The dissociative photodetachment ~DPD! of HCO2 2 and DCO2 2 was studied at 258 nm. State-resolved translational energy distributions were observed correlated to bending excitation in the CO2 product for the channel producing H/D1CO2, indicating very low rotational excitation in the products consistent with predissociation of a C2n HCO2 molecule. No evidence was found for dissociation into OH1CO...

We examine ultrafast dynamics in a coupled molecule-plasmon system. Using a new ultrafast Raman technique called surface enhanced-femtosecond stimulated Raman spectroscopy (SE-FSRS), we prove that plasmonic nanoparticles and adsorbed molecules are coupled by the appearance of Fano-like lineshapes, which arise from the interaction of narrowband vibrational coherences and the broadband plasmon re...

We have demonstrated the use of ab initio molecular dynamics (AIMD) trajectories to compute the vibrational energy levels of molecular systems in the context of the semiclassical initial value representation (SC-IVR). A relatively low level of electronic structure theory (HF/3-21G) was used in this proof-of-principle study. Formaldehyde was used as a test case for the determination of accurate ...

The accuracy of excited states calculated with Kohn-Sham density functional theory using the maximum overlap method has been assessed for the calculation of adiabatic excitation energies, excited state structures, and excited state harmonic and anharmonic vibrational frequencies for open-shell singlet excited states. The computed Kohn-Sham adiabatic excitation energies are improved significantl...

Amorphous diamond structures with more than 97% of sp3 bonding fraction are generated by quenching liquid carbon using tight-binding molecular-dynamics simulations. The electronic and vibrational properties the amorphous sample investigated.

Electronic and vibrational correlations report on the dynamics and structure of molecular species, yet revealing these correlations experimentally has proved extremely challenging. Here, we demonstrate a method that probes correlations between states within the vibrational and electronic manifold with quantum coherence selectivity. Specifically, we measure a fully coherent four-dimensional spec...