We investigate theoretically the interaction of polar molecules with optical lattices and microwave fields. We demonstrate the existence of frequency windows in the optical domain where the complex internal structure of the molecule does not influence the trapping potential of the lattice. In such frequency windows the Franck-Condon factors are so small that near-resonant interaction of vibrational levels of the molecule with the lattice fields have a negligible contribution to the polarizability and light-induced decoherences are kept to a minimum. In addition, we show that microwave fields can induce a tunable dipole-dipole interaction between ground-state rotationally symmetric (J=0) molecules. A combination of a carefully chosen lattice frequency and microwave-controlled interaction between molecules will enable trapping of polar molecules in a lattice and possibly realize molecular quantum logic gates. Our results are based on ab initio relativistic electronic structure calculations of the polar KRb and RbCs molecules combined with calculations of their rovibrational motion.
We employ heterodyne interferometry to investigate the effect of a single organic molecule on the phase of a propagating laser beam. We report on the first phase-contrast images of individual molecules and demonstrate a single-molecule electro-optical phase switch by applying a voltage to the microelectrodes embedded in the sample. Our results may find applications in single-molecule holography, fast optical coherent signal processing, and single-emitter quantum operations.
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 consider deflection of polarizable molecules by inhomogeneous optical fields, and analyze the role of molecular orientation and rotation in the scattering process. It is shown that molecular rotation induces spectacular rainbow-like features in the distribution of the scattering angle. Moreover, by preshaping molecular angular distribution with the help of short and strong femtosecond laser pulses, one may efficiently control the scattering process, manipulate the average deflection angle and its distribution, and reduce substantially the angular dispersion of the deflected molecules. We pr…
We introduce a new scheme for controlling the sense of molecular rotation. By varying the polarization and the delay between two ultrashort laser pulses, we induce unidirectional molecular rotation, thereby forcing the molecules to rotate clockwise/counterclockwise under field-free conditions. We show that unidirectionally rotating molecules are confined to the plane defined by the two polarization vectors of the pulses, which leads to a permanent anisotropy in the molecular angular distribution. The latter may be useful for controlling collisional cross-sections and optical and kinetic proces…
Doubly dipolar molecules exhibit complex internal spin-dynamics when electric and magnetic fields are both applied. Near magnetic trap minima, these spin-dynamics lead to enhancements in Majorana spin-flip transitions by many orders of magnitude relative to atoms, and are thus an important obstacle for progress in molecule trapping and cooling. We conclusively demonstrate and address this with OH molecules in a trap geometry where spin-flip losses can be tuned from over $200 \text{ s}^{-1} $ to below our $2\text{ s}^{-1}$ vacuum limited loss rate with only a simple external bias coil and with …
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…
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…
We propose a new mechanism to produce ultracold polar molecules with microwave fields. The proposed mechanism converts trapped ultracold atoms of different species into vibrationally excited molecules by a single microwave transition and entirely depends on the existence of a permanent dipole moment in the molecules. As opposed to production of molecules by photoassociation or magnetic-field Feshbach resonances our method does not rely on the structure and lifetime of excited states or existence of Feshbach resonances. In addition, we determine conditions for optimal creation of polar molecule…
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…
The quantum state of motion of a large and rotating polar molecule can lose coherence through the collisions with gas atoms. We show how the associated quantum master equation for the center of mass can be expressed in terms of the orientationally averaged differential and total scattering cross sections, for which we provide approximate analytic expressions. The master equation is then utilized to quantify collisional decoherence in a interference experiment with polar molecules.
A new method is proposed to calculate the polarization vector of a molecule in a monochromatic external field in the anomalous-despersion domain. The method takes into account the instantaneous switching of the field. A simple modification of the method allows one to consider a more general switching procedure. As an illustration of the method Fourier components of the polarization vector of the LiH molecule in the anomalous -dispersion domain is calculated.
We theoretically investigate trapping conditions for ultracold polar molecules in optical lattices, when external magnetic and electric fields are simultaneously applied. Our results are based on an accurate electronic-structure calculation of the polar $^{23}$Na$^{40}$K polar molecule in its absolute ground state combined with a calculation of its rovibrational-hyperfine motion. We find that an electric field strength of $5.26(15)$ kV/cm and an angle of $54.7^\circ$ between this field and the polarization of the optical laser lead to a trapping design for $^{23}$Na$^{40}$K molecules where dec…
We propose an alternative scenario for the generation of entanglement between rotational quantum states of two polar molecules. This entanglement arises from dipole-dipole interaction, and is controlled by a sequence of laser pulses simultaneously exciting both molecules. We study the efficiency of the process, and discuss possible experimental implementations with cold molecules trapped in optical lattices or in solid matrices. Finally, various entanglement detection procedures are presented, and their suitability for these two physical situations is analyzed.
We study the influence of thermal Casimir-Polder forces on the near-surface trapping of cold polar molecules, with emphasis on LiH and YbF near an Au surface at room temperature. We show that for a molecule initially prepared in its electronic and rovibrational ground state, the Casimir-Polder force oscillates with the molecule-wall separation. The non-resonant force contribution and the evanescent part of the resonant force contribution almost exactly cancel at high temperature which results in a saturation of the (attractive) force in this limit. A dynamical calculation reveals how the spati…
We present a method to design a finite decay rate for excited rotational states in polar molecules. The setup is based on a hybrid system of polar molecules with atoms driven into a Rydberg state. The atoms and molecules are coupled via the strong dipolar exchange interaction between two rotation levels of the polar molecule and two Rydberg states. Such a controllable decay rate opens the way to optically pump the hyperfine levels of polar molecules and it enables the application of conventional laser cooling techniques for cooling polar molecules into quantum degeneracy.
Spin-dependent Kapitza-Dirac scattering of electron beams from counterpropagating bichromatic laser waves in various polarization geometries is studied. The corresponding scattering probabilities are obtained by analytical and numerical solutions of the time-dependent Dirac equation, assuming a field frequency ratio of 2. When the fundamental field mode is circular-polarized, we show that spin dynamics are generally suppressed at low intensities, but can become distinct at high intensities. Conversely, when a linearly or elliptically polarized fundamental mode is combined with a second harmoni…
We show that detuned optical pulse trains with a modest spectral width can polarize nuclear spins in InAs quantum dots. The pulse bandwidth is large enough to excite a coherent superposition of both electron spin eigenstates in these negatively charged dots but narrow enough to give partial spectral selectivity between the eigenstates. The coherent precession of electron spin states and periodic excitation focuses the nuclear spin distribution, producing a discrete set of precession modes. The spectral selectivity generates a net nuclear polarization, through a mechanism that relies on optical…
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 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…
In this study, we investigate the structure of the polar alkali-Strontium diatomic molecules as possible candidates for the realization of samples of new species of ultracold polar molecules. Using a quantum chemistry approach based on Effective Core Potentials and Core Polarization Potentials, we model these systems as effective three valence electron systems, allowing for calculation of electronic properties with Full Configuration Interaction. The potential curve and the permanent dipole moment of the $^2Σ^+$ ground state are determined as functions of the internuclear distances for LiSr, N…
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 -> …
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 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…
We present and analyze a toolbox for the controlled manipulation of ultracold polar molecules, consisting of detection of molecules, atom-molecule entanglement, and engineering of dissipative dynamics. Our setup is based on fast chemical reactions between molecules and atoms leading to a quantum Zeno-based collisional blockade in the system. We demonstrate that the experimental parameters for achieving high fidelities can be found using a straightforward numerical optimization. We exemplify our approach for a system comprised of NaK molecules and Na atoms and we discuss the consequences of res…
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.
Qubit coherence times are critical to the performance of any robust quantum computing platform. For quantum information processing using arrays of polar molecules, a key performance parameter is the molecular rotational coherence time. We report a 93(7) ms coherence time for rotational state qubits of laser cooled CaF molecules in optical tweezer traps, over an order of magnitude longer than previous systems. Inhomogeneous broadening due to the differential polarizability between the qubit states is suppressed by tuning the tweezer polarization and applied magnetic field to a "magic" angle. Th…
Recently, it was predicted theoretically and verified experimentally that a pair of delayed and cross-polarized short laser pulses can create molecular ensembles with a well defined sense of rotation (clockwise or counterclockwise). Here we provide a comparative study of the classical and quantum aspects of the underlying mechanism for linear molecules and for symmetric tops, like benzene molecules, that were used for the first experimental demonstration of the effect. Very good quantitative agreement is found between the classical description of the process and the rigorous quantum mechanical…
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.
We investigate cooperative phenomena and superradiance for vibrational transitions in polar molecule spectroscopy when a high optical-depth (OD) sample is studied. Such cooperativity comes from the build-up of inter-particle coherence through dipole-dipole interactions and leads to the speed-up of decay process. We compare our calculation to recent work [Deiglmayr et al., Eur. Phys. J. D 65, 99 (2011)] and find very good agreement, suggesting that superradiant effects need to be included in a wide variety of ultracold molecule setups including vibrational and rotational states.
In the mean-field theory, the stabilization of polar chiral molecules is understood as a quantum phase transition where the mean-field ground state of molecules changes from the achiral eigenstate of the molecular Hamiltonian to one of the degenerated chiral states as the increase of the intermolecular interaction. Starting from the many-body Hamiltonian of the molecular gases with electric dipole-dipole interactions, we give the static non-linear Schrödinger equations without free parameters to explore the achiral-chiral transitions of polar chiral molecules. We find that the polar chiral mol…
We study a system of polar dipolar fermions in a two-dimensional optical lattice and show that multi-band Fermi-Hubbard model is necessary to discuss such system. By taking into account both on-site, and long-range interactions between different bands, as well as occupation-dependent inter- and intra-band tunneling, we predict appearance of novel phases in the strongly-interacting limit.
Recent experiments showed that the chemical reaction rate is modified, either increased or decreased, by strongly coupling a nuclear vibration mode to the single mode of an optical cavity. Herein we investigate how the rate of an electron-transfer reaction depends on the molecule-cavity coupling in the ultrastrong coupling regime, where the coupling strength is comparable in magnitude with both the vibrational and the cavity frequencies. We found two main factors that determine the modification of the reaction rate: the relative shifts of the energy levels induced by the coupling and the mixin…
Scattering resonances are an essential tool for controlling interactions of ultracold atoms and molecules. However, conventional Feshbach scattering resonances, which have been extensively studied in various platforms, are not expected to exist in most ultracold polar molecules due to the fast loss that occurs when two molecules approach at a close distance. Here, we demonstrate a new type of scattering resonances that is universal for a wide range of polar molecules. The so-called field-linked resonances occur in the scattering of microwave-dressed molecules due to stable macroscopic tetramer…
Ultracold polar molecules are an ideal platform for studying many-body physics with long-range dipolar interactions. Experiments in this field have progressed enormously, and several groups are pursuing advanced apparatus for manipulation of molecules with electric fields as well as single-atom-resolved in situ detection. Such detection has become ubiquitous for atoms in optical lattices and tweezer arrays, but has yet to be demonstrated for ultracold polar molecules. Here we present a proposal for the implementation of quantum gas microscopy for polar molecules, and specifically discuss a tec…
We report the measurement of the anisotropic AC polarizability of ultracold polar $^{40}$K$^{87}$Rb molecules in the ground and first rotationally excited states. Theoretical analysis of the polarizability agrees well with experimental findings. Although the polarizability can vary by more than 30%, a "magic" angle between the laser polarization and the quantization axis is found where the polarizability of the $|N=0,m_N=0>$ and the $|N=1,m_N=0>$ states match. At this angle, rotational decoherence due to the mismatch in trapping potentials is eliminated, and we observe a sharp increase in the …
We apply a microscopic theory of exciton-polaritons in cavity-confined monolayer transition-metal dichalcogenides including both optical polarizations in the monolayer plane, allowing to describe how chiral cavity photons interact with the valley degrees of freedom of the active material. Upon polariton formation, the degenerate excitons inhabiting the two inequivalent valleys are shown to assume bonding and antibonding superpositions as a result of cavity-mediated intravalley interactions combined with intervalley Coulomb interactions. This is representative of a polariton-induced coherent mi…
We propose and analyze a technique that allows to suppress inelastic collisions and simultaneously enhance elastic interactions between cold polar molecules. The main idea is to cancel the leading dipole-dipole interaction with a suitable combination of static electric and microwave fields in such a way that the remaining van-der-Waals-type potential forms a three-dimensional repulsive shield. We analyze the elastic and inelastic scattering cross sections relevant for evaporative cooling of polar molecules and discuss the prospect for the creation of crystalline structures.
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…
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.
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 exploration of cold polar molecules in different geometries is a rapidly developing experimental and theoretical pursuit. Recently, the implementation of optical lattices has enabled confinement in stacks of planes, the number of which is also controllable. Here we consider the bound state structure of two polar molecules confined in two adjacent planes as function of the polarization angle of the dipole moment of the molecules. We prove analytically and present numerical evidence for the existence of bound states for arbitrary dipole moments and polarization directions in this two-dimensi…
