Phonon Dephasing Dynamics in MoS<sub>2</sub>.

Sun, Liuyang; Kumar, Parveen; Liu, Zeyu; Choi, Junho; Fang, Bin; Roesch, Sebastian; Tran, Kha; Casara, Joshua et al. · Nano Lett · 2021

basic_science · Level V

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Abstract

A variety of quantum degrees of freedom, e.g., spins, valleys, and localized emitters, in atomically thin van der Waals materials have been proposed for quantum information applications, and they inevitably couple to phonons. Here, we directly measure the intrinsic optical phonon decoherence in monolayer and bulk MoS<sub>2</sub> by observing the temporal evolution of the spectral interference of Stokes photons generated by pairs of laser pulses. We find that a prominent optical phonon mode E<sub>2g</sub> exhibits a room-temperature dephasing time of ∼7 ps in both the monolayer and bulk. This dephasing time extends to ∼20 ps in the bulk crystal at ∼15 K, which is longer than previously thought possible. First-principles calculations suggest that optical phonons decay via two types of three-phonon processes, in which a pair of acoustic phonons with opposite momentum are generated.