We have measured the vibrational structures of the N 1s photoelectron mainline and satellites of the gaseous N2 molecule with the resolution better than 75 meV. The gerade and ungerade symmetries of the core-ionized (mainline) states are resolved energetically, and symmetry-dependent angular distributions for the satellite emission allow us to resolve the Sigma and Pi symmetries of the shake-up...

OF THE DISSERTATION Energy-resolved positron-molecule annihilation: Vibrational Feshbach resonances and bound states

A class of doubly excited electronic states of the hydrogen molecule is reported. The states are of S symmetry and are located ca. 200 000 cm 1 above the ground state and about 75 000 cm 1 above the ionization threshold. The electronic wave functions employed to described these states have been expanded in the basis of exponentially correlated Gaussian (ECG) functions with the nonlinear paramet...

first-principle calculations were carried out to investigate the adsorption of co over cun nanoclusters. the structural, spectroscopic and electronic properties like optimized geometries, homo (highest occupied molecular orbital) and lumo (lowest unoccupied molecular orbital) energy levels, binding energy, adsorption energy, vibrational frequency and density of states (doss) of the pure cun nan...

We propose using short-period superlattices as substrates to control the vibrational relaxation dynamics of adsorbate overlayers. The mass modulation of superlattices creates both band gaps and large spectral enhancements in the phonon density of states. These modifications can dramatically alter the coupling between vibrational modes of the adsorbate overlayer and the substrate lattice, thereb...

Unlike many other molecules having local modes, the highly excited C-H stretching states of CHD3 show well resolved experimental spectra and simple Fermi resonance behavior. In this paper the local mode features in this prototype molecule are examined using a curvilinear coordinate approach. Theory and experiment are used to identify the vibrational state coupling. Both kinetic and potential te...

Light-harvesting in photosynthesis is determined by the excitonic interactions in disordered antennae and the coupling of collective electronic excitations to fast nuclear motions, producing efficient energy transfer with a complicated interplay between exciton and vibrational coherences. In this chapter we apply 2DES to an excitonically coupled bacteriochlorophyll dimer, the B820 subunit of th...

A global, analytical potential energy surface for the ground electronic state of HOBr has been determined using highly correlated multireference configuration interaction wave functions and explicit basis set extrapolations of large correlation consistent basis sets. The ab initio data have been fit to an analytical functional form that accurately includes both the HOBr and HBrO minima, as well...

Readout of the final states of qubits is a crucial step towards implementing quantum computation in experiment. Although not scalable to large numbers of qubits per molecule, computational studies show that molecular vibrations could provide a significant (factor 2-5 in the literature) increase in the number of qubits compared to two-level systems. In this theoretical work, we explore the proce...

Double resonance excitation of vibrationally autoionizing states of the water molecule has been performed for the first time. Tunable, coherent vacuum ultraviolet light was used to excite selected rotational levels of the C̃ B1 state with one quantum of symmetric stretch vibrational energy ~100!, from which ~100! Rydberg states were excited with a second dye laser. The Rydberg character of the C̃...