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 ground state. Repetition of many pump-dump sequences together with collisional relaxation allows for accumulation of molecules in v=0.
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 demonstrate the production of ultracold polar RbCs molecules in their vibronic ground state, via photoassociation of laser-cooled atoms followed by a laser-stimulated state transfer process. The resulting sample of $X ^1Σ^+ (v=0)$ molecules has a translational temperature of $\sim100 μ$K and a narrow distribution of rotational states. With the method described here it should be possible to produce samples even colder in all degrees of freedom, as well as other bi-alkali species.
Using resonance-enhanced two-photon ionization, we detect ultracold, ground-state RbCs molecules formed via photoassociation in a laser-cooled mixture of 85Rb and 133Cs atoms. We obtain extensive bound-bound excitation spectra of these molecules, which provide detailed information about their vibrational distribution, as well as spectroscopic data on the RbCs ground a^3Σ^+ and excited (2)^3Σ^+, (1)^1Πstates. Analysis of this data allows us to predict strong transitions from observed excited levels to the absolute vibronic ground state of RbCs, potentially allowing the production of stable, ult…
Femtochemistry techniques have been instrumental in accessing the short time scales necessary to probe transient intermediates in chemical reactions. Here we take the contrasting approach of prolonging the lifetime of an intermediate by preparing reactant molecules in their lowest ro-vibronic quantum state at ultralow temperatures, thereby drastically reducing the number of exit channels accessible upon their mutual collision. Using ionization spectroscopy and velocity-map imaging of a trapped gas of potassium-rubidium molecules at a temperature of 500~nK, we directly observe reactants, interm…
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 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…
The study of low density, ultracold atomic Fermi gases is a promising avenue to understand fermion superfluidity from first principles. One technique currently used to bring Fermi gases in the degenerate regime is sympathetic cooling through a reservoir made of an ultracold Bose gas. We discuss a proposal for trapping and cooling of two-species Fermi-Bose mixtures into optical dipole traps made from combinations of laser beams having two different wavelengths. In these bichromatic traps it is possible, by a proper choice of the relative laser powers, to selectively trap the two species in such…
It has been roughly three decades since laser cooling techniques produced ultracold atoms, leading to rapid advances in a vast array of fields. Unfortunately laser cooling has not yet been extended to molecules because of their complex internal structure. However, this complexity makes molecules potentially useful for many applications. For example, heteronuclear molecules possess permanent electric dipole moments which lead to long-range, tunable, anisotropic dipole-dipole interactions. The combination of the dipole-dipole interaction and the precise control over molecular degrees of freedom …
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 …
Harnessing the potential wide-ranging quantum science applications of molecules will require control of their interactions. Here, we use microwave radiation to directly engineer and tune the interaction potentials between ultracold calcium monofluoride (CaF) molecules. By merging two optical tweezers, each containing a single molecule, we probe collisions in three dimensions. The correct combination of microwave frequency and power creates an effective repulsive shield, which suppresses the inelastic loss rate by a factor of six, in agreement with theoretical calculations. The demonstrated mic…
We report on the creation of ultracold 84Sr2 molecules in the electronic ground state. The molecules are formed from atom pairs on sites of an optical lattice using stimulated Raman adiabatic passage (STIRAP). We achieve a transfer efficiency of 30% and obtain 4x10^4 molecules with full control over the external and internal quantum state. STIRAP is performed near the narrow 1S0-3P1 intercombination transition, using a vibrational level of the 0u potential as intermediate state. In preparation of our molecule association scheme, we have determined the binding energies of the last vibrational l…
Orbital degree of freedom plays an important role in understanding exotic phenomena of strongly correlated materials. We study strongly correlated ultracold bosonic gases coupled to a high-finesse cavity, pumped by a blue-detuned laser in the transverse direction. Based on an extended Bose-Hubbard model with parameters adapted to recent experiments, we find that by tuning the reflection of pump laser, atoms can be selectively transferred to the odd-parity $p$-orbital, or to even-parity $d$-orbital band of a two-dimensional square lattice, accompanied with cavity-photon excitations. By interact…
We perform one- and two-photon high resolution spectroscopy on ultracold samples of RbCs Feshbach molecules with the aim to identify a suitable route for efficient ground-state transfer in the quantum-gas regime to produce quantum gases of dipolar RbCs ground-state molecules. One-photon loss spectroscopy allows us to probe deeply bound rovibrational levels of the mixed excited (A1Σ+ - b3Π0) 0+ molecular states. Two-photon dark state spectroscopy connects the initial Feshbach state to the rovibronic ground state. We determine the binding energy of the lowest rovibrational level |v"=0,J"=0> of t…
We perform magnetically-assisted Sisyphus laser cooling of the triatomic free radical strontium monohydroxide (SrOH). This is achieved with principal optical cycling in the rotationally closed $P\left(N"=1\right)$ branch of either the $\tilde{X}^{2}Σ^{+}\left(000\right)\leftrightarrow\tilde{A}^{2}Π_{1/2}\left(000\right)$ or the $\tilde{X}^{2}Σ^{+}\left(000\right)\leftrightarrow\tilde{B}^{2}Σ^{+}\left(000\right)$ vibronic transitions. Molecules lost into the excited vibrational states during the cooling process are repumped back through the $\tilde{B}\left(000\right)$ state for both the $\left(…
We report the production of ultracold RbCs molecules in the rovibronic ground state, i.e., $X^1Σ^+ (v=0, J=0)$, by short-range photoassociation to the $2^3Π_{0}$ state followed by spontaneous emission. We use narrowband depletion spectroscopy to probe the distribution of rotational levels formed in the $X ^1Σ^+(v=0)$ state. We conclude, based on selection rules, that the primary decay route to $X ^1Σ^+(v=0)$ is a two-step cascade decay that leads to as much as $33\%$ branching into the $J=0$ rotational level. The experimental simplicity of our scheme opens up the possibility of easier access t…
We present a general and highly efficient scheme for performing narrow-band Raman transitions between molecular vibrational levels using a coherent train of weak pump-dump pairs of shaped ultrashort pulses. The use of weak pulses permits an analytic description within the framework of coherent control in the perturbative regime, while coherent accumulation of many pulse pairs enables near unity transfer efficiency with a high spectral selectivity, thus forming a powerful combination of pump-dump control schemes and the precision of the frequency comb. The concept is presented analytically and …
Electron lattice potentials for ultracold atoms using circular Rydberg orbitals
Max-Planck Institut für Physik komplexer Systeme（马克斯·普朗克复杂系统物理研究所）；Joint Quantum Centre (JQC) Durham-Newcastle, Department of Chemistry, Durham University（杜伦大学化学系）；Physikalisches Institut and Center for Integrated Quantum Science and Technology, Universität Stuttgart（斯图加特大学第五物理研究所及综合量子科学技术中心）；Department of Physics and Astronomy, Purdue University（普渡大学物理与天文学系）
In the vicinity of a Feshbach resonance, a system of ultracold atoms on an optical lattice undergoes rich physical transformations which involve molecule formation and hopping of molecules on the lattice and thus goes beyond a single-band Hubbard model description. We propose to probe the behavior of this system with a harmonic modulation of the magnetic field, and thus of the scattering length, across the Feshbach resonance, as an alternative to lattice-depth modulation spectroscopy. In the regime in which the single-band Hubbard model is still valid, we provide simulation data for this type …
We study theoretically the interaction between two species of ultracold atoms confined into two layers of a finite separation, and demonstrate the existence of new types of confinement-induced interlayer bound and quasi-bound molecules: these novel exciton-like interlayer molecules appear for both positive and negative scattering lengths, and exist even for layer separations many times larger than the interspecies scattering length. The lifetime of the quasi-bound molecules grows exponentially with increasing layer separation, and they can therefore be observed in simple shaking experiments, a…
Continuous wave (CW) lasers are the enabling technology for producing ultracold atoms and molecules through laser cooling and trapping. The resulting pristine samples of slow moving particles are the de facto starting point for both fundamental and applied science when a highly-controlled quantum system is required. Laser cooled atoms have recently led to major advances in quantum information, the search to understand dark energy, quantum chemistry, and quantum sensors. However, CW laser technology currently limits laser cooling and trapping to special types of elements that do not include hig…
