Journal
NATURE COMMUNICATIONS
Volume 8, Issue -, Pages -Publisher
NATURE RESEARCH
DOI: 10.1038/ncomms15552
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Funding
- NSF [DMR-1306878, EFMA-1542747]
- Welch Foundation [F-1662]
- Humboldt fellowship
- German Research foundation (DFG) [GRK 1570, KO3612/1-1]
- DFG [Sonderforschungsbereich 787]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1306878] Funding Source: National Science Foundation
- Emerging Frontiers & Multidisciplinary Activities
- Directorate For Engineering [1542747] Funding Source: National Science Foundation
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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 MoSe2 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 similar to 20 and similar to 5meV 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.
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