Valley Depolarization in Monolayer Transition-Metal Dichalcogenides with Zone-Corner Acoustic Phonons

Abstract

Although single-layer transition-metal dichalcogenides with novel valley functionalities are promising candidate to realize valleytronic devices, the essential understanding of valley depolarization mechanisms is still incomplete. Based on pump-probe experiments performed for MoSe2 and WSe2 monolayers and corroborating analysis from density functional calculations, we demonstrate that coherent phonons at the K-point of the Brillouin zone can effectively mediate the valley transfer of electron carriers. In the MoSe2 monolayer case, we identify this mode as the flexural acoustic ZA(K) mode, which has broken inversion symmetry and thus can enable electron spin-flip during valley transfer. On the other hand, in the monolayer WSe2 case where spin-preserving inter-valley relaxations are preferred coherent LA(K) phonons with even inversion symmetry are efficiently generated. These findings establish that, while the specifics of inter-valley relaxations depend on the spin alignments of energy bands, the K-point phonons should be taken into account as an effective valley depolarization pathway in transition metal dichalcogenide monolayers.

8 pages, 5 figures

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Cited by in corpus (5)

• Local field effects in ultrafast light-matter interaction measured by pump-probe spectroscopy of monolayer MoSe${}_2$
• Photonics in Flatland: Challenges and Opportunities for Nanophotonics with 2D Semiconductors
• Dissecting intervalley coupling mechanisms in monolayer transition metal dichalcogenides
• Symmetric Domain Segmentation in WS2 Flakes: Correlating spatially resolved photoluminescence, conductance with valley polarization
• Phonon dynamics of a bulk WSe${}_2$ crystal excited by ultrashort near-infrared pulses