Grånäs, OscarVinichenko, DmitryKaxiras, Efthimios2016-12-022016Grånäs, Oscar, Dmitry Vinichenko, and Efthimios Kaxiras. 2016. “Establishing the limits of efficiency of perovskite solar cells from first principles modeling.” Scientific Reports 6 (1): 36108. doi:10.1038/srep36108. http://dx.doi.org/10.1038/srep36108.2045-2322http://nrs.harvard.edu/urn-3:HUL.InstRepos:29626189The recent surge in research on metal-halide-perovskite solar cells has led to a seven-fold increase of efficiency, from ~3% in early devices to over 22% in research prototypes. Oft-cited reasons for this increase are: (i) a carrier diffusion length reaching hundreds of microns; (ii) a low exciton binding energy; and (iii) a high optical absorption coefficient. These hybrid organic-inorganic materials span a large chemical space with the perovskite structure. Here, using first-principles calculations and thermodynamic modelling, we establish that, given the range of band-gaps of the metal-halide-perovskites, the theoretical maximum efficiency limit is in the range of ~25–27%. Our conclusions are based on the effect of level alignment between the perovskite absorber layer and carrier-transporting materials on the performance of the solar cell as a whole. Our results provide a useful framework for experimental searches toward more efficient devices.en-USJournal Article2016-12-0210.1038/srep36108