It is demonstrated that elastic collisions of ultracold atoms forming a heteronuclear collision complex can be manipulated by laboratory practicable dc electric fields. The mechanism of electric field control is based on the interaction of the instantaneous dipole moment of the collision pair with external electric fields. It is shown that this interaction is dramatically enhanced in the presence of a p-wave shape or Feshbach scattering resonance near the collision threshold, which leads to novel electric-field-induced Feshbach resonances.
We present expressions demonstrating that collisional decoherence of ultracold atoms or molecules in a coherent superposition of non-degenerate quantum states is suppressed when both the real and imaginary parts of the scattering lengths for the states in the coherent superposition are equal. We show that the rate of collisional decoherence can be enhanced or suppressed by varying an external magnetic field near a Feshbach resonance. For some resonances, the suppression is very dramatic. We propose a method for measuring the scattering length of ultracold particles in excited quantum states ex…
We discuss the properties of Rydberg atoms in a magnetic Ioffe-Pritchard trap being commonly used in ultracold atomic physics experiments. The Hamiltonian is derived and it is demonstrated how tight traps alter the coupling of the atom to the magnetic field. We solve the underlying Schroedinger equation of the system within a given n-manifold and show that for a sufficiently large Ioffe field strength the 2n^2-dimensional system of coupled Schroedinger equations decays into several decoupled multicomponent equations governing the center of mass motion. An analysis of the fully quantized center…
We show that ultracold chemical reactions can be manipulated and controlled by using Rydberg-dressed interactions. Scattering in the ultracold regime is sensitive to long-range interactions, especially when weakly bound (or quasi-bound) states exist near the collision threshold. We investigate how, by Rydberg-dressing a reactant, one enhances its polarizability and modifies the long-range van der Waals collision complex, which can alter chemical reaction rates by shifting the position of near threshold bound states. We carry out a full quantum mechanical scattering calculation for the benchmar…
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…
Ultracold molecules trapped in optical tweezers show great promise for the implementation of quantum technologies and precision measurements. We study a prototypical scenario where two interacting polar molecules placed in separate traps are controlled using an external electric field. This, for instance, enables a quantum computing scheme in which the rotational structure is used to encode the qubit states. We estimate the typical operation timescales needed for state engineering to be in the range of few microseconds. We further underline the important role of the spatial structure of the tw…
Interactions in a spin-polarized ultracold Fermi gas are governed by $p$-wave collisions and can be characterized by the $p$-wave scattering volume. Control of these collisions by Feshbach resonances is hampered by huge inelastic losses. Here, we suggest non-resonant light control of $p$-wave collisions, exploiting the anisotropic coupling of non-resonant light to the polarizability of the atoms. The $p$-wave scattering volume can be controlled by strong non-resonant light, in close analogy to the $s$-wave scattering length. For collision partners that are tightly trapped, the non-resonant lig…
We demonstrate coherent control of both the rotational and hyperfine state of ultracold, chemically stable $^{87}$Rb$^{133}$Cs molecules with external microwave fields. We create a sample of ~2000 molecules in the lowest hyperfine level of the rovibronic ground state N = 0. We measure the transition frequencies to 8 different hyperfine levels of the N = 1 state at two magnetic fields ~23 G apart. We determine accurate values of rotational and hyperfine coupling constants that agree well with previous calculations. We observe Rabi oscillations on each transition, allowing complete population tr…
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…
Heavy polar diatomic molecules are the leading candidates in searches for the permanent electric dipole moment of the electron (eEDM). Next-generation eEDM search experiments ideally require extremely large coherence times, in large ensembles of trapped molecules that have a high sensitivity to the eEDM. We consider a family of molecules, mercury-alkali diatomics, that can be feasibly produced from ultracold atoms. We present calculations of the effective electric fields experienced by the electron in these molecules. The combination of reasonably large effective electric fields, and a straigh…
By applying a circularly polarized and slightly blue-detuned microwave field with respect to the first excited rotational state of a dipolar molecule, one can engineer a long-range, shallow potential well in the entrance channel of the two colliding partners. As the applied microwave ac-field is increased, the long-range well becomes deeper and can support a certain numbers of bound states, which in turn bring the value of the molecule-molecule scattering length from a large negative value to a large positive one. We adopt an adimensional approach where the molecules are described by a rescale…
We demonstrate one-dimensional sub-Doppler laser cooling of a beam of YbF molecules to 100 $μ$K. This is a key step towards a measurement of the electron's electric dipole moment using ultracold molecules. We compare the effectiveness of magnetically-assisted and polarization-gradient sub-Doppler cooling mechanisms. We model the experiment and find good agreement with our data.
While attaining external field control of bimolecular chemical reactions has long been a coveted goal of physics and chemistry, the role of hyperfine interactions and dc magnetic fields in achieving such control has remained elusive. We develop an extended coupled-channel statistical theory of barrierless atom-diatom chemical reactions, and apply it to elucidate the effects of magnetic fields and hyperfine interactions on the ultracold chemical reaction Li($^2\text{S}_{1/2}$) + CaH($^2Σ^+$) $\to$ LiH($^1Σ^+$) + Ca($^1\text{S}_{0}$) on a newly developed set of ab initio potential energy surface…
Magnetically tunable Feshbach resonances for polar paramagnetic ground-state diatomics are too narrow to allow for magnetoassociation starting from trapped, ultracold atoms. We show that non-resonant light can be used to engineer the Feshbach resonances in their position and width. For non-resonant field strengths of the order of $10^9\,$W/cm$^2$, we find the width to be increased by three orders of magnitude, reaching a few Gauss. This opens the way for producing ultracold molecules with sizeable electric and magnetic dipole moments and thus for many-body quantum simulations with such particl…
Permanent electric dipole moments (EDMs) of fundamental particles such as the electron are signatures of parity and time-reversal violation due to physics beyond the standard model. EDM measurements probe new physics at energy scales well beyond the reach of present-day colliders. Recent advances in assembling molecules from ultracold atoms have opened up new opportunities for improving the reach of EDM experiments. But better measurement techniques, that are not limited by the magnetic field sensitivity of such molecules, are necessary before these opportunities can be fully exploited. We pre…
We consider ultracold collisions of polar molecules confined in a one dimensional optical lattice. Using a quantum scattering formalism and a frame transformation method, we calculate elastic and chemical quenching rate constants for fermionic molecules. Taking KRb molecules as a prototype, we find that the rate of quenching collisions is enhanced at zero electric field as the confinement is increased, but that this rate is suppressed when the electric field is turned on. For molecules with 500 nK of collision energy, for realistic molecular densities, and for achievable experimental electric …
We consider collisions of electric and magnetic polar molecules, taking the OH radical as an example, subject to combined electric and magnetic static fields. We show that the relative orientation of the fields has an important effect on the collision processes for different fields magnitude at different collision energies. This is due to the way the molecules polarize in the combined electric and magnetic fields and hence the way the electric dipole-dipole interaction rises. If OH molecules are confined in magnetic quadrupole traps and if an electric field is applied, molecular collisions wil…
We study the effects of a static electric field on the photoassociation of a heteronuclear atom-pair into a polar molecule. The interaction of permanent dipole moment with a static electric field largely affects the ground state continuum wave function of the atom-pair at short separations where photoassociation transitions occur according to Franck-Condon principle. Electric field induced anisotropic interaction between two heteronuclear ground state atoms leads to scattering resonances at some specific electric fields. Near such resonances the amplitude of scattering wave function at short s…
The scattering length is commonly used to characterize the strength of ultracold atomic interactions, since it is the leading parameter in the low-energy expansion of the scattering phase shift. Its value can be modified via a magnetic field, by using a Feshbach resonance. However, the effective range term, which is the second parameter in the phase shift expansion, determines the width of the resonance and gives rise to important properties of ultracold gases. Independent control over this parameter is not possible by using a magnetic field only. We demonstrate that a combination of magnetic …
The prospects for shielding ultracold, paramagnetic, dipolar molecules from inelastic and chemical collisions are investigated. Molecules placed in their first rotationally excited states are found to exhibit effective long-range repulsion for applied electric fields above a certain critical value, as previously shown for non-paramagnetic molecules. This repulsion can safely allow the molecules to scatter while reducing the risk of inelastic or chemically reactive collisions. Several molecular species of $^2Σ$ molecules of experimental interest -- RbSr, SrF, BaF, and YO -- are considered, and …
We report the observation of dipole-forbidden, but quadrupole-allowed, one-photon transitions to high Rydberg states in Rb. Using pulsed UV excitation of ultracold atoms in a magneto-optical trap, we excite $5s \to nd$ transitions over a range of principal quantum numbers $n=27-59$. Compared to dipole-allowed (E1) transitions from $5s \to np$, these E2 transitions are weaker by a factor of approximately 2000. We also report measurements of the anomalous $np_{3/2} : np_{1/2}$ fine-structure transition strength ratio for $n=28-75$. Both results are in agreement with theoretical predictions.
Electrons in an expanding ultracold plasma are expected to be in quasi-equilibrium, since the collision times are short compared to the plasma lifetime, yet we observe electrons evaporating out as the ion density decreases during expansion. We observe that a small electric field that shifts the electron cloud with respect to the ions increases the evaporation rate. We have calculated the spatial distribution of a zero-temperature electron cloud as a function of applied field and ion density, which is assumed to be Gaussian at all times. This calculation allows us to predict the flux of cold el…
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 -> …
Trapped ultracold neutrons (UCN) have for many years been the mainstay of experiments to search for the electric dipole moment (EDM) of the neutron, a critical parameter in constraining scenarios of new physics beyond the Standard Model. Because their energies are so low, UCN preferentially populate the lower region of their physical enclosure, and do not sample uniformly the ambient magnetic field throughout the storage volume. This leads to a substantial increase in the rate of depolarization, as well as to shifts in the measured frequency of the stored neutrons. Consequences for EDM measure…
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 rela…
We propose a new method to produce an electric and magnetic dipolar gas of ultracold dysprosium atoms. The pair of nearly degenerate energy levels of opposite parity, at 17513.33 cm$^{-1}$ with electronic angular momentum $J=10$, and at 17514.50 cm$^{-1}$ with $J=9$, can be mixed with an external electric field, thus inducing an electric dipole moment in the laboratory frame. For field amplitudes relevant to current-day experiments, we predict a magnetic dipole moment up to 13 Bohr magnetons, and an electric dipole moment up to 0.22 Debye, which is similar to the values obtained for alkali-met…
We theoretically study collisions between ultracold polar molecules that are polarized by microwave or static electric fields. We systematically study the dependence on field strength, microwave polarization, and detuning from rotational transitions. We calculate the loss in two-body collisions that is observable experimentally and compare to the results expected for purely first-order dipolar interactions. For ground state molecules polarized by a static electric field, the dynamics are accurately described by first-order dipolar interactions. For microwave dressing, instead, resonant dipolar…
Spin-orbit coupling (SOC) is an essential ingredient in topological materials, conventional and quantum-gas based alike.~Engineered spin-orbit coupling in ultracold atom systems --unique in their experimental control and measurement opportunities-- provides a major opportunity to investigate and understand topological phenomena.~Here we experimentally demonstrate and theoretically analyze a technique for controlling SOC in a two component Bose-Einstein condensate using amplitude-modulated Raman coupling.
We present a time-independent quantum formalism to describe the dynamics of molecules with permanent electric dipole moments in a two-dimensional confined geometry such as a one-dimensional optical lattice, in the presence of an electric field. Bose/Fermi statistics and selection rules play a crucial role in the dynamics. As examples, we compare the dynamics of confined fermionic and bosonic polar KRb molecules under different confinements and electric fields. We show how chemical reactions can be suppressed, either by a "statistical suppression" which applies for fermions at small electric fi…
We report on a measurement of the characteristic temperature of an ultracold rubidium ion source, in which a cloud of laser-cooled atoms is converted to ions by photo-ionization. Extracted ion pulses are focused on a detector with a pulsed-field technique. The resulting experimental spot sizes are compared to particle-tracking simulations, from which a source temperature $T = (1 \pm 2)$ mK and the corresponding transversal reduced emittance $ε_r = 7.9 X 10^{-9}$ m rad $\sqrt{\rm{eV}}$ are determined. We find that this result is likely limited by space charge forces even though the average numb…
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…
We theoretically study the dynamics of a trapped ion that is immersed in an ultracold gas of weakly bound atomic dimers created by a Feshbach resonance. Using quasi-classical simulations, we find a crossover from dimer dissociation to molecular ion formation depending on the binding energy of the dimers. The location of the crossover strongly depends on the collision energy and the time-dependent fields of the Paul trap. Deeply bound dimers lead to fast molecular ion formation, with rates approaching the Langevin collision rate $Γ'_\text{L}\approx4.8\times10^{-9}\,$cm$^3$s$^{-1}$. The kinetic …
Selection of "magic" trapping conditions with ultracold atoms or molecules, where pairs of internal states experience identical trapping potentials, brings substantial benefits to precision measurements and quantum computing schemes. Working at such conditions could ensure that detrimental effects of inevitable inhomogeneities across an ultracold sample are significantly reduced. However, this aspect of confinement remains unexplored for ultracold polar molecules. Here, we present means to control the AC Stark shift of rotational states of ultracold polar molecules, when subjected to both trap…
We describe a method for controlling many-body states in extended ensembles of Rydberg atoms, forming crystalline structures during laser excitation of a frozen atomic gas. Specifically, we predict the existence of an excitation number staircase in laser excitation of atomic ensembles into Rydberg states. Each step corresponds to a crystalline state with a well-defined of regularly spaced Rydberg atoms. We show that such states can be selectively excited by chirped laser pulses. Finally, we demonstarte that, sing quantum state transfer from atoms to light, such crystals can be used to create c…
We calculate pair potential curves for interacting Rydberg atoms in a constant electric field and use them to determine the effective $C_3$ dipole-dipole and $C_6$ van der Waals coefficients. We compare the $C_3$ and $C_6$ with experiments where the angle of a polarizing electric field is varied with respect to the axis of a quasi-1-dimensional trap at ultracold temperatures. The dipoles produced via polarization of the atoms have an angular dependent dipole-dipole interaction. We focus on the interaction potential of two rubidium Rydberg atoms in $50S_{1/2}$ states in the blockade regime. For…
Using a recently developed method for precisely controlling collision energy, we observe a dramatic suppression of inelastic collisions between an atom and ion (Ca + Yb$^+$) at low collision energy. This suppression, which is expected to be a universal phenomenon, arises when the spontaneous emission lifetime of the excited state is comparable to or shorter than the collision complex lifetime. We develop a technique to remove this suppression and engineer excited-state interactions. By dressing the system with a strong catalyst laser, a significant fraction of the collision complexes can be ex…
Controlling rovibrational state populations of polar molecules in inhomogeneous electric fields of the Stark deceleration: molecular dynamics and quantum chemistry simulations
We consider ultracold collisions of ground-state, heteronuclear alkali dimers that are susceptible to four-center chemical reactions 2 AB -> A2 + B2 even at sub-microKelvin temperature. These reactions depend strongly on species, temperature, electric field, and confinement in an optical lattice. We calculate ab initio van der Walls coefficients for these interactions, and use a quantum formalism to study the scattering properties of such molecules under an external electric field and optical lattice. We also apply a quantum threshold model to explore the dependence of reaction rates on the va…
Arrays of trapped ultracold molecules represent a promising platform for implementing a universal quantum computer. DeMille has detailed a prototype design based on Stark states of polar $^1Σ$ molecules as qubits. Herein, we consider an array of polar $^2Σ$ molecules which are, in addition, inherently paramagnetic and whose Hund's case (b) free-rotor states are Bell states. We show that by subjecting the array to combinations of concurrent homogeneous and inhomogeneous electric and magnetic fields, the entanglement of the array's Stark and Zeeman states can be tuned and the qubit sites address…
Ultracold collisions of LiO molecules in the $^{2}Π_{3/2}$ ground state are considered, under the influence of either an external magnetic or electric field. Inelastic collisions are shown to be suppressed in the presence of modest laboratory strength magnetic and electric fields. The rate of elastic collisions that rethermalize the thermal distribution, and the corresponding low rate of heating state-changing collisions, suggest that quantum degeneracy or even molecular Bose-Einstein condensation of LiO gas may be attainable, provided that the initial temperatures in the milliKelvin range are…
We investigate the prospects of controlling charge-exchange in ultracold collisions of heteroisotopic combinations of atoms and ions of the same element. The treatment, readily applicable to alkali or alkanine-earth metals, is illustrated in the process $^9$Be$^{+}$ + $^{10}$Be $\leftrightarrow$ $^{9}$Be + $^{10}$Be$^{+}$, which exhibits favorable electronic, nuclear, and hyperfine structure. Feshbach resonances are obtained from quantum scattering calculations in a standard coupled-channel formalism with non-BO terms originating from the nuclear kinetic operator. Near a narrow resonance predi…
We report on hyperfine-resolved spectroscopic measurements of the electric-dipole forbidden 5$p_{3/2} \to 8p_{1/2}$ transition in a sample of ultracold $^{87}$Rb atoms. The hyperfine selection rules enable the weak magnetic-dipole (M1) contribution to the transition strength to be distinguished from the much stronger electric-quadrupole (E2) contribution. An upper limit on the M1 transition strength is determined that is about 50 times smaller than an earlier experimental determination. We also calculate the expected value of the M1 matrix element and find that it is less than the upper limit …
We investigate the Bose-Einstein condensation (BEC, superfluidity) of particle-hole pairs in ultracold Fermionic atoms with repulsive interactionsand arbitrary polarization, which are trapped within optical lattices. Near a Feshbach resonance, the dynamics of particle-hole pairs can be described by a hard-core Bose-Hubbard model. The insulator - superfluid and charge-density-wave (CDW) - superfluid phase transitions can be induced by decreasing and increasing the potential depths with controlling the trapping laser intensity, respectively. The parameter and polarization dependence of the criti…
The properties of the electronic ground state of the polar and paramagnetic chromium--closed-shell-atom molecules have been investigated. State-of-the-art \textit{ab initio} techniques have been applied to compute the potential energy curves for the chromium--alkaline-earth-metal-atom, CrX (X = Be, Mg, Ca, Sr, Ba), and chromium--ytterbium, CrYb, molecules in the Born-Oppenheimer approximation for the $X^7Σ^+$ high-spin electronic ground state. The spin restricted open-shell coupled cluster method restricted to single, double, and noniterative triple excitations, RCCSD(T), was employed and the …
The dipolar collision between ultracold polar molecules is an important topic both by its own right from the fundamental point of view and for the successful exploration of many-body physics with strong and long-range dipolar interactions. Here, we report the investigation of collisions between ultracold ground-state sodium-rubidium molecules in electric fields with induced electric dipole moments as large as 0.7$\;$D. We observe a step-wise enhancement of losses due to the coupling between different partial waves induced by the increasingly stronger anisotropic dipolar interactions. Varying t…
We report the observation of coherent heteronuclear spin dynamics driven by inter-species spin-spin interaction in an ultracold spinor mixture, which manifests as periodical and well correlated spin oscillations between two atomic species. In particular, we investigate the magnetic field dependence of the oscillations and find a resonance behavior which depends on {\em both} the linear and quadratic Zeeman effects and the spin-dependent interaction. We also demonstrate a unique knob for controlling the spin dynamics in the spinor mixture with species-dependent vector light shifts. Our finds ar…
The Ca$^+$, Sr$^+$, Ba$^+$, and Yb$^+$ ions immersed in an ultracold gas of the Cr atoms are proposed as experimentally feasible heteronuclear systems in which ion-atom interactions at ultralow temperatures can be controlled with magnetically tunable Feshbach resonances without charge transfer and radiative losses. \textit{Ab initio} techniques are applied to investigate electronic-ground-state properties of the (CaCr)$^+$, (SrCr)$^+$, (BaCr)$^+$, and (YbCr)$^+$ molecular ions. The potential energy curves, permanent electric dipole moments, and static electric dipole polarizabilities are compu…
Understanding and controlling collisions is crucial to the burgeoning field of ultracold molecules. All experiments so far have observed fast loss of molecules from the trap. However, the dominant mechanism for collisional loss is not well understood when there are no allowed 2-body loss processes. Here we experimentally investigate collisional losses of nonreactive ultracold RbCs molecules, and compare our findings with the sticky collision hypothesis that pairs of molecules form long-lived collision complexes. We demonstrate that loss of molecules occupying their rotational and hyperfine gro…
We briefly introduce the formalism for describing dipolar molecules in an ultracold gaseous environment. This treatment includes the quantum mechanical states of the dipoles, the electric fields they produce, and their interactions with one another.
We investigate the properties of two interacting ultracold polar molecules described as distinguishable quantum rigid rotors, trapped in a one-dimensional harmonic potential. The molecules interact via a multichannel two-body contact potential, incorporating the short-range anisotropy of intermolecular interactions including dipole-dipole interaction. The impact of external electric and magnetic fields resulting in Stark and Zeeman shifts of molecular rovibrational states is also investigated. Energy spectra and eigenstates are calculated by means of the exact diagonalization. The importance a…
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 exper…
