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In recent years, quantum-dot-like single-photon emitters in atomically thin van der Waals materials have become a promising platform for future on-chip scalable quantum light sources with unique advantages over existing technologies, notably the potential for site-specific engineering. However, the required cryogenic temperatures for the functionality of these sources has been an inhibitor of their full potential. Existing methods to create emitters in 2D materials face fundamental challenges in extending the working temperature while maintaining the emitter's fabrication yield and purity. In this work, we demonstrate a method of creating site-controlled single-photon emitters in atomically thin WSe2 with high yield utilizing independent and simultaneous strain engineering via nanoscale stressors and defect engineering via electron-beam irradiation. Many of the emitters exhibit biexciton cascaded emission, single-photon purities above 95%, and working temperatures up to 150 K. This methodology, coupled with possible plasmonic or optical micro-cavity integration, furthers the realization of scalable, room-temperature, and high-quality 2D single- and entangled-photon sources.

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. [ABSTRACT FROM AUTHOR]

In recent years, quantum-dot-like single-photon emitters in atomically thin van der Waals materials have become a promising platform for future on-chip scalable quantum light sources with unique advantages over existing technologies, notably the potential for site-specific engineering. However, the required cryogenic temperatures for the functionality of these sources has been an inhibitor of their full potential. Existing methods to create emitters in 2D materials face fundamental challenges in extending the working temperature while maintaining the emitter's fabrication yield and purity. In this work, we demonstrate a method of creating site-controlled single-photon emitters in atomically thin WSe 2 with high yield utilizing independent and simultaneous strain engineering via nanoscale stressors and defect engineering via electron-beam irradiation. Many of the emitters exhibit biexciton cascaded emission, single-photon purities above 95%, and working temperatures up to 150 K. This methodology, coupled with possible plasmonic or optical micro-cavity integration, furthers the realization of scalable, room-temperature, and high-quality 2D single- and entangled-photon sources.