Photoinduced modulation of the excitonic resonance via coupling with coherent phonons in a layered semiconductor

The coupling of excitons with atomic vibrations plays a pivotal role on the nonequilibrium optical properties of layered semiconductors. However, how exciton-phonon coupling manifests in the time and energy domains is still an open debate between experiment and theory. By means of time-resolved broa...

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Main Authors: S. Mor, V. Gosetti, A. Molina-Sánchez, D. Sangalli, S. Achilli, V. F. Agekyan, P. Franceschini, C. Giannetti, L. Sangaletti, S. Pagliara
Format: Article
Language:English
Published: American Physical Society 2021-12-01
Series:Physical Review Research
Online Access:http://doi.org/10.1103/PhysRevResearch.3.043175
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author S. Mor
V. Gosetti
A. Molina-Sánchez
D. Sangalli
S. Achilli
V. F. Agekyan
P. Franceschini
C. Giannetti
L. Sangaletti
S. Pagliara
author_facet S. Mor
V. Gosetti
A. Molina-Sánchez
D. Sangalli
S. Achilli
V. F. Agekyan
P. Franceschini
C. Giannetti
L. Sangaletti
S. Pagliara
author_sort S. Mor
collection DOAJ
description The coupling of excitons with atomic vibrations plays a pivotal role on the nonequilibrium optical properties of layered semiconductors. However, how exciton-phonon coupling manifests in the time and energy domains is still an open debate between experiment and theory. By means of time-resolved broadband optical reflectivity combined with ab initio calculations of a bismuth tri-iodide single crystal, we set the spectral fingerprints for the optical detection of exciton-phonon coupling in layered semiconductors. Our joint experimental and theoretical effort allows us to unravel the impact of exciton-phonon coupling by microscopically relating the photoinduced coherent energy modulation of the excitonic resonance to coherent optical phonons. This enables us to track the extent of the photoinduced atomic displacement in real space. Our findings represent a step forward on the road to coherent manipulation of the excitonic properties on ultrafast timescales.
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spelling doaj.art-d2a17074702e4424905ef00365a5d0d22024-04-12T17:16:19ZengAmerican Physical SocietyPhysical Review Research2643-15642021-12-013404317510.1103/PhysRevResearch.3.043175Photoinduced modulation of the excitonic resonance via coupling with coherent phonons in a layered semiconductorS. MorV. GosettiA. Molina-SánchezD. SangalliS. AchilliV. F. AgekyanP. FranceschiniC. GiannettiL. SangalettiS. PagliaraThe coupling of excitons with atomic vibrations plays a pivotal role on the nonequilibrium optical properties of layered semiconductors. However, how exciton-phonon coupling manifests in the time and energy domains is still an open debate between experiment and theory. By means of time-resolved broadband optical reflectivity combined with ab initio calculations of a bismuth tri-iodide single crystal, we set the spectral fingerprints for the optical detection of exciton-phonon coupling in layered semiconductors. Our joint experimental and theoretical effort allows us to unravel the impact of exciton-phonon coupling by microscopically relating the photoinduced coherent energy modulation of the excitonic resonance to coherent optical phonons. This enables us to track the extent of the photoinduced atomic displacement in real space. Our findings represent a step forward on the road to coherent manipulation of the excitonic properties on ultrafast timescales.http://doi.org/10.1103/PhysRevResearch.3.043175
spellingShingle S. Mor
V. Gosetti
A. Molina-Sánchez
D. Sangalli
S. Achilli
V. F. Agekyan
P. Franceschini
C. Giannetti
L. Sangaletti
S. Pagliara
Photoinduced modulation of the excitonic resonance via coupling with coherent phonons in a layered semiconductor
Physical Review Research
title Photoinduced modulation of the excitonic resonance via coupling with coherent phonons in a layered semiconductor
title_full Photoinduced modulation of the excitonic resonance via coupling with coherent phonons in a layered semiconductor
title_fullStr Photoinduced modulation of the excitonic resonance via coupling with coherent phonons in a layered semiconductor
title_full_unstemmed Photoinduced modulation of the excitonic resonance via coupling with coherent phonons in a layered semiconductor
title_short Photoinduced modulation of the excitonic resonance via coupling with coherent phonons in a layered semiconductor
title_sort photoinduced modulation of the excitonic resonance via coupling with coherent phonons in a layered semiconductor
url http://doi.org/10.1103/PhysRevResearch.3.043175
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