Samenvatting
The efficient harnessing of hot carriers holds transformative potential for next-generation optoelectronic devices. Halide perovskites, with their remarkably long carrier lifetimes exceeding 10 picoseconds, stand at the forefront of this research frontier. Yet, a fundamental paradox persists: why does efficient hot carrier capture remain elusive despite these extended lifetimes? Here, this conundrum is unraveled by constructing a donor–acceptor model system: perovskite nanocrystal and fullerene hybrids. It is demonstrated that the challenge lies not only in the carrier lifetime itself but in the nature of the coupling between donor and acceptor components. Remarkably, it is discovered that the formation of ground-state complexes, with effective coupling across a wide energy range, not only overcomes the initially forbidden hot carrier capture within these hybrids but also dramatically enhances it, achieving a ≈76% hot carrier capture efficiency. This finding shifts the paradigm of hot carrier capture from extending carrier lifetimes to engineering donor–acceptor coupling, illuminating a path toward practical hot carrier applications.
| Originele taal-2 | Engels |
|---|---|
| Artikelnummer | 2415735 |
| Aantal pagina's | 9 |
| Tijdschrift | Advanced Functional Materials |
| Volume | 35 |
| Nummer van het tijdschrift | 8 |
| DOI's | |
| Status | Gepubliceerd - 19 feb. 2025 |
Bibliografische nota
Publisher Copyright:© 2024 The Author(s). Advanced Functional Materials published by Wiley-VCH GmbH.
Financiering
Y.L., J.J., and D.W. contributed equally to this work. The authors are very grateful to Prof. James Lloyd-Hughes (Department of Physics, University of Warwick, United Kingdom), and Dr. Maurizio Monti (Institute for Physics and Astronomy, Denmark) for their kind providing of the TTM fitting code and patient explanations about their code. The authors also appreciate the meaningful help on FTIR analysis from Prof. Ishida Takayuki (The University of Electro-Communications, Japan). This work was supported by the Japan Science and Technology Agency (JST) Mirai program (JPMJMI17EA), MEXT KAKENHI Grant (26286013, 17H02736), JST SPRING (Grant Number JPMJSP2131). S.T. and J.J. acknowledge funding by the Computational Sciences for Energy Research (CSER) tenure track program of Shell and NWO (Project number 15CST04-2) and NWO START-UP, the Netherlands. Y.L., J.J., and D.W. contributed equally to this work. The authors are very grateful to Prof. James Lloyd\u2010Hughes (Department of Physics, University of Warwick, United Kingdom), and Dr. Maurizio Monti (Institute for Physics and Astronomy, Denmark) for their kind providing of the TTM fitting code and patient explanations about their code. The authors also appreciate the meaningful help on FTIR analysis from Prof. Ishida Takayuki (The University of Electro\u2010Communications, Japan). This work was supported by the Japan Science and Technology Agency (JST) Mirai program (JPMJMI17EA), MEXT KAKENHI Grant (26286013, 17H02736), JST SPRING (Grant Number JPMJSP2131). S.T. and J.J. acknowledge funding by the Computational Sciences for Energy Research (CSER) tenure track program of Shell and NWO (Project number 15CST04\u20102) and NWO START\u2010UP, the Netherlands.