Manipulation of hot carrier cooling dynamics in two-dimensional Dion–Jacobson hybrid perovskites via Rashba band splitting

Jun Yin, Rounak Naphade, Partha Maity, Luis Gutiérrez-Arzaluz, Dhaifallah Almalawi, Iman S. Roqan, Jean-Luc Brédas (), Osman M. Bakr () and Omar F. Mohammed ()
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Jun Yin: Advanced Membranes and Porous Materials Center, Division of Physical Science and Engineering, King Abdullah University of Science and Technology
Rounak Naphade: KAUST Catalysis Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology
Partha Maity: Advanced Membranes and Porous Materials Center, Division of Physical Science and Engineering, King Abdullah University of Science and Technology
Luis Gutiérrez-Arzaluz: Advanced Membranes and Porous Materials Center, Division of Physical Science and Engineering, King Abdullah University of Science and Technology
Dhaifallah Almalawi: Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology
Iman S. Roqan: Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology
Jean-Luc Brédas: The University of Arizona
Osman M. Bakr: KAUST Catalysis Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology
Omar F. Mohammed: Advanced Membranes and Porous Materials Center, Division of Physical Science and Engineering, King Abdullah University of Science and Technology

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Hot-carrier cooling processes of perovskite materials are typically described by a single parabolic band model that includes the effects of carrier-phonon scattering, hot phonon bottleneck, and Auger heating. However, little is known (if anything) about the cooling processes in which the spin-degenerate parabolic band splits into two spin-polarized bands, i.e., the Rashba band splitting effect. Here, we investigated the hot-carrier cooling processes for two slightly different compositions of two-dimensional Dion–Jacobson hybrid perovskites, namely, (3AMP)PbI4 and (4AMP)PbI4 (3AMP = 3-(aminomethyl)piperidinium; 4AMP = 4-(aminomethyl)piperidinium), using a combination of ultrafast transient absorption spectroscopy and first-principles calculations. In (4AMP)PbI4, upon Rashba band splitting, the spin-dependent scattering of hot electrons is responsible for accelerating hot-carrier cooling at longer delays. Importantly, the hot-carrier cooling of (4AMP)PbI4 can be extended by manipulating the spin state of the hot carriers. Our findings suggest a new approach for prolonging hot-carrier cooling in hybrid perovskites, which is conducive to further improving the performance of hot-carrier-based optoelectronic and spintronic devices.

Date: 2021
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DOI: 10.1038/s41467-021-24258-7

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