Transient circular dichroism and exciton spin dynamics in all-inorganic halide perovskites

Weijie Zhao, Rui Su, Yuqing Huang, Jinqi Wu, Chee Fai Fong, Jiangang Feng and Qihua Xiong ()
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Weijie Zhao: Nanyang Technological University
Rui Su: Nanyang Technological University
Yuqing Huang: Nanyang Technological University
Jinqi Wu: Nanyang Technological University
Chee Fai Fong: Nanyang Technological University
Jiangang Feng: Nanyang Technological University
Qihua Xiong: Nanyang Technological University

Nature Communications, 2020, vol. 11, issue 1, 1-7

Abstract: Abstract All-inorganic metal halides perovskites (CsPbX3, X = Br or Cl) show strong excitonic and spin-orbital coupling effects, underpinning spin-selective excitonic transitions and therefore exhibiting great promise for spintronics and quantum-optics applications. Here we report spin-dependent optical nonlinearities in CsPbX3 single crystals by using ultrafast pump-probe spectroscopy. Many-body interactions between spin-polarized excitons act like a pseudo-magnetic field and thus lift the degeneracy of spin states resulting in a photoinduced circular dichroism. Such spontaneous spin splitting between “spin-up” and “spin-down” excitons can be several tens of milli-electron volts under intense excitations. The exciton spin relaxation time is ~20 picoseconds at very low pump fluence, the longest reported in the metal halides perovskites family at room temperature. The dominant spin-flip mechanism is attributed to the electron-hole exchange interactions. Our results provide essential understandings towards realizing practical spintronics applications of perovskite semiconductors.

Date: 2020
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DOI: 10.1038/s41467-020-19471-9

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