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Perovskite solar cells are one of the most attracting cells because ofremarkably improved power conversion efficiency (PCE) recently. Toward theirpractical application, it is important not only to increase the PCE but also toelucidate the deterioration mechanism. Here, we present operando directobservation of spin states in the cells using electron spin resonance (ESR)spectroscopy in order to investigate the operation and deterioration mechanismsfrom a microscopic viewpoint. By simultaneous measurements of solar-cell andESR characteristics of the same cell, the spin states in the hole-transportmaterial (HTM) spiro-OMeTAD are demonstrated to be changed at the molecularlevel, which varies the device performance under device operation. Thesevariations are ascribed to the change of hole transport by charge-carrierscatterings and filling of deep trapping levels in the HTM, and to interfacialelectric dipole layers formed at the HTM interfaces. In addition, reverseelectron transfer from TiO2 layer to the HTM layer is directly demonstrated atthe molecular level under ultraviolet light irradiation, which causes thedecrease in the HTM doping effect. Thus, conducting such operando microscopicinvestigation on the internal states in the cells would be useful to obtain anew further guideline for improving the device performance and durability.

Operando direct observation of spin states correlated with device performance in perovskite solar cells