We study the effects of a static electric field on the photoassociation of a heteronuclear atom-pair into a polar molecule. The interaction of permanent dipole moment with a static electric field largely affects the ground state continuum wave function of the atom-pair at short separations where photoassociation transitions occur according to Franck-Condon principle. Electric field induced anisotropic interaction between two heteronuclear ground state atoms leads to scattering resonances at some specific electric fields. Near such resonances the amplitude of scattering wave function at short separation increases by several orders of magnitude. As a result, photoaasociation rate is enhanced by several orders of magnitude near the resonances. We discuss in detail electric field modified atom-atom scattering properties and resonances. We calculate photoassociation rate that shows giant enhancement due to electric field tunable anisotropic resonances. We present selected results among which particularly important are the excitations of higher rotational levels in ultracold photoassociation due to electric field tunable resonances.
We study the time-resolved photoassociation of ultracold sodium in an optical dipole trap. The photoassociation laser excites pairs of atoms to molecular states of large total angular momentum at high intensities (above 20 kW/cm$^{2}$). Such transitions are generally suppressed at ultracold temperatures by the centrifugal barriers for high partial waves. Time-resolved ionization measurements reveal that the atoms are accelerated by the dipole potential of the photoassociation beam. We change the collision energy by varying the potential depth, and observe a strong variation of the photoassocia…
Ultracold metastable RbCs molecules are observed in a double species MOT through photoassociation near the Rb(5S$_{1/2}$)+Cs(6P$_{3/2}$) dissociation limit followed by radiative stabilization. The molecules are formed in their lowest triplet electronic state and are detected by resonant enhanced two-photon ionization through the previously unobserved $(3)^{3}Π\leftarrow a^{3}Σ^{+}$ band. The large rotational structure of the observed photoassociation lines is assigned to the lowest vibrational levels of the $0^+,0^-$ excited states correlated to the Rb(5P$_{1/2}$)+Cs(6S$_{1/2}$) dissociation l…
We have produced ultracold, polar RbCs* molecules via photoassociation in a laser-cooled mixture of Rb and Cs atoms. Using a model of the RbCs* molecular interaction which reproduces the observed rovibrational structure, we infer decay rates in our experiments into deeply bound singlet ground state RbCs vibrational levels as high as 5 x 10^5 s^-1 per level. Population in such deeply bound levels could be efficiently transferred to the vibrational ground state using a single stimulated Raman transition, opening the possibility to create large samples of stable, ultracold polar molecules.
The formation of ultracold metastable RbCs molecules is observed in a double species magneto-optical trap through photoassociation below the ^85Rb(5S_1/2)+^133Cs(6P_3/2) dissociation limit followed by spontaneous emission. The molecules are detected by resonance enhanced two-photon ionization. Using accurate quantum chemistry calculations of the potential energy curves and transition dipole moment, we interpret the observed photoassociation process as occurring at short internuclear distance, in contrast with most previous cold atom photoassociation studies. The vibrational levels excited by p…
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 f…
We report the first observation of photoassociation to the 2(1)Sigma(g)(+) state of 85Rb2 . We have observed two vibrational levels (v'=98, 99) below the 5s1/2+5p1/2 atomic limit and eleven vibrational levels (v'=102-112) above it. The photoassociation---and subsequent spontaneous emission---occur predominantly between 15 and 20 Bohr in a region of internuclear distance best described as a transition between Hund's case (a) and Hund's case (c) coupling. The presence of a g-wave shape resonance in the collision of two ground-state atoms affects the photoassociation rate and lineshape of the J'=…
We report on a resonantly coupled 2(1) - 4 (1) photoassociation resonance in LiRb. This pair of states displays interesting decay physics that hint at interference-like effects caused by two different decay paths. We observe decay to predominantly $X \ ^1Σ^+ \ v=43$, with significant numbers of molecules produced in $X \ ^1Σ^+ \ v=2$ - 12. This photoassociation resonance also produces $\sim$300 $X \ ^1Σ^+ \ v=0 \ J=0$ molecules/second. Finally, we identify a stimulated Raman adiabatic passage transfer pathway from $v=43$ to $v=0$ that has the potential to produce up to $2 \times 10^5$ LiRb mol…
We report the production of ultracold heteronuclear Cs$^*$Yb molecules through one-photon photoassociation applied to an ultracold atomic mixture of Cs and Yb confined in an optical dipole trap. We use trap-loss spectroscopy to detect molecular states below the Cs($^{2}P_{1/2}$) + Yb($^{1}S_{0}$) asymptote. For $^{133}$Cs$^{174}$Yb, we observe 13 rovibrational states with binding energies up to $\sim$500 GHz. For each rovibrational state we observe two resonances associated with the Cs hyperfine structure and show that the hyperfine splitting in the diatomic molecule decreases for more deeply …
We report the observation of microwave coherent control of rotational states of ultracold $^{85}$Rb$^{133}$Cs molecules formed in their vibronic ground state by short-range photoassociation. Molecules are formed in the single rotational state $X(v=0,J=1)$ by exciting pairs of atoms to the short-range state $(2)^{3}Π_{0^{-}} (v=11, J=0)$, followed by spontaneous decay. We use depletion spectroscopy to record the dynamic evolution of the population distribution and observe clear Rabi oscillations while irradiating on a microwave transition between coupled neighbouring rotational levels. A densit…
We establish a theoretical model to analyze the photoassociative (PA) spectroscopy of $(3)^3Σ^+$ state of $^{85}$Rb$^{133}$Cs molecule. The term energy, spin-spin coupling constants and hyperfine interaction constant of nine vibrational levels in the $(3)^3Σ^+$ state are determined. Based on the fitted term energy and rotation constant, the potential energy curve of $(3)^3Σ^+$ state is obtained by using the RKR method which is compared with the ab initial potential curve.
Ultracold molecules offer a broad variety of applications, ranging from metrology to quantum computing. However, forming "real" ultracold molecules, {\it i.e.} in deeply bound levels, is a very difficult proposition. Here, we show how photoassociation in the vicinity of a Feshbach resonance enhance molecular formation rates by several orders of magnitude. We illustrate this effect in heteronuclear systems, and find giant rate coefficients even in deeply bound levels. We also give a simple analytical expression for the photoassociation rates, and discuss future applications of the Feshbach Opti…
We show that the photoassociation (PA) rate of ultracold diatomic molecules in the vicinity of a Feshbach resonance could be used to probe variations of the electron-to-proton mass ratio $β= m_e/m_p$, a quantity related to other fundamental constants via the $Λ_{\mathrm{QCD}}$ scale. The PA rate exhibits two features near a Feshbach resonance, a minimum and a maximum, which are very sensitive to the details of the interactions and the exact mass of the system. The effect and detection threshold are illustrated in the formation rates of ultracold Li$_2$ and LiNa molecules by performing coupled-…
We demonstrate the direct formation of vibronic ground state RbCs molecules by photoassociation of ultracold atoms followed by radiative stabilization. The photoassociation proceeds through deeply-bound levels of the (2)^{3}Π_{0^{+}} state. From analysis of the relevant free-to-bound and bound-to-bound Franck-Condon factors, we have predicted and experimentally verified a set of photoassociation resonances that lead to efficient creation of molecules in the v=0 vibrational level of the X^{1}Σ^{+} electronic ground state. We also compare the observed and calculated laser intensity required to s…
We report the formation of ultracold $^{7}$Li$^{85}$Rb molecules in the $a^{3}Σ^{+}$ electronic state by photoassociation (PA) and their detection via resonantly enhanced multiphoton ionization (REMPI). With our dual-species Li and Rb magneto-optical trap (MOT) apparatus, we detect PA resonances with binding energies up to ~62 cm$^{-1}$ below the $^{7}$Li 2s $^{2}S_{1/2}$ $+$ $^{85}$Rb 5p $^{2}P_{1/2}$ asymptote. In addition, we use REMPI spectroscopy to probe the $a^{3}Σ^{+}$ state and excited electronic $3^{3} Π$ and $4^{3} Σ^{+}$ states, and identify $a^{3}Σ^{+} (v" = 7 - 13)$, $3^{3} Π(v'_…
The creation of ultracold molecules is currently limited to diatomic species. In this letter we present a theoretical description of the photoassociation of ultracold atoms and molecules to create ultracold excited triatomic molecules, thus being a novel example of light-assisted ultracold chemical reaction. The calculation of the photoassociation rate of ultracold Cs atoms with ultracold Cs$_2$ molecules in their rovibrational ground state is reported, based on the solution of the quantum dynamics involving the atom-molecule long-range interactions, and assuming a model potential for the shor…
Photoassociation of spin-polarized metastable helium to the three lowest rovibrational levels of the J=1, $0_u^+$ state asymptoting to 2$s {}^{3}$S$_{1}+2p {}^{3}$P$_{0}$ is studied using a second-order perturbative treatment of the line shifts valid for low laser intensities, and two variants of a non-perturbative close-coupled treatment, one based upon dressed states of the matter plus laser system, and the other on a modified radiative coupling which vanishes asymptotically, thus simulating experimental conditions. These non-perturbative treatments are valid for arbitrary laser intensities …
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.
Photoassociation of ultracold rubidium atoms with femtosecond laser pulses is studied theoretically. The spectrum of the pulses is cut off in order to suppress pulse amplitude at and close to the atomic resonance frequency. This leads to long tails of the laser pulse as a function of time giving rise to coherent transients in the photoassociation dynamics. They are studied as a function of cutoff position and chirp of the pulse. Molecule formation in the electronically excited state is attributed to off-resonant excitation in the strong-field regime.
We perform photoassociation spectroscopy in an ultracold $^{23}$Na-$^6$Li mixture to study the $c^3Σ^+$ excited triplet molecular potential. We observe 50 vibrational states and their substructure to an accuracy of 20 MHz, and provide line strength data from photoassociation loss measurements. An analysis of the vibrational line positions using near-dissociation expansions and a full potential fit is presented. This is the first observation of the $c^3Σ^+$ potential, as well as photoassociation in the NaLi system.
State-of-the-art {\em ab initio} techniques have been applied to compute the potential energy curves for the SrYb molecule in the Born-Oppenheimer approximation for the ground state and first fifteen excited singlet and triplet states within the coupled-cluster framework. The leading long-range coefficients describing the dispersion interactions at large interatomic distances are also reported. The electric transition dipole moments have been obtained as the first residue of the polarization propagator computed with the linear response coupled-cluster method restricted to single and double exc…
We show that coherence between two excited ro-vibrational states belonging to the same molecular electronic configuration arises quite naturally due to their interaction with electromagnetic vacuum. For initial preparation of a molecule in the desired ro-vibrational states, we propose to employ the method of ultracold photoassociation. Spontaneous decay of the excited molecule then gives rise to vacuum induced coherence between the excited ro-vibrational states. We demonstrate theoretically an interesting interplay of effects due to vacuum induced coherence and photoassociation. We apply our t…
This theoretical paper investigates the formation of ground state molecules from ultracold cesium atoms in a two-color scheme. Following previous work on photoassociation with chirped picosecond pulses [Luc-Koenig et al., Phys. Rev. A {\bf 70}, 033414 (2004)], we investigate stabilization by a second (dump) pulse. By appropriately choosing the dump pulse parameters and time delay with respect to the photoassociation pulse, we show that a large number of deeply bound molecules are created in the ground triplet state. We discuss (i) broad-bandwidth dump pulses which maximize the probability to f…
We predict feasibility of the photoassociative formation of Sr_2 molecules in arbitrary vibrational levels of the electronic ground state based on state-of-the-art ab initio calculations. Key is the strong spin-orbit interaction between the c^3Π_u, A^1Σ_u^+ and B^1Σ_u^+ states. It creates not only an effective dipole moment allowing free-to-bound transitions near the ^1S + ^3P_1 intercombination line but also facilitates bound-to-bound transitions via resonantly coupled excited state rovibrational levels to deeply bound rovibrational levels of the ground X^1Σ_g^+ potential, with v" as low as v…
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 photoa…
We report on measurements of the binding energies of several weakly bound vibrational states of the paramagnetic $^{174}$Yb$^{6}$Li molecule in the electronic ground state using two-photon spectroscopy in an ultracold atomic mixture confined in an optical dipole trap. We theoretically analyze the experimental spectrum to obtain an accurate description of the long-range potential of the ground state molecule. Based on the measured binding energies, we arrive at an improved value of the interspecies $s$-wave scattering length $a_{s0}=30$ $a_0$. Employing coherent two-photon spectroscopy we also …
We report photoassociation spectroscopy of ultracold $^{86}$Sr atoms near the intercombination line and provide theoretical models to describe the obtained bound state energies. We show that using only the molecular states correlating with the $^1S_0$$+$$^3P_1$ asymptote is insufficient to provide a mass scaled theoretical model that would reproduce the bound state energies for all isotopes investigated to date: $^{84}$Sr, $^{86}$Sr and $^{88}$Sr. We attribute that to the recently discovered avoided crossing between the $^1S_0$$+$$^3P_1$ $0_u^+$ ($^3Π_u$) and $^1S_0$$+$$^1D_2$ $0_u^+$ ($^1Σ^+_…
Two-color photoassociation of ground state $^6$Li$^{87}$Rb molecules via the $\mathrm{B}^1Π$ electronic state using short pulses near a magnetic Feshbach resonance is studied theoretically. A near-resonant magnetic field is applied to mix the hyperfine singlet and triplet components of the initial wave function and enhance the photoassociation rate, before the population is transferred to the ground state by a second pulse. We show that an increase of up to three orders of magnitude in the absolute number of molecules produced is attainable for deeply bound vibrational levels. This technique c…
We report on photoassociation (PA) spectroscopy of a degenerate Fermi gas of $^{173}$Yb atoms near the dissociation limit of the spin-forbidden ${^1}S_0-{^3}P_1$ intercombination transition. An atom-loss spectrum is measured from a trapped sample for a spectral range down to $-1$~GHz with respect to the $f=5/2 \rightarrow f^\prime=7/2$ atomic resonance. The spectrum shows eighty PA resonances, revealing the high nuclear spin nature of the system. We investigate the Zeeman effect on the spectrum near a detuning of $-0.8$~GHz, where we examine the quantum numbers of the Zeeman levels using vario…
We report the production of ultracold heteronuclear 7Li85Rb molecules in excited electronic states by photoassociation (PA) of ultracold 7Li and 85Rb atoms. PA is performed in a dual-species 7Li-85Rb magneto-optical trap (MOT) and the PA resonances are detected using trap loss spectroscopy. We identify several strong PA resonances below the Li (2s 2S1/2) + Rb (5p 2P3/2) asymptote and experimentally determine the long range C6 dispersion coefficients. We find a molecule formation rate (P_LiRb) of 3.5x10^7 s^-1 and a PA rate coefficient (K_PA) of 1.3x10^-10 cm^3/s, the highest among heteronuclea…
We experimentally investigate various processes present in the photoassociative interaction of an ultracold atomic sample with shaped femtosecond laser pulses. We demonstrate the photoassociation of pairs of rubidium atoms into electronically excited, bound molecular states using spectrally cut femtosecond laser pulses tuned below the rubidium D1 or D2 asymptote. Time-resolved pump-probe spectra reveal coherent oscillations of the molecular formation rate, which are due to coherent transient dynamics in the electronic excitation. The oscillation frequency corresponds to the detun-ing of the sp…
We report on two-photon photoassociation (PA) spectroscopy of ultracold heteronuclear LiRb molecules. This is used to determine the binding energies of the loosely bound levels of the electronic ground singlet and the lowest triplet states of LiRb. We observe strong two-photon PA lines with power broadened line widths greater than 20 GHz at relatively low laser intensity of 30 W/cm$^{2}$. The implication of this observation on direct atom to molecule conversion using stimulated Raman adiabatic passage (STIRAP) is discussed and the prospect for electronic ground state molecule production is the…
We report the production of ultracold 7Li85Rb molecules by photoassociation (PA) below the Li (2s 2S1/2) + Rb (5p 2P1/2) asymptote. We perform PA spectroscopy in a dual-species 7Li-85Rb magneto-optical trap (MOT) and detect the PA resonances using trap loss spectroscopy. We observe several strong PA resonances corresponding to the last few bound states, assign the lines and derive the long range C6 dispersion coefficients for the Li (2s 2S1/2) + Rb (5p 2P1/2) asymptote. We also report an excited-state molecule formation rate (P_LiRb) of ~10^7 s^-1 and a PA rate coefficient (K_PA) of ~4x10^-11 …
An experimental pump-probe study of the photoassociative creation of translationally ultracold rubidium molecules is presented together with numerical simulations of the process. The formation of loosely bound excited-state dimers is observed as a first step towards a fully coherent pump-dump approach to the stabilization of Rb$_2$ into its lowest ground vibrational states. The population that contributes to the pump-probe process is characterized and found to be distinct from a background population of pre-associated molecules.
Photoassociation, assembling molecules from atoms using laser light, is limited by the low density of atom pairs at sufficiently short interatomic separations. Here, we show that non-resonant light with intensities of the order of 10^10 W/cm^2 modifies the thermal cloud of atoms, enhancing the Boltzmann weight of shape resonances and pushing scattering states below the dissociation limit. This leads to an enhancement of photoassociation rates by several orders of magnitude and opens the way to significantly larger numbers of ground state molecules in a thermal ensemble than achieved so far.
We show that it is possible to excite higher rotational states J > 2 in ultracold photoassociation by two laser fields. Usually higher J states are suppressed in photoassociation at ultracold temperatures in the regime of Wigner threshold laws. We propose a scheme in which one strong laser field drives photoassociation transition close to either J = 1 or J = 2 rotational state of a particular vibrational level of an electronically excited molecule. The other laser field is tuned near photoassociation resonance with J > 2 rotational levels of the same vibrational state. The strong laser field i…
We explore the feasibility of optically forming long-range tetratomic and larger polyatomic molecules in their ground electronic state from ultracold pairs of polar molecules aligned by external fields. Depending on the relative orientation of the interacting diatomic molecules, we find that a tetratomic can be formed either as a weakly bound complex in a very extended halo state or as a pure long-range molecule composed of collinear or nearly-collinear diatomic molecules. The latter is a novel type of tetratomic molecule comprised of two diatomic molecules bound at long intermolecular range a…
Utilizing single-photon photoassociation, we have achieved ultracold rubidium molecules with a high number density that provides a new efficient approach toward molecular quantum degeneracy. A new detection mechanism for ultracold molecule utilizing the inelastic atom-molecule collision is demonstrated. The resonant coupling effect on the formation of the ${\rm X^1Σ^+_g}$ ground state ${\rm ^{85}Rb_2}$ allows for a sufficient number of more deeply bound ultracold molecules, which induced an additional trap loss and heating of the co-existing atoms owing to the inelastic atom-molecule collision…
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 b…
Ultracold paramagnetic and polar diatomic molecules are among the promising systems for quantum simulation of lattice-spin models. Unfortunately, their experimental observation is still challenging. Based on our recent \textit{ab-initio} calculations, we analyze the feasibility of all-optical schemes for the formation of ultracold $^{87}$Rb$^{84}$Sr bosonic molecules. First, we have studied the formation by photoassociation followed by spontaneous emission. The photoassociation rates to levels belonging to electronic states converging to the $^{87}$Rb$(5s\,^2S)$+$^{84}$Sr($5s5p\,^3P_{0,1,2}$) …
We present spectra of ultracold $^7$Li$^{85}$Rb molecules in their electronic ground state formed by spontaneous decay of weakly bound photoassociated molecules. Beginning with atoms in a dual species magneto-optical trap (MOT), weakly bound molecules are formed in the 4(1) electronic state, which corresponds to the B$^1Π$ state at short range. These molecules spontaneously decay to the electronic ground state and we use resonantly enhanced multiphoton ionization (REMPI) to determine the vibrational population distribution in the electronic ground states after spontaneous emission. Many of the…
The bound states of the fermionic ^3He(2 ^3S_1)+ ^3He(2 ^3P_j)system, where j=0,1,2, are investigated using the recently available ab initio short-range ${}^{1,3,5}Σ^{+}_{g,u}$ and ${}^{1,3,5}Π_{g,u}$ potentials computed by Deguilhem et al. (J. Phys. B: At. Mol. Opt. Phys., 2009, 42, 015102). Single-channel and multichannel calculations have been undertaken in order to investigate the effects of Coriolis and non-adiabatic couplings. The possible experimental observability of the theoretical levels is assessed using criteria based upon the short-range character of each level and their coupling …
We develop the theory for the Adiabatic Raman Photoassociation (ARPA) of ultracold atoms to form ultracold molecules in the presence of scattering resonances. Based on a computational method in which we replace the continuum with a discrete set of "effective modes", we show that the existence of resonances greatly aids in the formation of deeply bound molecular states. We illustrate our general theory by computationally studying the formation of $^{85}$Rb$_2$ molecules from pairs of colliding ultracold $^{85}$Rb atoms. The single-event transfer yield is shown to have a near-unity value for wid…
We theoretically study saturation effects induced by an external static electric field on photoassociation (PA) of a heteronuclear atom pair. A static electric field influences scattering wave-function of two heteronuclear atoms as described in [D. Chakraborty, J. Hazra and B. Deb, J. Phys. B. {\bf 44} 095201 (2011)]. For certain values of electric field strengths there exist anisotropic resonances in ground state scattering leading to a large modification of scattering wave-function at short and intermediate separations where photoassociative Franck-Condon overlap is significant. Photoassocia…
Ultracold photoassociation is typically performed at large internuclear separations, where the scattering wavefunction amplitude is large and Franck-Condon overlap is maximized. Recently, work by this group and others on alkali-metal diatomics has shown that photoassociation can efficiently form molecules at short internuclear distance in both homonuclear and heteronuclear dimers. We propose that this short-range photoassociation is due to excitation near the wavefunction amplitude maximum at the inner wall of the lowest triplet potential. We show that Franck-Condon factors from the highest-en…
We model combined photoassociation and Feshbach resonances in a Bose-Einstein condensate. When the magnetic field is far-off resonance, cross coupling between the two target molecules--enabled by the shared dissociation continuum--leads to an anomalous dispersive shift in the position of laser resonance, as well as unprecedented elimination and enhancement of resonant photoassociation via quantum interference. For off-resonant lasers, a dispersive shift and quantum interference appear similarly in resonant three-body Feshbach losses, except that the Feshbach node is tunable with intensity.
Photoassociation (PA) of ultracold metastable helium to the 2s2p manifold is theoretically investigated using a non-perturbative close-coupled treatment in which the laser coupling is evaluated without assuming the dipole approximation. The results are compared with our previous study [Cocks and Whittingham, Phys. Rev. A 80, 023417 (2009)] that makes use of the dipole approximation. The approximation is found to strongly affect the PA spectra because the photoassociated levels are weakly bound, and a similar impact is predicted to occur in other systems of a weakly bound nature. The inclusion …
We model the formation of stable heteronuclear molecules via pulsed Raman photoassociation of a two-component Bose-Einstein condensate near a strong Feshbach resonance, for both counterintuitive and intuitive pulse sequencing. Compared to lasers alone, weak Raman photoassociation is enhanced by as much as a factor of ten (five) for a counterintuitive (intuitive) pulse sequence, whereas strong Raman photoassociation is barely enhanced at all--regardless of pulse sequence. Stronger intra-atom, molecule, or atom-molecule collisions lead to an expected decrease in conversion efficiency, but strong…
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 observe long-range homonuclear diatomic $nD$ Rydberg molecules photoassociated out of an ultracold gas of $^{87}$Rb atoms for 34$\le n \le$40. The measured ground-state binding energies of $^{87}$Rb$(nD-5S_{1/2})$ molecular states are larger than those of their $^{87}$Rb$(nS-5S_{1/2})$ counterparts, showing the dependence of the molecular bond on the angular momentum of the Rydberg atom. We exhibit the transition of $^{87}$Rb$(nD-5S_{1/2})$ molecules from a molecular-binding-dominant regime at low $n$ to a fine-structure-dominant regime at high $n$ [akin to Hund's cases (a) and (c), respect…
We report on the anomalously high line strength of a single rotational level in the ultracold photoassociation of two 85Rb atoms to form 85Rb2. The v' = 111, J' = 5 level belongs to the Hund's case (c) 2 (0g+) state, which correlates to the Hund's case (a) 2 1 Σg+ state. Its strength is caused by coupling with a very near-resonant long-range state. The long-range component is the energetically degenerate v' = 155, J' = 5 level of the case (c) 2 (1g)$ state, correlating to the case (a) 1 1 Πg state. The line strength is enhanced by an order of magnitude through this coupling, relative to nearby…
We describe the realization of a dc electric-field trap for ultracold polar molecules, the thin-wire electrostatic trap (TWIST). The thin wires that form the electrodes of the TWIST allow us to superimpose the trap onto a magneto-optical trap (MOT). In our experiment, ultracold polar NaCs molecules in their electronic ground state are created in the MOT via photoassociation, achieving a continuous accumulation in the TWIST of molecules in low-field seeking states. Initial measurements show that the TWIST trap lifetime is limited only by the background pressure in the chamber.
We investigate the dynamical process of optically trapped X$^{1}$$Σ$$^{+}$ (v" = 0) state $^{85}$Rb$^{133}$Cs molecules distributing in J" = 1 and J" = 3 rotational states. The considered molecules, formed from short-range photoassociation of mixed cold atoms, are subsequently confined in a crossed optical dipole trap. Based on a phenomenological rate equation, we provide a detailed study of the dynamics of $^{85}$Rb$^{133}$Cs molecules during the loading and holding processes. The inelastic collisions of $^{85}$Rb$^{133}$Cs molecules in the X$^{1}$$Σ$$^{+}$ (v" = 0, J" = 1 and J" = 3) states …
With ultracold $^{88}$Sr in a 1D magic wavelength optical lattice, we performed narrow line photoassociation spectroscopy near the $^1$S$_0 - ^3$P$_1$ intercombination transition. Nine least-bound vibrational molecular levels associated with the long-range $0_u$ and $1_u$ potential energy surfaces were measured and identified. A simple theoretical model accurately describes the level positions and treats the effects of the lattice confinement on the line shapes. The measured resonance strengths show that optical tuning of the ground state scattering length should be possible without significan…
We have produced ultracold heteronuclear KRb molecules by the process of photoassociation in a two-species magneto-optical trap. Following decay of the photoassociated KRb*, the molecules are detected using two-photon ionization and time-of-flight mass spectroscopy of KRb$^+$. A portion of the metastable triplet molecules thus formed are magnetically trapped. Photoassociative spectra down to 91 cm$^{-1}$ below the K(4$s$) + Rb (5$p_{1/2}$) asymptote have been obtained. We have made assignments to all eight of the attractive Hund's case (c) KRb* potential curves in this spectral region.
Photoassociation of ultracold atoms induced by chirped picosecond pulses is analyzed in a non-perturbative treatment by following the wavepackets dynamics on the ground and excited surfaces. The initial state is described by a Boltzmann distribution of continuum scattering states. The chosen example is photoassociation of cesium atoms at temperature T=54 $μK$ from the $a^3 Σ_u^+(6s,6s)$ continuum to bound levels in the external well of the $0_g^-(6s+6p_{3/2})$ potential. We study how the modification of the pulse characteristics (carrier frequency, duration, linear chirp rate and intensity) ca…
We discuss the production of ultracold molecules in their electronic ground state by photoassociation employing electronically excited states with ion-pair character and strong spin-orbit interaction. A short photoassociation laser pulse drives a non-resonant three-photon transition for alkali atoms colliding in their lowest triplet state. The excited state wave packet is transferred to the ground electronic state by a second laser pulse, driving a resonant two-photon transition. After analyzing the transition matrix elements governing the stabilization step, we discuss the efficiency of popul…
We report on the production of ultracold heteronuclear YbLi* molecules in a dual-species magneto-optical trap by photoassociation (PA). The formation of the electronically excited molecules close to dissociation was observed by trap loss spectroscopy. We find 4 rovibrational states within a range of $250\,$GHz below the Yb($^1S_0$) + Li($^2P_{1/2}$) asymptote and observe isotopic PA line shifts in mixtures of $^6$Li with $^{174}$Yb, $^{172}$Yb, and $^{176}$Yb. We also describe our theoretical ab-initio calculation for the relevant electronic potentials and utilize it to analyze and identify th…
