Nanoscale-Resolved Surface-to-Bulk Electron Transport in CsPbBr3 Perovskite
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Date
2022-02-09
Publication Type
Journal Article
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Abstract
Describing the nanoscale charge carrier transport at surfaces and interfaces is fundamental for designing high-performance optoelectronic devices. To achieve this, we employ time- and angle-resolved photoelectron spectroscopy with ultraviolet pump and extreme ultraviolet probe pulses. The resulting high surface sensitivity reveals an ultrafast carrier population decay associated with surface-to-bulk transport, which was tracked with a sub-nanometer spatial resolution normal to the surface, and on a femtosecond time scale, in the case of the inorganic CsPbBr3 lead halide perovskite. The decay time exhibits a pronounced carrier density dependence, which is attributed via modeling to enhanced diffusive transport and concurrent recombination. The transport is found to approach an ordinary diffusive regime, limited by electron-hole scattering, at the highest excitation fluences. This approach constitutes an important milestone in our capability to probe hot-carrier transport at solid interfaces with sub-nanometer resolution in a theoretically and experimentally challenging, yet technologically relevant, high-carrier-density regime.
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published
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Journal / series
Volume
22 (3)
Pages / Article No.
1067 - 1074
Publisher
American Chemical Society
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Subject
nanoscale charge carrier transport; diffusion; ultrafast photoelectron spectroscopy; electronic structure; semiconductors; lead halide perovskites
Organisational unit
03934 - Kovalenko, Maksym / Kovalenko, Maksym
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Funding
186406 - Spin and recombination dynamics of excitons and carriers in metal halide perovskites (SNF)