Exciton and Phonon Radiative Linewidths in Monolayer Boron Nitride

The light-matter interaction in bulk semiconductors is in the strong-coupling regime with hybrid eigenstates, the so-called exciton polaritons and phonon polaritons. In two-dimensional (2D) systems, the translational invariance is broken in the direction perpendicular to the plane of the 2D system....

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Main Authors: G. Cassabois, G. Fugallo, C. Elias, P. Valvin, A. Rousseau, B. Gil, A. Summerfield, C. J. Mellor, T. S. Cheng, L. Eaves, C. T. Foxon, P. H. Beton, M. Lazzeri, A. Segura, S. V. Novikov
Format: Article
Language:English
Published: American Physical Society 2022-03-01
Series:Physical Review X
Online Access:http://doi.org/10.1103/PhysRevX.12.011057
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author G. Cassabois
G. Fugallo
C. Elias
P. Valvin
A. Rousseau
B. Gil
A. Summerfield
C. J. Mellor
T. S. Cheng
L. Eaves
C. T. Foxon
P. H. Beton
M. Lazzeri
A. Segura
S. V. Novikov
author_facet G. Cassabois
G. Fugallo
C. Elias
P. Valvin
A. Rousseau
B. Gil
A. Summerfield
C. J. Mellor
T. S. Cheng
L. Eaves
C. T. Foxon
P. H. Beton
M. Lazzeri
A. Segura
S. V. Novikov
author_sort G. Cassabois
collection DOAJ
description The light-matter interaction in bulk semiconductors is in the strong-coupling regime with hybrid eigenstates, the so-called exciton polaritons and phonon polaritons. In two-dimensional (2D) systems, the translational invariance is broken in the direction perpendicular to the plane of the 2D system. The light-matter interaction switches to the weak-coupling regime with a finite radiative lifetime of the matter excitations in 2D. Radiative phenomena have been extensively studied for 2D excitons in quantum wells and 2D crystals, but their counterpart has never been addressed for optical phonons in 2D. Here we present a parallel study of the exciton and phonon radiative linewidths in atomically thin layers of hexagonal boron nitride (h-BN), epitaxially grown on graphite. Reflectivity experiments are performed either in the deep ultraviolet for the excitonic resonance or in the midinfrared for the phononic one. A quantitative interpretation is implemented in the framework of a transfer matrix approach generalized to the case of monolayers with the inclusion of Breit-Wigner resonances of either excitonic or phononic nature. For the exciton we find a giant radiative broadening in comparison to other 2D crystals, with a value of ∼25  meV related to the strong excitonic effects in h-BN. For the phonon we provide the first estimation of the radiative linewidth of a 2D phonon, with a value of ∼0.2  meV in monolayer h-BN. Our results are found to be in good agreement with first-principles calculations. Our study unravels the existence of radiative states for optical phonons in 2D, with numerous perspectives for fundamental physics, optoelectronic applications in the midinfrared spectral range, and advanced thermal management, and h-BN is emerging as a model system in this novel topic.
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spelling doaj.art-da4eed7dc9d1474b89bea97bb5ddbc912022-12-21T23:52:13ZengAmerican Physical SocietyPhysical Review X2160-33082022-03-0112101105710.1103/PhysRevX.12.011057Exciton and Phonon Radiative Linewidths in Monolayer Boron NitrideG. CassaboisG. FugalloC. EliasP. ValvinA. RousseauB. GilA. SummerfieldC. J. MellorT. S. ChengL. EavesC. T. FoxonP. H. BetonM. LazzeriA. SeguraS. V. NovikovThe light-matter interaction in bulk semiconductors is in the strong-coupling regime with hybrid eigenstates, the so-called exciton polaritons and phonon polaritons. In two-dimensional (2D) systems, the translational invariance is broken in the direction perpendicular to the plane of the 2D system. The light-matter interaction switches to the weak-coupling regime with a finite radiative lifetime of the matter excitations in 2D. Radiative phenomena have been extensively studied for 2D excitons in quantum wells and 2D crystals, but their counterpart has never been addressed for optical phonons in 2D. Here we present a parallel study of the exciton and phonon radiative linewidths in atomically thin layers of hexagonal boron nitride (h-BN), epitaxially grown on graphite. Reflectivity experiments are performed either in the deep ultraviolet for the excitonic resonance or in the midinfrared for the phononic one. A quantitative interpretation is implemented in the framework of a transfer matrix approach generalized to the case of monolayers with the inclusion of Breit-Wigner resonances of either excitonic or phononic nature. For the exciton we find a giant radiative broadening in comparison to other 2D crystals, with a value of ∼25  meV related to the strong excitonic effects in h-BN. For the phonon we provide the first estimation of the radiative linewidth of a 2D phonon, with a value of ∼0.2  meV in monolayer h-BN. Our results are found to be in good agreement with first-principles calculations. Our study unravels the existence of radiative states for optical phonons in 2D, with numerous perspectives for fundamental physics, optoelectronic applications in the midinfrared spectral range, and advanced thermal management, and h-BN is emerging as a model system in this novel topic.http://doi.org/10.1103/PhysRevX.12.011057
spellingShingle G. Cassabois
G. Fugallo
C. Elias
P. Valvin
A. Rousseau
B. Gil
A. Summerfield
C. J. Mellor
T. S. Cheng
L. Eaves
C. T. Foxon
P. H. Beton
M. Lazzeri
A. Segura
S. V. Novikov
Exciton and Phonon Radiative Linewidths in Monolayer Boron Nitride
Physical Review X
title Exciton and Phonon Radiative Linewidths in Monolayer Boron Nitride
title_full Exciton and Phonon Radiative Linewidths in Monolayer Boron Nitride
title_fullStr Exciton and Phonon Radiative Linewidths in Monolayer Boron Nitride
title_full_unstemmed Exciton and Phonon Radiative Linewidths in Monolayer Boron Nitride
title_short Exciton and Phonon Radiative Linewidths in Monolayer Boron Nitride
title_sort exciton and phonon radiative linewidths in monolayer boron nitride
url http://doi.org/10.1103/PhysRevX.12.011057
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