arXiv subjects

Olivier Dulieu

Publications and source records attributed to Olivier Dulieu.

86 records · Page 5Linked to original sources

arXiv2009

Photoassociative molecular spectroscopy for atomic radiative lifetimes

When the atoms of a dimer remain most of the time very far apart, in so-called long-range molecular states, their mutual interaction is ruled by plain atomic properties. The high-resolution spectroscopic study of some molecular excited states populated by photoassociation of cold atoms (photoassociative spectroscopy) gives a good illustration of this property. It provides accurate determinations of atomic radiative lifetimes, which are known to be sensitive tests for atomic calculations. A number of such analyses has been performed up to now, for all stable alkali atoms and for some other atomic species (Ca, Sr, Yb). A systematic review of these determinations is attempted here, with special attention paid to accuracy issues.

physics.atom-ph↗

arXiv2009

Electronic structure of the Magnesium hydride molecular ion

In this paper, using a standard quantum chemistry approach based on pseudopotentials for atomic core representation, Gaussian basis sets, and effective core polarization potentials, we investigate the electronic properties of the MgH$^+$ ion. We first determine potential energy curves for several states using different basis sets and discuss their predicted accuracy by comparing our values of the well depths and position with other available results. We then calculate permanent and transition dipole moments for several transitions. Finally for the first time, we calculate the static dipole polarizability of MgH$^+$ as function of the interatomic distance. This study represents the first step towards the modeling of collisions between trapped cold Mg$^+$ ions and H$_2$ molecules.

quant-ph↗

arXiv2009

Systematic trends in electronic properties of alkali hydrides

Obtaining ultracold samples of dipolar molecules is a current challenge which requires an accurate knowledge of their electronic properties to guide the ongoing experiments. Alkali hydride molecules have permanent dipole significantly larger than those of mixed alkali species and, as pointed out by Taylor-Juarros et al. [Eur. Phys. J. D 31, 213 (2004)] and by Juarros et al. [Phys. Rev. A 73, 041403 (2006)], are thus good candidates for molecule formation. In this paper, using a standard quantum chemistry approach based on pseudopotentials for atomic core representation, large Gaussian basis sets, and effective core polarization potential, we systematically investigate the electronic properties of the alkali hydrides LiH to CsH, in order to discuss general trends of their behavior. We computed (for the first time for NaH, KH, RbH, and CsH) the variation of their static polarizability with the internuclear distance. Moreover, in addition to potential curves, we determine accurate values of permanent and transition dipole moments for ground and excited states depending on the internuclear distance. The behavior of electronic properties of all alkali hydrides is compared to each other, in the light of the numerous other data available in the literature. Finally, the influence of the quality of the representation of the hydrogen electronic affinity in the approach on the results is discussed.

physics.atom-ph↗

arXiv2008

Precision molecular spectroscopy for ground state transfer of molecular quantum gases

One possibility for the creation of ultracold, high-phase-space-density quantum gases of molecules in the rovibrational ground state relies on first associating weakly-bound molecules from quantum-degenerate atomic gases on a Feshbach resonance and then transfering the molecules via several steps of coherent two-photon stimulated Raman adiabatic passage (STIRAP) into the rovibronic ground state. Here, in ultracold samples of Cs_2 Feshbach molecules produced out of ultracold samples of Cs atoms, we observe several optical transitions to deeply bound rovibrational levels of the excited 0_u^+ molecular potentials with high resolution. At least one of these transitions, although rather weak, allows efficient STIRAP transfer into the deeply bound vibrational level |v=73> of the singlet X ^1Sigma_g^+ ground state potential, as recently demonstrated. From this level, the rovibrational ground state level |v=0, J=0> can be reached with one more transfer step. In total, our results show that coherent ground state transfer for Cs_2 is possible using a maximum of two successive two-photon processes or one single four-photon STIRAP process.

cond-mat.other↗

arXiv2008

Dark resonances for ground state transfer of molecular quantum gases

One possible way to produce ultracold, high-phase-space-density quantum gases of molecules in the rovibronic ground state is given by molecule association from quantum-degenerate atomic gases on a Feshbach resonance and subsequent coherent optical multi-photon transfer into the rovibronic ground state. In ultracold samples of Cs_2 molecules, we observe two-photon dark resonances that connect the intermediate rovibrational level |v=73,J=2> with the rovibrational ground state |v=0,J=0> of the singlet $X^1Σ_g^+$ ground state potential. For precise dark resonance spectroscopy we exploit the fact that it is possible to efficiently populate the level |v=73,J=2> by two-photon transfer from the dissociation threshold with the stimulated Raman adiabatic passage (STIRAP) technique. We find that at least one of the two-photon resonances is sufficiently strong to allow future implementation of coherent STIRAP transfer of a molecular quantum gas to the rovibrational ground state |v=0,J=0>.

quant-ph↗

arXiv2008

Efficient formation of deeply bound ultracold molecules probed by broadband detection

Using a non-selective broadband detection scheme we discovered an efficient mechanism of formation of ultracold Cs$_2$ molecules in deeply bound levels ($v=1-9$) of their electronic ground state X$^1 Σ_g^+$. They are formed by a one-photon photoassociation of ultracold cesium atoms in a manifold of excited electronic states, followed by a two-step spontaneous emission cascade. We were able to form about $10^5-10^6$ molecules per second in these low vibrational levels of the ground state. This detection scheme could be generalized to other molecular species for the systematic investigation of cold molecule formation mechanisms.

physics.atom-ph↗

arXiv2008

Calculations of static dipole polarizabilities of alkali dimers. Prospects for alignment of ultracold molecules

The rapid development of experimental techniques to produce ultracold alkali molecules opens the ways to manipulate them and to control their dynamics using external electric fields. A prerequisite quantity for such studies is the knowledge of their static dipole polarizabilities. In this paper, we computed the variations with internuclear distance and with vibrational index of the static dipole polarizability components of all homonuclear alkali dimers including Fr$_2$, and of all heteronuclear alkali dimers involving Li to Cs, in their electronic ground state and in their lowest triplet state. We use the same quantum chemistry approach than in our work on dipole moments (M. Aymar and O. Dulieu, J. Chem. Phys. 122, 204302 (2005)), based on pseudopotentials for atomic core representation, Gaussian basis sets, and effective potentials for core polarization. Polarizabilities are extracted from electronic energies using the finite-field method. For the heaviest species Rb$_2$, Cs$_2$ and Fr$_2$ and for all heteronuclear alkali dimers, such results are presented for the first time. The accuracy of our results on atomic and molecular static dipole polarizabilities is discussed by comparing our values with the few available experimental data and elaborate calculations. We found that for all alkali pairs, the parallel and perpendicular components of the ground state polarizabilities at the equilibrium distance $R_e$ scale as $(R_e)^3$, which can be related to a simple electrostatic model of an ellipsoidal charge distribution. Prospects for possible alignment and orientation effects with these molecules in forthcoming experiments are discussed.

physics.atom-ph↗

arXiv2008

Optical pumping and vibrational cooling of molecules

The methods producing cold molecules from cold atoms tend to leave molecular ensembles with substantial residual internal energy. For instance, Cs2 molecules initially formed via photoassociation of cold Cs atoms are in several vibrational levels, v, of the electronic ground state. Here we apply a broadband femtosecond laser that redistributes the vibrational population in the ground state via a few electronic excitation - spontaneous emission cycles. The laser pulses are shaped to remove the excitation frequency band of the v = 0 level, preventing re-excitation from that state. We observe a fast and efficient accumulation, about 70% of the initially detected molecules, in the lowest vibrational level, v = 0, of the singlet electronic state. The validity of this incoherent depopulation pumping method is very general and opens exciting prospects for laser cooling and manipulation of molecules.

physics.atom-ph↗

arXiv2008

Quantum Gas of Deeply Bound Ground State Molecules

We create an ultracold dense quantum gas of ground state molecules bound by more than 1000 wavenumbers by stimulated two-photon transfer of molecules associated on a Feshbach resonance from a Bose-Einstein condensate of cesium atoms. The transfer efficiency exceeds 80%. In the process, the initial loose, long-range electrostatic bond of the Feshbach molecule is coherently transformed into a tight chemical bond. We demonstrate coherence of the transfer in a Ramsey-type experiment and show that the molecular sample is not heated during the transfer. Our results show that the preparation of a quantum gas of molecules in arbitrary rovibrational states is possible and that the creation of a Bose-Einstein condensate of molecules in their rovibronic ground state is within reach.

cond-mat.other↗

arXiv2008

Precision measurements with polar molecules: the role of the black body radiation

In the perspective of the outstanding developments of high-precision measurements of fundamental constants using polar molecules related to ultimate checks of fundamental theories, we investigate the possibly counterproductive role of black-body radiation on a series of diatomic molecules which would be trapped and observed for long durations. We show that the absorption of black-body radiation at room temperature may indeed limit the lifetime of trapped molecules prepared in a well-defined quantum state. Several examples are treated, corresponding to pure rotational absorption, pure vibrational absorption or both. We also investigate the role of a black-body radiation-induced energy shift on molecular levels and how it could affect high-precision frequency measurements.

physics.atom-ph↗

arXiv2006

Efficient formation of strongly bound ultracold cesium molecules by photoassociation with tunneling

We calculate the rates of formation and detection of ultracold Cs_2 molecules obtained from the photoassociation of ultracold atoms through the double-well 0g- (6S1/2 + 6P3/2) state. We concentrate on two features previously observed experimentally and attributed to tunneling between the two wells [Vatasescu et al 2000 Phys. Rev. A 61 044701]. We show that the molecules obtained are in strongly bound levels (v''=5,6) of the metastable a3Sigma_u+ (6S1/2 + 6S1/2) ground electronic state.

physics.atom-ph↗

arXiv2006

Analysis of light-induced frequency shifts in the photoassociation of ultracold metastable helium atoms

We present an exhaustive analysis of the light-induced frequency shifts of the photoassociation lines of ultracold metastable 4He* atoms in a magnetic trap. The measurements of the shifts of several vibrational levels bound in the purely long-range J=1,0u+ potential linked to the 23S1-23P0 asymptote were reported in a previous paper and are analyzed here. The simplicity of this system makes it very appropriate for a detailed study. Indeed, the purely long-range character of the excited potential allows one to calculate exact excited molecular wavefunctions and to use asymptotic expansions at large internuclear distances of the ground state wavefunctions appearing in Franck-Condon type integrals. Moreover, the number of collisional channels to be considered is strongly reduced by the absence of hyperfine structure for 4He* and the use of polarized ultracold atoms and polarized light. This allows us to derive semi-analytical expressions for the shifts showing explicitly their linear dependences on the s-wave scattering length a of spin polarized metastable 4He* atoms. This explains how it is possible to derive the measurement of a from these shifts.

cond-mat.other↗

arXiv2006

Electronic properties of Francium diatomic compounds and prospects for cold molecule formation

In this work we investigate the possibility to create cold Fr$\_2$, RbFr, and CsFr molecules through photoassociation of cold atoms. Potential curves, permanent and transition dipole moments for the Francium dimer and for the RbFr and RbCs molecules are determined for the first time. The Francium atom is modelled as a one valence electron moving in the field of the Fr$^+$ core, which is described by a new pseudopotential with averaged relativistic effects, and including effective core polarization potential. The molecular calculations are performed for both the ionic species Fr$\_2^+$, RbFr$^+$, CsFr$^+$ and the corresponding neutral, through the CIPSI quantum chemistry package where we used new extended gaussian basis sets for Rb, Cs, and Fr atoms. As no experimental data is available, we discuss our results by comparison with the Rb$\_2$, Cs$\_2$, and RbCs systems. The dipole moment of CsFr reveals an electron transfer yielding a Cs$^+$Fr$^-$ arrangement, while in all other mixed alkali pairs the electron is transferred towards the lighter species. Finally the perturbative treatment of the spin-orbit coupling at large distances predicts that in contrast with Rb$\_2$ and Cs$\_2$, no double-well excited potential should be present in Fr$\_2$, probably preventing an efficient formation of cold dimers via photoassociation of cold Francium atoms.

quant-ph↗

arXiv2005

Calculation of accurate permanent dipole moments of the lowest $^{1,3} Σ^+$ states of heteronuclear alkali dimers using extended basis sets

The obtention of ultracold samples of dipolar molecules is a current challenge which requires an accurate knowledge of their electronic properties to guide the ongoing experiments. In this paper, we systematically investigate the ground state and the lowest triplet state of mixed alkali dimers (involving Li, Na, K, Rb, Cs) using a standard quantum chemistry approach based on pseudopotentials for atomic core representation, gaussian basis sets, and effective terms for core polarization effects. We emphasize on the convergence of the results for permanent dipole moments regarding the size of the gaussian basis set, and we discuss their predicted accuracy by comparing to other theoretical calculations or available experimental values. We also revisit the difficulty to compare computed potential curves among published papers, due to the differences in the modelization of core-core interaction.

quant-ph↗