Tuning relaxation and nonlinear upconversion of valley-exciton-polaritons in a monolayer semiconductor

Hangyong Shan, Jamie M. Fitzgerald, Roberto Rosati, Gilbert Leibeling, Kenji Watanabe, Takashi Taniguchi, Seth Ariel Tongay, Falk Eilenberger, Martin Esmann, Sven Höfling, Ermin Malic and Christian Schneider ()
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Hangyong Shan: Carl von Ossietzky University Oldenburg
Jamie M. Fitzgerald: Philipps-Universität Marburg
Roberto Rosati: Philipps-Universität Marburg
Gilbert Leibeling: Fraunhofer-Institute for Applied Optics and Precision Engineering IOF
Kenji Watanabe: 1-1 Namiki
Takashi Taniguchi: 1-1 Namiki
Seth Ariel Tongay: Arizona State University
Falk Eilenberger: Fraunhofer-Institute for Applied Optics and Precision Engineering IOF
Martin Esmann: Carl von Ossietzky University Oldenburg
Sven Höfling: Am Hubland
Ermin Malic: Philipps-Universität Marburg
Christian Schneider: Carl von Ossietzky University Oldenburg

Nature Communications, 2025, vol. 16, issue 1, 1-8

Abstract: Abstract Controlling exciton relaxation and energy conversion pathways via their coupling to photonic modes is a central task in cavity-mediated quantum materials research. In this context, the light-matter hybridization in optical cavities can lead to intriguing effects, such as modified carrier transport, enhancement of optical quantum yield, and control of chemical reaction pathways. Here, we investigate the impact of the strong light-matter coupling regime on energy conversion, both in relaxation and upconversion schemes, by utilizing a strongly charged MoSe2 monolayer embedded in a spectrally tunable open-access cavity. We find that the charge carrier gas yields a significantly modified photoluminescence response of cavity exciton-polaritons, dominated by an intra-cavity like pump scheme. In addition, upconversion luminescence emerges from a population transfer from fermionic trions to bosonic exciton-polaritons. Due to the availability of multiple optical modes in the tunable open cavity, it seamlessly meets the cavity-enhanced double resonance condition required for an efficient upconversion. The latter can be actively tuned via the cavity length in-situ, displaying nonlinear scaling in intensity and fingerprints of the valley polarization. This suggests mechanisms that include both trion-trion Auger scattering and phonon absorption as its underlying microscopic origin.

Date: 2025
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DOI: 10.1038/s41467-025-65737-5

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