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"=6. The spin-orbit interaction is responsible for both optical pathways. Therefore, those excited state levels that have the largest bound-to-bound transition moments to deeply bound ground state levels also exhibit a sufficient photoassociation probability, comparable to that of the lowest weakly bound excited state level previously observed by Zelevinsky et al. [Phys. Rev. Lett. 96, 203201 (2006)]. Our study paves the way for an efficient photoassociative production of Sr_2 molecules in ground state levels suitable for experiments testing the electron-to-proton mass ratio.
We report on the first observation of photoassociation near the ${}^2 S _\frac 1 2 + {}^3P_1$-asymptote in a mixture of ${}^{87}$Rb and ${}^{170}$Yb. In a search spanning binding energies between 0.1 GHz and 11 GHz, a single pair of interspecies PA resonances is detected around 3.1 GHz. These resonances are characterized by extracting PA rates, binding energies and Zeeman shift coefficients. Using one of these resonances, 2-photon-photoassociaton is performed, improving on previous measurements of the binding energies of the two least bound states in the electronic ground state and demonstrati…
The properties of photoassociation (PA) spectra near the intercombination line (the weak transition between $^{1}S_{0}$ and $^{3}P_{1}$ states) of group II atoms are theoretically investigated. As an example we have carried out a calculation for Calcium atoms colliding at ultra low temperatures of 1 mK, 1 $μ$K, and 1 nK. Unlike in most current photoassociation spectroscopy the Doppler effect can significantly affect the shape of the investigated lines. Spectra are obtained using Ca--Ca and Ca--Ca$^*$ short-range {\it ab initio} potentials and long-range van der Waals and resonance dipole poten…
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…
The properties of bosonic Ytterbium photoassociation spectra near the intercombination transition $^{1}S_{0}$--$^{3}P_{1}$ are studied theoretically at ultra low temperatures. We demonstrate how the shapes and intensities of rotational components of optical Feshbach resonances are affected by mass tuning of the scattering properties of the two colliding ground state atoms. Particular attention is given to the relationship between the magnitude of the scattering length and the occurrence of shape resonances in higher partial waves of the van der Waals system. We develop a mass scaled model of t…
We demonstrate Feshbach optimized photoassociation (FOPA) into the $0_{g}^{-} (5$S$_{1/2}+5$P$_{1/2}$) state in $^{85}$Rb$_{2}$. FOPA uses the enhancement of the amplitude of the initial atomic scattering wave function due to a Feshbach resonance to increase the molecular formation rate from photoassociation. We observe three vibrational levels, $v=$127, 140, and 150, with previously unmeasured binding energies of 256, 154, and 96 cm$^{-1}$. We measure the frequency, central magnetic field position, and magnetic field width of each Feshbach resonance. Our findings experimentally confirm that t…
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.
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…
Photoassociation of two ultracold rubidium atoms and the subsequent formation of stable molecules in the singlet ground and lowest triplet states is investigated theoretically. The method employs laser pulses inducing transitions via excited states correlated to the $5S+5P_{1/2}$ asymptote. Weakly bound molecules in the singlet ground or lowest triplet state can be created by a single pulse while the formation of more deeply bound molecules requires a two-color pump-dump scenario. More deeply bound molecules in the singlet ground or lowest triplet state can be produced only if efficient mechan…
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 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…
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…
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 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…
We present precise measurements of the optical Feshbach resonances (OFRs) of $^{174}$Yb atoms for the intercombination transition. We measure the photoassociation (PA) spectra of a pure $^{174}$Yb Bose-Einstein condensate, and determine the dependence of OFRs to PA laser intensities and frequencies for four least bound vibrational levels near the intercombination transition. We confirm that our measurements are consistent with the temporal decay of a BEC subjected to a PA beam in the vicinity of the fourth vibrational level from the dissociation limit.
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 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^+_…
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…
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 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 $a^{3}Σ^{+} (v" = 7 - 13)$, $3^{3} Π(v'_…
Using a non-selective broadband detection scheme we discovered an efficient mechanism of formation of ultracold Cs$_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 c…
Optical Feshbach resonances [Phys. Rev. Lett. 94, 193001 (2005)] and pump-dump photoassociation with short laser pulses [Phys. Rev. A 73, 033408 (2006)] have been proposed as means to coherently form stable ultracold alkali dimer molecules. In an optical Feshbach resonance, the intensity and possibly frequency of a cw laser are ramped up linearly followed by a sudden switch-off of the laser. This is applicable to tightly trapped atom pairs. In short-pulse photoassociation, the pump pulse forms a wave-packet in an electronically excited state. The ensuing dynamics carry the wave-packet to short…
We report photoassociative spectroscopy of $^{88}$Sr$_2$ in a magneto-optical trap operating on the ${^1S_0}\to{^3P_1}$ intercombination line at 689 nm. Photoassociative transitions are driven with a laser red-detuned by 600-2400 MHz from the ${^1S_0}\to{^1P_1}$ atomic resonance at 461 nm. Photoassociation takes place at extremely large internuclear separation, and the photoassociative spectrum is strongly affected by relativistic retardation. A fit of the transition frequencies determines the ${^1P_1}$ atomic lifetime ($τ=5.22 \pm 0.03$ ns) and resolves a discrepancy between experiment and re…
We demonstrate that a near-dissociation photoassociation resonance can be used to create a deeply bound molecular sample of ultracold NaCs. To probe the resulting vibrational distribution of the sample, we use a new technique that can be applied to any ultracold molecular system. We utilize a tunable pulsed dye laser to produce efficient spectroscopic scans ($\sim700$ cm$^{-1}$ at a time) in which we observe the $1^{1} Σ^{+}\rightarrow 2^{1}Σ^{+}-2^{3}Π$ vibrational progression, as well as the dissociation limit to the Cs 6$^{2}$P$_{3/2}$ asymptote. We assign $1^{1} Σ^{+}$$(\emph{v}$ = 4, 5, 6…
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…
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 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…
Using new experimental measurements of photoassociation resonances near the $^1\mathrm{S}_0 \rightarrow \phantom{ }^3\mathrm{P}_1$ intercombination transition in $^{84}$Sr and $^{86}$Sr, we present an updated study into the mass-scaling behavior of bosonic strontium dimers. A previous mass-scaling model [Borkowski et al., Phys. Rev. A 90, 032713 (2014)] was able to incorporate a large number of photoassociation resonances for $^{88}$Sr, but at the time only a handful of resonances close to the dissociation limit were known for $^{84}$Sr and $^{86}$Sr. In this work, we perform a more thorough m…
We have produced large samples of ultracold $^{88}$Sr$_2$ molecules in the electronic ground state in an optical lattice. The molecules are bound by 0.05 cm$^{-1}$ and are stable for several milliseconds. The fast, all-optical method of molecule creation via intercombination line photoassociation relies on a near-unity Franck-Condon factor. The detection uses a weakly bound vibrational level corresponding to a very large dimer. This is the first of two steps needed to create Sr$_2$ in the absolute ground quantum state. Lattice-trapped Sr$_2$ is of interest to frequency metrology and ultracold …
We investigate the possibility of forming deeply bound ultracold RbCs molecules by a two-color photoassociation experiment. We compare the results with those for Rb_2 in order to understand the characteristic differences between heteronuclear and homonuclear molecules. The major differences arise from the different long-range potential for excited states. Ultracold 85Rb and 133Cs atoms colliding on the X^1Sigma+ potential curve are initially photoassociated to form excited RbCs molecules in the region below the Rb(5S) + Cs(6P_1/2) asymptote. We explore the nature of the Omega=0^+ levels in thi…
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 report our spectroscopic studies of the $d \ ^3Π$ state of ultra-cold $^7$Li$^{85}$Rb using resonantly-enhanced multi-photon ionization and depletion spectroscopy with bound-to-bound transitions originating from the metastable $a \ ^3Σ^+$ state. We evaluate the potential of this state for use as the intermediate state in a STIRAP transfer scheme from triplet Feshbach LiRb molecules to the $X \ ^1Σ^+$ ground state, and find that the lowest several vibrational levels possess the requisite overlap with initial and final states, as well as convenient energies. Using depletion measurements, we m…
We propose an improved photoassociation scheme to produce ultracold molecules in their vibronic ground state for the generic case where non-adiabatic effects facilitating transfer to deeply bound levels are absent. Formation of molecules is achieved by short laser pulses in a Raman-like pump-dump process where an additional near-infrared laser field couples the excited state to an auxiliary state. The coupling due to the additional field effectively changes the shape of the excited state potential and allows for efficient population transfer to low-lying vibrational levels of the electronic gr…
We spectroscopically investigate the hyperfine, rotational and Zeeman structure of the vibrational levels $\text{v}'=0$, $7$, $13$ within the electronically excited $c^3Σ_g^+$ state of $^{87}\text{Rb}_2$ for magnetic fields of up to $1000\,\text{G}$. As spectroscopic methods we use short-range photoassociation of ultracold Rb atoms as well as photoexcitation of ultracold molecules which have been previously prepared in several well-defined quantum states of the $a^3Σ_u^+$ potential. As a byproduct, we present optical two-photon transfer of weakly bound Feshbach molecules into $a^3Σ_u^+$, $\tex…
We have studied the effect of resonant electronic state coupling on the formation of ultracold ground-state $^{85}$Rb$_2$. Ultracold Rb$_2$ molecules are formed by photoassociation (PA) to a coupled pair of $0_u^+$ states, $0_u^+(P_{1/2})$ and $0_u^+(P_{3/2})$, in the region below the $5S+5P_{1/2}$ limit. Subsequent radiative decay produces high vibrational levels of the ground state, $X ^1Σ_g^+$. The population distribution of these $X$ state vibrational levels is monitored by resonance-enhanced two-photon ionization through the $2 ^1Σ_u^+$ state. We find that the populations of vibrational l…
Photoassociation (PA) is a powerful technique to synthesize molecules directly and continuously from cold and ultracold atoms into deeply bound molecular states. In freespace, however, PA efficiency is constrained by the number of spontaneous decay channels linking the initial excited molecular state to a sea of final (meta)stable rovibronic levels. Here, we propose a novel scheme based on molecules strongly coupled to a guided photonic mode in a photonic crystal waveguide that turns PA into a powerful tool for near deterministic formation of ultracold molecules in their ground rovibrational l…
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 investigate the formation of weakly bound, electronically excited, heteronuclear 6Li40K* molecules by single-photon photoassociation in a magneto-optical trap. We performed trap loss spectroscopy within a range of 325 GHz below the Li(2S_(1/2))+K(4P_(3/2)) and Li(2S_(1/2))+K(4P_(1/2)) asymptotic states and observed more than 60 resonances, which we identify as rovibrational levels of 7 of 8 attractive long-range molecular potentials. The long-range dispersion coefficients and rotational constants are derived. We find large molecule formation rates of up to ~3.5x10^7s^(-1), which are shown t…
