Anomalous Stark Shift of Excitonic Complexes in Monolayer Semiconductor

TL;DR

This study reveals a universal anomalous Stark shift behavior in monolayer TMDCs, where electric fields induce a sign change in excitonic emission shifts due to competing effects, advancing understanding of many-body physics and device tunability.

Contribution

First demonstration of electric field-induced sign change in Stark shift across multiple excitonic species in monolayer TMDCs, supported by theoretical calculations.

Findings

Non-monotonic Stark shift observed with electric field.

Blue shift dominates at low fields due to suppressed binding energy.

Encapsulation environment influences Stark shift magnitude.

Abstract

Monolayer transition metal dichalcogenide semiconductors host strongly bound two-dimensional excitonic complexes, and form an excellent platform for probing many-body physics through manipulation of Coulomb interaction. Quantum confined Stark effect is one of the routes to dynamically tune the emission line of these excitonic complexes. In this work, using a high quality graphene/hBN/WS$_2$/hBN/Au vertical heterojunction, we demonstrate for the first time, an out-of-plane electric field driven change in the sign of the Stark shift from blue to red for four different excitonic species, namely, the neutral exciton, the charged exciton (trion), the charged biexciton, and the defect-bound exciton. Such universal non-monotonic Stark shift with electric field arises from a competition between the conventional quantum confined Stark effect driven red shift and a suppressed binding energy driven anomalous blue shift of the emission lines, with the latter dominating in the low field regime. We also find that the encapsulating environment of the monolayer TMDC plays an important role in wave function spreading, and hence in determining the magnitude of the blue Stark shift. The results for neutral and charged excitonic species are in excellent agreement with calculations from Bethe-Salpeter Equation that uses seven-band per spin tight binding Hamiltonian. The findings have important implications in probing many-body interaction in the two dimension as well as in developing layered semiconductor based tunable optoelectronic devices.