期刊
ACS ENERGY LETTERS
卷 6, 期 2, 页码 419-428出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.0c02270
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资金
- HyPerCells (a joint graduate school of the University of Potsdam and the Helmholtz-Zentrum Berlin)
- Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) [423749265, 424709669]
- Federal Ministry for Economic Affairs and Energy within the framework of the 7th Energy Research Programme (P3T-HOPE) [03EE1017C]
- Helmholtz International Research School HI-SCORE [HIRS-0008]
- HyPerCells Graduate School
- Swiss Federal Office of Energy [SI/501804-01]
- Swiss National Science Foundation [176552, CRSII5_171000]
- EU Horizon 2020 Marie Sklodowska-Curie Individual Fellowship under grant POSITS [747221]
- Marie Sklodowska-Curie Individual Fellowship from the European Union's Horizon 2020 Research and Innovation Program [747221]
- CSIRO Research Office
- Marie Curie Actions (MSCA) [747221] Funding Source: Marie Curie Actions (MSCA)
- Swiss National Science Foundation (SNF) [CRSII5_171000] Funding Source: Swiss National Science Foundation (SNF)
This study investigates halide segregation in methylammonium-free wide bandgap perovskites using photoluminescence quantum yield (PLQY) and advanced electron microscopy techniques. The research reveals that phase segregation and charge funnelling are essential for achieving high PLQYs, specifically at low energies, otherwise not achievable in non-segregated perovskites with a similar bandgap.
This work investigates halide segregation in methylammonium-free wide bandgap perovskites by photoluminescence quantum yield (PLQY) and advanced electron microscopy techniques. Our study reveals how the formation of nano-emitting low-energy domains embedded in a wide bandgap matrix, located at surfaces and grain boundaries, enables a PLQY up to 25%. Intensity-dependent PLQY measurement and PL excitation spectroscopy revealed efficient charge funnelling and the failure of optical reciprocity between absorption and emission, limiting the use of PLQY data to determine the quasi-Fermi level splitting (QFLS) in these layers. Concomitantly, the small spectral overlap between emission and absorption reduces photon re-absorption. We demonstrate that phase segregation and charge funnelling, although harmful for the radiative efficiency of the mixed phase, are essential for achieving high PLQYs, selectively at low energies, otherwise not achievable in non-segregated perovskites with a similar bandgap. This promotes the applicability of this phenomenon in thermally stable high-efficiency emitting devices and color-conversion heterostructures.
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