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We  present  herein  an  experimental  screening  study  that  assesses  how  partially  replacing  Pb  in methylammonium  lead  triiodide  perovskite  films  with  nine  different  alternative,  divalent  metal species,  B  = {Co, Cu, Fe, Mg, Mn, Ni, Sn, Sr, and Zn}, influences  photovoltaic performance and optical  properties.  Our  findings  indicate  the  perovskite  film  is  tolerant  to  most  of  the  considered homovalent  metal  species  with  lead-cobalt  compositions  yielding  the  highest  power  conversion efficiencies  when  less  than  6%  of  the  Pb2+ ions  are  replaced.  Through  subsequent  materials characterisation, we demonstrate  for the first time  that  partially substituting  Pb2+ at the B-sites of the perovskite  lattice  is  not  restricted  to  Group  IV  elements  but  is  also  possible  with  at  least  Co2+. Moreover, adjusting the molar ratio of Pb:Co in the mixed-metal perovskite affords new opportunities to  tailor  the  material  properties  while  maintaining  stabilised  device  efficiencies  above  16%  in optimised  solar  cells.  Specifically,  crystallographic  analysis  reveals  that  Co2+ incorporates  into  the  perovskite lattice and  increasing  its concentration can mediate a crystal structure transition from the cubic to tetragonal phase  at room-temperature. Likewise, Co2+ substitution  continually modifies the perovskite  work  function  and  band  edge  energies  without  either  changing  the  band  gap  or electronically  doping  the  intrinsic  material.  By  leveraging  this  orthogonal  dimension  of  electronic tunability,  we  achieve  remarkably  high  open-circuit voltages  up  to  1.08 V  with  an  inverted  device architecture  by  shifting  the  perovskite  into  a  more  favourable  energetic  alignment  with  the PEDOT:PSS hole transport material

Tailoring metal halide perovskites through metal substitution: influence on photovoltaic and material properties