Biexcitonic optical Stark effects in monolayer molybdenum diselenide
Journal
NATURE PHYSICS
Journal Volume
14
Journal Issue
11
Pages
1092
Date Issued
2018
Author(s)
Horng, J
Shen, YX
Cai, H
Wang, Alex
Yang, CS
Lin, CK
Zhao, SL
Watanabe, K
Taniguchi, T
Tongay, S
Wang, F
Abstract
Floquet states, where a periodic optical field coherently drives electrons in solids 1–3 , can enable novel quantum states of matter 4–6 . A prominent approach to realize Floquet states is based on the optical Stark effect. Previous studies on the optical Stark effect often treated the excited state in solids as free quasi-particles 3,7–12 . However, exciton–exciton interactions can be sizeably enhanced in low-dimensional systems and may lead to light–matter interactions that are qualitatively different from those in the non-interacting picture. Here we use monolayer molybdenum diselenide (MoSe 2 ) as a model system to demonstrate that the driving optical field can couple a hierarchy of excitonic states, and the many-body inter-valley biexciton state plays a dominant role in the optical Stark effect. Specifically, the exciton–biexciton coupling in monolayer MoSe 2 breaks down the valley selection rules based on the non-interacting exciton picture. The photon-dressed excitonic states exhibit an energy redshift, splitting or blueshift as the driving photon frequency varies below the exciton transition. We determine a binding energy of 21 meV for the inter-valley biexciton and a transition dipole moment of 9.3 debye for the exciton–biexciton transition. Our study reveals the crucial role of many-body effects in coherent light–matter interaction in atomically thin two-dimensional materials.
Subjects
ELECTRON-SPIN; MANIPULATION; EXCITONS; FIELD; MOS2
Publisher
NATURE PUBLISHING GROUP
Type
journal article