Proceedings of MATSUS Fall 2026 Conference (MATSUSFall26)
Publication date: 22nd July 2026
External chemical dopants are often used to increase the concentration of charge carriers in semiconductors. Internal self-doping mechanisms are less common. One such doping mechanism involves charge transfer from a charge reservoir to a framework with high electronic mobility, as recently studied in the layered semiconductor Bi2O2Se. Charge transfer from redox-active aromatic organic molecules to the inorganic layers has also been studied in 2D lead- and tin- halide perovskites, where the adaptable interplane distance can accommodate large conjugated molecules. However, 2D perovskites tend to exhibit low band dispersion, resulting in modest increases in conductivity upon doping. The 3D halide perovskites exhibit greater band dispersion, resulting in higher carrier mobility upon electronic doping, potentially enabling new applications. However, introducing charge reservoirs into the small cuboctahedral cavities of the 3D inorganic framework is difficult because redox-active molecules with extended π systems tend to be large. In this presentation, we show how we have recently described the inclusion of redox-active and redox-inactive aromatic organic cations in a family of expanded analogs of 3D halide perovskites. We also present their properties inside a diamond-anvil cell, where compressing the metal-halide framework raises 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 the 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 that tune the carrier concentration. Efforts to achieve the same phenomenon at ambient pressure will also be presented.
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