One‐dimensional C4N2H14PbBr4 is shown to have a quasi‐direct electronic band structure and strongly anisotropic transport with polarized broadband emission. A GW/Bethe–Salpeter excited‐state force formalism, supported by polarized Raman and temperature‐dependent photoluminescence, identifies low–frequency Pb–Br phonons that drive ultrafast exciton self‐
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