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Phonon coherences reveal the polaronic character of excitons in two-dimensional lead halide perovskites
摘要： Hybrid organic–inorganic semiconductors feature complex lattice dynamics due to the ionic character of the crystal and the softness arising from non-covalent bonds between molecular moieties and the inorganic network. Here we establish that such dynamic structural complexity in a prototypical two-dimensional lead iodide perovskite gives rise to the coexistence of diverse excitonic resonances, each with a distinct degree of polaronic character. By means of high-resolution resonant impulsive stimulated Raman spectroscopy, we identify vibrational wavepacket dynamics that evolve along different configurational coordinates for distinct excitons and photocarriers. Employing density functional theory calculations, we assign the observed coherent vibrational modes to various low-frequency (?50 cm?1) optical phonons involving motion in the lead iodide layers. We thus conclude that different excitons induce specific lattice reorganizations, which are signatures of polaronic binding. This insight into the energetic/configurational landscape involving globally neutral primary photoexcitations may be relevant to a broader class of emerging hybrid semiconductor materials.
关键词： resonant impulsive stimulated Raman spectroscopy,polaronic character,two-dimensional perovskites,density functional theory,excitons,phonon coherences
更新于2025-09-23 15:23:52
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Time-Resolved Impulsive Stimulated Raman Spectroscopy with Synchronized Triple Mode-Locked Lasers
摘要： A complete understanding of a photochemical reaction dynamics begins with real-time measurements of both electronic and vibrational structures of photoexcited molecules. Time-resolved impulsive stimulated Raman spectroscopy (TR-ISRS) with femtosecond actinic pump, Raman pump, and Raman probe pulses is one of the incisive techniques enabling one to investigate the structural changes of photoexcited molecules. Here, we demonstrate that such femtosecond TR-ISRS is feasible with synchronized triple mode-locked lasers without using any time-delay devices. Taking advantage of precise control of the three repetition rates independently, we could achieve automatic scanning of two delay times between the three pulses, which makes both rapid data acquisition and wide dynamic range measurement of the fifth-order TR-ISRS signal achievable. We thus anticipate that the present triple mode-locked laser-based TR-ISRS technique will be of critical use for long-term monitoring of photochemical reaction dynamics in condensed phases and biological systems.
关键词： pump-dump-probe,fifth-order electronic spectroscopy,impulsive stimulated Raman spectroscopy,femtosecond Raman scattering,Time-resolved vibrational spectroscopy
更新于2025-09-23 15:21:01