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S. Ospelkaus

Publications and source records attributed to S. Ospelkaus.

At least 19 recordsLinked to original sources

Blue-detuned molecular magneto-optical trap schemes based on bayesian optimization

Direct laser cooling and trapping of molecules to temperature below Doppler limit and density exceeding $10^8$ are challenging due to the sub-Doppler heating effects of molecular magneto-optical trap (MOT). In our previous paper [1], we presented a general approach to engineering the sub- Doppler force by tuning the AC stark shift with the addition of a blue detuned laser. Here, by employing the Bayesian optimization method to optical Bloch equations, we have identified multiple blue-detuned MOT schemes for the CaF molecule. From the three-dimensional Monte-Carlo simulation, we obtained a MOT temperature and density of 14 $\rm μK$ and $\rm 4.5 \times 10^8 cm^{-3}$, respectively. Our findings present a potential avenue for directly loading molecular MOTs into conservative traps, which can capitalize on the high density and low temperature of the MOT

physics.atom-ph

The electronic system $(2)^2Σ^+$ and $(1)^2Π$ of LiCa

High resolution Fourier transform spectroscopy and Laser induced fluorescence has been performed on LiCa in the infrared spectral range. We analyze rovibrational transitions of the $(2)^2Σ^+$--$X(1)^2Σ^+$ system of LiCa and find the $(2)^2Σ^+$ state to be perturbed by spin-orbit coupling to the $(1)^2Π$ state. We study the coupled system obtaining molecular parameters for the $(2)^2Σ^+$ and the $(1)^2Π$ state together with effective spin-orbit and spin-rotation coupling constants. The coupled system has also been evaluated by applying a potential function instead of rovibrational molecular parameters for the state $(2)^2Σ^+$. An improved analytic potential function of the $X(1)^2Σ^+$ state is derived, due to the extension of the observed rotational ladder.

physics.chem-ph

Engineering the sub-Doppler force in molecular magneto-optical traps

Current dual-frequency magneto-optical traps for ultracold molecules are plagued by sub-Doppler heating effects, making them vastly inferior to standard atomic MOTs. Here we demonstrate theoretically that the sub-Doppler effects in such a MOT can be engineered to provide cooling instead of heating. We give an intuitive picture how to achieve such cooling and show the cooling and trapping force results of the 16 level optical Bloch equations for the case of CaF molecules. From three-dimensional Monte Carlo simulations we estimate the temperature and density of our MOT to be $40 μK$ and $4 \times 10^8 cm^{-3}$ respectively for a molecule number of $10^5$.

physics.atom-ph

Characterizing the Zeeman slowing force for $^{40}$Ca$^{19}$F molecules

In this paper we investigate the feasibility of Zeeman slowing calcium monofluoride (CaF) molecules originating from a cryogenic buffer gas cell. We measure the $A^2Π_{1/2} (v=0, J=\frac{1}{2}) - X^2Σ_{1/2} (v=0, N=1)$ hyperfine spectrum of CaF in the Paschen-Back regime and find excellent agreement with theory. We then investigate the scattering rate of the molecules in a molecular Zeeman slower by illuminating them with light from a 10mW broad repumper and a 10mW multi-frequency slowing laser. By comparing our results to theory we can calculate the photon scattering rate at higher powers, leading to a force profile for Zeeman slowing. We show results from a simple 1D simulation demonstrating that this force is both strong and narrow enough to lead to significant compression, and slowing of the molecules to trappable velocities.

physics.atom-ph

Probing photoinduced two-body loss of ultracold non-reactive bosonic $^{23}$Na$^{87}$Rb and $^{23}$Na$^{39}$K molecules

We probe photo-induced loss for chemically stable bosonic $^{23}$Na$^{87}$Rb and $^{23}$Na$^{39}$K molecules in chopped optical dipole traps where the molecules spend a significant time in the dark. We expect the effective two-body decay to be largely suppressed in chopped traps due to the small expected complex lifetimes of about $13μ$s and $6μ$s for $^{23}$Na$^{87}$Rb and $^{23}$Na$^{39}$K respectively. However, instead we do observe near-universal loss even at the lowest chopping frequencies we can probe. Our data thus either suggest a so far unknown loss mechanism or a drastic underestimation of the complex lifetime by at least one to two orders of magnitude.

physics.atom-ph

Versatile electric fields for the manipulation of ultracold NaK molecules

In this paper, we present an electrode geometry for the manipulation of ultracold rovibrational ground state NaK molecules. The electrode system allows to induce a dipole moment in trapped diatomic NaK molecules with a magnitude up to $68 \%$ of their internal dipole moment along any direction in a given two-dimensional plane. The strength, the sign and the direction of the induced dipole moment is therefore fully tunable. Furthermore, the possibility to create strong electric field gradients provides the opportunity to address molecules in single layers of an optical lattice. The maximal relative variation of the electric field over the trapping volume is below $10^{-6}$. At the desired electric field value of 10 kV/cm this corresponds to a deviation of 0.01 V/cm. The electrode structure is made of transparent indium tin oxide and combines large optical access for sophisticated optical dipole traps and optical lattice configurations with the possibility to create versatile electric field configurations.

cond-mat.quant-gas

Multi-channel modeling and two photon coherent transfer paths in NaK

We explore possible pathways for the creation of ultracold polar NaK molecules in their absolute electronic and rovibrational ground state starting from ultracold Feshbach molecules. In particular, we present a multi-channel analysis of the electronic ground and K(4p)+Na(3s) excited state manifold of NaK, analyze the spin character of both the Feshbach molecular state and the electronically excited intermediate states and discuss possible coherent two-photon transfer paths from Feshbach molecules to rovibronic ground state molecules. The theoretical study is complemented by the demonstration of STIRAP transfer from the X^1Σ^+ (v=0) state to the a^3Σ^+ manifold on a molecular beam experiment.

physics.atom-ph

Controlling the quantum stereodynamics of ultracold bimolecular reactions

Chemical reaction rates often depend strongly on stereodynamics, namely the orientation and movement of molecules in three-dimensional space. An ultracold molecular gas, with a temperature below 1 uK, provides a highly unusual regime for chemistry, where polar molecules can easily be oriented using an external electric field and where, moreover, the motion of two colliding molecules is strictly quantized. Recently, atom-exchange reactions were observed in a trapped ultracold gas of KRb molecules. In an external electric field, these exothermic and barrierless bimolecular reactions, KRb+KRb -> K2+Rb2, occur at a rate that rises steeply with increasing dipole moment. Here we show that the quantum stereodynamics of the ultracold collisions can be exploited to suppress the bimolecular chemical reaction rate by nearly two orders of magnitude. We use an optical lattice trap to confine the fermionic polar molecules in a quasi-two-dimensional, pancake-like geometry, with the dipoles oriented along the tight confinement direction. With the combination of sufficiently tight confinement and Fermi statistics of the molecules, two polar molecules can approach each other only in a "side-by-side" collision, where the chemical reaction rate is suppressed by the repulsive dipole-dipole interaction. We show that the suppression of the bimolecular reaction rate requires quantum-state control of both the internal and external degrees of freedom of the molecules. The suppression of chemical reactions for polar molecules in a quasi-two-dimensional trap opens the way for investigation of a dipolar molecular quantum gas. Because of the strong, long-range character of the dipole-dipole interactions, such a gas brings fundamentally new abilities to quantum-gas-based studies of strongly correlated many-body physics, where quantum phase transitions and new states of matter can emerge.

quant-ph

Direct absorption imaging of ultracold polar molecules

We demonstrate a scheme for direct absorption imaging of an ultracold ground-state polar molecular gas near quantum degeneracy. A challenge in imaging molecules is the lack of closed optical cycling transitions. Our technique relies on photon shot-noise limited absorption imaging on a strong bound-bound molecular transition. We present a systematic characterization of this imaging technique. Using this technique combined with time-of-flight (TOF) expansion, we demonstrate the capability to determine momentum and spatial distributions for the molecular gas. We anticipate that this imaging technique will be a powerful tool for studying molecular quantum gases.

cond-mat.quant-gas

Dipolar collisions of polar molecules in the quantum regime

Ultracold polar molecules offer the possibility of exploring quantum gases with interparticle interactions that are strong, long-range, and spatially anisotropic. This is in stark contrast to the dilute gases of ultracold atoms, which have isotropic and extremely short-range, or "contact", interactions. The large electric dipole moment of polar molecules can be tuned with an external electric field; this provides unique opportunities such as control of ultracold chemical reactions, quantum information processing, and the realization of novel quantum many-body systems. In spite of intense experimental efforts aimed at observing the influence of dipoles on ultracold molecules, only recently have sufficiently high densities been achieved. Here, we report the observation of dipolar collisions in an ultracold molecular gas prepared close to quantum degeneracy. For modest values of an applied electric field, we observe a dramatic increase in the loss rate of fermionic KRb molecules due to ultrcold chemical reactions. We find that the loss rate has a steep power-law dependence on the induced electric dipole moment, and we show that this dependence can be understood with a relatively simple model based on quantum threshold laws for scattering of fermionic polar molecules. We directly observe the spatial anisotropy of the dipolar interaction as manifested in measurements of the thermodynamics of the dipolar gas. These results demonstrate how the long-range dipolar interaction can be used for electric-field control of chemical reaction rates in an ultracold polar molecule gas. The large loss rates in an applied electric field suggest that creating a long-lived ensemble of ultracold polar molecules may require confinement in a two-dimensional trap geometry to suppress the influence of the attractive dipolar interactions.

physics.atom-ph

Quantum-State Controlled Chemical Reactions of Ultracold KRb Molecules

How does a chemical reaction proceed at ultralow temperatures? Can simple quantum mechanical rules such as quantum statistics, single scattering partial waves, and quantum threshold laws provide a clear understanding for the molecular reactivity under a vanishing collision energy? Starting with an optically trapped near quantum degenerate gas of polar $^{40}$K$^{87}$Rb molecules prepared in their absolute ground state, we report experimental evidence for exothermic atom-exchange chemical reactions. When these fermionic molecules are prepared in a single quantum state at a temperature of a few hundreds of nanoKelvins, we observe p-wave-dominated quantum threshold collisions arising from tunneling through an angular momentum barrier followed by a near-unity probability short-range chemical reaction. When these molecules are prepared in two different internal states or when molecules and atoms are brought together, the reaction rates are enhanced by a factor of 10 to 100 due to s-wave scattering, which does not have a centrifugal barrier. The measured rates agree with predicted universal loss rates related to the two-body van der Waals length.

physics.atom-ph

Controlling the hyperfine state of rovibronic ground-state polar molecules

Ultracold molecules offer entirely new possibilities for the control of quantum processes due to their rich internal structure. Recently, near quantum degenerate gases of molecules have been prepared in their rovibronic ground state. For future experiments, it is crucial to also control their hyperfine state. Here, we report the preparation of a rovibronic ground state molecular quantum gas in a single hyperfine state and in particular in the absolute lowest quantum state. The demonstrated and presented scheme is general for bialkali polar molecules and allows the preparation of molecules in a single hyperfine state or in an arbitrary coherent superposition of hyperfine states. The scheme relies on electric-dipole, two-photon microwave transitions through rotationally excited states and makes use of electric nuclear quadrupole interactions to transfer molecular population between different hyperfine states.

physics.atom-ph

Ultracold polar molecules near quantum degeneracy

We report the creation and characterization of a near quantum-degenerate gas of polar $^{40}$K-$^{87}$Rb molecules in their absolute rovibrational ground state. Starting from weakly bound heteronuclear KRb Feshbach molecules, we implement precise control of the molecular electronic, vibrational, and rotational degrees of freedom with phase-coherent laser fields. In particular, we coherently transfer these weakly bound molecules across a 125 THz frequency gap in a single step into the absolute rovibrational ground state of the electronic ground potential. Phase coherence between lasers involved in the transfer process is ensured by referencing the lasers to two single components of a phase-stabilized optical frequency comb. Using these methods, we prepare a dense gas of $4\cdot10^4$ polar molecules at a temperature below 400 nK. This fermionic molecular ensemble is close to quantum degeneracy and can be characterized by a degeneracy parameter of $T/T_F=3$. We have measured the molecular polarizability in an optical dipole trap where the trap lifetime gives clues to interesting ultracold chemical processes. Given the large measured dipole moment of the KRb molecules of 0.5 Debye, the study of quantum degenerate molecular gases interacting via strong dipolar interactions is now within experimental reach.

physics.atom-ph

Heteronuclear quantum gas mixtures

This PhD tutorial article is a review of our experiments on heteronuclear quantum gas mixtures at the University of Hamburg. We introduce basic properties of trapped Fermi-Bose mixtures and demonstrate the achievement of large quantum degenerate mixtures of 40K and 87Rb. Using heteronuclear Feshbach resonances, we show how the heteronuclear interaction can be tuned, allowing us to induce phase separation and collapse for large repulsive and attractive interactions, respectively. We realize Fermi-Bose mixtures in 3D optical lattices as a novel quantum many-body system and study coherence properties of the mixture. Combining our experiments on lattices and Feshbach resonances, we present the first realization of ultracold heteronuclear Feshbach molecules. The molecules are created at individual sites of a 3D optical lattice. We discuss lifetime, binding energy and rf association efficiency in terms of a universal model and give an outlook for possible future developments.

cond-mat.other

A High Phase-Space-Density Gas of Polar Molecules

A quantum gas of ultracold polar molecules, with long-range and anisotropic interactions, would not only enable explorations of a large class of many-body physics phenomena, but could also be used for quantum information processing. We report on the creation of an ultracold dense gas of 40K87Rb polar molecules. Using a single step of STIRAP (STImulated Raman Adiabatic Passage) via two-frequency laser irradiation, we coherently transfer extremely weakly bound KRb molecules to the rovibrational ground state of either the triplet or the singlet electronic ground molecular potential. The polar molecular gas has a peak density of 10^12 cm^-3, and an expansion-determined translational temperature of 350 nK. The polar molecules have a permanent electric dipole moment, which we measure via Stark spectroscopy to be 0.052(2) Debye for the triplet rovibrational ground state and 0.566(17) Debye for the singlet rovibrational ground state. (1 Debye= 3.336*10^-30 C m)

quant-ph

Heteronuclear molecules in an optical dipole trap

We report on the creation and characterization of heteronuclear KRb Feshbach molecules in an optical dipole trap. Starting from an ultracold gas mixture of K-40 and Rb-87 atoms, we create as many as 25,000 molecules at 300 nK by rf association. Optimizing the association process, we achieve a conversion efficiency of 25%. We measure the temperature dependence of the rf association process and find good agreement with a phenomenological model that has previously been applied to Feshbach molecule creation by slow magnetic-field sweeps. We also present a measurement of the binding energy of the heteronuclear molecules in the vicinity of the Feshbach resonance and provide evidence for Feshbach molecules as deeply bound as 26 MHz.

cond-mat.other

Collisional stability of fermionic Feshbach molecules

Using a Feshbach resonance, we create ultracold fermionic molecules starting from a Bose-Fermi atom gas mixture. The resulting mixture of atoms and weakly bound molecules provides a rich system for studying few-body collisions because of the variety of atomic collision partners for molecules; either bosonic, fermionic, or distinguishable atoms. Inelastic loss of the molecules near the Feshbach resonance is dramatically affected by the quantum statistics of the colliding particles and the scattering length. In particular, we observe a molecule lifetime as long as 100 ms near the Feshbach resonance.

cond-mat.other

Ultracold dense gas of deeply bound heteronuclear molecules

Recently, the quest for an ultracold and dense ensemble of polar molecules has attracted strong interest. Polar molecules have bright prospects for novel quantum gases with long-range and anisotropic interactions, for quantum information science, and for precision measurements. However, high-density clouds of ultracold polar molecules have so far not been produced. Here, we report a key step towards this goal. Starting from an ultracold dense gas of heteronuclear 40K-87Rb Feshbach molecules with typical binding energies of a few hundred kHz and a negligible dipole moment, we coherently transfer these molecules into a vibrational level of the ground-state molecular potential bound by >10 GHz. We thereby increase the binding energy and the expected dipole moment of the 40K-87Rb molecules by more than four orders of magnitude in a single transfer step. Starting with a single initial state prepared with Feshbach association, we achieve a transfer efficiency of 84%. While dipolar effects are not yet observable, the presented technique can be extended to access much more deeply bound vibrational levels and ultimately those exhibiting a significant dipole moment. The preparation of an ultracold quantum gas of polar molecules might therefore come within experimental reach.

physics.atom-ph