Using femtosecond pump-probe ion imaging spectroscopy, we establish the key role of I(+) + I(-) ion-pair (IP) states in the predissociation dynamics of molecular iodine I2 excited to Rydberg states. Two-photon excitation of Rydberg states lying above the lowest IP state dissociation threshold (1st tier) is found to be followed by direct parallel transitions into IP states of the 1st tier asympt...

A state-selected beam of hydroxyl radicals is generated using a pulsed discharge source and hexapole field. The OH radicals are characterized by resonance-enhanced multiphoton ionization (REMPI) spectroscopy via the nested D 2Sigma- and 3 2Sigma- Rydberg states. Simplified spectra are observed from the selected |MJ|=3/2 component of the upper Lambda-doublet level of the lowest rotational state ...

Hydrogen molecules in selected core-nonpenetrating Rydberg-Stark states have been decelerated from a mean initial velocity of 500 m/s to zero velocity in the laboratory frame and loaded into a three-dimensional electrostatic trap. Trapping times, measured by pulsed electric field ionization of the trapped molecules, are found to be limited by collisional processes. As Rydberg states can be deex...

Excited state unimolecular reactions of some polyenes exhibit localization of their dynamics at a single ethylenic double bond. Here we present studies of the fundamental photophysical processes in the ethylene unit itself. Combined femtosecond time-resolved photoelectron spectroscopy (TRPES) and ab initio quantum chemical calculations was applied to the study of excited state dynamics in cis-b...

We have demonstrated a rovibrational-state-selected photoionization experiment using an IR laser and high-resolution VUV-synchrotron radiation. The VUV photoionization of acetylene [C2H2(Xtilde; (1)Sigma(+)(g);nu(3)=1,J(')=8 or 10)] prepared by IR excitation reveals three strong autoionizing Rydberg series converging to C2H+2(Xtilde; (2)Pi(u);nu(+)(3)=1) with little ion background interference....

Ultrashort, nearly unipolar electric field pulses are used to produce novel dynamic states in Rydberg atoms. A single 500 fsec field pulse redistributes essentially all of the population from a single stationary Rydberg state to hundreds of different final states. The dynamic evolution of the nonstationary wave packet is monitored using a second, time-delayed pulse. The time-dependent momentum-...

An intuitive scheme for controlling the rotational quantum state of a Rydberg molecule is demonstrated experimentally. We determine the accumulated phase difference between the various components of a molecular electron wave packet, and then employ a sequence of phase-locked optical pulses to selectively enhance or depopulate specific rotational states. The angular momentum composition of the r...

We propose a Ramsey interferometry experiment using an entangled state of N atoms to reach the Heisenberg limit for the estimation of an atomic phase shift if the atom number parity is perfectly determined. In a more realistic situation, due to statistical fluctuations of the atom source and the finite detection efficiency, the parity is unknown. We then achieve about half the Heisenberg limit....

By coupling a probe transition to a Rydberg state using electromagnetically induced transparency (EIT) we map the strong dipole-dipole interactions onto an optical field. We characterize the resulting cooperative optical nonlinearity as a function of probe strength and density. We demonstrate good quantitative agreement between the experiment and an N-atom cooperative model for N=3 atoms per bl...