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 determined. The molecular ions were found to be from associative ionization in Na(nL)+Na(3S) collisions. Rate constants of associative ionization have been measured using an original method based on relative measurements of Na_{2}^{+} and Na^{+} ion signals.
Coherence relaxation in Na vapor was studied utilizing a pump-probe method with femtosecond pulses. The coherence was created by the pump pulse, which excited the Na atoms to the 4S state. The atoms were further excited to the 7P state by the probe pulse. As a result a coherent UV radiation was emitted by the atoms. This emission was used to study the relaxation of both the 4S-3S and 7P-3S coherent superpositions. The relaxation is mainly due to collisions with the Ar atoms serving as a buffer gas. Coherence relaxation times and collisional cross-sections for the Na-Ar collision pairs were ext…
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…
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…
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 experimentally demonstrate an original method to measure very accurately the density of a frozen Rydberg gas. It is based on the use of adiabatic transitions induced by the long-range dipole-dipole interaction in pairs of nearest neighbor Rydberg atoms by sweeping an electric field with time. The efficiency of this two-body process is experimentally tunable, depends strongly on the density of the gas and can be accurately calculated. The analysis of this efficiency leads to an accurate determination of the Rydberg gas density, and to a calibration of the Rydberg detection. Our method does n…
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…
Rydberg states of atoms are of great current interest for quantum manipulation of mesoscopic samples of atoms. Long-range Rydberg-Rydberg interactions can inhibit multiple excitations of atoms under the appropriate conditions. These interactions are strongest when resonant collisional processes give rise to long-range C_3/R^3 interactions. We show in this paper that even under resonant conditions C_3 often vanishes so that care is required to realize full dipole blockade in micron-sized atom samples.
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 have developed an all-optical method for measuring the lifetimes of $n S$ and $n D$ Rydberg states and demonstrate its capabilities with measurements on a dilute cloud of ultracold ${}^{87}$Rb atoms in a cryogenic environment. The method is based on the time-resolved observation of resonant light absorption by ground state atoms and selective transfer of Rydberg atoms into the ground state at varying delay times in order to reconstruct Rydberg decay curves. Our measurements of the ${}^{87}$Rb $30S_{1/2}$ state indicate an increase of the lifetime at lowered environment temperatures, as expe…
We demonstrate the first deterministic entanglement of two individually addressed neutral atoms using a Rydberg blockade mediated controlled-NOT gate. Parity oscillation measurements reveal an entanglement fidelity of $F=0.58\pm0.04$, which is above the entanglement threshold of $F=0.5$, without any correction for atom loss, and $F=0.71\pm0.05$ after correcting for background collisional losses. The fidelity results are shown to be in good agreement with a detailed error model.
Cold Rydberg atoms exposed to strong magnetic fields possess unique properties which open the pathway for an intriguing many-body dynamics taking place in Rydberg gases consisting of either matter or anti-matter systems. We review both the foundations and recent developments of the field in the cold and ultracold regime where trapping and cooling of Rydberg atoms have become possible. Exotic states of moving Rydberg atoms such as giant dipole states are discussed in detail, including their formation mechanisms in a strongly magnetized cold plasma. Inhomogeneous field configurations influence t…
Assemblies of highly excited Rydberg atoms in an ultracold gas can be set into motion by a combination of van-der-Waals and resonant dipole-dipole interactions. Thereby, the collective electronic Rydberg state might change due to non-adiabatic transitions, in particular if the configuration encounters a conical interaction. For the experimentally most accessible scenario, in which the Rydberg atoms are initially randomly excited in a three-dimensional bulk gas under blockade conditions, we numerically show that non-adiabatic transitions can be common when starting from the most energetic repul…
We have investigated the wave-function feature of Rydberg sodium in a uniform electric field and found that the core-induced interaction of non-hydrogenic atom in electric field can be directly visualized in the wave-function. As is well known, the hydrogen atom in electric field can be separated in parabolic coordinates (η, ξ), whose eigen-function can show a clear pattern towards negative and positive directions corresponding to the so-called red and blue states without ambiguity, respectively. It can be served as a complete orthogonal basis set to study the core-induced interaction of non-h…
We report on the observation of interactions between ultracold Rydberg atoms and ions in a Paul trap. The rate of observed inelastic collisions, which manifest themselves as charge transfer between the Rydberg atoms and ions, exceeds that of Langevin collisions for ground state atoms by about three orders of magnitude. This indicates a huge increase in interaction strength. We study the effect of the vacant Paul trap's electric fields on the Rydberg excitation spectra. To quantitatively describe the exhibited shape of the ion loss spectra, we need to include the ion-induced Stark shift on the …
We have developed a simple analytical model describing multi-atom signals that are measured in experiments on dipole-dipole interaction at resonant collisions of a few Rydberg atoms. It has been shown that finite efficiency of the selective field-ionization detector leads to the mixing up of the spectra of resonant collisions registered for various numbers of Rydberg atoms. The formulas which help to estimate an appropriate mean Rydberg atom number for a given detection efficiency are presented. We have found that a measurement of the relation between the amplitudes of collisional resonances o…
Applicability of Rydberg atoms to quantum computers is examined from experimental point of view. In many theoretical proposals appeared recently, excitation of atoms into highly excited Rydberg states was considered as a way to achieve quantum entanglement in cold atomic ensembles via dipole-dipole interaction that could be strong for Rydberg atoms. Appropriate conditions to realize a conditional quantum phase gate have been analyzed. We also present the results of modeling experiments on microwave spectroscopy of single- and multi-atom excitations at the one-photon 37S-37P and two-photon 37S-…
We discuss laser dressed dipolar and Van der Waals interactions between atoms and polar molecules, so that a cold atomic gas with laser admixed Rydberg levels acts as a designed reservoir for both elastic and inelastic collisional processes. The elastic scattering channel is characterized by large elastic scattering cross sections and repulsive shields to protect from close encounter collisions. In addition, we discuss a dissipative (inelastic) collision where a spontaneously emitted photon carries away (kinetic) energy of the collision partners, thus providing a significant energy loss in a s…
We study dispersive optical nonlinearities of short pulses propagating in high number density, warm atomic vapors where the laser resonantly excites atoms to Rydberg $P$-states via a single-photon transition. Three different regimes of the light-atom interaction, dominated by either Doppler broadening, Rydberg atom interactions, or decay due to thermal collisions between groundstate and Rydberg atoms, are described. We show that using fast Rabi flopping and strong Rydberg atom interactions, both in the order of gigahertz, can overcome the Doppler effect as well as collisional decay, leading to…
We present the results of experiments demonstrating the spectroscopic detection of Förster resonance energy transfer from NH$_3$ in the $X\,^1A_1$ ground electronic state to helium atoms in 1s$n$s\,$^3$S$_1$ Rydberg levels, where $n=37$ and $n=40$. For these values of $n$ the 1s$n$s\,$^3$S$_1\rightarrow$1s$n$p\,$^3$P$_J$ transitions in helium lie close to resonance with the ground-state inversion transitions in NH$_3$, and can be tuned through resonance using electric fields of less than 10~V/cm. In the experiments, energy transfer was detected by direct state-selective electric field ionizati…
In plasmas at very low temperatures formation of neutral atoms is dominated by collisional three-body recombination, owing to the strong ~ T^(-9/2) scaling of the corresponding recombination rate with the electron temperature T. While this law is well established at high temperatures, the unphysical divergence as T -> 0 clearly suggest a breakdown in the low-temperature regime. Here, we present a combined molecular dynamics-Monte-Carlo study of electron-ion recombination over a wide range of temperatures and densities. Our results reproduce the known behavior of the recombination rate at high …
In our previous research, it has been demonstrated that such inelastic processes in atom Rydberg-atom collisions, as chemi-ionization and (n-n') mixing, should be considered together. Here we will review the present state of the art and the actual problems will be discussed. In this context, we will consider the influence of the (n-n')-mixing during a symmetric atom Rydberg-atom collision processes on the intensity of chemi-ionization process. It will be taken into account H(1s) + H*(n) collisional systems, where the principal quantum number n $>>$ 1. It will be demonstrated that the inclusion…
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 ion…
Current theory and measurements establish the age of the universe as ca. 13.8 billion years. For the first several hundred million years of its existence, it was a dark, opaque void. After that, the hydrogen atoms comprising most of the "ordinary" matter began to condense and ionize, eventually forming the first stars that would illuminate the sky. Details of how these "primordial" stars formed have been widely debated, but remain elusive. A central issue in this process is the mechanism by which the primordial gas (mainly hydrogen and helium atoms) collected via the action of dark matter cool…
Observation of resonant monopole-dipole energy transfer between Rydberg atoms and polar molecules
University College London（伦敦大学学院）；Department of Physics, Harvard University（哈佛大学物理系）；Instituto Carlos I de Física Teórica y Computacional, and Departamento de Física Atómica, Molecular y Nuclear, Universidad de Granada（格拉纳达大学理论计算物理卡洛斯一世研究所及原子、分子和核物理系）；Department of Physics and Astronomy, University College London（伦敦大学学院物理与天文系）
We experimentally demonstrate robust selective excitation and attenuation of atomic Rydberg level populations in sodium vapor (Na I) using intense laser pulses in the strong field limit ($> 10^{12} W/cm^{2}$). The coherent control of the atomic population and related ionization channels is realized for intensities above the over-the-barrier ionization intensity. A qualitative model predicts that this strong field coherent control arises through the manifestation of a Freeman resonance.
The complex processes leading to the collisional population of ultra-long-lived Rydberg states with very high angular momentum can be explained surprisingly well using classical mechanics. In this article, we explain the reason behind this striking agreement between classical theory and experiment by showing that the classical and quantum dynamics of Rydberg electrons in weak, slowly varying external fields agree beyond the mandates of Ehrenfest's Theorem. In particular, we show that the expectation values of angular momentum and Runge-Lenz vectors in hydrogenic eigenstates obey exactly the sa…
New experiments were proposed recently to investigate the regime of cold atomic and molecular ion-atom collision processes in a special hybrid neutral-atom--ion trap under high vacuum conditions. The collisional cooling of laser pre-cooled Ca$^+$ ions by ultracold Na atoms is being studied. Modeling this process requires knowledge of the radiative lifetime of the excited singlet A$^1Σ^+$ state of the (NaCa)$^+$ molecular system. We calculate the rate coefficient for radiative charge transfer using a semiclassical approach. The dipole radial matrix elements between the ground and the excited st…
We report the first unambiguous observational evidence of Rydberg Enhanced Recombination (RER), a potentially important recombination mechanism that has hitherto been unexplored in low-temperature photoionized plasmas. RER shares similarities with dielectronic recombination, with the difference that the electron is captured into a highly excited state below the ionization threshold -- rather than above the threshold -- of the recombining ion. We predict transitions of carbon and oxygen ions that are formed via the RER process, and their relative strengths with collisional-radiative spectral mo…
