Coherent time evolution of highly excited Rydberg states in pulsed electric field: Opening a stringent way to selectively field-ionize the highly excited states
M. Tada, Y. Kishimoto, I. Ogawa, H. Funahashi, K. Yamamoto, S. Matsuki
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 is considered to be a manifestation of the strong coherence effect in the time evolution of the Rydberg states in pulsed electric field and opens a new effective way to stringently select a low-l state from the nearby states by field ionization.
The yield of neutral excited atoms and low-energy photoelectrons generated by the electron dynamics in the combined Coulomb and laser field after tunneling is investigated. We present results of Monte-Carlo simulations built on the two-step semiclassical model, as well as analytic estimates and scaling relations for the population trapping into the Rydberg states. It is shown that mainly those electrons are captured into bound states of the neutral atom that due to their initial conditions (i) have moderate drift momentum imparted by the laser field and (ii) avoid strong interaction ("hard" co…
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…
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…
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…
Neutral atom arrays are promising for large-scale quantum computing especially because it is possible to prepare large-scale qubit arrays. An unsolved issue is how to selectively excite one qubit deep in a 3D atomic array to Rydberg states. In this work, we show two methods for this purpose. The first method relies on a well-known result: in a dipole transition between two quantum states driven by two off-resonant fields of equal strength but opposite detunings $\pmΔ$, the transition is characterized by two counter-rotating Rabi frequencies $Ωe^{\pm iΔt}$~[or $\pmΩe^{\pm iΔt}$ if the two field…
We investigate the phenomenon of optical bistability in a driven ensemble of Rydberg atoms. By performing two experiments with thermal vapors of rubidium and cesium, we are able to shed light onto the underlying interaction mechanisms causing such a non-linear behavior. Due to the different properties of these two atomic species, we conclude that the large polarizability of Rydberg states in combination with electric fields of spontaneously ionized Rydberg atoms is the relevant interaction mechanism. In the case of rubidium, we directly measure the electric field in a bistable situation via tw…
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 …
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…
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…
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 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 on the formation of ultralong-range Rydberg D-state molecules via photoassociation in an ultracold cloud of rubidium atoms. By applying a magnetic offset field on the order of 10 G and high resolution spectroscopy, we are able to resolve individual rovibrational molecular states. A full theory, using the Born-Oppenheimer approximation including s- and p-wave scattering, reproduces the measured binding energies. The calculated molecular wavefunctions show that in the experiment we can selectively excite stationary molecular states with an extraordinary degree of alignment or anti-alig…
We report a systematic experimental and numerical study of the expansion of ultra-cold Rydberg plasmas. Specifically, we have measured the asymptotic expansion velocities, $v_0$, of ultra-cold neutral plasmas (UNPs) which evolve from cold, dense samples of Rydberg rubidium atoms using ion time-of-flight spectroscopy. From this, we have obtained values for the effective initial plasma electron temperature, $T_{e,0} = m_{ion} v_0^2/k_B$ (where $m_{ion}$ is the Rb$^+$ ion mass), as a function of the original Rydberg atom density and binding energy, $E_{b,i}$. We have also simulated numerically th…
Rydberg atoms, with one highly-excited, nearly-ionized electron, have extreme sensitivity to electric fields, including microwave fields ranging from 100 MHz to over 1 THz. Here we show that room-temperature Rydberg atoms can be used as sensitive, high bandwidth, microwave communication antennas. We demonstrate near photon-shot-noise limited readout of data encoded in amplitude-modulated 17 GHz microwaves, using an electromagnetically-induced-transparency (EIT) probing scheme. We measure a photon-shot-noise limited channel capacity of up to 8.2 Mbit/s and implement an 8-state phase-shift-keyin…
High-resolution photoelectron momentum distributions of Xe atoms ionized by 800-nm linearly polarized laser fields have been traced at intensities from 1.1*1013 to 3.5*1013W/cm2 using velocity-map imaging techniques. At certain laser intensities, the momentum spectrum exhibits a distinct double-ring structure for low-order above-threshold ionization, which appears to be absent at lower or higher laser intensities. By investigating the intensity-resolved photoelectron energy spectrum, we find that this double-ring structure originates from resonant multiphoton ionization involving multiple Rydb…
At intermediate to high densities, electron (de-)excitation collisions are the dominant process for populating or depopulating high Rydberg states. In particular, the accurate knowledge of the energy changing ($n$-changing) collisional rates is determinant for predicting the radio recombination spectra of gaseous nebula. The different datasets present in the literature come either from impact parameter calculations or semi-empirical fits and the rate coefficients agree within a factor of two. We show in this paper that these uncertainties cause errors lower than 5% in the emission of radio rec…
Ionized geocosmic media parameters in a thermal and a subthermal range of energy have a number of unique features. The photoresonance plasma that is formed by optical excitation of the lowest excited (resonance) atomic states is one example of conversion of radiation energy into electrical one. Since spontaneous fluorescence of excited atoms is probabilistic, the description of the radiating quantized system evolution along with photons energy transfer in a cold atoms medium, should include elements of stochastic dynamics. Finally, the chaotic dynamics of a weakly bound Rydberg electron over a…
We theoretically investigate high-order harmonic generation (HHG) in Rydberg atoms driven by spatially inhomogeneous laser fields, induced, for instance, by plasmonic enhancement. It is well known that the laser intensity should to exceed certain threshold in order to generate HHG, when noble gas atoms in their ground state are used as an active medium. One way to enhance the coherent light coming from a conventional laser oscillator is to take advantage of the amplification obtained by the so-called surface plasmon polaritons, created when a low intensity laser field is focused onto a metalli…
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…
An autoionizing resonance in molecular N$_2$ is excited by an ultrashort XUV pulse and probed by a subsequent weak IR pulse, which ionizes the contributing Rydberg states. Time- and angular-resolved photoelectron spectra recorded with a velocity map imaging spectrometer reveal two electronic contributions with different angular distributions. One of them has an exponential decay rate of $20\pm5$ fs, while the other one is shorter than 10 fs. This observation is interpreted as a manifestation of interference stabilization involving the two overlapping discrete Rydberg states. A formalism of int…
Photoelectron momentum distributions from strong-field ionization of carbonyl sulfide with 800 nm central-wavelength laser pulses at various peak intensities from $4.6$ to $13\times10^{13}$ W/cm$^2$ were recorded and analyzed regarding resonant Rydberg states and photoelectron orbital angular momentum. The evaluation of the differentials of the momentum distributions with respect to the peak intensity highly suppressed the impact of focal volume averaging and allowed for the unambiguous recognition of Freeman resonances. As a result, previously made assignments of photoelectron lines could be …
We present a full quantal study on the dissociation of a weakly bound molecular ion in the presence of an external time-dependent electric field. We focus on the dissociation dynamics of a molecular ion in a Paul trap relevant for atom-ion hybrid traps. Our results show that a weakly bound molecular ion survives in a Paul trap giving a theoretical ground to previous experimental findings [A. Krükow et al. Phys. Rev. Lett. 116, 193201 (2016) and A. Mohammadi et al. Phys. Rev. Research 3, 013196 (2021)]. In particular, we find that weakly bound molecular ions are more likely to survive in traps …
