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Crystal Orientation Drives the Interface Physics at 2/3-Dimensional Hybrid Perovskites



Lee J. Richter, Ahmad R. Kirmani, Marine E. Bouduban, Valentine I. Queloz, Valentina M. Caselli, Kyung T. Cho, Sanghyun Paek, Cristina Roldan-Carmona, Jacques E. Moser, Tom J. Savenije, Mohammad K. Nazeeruddin, Giulia Grancini


Combining halide perovskites with tailored dimensionality into two/three-dimensional (2D/3D) systems has revealed a powerful strategy to boost the performances of perovskite photovoltaics (PVs). Despite recent advances, a clear understanding of the intimate link between interface structure and physics is still missing, leading so far to a blind optimization of the 2D/3D PVs. Here, we reveal the impact of 2D/3D crystal alignment in driving interface charge-recombination dynamics. The 2D crystal growth and orientation is manipulated by specific fluorination of phenethylammonium (PEA), used here as the organic cation backbone of the 2D component. By means of time-resolved optoelectronic analysis from femto- to microsecond, we demonstrate a static function of the 2D as an electron barrier and homogeneous surface passivant, together with a dynamic role in retarding back charge recombination. Our results reveal a crucial dependence of such beneficial effects with the 2D crystal orientation, leading to an enhanced open circuit voltage (VOC) if 2D lies parallel on the 3D. Such findings provide a deep understanding and delineate precise guidelines for the smart design of multidimensional perovskite interfaces for advanced PV and beyond.
Journal of Physical Chemistry Letters


photovolataic, thin film, GIXD, perovskite


Richter, L. , Kirmani, A. , Bouduban, M. , Queloz, V. , Caselli, V. , Cho, K. , Paek, S. , Roldan-Carmona, C. , Moser, J. , Savenije, T. , Nazeeruddin, M. and Grancini, G. (2019), Crystal Orientation Drives the Interface Physics at 2/3-Dimensional Hybrid Perovskites, Journal of Physical Chemistry Letters, [online], (Accessed June 13, 2024)


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Created September 9, 2019, Updated April 14, 2020