Deeply bound cold caesium molecules formed after 0(-)(g) resonant coupling.

Translationally cold caesium molecules are created by photoassociation below the 6s + 6p(1/2) excited state and selectively detected by resonance enhanced two photon ionization (RE2PI). A series of excited vibrational levels belonging to the 0(-)(g) symmetry is identified. The regular progression of the vibrational spacings and of the rotational constants of the 0(-)(g) (6s + 6p(1/2)) levels is strongly altered in two energy domains. These deviations are interpreted in terms of resonant coupling with deeply bound energy levels of two upper 0(-)(g) states dissociating into the 6s + 6p(3/2) and 6s + 5d(3/2) asymptotes. A theoretical model is proposed to explain the coupling and a quantum defect analysis of the perturbed level position is performed. Moreover, the resonant coupling changes dramatically the spontaneous decay products of the photoexcited molecules, strongly enhancing the decay into deeply bound levels of the a(3)Σ(+)(u) triplet state and of the X(1)Σ(+)(g) ground state. These results may be relevant when conceiving population transferring schemes in cold molecule systems.

An optical-optical double resonance experiment in LiH molecules: lifetime measurements in the C state.

An optical-optical double resonance sub-Doppler experiment is used to measure short nonradiative lifetimes in the C (1)Sigma(+) state of LiH. These lifetimes are expected to result from the strong electronic interaction between the C (1)Sigma(+) state and the continuum of the A (1)Sigma(+) state and to vary with the vibrational quantum number, from nanoseconds to milliseconds. The experimental setup combines a molecular beam of LiH, a first cw laser beam locked to a given A-X absorption line, and a second cw laser beam scanned over C-A absorption profiles. Analysis of these absorption profiles in terms of Voigt profiles shows that their Lorentzian components significantly vary with the vibrational quantum numbers of the C state. Nonradiative decay rates deduced this way are systematically larger than the calculated ones but their variations are similar. Coherent saturation effects cannot be invoked to explain this discrepancy.