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

Jun Yin, Rounak Naphade, Partha Maity, Luis Gutierrez Arzaluz, Dhaifallah R. Almalawi, Iman S. Roqan, Jean-Luc Bredas, Osman Bakr, Omar F. Mohammed

Research output: Contribution to journalArticlepeer-review

46 Scopus citations

Abstract

AbstractHot-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.
Original languageEnglish (US)
JournalNature Communications
Volume12
Issue number1
DOIs
StatePublished - Jun 28 2021

Bibliographical note

KAUST Repository Item: Exported on 2021-06-30
Acknowledgements: This work was supported by the King Abdullah University of Science and Technology (KAUST) and the College of Science of the University of Arizona. J.Y., J.L.B., and O.F.M. acknowledge the Supercomputing Laboratory at KAUST for their computational and storage resources, as well as their gracious assistance.

ASJC Scopus subject areas

  • General Biochemistry, Genetics and Molecular Biology
  • General Chemistry
  • General Physics and Astronomy

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