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...

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...

Deprotonated thymine can exist in two different forms, depending on which of its two N sites is deprotonated: N1[T–H] or N3[T–H] . Here we report a photodetachment study of the N1[T–H] isomer cooled in a cryogenic ion trap and the observation of an excited dipole-bound state. Eighteen vibrational levels of the dipole-bound state are observed, and its vibrational ground state is found to be 238 ...

Enantioenriched square-pyramidal oxo- and sulfidorhenium(v) complexes have been prepared and their stereochemistry studied by vibrational circular dichroism (VCD) spectroscopy.

We developed an efficient approach to study the coherent control of vibrational state-to-state transitions. The approximations employed in our model are valid in the regime of the low vibrational excitation specific to the vibrational quantum computer. Using this approach we explored how the vibrational properties of a two-qubit system affect the accuracy of subpicosecond quantum gates. The opt...

We use a 6.8-fs laser as the light source for broad-band femtosecond pump-probe real-time vibrational spectroscopy to investigate both electronic relaxation and vibrational dynamics of the Q(y)-band of Chl-a at 293 K. More than 25 vibrational modes coupled to the Q(y) transition are observed. Eleven of them have been clarified predominantly due to the excited state, and six of them are conclude...

The photoelectron spectra of FeO and FeO2 2 are obtained at 3.49 eV photon energy. Transitions to the ground state ~D! and three low-lying excited states ~S, S, and D! of FeO are observed. The two low-spin excited states found at 6770 and 8310 cm above the ground state, respectively, have not been observed before. The two S states, characteristic of detachment of a nonbonding electron from the ...

We demonstrate vibrational cooling of anions via collisions with a background gas in an ion trap attached to a cryogenically controlled cold head (10-400 K). Photoelectron spectra of vibrationally cold C60(-) anions, produced by electrospray ionization and cooled in the cold ion trap, have been obtained. Relative to spectra taken at room temperature, vibrational hot bands are completely elimina...

Impulsive excitation of molecular vibration is known to induce wave packets in both the ground state and excited state. Here, the ultrafast dynamics of PYP was studied by pump-probe spectroscopy using a sub-8 fs pulse laser at 400 nm. The broadband spectrum of the UV pulse allowed us to detect the pump-probe signal covering 360-440 nm. The dependence of the vibrational phase of the vibrational ...

The possibility of electron attachment to the valence 3 state of CO is examined using an ab initio bound-state multireference con guration interaction approach. The resulting resonance has 4 symmetry; the higher vibrational levels of this resonance state coincide with, or are nearly coincident with, levels of the parent a state. Collisional relaxation to the lowest vibrational levels in hot pla...