Impact of Surface Adsorbates and Dimensionality on Templating of Halide Perovskites

E. Fransson, J. Wiktor, and P. Erhart
doi: 10.48550/arXiv.2405.08336
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Two-dimensional (2D) halide perovskites (HPs) are promising materials for various optoelectronic applications, yet a comprehensive understanding of their dynamics is still elusive. Here, we offer insight into the dynamics of prototypical 2D HPs based on MAPbI3 as a function of linker molecule and the number of perovskite layers using atomic scale simulations. We show that the layers closest to the linker undergo transitions that are distinct from those of the interior layers. These transitions can take place anywhere between a few tens of Kelvin below to more than 100 K above the cubic-tetragonal transition of bulk MAPbI3. In combination with the thickness of the perovskite layer this enables one to template phase transitions and tune the dynamics over a wide temperature range. Our results thereby reveal the details of an important and generalizable design mechanism for tuning the properties of these materials.