Long-Lived Hot Carriers in Two-Dimensional Perovskites: The Role of Alternating Cations in Interlayer Space

Qi Wei, Hui Ren, Jinjie Liu, Qi Liu, Chenhao Wang, Ting Wai Lau, Luwei Zhou, Tieyuan Bian, Yifan Zhou, Pengzhi Wang, Qiong Lei, Omar F. Mohammed, Mingjie Li, Jun Yin

Research output: Journal article publicationJournal articleAcademic researchpeer-review

3 Citations (Scopus)

Abstract

Solar absorbers featuring prolonged hot-carrier (HC) cooling are highly desired for the development of HC solar cells. Two-dimensional (2D) hybrid perovskites are known for their exceptional stability and tunable optoelectronic properties. Nevertheless, their hot-carrier dynamics have been inadequately investigated. Here, we demonstrate ultraslow hot-carrier cooling with a lifetime >2 ns and long HC diffusion length in 2D (ACA)(MA)PbI4 (ACA = acetamidinium) with alternating cations in the interlayer space (ACI), surpassing those of 3D MAPbBr3 and 2D Ruddlesden-Popper (PEA)2PbI4. Our nonadiabatic molecular dynamics simulations with spin-orbit coupling show that the enhanced HC cooling in the ACI-phase 2D perovskite is due to multiple split-off bands and reduced electron-phonon coupling. Furthermore, the hot electrons can be efficiently extracted from (ACA)(MA)PbI4 and then transferred to the electron-transporting layer. These new insights highlight the benefit of manipulating interlayer cations in 2D perovskites as an advantageous approach to control long-lived hot carriers, thus potentially enhancing photovoltaic device performance.

Original languageEnglish
Pages (from-to)4315-4322
Number of pages8
JournalACS Energy Letters
Volume8
Issue number10
DOIs
Publication statusPublished - Sept 2023

ASJC Scopus subject areas

  • Chemistry (miscellaneous)
  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Energy Engineering and Power Technology
  • Materials Chemistry

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