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Neutral and charged inter-valley biexcitons in monolayer MoSe2
Neutral and charged inter-valley biexcitons in monolayer MoSe2
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Neutral and charged inter-valley biexcitons in monolayer MoSe2
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Neutral and charged inter-valley biexcitons in monolayer MoSe2
Neutral and charged inter-valley biexcitons in monolayer MoSe2

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Neutral and charged inter-valley biexcitons in monolayer MoSe2
Neutral and charged inter-valley biexcitons in monolayer MoSe2
Journal Article

Neutral and charged inter-valley biexcitons in monolayer MoSe2

2017
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Overview
In atomically thin transition metal dichalcogenides (TMDs), reduced dielectric screening of the Coulomb interaction leads to strongly correlated many-body states, including excitons and trions, that dominate the optical properties. Higher-order states, such as bound biexcitons, are possible but are difficult to identify unambiguously using linear optical spectroscopy methods. Here, we implement polarization-resolved two-dimensional coherent spectroscopy (2DCS) to unravel the complex optical response of monolayer MoSe 2 and identify multiple higher-order correlated states. Decisive signatures of neutral and charged inter-valley biexcitons appear in cross-polarized two-dimensional spectra as distinct resonances with respective ∼20 and ∼5 meV binding energies—similar to recent calculations using variational and Monte Carlo methods. A theoretical model considering the valley-dependent optical selection rules reveals the quantum pathways that give rise to these states. Inter-valley biexcitons identified here, comprising of neutral and charged excitons from different valleys, offer new opportunities for developing ultrathin biexciton lasers and polarization-entangled photon sources. Atomically thin transition metal dichalcogenides host excitons and trions, however higher-order states, although possible, are difficult to identify experimentally. Here, the authors perform polarization-resolved coherent spectroscopy to unveil the signature of neutral and charged inter-valley biexcitons in monolayer MoSe 2 .