Mechanism of Additive-Assisted Room-Temperature Processing of Metal Halide Perovskite Thin Films
Abstract
Perovskite solar cells have received substantial attention due to their potential for low-cost photovoltaic devices on flexible or rigid substrates. Thiocyanate (SCN)-containing additives, such as MASCN (MA = methylammonium), have been shown to control perovskite film crystallization and the film microstructure to achieve effective room-temperature perovskite absorber processing. Nevertheless, the crystallization pathways and mechanisms of perovskite formation involved in MASCN additive processing are far from clear. Using in situ X-ray diffraction and photoluminescence, we investigate the crystallization pathways of MAPbI3 and reveal the mechanisms of additive-assisted perovskite formation during spin coating and subsequent N2 drying. In this work, we confirm that MASCN induces large precursor aggregates in solution and, during spin coating, promotes the formation of the perovskite phase with lower nucleation density and overall larger initial nuclei size, which forms upon reaching supersaturation in solution, in addition to intermediate solvent-complex phases. Finally, during the subsequent N2 drying, MASCN facilitates the dissociation of these precursor aggregates and the solvate phases, leading to further growth of the perovskite crystals. Our results show that the nature of the intermediate phases and their formation/dissociation kinetics determine the nucleation and growth of the perovskite phase, which subsequently impact the film microstructure. These findings providemore »
- Authors:
-
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Duke Univ., Durham, NC (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Univ. of Colorado, Boulder, CO (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1777974
- Alternate Identifier(s):
- OSTI ID: 1782080
- Grant/Contract Number:
- AC02-05CH11231; AC36-08G028308; AC02-76SF00515; SC0004993
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 13; Journal Issue: 11; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; room-temperature processing; additive engineering; halide perovskites; crystallization dynamics; film formation mechanism; precursor aggregates; in situ GIWAXS; in situ photoluminescence
Citation Formats
Abdelsamie, Maged, Li, Tianyang, Babbe, Finn, Xu, Junwei, Han, Qiwei, Blum, Volker, Sutter-Fella, Carolin M., Mitzi, David B., and Toney, Michael F. Mechanism of Additive-Assisted Room-Temperature Processing of Metal Halide Perovskite Thin Films. United States: N. p., 2021.
Web. doi:10.1021/acsami.0c22630.
Abdelsamie, Maged, Li, Tianyang, Babbe, Finn, Xu, Junwei, Han, Qiwei, Blum, Volker, Sutter-Fella, Carolin M., Mitzi, David B., & Toney, Michael F. Mechanism of Additive-Assisted Room-Temperature Processing of Metal Halide Perovskite Thin Films. United States. https://doi.org/10.1021/acsami.0c22630
Abdelsamie, Maged, Li, Tianyang, Babbe, Finn, Xu, Junwei, Han, Qiwei, Blum, Volker, Sutter-Fella, Carolin M., Mitzi, David B., and Toney, Michael F. Tue .
"Mechanism of Additive-Assisted Room-Temperature Processing of Metal Halide Perovskite Thin Films". United States. https://doi.org/10.1021/acsami.0c22630. https://www.osti.gov/servlets/purl/1777974.
@article{osti_1777974,
title = {Mechanism of Additive-Assisted Room-Temperature Processing of Metal Halide Perovskite Thin Films},
author = {Abdelsamie, Maged and Li, Tianyang and Babbe, Finn and Xu, Junwei and Han, Qiwei and Blum, Volker and Sutter-Fella, Carolin M. and Mitzi, David B. and Toney, Michael F.},
abstractNote = {Perovskite solar cells have received substantial attention due to their potential for low-cost photovoltaic devices on flexible or rigid substrates. Thiocyanate (SCN)-containing additives, such as MASCN (MA = methylammonium), have been shown to control perovskite film crystallization and the film microstructure to achieve effective room-temperature perovskite absorber processing. Nevertheless, the crystallization pathways and mechanisms of perovskite formation involved in MASCN additive processing are far from clear. Using in situ X-ray diffraction and photoluminescence, we investigate the crystallization pathways of MAPbI3 and reveal the mechanisms of additive-assisted perovskite formation during spin coating and subsequent N2 drying. In this work, we confirm that MASCN induces large precursor aggregates in solution and, during spin coating, promotes the formation of the perovskite phase with lower nucleation density and overall larger initial nuclei size, which forms upon reaching supersaturation in solution, in addition to intermediate solvent-complex phases. Finally, during the subsequent N2 drying, MASCN facilitates the dissociation of these precursor aggregates and the solvate phases, leading to further growth of the perovskite crystals. Our results show that the nature of the intermediate phases and their formation/dissociation kinetics determine the nucleation and growth of the perovskite phase, which subsequently impact the film microstructure. These findings provide mechanistic insights underlying room-temperature, additive-assisted perovskite processing and help guide further development of such facile room-temperature synthesis routes.},
doi = {10.1021/acsami.0c22630},
journal = {ACS Applied Materials and Interfaces},
number = 11,
volume = 13,
place = {United States},
year = {Tue Mar 09 00:00:00 EST 2021},
month = {Tue Mar 09 00:00:00 EST 2021}
}
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