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https://doi.org/10.1103/physre...
Article . 2022 . Peer-reviewed
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https://dx.doi.org/10.48550/ar...
Article . 2022
License: CC BY
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Exciton-phonon interaction calls for a revision of the “exciton” concept

Authors: Paleari Fulvio; Marini Andrea;

Exciton-phonon interaction calls for a revision of the “exciton” concept

Abstract

The concept of \textit{optical} exciton - a photo-excited bound electron-hole pair within a crystal - is routinely used to interpret and model a wealth of excited-state phenomena in semiconductors. Beside originating sub-band gap signatures in optical spectra, optical excitons have also been predicted to condensate, diffuse, recombine, relax. However, all these phenomena are rooted on a theoretical definition of the excitonic state based on the following simple picture: "excitons" are actual particles that both appear as peaks in the linear absorption spectrum and also behave as well-defined quasiparticles. In this paper we show, instead, that the electron-phonon interaction decomposes the initial optical excitons into \textit{elemental} excitons, the latter being a different kind of bound electron-hole pairs lacking the effect caused by the induced, classical, electric field. This is demonstrated within a many-body perturbation theory approach starting from the interacting electronic Hamiltonian including both electron-phonon and electron-hole interactions. We then apply the results on two realistic systems, monolayer MoS$_2$ (where the lowest-bound exciton is optically inactive) and monolayer MoSe$_2$ (where it is optically active), using first-principles methods to compute the exciton-phonon coupling matrix elements. Among the consequences of optical-elemental decomposition, we point to a homogeneous broadening of absorption peaks occurring even for the lowest-bound optical exciton, we demonstrate this by computing exciton-phonon transition rates. More generally, our findings suggest that the optical excitons gradually lose their initial structure and evolve as elemental excitons. These states can be regarded as the real intrinsic excitations of the interacting system, the ones that survive when the external perturbation and the induced electric fields have vanished.

18 pages, 8 figures

Country
Italy
Keywords

Condensed Matter - Materials Science, Absorption spectroscopy, Computation theory, Electric fields, Electrons, Excited states, Layered semiconductors, Molybdenum compounds, Monolayers, Perturbation techniques, Selenium compounds, Sulfur compounds, Absorption spectroscopy; Computation theory; Electric fields; Electrons; Excited states; Layered semiconductors; Molybdenum compounds; Monolayers; Perturbation techniques; Selenium compounds; Sulfur compounds, Materials Science (cond-mat.mtrl-sci), FOS: Physical sciences

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selected citations
These citations are derived from selected sources.
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
15
Top 10%
Average
Top 10%
Green
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