期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 12, 期 38, 页码 9328-9335出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.1c02929
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资金
- National Key Research and Development Program of China [2020YFB1506400]
- National Natural Science Foundation of China [11974257]
- Jiangsu Distinguished Young Talent Funding [BK20200003]
- Yunnan Provincial Key S T Program [202002AB080001-1]
- Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
- China Postdoctoral Science Foundation [2020M671570]
A unified defect theory for light-soaking effects in lead halide perovskites is proposed, explaining how light illumination promotes transitions between energetically stable and metastable atomic configurations. This theory helps rationalize contradictory experimental results and provides insights for minimizing anomalous light-soaking effects to achieve high-performance stable PSCs.
Perovskite solar cells (PSCs) exhibit large, reversible, and bidirectional lightsoaking effects (LSEs); however, these anomalous LSEs are poorly understood, limiting the stability engineering and commercialization. We present a unified defect theory for the LSEs in lead halide perovskites by reconciling their defect photochemistry, ionic migration, and carrier dynamics. We considered typical detrimental defects (I-Pb, I-i, V-I) and observed that two atomic configurations were favored, where the carrier lifetime of one configuration was nearly 1 order of magnitude longer than that in the other. First-principles calculations showed that light illumination promotes ion-diffusion-assisted transitions from energetically stable configurations to metastable configurations, which are converted back to stable configurations in the dark. Fermi-level-dependent formation energies of stable/metastable configurations were used to rationalize contradictory experimental results of anomalous LSEs in PSCs observed in various studies, thus providing insights for minimizing the LSE to achieve high-performance stable PSCs.
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