Valley-selective optical Stark effect probed by Kerr rotation

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.

9 pages, 4 figures, supplementary information

References in corpus (10)

• Measurement of the optical dielectric function of transition metal dichalcogenide monolayers: MoS2, MoSe2, WS2 and WSe2
• Valley Dependent Optoelectronics from Inversion Symmetry Breaking
• Ultrafast Generation of Pseudo-magnetic Field for Valley Excitons in WSe2 Monolayers
• Exciton Valley Dynamics probed by Kerr Rotation in WSe2 Monolayers
• Ultrafast Manipulation of Valley Pseudospin
• Probing the influence of dielectric environment on excitons in monolayer WSe2: Insight from high magnetic fields
• Large, valley-exclusive Bloch-Siegert shift in monolayer WS2
• Mutual Photoluminescence Quenching and Photovoltaic Effect in Large-Area Single-Layer MoS2-Polymer Heterojunctions
• Observation of intervalley biexcitonic optical Stark effect in monolayer WS2
• Time-resolved Kerr rotation spectroscopy of valley dynamics in single-layer MoS2