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

David Giovanni, Jia Wei Melvin Lim, Zhongcheng Yuan, Swee Sien Lim, Marcello Righetto, Jian Qing, Qiannan Zhang, Herlina Arianita Dewi, Feng Gao, Subodh Gautam Mhaisalkar, Nripan Mathews and Tze Chien Sum ()
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David Giovanni: Nanyang Technological University
Jia Wei Melvin Lim: Nanyang Technological University
Zhongcheng Yuan: Linköping University
Swee Sien Lim: Nanyang Technological University
Marcello Righetto: Nanyang Technological University
Jian Qing: Linköping University
Qiannan Zhang: Nanyang Technological University
Herlina Arianita Dewi: Research Techno Plaza
Feng Gao: Linköping University
Subodh Gautam Mhaisalkar: Research Techno Plaza
Nripan Mathews: Research Techno Plaza
Tze Chien Sum: Nanyang Technological University

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41467-019-11251-4

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