Valley-selective optical Stark effect probed by Kerr rotation

TL;DR

This paper demonstrates that time-resolved Kerr rotation is a more sensitive and precise method than reflectance for detecting valley-selective optical Stark effects in monolayer TMDCs, enabling better control of valley pseudospin.

Contribution

The study introduces time-resolved Kerr rotation as a superior technique for probing valley-specific optical Stark shifts in TMDC monolayers, surpassing reflectance-based methods in sensitivity and accuracy.

Findings

Kerr rotation improves Stark effect detection sensitivity fivefold.

Observation of valley- and energy-selective Stark shifts in monolayer MoS$_2$.

Enhanced understanding of ultrafast valley manipulation in layered materials.

Abstract

The ability to monitor and control distinct states is at the heart of emerging quantum technologies. The valley pseudospin in transition metal dichalcogenide (TMDC) monolayers is a promising degree of freedom for such control, with the optical Stark effect allowing for valley-selective manipulation of energy levels in WS$_2$ and WSe$_2$ using ultrafast optical pulses. Despite these advances, understanding of valley-sensitive optical Stark shifts in TMDCs has been limited by reflectance-based detection methods where the signal is small and prone to background effects. More sensitive polarization-based spectroscopy is required to better probe ultrafast Stark shifts for all-optical manipulation of valley energy levels. Here, we show time-resolved Kerr rotation to be a more sensitive probe of the valley-selective optical Stark effect in monolayer TMDCs. Compared to the established time-resolved reflectance methods, Kerr rotation is less sensitive to background effects. Kerr rotation provides a five-fold improvement in the signal-to-noise ratio of the Stark effect optical signal and a more precise estimate of the energy shift. This increased sensitivity allows for observation of an optical Stark shift in monolayer MoS$_2$ that exhibits both valley- and energy-selectivity, demonstrating the promise of this method for investigating this effect in other layered materials and heterostructures.