A general scheme for rotational cooling of diatomic heteronuclear molecules is proposed. It uses a superconducting microwave cavity to enhance the spontaneous decay via Purcell effect. Rotational cooling can be induced by sequentially tuning each rotational transition to cavity resonance, starting from the highest transition level to the lowest using an electric field. Electrostatic multipoles can be used to provide large confinement volume with essentially homogeneous background electric field.
The ground electronic, vibrational and rotational state of the OH molecule is currently of interest as it can be manipulated by electric and magnetic fields for experimental studies in ultracold chemistry and quantum degeneracy. Based on our recent exact solution of the corresponding effective Stark-Zeeman Hamiltonian, we present an analytical study of the crossings and avoided crossings in the spectrum. These features are relevant to non-adiabatic transitions, conical intersections and Berry phases. Specifically, for an avoided crossing employed in the evaporative cooling of OH, we compare ou…
We propose a method to read-out the spin-state of an electron in a quantum dot in a Voigt geometry magnetic field using cycling transitions induced by the AC Stark effect. We show that cycling transitions can be made possible by a red-detuned, circularly-polarized laser, which modifies the spin eigenstates and polarization selection rules via the AC Stark effect. A Floquet-Liouville supermatrix approach is used to calculate the time-evolution of the density matrix under the experimental conditions of a spin read-out operation. With an overall detection efficiency of 2.5%, the read-out is a sin…
Proposals for quantum computing using rotational states of polar molecules as qubits have previously considered only diatomic molecules. For these the Stark effect is second-order, so a sizable external electric field is required to produce the requisite dipole moments in the laboratory frame. Here we consider use of polar symmetric top molecules. These offer advantages resulting from a first-order Stark effect, which renders the effective dipole moments nearly independent of the field strength. That permits use of much lower external field strengths for addressing sites. Moreover, for a parti…
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 show that combined permanent and induced electric dipole interactions of polar and polarizable molecules with collinear electric fields lead to a sui generis topology of the corresponding Stark energy surfaces and of other observables - such as alignment and orientation cosines - in the plane spanned by the permanent and induced dipole interaction parameters. We find that the loci of the intersections of the surfaces can be traced analytically and that the eigenstates as well as the number of their intersections can be characterized by a single integer index. The value of the index, distinc…
Detecting the internal state of polar molecules is a substantial challenge when standard techniques such as resonance-enhanced multi photon ionization (REMPI) or laser-induced fluorescense (LIF) do not work. As this is the case for most polyatomic molecule species, we here investigate an alternative based on state selective removal of molecules from an electrically trapped ensemble. Specifically, we deplete molecules by driving rotational and/or vibrational transitions to untrapped states. Fully resolving the rotational state with this method can be a considerable challenge as the frequency di…
Stark deceleration enables the production of cold and dense molecular beams with applications in trapping, collisional studies, and precision measurement. Improving the efficiency of Stark deceleration, and hence the achievable molecular densities, is central to unlock the full potential of such studies. One of the chief limitations arises from the transverse focusing properties of Stark decelerators. We introduce a new operation strategy that circumvents this limit without any hardware modifications, and experimentally verify our results for hydroxyl radicals. Notably, improved focusing resul…
We experimentally study the optical- and terahertz- induced rotational dynamics of asymmetric molecules in the gas phase. Terahertz and optical fields are identified as two distinct control handles over asymmetric molecules, as they couple to the rotational degrees of freedom via the molecular- dipole and polarizability selectively. The distinction between those two rotational handles is highlighted by different types of quantum revivals observed in long duration (>100ps) field-free rotational evolution. The experimental results are in excellent agreement with Random Phase Wave Function simula…
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…
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…
The Stark resonance parameters for the $3a_{1}$ molecular orbital of H$_{2}$O are computed by solving a system of partial differential equations in spherical polar coordinates. The starting point of the calculation is the quantum potential derived for this orbital from a single-center expanded Hartree-Fock orbital. The resonance positions and widths are obtained after applying an exterior complex scaling technique to describe the ionization regime for external fields applied along the two distinct $\hat{z}$ directions associated with the symmetry axis. The procedure thus avoids the computation…
We study theoretically the collective dynamics of rotational excitations of polar molecules loaded into an optical lattice in two dimensions. These excitations behave as hard-core bosons with a relativistic energy dispersion arising from the dipolar coupling between molecules. This has interesting consequences for the collective many-body phases. The rotational excitations can form a Bose-Einstein condensate at non-zero temperature, manifesting itself as a divergent $T_2$ coherence time of the rotational transition even in the presence of inhomogeneous broadening. The dynamical evolution of a …
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 polar molecules trapped on an optical lattice is a many-body system that, under appropriate conditions, may support collective excitations reminiscent of excitons in solid state crystals. Here, we discuss the rotational excitations of molecules on an optical lattice leading to rotational Frenkel excitons. Apart from solid hydrogen, there is no other natural system that exhibits rotational excitons. The rotational excitons have unique properties that can be exploited for tuning non-linear exciton interactions and exciton-impurity scattering by applying an external electric field. We s…
We present single-molecule and macroscopic calculations showing that laser-induced Stark shifts contribute significantly to the phase of high-order harmonics from polar molecules. This is important for orbital tomography, where phases of field-free dipole matrix elements are needed in order to reconstruct molecular orbitals. We derive an analytical expression that allows the first-order Stark phase to be subtracted from experimental measurements.
We propose and analyze an electrostatic-optical nano-scale trap for cold diatomic polar molecules. The main ingredient of our proposal is an square-array of ferroelectric nano-rods {with alternating polarization}. We show that, in contrast to electrostatic traps using the linear Stark effect, a quadratic Stark potential supports long-lived trapped states. The molecules are kept at a fixed height from the nano-rods by a standing-wave optical dipole trap. For the molecules and materials considered, we find that nano-traps with trap frequency up to 1MHz, ground-state width $\sim20$nm with lattice…
We present precision spectroscopy on electrically trapped formaldehyde (H$_2$CO), demonstrating key attributes which will enable molecular spectroscopy with unprecedented precision. Our method makes use of a microstructured electric trap with homogeneous fields in the trap center and rotational transitions with minimal Stark broadening at a 'magic' offset electric field. Using molecules cooled to the low millikelvin temperature regime via optoelectrical Sisyphus cooling, we reduce Stark broadening on the $J=5\leftarrow4$ ($K=3$) transition at 364 GHz to well below 1 kHz, observe Doppler-limite…
We made use of supersymmetric (SUSY) quantum mechanics to find a condition under which the Stark effect problem for a polar and polarizable closed-shell diatomic molecule subject to collinear electrostatic and nonresonant radiative fields becomes exactly solvable. The condition, $Δω= \frac{ω^2}{4 (m+1)^2}$, connects values of the dimensionless parameters $ω$ and $Δω$ that characterize the strengths of the permanent and induced dipole interactions of the molecule with the respective fields. The exact solutions are obtained for the $|\tilde{J}=m,m;ω,Δω>$ family of "stretched" states. The field-f…
We conducted series of experiments on observing a Stark-type effect in superfluid $^4$He in presence of relative laminar flows of the normal and superfluid components. It is designed a measurement cell which allows us to simultaneously create hydrodynamic flows in the liquid and to carry out high-frequency radio-measurements at external electric field. We used a dielectric disk resonator that made possible to cover a wide frequency range. In our experiments it was registered the spectrum of the dielectric disk resonator modes, as well as narrow lines of absorption of a microwave radiation in H…
