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Cesium Rydberg states ionization study by 3-D ion-electron correlation

Raphaël Hahn, Azer Trimeche, C. Lopez, D. Comparat, Y. J. Picard

Published Nov 23, 2020• 0 citations
OpenAlex

Abstract

We study the excitation and ionization of cesium Rydberg states in an electric field (∼ 2200 V/cm) near the classical field ionization threshold (∼ −280 cm −1 binding energy at this field) by 3-D ionelectron coincidence spectroscopy. Cesium atoms are produced by an effusive oven and excited with lasers to Stark-shifted Rydberg states or directly ionised. Using a double Time of Flight setup we record 3-D (X, Y, Time of Flight) coincidence imaging of cesium produced electrons and ions. Above-threshold photo-ionisation creates broad images with poor electron/ion-coordinates correlation. Depending on the coupling of particular Rydberg states to the continuum, various images and correlations are observed. Fast ionising states show very good correlations and reveal the electric field lines, creating an efficient electric field mapping of the ionisation region. Slow ionising states show that the relatively high atomic velocity is detrimental to the correlations. Experimental data are accurately reproduced by detailed Monte Carlo excitation and ionization simulations based on Stark maps obtained with local-frame transformation (LFT) theory. Spectroscopic LFT agreement is usually very good with better that hundreds of MHz accuracy but on particular states several GHz discrepancy is found. The study can be used to select appropriate states for the creation of ion and electron beams with high brightness, good correlation and low energy dispersion, as well as to provide a detailed analysis of LFT-theory shortcomings.

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We study the excitation and ionization of cesium Rydberg states in an electric field (∼ 2200 V/cm) near the classical field ionization threshold (∼ −280 cm −1 binding energy at this field) by 3-D ionelectron coincidence spectroscopy. Cesium atoms are produced by an effusive oven and excited with lasers to Stark-shifted Rydberg states or directly ionised. Using a double Time of Flight setup we record 3-D (X, Y, Time of Flight) coincidence imaging of cesium produced electrons and ions. Above-threshold photo-ionisation creates broad images with poor electron/ion-coordinates correlation. Depending on the coupling of particular Rydberg states to the continuum, various images and correlations are observed. Fast ionising states show very good correlations and reveal the electric field lines, creating an efficient electric field mapping of the ionisation region. Slow ionising states show that the relatively high atomic velocity is detrimental to the correlations. Experimental data are accurately reproduced by detailed Monte Carlo excitation and ionization simulations based on Stark maps obtained with local-frame transformation (LFT) theory. Spectroscopic LFT agreement is usually very good with better that hundreds of MHz accuracy but on particular states several GHz discrepancy is found. The study can be used to select appropriate states for the creation of ion and electron beams with high brightness, good correlation and low energy dispersion, as well as to provide a detailed analysis of LFT-theory shortcomings.
We study the excitation and ionization of cesium Rydberg states in an electric field ($\ensuremath{\approx}\phantom{\rule{0.16em}{0ex}}2200\phantom{\rule{4pt}{0ex}}\mathrm{V}/\mathrm{cm}$) near the classical field-ionization threshold ($\ensuremath{\approx}\ensuremath{-}280\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$ binding energy) by three-dimensional (3D) ion-electron coincidence spectroscopy. Cesium atoms are produced by an effusive oven and excited with lasers to Stark-shifted Rydberg states or directly ionized. Using a double time-of-flight setup we record 3D (X,YX, YX,Y, time of flight) coincidence imaging of electrons and ions. Above-threshold photoionization creates broad images with poor electron-ion spatial correlation. Fast ionizing states produce very good correlations and the images reveal the electric-field map of the ionization region. Slow ionizing states show that the relatively high atomic velocity is detrimental to the correlations. Experimental data are accurately reproduced by detailed Monte Carlo excitation and ionization simulations based on Stark maps obtained with local-frame transformation (LFT) theory. Agreement between our spectroscopic experiment and LFT theory is very good, with better that hundreds of megahertz accuracy. But, on rare particular states, several gigahertz discrepancy is found. This study can be used to select appropriate states for the creation of ion and electron beams with high brightness, good correlation, and low energy dispersion.
Rydberg atoms, i.e. atoms with one or more highly excited electrons, show exaggerated properties compared to ground state atoms. For example, their energy levels are very sensitive to external electric fields (Stark effect) and they exhibit strong interatomic interactions, which can lead to a suppression of excitation known as the Rydberg blockade. The latter property makes Rydberg atoms promising candidates for quantum simulation and quantum computing. This work describes the direct observation of the excitation blockade for highly Stark-shifted Rydberg atoms induced by controllable dipole-dipole interactions. We investigate the electric field region around and above the classical ionization threshold, which is typically not considered suitable for blockade experiments. We excite Rydberg atoms in the energy region corresponding to the unperturbed 43S1/2 state at electric fields around 127V/cm out of a magneto-optically trapped cloud of 87Rb atoms with a temperature of 150 μK. We tune the dipole-dipole interaction by the applied electric field thus changing the electric dipole moment of the excited state. The position of the Rydberg atoms is detected by ionization and subsequent ion imaging; the controlled ionization of the atoms is achieved by adiabatic transfer of the Rydberg state to an ionizing state. For the spatially resolved detection of the atoms, a high resolution ion microscope for cold atoms has been developed and experimentally characterized. It features a maximum magnification of 1000 and sub-micrometer spatial resolution. A theoretical treatment of highly Stark-shifted Rydberg states is developed introducing a complex absorbing potential. It is capable of predicting the ionization rates of the Rydberg states for a wide range of electric fields and energies with only one free parameter. Together with the numerical calculations, measurements of the ionization spectra for different Rydberg states are presented. The 43S1/2 state is measured in an electric-field range from 125V/cm to 165V/cm (classical ionization limit 127V/cm), the 70S1/2 state in an electric-field range from 15V/cm to 35V/cm (classical ionization limit 16.1V/cm) and the 100S1/2 state in an electric-field range from 7V/cm to 19V/cm (classical ionization limit 3.7V/cm). Our results show an intricate energy level structure with broad, strongly ionizing states as well as sharp, nearly non-ionizing states. The numerical calculations are also used for the prediction of selective field ionization spectra and the results are used to identify Förster resonances in the Stark spectrum of the 45D5/2 state. Complementary to the spatially resolved measurements in high electric fields, the Rydberg blockade effect is also observed via the excitation number statistics at Förster resonances.
We study Rydberg ionization in an electric field in order to produce monochromatic ion and electron beams. We present an experimental study of the photoexcitation and ionization of high quantum-defect states, using excitation from the 7s7s7s state in cesium to Rydberg states in the presence of a uniform electric field. Such states can exhibit complex ionization behavior, for instance, highly localized growth in the ionization rate due to interference effects. The data are well reproduced by the WKB quantum-defect and frame transformation methods with no adjustable parameters. This indicates that large changes in the Rydberg ionization rate from small changes in electric field are possible when a nearly stable state crosses a more unstable state. A fast variation of the ionization rate with electric field allows for the production of beams with very low energy dispersion. We develop a simple two-level model to predict the voltage and spatial resolution that would occur when atoms are prepared in a state with such sharp ionization in electric field. This confirms that Rydberg forced ionization in an electric field presents a pathway for the production of high-brightness, highly monochromatic ion and electron beams.
We investigate the field ionization spectra of ultracold cesium Rydberg atoms in dc electric field. The ionization thresholds of different electric fields are measured and shift of the ionization threshold relative to field-free ionization threshold is accurately described by (6.06 ± 0.14) F 1/2 , which is in good agreement with the classical saddle-point model for field ionization. We obtain the field-free ionization threshold of cesium (6P 3/2 ) as 19674.89 ± 2.99 cm −1 by fitting experimental data.
The authors have studied phenomena related to the ionisation of indium Rydberg atoms by an external electric field. The indium atoms are excited in an atomic beam apparatus by pulsed dye laser light. The high-lying states are populated in one step from the ground state by an ultraviolet, frequency-doubled dye laser or by stepwise excitation using two dye lasers in the visible region. Shortly after the excitation, an electric field is applied in the interaction region which causes ionisation of the highly excited atoms. The authors have investigated (i) the lowest adiabatic ionisation threshold over a wide range of n values and compared the results with model predictions, (ii) the structure in the adiabatic part of the ionisation spectrum, and (iii) the transition from adiabatic to diabatic ionisation as a function of the slew rate of the ionising field pulse and the quantum defect and quantum numbers of the atomic state concerned. The ionisation signal is demonstrated to shift considerably towards higher field strengths with increasing slew rate. A qualitative explanation is presented and consequences for the detection efficiency are mentioned. Differences in the field ionisation behaviour between nearly degenerate excited states are demonstrated and exploited to achieve selective detection of fine-structure and even hyperfine-structure states.
Stark spectra of barium Rydberg states above the classical field-ionization limit have been recorded at high density of states employing high-resolution laser spectroscopy. The spectra, taken at a binding energy of about \ensuremath{\varepsilon}\ensuremath{\approxeq}-55 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ with respect to zero-field threshold and at electric-field strengths F\ensuremath{\approxeq}100 V/cm exhibit dramatic variations in line profiles with increasing external field strength. The WKB quantum-defect theory of the Stark effect of nonhydrogenic atoms was used to analyze the recorded spectra, and excellent agreement between measured and calculated line profiles was achieved. Core-induced coupling of closed and open hydrogenic Stark channels was found to contribute dominantly to the linewidth of the recorded Stark resonances. In addition, a reformulation of this theory by McNicholl, Ivri, and Bergeman (unpublished) in terms of a configuration-interaction model was employed to analyze a particular avoided crossing of several Stark components. In this way recorded line profiles were parametrized within a limited model to obtain resonance energies, linewidths, and Fano q parameters.