Constructive molecular configurations for surface-defect passivation of perovskite photovoltaics

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Science  20 Dec 2019:
Vol. 366, Issue 6472, pp. 1509-1513
DOI: 10.1126/science.aay9698

Optimizing surface passivation

Unproductive charge recombination at surface defects can limit the efficiency of hybrid perovskite solar cells, but these defects can be passivated by the binding of small molecules. Wang et al. studied three such small molecules—theophylline, caffeine, and theobromine—that bear both carbonyl and amino groups. For theophylline, hydrogen bonding of the amino hydrogen to surface iodide optimized the carbonyl interaction with a lead antisite defect and improved the efficiency of a perovskite cell from 21 to 22.6%.

Science, this issue p. 1509


Surface trap–mediated nonradiative charge recombination is a major limit to achieving high-efficiency metal-halide perovskite photovoltaics. The ionic character of perovskite lattice has enabled molecular defect passivation approaches through interaction between functional groups and defects. However, a lack of in-depth understanding of how the molecular configuration influences the passivation effectiveness is a challenge to rational molecule design. Here, the chemical environment of a functional group that is activated for defect passivation was systematically investigated with theophylline, caffeine, and theobromine. When N-H and C=O were in an optimal configuration in the molecule, hydrogen-bond formation between N-H and I (iodine) assisted the primary C=O binding with the antisite Pb (lead) defect to maximize surface-defect binding. A stabilized power conversion efficiency of 22.6% of photovoltaic device was demonstrated with theophylline treatment.

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