We report here on the production of an ultracold gas of tightly bound Rb2 molecules in the ro-vibrational triplet ground state, close to quantum degeneracy. This is achieved by optically transferring weakly bound Rb2 molecules to the absolute lowest level of the ground triplet potential with a transfer efficiency of about 90%. The transfer takes place in a 3D optical lattice which traps a sizeable fraction of the tightly bound molecules with a lifetime exceeding 200 ms.
We present a rigorous study of vibrational relaxation in p-H2 + p-H2 collisions at cold and ultracold temperatures and identify an efficient mechanism of ro-vibrational energy transfer. If the colliding molecules are in different rotational and vibrational levels, the internal energy may be transferred between the molecules through an extremely state-selective process involving simultaneous conservation of internal energy and total rotational angular momentum. The same transition in collisions of distinguishable molecules corresponds to the rotational energy transfer from one vibrational state…
Sending multiple messages on qubits encoded in different vibrational modes of cold atoms or ions along a transmission waveguide requires to merge first and then separate the modes at input and output ends. Similarly, different qubits can be stored in the modes of a trap and be separated later. We design the fast splitting of a harmonic trap into an asymmetric double well so that the initial ground vibrational state becomes the ground state of one of two final wells, and the initial first excited state becomes the ground state of the other well. This might be done adiabatically by slowly deform…
The coupling of internal electronic excitations to vibrational modes of the external motion of ultracold atoms in an optical lattice is studied here in using a perturbation expansion in small atomic displacements. In the Mott insulator case with one atom per site, the resonance dipole-dipole coupling between neighboring sites can induce emission and absorption of vibrational quanta. Within a cavity in the strong exciton-photon coupling regime such coupling results in polariton-vibration interactions, which create a significant thermalization mechanism for polaritons toward their minimum energy…
We theoretically explore photoassociation by Adiabatic Passage of two colliding cold ^{85}Rb atoms in an atomic trap to form an ultracold Rb_2 molecule. We consider the incoherent thermal nature of the scattering process in a trap and show that coherent manipulations of the atomic ensemble, such as adiabatic passage, are feasible if performed within the coherence time window dictated by the temperature, which is relatively long for cold atoms. We show that a sequence of ~2*10^7 pulses of moderate intensities, each lasting ~750 ns, can photoassociate a large fraction of the atomic ensemble at t…
We propose a process to convert ultracold metastable Cs$_2$ molecules in their lowest triplet state into (singlet) ground state molecules in their lowest vibrational levels. Molecules are first pumped into an excited triplet state, and the triplet-singlet conversion is facilitated by a two-step spontaneous decay through the coupled $A^{1}Σ_{u}^{+} \sim b ^{3}Π_{u}$ states. Using spectroscopic data and accurate quantum chemistry calculations for Cs$_2$ potential curves and transition dipole moments, we show that this process has a high rate and competes favorably with the single-photon decay ba…
Precision measurements with ultracold molecules require development of robust and sensitive techniques to produce and interrogate the molecules. With this goal, we theoretically analyze factors that affect frequency measurements between rovibrational levels of the Sr$_2$ molecule in the electronic ground state. This measurement can be used to constrain the possible time variation of the proton-electron mass ratio. Sr$_2$ is expected to be a strong candidate for achieving high precision due to the spinless nature and ease of cooling and perturbation-free trapping of Sr \cite{Zelevinsky2008}. Th…
In recent experiments on ultracold matter, molecules have been produced from ultracold atoms by photoassociation, Feshbach resonances, and three-body recombination. The created molecules are translationally cold, but vibrationally highly excited. This will eventually lead them to be lost from the trap due to collisions. We propose shaped laser pulses to transfer these highly excited molecules to their ground vibrational level. Optimal control theory is employed to find the light field that will carry out this task with minimum intensity. We present results for the sodium dimer. The final targe…
We present the results of an experimental and theoretical study of the electronically excited $\tripletex$ state of $^{87}$Rb$_2$ molecules. The vibrational energies are measured for deeply bound states from the bottom up to $v'=15$ using laser spectroscopy of ultracold Rb$_2$ Feshbach molecules. The spectrum of each vibrational state is dominated by a 47\,GHz splitting into a $\cog$ and $\clg$ component caused mainly by a strong second order spin-orbit interaction. Our spectroscopy fully resolves the rotational, hyperfine, and Zeeman structure of the spectrum. We are able to describe to first…
We have produced ultracold heteronuclear YbRb$^*$ molecules in a combined magneto-optical trap by photoassociation. The formation of electronically excited molecules close to the dissociation limit was observed by trap loss spectroscopy in mixtures of $^{87}$Rb with $^{174}$Yb and $^{176}$Yb. The molecules could be prepared in a series of vibrational levels with resolved rotational structure, allowing for an experimental determination of the long-range potential in the electronically excited state.
It is found that all the {\em singlet orbital pairing} instabilities are {\em absent} in a class of spin-polarized multi-orbital systems with quadratic band touching, which opens the way for {\em triplet orbital pairing} order. The ground states are found to be {\em non-Abelian} states with p-wave orbital pairing in checkerboard (away from 1/2 filling) and kagome (above 1/3 filling) lattices with {\em isotropic} attractive interaction which can be realized in ultracold multi-orbital optical lattices. The special property of such systems is generalized to more classes of multi-orbital systems, …
The formation of ultracold molecules via stimulated emission followed by a radiative deexcitation cascade in the presence of a static electric field is investigated. By analyzing the corresponding cross sections, we demonstrate the possibility to populate the lowest rotational excitations via photoassociation. The modification of the radiative cascade due to the electric field leads to narrow rotational state distributions in the vibrational ground state. External fields might therefore represent an additional valuable tool towards the ultimate goal of quantum state preparation of molecules.
We demonstrate the conversion of cold Cs_{2} molecules initially distributed over several vibrational levels of the lowest triplet state a^{3}Σ_{u}^{+} into the singlet ground state X^{1}Σ_{g}^{+}. This conversion is realized by a broadband laser exciting the molecules to a well-chosen state from which they may decay to the singlet state throug\textcolor{black}{h two sequential single-photon emission steps: Th}e first photon populates levels with mixed triplet-singlet character, making possible a second spontaneous emission down to several vibrational levels of the X^{1}Σ_{g}^{+} states. By ad…
We create fermionic dipolar $^{23}$Na$^6$Li molecules in their triplet ground state from an ultracold mixture of $^{23}$Na and $^6$Li. Using magneto-association across a narrow Feshbach resonance followed by a two-photon STIRAP transfer to the triplet ground state, we produce $3\,{\times}\,10^4$ ground state molecules in a spin-polarized state. We observe a lifetime of $4.6\,\text{s}$ in an isolated molecular sample, approaching the $p$-wave universal rate limit. Electron spin resonance spectroscopy of the triplet state was used to determine the hyperfine structure of this previously unobserve…
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 explore the electroluminescence efficiency for a quantum mechanical model of a large number of molecular emitters embedded in an optical microcavity. We characterize the circumstances under which a microcavity enhances harvesting of triplet excitons via reverse intersystem-crossing (R-ISC) into singlet populations that can emit light. For that end, we develop a time-local master equation in a variationally optimized frame which allows for the exploration of the population dynamics of chemically relevant species in different regimes of emitter coupling to the condensed phase vibrational bath…
Starting from an ultracold sample of ground-state $^{23}$Na$^{87}$Rb molecules, we investigate the lowest ro-vibrational level of the $b^3Π$ state with high resolution laser spectroscopy. This electronic spin-forbidden $X^1Σ^+ \leftrightarrow b^3Π$ transition features a nearly diagonal Franck-Condon factor and has been proposed useful for probing and manipulating the ultracold molecular gas. We measure the transition strength directly by probing the ac Stark shift induced by near resonance light and determine the total excited-state spontaneous emission rate by observing the loss of molecules.…
We investigate cooperative phenomena and superradiance for vibrational transitions in polar molecule spectroscopy when a high optical-depth (OD) sample is studied. Such cooperativity comes from the build-up of inter-particle coherence through dipole-dipole interactions and leads to the speed-up of decay process. We compare our calculation to recent work [Deiglmayr et al., Eur. Phys. J. D 65, 99 (2011)] and find very good agreement, suggesting that superradiant effects need to be included in a wide variety of ultracold molecule setups including vibrational and rotational states.
We have obtained accurate ab initio quartet potentials for the diatomic metastable triplet helium + alkali-metal (Li, Na, K, Rb) systems, using all-electron restricted open-shell coupled cluster singles and doubles with noniterative triples corrections [CCSD(T)] calculations and accurate calculations of the long-range $C_6$ coefficients. These potentials provide accurate ab initio quartet scattering lengths, which for these many-electron systems is possible, because of the small reduced masses and shallow potentials that results in a small amount of bound states. Our results are relevant for u…
We have investigated the ultracold interspecies scattering properties of metastable triplet He and Rb. We performed state-of-the-art ab initio calculations of the relevant interaction potential, and measured the interspecies elastic cross section for an ultracold mixture of metastable triplet $^4$He and $^{87}$Rb in a quadrupole magnetic trap at a temperature of 0.5 mK. Our combined theoretical and experimental study gives an interspecies scattering length $a_{4+87}=+17^{+1}_{-4}$ $a_0$, which prior to this work was unknown. More general, our work shows the possibility of obtaining accurate sc…
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 …
Photoassociation of ultracold atoms is shown to lead to alignment of the product molecules along the excitation laser polarization axis. We theoretically investigate pulsed photoassociation of $^{87}Rb$ atoms into a specific weakly-bound level of the a $^3Σ_u^+$ metastable electronic state and find both stationary and time-dependent field-free alignment. Although a transform-limited pulse yields significant alignment, a frequency-chirped pulse dramatically enhances the molecular formation rate at the cost of a slight decrease in the alignment. Employing multiple pulses synchronized with the vi…
We report results for reaction and vibrational quenching of the collision D with para-H$_2$($v,j=0$) and ortho-H$_2$($v,j=1$) at cold and ultracold temperatures. We investigate the effect of nuclear spin symmetry for barrier dominated processes ($0\le v\le 4$) and for one barrierless case ($v=5$). We find resonant structures for energies in the range corresponding to 0.01--10 K, which depend on the nuclear spin of H$_2$, arising from contributions of specific partial waves. We discuss the implications on the results in this benchmark system for ultracold chemistry.
Ultracold LiCs molecules in the absolute ground state X$^1Σ^+$, v"=0, J"=0 are formed via a single photo-association step starting from laser-cooled atoms. The selective production of v"=0, J"=2 molecules with a 50-fold higher rate is also demonstrated. The rotational and vibrational state of the ground state molecules is determined in a setup combining depletion spectroscopy with resonant-enhanced multi-photon ionization time-of-flight spectroscopy. Using the determined production rate of up to 5x10^3 molecules/s, we describe a simple scheme which can provide large samples of externally and i…
Ultracold ground-state molecules can be formed from ultracold atoms via photoassociation followed by a spontaneous emission process. Typically, the molecular products are distributed over a range of final states. Here, we propose to use an optical cavity with high cooperativity to selectively enhance the population of a pre-determined final state by controlling the spontaneous emission. During this process, a photon will be emitted into the cavity mode. Detection of this photon heralds a single reaction. We discuss the efficiency and the dynamics of cavity-assisted molecule formation in the fr…
A first principles study of the dynamics of $^6$Li($^{2}$S) + $^6$Li$^{174}$Yb($^2Σ^+$)$ \to ^6$Li$_2(^1Σ^+$) + $^{174}$Yb($^1$S) reaction is presented at cold and ultracold temperatures. The computations involve determination and analytic fitting of a three-dimensional potential energy surface for the Li$_2$Yb system and quantum dynamics calculations of varying complexities, ranging from exact quantum dynamics within the close-coupling scheme, to statistical quantum treatment, and universal models. It is demonstrated that the two simplified methods yield zero-temperature limiting reaction rat…
We report the observation and analysis of the $3\,^3Π_Ω$ double-minimum electronic excited state of $^{39}$K$^{85}$Rb. The spin-orbit components ($0^{+}, 0^{-}, 1$ and 2) of this state are investigated based on potentials developed from the available \emph{ab initio} potential curves. We have assigned the vibrational levels $v'=2-11$ of the $3\,^3Π_{1,2}$ potentials and $v'=2-12$ of the $3\,^3Π_{0^{+/-}}$ potential. We compare our experimental observations of the $3\,^3Π_Ω$ state with predictions based on theoretical potentials. The observations are based on resonance enhanced multiphoton ioni…
We report on the creation of bosonic NaCs molecules in their absolute rovibrational ground state via stimulated Raman adiabatic passage. We create ultracold gases with up to 22,000 dipolar NaCs molecules at a temperature of 300(50) nK and a peak density of $1.0(4) \times 10^{12}$ cm$^{-3}$. We demonstrate comprehensive quantum state control by preparing the molecules in a specific electronic, vibrational, rotational, and hyperfine state. Employing the tunability and strength of the permanent electric dipole moment of NaCs, we induce dipole moments of up to 2.6 D. Dipolar systems of NaCs molecu…
Trapping ultracold molecules in conservative traps is essential for applications -- such as quantum state-controlled chemistry, quantum simulations, and quantum information processing. These applications require high densities or phase-space densities. We report magnetic trapping of NaLi molecules in the triplet ground state at high density ($\approx 10^{11} \; \rm{cm}^{-3}$) and ultralow temperature ($\approx 1\;{\rm μK}$). Magnetic trapping at these densities allows studies on both atom-molecule and molecule-molecule collisions in the ultracold regime in the absence of trapping light, which …
Recently it has been shown that pairs of atoms can form metastable bonds due to non-conservative forces induced by dissipation [Lemeshko&Weimer, Nature Comm. 4, 2230 (2013)]. Here we study the dynamics of interaction-induced coherent population trapping - the process responsible for the formation of dissipatively bound molecules. We derive the effective dissipative potentials induced between ultracold atoms by laser light, and study the time evolution of the scattering states. We demonstrate that binding occurs on short timescales of ~10 microseconds, even if the initial kinetic energy of the …
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 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…
Cooling the rotation and the vibration of molecules by broadband light sources was possible for trapped molecular ions or ultracold molecules. Because of a low power spectral density, the cooling timescale has never fell below than a few milliseconds. Here we report on rotational and vibrational cooling of a supersonic beam of barium monofluoride molecules in less than 440 $μ$s. Vibrational cooling was optimized by enhancing the spectral power density of a semiconductor light source at the underlying molecular transitions allowing us to transfer all the populations of $v''=1-3$ into the vibrat…
We study ultracold long-range collisions of heteronuclear alkali-metal dimers with a reservoir gas of alkali-metal Rydberg atoms in a two-photon laser excitation scheme. In a low density regime where molecules remain outside the Rydberg orbits of the reservoir atoms, we show that the two-photon photoassociation (PA) of the atom-molecule pair into a long-range bound trimer state is efficient over a broad range of atomic Rydberg channels. As a case study, we obtain the PA lineshapes for the formation of trimers composed of KRb molecules in the rovibrational ground state and excited Rb atoms in t…
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 have calculated the isotropic $C\_6$ coefficients characterizing the long-range van der Waals interaction between two identical heteronuclear alkali-metal diatomic molecules in the same arbitrary vibrational level of their ground electronic state $X^1Σ^+$. We consider the ten species made up of $^7$Li, $^{23}$Na, $^{39}$K, $^{87}$Rb and $^{133}$Cs. Following our previous work [M.~Lepers \textit{et.~al.}, Phys.~Rev.~A \textbf{88}, 032709 (2013)] we use the sum-over-state formula inherent to the second-order perturbation theory, composed of the contributions from the transitions within the gr…
Since their first experimental observation, ultralong-range Rydberg molecules consisting of a highly excited Rydberg atom and a ground state atom have attracted the interest in the field of ultracold chemistry. Especially the intriguing properties like size, polarizability and type of binding they inherit from the Rydberg atom are of interest. An open question in the field is the reduced lifetime of the molecules compared to the corresponding atomic Rydberg states. In this letter we present an experimental study on the lifetimes of the ^3Σ(5s-35s) molecule in its vibrational ground state and i…
