Ultrafast pseudospin quantum beats in multilayer WSe$_2$ and MoSe$_2$

TL;DR

This study reveals ultrafast pseudospin quantum beats in multilayer WSe$_2$ and MoSe$_2$, demonstrating layer-dependent valley pseudospin dynamics and potential for high-speed pseudospin manipulation.

Contribution

It provides the first experimental observation of pseudospin quantum beats in multilayer TMDCs and confirms their origin through first-principles calculations.

Findings

Multilayer samples show pronounced quantum beats in TRFE signals.

In-plane exciton g-factors are near those of out-of-plane, indicating layer locking.

Ultrafast pseudospin rotations occur at GHz to THz frequencies.

Abstract

Layered van-der-Waals materials with hexagonal symmetry offer an extra degree of freedom to their electrons, the so called valley index or valley pseudospin. This quantity behaves conceptually like the electron spin and the term valleytronics has been coined. In this context, the group of semiconducting transition-metal dichalcogenides (TMDC) are particularly appealing, due to large spin-orbit interactions and a direct bandgap at the K points of the hexagonal Brillouin zone. In this work, we present investigations of excitonic transitions in mono- and multilayer WSe$_2$ and MoSe$_2$ materials by time-resolved Faraday ellipticity (TRFE) with in-plane magnetic fields, $B_{\parallel}$, of up to 9 T. In monolayer samples, the measured TRFE time traces are almost independent of $B_{\parallel}$, which confirms a close to zero in-plane exciton $g$ factor $g_\parallel$, consistent with first-principles calculations. In stark contrast, we observe pronounced temporal oscillations in multilayer samples for $B_{\parallel}>0$. Remarkably, the extracted in-plane $g_\parallel$ are very close to reported out-of-plane exciton $g$ factors of the materials, namely $|g_{\parallel 1s}|=3.1\pm 0.2$ and $2.5\pm0.2$ for the 1s A excitons in WSe$_2$ and MoSe$_2$ multilayers, respectively. Our first-principles calculations nicely confirm the presence of a non-zero $g_{\parallel}$ for the multilayer samples. We propose that the oscillatory TRFE signal in the multilayer samples is caused by pseudospin quantum beats of excitons, which is a manifestation of spin- and pseudospin layer locking in the multilayer samples. Our results demonstrate ultrafast pseudospin rotations in the GHz- to THz frequency range, which pave the way towards ultrafast pseudospin manipulation in multilayer TMDC samples.