Theory of time-resolved sum-frequency generation and its applications to vibrational dynamics of water.
نویسندگان
چکیده
A molecular theory of time-resolved sum-frequency generation (SFG) has been developed. The theoretical framework is constructed using the coupled-oscillator model in the adiabatic approximation. This theory can treat not only the vibrational spectroscopy but also vibrational dynamics. An application of this theory is also provided for estimation of the time constants of the intermolecular vibrational energy transfer between water molecules. This approach can be used for molecular analysis of the experimental results of Shen at al. on the SFG studies of vibrational dynamics of water.
منابع مشابه
Femtosecond time-resolved broadband electronic sum frequency generation for the investigation of electron and exciton dynamics
Time-resolved sum-frequency generation is an established tool to investigate ultrafast vibrational dynamics with surface and interface specificity. We present an extension of the technique to the regime of electronic transitions based on a compressed white light continuum. It is used to probe the non-equilibrium dynamics of excitonic resonances in the non-centrosymmetric oxide ZnO, where we dem...
متن کاملOrientational motions of vibrational chromophores in molecules at the air/water interface with time-resolved sum frequency generation.
The first time-resolved experiments in which interfacial molecules are pumped to excited electronic states and probed by vibrational sum frequency generation (SFG) are reported. This method was used to measure the out-of-plane rotation dynamics, i.e. time dependent changes in the polar angle, of a vibrational chromophore of an interfacial molecule. The chromophore is the carbonyl group, the rot...
متن کاملElucidating low-frequency vibrational dynamics in calcite and water with time-resolved third-harmonic generation spectroscopy.
Low-frequency vibrations are foundational for material properties including thermal conductivity and chemical reactivity. To resolve the intrinsic molecular conformational dynamics in condensed phase, we implement time-resolved third-harmonic generation (TRTHG) spectroscopy to unravel collective skeletal motions in calcite, water, and aqueous salt solution in situ. The lifetime of three Raman-a...
متن کاملDynamics of excited state electron transfer at a liquid interface using time-resolved sum frequency generation
Femtosecond time resolved vibrational sum frequency generation has been used for the first time to probe a chemical reaction involving interfacial molecules pumped into their excited electronic states. The ultrafast dynamics of electron transfer from ground state N,N-dimethylaniline (DMA) to photoexcited coumarin 314 at a water/DMAmonolayer interface was obtained. The forward electron transfer ...
متن کاملCapturing the Ultrafast Vibrational Decoherence of Hydrogen Bonding in Interfacial Water.
Vibrational sum-frequency generation (vSFG) measurements in the frequency and time domains reveal that the interfacial hydrogen bonded OH stretch at the water/calcium fluoride interface is composed of two populations oriented oppositely. The time-resolved vSFG free-induction decay suggested that, whereas the strongly hydrogen bonded OH vibrational stretches, centered near 3140 ± 11 cm-1, are or...
متن کاملذخیره در منابع من
با ذخیره ی این منبع در منابع من، دسترسی به آن را برای استفاده های بعدی آسان تر کنید
عنوان ژورنال:
- The journal of physical chemistry. A
دوره 111 37 شماره
صفحات -
تاریخ انتشار 2007