Exciton and Phonon Radiative Linewidths in Monolayer Boron Nitride

Cassabois, G.; Fugallo, G.; Elias, C.; Valvin, P.; Rousseau, A.; Gil, B.; Summerfield, A.; Mellor, C. J.; Cheng, T. S.; Eaves, L.; Foxon, C. T.; Beton, P. H.; Lazzeri, M.; Segura, A.; Novikov, S. V.

Abstract

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 (hBN), epitaxially grown on graphite. Reflectivity experiments are performed either in the deep-ultraviolet for the excitonic resonance or in the mid-infrared 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 BreitWigner 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 hBN. 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 hBN. 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 mid-infrared spectral range, and advanced thermal management, and hBN is emerging as a model system in this novel topic.

Citation

Cassabois, G., Fugallo, G., Elias, C., Valvin, P., Rousseau, A., Gil, B., Summerfield, A., Mellor, C. J., Cheng, T. S., Eaves, L., Foxon, C., Beton, P., Lazzeri, M., Segura, A., & Novikov, S. (2022). Exciton and Phonon Radiative Linewidths in Monolayer Boron Nitride. Physical Review X, 12(1), Article 011057. https://doi.org/10.1103/physrevx.12.011057

• Journal Article Type: Article
• Acceptance Date: Jan 11, 2022
• Online Publication Date: Mar 24, 2022
• Publication Date: Mar 24, 2022
• Deposit Date: Jan 26, 2022
• Publicly Available Date: Mar 25, 2022
• Journal: Physical Review X
• Electronic ISSN: 2160-3308
• Publisher: American Physical Society
• Peer Reviewed: Peer Reviewed
• Volume: 12
• Issue: 1
• Article Number: 011057
• DOI: https://doi.org/10.1103/physrevx.12.011057
• Keywords: General Physics and Astronomy
• Public URL: https://nottingham-repository.worktribe.com/output/7340107
• Publisher URL: https://journals.aps.org/prx/abstract/10.1103/PhysRevX.12.011057