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<p>Moiré 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 moiré-trapped interlayer excitons in 2<i>H</i>-stacked MoSe<sub>2</sub>/WSe<sub>2</sub> heterobilayers via chiral <i>E</i><sup><i>″</i></sup> in-plane optical phonons at the <i>Γ</i>-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 ~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 moiré systems, opening new opportunities for valleytronic and quantum photonic applications.</p>

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Photoexcitation of moiré-trapped interlayer excitons via chiral phonons

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年6月2日

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  • Antoine Borel,
  • Tatyana V. Ivanova,
  • Jorge Cervantes-Villanueva,
  • Prokhor Thor,
  • Hyeonjun Baek,
  • Takashi Taniguchi,
  • Kenji Watanabe,
  • Alejandro Molina-Sánchez,
  • Brian D. Gerardot,
  • Mauro Brotons-Gisbert

摘要

Moiré 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 moiré-trapped interlayer excitons in 2H-stacked MoSe2/WSe2 heterobilayers via chiral E″ in-plane optical phonons at the Γ-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 ~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 moiré systems, opening new opportunities for valleytronic and quantum photonic applications.