Tailoring Exciton Dynamics in TMDC Heterobilayers in the Quantum Plasmonic Regime

• URL: http://arxiv.org/abs/2306.06337v1
• Date: Sat, 10 Jun 2023 03:19:42 GMT
• Title: Tailoring Exciton Dynamics in TMDC Heterobilayers in the Quantum Plasmonic Regime
• Authors: Mahfujur Rahaman, Gwangwoo Kim, Kyung Yeol Ma, Seunguk Song, Hyeon Suk Shin, and Deep Jariwala
• Abstract summary: Control of excitons in transition metal dichalcogenides (TMDCs) is interesting for tailoring light-matter interactions. We investigated excitons dynamics in TMDC heterobilayers via locally controlled junction current. Our results show that tip-induced radiative relaxation of intralayer (interlayer) excitons becomes dominant in the quantum tunneling regime.
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• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: Control of excitons in transition metal dichalcogenides (TMDCs) and their heterostructures is fundamentally interesting for tailoring light-matter interactions and exploring their potential applications in high-efficiency optoelectronic and nonlinear photonic devices. While both intra- and interlayer excitons in TMDCs have been heavily studied, their behavior in the quantum tunneling regime, in which the TMDC or its heterostructure is optically excited and concurrently serves as a tunnel junction barrier, remains unexplored. Here, using the degree of freedom of a metallic probe in an atomic force microscope, we investigated both intralayer and interlayer excitons dynamics in TMDC heterobilayers via locally controlled junction current in a finely tuned sub-nanometer tip-sample cavity. Our tip-enhanced photoluminescence measurements reveal a significantly different exciton-quantum plasmon coupling for intralayer and interlayer excitons due to different orientation of the dipoles of the respective e-h pairs. Using a steady-state rate equation fit, we extracted field gradients, radiative and nonradiative relaxation rates for excitons in the quantum tunneling regime with and without junction current. Our results show that tip-induced radiative (nonradiative) relaxation of intralayer (interlayer) excitons becomes dominant in the quantum tunneling regime due to the Purcell effect. These findings have important implications for near-field probing of excitonic materials in the strong-coupling regime.

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