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Factors Enabling Delocalized Charge-Carriers in Pnictogen-Based Solar Absorbers: In-depth Investigation into CuSbSe2

Inorganic semiconductors based on heavy pnictogen cations (Sb3+ and Bi3+) have gained significant attention as potential nontoxic and stable alternatives to lead-halide perovskites for solar cell applications. A limitation of these novel materials, which is being increasingly commonly found, is carrier localization, which substantially reduces mobilities and diffusion lengths. Herein, the layered příbramite CuSbSe2 is investigated and discovered to have delocalized free carriers, as shown through optical pump terahertz probe spectroscopy and temperature-dependent mobility measurements. Using a combination of theory and experiment, it is found that the underlying factors are: 1) weak coupling to acoustic phonons due to low deformation potentials, as lattice distortions are primarily accommodated through rigid inter-layer movement rather than straining inter-atomic bonds, and 2) weak coupling to optical phonons due to the ionic contributions to the dielectric constant being low compared to electronic contributions. This work provides important insights into how pnictogen-based semiconductors avoiding carrier localization could be identified.