Tracking intramolecular energy redistribution dynamics in aryl halides: the effect of halide mass

Abstract

Selective excitation of C–H, C–C, CX1 and CX2 modes in an orderly manner, detection of intramolecular energy redistribution in aryl halides are performed by time- and frequency-resolved Coherent Anti-Stokes Raman Scattering (CARS) spectroscopy.

Molecular Dynamics and Energy Transfer in Pure Aniline and Rh101+/Aniline Mixed Solution Measured by Ultrafast Spectroscopy

“…Another reason for choosing aniline in our study is that many articles have report electron transfer of Rh101 + /aniline in the electronic excited state, but little attention has been paid to study the dynamics processes in the electronic ground state. [13][14][15][16] In our manuscript, vibrational dynamics happen in in the electronic ground state, and we have described vibrational energy transfer before chemical reaction. In our work, we study the effect of hydrogen bonds on vibrational dynamics and energy transfer processes before degradation.…”

“…[8,17,18] Before a chemical bond breaks, a molecule undergoes a series of changes, i. e., deformation of the molecular structure in the first step, activation of vibrational modes in the second step, and energy redistribution in the third step, and finally, the chemical bond is broken. [19,20] Femtosecond time-and frequency-resolved CARS spectroscopy is an ultrafast technique developed to investigate fast molecular processes. It can simultaneously excite most vibrational modes and detect dynamic processes, e. g., molecular structure deformation, dephasing time, and energy transfer pathway.…”

“…Aniline has simple structure and it consists of amino group and a benzene ring, the influence of substituent (amino group) on vibrational energy transfer or vibrational dynamics can be seen clearly. Another reason for choosing aniline in our study is that many articles have report electron transfer of Rh101 + /aniline in the electronic excited state, but little attention has been paid to study the dynamics processes in the electronic ground state [13–16] . In our manuscript, vibrational dynamics happen in in the electronic ground state, and we have described vibrational energy transfer before chemical reaction.…”

Tracking vibrational energy transfer and molecular dynamics in nitromethane and nitromethane/methanol mixed solutions by ultrafast spectroscopy

“…Detail information on selective excitation CARS was discussed before. 19 In another experiment, the pump pulse laser was fixed at 800 nm, and the Stokes pulse was irradiated onto a sapphire crystal to generate white light with the spectral region from 650 to 920 nm. In the collective excitation CARS experiment, a long-wavelength pass filter cut off the wavelength below 808 nm, so the vibrational modes from 0 to 1500 cm À1 could be collectively excited.…”

Role of electron in intramolecular vibrational energy redistribution: a simulation of time- and frequency-resolved CARS spectrum

“…Recently, TFR-CARS experiments have been performed in our laboratory to track the coherent intramolecular vibrational energy transfer in liquid benzene 9 and a series of structurally relevant monosubstituted benzenes. 10 Take the experimental results of liquid benzene for instance, when the C–H stretching vibrational modes of benzene at about 3000 cm −1 (parent modes) were selectively excited, vibrational modes around 1000 cm −1 (daughter modes) far away from the direct excitation region were observed. The experimental results manifest the existence of IVR and the practicability of tracking IVR by CARS.…”