Geometry optimizations of all cluster models were carried out in solution with Integral Equation Formalism Polarizable Continuum Model (IEFPCM) as implemented in Gaussian09. The B3LYP functional in conjunction with the 6-31+g(d) basis set was employed to optimize the geometries. Frequency calculations at the same level of theory were carried out to verify the nature of the stationary points enc...

Highly efficient and specific energy transfer mechanisms that involve rotation-rotation, vibration-vibration, and vibration-rotation exchange in diatomic molecules are examined theoretically in ultracold H(2), D(2), and HD self-collisions as a function of initial vibrational level v. The three quasiresonant mechanisms are found to operate for all vibrational levels and yield complex scattering ...

As the simplest molecule in nature, the hydrogen molecular ion provides a unique system for studying molecules in intense laser fields. In this thesis, the Coulomb explosion and photodissociation channel of H 2 and D + 2 have been investigated with 790-nm, sub-100fs laser pulses by employing a high-resolution photofragment imaging technique. Unlike most experiments, where neutral molecules were...

Two-dimensional electron energy-loss spectra of acrylonitrile are presented in the incident energy range 0.095-0.9 eV, where the incoming electron is temporarily captured in the lowest π* orbital. The cross section is plotted as a function of the incident electron energy that determines which vibrational resonant anion state is populated, and of the electron energy loss, that shows into which f...

Ab initio all-electron molecular-orbital calculations are carried out to study the structures and relative stability of low-energy silicon clusters (Si(n),n = 12-20). Selected geometric isomers include those predicted by Ho et al. [Nature (London) 392, 582 (1998)] based on an unbiased search with tight-binding/genetic algorithm, as well as those found by Rata et al. [Phys. Rev. Lett. 85, 546 (2...

The mechanism of vibrational energy flow is studied in a regime where a diffusion equation is likely to break down, i.e., on length scales of a few chemical bonds and time scales of a few picoseconds. This situation occurs, for example, during photochemical reactions in protein environment. To that end, a toy model is introduced that on the one hand mimics the vibrational normal mode distributi...

We study the quantum transport and the nonequilibrium vibrational states of a quantum dot embedded between a normal-conducting and a superconducting lead with the charge on the quantum dot linearly coupled to a harmonic oscillator of frequency ω. To the leading order in the charge-vibration interaction, we calculate the current and the nonequilibrium phonon occupation by the Keldsyh Green’s fun...

Proteins have been shown to exhibit strange/anomalous dynamics displaying non-Debye density of vibrational states, anomalous spread of vibrational energy, large conformational changes, nonexponential decay of correlations, and nonexponential unfolding times. The anomalous behavior may, in principle, stem from various factors affecting the energy landscape under which a protein vibrates. Investi...