We have applied nuclear inelastic scattering (NIS) and computational predictions based on density functional theory (DFT) to explore the vibrational dynamics of Fe in a trinuclear oxo-bridged iron(III) complex. Quantitative comparison of the experimentally measured vibrational dynamics of the Mössbauer nuclei Fe, with normal mode analysis, calculated via quantum chemical calculation based on DF...

We report a new ab initio study of the acetylene T3 potential energy surface, which clarifies the nature of its energy minimum, and present computed equilibrium geometries and diabatic frequencies. This information enables the computation of harmonic vibrational overlap integrals of T3 vibrational levels with the S1 3nu3 state. The results of this calculation support the interpretation of two l...

The ultrafast vibrational dynamics of HDO:D(2)O ice at 180 K in anionic reverse micelles is studied by midinfrared femtosecond pump-probe spectroscopy. Solutions containing reverse micelles are cooled to low temperatures by a fast-freezing procedure. The heating dynamics of the micellar solutions is studied to characterize the micellar structure. Small reverse micelles with a water content up t...

Vibrational energy relaxation of the NH-, OH-, and OD-stretching modes in hydrogen-bonded liquids has been investigated by means of infrared pump-probe spectroscopy. The relaxation rates have been determined both in neat liquids and in isotopic mixtures with systematically varied isotope fractions. In all liquids, the vibrational relaxation rate increases as the isotope fraction is increased an...

Ultrafast vibrational dynamics of small molecules on platinum (Pt) layers in water are investigated using 2D attenuated total reflectance IR spectroscopy. Isotope combinations of carbon monoxide and cyanide are used to elucidate inter-adsorbate and substrate-adsorbate interactions. Despite observed cross-peaks in the CO spectra, we conclude that the molecules are not vibrationally coupled. Rath...

Sum frequency vibrational spectra for hexadecanethiol (HDT) adsorbed on thin gold film deposited on the surface of a CaF2 prism have been measured using total-internal reflection broad-bandwidth sum frequency generation (TIR-BBSFG) spectroscopy. The bands attributed to the CH3 symmetric and asymmetric stretching vibrational modes were observed in the sum frequency vibrational spectra. The orien...

The coupling between the OD stretch v=2 level and benzene-ring modes in 2-methoxyphenol-OD (hydroxyl H replaced by D) is observed with ultrafast two-dimensional (2D) IR vibrational echo spectroscopy. Because of this coupling, the 1-2 transition peak in the 2D spectrum is split into a doublet with peaks of approximately equal amplitudes. Several molecules and solvents were used to study this phe...

Ultrafast UV-vibrational spectroscopy was used to investigate how vibrational excitation of the bridge changes photoinduced electron transfer between donor (dimethylaniline) and acceptor (anthracene) moieties bridged by a guanosine-cytidine base pair (GC). The charge-separated (CS) state yield is found to be lowered by high-frequency bridge mode excitation. The effect is linked to a dynamic mod...

This article summarizes the methodological progress that has been made in the vibrational spectroscopy of isolated polynuclear metal oxide clusters, with particular emphasis on free electron laser-based infrared action spectroscopy of gas phase clusters, over the last decade. The possibilities, limitations and prospects of the various experimental approaches are discussed using representative e...

We perform photoassociation spectroscopy in an ultracold 23Na-6Li mixture to study the c3Σ+ excited triplet molecular potential. We observe 50 vibrational states and their substructure to an accuracy of 20 MHz, and provide line strength data from photoassociation loss measurements. An analysis of the vibrational line positions using near-dissociation expansions and a full potential fit is prese...