We reveal coherent exciton-phonon interactions in the two-dimensional (2D) layered hybrid organic-inorganic semiconductor silver phenylselenolate (AgSePh). Using femtosecond resonant impulsive vibrational spectroscopy and non-resonant Raman scattering, we identify multiple hybrid organic-inorganic vibrational modes that strongly couple to the excitonic transitions and characterize their behavior. Calculations by density functional perturbation theory show that these strongly coupled modes exhibit large out-of-plane silver atomic motions and silver-selenium spacing displacements. Moreover, analysis of photoluminescence spectral splitting and temperature-dependent peak shifting/linewidth broadening reveals that light emission in AgSePh is most strongly affected by a compound 100 cm⁻¹ mode involving the wagging motion of phenylselenolate ligands and accompanying metal-chalcogen stretching. Finally, red shifting of vibrational modes with increasing temperature reveals a high degree of anharmonicity arising from non-covalent interactions between phenyl rings. These findings reveal the unique effects of hybrid vibrational modes in organic-inorganic semiconductors and motivate future work aimed at specifically engineering such interactions through chemical and structural modification.

我们揭示了二维（2D）层状杂化有机-无机半导体苯基硒酸银（AgSePh）中的相干激子-声子相互作用。使用飞秒共振脉冲振动光谱和非共振拉曼散射，我们识别了多种与激子跃迁强烈耦合的混合有机-无机振动模式并表征了它们的行为。密度泛函微扰理论的计算表明，这些强耦合模式表现出大的面外银原子运动和银硒间距位移。此外，对光致发光光谱分裂和温度依赖性峰移/线宽展宽的分析表明，AgSePh中的光发射受化合物100 cm ^-1模式的影响最强烈，涉及硒酸苯酯配体的摇摆运动和伴随的金属硫属元素拉伸。最后，随着温度升高振动模式的红移揭示了苯环之间的非共价相互作用引起的高度非和谐性。这些发现揭示了有机-无机半导体中混合振动模式的独特效应，并激发了未来旨在通过化学和结构修饰专门设计此类相互作用的工作。