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147
result(s) for
"Ospelkaus, S"
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Controlling the quantum stereodynamics of ultracold bimolecular reactions
by
Chotia, A.
,
Jin, D. S.
,
Wang, D.
in
Atomic
,
Chemical reactions
,
Classical and Continuum Physics
2011
Molecular collisions in the quantum regime represent a new opportunity to explore chemical reactions. Recently, atom-exchangereactions were observed in a trapped ultracold gas of KRb molecules. In an external electric field, these polar molecules can easily be oriented and the exothermic and barrierless bimolecular reactions, KRb+KRb→K
2
+Rb
2
, occur at a rate that rises steeply with increasing dipole moment. Here we demonstrate the suppression of the bimolecular chemical reaction rate by nearly two orders of magnitude when 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 under repulsive dipole–dipole interactions. The suppression of chemical reactions is a prerequisite for the realization of new molecule-based quantum systems.
The investigation of how chemical reactions depend on molecular orientation has a long history. In particular, the spatial anisotropy of the dipole–dipole interaction between polar molecules leads to a dependence of stereodynamics of collisions on long-range interactions. A study with ultracold molecules, where all internal and external states of the molecules can be controlled, now extends such studies into the quantum regime.
Journal Article
A Zeeman slower for diatomic molecules
2018
We present a novel slowing scheme for beams of laser-coolable diatomic molecules reminiscent of Zeeman slowing of atomic beams. The scheme results in efficient compression of the one-dimensional velocity distribution to velocities trappable by magnetic or magneto-optical traps. We experimentally demonstrate our method in an atomic testbed and show an enhancement of flux below v = 35 m s−1 by a factor of 20 compared to white light slowing. 3D Monte Carlo simulations performed to model the experiment show excellent agreement. We apply the same simulations to the prototype molecule 88Sr19F and expect 15% of the initial flux to be continuously compressed in a narrow velocity window at around 10 m s−1. This is the first experimentally shown continuous and dissipative slowing technique in molecule-like level structures, promising to provide the missing link for the preparation of large ultracold molecular ensembles.
Journal Article
Quantum-State Controlled Chemical Reactions of Ultracold Potassium-Rubidium Molecules
by
Neyenhuis, B
,
Quéméner, G
,
Jin, D.S
in
Angular momentum
,
Atomic and molecular collision processes and interactions
,
Atomic and molecular physics
2010
How does a chemical reaction proceed at ultralow temperatures? Can simple quantum mechanical rules such as quantum statistics, single partial-wave scattering, and quantum threshold laws provide a clear understanding of the molecular reactivity under a vanishing collision energy? Starting with an optically trapped near-quantum-degenerate gas of polar ⁴⁰K⁸⁷Rb molecules prepared in their absolute ground state, we report experimental evidence for exothermic atom-exchange chemical reactions. When these fermionic molecules were prepared in a single quantum state at a temperature of a few hundred nanokelvin, we observed p-wave-dominated quantum threshold collisions arising from tunneling through an angular momentum barrier followed by a short-range chemical reaction with a probability near unity. When these molecules were prepared in two different internal states or when molecules and atoms were brought together, the reaction rates were enhanced by a factor of 10 to 100 as a result of 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.
Journal Article
High Phase-Space-Density Gas of Polar Molecules
2008
A quantum gas of ultracold polar molecules, with long-range and anisotropic interactions, not only would enable explorations of a large class of many-body physics phenomena but also could be used for quantum information processing. We report on the creation of an ultracold dense gas of potassium-rubidium (⁴⁰K⁸⁷Rb) polar molecules. Using a single step of STIRAP (stimulated Raman adiabatic passage) with 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 10¹² per cubic centimeter and an expansion-determined translational temperature of 350 nanokelvin. The polar molecules have a permanent electric dipole moment, which we measure with Stark spectroscopy to be 0.052(2) Debye (1 Debye = 3.336 x 10⁻³⁰ coulomb-meters) for the triplet rovibrational ground state and 0.566(17) Debye for the singlet rovibrational ground state.
Journal Article
Dipolar collisions of polar molecules in the quantum regime
2010
Quantum collisions
Ultracold polar molecules offer the possibility of exploring quantum gases with inter-particle interactions that are strong, long-range and spatially anisotropic. Here, Ni
et al
. report the experimental observation of dipolar collisions in an ultracold gas of fermionic
40
K
87
Rb molecules. For modest values of an applied electric field, they observe a dramatic increase in the loss rate due to ultracold chemical reactions.
Ultracold polar molecules offer the possibility of exploring quantum gases with interparticle interactions that are strong, long-range and spatially anisotropic. Here, dipolar collisions in an ultracold gas of fermionic potassium–rubidium molecules have been experimentally observed. The results show how the long-range dipolar interaction can be used for electric-field control of chemical reaction rates in an ultracold gas of polar molecules.
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 much studied dilute gases of ultracold atoms, which have isotropic and extremely short-range (or ‘contact’) interactions. Furthermore, the large electric dipole moment of polar molecules can be tuned using an external electric field; this has a range of applications such as the control of ultracold chemical reactions
1
, the design of a platform for quantum information processing
2
,
3
,
4
and the realization of novel quantum many-body systems
5
,
6
,
7
,
8
. Despite intense experimental efforts aimed at observing the influence of dipoles on ultracold molecules
9
, only recently have sufficiently high densities been achieved
10
. Here we report the experimental 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 pronounced increase in the loss rate of fermionic potassium–rubidium molecules due to ultracold 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 in a relatively simple model based on quantum threshold laws for the scattering of fermionic polar molecules. In addition, we directly observe the spatial anisotropy of the dipolar interaction through 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 gas of polar molecules. Furthermore, 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, ‘head-to-tail’, dipolar interactions
11
,
12
,
13
,
14
.
Journal Article
Maximizing the capture velocity of molecular magneto-optical traps with Bayesian optimization
by
Stepanova, M
,
Kaebert, P
,
Poll, T
in
Bayesian analysis
,
Bayesian optimization
,
Calcium fluoride
2021
Magneto-optical trapping (MOT) is a key technique on the route towards ultracold molecular ensembles. However, the realization and optimization of magneto-optical traps with their wide parameter space is particularly difficult. Here, we present a very general method for the optimization of molecular magneto-optical trap operation by means of Bayesian optimization. As an example for a possible application, we consider the optimization of a calcium fluoride MOT for maximum capture velocity. We find that both the X 2 Σ + to A 2 Π 1/2 and the X 2 Σ + to B 2 Σ + transition to allow for capture velocities with 24 m s −1 and 23 m s −1 respectively at a total laser power of 200 mW. In our simulation, the optimized capture velocity depends logarithmically on the beam power within the simulated power range of 25 to 400 mW. Applied to heavy molecules such as BaH, BaF, YbF and YbOH with their low capture velocity MOTs it might offer a route to far more robust MOT.
Journal Article
Characterizing the Zeeman slowing force for 40Ca19F molecules
2021
In this paper we investigate the feasibility of Zeeman slowing calcium monofluoride molecules originating from a cryogenic buffer gas cell. We measure the \\({A}^{2}{{\\Pi}}_{1/2}(v=0,J=\\frac{1}{2})-{X}^{2}{{\\Sigma}}_{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 10 mW broad repumper and a 10 mW 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 narrow enough in velocity space to lead to significant velocity compression, and slowing of the molecules to trappable velocities.
Journal Article
Efficient state transfer in an ultracold dense gas of heteronuclear molecules
by
Zirbel, J. J.
,
Jin, D. S.
,
Pe’er, A.
in
Atomic
,
Atoms & subatomic particles
,
Classical and Continuum Physics
2008
A rich internal structure and long-range interactions between them make molecules with non-vanishing dipole moments interesting for many applications. An experiment demonstrating the efficient transfer of loosely bound heteronuclear molecules into more deeply bound energy levels indicates a route towards producing dense ensembles of cold polar molecules.
Polar molecules have bright prospects for novel quantum gases with long-range and anisotropic interactions
1
, and could find uses in quantum information science
2
and in precision measurements
3
,
4
,
5
. However, high-density clouds of ultracold polar molecules have so far not been produced. Here, we report a key step towards this goal. We start from an ultracold dense gas of loosely bound
40
K
87
Rb Feshbach molecules
6
,
7
with typical binding energies of a few hundred kilohertz, and coherently transfer these molecules in a single transfer step into a vibrational level of the ground-state molecular potential bound by more than 10 GHz. Starting with a single initial state prepared with Feshbach association
8
, we achieve a transfer efficiency of 84%. Given favourable Franck–Condon factors
9
,
10
, the presented technique can be extended to access much more deeply bound vibrational levels and those exhibiting a significant dipole moment.
Journal Article
Versatile electric fields for the manipulation of ultracold NaK molecules
2016
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. 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−1 this corresponds to a deviation of 0.01 V cm−1. Furthermore, the possibility to create strong electric field gradients provides the opportunity to address molecules in single layers of an optical lattice. 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.
Journal Article
Characterizing the Zeeman slowing force for 40 Ca 19 F molecules
2021
In this paper we investigate the feasibility of Zeeman slowing calcium monofluoride molecules originating from a cryogenic buffer gas cell. We measure the A 2 Π 1 / 2 ( v = 0 , J = 1 2 ) − X 2 Σ 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 10 mW broad repumper and a 10 mW 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 narrow enough in velocity space to lead to significant velocity compression, and slowing of the molecules to trappable velocities.
Journal Article