Proceedings of Online nanoGe Fall Meeting 20 (OnlineNFM20)
Publication date: 4th October 2020
Vacancy-ordered triple perovskites have recently come under the scientific spotlight as promising materials for high-performance next-generation optoelectronic technologies.[1,2] Their A3B2X9 stoichiometry facilitates the replacement of the toxic Pb2+ cation with a benign isolectronic B3+ cation (e.g. Bi3+ or Sb3+), while preserving the perovskite crystal structure. Unfortunately, however, these materials tend to exhibit large bandgaps (> 2 eV), impeding their application in many photo-catalytic/voltaic devices.[3,4]
In this work, we demonstrate a drastic shift of over 1 eV in the optical absorption onset of Cs3Bi2Br9 (from 2.58 eV to 1.39 eV), upon doping with tin. Through a combination of detailed theoretical and experimental characterisation of this novel material, we elucidate the origin of broadband absorption. Sn is found to disproportionate in the doped material, inducing a strong intervalence charge transfer (IVCT) transition, whilst preserving the structural integrity of the perovskite framework.
Our work provides valuable insight regarding the effects of mixed-valency and structure-property relationships in perovskite-inspired materials, guiding design strategies and expanding the compositional space of candidate materials. Moreover, we anticipate that this massive reduction in absorption onset could aid charge transport and/or photo-catalytic performance, opening the door to unexplored applications of this material class.
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