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Charge Reservoirs in an Expanded Halide Perovskite Analog: Enhancing High-Pressure Conductivity through Redox-Active Molecules
Roc Matheu (roc.matheu@ub.edu)
Departament de Química Inorgànica i Orgànica, Universitat de Barcelona.
As halide perovskites and their derivatives are being developed for numerous optoelectronic applications, controlling their electronic doping remains a fundamental challenge. We have recently discovered a novel strategy of using redox-active organic molecules as stoichiometric electron acceptors in new expanded perovskite analogs. Compressing the metal-halide framework drives up the valence band relative to the acceptor orbitals of the organic molecules. Thus, the material’s electronic conductivity increases by a factor of 105 with pressure, reaching 50(17) S cm–1 at 60 GPa, exceeding the high-pressure conductivities of most halide perovskites. This conductivity enhancement is attributed to an increased hole density created by reduction of the redox-active molecules. This work elevates the role of organic cations in 3D metal-halides, from templating the structure to serving as charge reservoirs for tuning the carrier concentration.