Neutral and charged inter-valley biexcitons in monolayer MoSe2

Kai Hao, Judith F. Specht, Philipp Nagler, Lixiang Xu, Kha Tran, Akshay Singh, Chandriker Kavir Dass, Christian Schüller, Tobias Korn, Marten Richter, Andreas Knorr, Xiaoqin Li () and Galan Moody ()
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Kai Hao: University of Texas at Austin
Judith F. Specht: Institut für Theoretische Physik, Nichtlineare Optik und Quantenelektronik, Technische Universität Berlin
Philipp Nagler: University of Regensburg
Lixiang Xu: University of Texas at Austin
Kha Tran: University of Texas at Austin
Akshay Singh: University of Texas at Austin
Chandriker Kavir Dass: University of Texas at Austin
Christian Schüller: University of Regensburg
Tobias Korn: University of Regensburg
Marten Richter: Institut für Theoretische Physik, Nichtlineare Optik und Quantenelektronik, Technische Universität Berlin
Andreas Knorr: Institut für Theoretische Physik, Nichtlineare Optik und Quantenelektronik, Technische Universität Berlin
Xiaoqin Li: University of Texas at Austin
Galan Moody: National Institute of Standards & Technology

Nature Communications, 2017, vol. 8, issue 1, 1-7

Abstract: Abstract 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 ∼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.

Date: 2017
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DOI: 10.1038/ncomms15552

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