Probing Nonlinear Interactions of Dipolar Interlayer Excitons in MoSe2/WSe2 Heterobilayers
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 MoSe2/WSe2 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.
Related
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BibTeX
@misc{shradha2026probing,
title = {{Probing Nonlinear Interactions of Dipolar Interlayer Excitons in MoSe$_2$/WSe$_2$ Heterobilayers}},
author = {Sai Shradha and Luc F. Oswald and Md Tarik Hossain and Lukas Krelle and Nicole Engel and Axel Printschler and Julian Führer and Honey Jayeshkumar Shah and Daria I. Markina and Kenji Watanabe and Takashi Taniguchi and Andrey Turchanin and Bernhard Urbaszek},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.01149},
eprint = {2609.01149},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.01149},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Probing Nonlinear Interactions of Dipolar Interlayer Excitons in MoSe_2/WSe_2 Heterobilayers
AU - Sai Shradha
AU - Luc F. Oswald
AU - Md Tarik Hossain
AU - Lukas Krelle
AU - Nicole Engel
AU - Axel Printschler
AU - Julian Führer
AU - Honey Jayeshkumar Shah
AU - Daria I. Markina
AU - Kenji Watanabe
AU - Takashi Taniguchi
AU - Andrey Turchanin
AU - Bernhard Urbaszek
PY - 2026
DA - 2026/09/01
PB - arXiv
DO - 10.48550/arxiv.2609.01149
UR - https://arxiv.org/abs/2609.01149
AB - 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.
ER -