Double Perovskites overtaking the single perovskites : A set of new solar harvesting materials with much higher stability and efficiency

Abstract: Hybrid Lead halide perovskites, despite having unique intrinsic properties with the possibility of flexible synthesis and device fabrication, still suffer from two fundamental issues, i.e. stability in external environment and toxicity due to lead. More recently, double perovskite materials have emerged as a promising choice. The main outcome from various studies on this class can essentially be summarized into two categories, (i) either they have indirect band gap or (ii) direct but large optical band gap, which are not suitable for solar devices. Here we propose a combinatorial set of stable double perovskite materials, Cs$2$BB$^{'}$X$_6$ (for various B, B$^{'}$) (X=Cl,Br,I), which show indirect to direct band gap transition via small Pb$^{+2}$ doping. This kind of doping has helped to change the topology of band structure triggering an optically allowed transition from valence band maxima to conduction band minima. It also reduces the band gap significantly, bringing it well in the visible region. Simulation reveals comparable/higher absorption coefficient and solar efficiency with respect to the state of the art photovoltaic absorber material CH$_3$NH$_3$PbI$_3$. Our experimentally measured properties on Cs$_2$(Ag${0.75}$Pb${0.25}$)(Bi${0.75}$Pb$_{0.25}$)Br$_6$ agrees fairly well with the theoretical predictions. With higher stability than CH$_3$NH$_3$PbI$_3$, this material shows the potential to be a better candidate.