High-entropy alloy screening for halide perovskites

As the concept of high-entropy alloying (HEA) extends beyond metals, new materials screening methods are needed. Halide perovskites (HP) are a prime case study because greater stability is needed for photovoltaics applications, and there are 322 experimentally observed HP end-members, which leads to more than 1057 potential alloys. We screen HEAHP by first calculating the configurational entropy of 106 equimolar alloys with experimentally observed end-members. To estimate enthalpy at low computational cost, we turn to the delta-lattice parameter approach, a well-known method for predicting III-V alloy miscibility. To generalize the approach for non-cubic crystals, we introduce the parameter of unit cell volume coefficient of variation (UCV), which does a good job of predicting the experimental HP miscibility data. We use plots of entropy stabilization versus UCV to screen promising alloys and identify 102 HEAHP of interest. We demonstrate the new concept of using unit cell volume coefficient of variation to approximate the enthalpic penalty of high-entropy alloy (HEA) candidates, and use it along with configurational entropy to map promising HEA halide perovskites.