoS<sub>2</sub> with hybrid functionals and meta-GGAs, we show that these methods systematically enhance electron-phonon couplings relative to semilocal DFT, reflecting reduced dielectric overscreening. Accurate intensities require eigenvalues and electron-phonon matrix elements to be treated consistently at the same level of theory; among the approaches tested, hybrid functionals agree best with experiment, opening the door to systematic beyond-DFT Raman characterization of 2D materials.</p>

Identifier
DOI https://doi.org/10.24435/materialscloud:dx-md
Related Identifier https://doi.org/10.48550/arXiv.2608.00269
Related Identifier https://archive.materialscloud.org/communities/mcarchive
Related Identifier https://doi.org/10.24435/materialscloud:xj-n4
Metadata Access https://archive.materialscloud.org/oai2d?verb=GetRecord&metadataPrefix=oai_dc&identifier=oai:materialscloud.org:dtx5k-64229
Provenance
Creator Poliukhin, Aleksandr; Aubry, Corto Babs; Bastonero, Lorenzo; Marzari, Nicola
Publisher Materials Cloud
Contributor Poliukhin, Aleksandr
Publication Year 2026
Rights info:eu-repo/semantics/openAccess; Creative Commons Attribution 4.0 International; https://creativecommons.org/licenses/by/4.0/legalcode
OpenAccess true
Contact archive(at)materialscloud.org
Representation
Language English
Resource Type info:eu-repo/semantics/other
Format application/gzip; application/octet-stream
Discipline Materials Science and Engineering