We present a novel scheme for quantum manipulation in ultrafast diatomic molecules. A pump mechanism is used to create a coherent superposition of the D + 2 vibrations. A short, intense, control pulse is applied, after a fractional coherence time, to create selective interferences. A 'chessboard' pattern of states can be realised in which the set of even/odd numbered vibrational states can be a...

Slow photoelectron velocity-map imaging (SEVI) spectroscopy has been used to study the vibronic structure of gas-phase α- and β-naphthyl radicals (C(10)H(7)). SEVI of cryogenically cooled anions yields spectra with <4 cm(-1) resolution, allowing for the observation and interpretation of congested vibrational structure. Isomer-specific photoelectron spectra of detachment to the radical ground el...

In sodium dimer the 2 (3)Pi(g), 3 (3)Pi(g), and 4 (3)Sigma(g) (+) electronic states are coupled; the coupling of the two (3)Pi(g) states is due to vibrational motion while the nonadiabatic interaction between the (3)Sigma(g) (+) and the (3)Pi(g) states-in particular, the 3 (3)Pi(g) state-is mediated by rotational interaction. The resulting vibronic problem is studied in some detail. The bound v...

Strong coupling of electronic and vibrational degrees of freedom entails a low-bias suppression of the current through single-molecule devices, termed the Franck-Condon blockade. In the limit of slow vibrational relaxation, transport in the Franck-Condon-blockade regime proceeds via avalanches of large numbers of electrons, which are interrupted by long waiting times without electron transfer. ...

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...

We present a proposal for protecting states against decoherence, based on the engineering of pointer states. We apply this procedure to the vibrational motion of a trapped ion, and show how to protect qubits, squeezed states, approximate phase eigenstates, and superpositions of coherent states.

We develop a first principles theoretical description of femtosecond double-pump single-molecule signals of molecular aggregates. We incorporate all singly excited electronic states and vibrational modes with significant exciton-phonon coupling into a system Hamiltonian and treat the ensuing system dynamics within the Davydov D1 Ansatz. The remaining intra- and inter-molecular vibrational modes...

Quasi-classical trajectories have been integrated to study the vibrational relaxation of the O + NO(v) process as a function of the initial vibrational quantum number for T = 298 K, 1500 K, and 3000 K. Two reliable potential energy surfaces have been employed for the A' and A'' doublet states of NO2. The calculated vibrational relaxation rate constants show a nearly v-independent behavior at ro...

We form a one-dimensional optical lattice for Cs atoms using light tuned a few thousand linewidths below atomic resonance. Atoms are selectively loaded into deeply bound states by adiabatic transfer from a superimposed, near-resonance optical lattice. This yields a mean vibrational excitation n̄'0.3 and localization Dz 'l/20. Light scattering subsequently heats the atoms, but the initial rate is...

We have performed an approximate ab initio calculation of vibrational properties of hydrogenated amorphous silicon (a-Si:H) using a molecular dynamics method. A 216-atom model for pure amorphous silicon (a-Si) has been employed as a starting point for our a-Si:H models with voids that were made by removing a cluster of silicon atoms out of the bulk and terminating the resulting dangling bonds w...