Ab Initio Approach to Second-order Resonant Raman Scattering Including Exciton-Phonon Interaction

Abstract Raman spectra obtained by the inelastic scattering of light by crystalline solids contain contributions from first-order vibrational processes (e.g. the emission or absorption of one phonon, a quantum of vibration) as well as higher-order processes with at least two phonons being involved....

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Autores principales:	Yannick Gillet, Stefan Kontur, Matteo Giantomassi, Claudia Draxl, Xavier Gonze
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2017
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/2d74045dce804d62aa92ee2da54ef390
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spelling	oai:doaj.org-article:2d74045dce804d62aa92ee2da54ef3902021-12-02T16:08:09ZAb Initio Approach to Second-order Resonant Raman Scattering Including Exciton-Phonon Interaction10.1038/s41598-017-07682-y2045-2322https://doaj.org/article/2d74045dce804d62aa92ee2da54ef3902017-08-01T00:00:00Zhttps://doi.org/10.1038/s41598-017-07682-yhttps://doaj.org/toc/2045-2322Abstract Raman spectra obtained by the inelastic scattering of light by crystalline solids contain contributions from first-order vibrational processes (e.g. the emission or absorption of one phonon, a quantum of vibration) as well as higher-order processes with at least two phonons being involved. At second order, coupling with the entire phonon spectrum induces a response that may strongly depend on the excitation energy, and reflects complex processes more difficult to interpret. In particular, excitons (i.e. bound electron-hole pairs) may enhance the absorption and emission of light, and couple strongly with phonons in resonance conditions. We design and implement a first-principles methodology to compute second-order Raman scattering, incorporating dielectric responses and phonon eigenstates obtained from density-functional theory and many-body theory. We demonstrate our approach for the case of silicon, relating frequency-dependent relative Raman intensities, that are in excellent agreement with experiment, to different vibrations and regions of the Brillouin zone. We show that exciton-phonon coupling, computed from first principles, indeed strongly affects the spectrum in resonance conditions. The ability to analyze second-order Raman spectra thus provides direct insight into this interaction.Yannick GilletStefan KonturMatteo GiantomassiClaudia DraxlXavier GonzeNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 7, Iss 1, Pp 1-10 (2017)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Yannick Gillet Stefan Kontur Matteo Giantomassi Claudia Draxl Xavier Gonze Ab Initio Approach to Second-order Resonant Raman Scattering Including Exciton-Phonon Interaction
description	Abstract Raman spectra obtained by the inelastic scattering of light by crystalline solids contain contributions from first-order vibrational processes (e.g. the emission or absorption of one phonon, a quantum of vibration) as well as higher-order processes with at least two phonons being involved. At second order, coupling with the entire phonon spectrum induces a response that may strongly depend on the excitation energy, and reflects complex processes more difficult to interpret. In particular, excitons (i.e. bound electron-hole pairs) may enhance the absorption and emission of light, and couple strongly with phonons in resonance conditions. We design and implement a first-principles methodology to compute second-order Raman scattering, incorporating dielectric responses and phonon eigenstates obtained from density-functional theory and many-body theory. We demonstrate our approach for the case of silicon, relating frequency-dependent relative Raman intensities, that are in excellent agreement with experiment, to different vibrations and regions of the Brillouin zone. We show that exciton-phonon coupling, computed from first principles, indeed strongly affects the spectrum in resonance conditions. The ability to analyze second-order Raman spectra thus provides direct insight into this interaction.
format	article
author	Yannick Gillet Stefan Kontur Matteo Giantomassi Claudia Draxl Xavier Gonze
author_facet	Yannick Gillet Stefan Kontur Matteo Giantomassi Claudia Draxl Xavier Gonze
author_sort	Yannick Gillet
title	Ab Initio Approach to Second-order Resonant Raman Scattering Including Exciton-Phonon Interaction
title_short	Ab Initio Approach to Second-order Resonant Raman Scattering Including Exciton-Phonon Interaction
title_full	Ab Initio Approach to Second-order Resonant Raman Scattering Including Exciton-Phonon Interaction
title_fullStr	Ab Initio Approach to Second-order Resonant Raman Scattering Including Exciton-Phonon Interaction
title_full_unstemmed	Ab Initio Approach to Second-order Resonant Raman Scattering Including Exciton-Phonon Interaction
title_sort	ab initio approach to second-order resonant raman scattering including exciton-phonon interaction
publisher	Nature Portfolio
publishDate	2017
url	https://doaj.org/article/2d74045dce804d62aa92ee2da54ef390
work_keys_str_mv	AT yannickgillet abinitioapproachtosecondorderresonantramanscatteringincludingexcitonphononinteraction AT stefankontur abinitioapproachtosecondorderresonantramanscatteringincludingexcitonphononinteraction AT matteogiantomassi abinitioapproachtosecondorderresonantramanscatteringincludingexcitonphononinteraction AT claudiadraxl abinitioapproachtosecondorderresonantramanscatteringincludingexcitonphononinteraction AT xaviergonze abinitioapproachtosecondorderresonantramanscatteringincludingexcitonphononinteraction
_version_	1718384584302788608

Ab Initio Approach to Second-order Resonant Raman Scattering Including Exciton-Phonon Interaction

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