The large electric dipole moments associated with highly excited Rydberg states of atoms and molecules make gas-phase samples in these states very well suited to deceleration and trapping using inhomogeneous electric fields. The methods of Rydberg-Stark deceleration with which this can be achieved are reviewed here. Using these techniques, the longitudinal motion of beams of atoms and molecules moving at speeds as high as 2500~m/s have been manipulated, with changes in kinetic energy of up to $|ΔE_{\mathrm{kin}}|=1.3\times10^{-20}$~J ($|ΔE_{\mathrm{kin}}|/e=80$~meV or $|ΔE_{\mathrm{kin}}|/hc=650$~cm$^{-1}$) achieved, while decelerated and trapped samples with number densities of $10^6$--$10^7$~cm$^{-3}$ and translational temperatures of $\sim150$~mK have been prepared. Applications of these samples in areas of research at the interface between physics and physical chemistry are discussed.
Controlling rovibrational state populations of polar molecules in inhomogeneous electric fields of the Stark deceleration: molecular dynamics and quantum chemistry simulations
We report the Stark deceleration of CaF molecules in the strong-field seeking ground state and in a weak-field seeking component of a rotationally-excited state. We use two types of decelerator, a conventional Stark decelerator for the weak-field seekers, and an alternating gradient decelerator for the strong-field seekers, and we compare their relative merits. We also consider the application of laser cooling to increase the phase-space density of decelerated molecules.
We produce SO_2 molecules with a centre of mass velocity near zero using a Stark decelerator. Since the initial kinetic energy of the supersonic SO_2 molecular beam is high, and the removed kinetic energy per stage is small, 326 deceleration stages are necessary to bring SO_2 to a complete standstill, significantly more than in other experiments. We show that in such a decelerator possible loss due to coupling between the motional degrees of freedom must be considered. Experimental results are compared with 3D Monte-Carlo simulations and the quantum state selectivity of the Stark decelerator i…
The Stark deceleration of OH radicals in both low-field-seeking and high-field-seeking levels of the rovibronic ${}^2Π_{3/2},v=0,J=3/2$ ground state is demonstrated using a single experimental setup. Applying alternating-gradient focusing, OH radicals in their low-field-seeking ${}^2Π_{3/2},v=0,J=3/2,f$ state have been decelerated from 345 m/s to 239 m/s, removing 50 % of the kinetic energy using only 27 deceleration stages. The alternating-gradient decelerator allows to independently control longitudinal and transverse manipulation of the molecules. Optimized high-voltage switching sequences …
We have measured the AC-Stark shift of the $14D_{5/2}$ Rydberg state of rubidium 87 in an optical dipole trap formed by a focussed CO$_2$-laser. We find good quantitative agreement with the model of a free electron experiencing a ponderomotive potential in the light field. In order to reproduce the observed spectra we take into account the broadening of the Rydberg state due to photoionization. The extracted cross-section is compatible with previous measurements on neighboring Rydberg states.
Stark deceleration has been utilized for slowing and trapping several species of neutral, ground-state polar molecules generated in a supersonic beam expansion. Due to the finite physical dimension of the electrode array and practical limitations of the applicable electric fields, only molecules within a specific range of velocities and positions can be efficiently slowed and trapped. These constraints result in a restricted phase space acceptance of the decelerator in directions both transverse and parallel to the molecular beam axis; hence, careful modeling is required for understanding and …
We report on experiments exploring Stark-tuned Förster resonances between Rydberg atoms with unprecedented resolution in the Förster defect. The individual resonances are expected to exhibit different angular dependencies, opening the possibility to tune not only the interaction strength but also the angular dependence of the pair state potentials by an external electric field. We achieve a high resolution by optical Ramsey interferometry for Rydberg atoms combined with electric field pulses. The resonances are detected by a loss of visibility in the Ramsey fringes due to resonances in the int…
Nitric oxide (NO) molecules initially traveling at 795 m/s in pulsed supersonic beams have been photoexcited to long-lived hydrogenic Rydberg-Stark states, decelerated and electrostatically trapped in a cryogenically cooled, chip-based transmission-line Rydberg-Stark decelerator. The decelerated and trapped molecules were detected $in$ $situ$ by pulsed electric field ionization. The operation of the decelerator was validated by comparison of the experimental data with the results of numerical calculations of particle trajectories. Studies of the decay of the trapped molecules on timescales up …
Cold atoms in highly excited Rydberg states are promising candidates to implement quantum logic gates of a quantum computer via long-range dipole-dipole interaction. Two-qubit gates require a controlled interaction of only two close Rydberg atoms. We report on the first spectroscopic observation of the resonant dipole-dipole interaction between two cold rubidium Rydberg atoms confined in a small laser excitation volume. The interaction strength was controlled by fine-tuning of the Rydberg levels into a Forster resonance using the Stark effect. The observed resonance line shapes are in good agr…
Precision measurements of transitions between singlet ($S=0$) Rydberg states of H$_2$ belonging to series converging on the $\mathrm{X}^+\,^2Σ_g^+(v^+=0,N^+=0)$ state of H$_2^+$ have been carried out by millimetre-wave spectroscopy under field-free conditions and in the presence of weak static electric fields. The Stark effect mixes states with different values of the orbital-angular-momentum quantum number $\ell$ and leads to quadratic Stark shifts of low-$\ell$ states and to linear Stark shifts of the nearly degenerate manifold of high-$\ell$ states. Transitions to the Stark manifold were ob…
We report on the observation and numerical calculation of ionization spectra of highly Stark-shifted Rydberg states of rubidium beyond the classical ionization threshold. In the numerical calculations, a complex absorbing potential (CAP) allows us to predict the energy levels and ionization rates of Rydberg states in this regime. Our approach of adjusting the CAP to the external electric field reduces the number of free parameters from one per resonance to a single one. Furthermore, we have measured the ionization spectra of magneto-optically trapped rubidium atoms which are excited to princip…
The spatial evolution of the Rydberg blockade is studied taking into account Stark-split energy levels across several manifolds. We find that the unexpected restoration of a blockaded Rydberg excitation at small interatomic distances, e.g., experimentally observed by P.Schauss, et al. [Nature 491, 87 (2012)], can be explained by the perturbed energy levels from neighboring manifolds that enter the energy window of excitation defined by the bandwidth of the exciting laser. The same mechanism can also explain why the pair correlation function of Rydberg atoms remains nonzero in the entire region…
We report on the measurement of Stark shifted energy levels of $^{87}$Rb Rydberg atoms in static electric fields by means of electromagnetically induced transparency (EIT). Electric field strengths of up to 500V/cm, ranging beyond the classical ionisation threshold, were applied using electrodes inside a glass cell with rubidium vapour. Stark maps for principal quantum numbers $n=35$ and $n=70$ have been obtained with high signal-to-noise ratio for comparison with results from ab initio calculations following the method described in [M. L. Zimmerman et al., Phys. Rev. A 20, 2251 (1979)], which…
Experimental and theoretical studies of the effects of weak radio-frequency electric fields on Rydberg-Stark states with electric dipole moments as large as 10000 D are reported. High-resolution laser spectroscopic studies of Rydberg states with principal quantum number $n=52$ and $53$ were performed in pulsed supersonic beams of metastable helium with the excited atoms detected by pulsed electric field ionisation. Experiments were carried out in the presence of sinusoidally oscillating electric fields with frequencies of 20~MHz, amplitudes of up to 120~mV/cm, and dc offsets of up to 4.4~V/cm.…
The ac Stark effect was used to induce resonant energy transfer between translationally cold Rydberg atoms. The Rb Rydberg atoms were obtained by laser excitation of cold atoms from a magneto-optical trap. Using two-photon microwave spectroscopy of the 49s_{1/2}-50s_{1/2} transition, the field strength of a 28.5 GHz dressing field was calibrated. When this dressing field was set at specific field strengths, the two-atom dipole-dipole process 43d_{5/2} + 43d_{5/2} -> 45p_{3/2} + 41f was dramatically enhanced, due to induced degeneracy of the initial and final states. A series of observed resona…
We describe the production of cold, slow-moving LiH molecules. The molecules are produced in the ground state using laser ablation and supersonic expansion, and 68% of the population is transferred to the rotationally excited state using narrowband radiation at the rotational frequency of 444GHz. The molecules are then decelerated from 420m/s to 53m/s using a 100 stage Stark decelerator. We demonstrate and compare two different deceleration modes, one where every stage is used for deceleration, and another where every third stage decelerates and the intervening stages are used to focus the mol…
Results of numerical Monte Carlo simulations for the Stark-tuned Förster resonance and dipole blockade between two to five cold rubidium Rydberg atoms in various spatial configurations are presented. The effects of the atoms' spatial uncertainties on the resonance amplitude and spectra are investigated. The feasibility of observing coherent Rabi-like population oscillations at a Förster resonance between two cold Rydberg atoms is analyzed. Spectra and the fidelity of the Rydberg dipole blockade are calculated for various experimental conditions, including nonzero detuning from the Förster reso…
A spectroscopic study of Rydberg states of helium ($n$ = 30 and 45) in magnetic, electric and combined magnetic and electric fields with arbitrary relative orientations of the field vectors is presented. The emphasis is on two special cases where (i) the diamagnetic term is negligible and both paramagnetic Zeeman and Stark effects are linear ($n$ = 30, $B \leq$ 120 mT and $F$ = 0 - 78 V/cm ), and (ii) the diamagnetic term is dominant and the Stark effect is linear ($n$ = 45, $B$ = 277 mT and $F$ = 0 - 8 V/cm). Both cases correspond to regimes where the interactions induced by the electric and …
Precision spectroscopy of the fine and hyperfine structures of high molecular Rydberg-Stark states: Metrology of molecular hydrogen ions
ETH Zürich（苏黎世联邦理工学院）；Vrije Universiteit Amsterdam（阿姆斯特丹自由大学）；Université Paris-Saclay（巴黎萨克雷大学）；Centre National de la Recherche Scientifique（法国国家科学研究中心）
We report on Rydberg spectroscopy of ultracold atoms in an atom-ion hybrid trap for probing the electric fields in a mixture of atoms and ions. We obtain spectra which exhibit excitation gaps corresponding to avoided level crossings in the Stark map. From these measurements we can conclude that the ground state atoms experience electrical fields of up to 250 V/cm. There is, however, a difficulty in interpreting the results, because some data indicate that the electrical fields are produced by the ions while other data indicate that they stem from the Paul trap. We discuss possible scenarios fo…
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.
Three-dimensional three-photon Stark spectroscopy of a single Rb Rydberg atom in an ultrahigh-vacuum glass cell with eight electrodes
Rzhanov Institute of Semiconductor Physics SB RAS（列扎诺夫半导体物理研究所西伯利亚分院）；Novosibirsk State University（新西伯利亚国立大学）；Institute of Laser Physics SB RAS（激光物理研究所西伯利亚分院）
Electrometry is performed using Rydberg states to evaluate the quadratic Stark shift of the $5s^2$ $^1\textrm{S}_0-5s5p$ $^3\textrm{P}_0$ clock transition in strontium. By measuring the Stark shift of the highly excited $5s75d\;^1\textrm{D}_2$ state using electromagnetically induced transparency, we characterize the electric field with sufficient precision to provide tight constraints on the systematic shift to the clock transition. Using the theoretically derived, and experimentally verified, polarizability for this Rydberg state we can measure the residual field with an uncertainty well belo…
We present a study of a cold strontium Rydberg gas. The narrowband laser excitation of Rydberg states in the range n=20-80 from a 6~mK cloud of strontium atoms is detected using the spontaneous ionization of the Rydberg atoms. Using a high-resolution step-scanning technique, we perform detailed measurements of the Stark maps of selected Rydberg states. We find excellent agreement between the measured Stark maps and a numerical calculation based on an independent-electron model. Finally we show that excitation of the second valence electron can be used to probe the dynamics of the Rydberg gas w…
Floquet Interpretation of Avoided Crossings in AC Stark-Shifted Rydberg-EIT Spectra
National Institute of Standards and Technology（美国国家标准与技术研究院）；Department of Electrical, Computer, and Engineering, University of Colorado, Boulder（科罗拉多大学博尔德分校电气、计算机与工程学院）
Dipole-dipole interactions between helium atoms in Rydberg-Stark states with principal quantum number $n=53$ and approximately linear Stark energy shifts, resulting from induced electric dipole moments of approximately 7900 D, have been investigated experimentally. The experiments were performed in pulsed supersonic metastable helium beams, with particle number densities of up to $\sim10^9$ cm$^{-3}$. In the presence of amplitude-modulated, radio-frequency electric fields, changes in the spectral intensity distributions associated with the transitions to these states that are attributed to dip…
We have developed a quite stringent method in selectivity to ionize the low angular- momentum ($\ell$) states which lie below and above the adjacent manifold in highly excited Rb Rydberg atoms. The method fully exploits the pulsed field-ionization characteristics of the manifold states in high slew-rate regime: Specifically the low $\ell$ state below (above) the adjacent manifold is firstly transferred to the lowest (highest) state in the manifold via the adiabatic transition at the first avoided crossing in low slew-rate regime, and then the atoms are driven to a high electric field for ioniz…
We report on the deceleration of a beam of SrF molecules from 290 to 120~m/s. Following supersonic expansion, the molecules in the $X^2Σ$ ($v=0$, $N=1$) low-field seeking states are trapped by the moving potential wells of a traveling-wave Stark decelerator. With a deceleration strength of 9.6 km/s$^2$ we have demonstrated the removal of 85 % of the initial kinetic energy in a 4 meter long modular decelerator. The absolute amount of kinetic energy removed is a factor 1.5 higher compared to previous Stark deceleration experiments. The demonstrated decelerator provides a novel tool for the creat…
Angle-of-Arrival Determination of Radio-Frequency Fields Using Stark-Shifted Rydberg-EIT Spectra
National Institute of Standards and Technology（美国国家标准与技术研究院）；Department of Electrical, Computer, and Energy Engineering, University of Colorado, Boulder（科罗拉多大学博尔德分校电气、计算机与能源工程系）
Cryogenic buffer-gas beams are a promising method for producing bright sources of cold molecular radicals for cold collision and chemical reaction experiments. In order to use these beams in studies of reactions with controlled collision energies, or in trapping experiments, one needs a method of controlling the forward velocity of the beam. A Stark decelerator can be an effective tool for controlling the mean speed of molecules produced by supersonic jets, but efficient deceleration of buffer-gas beams presents new challenges due to longer pulse lengths. Traveling-wave decelerators are unique…
We demonstrate the single-photon Rydberg excitation of cesium atoms in a magneto-optical trap (MOT). We excite atoms directly from ${{6S}_{1/2}}$ ground state to ${{nP}_{3/2}}(n=70-100)$ Rydberg state with a narrow-linewidth 319 nm ultra-violet laser. The detection of Rydberg states is performed by monitoring the reduction of fluorescence signal of the MOT as partial population on ${{6S}_{1/2}} (F = 4)$ ground state are transferred to Rydberg state. We clearly observe Autler-Townes doublet in the trap-loss spectra due to the cooling lights. Utilizing the large electric polarizibility of Rydber…
We propose a promising scheme to decelerate a cw filtering out molecular beam using a red-detuned quasi-cw semi-Gaussian laser beam. By using Monte-Carlo simulation method, we demonstrate this optical Stark deceleration scheme, and study its decelerated dynamic process for a cw ND3 molecular beam as well as the dependence of the deceleration effect on the border width of the semi-Gaussian beam. Our study shows that the proposed scheme can be used to efficiently slow a cw ND3 molecular beam, and obtain a relative average kinetic-energy loss of 9.33% by using a single semi-Gaussian beam with a w…
Trapping a Rydberg atom close to a surface is an important step towards the realisation of many proposals of quantum information or hybrid quantum systems. One of the challenges in these experiments is to overcome the electric field emanating from contaminations on the surface. Here we report on measurements of an electric field created by $^{87}$Rb atoms absorbed on a 25$\,$nm thick layer of SiO$_2$, covering a 90$\,$nm layer of Au. The electric field is measured using a two-photon transition to the 23$D_{5/2}$ and 25$S_{1/2}$ state. The electric field value that we measure is higher than typ…
Splitting the energy levels of a hydrogen-like atom by the electric field nonuniform at the atomic scale is studied. This situation is important for the multi-level treatment of the phenomenon of Rydberg blockade [Yu.V. Dumin, J. Phys. B, v.47, p.175502 (2014)]. An explicit formula for the energy levels is derived. A typical value of the energy shift by the electric field gradient turns out to be proportional to the 4th power of the principal quantum number (i.e., the square of atomic size), as would be expected from a qualitative consideration. Finally, the fine spatial structure of the Rydbe…
Inhomogeneous electric fields generated above two-dimensional electrode structures have been used to transversely split beams of helium Rydberg atoms into pairs of spatially separated components. The atomic beams had initial longitudinal speeds of between 1700 and 2000 m/s and were prepared in Rydberg states with principle quantum number $n=52$ and electric dipole moments of up to 8700 D by resonance-enhanced two-color two-photon laser excitation from the metastable 1s2s $^3$S$_1$ level. Upon exiting the beam splitter the ensembles of Rydberg atoms were separated by up to 15.6 mm and were dete…
Radiative and collisional constants of excited atoms contain the matrix elements of the dipole transitions and when they are blocked one can expect occurring a number of interesting phenomena in radiation-collisional kinetics. In recent astrophysical studies of IR emission spectra it was revealed a gap in the radiation emitted by Rydberg atoms ($RA$) with values of the principal quantum number of $n\approx10$. Under the presence of external electric fields a rearrangement of $RA$ emission spectra is possible to associate with manifestations of the Stark effect. The threshold for electric field…
We demonstrate feedback control optimization for the Stark deceleration and trapping of neutral polar molecules using evolutionary strategies. In a Stark-decelerator beamline pulsed electric fields are used to decelerate OH radicals and subsequently store them in an electrostatic trap. The efficiency of the deceleration and trapping process is determined by the exact timings of the applied electric field pulses. Automated optimization of these timings yields an increase of 40 % of the number of trapped OH radicals.
A method for performing a precision measurement of the Rydberg constant, $R_{\infty}$, using cold circular Rydberg atoms is proposed. These states have long lifetimes, as well as negligible quantum-electrodynamics (QED) and no nuclear-overlap corrections. Due to these advantages, the measurement can help solve the "proton radius puzzle" [Bernauer, Pohl, Sci. Am. 310, 32 (2014)]. The atoms are trapped using a Rydberg-atom optical lattice, and transitions are driven using a recently-demonstrated lattice-modulation technique to perform Doppler-free spectroscopy. The circular-state transition freq…
We report on the observation of the motional Stark effect of highly excited $^{87}$Rb Rydberg atoms moving in the presence of a weak homogeneous magnetic field in a vapor cell. Employing electromagnetically induced transparency for spectroscopy of an atomic vapor, we observe the velocity-, quantum state- and magnetic field-dependent transition frequencies between the ground and Rydberg excited states. For atoms moving at velocities around $400\,\mathrm{m/s}$, the principal quantum number $n=100$ of the valence electron, and a magnetic field of $B=100\,\mathrm{G}$, we measure a motional Stark s…
High-fidelity entangled Bell states are of great interest in quantum physics. Entanglement of ultracold neutral atoms in two spatially separated optical dipole traps is promising for implementation of quantum computing and quantum simulation and for investigation of Bell states of material objects. We propose a new method to entangle two atoms via long-range Rydberg-Rydberg interaction. Alternatively to previous approaches, based on Rydberg blockade, we consider radiofrequency-assisted Stark-tuned Förster resonances in Rb Rydberg atoms. To reduce the sensitivity of the fidelity of Bell states …
Supersonic beams of hydrogen atoms, prepared selectively in Rydberg-Stark states of principal quantum number $n$ in the range between 25 and 35, have been deflected by 90$^\circ$, decelerated and loaded into off-axis electric traps at initial densities of $\approx 10^6$ atoms/cm$^{-3}$ and translational temperatures of 150 mK. The ability to confine the atoms spatially was exploited to study their decay by radiative and collisional processes. The evolution of the population of trapped atoms was measured for several milliseconds in dependence of the principal quantum number of the initially pre…
Helium atoms in high- and low-field-seeking Rydberg states with linear and quadratic Stark shifts have been confined in two dimensions and guided over a distance of 150 mm using time-varying inhomogeneous electric fields. This was achieved with an electrode structure composed of four parallel cylindrical rods to which voltages were applied to form oscillating and rotating saddle-point fields. These two modes of operation result in time-averaged pseudopotentials that confine samples in high- and low-field-seeking states about the axis of the device. The experimental data have been compared to t…
We develop a theoretical understanding of trapping divalent Rydberg atoms in optical lattices. Because the size of the Rydberg electron cloud can be comparable to the scale of spatial variations of laser intensity, we pay special attention to averaging optical fields over the atomic wavefunctions. Optical potential is proportional to the ac Stark polarizability. We find that in the independent particle approximation for the valence electrons, this polarizability breaks into two contributions: the singly ionized core polarizability and the contribution from the Rydberg electron. Unlike the usua…
We have designed and implemented a new Stark decelerator based on wire electrodes, which is suitable for ultrahigh vacuum applications. The 100 deceleration stages are fashioned out of 0.6 mm diameter tantalum and the array's total length is 110 mm, approximately 10 times smaller than a conventional Stark decelerator with the same number of electrode pairs. Using the wire decelerator, we have removed more than 90% of the kinetic energy from metastable CO molecules in a beam.
We present experiments on decelerating and trapping ammonia molecules using a combination of a Stark decelerator and a traveling wave decelerator. In the traveling wave decelerator a moving potential is created by a series of ring-shaped electrodes to which oscillating high voltages are applied. By lowering the frequency of the applied voltages, the molecules confined in the moving trap are decelerated and brought to a standstill. As the molecules are confined in a true 3D well, this new kind of deceleration has practically no losses, resulting in a great improvement on the usual Stark deceler…
