Light-induced Kondo-like exciton-spin interaction in neodymium(II) doped hybrid perovskite

Xudong Xiao, Kyaw Zin Latt, Jue Gong, Taewoo Kim, Justin G. Connell, Yuzi Liu, H. Christopher Fry, John E. Pearson, Owen S. Wostoupal, Mengyuan Li, Calvin Soldan, Zhenzhen Yang, Richard D. Schaller, Benjamin T. Diroll (), Saw Wai Hla () and Tao Xu ()
Additional contact information
Xudong Xiao: Northern Illinois University
Kyaw Zin Latt: Argonne National Laboratory
Jue Gong: Northern Illinois University
Taewoo Kim: Argonne National Laboratory
Justin G. Connell: Argonne National Laboratory
Yuzi Liu: Argonne National Laboratory
H. Christopher Fry: Argonne National Laboratory
John E. Pearson: Argonne National Laboratory
Owen S. Wostoupal: Northern Illinois University
Mengyuan Li: Northern Illinois University
Calvin Soldan: Northern Illinois University
Zhenzhen Yang: Argonne National Laboratory
Richard D. Schaller: Argonne National Laboratory
Benjamin T. Diroll: Argonne National Laboratory
Saw Wai Hla: Argonne National Laboratory
Tao Xu: Northern Illinois University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Tuning the properties of a pair of entangled electron and hole in a light-induced exciton is a fundamentally intriguing inquiry for quantum science. Here, using semiconducting hybrid perovskite as an exploratory platform, we discover that Nd2+-doped CH3NH3PbI3 (MAPbI3) perovskite exhibits a Kondo-like exciton-spin interaction under cryogenic and photoexcitation conditions. The feedback to such interaction between excitons in perovskite and the localized spins in Nd2+ is observed as notably prolonged carrier lifetimes measured by time-resolved photoluminescence, ~10 times to that of pristine MAPbI3 without Nd2+ dopant. From a mechanistic standpoint, such extended charge separation states are the consequence of the trap state enabled by the antiferromagnetic exchange interaction between the light-induced exciton and the localized 4 f spins of the Nd2+ in the proximity. Importantly, this Kondo-like exciton-spin interaction can be modulated by either increasing Nd2+ doping concentration that enhances the coupling between the exciton and Nd2+ 4 f spins as evidenced by elongated carrier lifetime, or by using an external magnetic field that can nullify the spin-dependent exchange interaction therein due to the unified orientations of Nd2+ spin angular momentum, thereby leading to exciton recombination at the dynamics comparable to pristine MAPbI3.

Date: 2024
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DOI: 10.1038/s41467-024-50196-1

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