In the perspective of the outstanding developments of high-precision measurements of fundamental constants using polar molecules related to ultimate checks of fundamental theories, we investigate the possibly counterproductive role of black-body radiation on a series of diatomic molecules which would be trapped and observed for long durations. We show that the absorption of black-body radiation at room temperature may indeed limit the lifetime of trapped molecules prepared in a well-defined quantum state. Several examples are treated, corresponding to pure rotational absorption, pure vibrational absorption or both. We also investigate the role of a black-body radiation-induced energy shift on molecular levels and how it could affect high-precision frequency measurements.
A new formalism and computer code, ASTRA (AttoSecond TRAnsitions), has been developed to treat the interactions of short, intense radiation with molecules. The formalism makes extensive use of transition density matrices, computed using a state-of-the-art quantum chemistry code (LUCIA), to efficiently calculate the many-body inter-channel-coupling interactions required to simulate the highly correlated electron dynamics due to atoms and molecules exposed to attosecond laser radiation.
A model for positron binding to polar molecules is considered by combining the dipole potential outside the molecule with a strongly repulsive core of a given radius. Using existing experimental data on binding energies leads to unphysically small core radii for all of the molecules studied. This suggests that electron-positron correlations neglected in the simple model play a large role in determining the binding energy. We account for these by including polarization potential via perturbation theory and non-perturbatively. The perturbative model makes reliable predictions of binding energies…
Photoelectron angular distributions (PADs) of oriented polar molecules in response to different polarized lasers are systematically investigated. It is found that the PADs of polar CO molecules show three distinct styles excited by linearly, elliptically and circularly polarized lasers respectively. In the case of elliptical polarization, a deep suppression is observed along the major axis and the distribution concentrates approximately along the minor axis. Additionally, it is also found that the concentrated distributions rotate clockwise as the ellipticity increases. Our investigation prese…
A systematic study of the leading isotropic van der Waals coefficients for the alkali-metal atom + molecule and molecule + molecule systems is presented. Dipole moments and static and dynamic dipole polarizabilities are calculated employing high-level quantum chemistry calculations. The dispersion, induction, and rotational parts of the isotropic van der Waals coefficient are evaluated. The known van der Waals coefficients are then used to derive characteristics essential for simple models of the collisions involving the corresponding ultracold polar molecules.
We solve the hydrodynamic-ballistic equations of motion for a one-dimensional time-dependent Thomas-Fermi model of Cl_2 exposed to an intense subpicosecond laser field, and observe simultaneous multielectron ionization and molecular dissociation. The fragment kinetic energy defect with respect to the simple Coulomb explosion picture is found to originate in ejected-electron screening of the escaping fragments; its magnitude agrees with that observed in recent experiments.
We explore one-dimensional (1-D) samples of ultracold polar molecules with attractive dipole-dipole interactions and show the existence of a repulsive barrier due to a strong quadrupole interaction between molecules. This barrier can stabilize a gas of ultracold KRb molecules and even lead to long-range wells supporting bound states between molecules. The properties of these wells can be controlled by external electric fields, allowing the formation of long polymer-like chains of KRb, and studies of quantum phase transitions by varying the effective interaction between molecules. We discuss th…
We demonstrate the production of ultracold polar RbCs molecules in their vibronic ground state, via photoassociation of laser-cooled atoms followed by a laser-stimulated state transfer process. The resulting sample of $X ^1Σ^+ (v=0)$ molecules has a translational temperature of $\sim100 μ$K and a narrow distribution of rotational states. With the method described here it should be possible to produce samples even colder in all degrees of freedom, as well as other bi-alkali species.
Optical pumping by blackbody radiation is a feature shared by all polar molecules and fundamentally limits the time that these molecules can be kept in a single quantum state in a trap. To demonstrate and quantify this, we have monitored the optical pumping of electrostatically trapped OH and OD radicals by room-temperature blackbody radiation. Transfer of these molecules to rotationally excited states by blackbody radiation at 295 K limits the $1/e$ trapping time for OH and OD in the $X^{2}Π_{3/2},v''=0,J''=3/2(f)$ state to 2.8 s and 7.1 s, respectively.
A highly sensitive, general, and preferably nondestructive technique to detect polar molecules would greatly advance a number of fields, in particular quantum science with cold and ultracold molecules. Here, we propose using resonant energy transfer between molecules and Rydberg atoms to detect molecules. Based on an energy transfer cross section of $>10^{-6}\,$cm$^2$ for sufficiently low collision energies, a near unit efficiency non-destructive detection of basically any polar molecule species in a well defined internal state should be possible.
The coherent radiation spectrum of two-level polar molecules with UV transition is studied at the multiphoton resonant excitation by a moderately strong laser field. The spectrum corresponding to harmonic generation and low-frequency radiation is investigated both analytically and numerically. Specifically, a mechanism for generation of intense smoothly tunable terahertz radiation by two-level molecular configurations (with dynamic Stark shifts) possessing permanent dipole moments, is considered.
The collisions between linear polar molecules, trapped in a microwave field with circular polarization, are theoretically analyzed. The microwave trap suggested by DeMille \cite{DeMille} seems to be rather advantageous in comparison with other traps. Here we have demonstrated that the microwave trap can provide a successful evaporative cooling for polar molecules in a rather broad range of frequencies of the AC-field. We suggested that not only ground state polar molecules but also molecules in some other states can be safely trapped. But the state in which molecules can be safely loaded and t…
We calculate the rate of the spontaneous magnetic dipole radiation transitions from ortho- to para-states of the hydrogen molecule at the room temperature with the radiation wavelengths about 0.01 - 0.1 cm. Exponentially small differences between the rotational energies and heat capacities of parahydrogen and orthohydrogen molecules and also diatomic molecules consisting of different hydrogen atoms for high temperatures are derived.
We demonstrate multiple photon cycling and radiative force deflection on the triatomic free radical strontium monohydroxide (SrOH). Optical cycling is achieved on SrOH in a cryogenic buffer-gas beam by employing the rotationally closed $P\left(N''=1\right)$ branch of the vibronic transition $\tilde{X}^{2}Σ^{+}\left(000\right)\leftrightarrow\tilde{A}^{2}Π_{1/2}\left(000\right)$. A single repumping laser excites the Sr-O stretching vibrational mode, and photon cycling of the molecule deflects the SrOH beam by an angle of $0.2^{\circ}$ via scattering of $\sim100$ photons per molecule. This approa…
Electric deflection measurements on liquid helium nanodroplets doped with individual polar molecules demonstrate that the cold superfluid matrix enables full orientation of the molecular dipole along the external field. This translates into a deflection force which is increased enormously by comparison with typical deflection experiments, and it becomes possible to measurably deflect neutral doped droplets with masses of tens to hundreds of thousands of Daltons. This approach permits preparation and study of continuous fluxes of fully oriented polar molecules and is broadly and generally appli…
We propose a method for sensitive parallel detection of low-frequency electromagnetic fields based on the fine structure interactions in paramagnetic polar molecules. Compared to the recently implemented scheme employing ultracold $^{87}$Rb atoms [B{ö}hi \textit{et al.}, Appl. Phys. Lett. \textbf{97}, 051101 (2010)], the technique based on molecules offers a 100-fold higher sensitivity, the possibility to measure both the electric and magnetic field components, and a probe of a wide range of frequencies from the dc limit to the THz regime.
The Formation of metastable molecules (Feshbach resonances) at the collision of two atoms and subsequent stimulated transition to a lower unbound electronic molecular state, with emission of a photon of the laser radiation has been investigated. This can develop, in particular, for $Rb_2$ molecules due to resonance scattering of two $Rb$ atoms. The considered process is a basis for the creation of excimer lasers. Expressions for the cross sections of elastic and inelastic resonance scattering and the intensity of the stimulated emission of the photons have been obtained.
A detailed treatment of an electro-optical trap for polar molecules, realized by embedding an optical trap within a uniform electrostatic field, is presented and the trap's properties analyzed and discussed. The electro-optical trap offers significant advantages over an optical trap that include an increased trap depth and conversion of alignment of the trapped molecules to marked orientation. Tilting the polarization plane of the optical field with respect to the electrostatic field diminishes both the trap depth and orientation and lifts the degeneracy of the $\pm M$ states of the trapped mo…
We discuss the possibility of trapping polar molecules in the standing-wave electromagnetic field of a microwave resonant cavity. Such a trap has several novel features that make it very attractive for the development of ultracold molecule sources. Using commonly available technologies, microwave traps can be built with large depth (up to several Kelvin) and acceptance volume (up to several cm^3), suitable for efficient loading with currently available sources of cold polar molecules. Unlike most previous traps for molecules, this technology can be used to confine the strong-field seeking abso…
We study the ionization dynamics of oriented HeH$^+$ in strong linearly-polarized laser fields by numerically solving the time-dependent Schrödinger equation. The calculated photoelectron momentum distributions for parallel orientation show a striking asymmetric structure. With a developed model pertinent to polar molecules, we trace the electron motion in real time. We show that this asymmetric structure arises from the interplay of the Coulomb effect and the permanent dipole in strong laser fields. This structure can be used to probe the degree of orientation which is important in ultrafast …
We perform a comprehensive investigation of Förster resonant energy transfer in a room-temperature thermal mixture of ammonia molecules and rubidium Rydberg atoms. Fully state-resolved measurement of the Rydberg-atom populations is achieved by combining millimeter-wave state transfer with state-selective field ionization. This allows aspects of the energy transfer process such as state dependence, ammonia pressure dependence, and dependence on the energy resonance condition to be investigated in detail. Our results pave the way for future quantum experiments combining polar molecules and Rydbe…
We determine trapping conditions for ultracold polar molecules, where pairs of internal states experience identical trapping potentials. Such conditions could ensure that detrimental effects of inevitable inhomogeneities across an ultracold sample are significantly reduced. In particular, we investigate the internal rovibronic and hyperfine quantum states of ultracold fermionic ground-state $^{40}$K$^{87}$Rb polar molecules, when static magnetic, static electric, and trapping laser fields are simultaneously applied. Understanding the effect of changing the relative orientation or polarization …
We demonstrate direct cooling of gaseous formaldehyde (H2CO) to the microkelvin regime. Our approach, optoelectrical Sisyphus cooling, provides a simple dissipative cooling method applicable to electrically trapped dipolar molecules. By reducing the temperature by three orders of magnitude and increasing the phase-space density by a factor of ~$10^4$ we generate an ensemble of $3\cdot10^5$ molecules with a temperature of about 420μK, populating a single rotational state with more than 80% purity.
We show that an ensemble of polar molecules trapped in an optical lattice can be considered as a controllable open quantum system. The coupling between collective rotational excitations and the motion of the molecules in the lattice potential can be controlled by varying the strength and orientation of an external DC electric field as well as the intensity of the trapping laser. The system can be described by a generalized Holstein Hamiltonian with tunable parameters and can be used as a quantum simulator of excitation energy transfer and polaron phenomena. We show that the character of excita…
A theoretical study of the rotational dynamics of a linear polar molecule in a two-color non-resonant cw laser field is presented. By systematically considering the interactions of this field with the electric dipole moment, polarizability and hyperpolarizability of the molecule, the effect of the symmetries of the Hamiltonian on the orientation and alignment is explored in a regime where the time-average approximation does not hold. It is shown that the alignment and orientation satisfy certain symmetries as a function of the phases and field strengths. On average a one-color cw laser field d…
We explore the electronic structure of ultralong-range pentaatomic Rydberg molecules from a merger of a Rydberg atom and two ground state heteronuclear diatomic molecules. Our focus is on the interaction of Rb($23s$) and Rb($n=20$, $l\ge 3$) Rydberg states with ground and rotationally excited KRb diatomic polar molecules. For symmetric and asymmetric configurations of the pentaatomic Rydberg molecule, we investigate the metamorphosis of the Born-Oppenheimer potential curves, essential for the binding of the molecule, with varying distance from the Rydberg core and analyze the alignment and ori…
We describe the realization of a dc electric-field trap for ultracold polar molecules, the thin-wire electrostatic trap (TWIST). The thin wires that form the electrodes of the TWIST allow us to superimpose the trap onto a magneto-optical trap (MOT). In our experiment, ultracold polar NaCs molecules in their electronic ground state are created in the MOT via photoassociation, achieving a continuous accumulation in the TWIST of molecules in low-field seeking states. Initial measurements show that the TWIST trap lifetime is limited only by the background pressure in the chamber.
The collisional stability of ultracold polar molecules in electrostatic traps is considered. Rate constants for collisions that drive molecules from weak-field-seeking to strong-field-seeking states are estimated using a simple model. The rates are found to be quite large, of order 10^{-12} - 10^{-10} cm^3/sec, and moreover to grow rapidly in an externally applied electric field. It is argued that these results are generic for polar molecules, and that therefore polar molecules should be trapped by other than electrostatic means.
We demonstrate loading of SrF molecules into an optical dipole trap (ODT) via in-trap $Λ$-cooling. We find that this cooling can be optimized by a proper choice of relative ODT and $Λ$ beam polarizations. In this optimized configuration, we observe molecules with temperatures as low as 14(1) $μ$K in traps with depths up to 570 $μ$K. With optimized parameters, we transfer $\!\sim\!5$% of molecules from our radio-frequency magneto-optical trap into the ODT, at a density of $\sim\!2\times 10^{9}$ cm$^{-3}$, a phase space density of $\sim\!2\times 10^{-7}$, and with a trap lifetime of $\!\sim\!1$ …
We study the possibility to use interaction between a polar molecule in the ground electronic and vibrational state and a Rydberg atom to construct two-qubit gates between molecular qubits and to coherently control molecular states. A polar molecule within the electron orbit in a Rydberg atom can either shift the Rydberg state, or form Rydberg molecule. Both the atomic shift and the Rydberg molecule states depend on the initial internal state of the polar molecule, resulting in molecular state dependent van der Waals or dipole-dipole interaction between Rydberg atoms. Rydberg atoms mediated in…
Focusing optics for neutral molecules finds application in shaping and steering molecular beams. Here we present an electrostatic elliptical mirror for polar molecules consisting of an array of microstructured gold electrodes deposited on a glass substrate. Alternating positive and negative voltages applied to the electrodes create a repulsive potential for molecules in low-field-seeking states. The equipotential lines are parallel to the substrate surface, which is bent in an elliptical shape. The mirror is characterized by focusing a beam of metastable CO molecules and the results are compar…
We explore the external electric field control of a species of ultralong-range molecules that emerge from the interaction of a ground state polar molecule with a Rydberg atom. The external field mixes the Rydberg electronic states and therefore strongly alters the electric field seen by the polar diatomic molecule due to the Rydberg electron. As a consequence, the adiabatic potential energy curves responsible for the molecular binding can be tuned in such a way that an intersection with neighboring curves occurs. The latter leads to admixture of s-wave character in the Rydberg wave function an…
The prospects of sympathetic cooling of polar molecules with magnetically co-trapped alkali-metal atoms are generally considered poor due to strongly anisotropic atom-molecule interactions leading to large spin relaxation rates. Using rigorous quantum scattering calculations based on ab initio interaction potentials, we show that inelastic spin relaxation in low-temperature collisions of CaH(2Sigma) molecules with Li and Mg atoms occurs at a slow rate despite the strongly anisotropic interactions. This unexpected result, which we rationalize using multichannel quantum defect theory, opens up t…
The present work reports on the generation of short-pulse coherent extreme ultraviolet radiation of controlled polarization. The proposed strategy is based on high-order harmonics generated in pre-aligned molecules. Field-free molecular alignment produced by a short linearly-polarized infrared laser pulse is used to break the isotropy of a gas medium. Driving the aligned molecules by a circularly-polarized infrared pulse allows to transfer the anisotropy of the medium to the polarization of the generated harmonic light. The ellipticity of the latter is controlled by adjusting the angular distr…
In the present work, we demonstrate the possibility of controlling by an external field the dynamics of collective excitations (excitons) of molecules on an optical lattice. We show that a suitably chosen two-species mixture of ultracold polar molecules loaded on an optical lattice forms a phononless crystal, where exciton-impurity interactions can be controlled by applying an external electric field. This can be used for the controlled creation of many-body entangled states of ultracold molecules and the time-domain quantum simulation of disorder-induced localization and delocalization of qua…
The internal electric field of a Rydberg atom electron can bind a polar molecule to form a giant ultralong-range stable polyatomic molecule. Such molecules not only share their properties with Rydberg atoms, they possess huge permanent electric dipole moments and in addition allow for coherent control of the polar molecule orientation. In this work, we include additional Rydberg manifolds which couple to the nearly degenerate set of Rydberg states employed in [S. T. Rittenhouse and H. R. Sadeghpour, Phys. Rev. Lett. 104, 243002 (2010)]. The coupling of a set of $(n+3)s$ Rydberg states with the…
We have produced ultracold, polar RbCs* molecules via photoassociation in a laser-cooled mixture of Rb and Cs atoms. Using a model of the RbCs* molecular interaction which reproduces the observed rovibrational structure, we infer decay rates in our experiments into deeply bound singlet ground state RbCs vibrational levels as high as 5 x 10^5 s^-1 per level. Population in such deeply bound levels could be efficiently transferred to the vibrational ground state using a single stimulated Raman transition, opening the possibility to create large samples of stable, ultracold polar molecules.
We predict that pairs of polar molecules can be weakly bound together in an ultracold environment, provided that a dc electric field is present. The field that links the molecules together also strongly influences the basic properties of the resulting dimer, such as its binding energy and predissociation lifetime. Because of their long-range character these dimers will be useful in disentangling cold collision dynamics of polar molecules. As an example, we estimate the microwave photoassociation yield for OH-OH cold collisions.
Because molecules can have their orientation locked when embedded into a solid rare-gas matrix, their hyperfine structure is strongly perturbed relative to the freely rotating molecule. The addition of an electric field further perturbs the structure, and fields parallel and antiparallel to the molecular orientation result in different shifts of the hyperfine structure. These shifts enable the selective detection of molecules with different orientations relative to the axes of a rare-gas crystal, which will be an important ingredient of an improved electron electric dipole moment measurement u…
We present theoretical calculations for polarization and ellipticity of high-order harmonics from aligned N$_2$, CO$_2$, and O$_2$ molecules generated by linearly polarized lasers. Within the rescattering model, the two polarization amplitudes of the harmonics are determined by the photo-recombination amplitudes for photons emitted parallel and perpendicular to the direction of the {\em same} returning electron wave packet. Our results show clear species-dependent polarization states, in excellent agreement with experiments. We further note that the measured polarization ellipse of the harmoni…
We explore the total cross section of ground state polar molecules in an electric field at various energies, focusing on RbCs and RbK. An external electric field polarizes the molecules and induces strong dipolar interactions leading to non-zero partial waves contributing to the scattering even as the collision energy goes to zero. This results in the need to compute scattering problems with many different values of total M to converge the total cross section. An accurate and efficient approximate total cross section is introduced and used to study the low field temperature dependence. To unde…
We present a detailed description on how to build a Thin WIre electroStatic Trap (TWIST) for ultracold polar molecules. It is the first design of an electrostatic trap that can be superimposed directly onto a magneto optical trap (MOT). We can thus continuously produce ultracold polar molecules via photoassociation from a two species MOT and instantaneously trap them in the TWIST without the need for complex transfer schemes. Despite the spatial overlap of the TWIST and the MOT, the two traps can be operated and optimized completely independently due to the complementary nature of the utilized…
We investigate the rovibrational population redistribution of polar molecules in the electronic ground state induced by spontaneous emission and blackbody radiation. As a model system we use optically trapped LiCs molecules formed by photoassociation in an ultracold two-species gas. The population dynamics of vibrational and rotational states is modeled using an ab-initio electric dipole moment function and experimental potential energy curves. Comparison with the evolution of the v"=3 electronic ground state yields good qualitative agreement. The analysis provides important input to assess ap…
State-dependent optical tweezers can be used to trap a pair of molecules with a separation much smaller than the wavelength of the trapping light, greatly enhancing the dipole-dipole interaction between them. Here we describe a general approach to producing these state-dependent potentials using the tensor part of the ac Stark shift and show how it can be used to carry out two-qubit gates between pairs of molecules. The method is applicable to broad classes of molecules including bialkali molecules produced by atom association and those amenable to direct laser cooling.
We demonstrate the deceleration of heavy polar molecules in low-field seeking states by combining a cryogenic source and a travelling-wave Stark decelerator. The cryogenic source provides a high intensity beam with low speed and temperature, and the travelling-wave decelerator provides large deceleration forces and high phase-space acceptance. We prove these techniques using YbF molecules and find the experimental data to be in excellent agreement with numerical simulations. These methods extend the scope of Stark deceleration to a very wide range of molecules.
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 proposed a general Zeeman slower scheme applicable to the majority of the laser-coolable molecules. Different from previous schemes, the key idea of our scheme lies in that the compensation of the detuning with the magnetic field is done for the repumping laser instead of the cooling laser. Only atoms or molecules with the right velocity will be repumped and laser slowed. Such scheme is more feasible for molecules with complex energy sturcutres. We apply this scheme for molecules with large Landé g-factor of the excited states and polyatomic molecules, and it shows a better slowing efficien…
We show that dressing polar molecules with a far-off-resonant optical field leads to new types of intermolecular potentials, which undergo a crossover from the inverse-power to oscillating behavior depending on the intermolecular distance, and whose parameters can be tuned by varying the laser intensity and wavelength. We present analytic expressions for the potential energy surfaces, thereby providing direct access to the parameters of an optical field required to design intermolecular interactions experimentally.
We investigate the use of microwave radiation to produce a repulsive shield between pairs of ultracold polar molecules and prevent collisional losses that occur when molecular pairs reach short range. We carry out coupled-channels calculations on RbCs+RbCs and CaF+CaF collisions in microwave fields. We show that effective shielding requires predominantly circular polarization, but can still be achieved with elliptical polarization that is around 90% circular.
Polar molecules are desirable systems for quantum simulations and cold chemistry. Molecular ions are easily trapped, but a bias electric field applied to polarize them tends to accelerate them out of the trap. We present a general solution to this issue by rotating the bias field slowly enough for the molecular polarization axis to follow but rapidly enough for the ions to stay trapped. We demonstrate Ramsey spectroscopy between Stark-Zeeman sublevels in 180Hf19F+ with a coherence time of 100 ms. Frequency shifts arising from well-controlled topological (Berry) phases are used to determine mag…
We analyze in detail the possibility to use charge-dipole interaction between a single polar molecule or a 1D molecular array and a single Rydberg atom to read out rotational populations. The change in the Rydberg electron energy is conditioned on the rotational state of the polar molecules, allowing for realization of a CNOT quantum gate between the molecules and the atom. Subsequent readout of the atomic fluorescence results in a non-destructive measurement of the rotational state. We study the interaction between a 1D array of polar molecules and an array or a cloud of atoms in a Rydberg su…
Fully internal and motional state controlled and individually manipulable polar molecules are desirable for many quantum science applications leveraging the rich state space and intrinsic interactions of molecules. While prior efforts at assembling molecules from their constituent atoms individually trapped in optical tweezers achieved such a goal for exactly one molecule, here we extend the technique to an array of five molecules, unlocking the ability to study molecular interactions. We detail the technical challenges and solutions inherent in scaling this system up. With parallel preparatio…
It has long been expected that quantum degenerate gases of molecules would open access to a wide range of phenomena in molecular and quantum sciences. However, the very complexity that makes ultracold molecules so enticing has made reaching degeneracy an outstanding experimental challenge over the past decade. We now report the production of a Fermi degenerate gas of ultracold polar molecules of potassium--rubidium (KRb). Through coherent adiabatic association in a deeply degenerate mixture of a rubidium Bose-Einstein condensate and a potassium Fermi gas, we produce molecules at temperatures b…
