4.8 Article

Experimental and Theoretical Studies of Magnetic Circular Dichroism for Chiral Lead Halide Perovskites

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CHEMISTRY OF MATERIALS
卷 35, 期 4, 页码 1667-1673

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AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.2c03320

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In this study, a joint experimental and theoretical research is conducted to investigate the circular dichroism (CD) and magnetic circular dichroism (MCD) of highly crystalline and solution-processable chiral lead halide perovskites. The experimental results show that the MCD strengths of the chiral perovskites can be remarkably enhanced with increasing fields up to +/- 1.6 T. The study is important in elucidating the microscopic origin of optical activities in chiral perovskites using magnetic fields as a tool.
Chiral lead halide perovskites (LHPs) exhibit pronounced absorption or transmission circular dichroism (CD), which can be efficiently tuned by externally applied magnetic fields, giving rise to magnetic circular dichroism (MCD). To date, a systematic understanding of natural optical activities (NOAs) and magneto-optical activities (MOAs) in LHPs on an equal footing is still lacking. In this work, a joint experimental and theoretical study is carried out systematically in order to establish a unified picture of CD and MCD via a gyration vector for highly crystalline and solution-processable chiral LHPs. Experimentally, MCD strengths that appear near photoabsorption band edges of the chiral LHPs can be enhanced remarkably with increasing fields up to +/- 1.6 T. The experimental results can be well accounted for by a theory based on excitonic states, material chirality, and field dependence of the gyration vector. Importantly, numerical values of the exciton's g-factor and chirality-induced spin-orbit coupling (SOC) strength can be extracted. Our work suggests that the magnetic field can be an important tool to elucidate the microscopic origin of NOA in chiral LHPs.

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