arXiv subjects

O. Dulieu

Publications and source records attributed to O. Dulieu.

33 records · Page 2Linked to original sources

arXiv2011

Formation of ultracold metastable Rb2 molecules in their v"=0 level by blue-detuned photoassociation

We report on the observation of blue-detuned photoassociation in Rb2, in which vibrational levels are energetically above the corresponding excited atomic asymptote. 85Rb atoms in a MOT were photoassociated at short internuclear distances to levels of the (1)3Pi g state at a rate of approximately 5x10^4 molecules/s. We have observed most of the predicted vibrational levels for all four spin-orbit components 0g+, 0g-, 1g, and 2g, including levels of the 0g+ outer well. These molecules decay to the metastable a3Sigma u+ state, some preferentially to the v"=0 level, as we have observed for photoassociation to the v'=8 level of the 1g component.

physics.atom-ph↗

arXiv2011

Global analysis of data on the spin-orbit coupled $A^{1}Σ_{u}^{+}$ and $b^{3}Π_{u}$ states of Cs2

We present experimentally derived potential curves and spin-orbit interaction functions for the strongly perturbed $A^{1}Σ_{u}^{+}$ and $b^{3}Π_{u}$ states of the cesium dimer. The results are based on data from several sources. Laser-induced fluorescence Fourier transform spectroscopy (LIF FTS) was used some time ago in the Laboratoire Aimé Cotton primarily to study the $X ^{1}Σ_{g}^{+}$ state. More recent work at Tsinghua University provides information from moderate resolution spectroscopy on the lowest levels of the $b^{3}Π_{0u}^{\pm}$ states as well as additional high resolution data. From Innsbruck University, we have precision data obtained with cold Cs$_{2}$ molecules. Recent data from Temple University was obtained using the optical-optical double resonance polarization spectroscopy technique, and finally, a group at the University of Latvia has added additional LIF FTS data. In the Hamiltonian matrix, we have used analytic potentials (the Expanded Morse Oscillator form) with both finite-difference (FD) coupled-channels and discrete variable representation (DVR) calculations of the term values. Fitted diagonal and off-diagonal spin-orbit functions are obtained and compared with {\it ab initio} results from Temple and Moscow State universities.

physics.atom-ph↗

arXiv2011

Photoassociation of a cold atom-molecule pair II: second order perturbation approach

The electrostatic interaction between an excited atom and a diatomic ground state molecule in an arbitrary rovibrational level at large mutual separations is investigated with a general second-order perturbation theory, in the perspective of modeling the photoassociation between cold atoms and molecules. We find that the combination of quadrupole-quadrupole and van der Waals interactions compete with the rotational energy of the dimer, limiting the range of validity of the perturbative approach to distances larger than 100 a.u.. Numerical results are given for the long-range interaction between Cs and Cs$_2$, showing that the photoassociation is probably efficient whatever the Cs$_2$ rotational energy.

quant-ph↗

arXiv2010

Photoassociation of a cold atom-molecule pair: long-range quadrupole-quadrupole interactions

The general formalism of the multipolar expansion of electrostatic interactions is applied to the calculation the potential energy between an excited atom (without fine structure) and a ground state diatomic molecule at large separations. Both partners exhibit a permanent quadrupole moment, so that their mutual quadrupole-quadrupole long-range interaction is attractive enough to bind trimers. Numerical results are given for an excited Cs(6P) atom and a ground state Cs2 molecule. The prospects for achieving photoassociation of a cold atom/dimer pair is thus discussed and found promising. The formalism can be easily generalized to the long-range interaction between molecules to investigate the formation of cold tetramers.

quant-ph↗

arXiv2010

Influence of a Feshbach resonance on the photoassociation of LiCs

We analyse the formation of ultracold 7Li133Cs molecules in the rovibrational ground state through photoassociation into the B1Pi state, which has recently been reported [J. Deiglmayr et al., Phys. Rev. Lett. 101, 133004 (2008)]. Absolute rate constants for photoassociation at large detunings from the atomic asymptote are determined and are found to be surprisingly large. The photoassociation process is modeled using a full coupled-channel calculation for the continuum state, taking all relevant hyperfine states into account. The enhancement of the photoassociation rate is found to be caused by an `echo' of the triplet component in the singlet component of the scattering wave function at the inner turning point of the lowest triplet a3Sigma+ potential. This perturbation can be ascribed to the existence of a broad Feshbach resonance at low scattering energies. Our results elucidate the important role of couplings in the scattering wave function for the formation of deeply bound ground state molecules via photoassociation.

physics.atom-ph↗

arXiv2010

The permanent dipole moment of LiCs in the ground state

Recently we demonstrated the formation of ultracold polar LiCs molecules in deeply bound levels of the X1S+ ground state, including the rovibrational ground state [J. Deiglmayr et al., Phys. Rev. Lett. 101, 133004 (2008)]. Here we report on the first experimental determination of the permanent electric dipole moment of deeply bound LiCs molecules. For X1S+,v"=2 and v"=3 we measure values of mu=5.5(2) Debye and 5.3(2) Debye respectively.

physics.atom-ph↗

arXiv2010

Potential energy and dipole moment surfaces of H3- molecule

A new potential energy surface for the electronic ground state of the simplest triatomic anion H3- is determined for a large number of geometries. Its accuracy is improved at short and large distances compared to previous studies. The permanent dipole moment surface of the state is also computed for the first time. Nine vibrational levels of H3- and fourteen levels of D3- are obtained, bound by at most ~70 cm^{-1} and ~ 126 cm^{-1} respectively. These results should guide the spectroscopic search of the H3- ion in cold gases (below 100K) of molecular hydrogen in the presence of H3- ions.

physics.atom-ph↗

arXiv2009

Formation of the simplest stable negative molecular ion H3- in interstellar medium

We present the theory of radiative association of atoms and molecules, and we apply it to the (H$_2$-H$^-$) van der Waals complex. We discuss the possibility for the H$_3^-$ ion to be formed in the interstellar medium in an environment with abundant ionized molecular hydrogen H$_2^+$. The observation of H$_3^-$ would also be a probe for the presence of H$^-$ in the interstellar medium. By computing the electronic structure of the H$_3^-$ ion, we determine its dipole moment, bound states, rotational constants, predissociated vibrational resonances and their lifetimes, and suggest a way to detect the ion in the interstellar medium.

physics.atom-ph↗

arXiv2009

High-resolution spectroscopy of triplet states of Rb2 by femtosecond pump-probe photoionization of doped helium nanodroplets

The dynamics of vibrational wave packets in triplet states of rubidium dimers (Rb2) formed on helium nanodroplets are studied using femtosecond pump-probe photoionization spectroscopy. Due to fast desorption of the excited Rb2 molecules off the droplets and due to their low internal temperature, wave packet oscillations can be followed up to very long pump-probe delay times >1.5ns. In the first excited triplet state (1)^3Σ_g^+, full and fractional revivals are observed with high contrast. Fourier analysis provides high-resolution vibrational spectra which are in excellent agreement with ab initio calculations.

physics.atm-clus↗

arXiv2008

Formation of ultracold dipolar molecules in the lowest vibrational levels by photoassociation

We recently reported the formation of ultracold LiCs molecules in the rovibrational ground state X1Sigma+,v''=0,J''=0 [J. Deiglmayr et al., PRL 101, 133004 (2008)]. Here we discuss details of the experimental setup and present a thorough analysis of the photoassociation step including the photoassociation line shape. We predict the distribution of produced ground state molecules using accurate potential nergy curves combined with an ab-initio dipole transition moment and compare this prediction with experimental ionization spectra. Additionally we improve the value of the dissociation energy for the X1Sigma+ state by high resolution spectroscopy of the vibrational ground state.

physics.atom-ph↗

arXiv2008

Formation of ultracold polar molecules in the rovibrational ground state

Ultracold LiCs molecules in the absolute ground state X$^1Σ^+$, v"=0, J"=0 are formed via a single photo-association step starting from laser-cooled atoms. The selective production of v"=0, J"=2 molecules with a 50-fold higher rate is also demonstrated. The rotational and vibrational state of the ground state molecules is determined in a setup combining depletion spectroscopy with resonant-enhanced multi-photon ionization time-of-flight spectroscopy. Using the determined production rate of up to 5x10^3 molecules/s, we describe a simple scheme which can provide large samples of externally and internally cold dipolar molecules.

quant-ph↗

arXiv2005

Study of coupled states for the (4s^{2})^{1}S + (4s4p)^{3}P asymptote of Ca_{2}

The coupled states A^{1}Σ_{u}^{+} (^{1}D +}1}S), c^{3}Π_{u} (^{3}P + ^{1}S) and a^{3}Σ_{u}^{+} (^{3}P +}1}S) of the calcium dimer are investigated in a laser induced fluorescence experiment combined with high-resolution Fourier-transform spectroscopy. A global deperturbation analysis of the observed levels, considering a model, which is complete within the subspace of relevant neighboring states, is performed using the Fourier Grid Hamiltonian method. We determine the potential energy curve of the A^{1}Σ_{u}^{+} and c^{3}Π_{u} states and the strengths of the couplings between them. The c^{3}Π_{u} and \as states are of particular importance for the description of collisional processes between calcium atoms in the ground state ^{1}S_{0} and excited state ^{3}P_{1} applied in studies for establishing an optical frequency standard with Ca.

physics.atm-clus↗

arXiv2004

Photoassociation inside an optical dipole trap: absolute rate coefficients and Franck-Condon factors

We present quantitative measurements of the photoassociation of cesium molecules inside a far-detuned optical dipole trap. A model of the trap depletion dynamics is derived which allows to extract absolute photoassociation rate coefficients for the initial single-photon photoassociation step from measured trap-loss spectra. The sensitivity of this approach is demonstrated by measuring the Franck-Condon modulation of the weak photoassociation transitions into the low vibrational levels of the outer well of the 0g- state that correlates to the 6s+6p3/2 asymptote. The measurements are compared to theoretical predictions. In a magneto-optical trap these transitions have previously only been observed indirectly through ionization of ground state molecules.

physics.atom-ph↗

arXiv2004

Saturation of Cs2 Photoassociation in an Optical Dipole Trap

We present studies of strong coupling in single-photon photoassociation of cesium dimers using an optical dipole trap. A thermodynamic model of the trap depletion dynamics is employed to extract absolute rate coefficents. From the dependence of the rate coefficient on the photoassociation laser intensity, we observe saturation of the photoassociation scattering probability at the unitarity limit in quantitative agreement with the theoretical model by Bohn and Julienne [Phys. Rev. A, 60, 414 (1999)]. Also the corresponding power broadening of the resonance width is measured. We could not observe an intensity dependent light shift in contrast to findings for lithium and rubidium, which is attributed to the absence of a p or d-wave shape resonance in cesium.

physics.atom-ph↗

arXiv2003

Optical Manipulation of Long-range Interactions at the 3s+3p Asymptote of Na$_2$

We investigate the influence of a laser field, which is near-resonant to the atomic sodium 3$^2$P$_{1/2}$ $\to$ 3$^2$D$_{3/2}$ transition, on the last bound levels of the A$^1Σ^+_u$ state in Na$_2$. In a molecular beam experiment level shifts up to $\approx$ 100 MHz and light induced line broadenings were observed using an optical double resonance excitation scheme. Moreover, the coupling laser can reduce the number of bound levels of the A state by one or more units, which effectively means that in the picture of a collision of a 3$^2$S$_{1/2}$ and a 3$^2$P$_{1/2}$-atom the scattering phase is altered by more than $π$. The observed effects are interpreted as light induced couplings of the A$^1Σ^+_u$ state, which correlates to the 3s$_{1/2}$+3p$_{1/2}$ asymptote, to the $4^1Σ^+_g$ and $2^1Π_g$ states at the 3s$_{1/2}$+3d$_{3/2}$ asymptote. We performed multi-channel calculations, applying the mapped Fourier grid method, which reproduce our experimentally observed level shifts well.

physics.atm-clus↗