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Probing Nonlinear Interactions of Dipolar Interlayer Excitons in MoSe$_2$/WSe$_2$ Heterobilayers
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- DOI
- 10.48550/arxiv.2609.01149
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Abstract
Interlayer excitons in transition-metal dichalcogenide heterobilayers possess intrinsic out-of-plane dipole moments, providing a platform for investigating exciton-exciton interactions at high densities. Here, we use excitation-energy-dependent photoluminescence excitation (PLE) spectroscopy to probe the nonlinear response of dipolar interlayer excitons in chemical vapor deposition-grown MoSe$_2$/WSe$_2$ heterobilayers. By tuning the excitation energy across intralayer exciton resonances at fixed excitation power, we selectively vary the population injected into the interlayer exciton states. Resonant excitation drives the system into a nonlinear regime, leading to saturation of the interlayer exciton photoluminescence and an apparent broadening of the intralayer $1s$ resonances in the PLE spectra. At the same time, the interlayer exciton emission exhibits a pronounced blueshift, reaching approximately 2.5 meV at 4 K and 1 meV at 75 K. The blueshift increases systematically with the interlayer exciton population and is consistent with a net repulsive exciton-exciton interaction, with contributions from dipole-dipole repulsion in the density regime investigated. Our results establish PLE as a sensitive approach for accessing the nonlinear, high-density regime of interlayer excitons and probing their interactions in van der Waals heterostructures.
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