Ultracold Temperatures Research Articles

Ultracold collisions and reactions of vibrationally excited OH radicals with oxygen atoms

We report a quantum dynamics study of O + OH (v = 1, j = 0) collisions on its ground electronic state, employing two different potential energy surfaces: the DIMKP surface by Kendrick and Pack, and the XXZLG surface by Xu et al. A time-independent quantum mechanical method based on hyperspherical coordinates has been adopted for the dynamics calculations. Energy-dependent probabilities and rate coefficients are computed for the elastic, inelastic, and reactive channels over the collision energy range E(coll) = 10(-10)-0.35 eV, for J = 0 total angular momentum. Initial state-selected reaction rate coefficients are also calculated from the J = 0 reaction probabilities by applying a J-shifting approximation, for temperatures in the range T = 10(-6)-700 K. Our results show that the dynamics of the collisional process and its outcome are strongly influenced by long-range forces, and chemical reactivity is found to be sensitive to the choice of the potential energy surface. For O + OH (v = 1, j = 0) collisions at low temperatures, vibrational relaxation of OH competes with reactive scattering. Since long-range interactions can facilitate vibrational relaxation processes, we find that the DIMKP potential (which explicitly includes van der Waals dispersion terms) favours vibrational relaxation over chemical reaction at low temperatures. On the DIMKP potential in the ultracold regime, the reaction rate coefficient for O + OH (v = 1, j = 0) is found to be a factor of thirteen lower than that for O + OH (v = 0, j = 0). This significantly high reactivity of OH (v = 0, j = 0), compared to that of OH (v = 1, j = 0), is attributed to enhancement caused by the presence of a HO(2) quasibound state (scattering resonance) with energy near the O + OH (v = 0, j = 0) dissociation threshold. In contrast, the XXZLG potential does not contain explicit van der Waals terms, being just an extrapolation by a nearly constant function at large O-OH distances. Therefore, long-range potential couplings are absent in calculations using the XXZLG surface, which does not induce vibrational relaxation as efficiently as the DIMKP potential. The XXZLG potential leads to a slightly higher reactivity (a factor of 1.4 higher) for O + OH (v = 1, j = 0) compared to that for O + OH (v = 0, j = 0) at ultracold temperatures. Overall, both potential surfaces yield comparable values of reaction rate coefficients at low temperatures for the O + OH (v = 1, j = 0) reaction.

Quantum superchemistry of de Broglie waves: New wonderland at ultracold temperature

The experimental realization of atomic Bose-Einstein condensation at ultracold temperature has led to rapid advances in creating and manipulating cold molecules, and which has given birth to a new research field of quantum matter-wave superchemistry. Contrary to the classical Arrhenius law, the tunneling-dominated ultracold reactions can be realized through the highly-controlled magneto-optical technique. Novel quantum effects have been identified in these cold reactions, such as the super-selectivity rule in dissociating triatomic molecules, and the quantum size (vessel-shape) effect. In this review, we focus on a variety of new achievements in this fascinating matter-wave wonderland, including the quantum finite-number effect and double-slit interference in assembling cold molecules, the quantum noise in triggering collective abstraction reaction, and the magnetic phase transition in a laser-catalyzed quantum spin-mixing gas. The practical applications of matter-wave superchemistry are also introduced, such as the optical information storage via quantum photo-association, and the laser-enhanced creation of spinor or even chiral molecules.

Rydberg Trimers and Excited Dimers Bound by Internal Quantum Reflection

In a combined experimental and theoretical effort we report on two novel types of ultracold long-range Rydberg molecules. First, we demonstrate the creation of triatomic molecules of one Rydberg atom and two ground-state atoms in a single-step photoassociation. Second, we assign a series of excited dimer states that are bound by a so far unexplored mechanism based on internal quantum reflection at a steep potential drop. The properties of the Rydberg molecules identified in this work qualify them as prototypes for a new type of chemistry at ultracold temperatures.

Laser cooling of a diatomic molecule

It has been roughly three decades since laser cooling techniques produced ultracold atoms, leading to rapid advances in a wide array of fields. Laser cooling has not yet been extended to molecules because of their complex internal structure. However, this complexity makes molecules potentially useful for a wide range of applications. For example, heteronuclear molecules possess permanent electric dipole moments that 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 possible at ultracold temperatures makes ultracold molecules attractive candidates for use in quantum simulations of condensed-matter systems and in quantum computation. Also, ultracold molecules could provide unique opportunities for studying chemical dynamics and for tests of fundamental symmetries. Here we experimentally demonstrate laser cooling of the polar molecule strontium monofluoride (SrF). Using an optical cycling scheme requiring only three lasers, we have observed both Sisyphus and Doppler cooling forces that reduce the transverse temperature of a SrF molecular beam substantially, to a few millikelvin or less. At present, the only technique for producing ultracold molecules is to bind together ultracold alkali atoms through Feshbach resonance or photoassociation. However, proposed applications for ultracold molecules require a variety of molecular energy-level structures (for example unpaired electronic spin, Omega doublets and so on). Our method provides an alternative route to ultracold molecules. In particular, it bridges the gap between ultracold (submillikelvin) temperatures and the ∼1-K temperatures attainable with directly cooled molecules (for example with cryogenic buffer-gas cooling or decelerated supersonic beams). Ultimately, our technique should allow the production of large samples of molecules at ultracold temperatures for species that are chemically distinct from bialkalis.

Creating a quantum degenerate gas of stable molecules via weak photoassociation

Quantum degenerate molecules represent a new paradigm for fundamental studies and practical applications. Association of already quantum degenerate atoms into molecules provides a crucial shortcut around the difficulty of cooling molecules to ultracold temperatures. Whereas association can be induced with either laser or magnetic fields, photoassociation requires impractical laser intensity to overcome poor overlap between the atom pair and molecular wave functions, and experiments are currently restricted to magnetoassociation. Here we model realistic production of a quantum degenerate gas of stable molecules via two-photon photoassociation of Bose-condensed atoms. An adiabatic change of the laser frequency converts the initial atomic condensate almost entirely into stable molecular condensate, even for low-intensity lasers. Results for dipolar LiNa provide an upper bound on the necessary photoassociation laser intensity for alkali-metal atoms $~$$30$ W/cm${}^{2}$, indicating a feasible path to quantum degenerate molecules beyond magnetoassociation.

Creating cold stationary molecular gases by optical Stark deceleration

The deceleration of molecules from cold molecular beams using electric and magnetic fields has become an important means for producing stationary, cold dipolar or paramagnetic molecular gases that can be trapped and potentially cooled to ultra-cold temperatures in the μK range. We report on a general scheme for the creation of cold molecules of essentially any type by deceleration of a cold molecular beam using intense optical fields. Deceleration of benzene molecules to zero velocity is achieved by utilizing a single half oscillation of the center-of-mass motion of the molecules within a moving optical lattice. The lattice traveling at half the speed of the molecular beam is created by the interference of two near-counter-propagating fields at different frequencies. We show that by rapidly switching on the optical lattice for approximately the time required for a half oscillation, a bunch of approximately 105 benzene molecules can be rapidly decelerated and brought to rest in the laboratory frame.

Rotational excitations in two-color photoassociation

We show that it is possible to excite higher rotational states J > 2 in ultracold photoassociation by two laser fields. Usually higher J states are suppressed in photoassociation at ultracold temperatures in the regime of Wigner threshold laws. We propose a scheme in which one strong laser field drives photoassociation transition close to either J = 1 or J = 2 rotational state of a particular vibrational level of an electronically excited molecule. The other laser field is tuned near photoassociation resonance with J > 2 rotational levels of the same vibrational state. The strong laser field induces a strong continnum-bound dipole coupling. The resulting dipole force between two colliding atoms modifies the continnum states forming continnum-bound dressed states with a significant component of higher partial waves in the continnum configuration. When the second laser is scanned near the resonance of the higher J states, these states become populated due to photoassociative transitions from the modified continnum.

Strong dependence of ultracold chemical rates on electric dipole moments

We use the quantum threshold laws combined with a classical capture model to provide an analytical estimate of the chemical quenching cross sections and rate coefficients of two colliding particles at ultralow temperatures. We apply this quantum threshold model (QT model) to indistinguishable fermionic polar molecules in an electric field. At ultracold temperatures and in weak electric fields, the cross sections and rate coefficients depend only weakly on the electric dipole moment d induced by the electric field. In stronger electric fields, the quenching processes scale as d^{4(L+1/2)} where L>0 is the orbital angular momentum quantum number between the two colliding particles. For p-wave collisions (L=1) of indistinguishable fermionic polar molecules at ultracold temperatures, the quenching rate thus scales as d^6. We also apply this model to pure two dimensional collisions and find that chemical rates vanish as d^{-4} for ultracold indistinguishable fermions. This model provides a quick and intuitive way to estimate chemical rate coefficients of reactions occuring with high probability.

Calculation of Scattering Parameters for Ultracold K–Cs Elastic Collisions

A theoretical study of elastic scattering properties in a mixture of 39K and 133Cs atoms at cold and ultracold temperatures is reported in this paper. Based on the new constructed accurate singlet X 1∑+ and triplet a 3∑+ states interatomic potentials for 39K133Cs mixture, the interspecies s-wave scattering lengths and the p-wave scattering volumes are calculated by the variable phase method and the semiclassical method, respectively. Good agreement between two methods is obtained. The mass dependence of the scattering data by considering all isotopomers is explored, and the numbers of bound states supported by the molecular potentials for each isotopomer are also calculated.

Geometric bonding effects in the X A21, A Σ2u+, and B Π2g states of Li2F

Published ab initio and pseudopotential calculations for the dialkali halide systems suggest that the preferred colinear geometry is for the metal to approach the metal end of the alkali halide. Here, ab initio calculations on the Li2F system reveal that the well depth on the halide side in this radical is much deeper and is a local saddle point associated with the ionic nonlinear global minima. Although many features of the pseudopotential surfaces are confirmed, significant differences are apparent including the existence of a linear excited A Σ2u+ state instead of a triangular one, a considerably deeper global minimum some 50% lower in energy and a close approach between the X A21 and the A Σ2u+ states, with the A Σ2u+ minimum 87 kJ mol−1 below the ground state asymptote. All the results can be rationalised as the avoided crossings between a long range, covalent potential dominant within the LiLiF geometry and an ionic state that forms the global minimum. Calculations on the third A2′ potential indicate that even for Li+LiF collisions at ultracold temperatures the collision dynamics could involve as many as three electronic states.

Ribonuclear inclusions as biomarker of myotonic dystrophy type 2, even in improperly frozen or defrozen skeletal muscle biopsies.

Myotonic dystrophy type 2 (DM2) is a dominantly inherited disorder caused by a CCTG repeat expansion in intron 1 of ZNF9 gene. The size and the somatic instability of DM2 expansion complicate the molecular diagnosis of DM2. In situ hybridization represents a rapid and sensitive method to obtain a definitive diagnosis in few hours, since it allows the direct visualization of the mutant mRNA foci on skeletal muscle sections. This approach makes the muscle biopsy an important tool for definitive diagnosis of DM2. Consequently, a rapid freezing at ultra cold temperature and a good storage of muscle specimens are essential to avoid morphologic alterations and nucleic acids degradation. However incorrect freezing or thawing may accidentally occur. In this work we report that fluorescence in situ hybridization may be applied on improperly frozen or inappropriately stored muscle biopsies since foci of mutant mRNA are well preserved and can still be detected in muscle sections no more useful for histopathological evaluation.

Analytic description of atomic interaction at ultracold temperatures: The case of a single channel

We present analytic descriptions of atomic interaction at ultracold temperatures using both single-channel and multichannel quantum-defect theories. In the case of a single channel, addressed in this paper, the expansion of [B. Gao, Phys. Rev. A \textbf{58}, 4222 (1998)] is generalized to higher orders for angular momentum $l\ge 2$ to give a more complete description of ultracold scattering, including an analytic description of ultracold shape resonances of arbitrary $l$. We also introduce a generalized scattering length that is well defined and useful for all partial waves, to replace the traditional definition that fails for $l\ge 2$ due to the long-range van der Waals interaction. The results are used in a companion paper to derive analytic descriptions of atomic interaction around a magnetic Feshbach resonance of arbitrary angular momentum $l$.

Ribonuclear inclusions as biomarker of myotonic dystrophy type 2, even in improperly frozen or defrozen skeletal muscle biopsies

Myotonic dystrophy type 2 (DM2) is a dominantly inherited disorder caused by a CCTG repeat expansion in intron 1 of ZNF9 gene. The size and the somatic instability of DM2 expansion complicate the molecular diagnosis of DM2. In situ hybridization represents a rapid and sensitive method to obtain a definitive diagnosis in few hours, since it allows the direct visualization of the mutant mRNA foci on skeletal muscle sections. This approach makes the muscle biopsy an important tool for definitive diagnosis of DM2. Consequently, a rapid freezing at ultra cold temperature and a good storage of muscle specimens are essential to avoid morphologic alterations and nucleic acids degradation. However incorrect freezing or thawing may accidentally occur. In this work we report that fluorescence in situ hybridization may be applied on improperly frozen or inappropriately stored muscle biopsies since foci of mutant mRNA are well preserved and can still be detected in muscle sections no more useful for histopathological evaluation.

Magnetic field modification of ultracold molecule–molecule collisions

We present an accurate quantum mechanical study of molecule–molecule collisions in the presence of a magnetic field. The work focuses on the analysis of elastic scattering and spin relaxation in collisions of O2(3Σg–) molecules at cold (∼0.1 K) and ultracold (∼10–6 K) temperatures. Our calculations show that magnetic spin relaxation in molecule–molecule collisions is extremely efficient except at magnetic fields below 1 mT. The rate constant for spin relaxation at T=0.1 K and a magnetic field of 0.1 T is found to be as large as 6.1×10–11 cm–3 s–1. The magnetic field dependence of elastic and inelastic scattering cross sections at ultracold temperatures is dominated by a manifold of Feshbach resonances with the density of ∼100 resonances per Tesla for collisions of molecules in the absolute ground state. This suggests that the scattering length of ultracold molecules in the absolute ground state can be effectively tuned in a very wide range of magnetic fields. Our calculations demonstrate that the number and properties of the magnetic Feshbach resonances are dramatically different for molecules in the absolute ground and excited spin states. The density of Feshbach resonances for molecule–molecule scattering in the low-field-seeking Zeeman state is reduced by a factor of 10.

Direct evaporative cooling ofK41into a Bose-Einstein condensate

We have investigated the collisional properties of $^{41}\text{K}$ atoms at ultracold temperatures. To demonstrate the possibility of using $^{41}\text{K}$ as a coolant, a Bose-Einstein condensate of $^{41}\text{K}$ atoms in the stretched state $(F=2,{m}_{F}=2)$ was created by direct evaporative cooling in a magnetic trap. An upper bound of the three-body loss coefficient for atoms in the condensate was determined to be $4(2)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}29}\text{ }{\text{cm}}^{\ensuremath{-}6}\text{ }{\text{s}}^{\ensuremath{-}1}$. A Feshbach resonance in the $F=1,\text{ }{m}_{F}=\ensuremath{-}1$, state was observed at 51.35(10) G, which is in good agreement with theoretical prediction.

Calculation of the elastic collision properties of Na and Li atoms at ultracold temperature

This paper firstly reports a theoretical study of elastic scattering properties in a mixture of 23Na and 7Li atoms at cold and ultracold temperatures in detail. Based on the new constructed accurate singlet X1 Σ+g and the triplet α3Σ+u states interatomic potentials for 23Na7Li mixture, it calculates the scattering lengths and the effective ranges by three computational methods, and obtains good agreements. Using the mass scaling method, it also calculates 23Na6Li scattering lengths and s-wave and total elastic cross sections, whose rich resonance structures were found and interpreted in terms of quasibound diatomic levels trapped behind a centrifugal barrier.

Probing Interactions Between Ultracold Fermions

At ultracold temperatures, the Pauli exclusion principle suppresses collisions between identical fermions. This has motivated the development of atomic clocks with fermionic isotopes. However, by probing an optical clock transition with thousands of lattice-confined, ultracold fermionic strontium atoms, we observed density-dependent collisional frequency shifts. These collision effects were measured systematically and are supported by a theoretical description attributing them to inhomogeneities in the probe excitation process that render the atoms distinguishable. This work also yields insights for zeroing the clock density shift.

Magnetic-field-induced interference of scattering states in ultracold collisions

We propose a general method to induce interference between scattering wave functions in atomic and molecular collisions at ultracold temperatures by using a static magnetic field. The scheme is based on the preparation of collision partners in coherent superpositions of Zeeman states. The magnetic field is used to induce interference between two incoming channels. As an illustrative example, we consider ultracold collisions between $^{7}\mathrm{Li}$ and $^{133}\mathrm{Cs}$ atoms, and show that ratios of state resolved collision cross sections can be enhanced by engineering the preparation of the initial coherent superpositions.

Creating ultracold molecules by collisions with ultracold rare-gas atoms in an optical trap

We study collisions of para-${\mathrm{H}}_{2}$ with five rare-gas atomic species (He, Ne, Ar, Kr, and Xe) over the range from $1\phantom{\rule{0.3em}{0ex}}\mathrm{K}\phantom{\rule{0.3em}{0ex}}\text{to}\phantom{\rule{0.3em}{0ex}}1\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{K}$ and evaluate the feasibility of sympathetic cooling ${\mathrm{H}}_{2}$ with ultracold ground state rare-gas atoms co-trapped within a deep optical trap. Collision cross sections over this large temperature range show that all of these species could be used to cool ${\mathrm{H}}_{2}$ to ultracold temperatures and that argon and helium are the most promising species for future experiments. A simple yet accurate method for calculating the microscopic observables needed in the present analysis is also described, as well as the sensitivity of the calculated cross sections to the potential energy surface used.

Optical lattice clocks with non-interacting bosons and fermions

Quantum statistics fundamentally controls the way particles interact; bosons tend to bunch together, whereas fermions repulse each other. As a consequence, statistically different isotopes are found in different macroscopic quantum states at ultracold temperatures. This is related to the total atomic spin, which forces atoms to couple to ambient fields. In designing high-precision atomic clocks that operate at a fractional uncertainty of 10−15 or less, quantum statistics and therefore the spins of the interrogated atoms have an essential role in determining the clocks’ ultimate performance. Here, we discuss the design of optical lattice clocks in view of the quantum statistics and lattice geometries. We propose two configurations that both make the interrogated atoms non-interacting: spin-polarized fermions in a one-dimensional (1D) and bosons in a 3D lattice. A 3D clock with bosonic 88Sr is demonstrated for the first time, in addition to a 1D clock with fermionic 87Sr. The sequential operation of the two clocks enables us to evaluate the clock stability with an uncertainty below 1×10−15 and to determine the isotope shift with significant reduction of the uncertainty related to atomic collisions. Optical lattice clocks, in which trapped atoms serve as a frequency reference, are promising candidates for next-generation atomic clocks. Depending on whether bosons or fermions are loaded into the lattice, fundamentally different design principles apply, as has now been shown.