| Title: |
Unveiling the role of halide mixing in the crystallization kinetics and charge transfer mechanisms of wide-bandgap organic–inorganic halide perovskites |
| Authors: |
Li, Nian; Pratap, Shambhavi; Guo, Renjun; He, Zirui; Liang, Suzhe; Jia, Xiangkun; Gholipoor, Mohammad; Babbe, Finn; Barchi, Nicola S; Slack, Jonathan L; Tamura, Nobumichi; Qiao, Liang; Sutter-Fella, Carolin M; Müller-Buschbaum, Peter |
| Source: |
Energy & Environmental Science, vol 18, iss 24 |
| Publisher Information: |
eScholarship, University of California |
| Publication Year: |
2025 |
| Collection: |
University of California: eScholarship |
| Subject Terms: |
3403 Macromolecular and Materials Chemistry (for-2020); 34 Chemical Sciences (for-2020); 3406 Physical Chemistry (for-2020); 40 Engineering (for-2020); 4016 Materials Engineering (for-2020); Energy (science-metrix) |
| Subject Geographic: |
10460 - 10472 |
| Description: |
Understanding the crystallization kinetics of Br–I mixed-halide WBG perovskite films, and their correlation to the crystallographic structure and charge transfer dynamics, is critical for advancing WBG perovskite devices. Despite many efforts to increase the photovoltaic performances of wide-bandgap (WBG, with a Br content above 20%) perovskite solar cells based on bromine–iodine (Br–I) mixed-halide perovskites, understanding the crystallization kinetics of WBG perovskite films, as well as the role of Br mixing in the crystallization kinetics, is still lacking. Furthermore, an overlooked aspect is the correlation of the halide compositions, crystallization kinetics, crystallographic structure, and charge transfer dynamics. Here, we unveil that Br–I mixed-halide WBG perovskite films undergo two intrinsically different crystallization kinetic processes. One is the intermediate solvent-complex phase-assisted growth (I-rich), and the other is top-to-bottom downward growth (Br-rich). Such downward growth (including high Br concentrations) correlates with the formation of a highly vertically oriented perovskite film, which is accompanied by defect formation caused by a dissolving and recrystallization process coupled with halide homogenization. Consequently, Br-rich WBG perovskite films exhibit enhanced charge carrier transport, but are concurrently plagued by non-radiative charge recombination. Addressing this fundamental perspective is critical to precisely tailor Br-related crystallization, which significantly affects the structure and optoelectronic properties of WBG perovskite films and devices. |
| Document Type: |
article in journal/newspaper |
| File Description: |
application/pdf |
| Language: |
unknown |
| Relation: |
qt6rf2z660; https://escholarship.org/uc/item/6rf2z660; https://escholarship.org/content/qt6rf2z660/qt6rf2z660.pdf |
| DOI: |
10.1039/d5ee05540g |
| Availability: |
https://escholarship.org/uc/item/6rf2z660; https://escholarship.org/content/qt6rf2z660/qt6rf2z660.pdf; https://doi.org/10.1039/d5ee05540g |
| Rights: |
CC-BY |
| Accession Number: |
edsbas.944E82B9 |
| Database: |
BASE |