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Author: Goetz, Katelyn P. ×

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    Ultrafast vibrational control of organohalide perovskite optoelectronic devices using vibrationally promoted electronic resonance
    (Basingstoke : Nature Publishing Group, 2023) Gallop, Nathaniel. P.; Maslennikov, Dmitry R.; Mondal, Navendu; Goetz, Katelyn P.; Dai, Zhenbang; Schankler, Aaron M.; Sung, Woongmo; Nihonyanagi, Satoshi; Tahara, Tahei; Bodnarchuk, Maryna I.; Kovalenko, Maksym V.; Vaynzof, Yana; Rappe, Andrew M.; Bakulin, Artem A.
    Vibrational control (VC) of photochemistry through the optical stimulation of structural dynamics is a nascent concept only recently demonstrated for model molecules in solution. Extending VC to state-of-the-art materials may lead to new applications and improved performance for optoelectronic devices. Metal halide perovskites are promising targets for VC due to their mechanical softness and the rich array of vibrational motions of both their inorganic and organic sublattices. Here, we demonstrate the ultrafast VC of FAPbBr3 perovskite solar cells via intramolecular vibrations of the formamidinium cation using spectroscopic techniques based on vibrationally promoted electronic resonance. The observed short (~300 fs) time window of VC highlights the fast dynamics of coupling between the cation and inorganic sublattice. First-principles modelling reveals that this coupling is mediated by hydrogen bonds that modulate both lead halide lattice and electronic states. Cation dynamics modulating this coupling may suppress non-radiative recombination in perovskites, leading to photovoltaics with reduced voltage losses.
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    Remarkable performance recovery in highly defective perovskite solar cells by photo-oxidation
    (London [u.a.] : RSC, 2023) Goetz, Katelyn P.; Thome, Fabian T. F.; An, Qingzhi; Hofstetter, Yvonne J.; Schramm, Tim; Yangui, Aymen; Kiligaridis, Alexander; Loeffler, Markus; Taylor, Alexander D.; Scheblykin, Ivan G.; Vaynzof, Yana
    Exposure to environmental factors is generally expected to cause degradation in perovskite films and solar cells. Herein, we show that films with certain defect profiles can display the opposite effect, healing upon exposure to oxygen under illumination. We tune the iodine content of methylammonium lead triiodide perovskite from understoichiometric to overstoichiometric and expose them to oxygen and light prior to the addition of the top layers of the device, thereby examining the defect dependence of their photooxidative response in the absence of storage-related chemical processes. The contrast between the photovoltaic properties of the cells with different defects is stark. Understoichiometric samples indeed degrade, demonstrating performance at 33% of their untreated counterparts, while stoichiometric samples maintain their performance levels. Surprisingly, overstoichiometric samples, which show low current density and strong reverse hysteresis when untreated, heal to maximum performance levels (the same as untreated, stoichiometric samples) upon the photooxidative treatment. A similar, albeit smaller-scale, effect is observed for triple cation and methylammonium-free compositions, demonstrating the general application of this treatment to state-of-the-art compositions. We examine the reasons behind this response by a suite of characterization techniques, finding that the performance changes coincide with microstructural decay at the crystal surface, reorientation of the bulk crystal structure for the understoichiometric cells, and a decrease in the iodine-to-lead ratio of all films. These results indicate that defect engineering is a powerful tool to manipulate the stability of perovskite solar cells.