4.6 Article

The Significance of Polarons and Dynamic Disorder in Halide Perovskites

期刊

ACS ENERGY LETTERS
卷 6, 期 6, 页码 2162-2173

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.1c00506

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资金

  1. Center for Non-Perturbative Studies of Functional Materials - Computational Materials Sciences Program of the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division
  2. Molecular Foundry, a DOE Office of Science User Facility - Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
  3. U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-FG0207ER46431]
  4. Office of Science of the U.S. Department of Energy [DE-AC0205CH11231]
  5. National Science Foundation Graduate Research Fellowship [DGE-1644869]
  6. Alexander von Humboldt Foundation
  7. German Excellence Initiative
  8. European Union Seventh Framework Programme [291763]
  9. Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy [EXC 2089/1-390776260]
  10. [NSF-CHE-1954791]

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The development of halide perovskite semiconductors has led to significant technological breakthroughs in the fields of photovoltaics and light-emitting diodes, but it has also raised intriguing fundamental properties that demand explanation. Despite the existence of polaronic behavior in these systems, standard models used to describe a polaron mechanism appear to be strongly violated in these materials, highlighting the importance of alternative concepts like dynamic disorder to explain their physical characteristics.
The development of halide perovskite semiconductors led to various technological breakthroughs in optoelectronics, in particular in the areas of photovoltaics and light-emitting diodes. Additionally, the study of their fundamental properties has uncovered intriguing puzzles that demand explanation. Polaronic effects associated with the coupling microscopic mechanism to explain various unusual experimental of electrons and holes to polar lattice vibrations are often invoked as a - observations. While some form of polaronic behavior undoubtedly exists in these systems, several assumptions underlying standard models used to describe a polaron mechanism appear to be strongly violated in these materials. In this Perspective, we investigate the role of polaronic effects in halide perovskites and summarize signatures and failures of the polaron picture to explain physical characteristics of the materials. We highlight the importance of the complementary dynamic disorder concept that can rationalize various key properties of halide perovskites for which standard polaron and band-theory pictures of carrier transport fail.

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