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• W4286498085 abstract "Isolated polyhedra constituting the framework of Cs2SnI6 renders surplus degrees of dynamic freedom making it an abode of inherent anharmonicity. The ensuing properties of the integrated devices are, thus, inevitably governed by the underlying lattice vibrational dynamics. Here, with the aid of femtosecond transient absorption (TA) spectroscopy, we have made an attempt to capture a real-time picture of the vibrational modes prevalent in the Cs2SnI6 system and allocate the origin of the, thus far, unidentified modes. Further, we have also inspected the generation mechanism of the fully symmetric coherent phonon mode “A1g” which is manifested as strong oscillations in the time domain data for Cs2SnI6 and also the other low symmetry modes observable in the frequency domain in the unified framework of displacive excitation and impulsive scattering. As another major accomplishment, we pinpointed the position of the theoretically predicted yet never experimentally observed silent modes which usually are left undetected in the conventional frequency domain spectroscopic techniques. Strong support has been lent from the phase analysis of the excitation pump and intensity-dependent TA measurements. Subsequent to accounting for all the modes, the anharmonicity of the phonon modes, a straightforward consequence of phonon–phonon coupling, has been addressed. Furthermore, we executed temperature-dependent investigations which together with the pump-dependent studies provide insights into the extent of carrier-phonon coupling. All this critical information regarding the phonon modes can lend assistance in improving the performance of the devices based on Cs2SnI6." @default.
• W4286498085 created "2022-07-22" @default.
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• W4286498085 date "2022-07-21" @default.
• W4286498085 modified "2023-10-16" @default.
• W4286498085 title "Mapping the Real-Time Vibrational Infrastructure of Cs₂SnI₆ Nanocrystals through Coherent Phonon Dynamics" @default.
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• W4286498085 doi "https://doi.org/10.1021/acsphotonics.2c00512" @default.
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