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

TL;DR

This study reveals how zone-corner acoustic phonons mediate valley depolarization in monolayer transition-metal dichalcogenides, with implications for valleytronic device design and understanding of electron spin-flip mechanisms.

Contribution

It identifies specific zone-corner phonons as key mediators of valley depolarization, supported by pump-probe experiments and density functional calculations.

Findings

ZA(K) phonons enable spin-flip valley transfer in MoSe2.

LA(K) phonons facilitate spin-preserving inter-valley relaxation in WSe2.

Zone-corner phonons are crucial for understanding valley depolarization pathways.

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.