Unveiling Ultrafast Spin-Valley Dynamics and Phonon-Mediated Charge Transfer in MoSe$_{2}$/WSe$_{2}$ Heterostructures

We use helicity-resolved ultrafast transient absorption spectroscopy to study spin-valley polarization dynamics in a vertically stacked MoSe$_{2}$/WSe$_{2}$ heterostructure. The experimental findings reveal details of interlayer charge transfer on ultrafast timescales, showing that the spin-valley p...

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Hauptverfasser: Wagner, Julian, Bernhardt, Robin, Rieland, Lukas, Abdul-Aziz, Omar, Li, Qiuyang, Zhu, Xiaoyang, Conte, Stefano Dal, Cerullo, Giulio, van Loosdrecht, Paul H. M, Hedayat, Hamoon
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Sprache:eng
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Zusammenfassung:We use helicity-resolved ultrafast transient absorption spectroscopy to study spin-valley polarization dynamics in a vertically stacked MoSe$_{2}$/WSe$_{2}$ heterostructure. The experimental findings reveal details of interlayer charge transfer on ultrafast timescales, showing that the spin-valley polarized state of photoexcited carriers is conserved during the charge transfer and formation of interlayer excitons. Our results confirm that phonon scattering mediates the interlayer charge transfer process, while a high phonon population at elevated temperatures causes a significant decrease in spin-valley selective charge transfer. Moreover, the experimental findings demonstrate the possibility that interlayer excitons and their spin-valley polarization can be probed in the optical response of intralayer excitons. These findings pave the way for ultrafast detection, control, and manipulation of spin-valley polarized excitons in transition metal dichalcogenide-based 2D heterostructures.
DOI:10.48550/arxiv.2411.14180