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Physical Review Letters

Localized Vibrations of Trapped Molecules

J. S. Downes, John William White, Peter A. Egelstaff, V. S. Rainey

Published Sep 5, 1966• 17 citations
Publisher
DOI
10.1103/physrevlett.17.533

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Physical Review A•Mar 1, 1999•57 citations
Trapping vibrational energy into one single bond is a key problem of bond-selective chemistry. We explored this possibility by means of restricting local mode wavepacket dephasing with multi-color laser field. The vibrational excitation and evolution of molecules in weak and strong multi-color laser fields are discussed by field-quantization method and semi-classical method. The results demonstrate that population can not be trapped in a local mode wave-packet using multi-color weak field, while it is possible to trap vibrational population between the ground state and local mode vibration by making use of power-broadening induced by strong laser field and the interference between two wave-packets excited by two strong laser of different frequencies.
Polar molecules in selected quantum states can be guided, decelerated and trapped using electric fields created by microstructured electrodes on a chip. Here we demonstrate that transitions between two vibrational quantum states can be induced while the molecules are trapped above the chip. We use CO molecules, prepared in the J = 1 rotational level of the a 3Π1, v = 0 state and induce the transition to either the J = 1 or the J = 2 level in the vibrationally excited a 3Π1, v = 1 state with pulsed, narrowband IR radiation. First, the vibrational excitation is studied using CO molecules in a freely propagating molecular beam, in a well-defined homogeneous electric field. Then, we demonstrate that the IR radiation can be coupled to CO molecules that are trapped less than 50 µm above the chip by guiding molecules in the v = 0 level to the center of the chip where they are pumped to the v = 1 level. The molecules remain trapped and are then guided off the chip and state-selectively detected.
Vibrational relaxation of trapped molecules due to collisions with cold atoms is investigated using the results of quantum-mechanical scattering calculations. Trap loss is analyzed using an exactly solvable kinetic model that includes direct collisional quenching and an indirect process of vibrational predissociation. At low atom density, the relaxation is due primarily to collisional quenching. At high atom density, the relaxation involves additional time scales due to the formation and decay of van der Waals complexes. It is shown that the most weakly bound state of the van der Waals complex for a given diatomic vibrational level controls the relaxation at all atom densities. Possible experiments using trapped molecules are discussed.