We have studied an ionization of alkali-metal Rydberg atoms by blackbody radiation (BBR). The results of the theoretical calculations of ionization rates of Li, Na, K, Rb and Cs Rydberg atoms are presented. Calculations have been performed for nS, nP and nD states which are commonly used in a variety of experiments, at principal quantum numbers n=8-65 and at the three ambient temperatures of 77, 300 and 600 K. A peculiarity of our calculations is that we take into account the contributions of BBR-induced redistribution of population between Rydberg states prior to photoionization and field ionization by extraction electric field pulses. The obtained results show that these phenomena affect both the magnitude of measured ionization rates and shapes of their dependences on n. A Cooper minimum for BBR-induced transitions between bound Rydberg states of Li has been found. The calculated ionization rates are compared with our earlier measurements of BBR-induced ionization rates of Na nS and nD Rydberg states with n=8-20 at 300 K. A good agreement for all states except nS with n>15 is observed. Useful analytical formulas for quick estimation of BBR ionization rates of Rydberg atoms are presented. Application of BBR-induced ionization signal to measurements of collisional ionization rates is demonstrated.
We show that optical spectroscopy of Rydberg states can provide accurate {\em in situ} thermometry at room-temperature. Transitions from a metastable state to Rydberg states with principal quantum numbers of 25 to 30 have 200 times larger fractional frequency sensitivities to blackbody radiation than the Strontium clock transition. We demonstrate that magic wavelength lattices exist for both Strontium and Ytterbium transitions between the metastable and Rydberg states. Frequency measurements of Rydberg transitions with $10^{-16}$ accuracy provide $10 \, \mathrm{mK}$ resolution and yield a blac…
Results of theoretical calculations of ionization rates of Rb and Na Rydberg atoms by blackbody radiation (BBR) are presented. Calculations have been performed for nS, nP and nD states of Na and Rb, which are commonly used in a variety of experiments, at principal quantum numbers n=8-65 and at three ambient temperatures of 77, 300 and 600 K. A peculiarity of our calculations is that we take into account the contributions of BBR-induced redistribution of population between Rydberg states prior to photoionization and field ionization by extraction electric field pulses. The obtained results show…
We report experimental measurements of the rates of blackbody radiation-induced transitions between high-lying (n>60) S, P and D Rydberg levels of rubidium atoms in a magneto-optical trap using a hybrid field ionization and state-selective depumping technique. Our results reveal significant deviations of the measured transition rates from theory for well-defined ranges of the principal quantum number. We assume that the most likely cause for those deviations is a modified blackbody spectrum inside the glass cell in which the magneto-optical trap is formed, and we test this assumption by instal…
We report the sudden and spontaneous evolution of an initially correlated gas of repulsively interacting Rydberg atoms to an ultracold plasma. Under continuous laser coupling we create a Rydberg ensemble in the strong blockade regime, which at longer times undergoes an ionization avalanche. By combining optical imaging and ion detection, we access the full information on the dynamical evolution of the system, including the rapid increase in the number of ions and a sudden depletion of the Rydberg and ground state densities. Rydberg-Rydberg interactions are observed to strongly affect the dynam…
Blackbody radiation (BBR) sources are calculable radiation sources that are frequently used in radiometry, temperature dissemination, and remote sensing. Despite their ubiquity, blackbody sources and radiometers have a plethora of systematics. We envision a new, primary route to measuring blackbody radiation using ensembles of polarizable quantum systems, such as Rydberg atoms and diatomic molecules. Quantum measurements with these exquisite electric field sensors could enable active feedback, improved design, and, ultimately, lower radiometric and thermal uncertainties of blackbody standards.…
An ensemble of excited atoms can synchronize emission of light collectively in a process known as superradiance when its characteristic size is smaller than the wavelength of emitted photons. The underlying superradiance depends strongly on electromagnetic (photon) fields surrounding the atomic ensemble. High mode densities of microwave photons from $300\,$K blackbody radiation (BBR) significantly enhance decay rates of Rydberg states to neighbouring states, enabling superradiance that is not possible with bare vacuum induced spontaneous decay. Here we report observations of the superradiance …
We report on the behaviour of the ionization avalanche in an ensemble of ultracold 87Rb atoms coupled to a high lying Rydberg state and investigate extensions to the current model by including the effects of three-body recombination and plasma expansion. To separate the two effects we study the time dependence of the plasma formation at various densities as well as for different nS and nD states. At medium densities and low n we observe the onset of the avalanche as has been reported in other experiments, as well as a subsequent turn-off of the avalanche for longer excitation times, which we a…
We have studied the behavior of cold Rydberg atoms embedded in an ultracold plasma. We demonstrate that even deeply bound Rydberg atoms are completely ionized in such an environment, due to electron collisions. Using a fast pulse extraction of the electrons from the plasma we found that the number of excess positive charges, which is directly related to the electron temperature Te, is not strongly affected by the ionization of the Rydberg atoms. Assuming a Michie-King equilibrium distribution, in analogy with globular star cluster dynamics, we estimate Te. Without concluding on heating or cool…
We report clear evidence of the role of dipole-dipole interaction in Penning ionization of Rydberg atoms, leading to the formation of an ultracold plasma. Penning ionization of np Rydberg Cesium atoms is prevented for states with in n < 42, which correspond to a repulsive potential, but it does not occur for n larger than 42, corresponding to an attractive potential. Blackbody radiation is mostly responsible for the background and initial ionization, although ion-Rydberg collisions and population transfer due to limited superradiance may have to be considered.
We study the field-ionization threshold behavior when a Rydberg atom is ionized by a short single-cycle pulse field. Both hydrogen and sodium atoms are considered. The required threshold field amplitude is found to scale \emph{inversely} with the binding energy when the pulse duration becomes shorter than the classical Rydberg period, and, thus, more weakly bound electrons require larger fields for ionization. This threshold scaling behavior is confirmed by both 3D classical trajectory Monte Carlo simulations and numerically solving the time-dependent Schrödinger equation. More surprisingly, t…
We experimentally studied the Rydberg level shift caused by the electric field, which is generated by Rydberg atom collision induced ionization in a cesium atomic ensemble. The density of charged particles caused by collisions between Rydberg atoms is changed by controlling the ground-state atomic density and optical excitation process. We measured the Rydberg level shift using Rydberg electromagnetically-induced-transparency (EIT) spectroscopy, and interpreted the physical origin using a semi-classical model. The experimental results are in good agreement with the numerical simulation. These …
The results of a theoretical investigation of prompt many-body ionization are reported. Our calculations address an experiment that reported ionization in Rydberg gases for densities two orders of magnitude less than expected from ionization between pairs of atoms. The authors argued that the results were due to the simultaneous interaction between many atoms. We performed classical calculations for many interacting Rydberg atoms with the ions fixed in space and have found that the many atom interaction does allow ionization at lower densities than estimates from two atom interactions. However…
A fully classical explanation of the nonhydrogenic ionization threshold for low angular momentum Rydberg states of Alkali-metal atoms in a linearly polarized low frequency monochromatic microwave field is given: the classical equivalent to the quantum rate-limiting step, which is responsible for the n^(-5) scaling and which according to the literature initiates what then continues as essentially classical diffusion, is found.
Collisional ionization between two Rydberg atoms in relative motion is examined. A classical trajectory Monte Carlo method is used to determine the cross sections associated with Penning ionization. The dependence of the ionization cross section on the magnitude and the direction of orbital angular momentum of the electrons and the direction of the Laplace-Runge-Lenz vector of the electrons is studied. For a given magnitude of angular momentum, there can exist a difference of a factor of up to $\sim2.5$ in the ionization cross section between the orientation with the highest and the lowest ion…
Tunnel ionization rates of triplet Rydberg states in helium with principal quantum numbers close to 37 have been measured in electric fields at the classical ionization threshold of $\sim197$ V/cm. The measurements were performed in the time domain by combining high-resolution continuous-wave laser photoexcitation and pulsed electric field ionization. The observed tunnel ionization rates range from $10^5$ s$^{-1}$ to $10^7$ s$^{-1}$ and have, together with the measured atomic energy-level structure in the corresponding electric fields, been compared to the results of calculations of the eigenv…
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…
We present an experimental and theoretical study of the chaotic ionization of quasi-one-dimensional potassium Rydberg wavepackets via a phase-space turnstile mechanism. Turnstiles form a general transport mechanism for numerous chaotic systems, and this study explicitly illuminates their relevance to atomic ionization. We create time-dependent Rydberg wavepackets, subject them to alternating applied electric-field "kicks", and measure the electron survival probability. Ionization depends not only on the initial electron energy, but also on the phase-space position of the electron with respect …
New experimental quantum simulation platforms have recently been implemented with divalent atoms trapped in optical tweezer arrays with promising performance. The second valence electron also brings new propects through the so-called Isolated Core Excitation (ICE), however autoionization presents a strong limitation to this use. In this study, we propose and demonstrate a new approach to applying a sizable light shift to a Rydberg state with close-to-resonant ICE while avoiding auto-ionization. In particular, we have investigated ICE of ytterbium atoms in $^1S_0$ Rydberg states. Spectroscopic …
Quantum control of the pathway along which a Rydberg electron field ionizes is experimentally and computationally demonstrated. Selective field ionization is typically done with a slowly rising electric field pulse. The $(1/n^*)^4$ scaling of the classical ionization threshold leads to a rough mapping between arrival time of the electron signal and principal quantum number of the Rydberg electron. This is complicated by the many avoided level crossings that the electron must traverse on the way to ionization, which in general leads to broadening of the time-resolved field ionization signal. In…
It is well-known from numerical and experimental results that the fraction of Rydberg states (excited neutral atoms) created by tunnel ionization declines dramatically with increasing ellipticity of laser light. We present a method to analyze this dependence on ellipticity, deriving a probability distribution of Rydberg states that agrees closely with recent experimental [1] and numerical results. In particular, contradicting the existing proposed mechanism [1] and general expectations, our results indicate that the dependence of Rydberg yield on laser ellipticity is not caused by a rescatteri…
Pulsed field ionization of high-$n$ (90 $\leq n \leq$ 150) manifold states in Rb Rydberg atoms has been investigated in high slew-rate regime. Two peaks in the field ionization spectra were systematically observed for the investigated $n$ region, where the field values at the lower peak do not almost depend on the excitation energy in the manifold, while those at the higher peak increase with increasing excitation energy. The fraction of the higher peak component to the total ionization signals increases with increasing $n$, exceeding 80% at $n$ = 147. Characteristic behavior of the peak compo…
Rydberg atoms excited by cold blackbody radiation are shown to display long-lived quantum coherences on timescales of tens of picoseconds. By solving non-Markovian equations of motion with no free parameters we obtain the time evolution of the density matrix, and demonstrate that the blackbody-induced temporal coherences manifest as slowly decaying (100 ps) quantum beats in time-resolved fluorescence. An analytic model shows the dependence of the coherent dynamics on the energy splitting between atomic eigenstates, transition dipole moments, and coherence time of the radiation. Experimental de…
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…
Multi-step laser resonance ionization spectroscopy of lutetium (Lu) has been performed at TRIUMF's off-line laser ion source test stand. The even-parity Rydberg series $6s^2nd$ $^2D_{3/2}$, $6s^2nd$ $^2D_{5/2}$ and $6s^2ns$ $^2S_{1/2}$ were observed converging to the 6s$^2$ ionization potential. The experimental results has been compared to previous work. 51 levels of Rydberg series $6s^2nd$ $^2D_{5/2}$ and 52 levels of Rydberg series $6s^2ns$ $^2S_{1/2}$ were reported new. Additionally six even-parity autoionization (AI) series converging to Lu ionic states $5d6s$ $^3D_1$ and $5d6s$ $^3D_2$ w…
Collisional and thermal ionization of sodium nS and nD Rydberg atoms with n=8-20 has been studied. The experiments were performed using a two-step pulsed laser excitation in an effusive atomic beam at atom density of about 2 10^{10} cm^{-3}. Molecular and atomic ions from associative, Penning, and thermal ionization processes were detected. It has been found that the atomic ions were created mainly due to photoionization of Rydberg atoms by photons of blackbody radiation at the ambient temperature of 300K. Blackbody ionization rates and effective lifetimes of Rydberg states of interest were de…
I show that the theory developed for quantum delocalization of an excited Hydrogen atom in a two-frequency linearly polarized microwave field can be used with a few adaptions to explain the quantum delocalization of Alkali atoms in a linearly polarized monochromatic field in the regime where it deviates from Hydrogenic behaviour. Comparison with numerical and laboratory experiments is satisfactory: apart from a constant factor, independent from the microwave frequency, the same dependence from the initial quantum number is observed.
In the combination of crossed electric and magnetic fields and the Coulomb field of the atomic nucleus the spectrum of the Rydberg electron in the vicinity of the Stark saddle-point are investigated at a quantum mechanical level. The results expose a quantum anomaly dissociation: quasibound states near and above the saddle-point ionization limit predicted at the semi-classical level disappear at a quantum mechanical level.
We study a novel regime of the Rydberg excitation blockade using highly Stark-shifted, yet long-living, states of Rb atoms subject to electric fields above the classical ionization limit. Such states allow tuning the dipole-dipole interaction strength while their ionization rate can be changed over two orders of magnitude by small variations of the electric field. We demonstrate laser excitation of the interacting Rydberg states followed by their detection using controlled ionization and magnified imaging with high spatial and temporal resolution. Our work reveals the hitherto unexplored possi…
In this article the history and the current state of research of the chemiionization processes in atom-Rydberg atom collisions is presented. The principal assumptions of the model of such processes based on the dipole resonance mechanism, as well as the problems of stochastic ionization in atom-Rydberg atom collisions, are exposed. The properties of the collision kinetics in atom beams of various types used in contemporary experimentations are briefly described. Results of the calculation of the chemi-ionization rate coefficients are given and discussed for the range of the principal quantum n…
We have performed classical trajectory Monte Carlo (CTMC) studies of electron capture and ionization in multiply charged (Q=8) ion-Rydberg atom collisions at intermediate impact velocities. Impact parallel to the minor and to the major axis, respectively, of the initial Kepler electron ellipse has been investigated. The important role of the initial electron momentum distribution found for singly charged ion impact is strongly disminished for higher projectile charge, while the initial spatial distribution remains important for all values of Q studied.
We report new frequency-comb-based measurements of Ca Rydberg energy levels. Counter-propagating laser beams at 390 nm and 423 nm excite Ca atoms from the $4s^2~^1\mbox{S}_0$ ground state to $4sns~^1\mbox{S}_0$ Rydberg levels with $n$ ranging from 40 to 110. Near-resonant two-photon two-color excitation of atoms in a thermal beam makes it possible to eliminate the first-order Doppler shift. The resulting lineshapes are symmetric and Gaussian. We verify laser metrology and absolute accuracy by reproducing measurements of well-known transitions in Cs, close to the fundamental wavelengths of our …
Circular Rydberg states are ideal tools for quantum technologies, with huge mutual interactions and extremely long lifetimes in the tens of milliseconds range, two orders of magnitude larger than those of laser-accessible Rydberg states. However, such lifetimes are observed only at zero temperature. At room temperature, blackbody-radiation-induced transfers annihilate this essential asset of circular states, which have thus been used mostly so far in specific, complex cryogenic experiments. We demonstrate here, on a laser-cooled atomic sample, a circular state lifetime of more than one millise…
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 study the time dependence of the ionization probability of Rydberg atoms driven by a microwave field. The quantum survival probability follows the classical one up to the Heisenberg time and then decays inversely proportional to time, due to tunneling and localization effects. We provide parameter values which should allow one to observe such decay in laboratory experiments. Relations to the $1/f$ noise are also discussed.
The microwave ionization of internally chaotic Rydberg atoms is studied analytically and numerically. The internal chaos is induced by magnetic or static electric fields. This leads to a chaotic enhancement of microwave excitation. The dynamical localization theory gives a detailed description of the excitation process even in a regime where up to few thousands photons are required to ionize one atom. Possible laboratory experiments are also discussed.
We present time-resolved spectroscopic measurements of Rydberg-Rydberg interactions in an ultracold gas, revealing the pair dynamics induced by long-range van der Waals interactions between the atoms. By detuning the excitation laser, a specific pair distribution is prepared. Penning ionization on a microsecond timescale serves as a probe for the pair dynamics under the influence of the attractive long-range forces. Comparison with a Monte Carlo model not only explains all spectroscopic features but also gives quantitative information about the interaction potentials. The results imply that th…
We report on the measurement of electron emission after the interaction of strong laser pulses with atoms and molecules. These electrons originate from high-lying Rydberg states with quantum numbers up to $n \lesssim 120$ formed by frustrated field ionization. Simulations show that both tunneling ionization by a weak dc field and photoionization by the black-body radiation contribute to delayed electron emission on the nano- to microsecond scale. We measured ionization rates from these Rydberg states by coincidence spectroscopy. Further, the dependence of the Rydberg-state production on the el…
Coherent time evolution of highly excited Rydberg states in Rb (98 < n < 150) under pulsed electric field in high slew-rate regime was investigated with the field ionization detection. The electric field necessary to ionize the Rydberg states was found to take discrete values successively depending on the slew rate. Specifically the slew-rate dependence of the ionization field varies with the quantum defect value of the states, i.e. with the energy position of the states relative to the adjacent manifold. This discrete transitional behavior of the ionization field observed for the first time i…
This work reports on the application of a novel electric field-ionization setup for high-resolution laser spectroscopy measurements on bunched fast atomic beams in a collinear geometry. In combination with multi-step resonant excitation to Rydberg states using pulsed lasers, the field ionization technique demonstrates increased sensitivity for isotope separation and measurement of atomic parameters over non-resonant laser ionization methods. The setup was tested at the Collinear Resonance Ionization Spectroscopy experiment at ISOLDE-CERN to perform high-resolution measurements of transitions i…
A complete set of spectroscopic data is indispensable when using Rydberg states of trapped ions for quantum information processing. We carried out Rydberg series spectroscopy for $nS_{1/2}$ states with $38 \leq n \leq 65$ and for $nD_{5/2}$ states with $37\leq n \leq 50$ on a single trapped $^{40}$Ca$^+$ ion. From a nonlinear regression to resonance frequencies, we determined the ionization energy of 2 870 575.582(15) GHz, measured 60 times more accurately as compared to the accepted value and contradicting it by 7.5 standard deviations. We confirm quantum defect values of $δ_{S_{1/2}}=1.80299…
We investigate numerically and analytically the intensity dependence of the fraction of electrons that end up in a Rydberg state after strong-field ionization with linearly polarized light. We find that including the intensity dependent distribution of ionization times and non-adiabatic effects leads to a better understanding of experimental results. Furthermore, we observe using Classical Trajectory Monte Carlo simulations that the intensity dependence of the Rydberg yield changes with wavelength and that the previously observed power-law dependence breaks down at longer wavelengths. Our work…
We investigate a possible mechanism for the autoionization of ultracold Rydberg gases, based on the resonant coupling of Rydberg pair states to the ionization continuum. Unlike an atomic collision where the wave functions begin to overlap, the mechanism considered here involves only the long-range dipole interaction and is in principle possible in a static system. It is related to the process of intermolecular Coulombic decay (ICD). In addition, we include the interaction-induced motion of the atoms and the effect of multi-particle systems in this work. We find that the probability for this io…
The electron signals from the field ionization of two closely-spaced Rydberg states of \mbox{rubidium-85} are separated using quantum control. In selective field ionization, the state distribution of a collection of Rydberg atoms is measured by ionizing the atoms with a ramped electric field. Generally, atoms in higher energy states ionize at lower fields, so ionized electrons which are detected earlier in time can be correlated with higher energy Rydberg states. However, the resolution of this technique is limited by the Stark effect. As the electric field is increased, the electron encounter…
Recent experiments have demonstrated the spontaneous evolution of a gas of ultracold Rydberg atoms into an expanding ultracold plasma, as well as the reverse process of plasma recombination into highly excited atomic states. Treating the evolution of the plasma on the basis of kinetic equations, while ionization/excitation and recombination are incorporated using rate equations, we have investigated theoretically the Rydberg-to-plasma transition. Including the influence of spatial correlations on the plasma dynamics in an approximate way we find that ionic correlations change the results only …
We characterized the pulsed Rydberg-positronium production inside the AEgIS (Antimatter Experiment: Gravity, Interferometry, Spectroscopy) apparatus in view of antihydrogen formation by means of a charge exchange reaction between cold antiprotons and slow Rydberg-positronium atoms. Velocity measurements on positronium along two axes in a cryogenic environment (10K) and in 1T magnetic field were performed. The velocimetry was done by MCP-imaging of photoionized positronium previously excited to the $n=3$ state. One direction of velocity was measured via Doppler-scan of this $n=3$-line, another …
The dipole blockade effect at laser excitation of mesoscopic ensembles of Rydberg atoms lies in the fact that the excitation of one atom to a Rydberg state blocks the excitation of other atoms due to the shift in the collective energy levels of interacting Rydberg atoms. It is used to obtain the entangled qubit states based on single neutral atoms in optical traps. In this paper, we present our experimental results on the observation of the dipole blockade for mesoscopic ensembles of 1-5 atoms when they are detected by the selective field ionization method. We investigated the spectra of the t…
Ionization energies for Rydberg $^4 \mathrm{He}$ ($1snp\,^{1,3}P$) states using the correlated B-spline basis function method
Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences（中国科学院精密测量科学与技术创新院）；University of Chinese Academy of Sciences（中国科学院大学）
Photoionization spectra of Se have been studied by step-wise resonance laser ionization. The Rydberg series 4s$^2$4p$^3$($^4$S)np $^3$P$_{0,1,2}$ and 4s$^2$4p$^3$($^4$S)np $^5$P$_{1,2,3}$ were measured via different excitation schemes. Using the Rydberg series 4s$^2$4p$^3$($^4$S)np $^3$P$_2$ with n=15-33, the ionization potential of Se was determined with improved precision to 76658.15(2)$_{stat}$(4)$_{sys}$ cm$^{-1}$, which resolved the discrepancy in previous literatures. Autoionizing (AI) spectra between the IP and two neighboring converging limits of the Se ionic states 4s$^2$4p$^3$($^2$D$…
