Ultrafast long-range spin-funneling in solution-processed Ruddlesden-Popper halide perovskites

Nature Communications
David GiovanniTze Chien Sum

Abstract

Room-temperature spin-based electronics is the vision of spintronics. Presently, there are few suitable material systems. Herein, we reveal that solution-processed mixed-phase Ruddlesden-Popper perovskite thin-films transcend the challenges of phonon momentum-scattering that limits spin-transfer in conventional semiconductors. This highly disordered system exhibits a remarkable efficient ultrafast funneling of photoexcited spin-polarized excitons from two-dimensional (2D) to three-dimensional (3D) phases at room temperature. We attribute this efficient exciton relaxation pathway towards the lower energy states to originate from the energy transfer mediated by intermediate states. This process bypasses the omnipresent phonon momentum-scattering in typical semiconductors with stringent band dispersion, which causes the loss of spin information during thermalization. Film engineering using graded 2D/3D perovskites allows unidirectional out-of-plane spin-funneling over a thickness of ~600 nm. Our findings reveal an intriguing family of solution-processed perovskites with extraordinary spin-preserving energy transport properties that could reinvigorate the concepts of spin-information transfer.

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Citations

Jun 3, 2020·Nature Communications·Marcello RighettoTze Chien Sum
Jul 19, 2020·Nature Communications·Jia GuoGuichuan Xing
Jun 22, 2021·IScience·Kunping GuoFranco Cacialli
Feb 6, 2020·The Journal of Physical Chemistry Letters·Meng ZhouHe Wang
Feb 20, 2020·ACS Nano·Christopher C PriceVivek B Shenoy
Sep 29, 2020·Journal of the American Chemical Society·Laura PiveteauMaksym V Kovalenko
Nov 13, 2021·Journal of the American Chemical Society·Xihan ChenMatthew C Beard

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