This article reviews the current state of the art in the field of cold and ultracold molecules and demonstrates that chemical reactions, inelastic collisions and dissociation of molecules at subKelvin temperatures can be manipulated with external electric or magnetic fields. The creation of ultracold molecules may allow for spectroscopy measurements with extremely high precision and tests of fundamental symmetries of nature, quantum computation with molecules as qubits, and controlled chemistry. The probability of chemical reactions and collisional energy transfer can be very large at temperatures near zero Kelvin. The collision energy of ultracold atoms and molecules is much smaller than perturbations due to interactions with external electric or magnetic fields available in the laboratory. External fields may therefore be used to induce dissociation of weakly bound molecules, stimulate forbidden electronic transitions, suppress the effect of centrifugal barriers in outgoing reaction channels or tune Feshbach resonances that enhance chemical reactivity.
We present a simple method for determination of absolute vibrational numbering of isolated near dissociation levels in diatomic molecules, usually observed in cold physics experiments. The method is based on the isotope shift and works even when energies of only two levels from one isotopologue and one level from another isotopologue have been measured. It is demonstrated on data from recently reported precise measurements of binding energies of levels lying close to the dissociation limits in ultracold Yb2, CsYb, RbSr and RbYb molecules. Its predictions agree with these of much more elaborate…
This review describes recent experimental and theoretical advances in forming molecules in ultracold gases of trapped alkali metal atoms, both by magnetic tuning through Feshbach resonances and by photoassociation. Molecular Bose-Einstein condensation of long-range states of both boson dimers and fermion dimers was achieved in 2002-3. Condensates of boson dimers were found to be short-lived, but long-lived condensates of fermion dimers have been produced. Signatures of triatomic and tetraatomic molecules have recently been observed. Both homonuclear and heteronuclear molecules have been formed…
We report efficient all-optical creation of an ultracold gas of alkaline-earth-metal dimers, $^{88}\rm{Sr}_2$, in their absolute ground state. Starting with weakly bound singlet molecules formed by narrow-line photoassociation in an optical lattice, followed by stimulated Raman adiabatic passage (STIRAP) via a singlet-dominant channel in the $(1)0_u^+$ excited potential, we prepare pure samples of more than 5500 molecules in $X^1Σ_g^+(v=0,J=0)$. We observe two-body collisional loss rates close to the universal limit for both the least bound and most bound vibrational states in $X^1Σ_g^+$. We d…
We present an accurate quantum mechanical study of molecule-molecule collisions in the presence of a magnetic field. The work focusses on the analysis of elastic scattering and spin relaxation in collisions of O2(3Sigma_g) molecules at cold (~0.1 K) and ultracold (~10^{-6} K) temperatures. Our calculations show that magnetic spin relaxation in molecule-molecule collisions is extremely efficient except at magnetic fields below 1 mT. The rate constant for spin relaxation at T=0.1 K and a magnetic field of 0.1 T is found to be as large as 6.1 x 10^{-11} cm3/s. The magnetic field dependence of ela…
We explore the quantum dynamics of heteronuclear atomic collisions in waveguides and demonstrate the existence of a novel mechanism for the resonant formation of polar molecules. The molecular formation probabilities can be tuned by changing the trap frequencies characterizing the transverse modes of the atomic species. The origin of this effect is the confinement-induced mixing of the relative and center of mass motions in the atomic collision process leading to a coupling of the diatomic continuum to center of mass excited molecular states in closed transverse channels.
We report on the creation of an ultracold dipolar gas of fermionic $^{23}$Na$^{40}$K molecules in their absolute rovibrational and hyperfine ground state. Starting from weakly bound Feshbach molecules, we demonstrate hyperfine resolved two-photon transfer into the singlet ${\rm X}^1Σ^+ |v{=}0,J{=}0\rangle$ ground state, coherently bridging a binding energy difference of 0.65 eV via stimulated rapid adiabatic passage. The spin-polarized, nearly quantum degenerate molecular gas displays a lifetime longer than 2.5 s, highlighting NaK's stability against two-body chemical reactions. A homogeneous …
We demonstrate the transfer of $^{23}$Na$^{40}$K molecules from a closed-channel dominated Feshbach-molecule state to the absolute ground state. The Feshbach molecules are initially created from a gas of sodium and potassium atoms via adiabatic ramping over a Feshbach resonance at 78.3$\,$G. The molecules are then transferred to the absolute ground state using stimulated Raman adiabatic passage with an intermediate state in the spin-orbit-coupled complex $|c^3 Σ^+, v=35, J=1 \rangle \sim |B^1Π, v=12, J=1\rangle$. Our measurements show that the pump transition dipole moment linearly increases w…
We investigate theoretically the long-range electrostatic interactions between a ground-state homonuclear alkali-metal dimer and an excited alkali-metal atom taking into account its fine-structure. The interaction involves the combination of first-order quadrupole-quadrupole and second-order dipole-dipole effects. Depending on the considered species, the atomic spin-orbit may be comparable to the atom-molecule electrostatic energy and to the dimer rotational structure. Here we extend our general description in the framework of the second-order degenerate perturbation theory [M. Lepers and O. D…
We report a comparison between two absolute gravimeters: the LNE-SYRTE cold atoms gravimeter and FG5#220 of Leibniz Universität of Hannover. They rely on different principles of operation: atomic and optical interferometry. Both are movable which enabled them to participated to the last International Comparison of Absolute Gravimeters (ICAG'09) at BIPM. Immediately after, their bilateral comparison took place in the LNE watt balance laboratory and showed an agreement of 4.3 +/- 6.4 μGal.
We report a detailed molecular spectroscopy study on the lowest excited electronic states of $^{23}\rm{Na}^{87}\rm{Rb}$ for producing ultracold $^{23}\rm{Na}^{87}\rm{Rb}$ molecules in the electronic, rovibrational and hyperfine ground state. Starting from weakly-bound Feshbach molecules, a series of vibrational levels of the $A^{1}Σ^{+}-b^{3}Π$ coupled excited states were investigated. After resolving, modeling and interpreting the hyperfine structure of several lines, we successfully identified a long-lived level resulting from the accidental hyperfine coupling between the $0^+$ and $0^-$ com…
We report the creation of ultralong-range Sr$_2$ molecules comprising one ground-state $5s^2$ $^1S_0$ atom and one atom in a $5sns$ $^3S_1$ Rydberg state for $n$ ranging from 29 to 36. Molecules are created in a trapped ultracold atomic gas using two-photon excitation near resonant with the $5s5p$ $^3P_1$ intermediate state, and their formation is detected through ground-state atom loss from the trap. The observed molecular binding energies are fit with the aid of first-order perturbation theory that utilizes a Fermi pseudopotential with effective $s$-wave and $p$-wave scattering lengths to de…
We report measurements of the hyperfine coupling constant for the $8p \ ^2P_{1/2}$ level of atomic cesium, $^{133}$Cs, with a relative uncertainty of $\sim$0.019\%. Our result is $A = 42.933 \: (8)$ MHz, in good agreement with recent theoretical results. We also examine the hyperfine structure of the $8p \ ^2P_{3/2}$ state, and derive new values for the state energies of the $8p \ ^2P_{1/2}$ and $8p \ ^2P_{3/2}$ states of cesium.
Precise calculations of core properties in heavy-atom systems which are described by the operators heavily concentrated in atomic cores, like to hyperfine structure and P,T-parity nonconservation effects, usually require accounting for relativistic effects. Unfortunately, completely relativistic treatment of molecules containing heavy elements is very consuming already at the stages of calculation and transformation of two-electron integrals with a basis set of four-component spinors. In turn, the relativistic effective core potential (RECP) calculations of valence (spectroscopic, chemical etc…
We measure the absolute absorption cross section of molecules using a matter-wave interferometer. A nanostructured density distribution is imprinted onto a dilute molecular beam through quantum interference. As the beam crosses the light field of a probe laser some molecules will absorb a single photon. These absorption events impart a momentum recoil which shifts the position of the molecule relative to the unperturbed beam. Averaging over the shifted and unshifted components within the beam leads to a reduction of the fringe visibility, enabling the absolute absorption cross section to be ex…
We report the absolute frequency measurement of the 5s2 1S0-5s5p 3P0 transition in 87Sr optical lattice clock (Sr1) at National Time Service Center (NTSC). Its systematic frequency shifts are evaluated carefully with a total relative uncertainty of 5.1E10-17. The measured absolute frequency is 429 228 004 229 872.91(18) Hz with a relative uncertainty of 4.13E10-16, with reference to the ensemble of primary and secondary frequency standards published in the Circular T bulletin by BIPM through a global navigation satellite system (GNSS) link.
We report measurements of the absolute energies of the hyperfine components of the $12s \ ^2S_{1/2}$ and $13s \ ^2S_{1/2}$ levels of atomic cesium, $^{133}$Cs. Using the frequency difference between these components, we determine the hyperfine coupling constants for these states, and report these values with a relative uncertainty of $\sim$0.06 %. We also examine the hyperfine structure of the $11d \ ^2D_{J}$ ($J=3/2, 5/2$) states, and resolve the sign ambiguity of the hyperfine coupling constants from previous measurements of these states. We also derive new, high precision values for the sta…
A new iterative version of population projection analysis is formulated and applied to determine relativistic effective atomic configurations of superheavy elements Cn and Fl and their lighter homologues (Hg and Pb) in the molecules of their fluorides and oxides. The dependence of the computed populations on the initial reference atomic spinors is completely avoided. The difference in population of atomic spinors with the same orbital angular momentum and different total angular momenta is demonstrated to be essential for understanding the peculiarities of chemical bonding in superheavy elemen…
We discuss laser dressed dipolar and Van der Waals interactions between atoms and polar molecules, so that a cold atomic gas with laser admixed Rydberg levels acts as a designed reservoir for both elastic and inelastic collisional processes. The elastic scattering channel is characterized by large elastic scattering cross sections and repulsive shields to protect from close encounter collisions. In addition, we discuss a dissipative (inelastic) collision where a spontaneously emitted photon carries away (kinetic) energy of the collision partners, thus providing a significant energy loss in a s…
We report the direct comparison between the stabilities of two mobile absolute gravimeters of different technology: the LNE-SYRTE Cold Atom Gravimeter and FG5X\#216 of the Université du Luxembourg. These instruments rely on two different principles of operation: atomic and optical interferometry. The comparison took place in the Walferdange Underground Laboratory for Geodynamics in Luxembourg, at the beginning of the last International Comparison of Absolute Gravimeters, ICAG-2013. We analyse a 2h10 duration common measurement, and find that the CAG shows better immunity with respect to change…
We give a detailed account of the theoretical analysis and the experimental results of an x-ray-diffraction experiment on quantum-state selected and strongly laser-aligned gas-phase ensembles of the prototypical large asymmetric rotor molecule 2,5-diiodobenzonitrile, performed at the Linac Coherent Light Source [Phys. Rev. Lett. 112, 083002 (2014)]. This experiment is the first step toward coherent diffractive imaging of structures and structural dynamics of isolated molecules at atomic resolution, i. e., picometers and femtoseconds, using x-ray free-electron lasers.
The absolute frequency measurement for all of the hyperfine transitions of 6P1/2 -> 7S1/2 using a self-referencing frequency comb is reported. This transition can be used as a bench marker for the accurate atomic wave function, and then improve the calculation of the atomic parity- non-conservation (PNC). The frequency center is precisely determined by saturation spectroscopy utilizing a pair of the counter-propagating laser beams intersecting with atomic beam. Such a Doppler-free profile has been improved to 350 kHz in the absolute frequency measurement. The 7S1/2 state hyperfine splittings h…
The detection of single molecules has facilitated many advances in life- and material-sciences. Commonly, it founds on the fluorescence detection of single molecules, which are for example attached to the structures under study. For fluorescence microscopy and sensing the crucial parameters are the collection and detection efficiency, such that photons can be discriminated with low background from a labeled sample. Here we show a scheme for filtering the excitation light in the optical detection of single stranded labeled DNA molecules. We use the narrow-band filtering properties of a hot atom…
We present a novel slowing scheme for beams of laser-coolable diatomic molecules reminiscent of Zeeman slowing of atomic beams. The scheme results in efficient compression of the 1-dimensional velocity distribution to velocities trappable by magnetic or magneto-optical traps. 3D Monte Carlo simulations for the prototype molecule $^{88}\mathrm{Sr}^{19}\mathrm{F}$ and experiments in an atomic testbed demonstrate a performance comparable to traditional atomic Zeeman slowing and an enhancement of flux below v=35 m/s by a factor of $\approx 20$ compared to white-light slowing. This is the first exp…
The highly forbidden $^2$S$_{1/2} \rightarrow ^2$F$_{7/2}$ electric octupole transition in $^{171}$Yb$^+$ is a potential candidate for a redefinition of the SI second. We present a measurement of the absolute frequency of this optical transition, performed using a frequency link to International Atomic Time to provide traceability to the SI second. The $^{171}$Yb$^+$ optical frequency standard was operated for 76% of a 25-day period, with the absolute frequency measured to be 642 121 496 772 645.14(26) Hz. The fractional uncertainty of $4.0 \times 10 ^{-16}$ is comparable to that of the best p…
We measure inelastic collisions between ultracold CaF molecules by combining two optical tweezers, each containing a single molecule. We observe collisions between $^2Σ$ CaF molecules in the absolute ground state $|X,v=0, N=0,F=0\rangle$, and in excited hyperfine and rotational states. In the absolute ground state, we find a two-body loss rate of $7(4) \times 10^{-11} \text{cm}^{3}/\text{s}$, which is below, but close to the predicted universal loss rate.
The absolute frequency of the $^{87}{\rm Sr}$ clock transition measured in 2015 was reevaluated using an improved frequency link to the SI second. The scale interval of International Atomic Time (TAI) that we used as the reference was calibrated for an evaluation interval of five days instead of the conventional interval of one month which is regularly employed in Circular T. The calibration on a five-day basis removed the uncertainty in assimilating the TAI scale of the five-day mean to that of the one-month mean. The reevaluation resulted in the total uncertainty of $10^{-16}$ level for the …
We report the successful production of an ultracold sample of absolute ground-state $^{23}$Na$^{87}$Rb molecules. Starting from weakly-bound Feshbach molecules formed via magneto-association, the lowest rovibrational and hyperfine level of the electronic ground state is populated following a high efficiency and high resolution two-photon Raman process. The high purity absolute ground-state samples have up to 8000 molecules and densities of over $10^{11}$ cm$^{-3}$. By measuring the Stark shifts induced by external electric fields, we determined the permanent electric dipole moment of the absol…
We investigate magnetoassociation of ultracold Feshbach molecules from a Bose- Einstein condensate of Cs atoms and explore the spectrum of weakly bound molecular states close to the atomic threshold. By exploiting the variation of magnetic field experienced by a molecular cloud falling in the presence of a magnetic field gradient, we demonstrate the repeated output coupling of molecules from a single atomic cloud using a Feshbach resonance at 19.89 G. Using this method we are able to produce up to 24 separate pulses of molecules from a single atomic condensate, with a molecular pulse created e…
We present the prospects for photoassociation, optical control of interspecies scattering lengths and finally, the production of ultracold absolute ground state molecules in the Rb+Hg system. We use the "gold standard" ab initio methods for the calculations of ground (CCSD(T)) and excited state (EOM-CCSD) potential curves. The RbHg system, thanks to the wide range of stable Hg bosonic isotopes, offers possibilities for mass-tuning of ground state interactions. The optical lengths describing the strengths of optical Feshbach resonances near the Rb transitions are favorable even at large laser d…
We have successfully implemented the first simultaneous magneto-optical trapping (MOT) of lithium ($^6$Li) and ytterbium ($^{174}$Yb) atoms, towards production of ultracold polar molecules of LiYb. For this purpose, we developed the dual atomic oven which contains both atomic species as an atom source and successfully observed the spectra of the Li and Yb atoms in the atomic beams from the dual atomic oven. We constructed the vacuum chamber including the glass cell with the windows made of zinc selenium (ZnSe) for the CO$_2$ lasers, which are the useful light sources of optical trapping for ev…
Theoretical Proposal of a Digital Closed-Loop Thermal Atomic-Beam Interferometer for High-Bandwidth, Wide-Dynamic-Range, and Simultaneous Absolute Acceleration-Rotation Sensing
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…
The ytterbium atom is widely used in the fields of atomic physics, cavity quantum electrodynamics, quantum information processing and optical frequency standards. There is however a strong dispersion among the reported values of the ${}^1{\rm S}_0 \rightarrow {}^1{\rm P}_1$ transition frequency. In this article, we present two independent measurements of the absolute frequency of this transition performed with two different wavemeters using atomic fluorescence spectroscopy. The cancellation of Doppler shifts is obtained by fine tuning the angle between the probe laser and the atomic beam. The …
Cold inelastic collisions between confined cesium (Cs) atoms and Cs$\_2$ molecules are investigated inside a CO$\_2$ laser dipole trap. Inelastic atom-molecule collisions can be observed and measured with a rate coefficient of $\sim 2.5 \times 10^{-11} $cm$^3$ s$^{-1}$, mainly independent of the molecular ro-vibrational state populated. Lifetimes of purely atomic and molecular samples are essentially limited by rest gas collisions. The pure molecular trap lifetime ranges 0,3-1 s, four times smaller than the atomic one, as is also observed in a pure magnetic trap. We give an estimation of the i…
We consider the two-color photooassociation of a quantum degenerate atomic gas into ground-state diatomic molecules via a molecular dark state. This process can be described in terms of a lambda level scheme that is formally analogous to the situation in electromagnetically-induced transparency (EIT) in atomic systems, and therefore can result in slow light propagation. We show that the group velocity of the light field depends explicitly on whether the atoms are bosons or fermions, as well as on the existence or absence of a pairing gap in the case of fermions, so that the measurement of the …
We present relativistic many-body calculations of atomic and molecular Schiff-moment interaction constants including interelectron correlation effects using atomic Gaussian basis sets specifically optimized for the Schiff interaction. Our present best results employing a Gaussian nuclear density function are $α_{\text{SM}} = (0.364 \pm 0.025) \times 10^{-17} \frac{e \text{cm}}{e \text{fm}^3}$ for atomic $^{129}$Xe, $α_{\text{SM}} = (-2.40 \pm 0.24) \times 10^{-17} \frac{e \text{cm}}{e \text{fm}^3}$ for atomic $^{199}$Hg, and $W_{\text{SM}} = (39967\pm 3600)$ a.u. for the thallium nucleus in th…
According to the Schiff theorem, the atomic electrons completely screen the atomic nucleus from an external static electric field. However, this is not the case if the field is time-dependent. Electronic orbitals in atoms either shield the nucleus from an oscillating electric field when the frequency of the field is off the atomic resonances or enhance this field when its frequency approaches an atomic transition energy. In molecules, not only electronic, but also rotational and vibrational states are responsible for the screening of oscillating electric fields. As will be shown in this paper,…
