Efficient Formation of Ultracold Molecules with Chirped Nanosecond Pulses.

We describe experiments and associated quantum simulations involving the production of ultracold (87)Rb2 molecules with nanosecond pulses of frequency-chirped light. With appropriate chirp parameters, the formation is dominated by coherent processes. For a positive chirp, excited molecules are produced by photoassociation early in the chirp, and then transferred into high vibrational levels of the lowest triplet state by stimulated emission later in the chirp. Generally good agreement is seen between the data and the simulations. Shaping of the chirp can lead to a significant enhancement of the formation rate. Further improvements using higher intensities and different intermediate states are predicted.

Enhancement of Ultracold Molecule Formation Using Shaped Nanosecond Frequency Chirps.

We demonstrate that judicious shaping of a nanosecond-time-scale frequency chirp can dramatically enhance the formation rate of ultracold (87)Rb(2) molecules. Starting with ultracold (87)Rb atoms, we apply pulses of frequency-chirped light to first photoassociate the atoms into excited molecules and then, later in the chirp, deexcite these molecules into a high vibrational level of the lowest triplet state a (3)Σ(u)(+). The enhancing chirp shape passes through the absorption and stimulated emission transitions relatively slowly, thus increasing their adiabaticity, but jumps quickly between them to minimize the effects of spontaneous emission. Comparisons with quantum simulations for various chirp shapes support this enhancement mechanism.

Evanescent-wave mirror for ultracold diatomic polar molecules.

We describe the interaction of an ultracold diatomic polar molecule with an evanescent-wave mirror. Several features of this system are explored, such as the coupling between internal rovibrational states of the molecule and the laser field. Numerical simulations show quantum reflection and state selection under attainable physical conditions. Such molecular optics components will facilitate the manipulation and trapping of ultracold molecules, and might serve in future applications in several fields, e.g., as devices to filter and select a state for ultracold chemistry, to measure extremely low temperatures of molecules, or to manipulate states for quantum information processing.

A phase-space approach to the T1 right arrow-wavy S0 radiationless decay in benzene: the effect of deuteration.

The influence of full deuteration on the T1 right arrow-wavy S0 intersystem crossing in benzene is studied by a phase space approach. A full treatment of all the vibrational modes in the molecule leads to a ratio of the rate between the two isotopomers which is very close to the experimental value. Several aspects of the results are compared to previous estimates, and the effects of anharmonicity on the rates and accepting modes are examined. This first successful application of the method to a real physical system encourages the possibility of establishing a routine procedure for simple calculations of transition rates even for relatively large molecules.