The post-discharge kinetics is a very complex problem. Various radiative and non-radiative processes lead during the post-discharge period to the establishing of thermodynamic equilibrium. Generally, all these processes are vibrationally specific. A special interest deals with the processes of metastables. In presented numeric model of nitrogen plasma, the vibrational distribution function (VDF...

Multidimensional nonlinear spectroscopy, in the electronic and vibrational regimes, has reached maturity. To date, no experimental technique has combined the advantages of 2D electronic spectroscopy and 2D infrared spectroscopy, monitoring the evolution of the electronic and nuclear degrees of freedom simultaneously. The interplay and coupling between the electronic state and vibrational manifo...

Vibrational excitation of HCl molecules (m = 0 ! 1) has been observed when HCl molecular beams at energies of 0.59–1.37 eV are scattered from a Au(111) surface at low surface temperature (Ts = 273 K). The incident and scattered HCl is probed state-selectively using 2 + 1 REMPI. The vibrational excitation probability depends strongly on incidence kinetic energy, Ei, exhibiting a threshold near E...

We report high resolution state-to-state time-of-flight (TOF) measurements for scattering of HCl(v=2, J=1) from a Au(111) single crystal surface for both vibrationally elastic (v=2-->2) as well as inelastic (v=2-->1) channels at seven incidence energies between 0.28 and 1.27 eV. The dependences of the TOF results on final HCl rotational state and surface temperature are also reported. The trans...

We evaluate the shifts imparted to vibrational and rotational levels of a linear molecule by a nonresonant laser field at intensities of up to 10(12) W/cm(2). Both types of shift are found to be either positive or negative, depending on the initial rotational state acted upon by the field. An adiabatic field-molecule interaction imparts a rotational energy shift which is negative and exceeds th...

Highly accurate quantum-mechanical calculations az presented for highly excited vibrational states of HzO. The vibration Hamiltonian operator Hvib for a nonlinear triatomic molecule is given in Radau coordinates. A direct product basis is chosen, and the Hvib matrix is evaluated in the discrete variable representation (DVR) for the symmetrized Radau coordinates. Vibrational eigenstates are comp...

The vibrational configuration interaction method used to obtain static vibrational (hyper)polarizabilities is extended to dynamic nonlinear optical properties in the infinite optical frequency approximation. Illustrative calculations are carried out on H(2)O and NH(3). The former molecule is weakly anharmonic while the latter contains a strongly anharmonic umbrella mode. The effect on vibration...

We study the vibrational energy relaxation (VER) and collisional dephasing as channels of coherence loss in a vibrational mode that is selectively excited using chirped pulse adiabatic passage in the Raman configuration. Based on the dressed state picture analysis we propose a method to reduce decoherence using femtosecond chirped pulse trains. When applied with a period close to the VER time, ...

A modified Landau-Teller equation for vibrational relaxation in the condensed phase is proposed. This equation differs from previous approaches by accounting for the fluctuations of the energies of the vibrational levels that result from the interactions with the surroundings (bath). In the conventional approach the effects of the bath are only included in the coupling between the relaxing and ...