Bright and Dark Exciton Coherent Coupling and Hybridization Enabled by External Magnetic Fields.

Mapara, Varun; Barua, Arup; Turkowski, Volodymyr; Trinh, M Tuan; Stevens, Christopher; Liu, Hengzhou; Nugera, Florence A; Kapuruge, Nalaka et al. · Nano Lett · 2022

basic_science · Level V

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Abstract

Magnetic field- and polarization-dependent measurements on bright and dark excitons in monolayer WSe<sub>2</sub> combined with time-dependent density functional theory calculations reveal intriguing phenomena. Magnetic fields up to 25 T parallel to the WSe<sub>2</sub> plane lead to a partial brightening of the energetically lower lying exciton, leading to an increase of the dephasing time. Using a broadband femtosecond pulse excitation, the bright and partially allowed excitonic state can be excited simultaneously, resulting in coherent quantum beating between these states. The magnetic fields perpendicular to the WSe<sub>2</sub> plane energetically shift the bright and dark excitons relative to each other, resulting in the hybridization of the states at the K and K' valleys. Our experimental results are well captured by time-dependent density functional theory calculations. These observations show that magnetic fields can be used to control the coherent dephasing and coupling of the optical excitations in atomically thin semiconductors.