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arXiv · 2512.21125

Photoexcitation of moir\'e-trapped interlayer excitons via chiral phonons

A. Borel·T. V. Ivanova·J. Cervantes-Villanueva·P. Thor·H. Baek·T. Taniguchi·K. Watanabe·A. Molina-Sanchez·B. D. Gerardot·M. Brotons-Gisbert
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Abstract

Moir\'e superlattices in transition-metal dichalcogenide semiconductor heterobilayers enable the quantum confinement of interlayer excitons with large out-of-plane permanent electric dipoles and spin-valley control. Here, we report a novel phonon-assisted excitation mechanism of individual moir\'e-trapped interlayer excitons in 2H-stacked MoSe$_2$/WSe$_2$ heterobilayers via chiral $E^{\prime\prime}$ in-plane optical phonons at the {\Gamma}-point. This excitation pathway preserves valley-selective optical selection rules and enables deterministic generation of individual interlayer excitons with defined helicity, emitting within a spectrally narrow energy spread. Through photoluminescence excitation spectroscopy in both the ensemble and quantum emitter regimes, we identify a fixed phonon energy of $\sim$23 meV mediating the process. First-principles calculations corroborate the symmetry and energy of the relevant phonon mode and its coupling to interlayer excitons, providing microscopic support for the observed valley-selective phonon-assisted excitation mechanism. Our results highlight the utility of chiral phonons as a tool for controlled excitation of quantum emitters in TMD moir\'e systems, opening new opportunities for valleytronic and quantum photonic applications.

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A. Borel, T. V. Ivanova, J. Cervantes-Villanueva, P. Thor, H. Baek, T. Taniguchi, K. Watanabe, A. Molina-Sanchez, B. D. Gerardot, M. Brotons-Gisbert. 2025-12-24. Photoexcitation of moir\'e-trapped interlayer excitons via chiral phonons. https://arxiv.org/abs/2512.21125

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