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Physical Review A

High-lying Rydberg atoms surviving intense laser fields

Meng Zhao, YanLan Wang, Wei Quan, XuanYang Lai, Hongping Liu, Jian-Duo Lu, Xiaojun Liu

Published Oct 28, 2021• 10 citations
Publisher

Abstract

In this work, we have experimentally and theoretically investigated the high-lying Rydberg state excitation for noble gas atoms subject to an intense near-infrared laser field. To obtain the signal of these high-lying Rydberg atoms which are further ionized by a constant electric field $({F}_{c})$, coincident detection of the photoelectrons and photoions with well-chosen arrival times is performed. Based on a fitting to the time dependence of the coincidently measured photofragment yields with a semiempirical formula, we can extract a principal quantum number distribution (PQND) of the population of the excited states in a range closely related to the strength of ${F}_{c}$. The extracted valid PQND is in qualitative agreement with a semiclassical model calculation. Our work thus provides a method to extract the PQND and study the ultrafast high-lying Rydberg state excitation.

DOI
10.1103/physreva.104.043115

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In this work, we have experimentally and theoretically investigated the high-lying Rydberg state excitation for noble gas atoms subject to an intense near-infrared laser field. To obtain the signal of these high-lying Rydberg atoms which are further ionized by a constant electric field (Fc)({F}_{c})(Fc​), coincident detection of the photoelectrons and photoions with well-chosen arrival times is performed. Based on a fitting to the time dependence of the coincidently measured photofragment yields with a semiempirical formula, we can extract a principal quantum number distribution (PQND) of the population of the excited states in a range closely related to the strength of Fc{F}_{c}Fc​. The extracted valid PQND is in qualitative agreement with a semiclassical model calculation. Our work thus provides a method to extract the PQND and study the ultrafast high-lying Rydberg state excitation.
Using state-selective field ionization, the state distributions of Rydberg atoms in cold Rydberg gases are measured for various initially excited Rydberg levels, populations, and evolution times. We provide direct experimental evidence for lll-changing collisions that we previously observed indirectly [S. K. Dutta, D. Feldbaum, A. Walz-Flannigan, J. R. Guest, and G. Raithel, Phys. Rev. Lett. 86, 3993 (2001)]. We also observe nnn-mixing and find that its effects are largely in agreement with recent theoretical work on nnn-changing collisions between electrons and Rydberg atoms, thus enabling an estimation of the electron temperature. Unexpectedly large populations of atoms are found in states with principal quantum numbers much lower than that of the initially excited atoms. We explain this observation by collisions between high-lll Rydberg atoms, which are highly polar and can collide due to static electric-dipole forces between them.
Using field ionization combined with the direct detection of excited neutral atoms we measured the distribution of principal quantum number n of excited He Rydberg states after strong-field excitation at laser intensities well in the tunneling regime. Our results confirm theoretical predictions from semiclassical and quantum mechanical calculations and simultaneously underpin the validity of the semiclassical frustrated tunneling ionization model. Moreover, since our experimental detection scheme is spin sensitive in the case of He atoms, we show that strong-field excitation leads to strong population of triplet states. The origin of it lies in the fact that high angular momentum states are accessible in strong-field excitation. Thus, singlet-triplet transitions become possible due to the increased importance of spin-orbit interaction rather than due to direct laser induced spin-flip processes.
Rydberg-state excitation of atoms in strong infrared laser fields provides a new complementary aspect of the perspective of atom--strong field interactions. In this article, we perform an experimental and theoretical study on the corresponding process of diatomic molecules, N2{\mathrm{N}}_{2}N2​ and O2{\mathrm{O}}_{2}O2​. We show that neutral molecules can also survive strong 800-nm laser fields in high Rydberg states, while their behavior is remarkably different in comparison with their companion atoms, Ar and Xe. The Rydberg excitation of N2{\mathrm{N}}_{2}N2​ generally behaves similarly to Ar, while that of O2{\mathrm{O}}_{2}O2​ is more significantly suppressed than the ionization compared to Xe in a high intensity region, which can be understood in the frame of a semiclassical picture, together with their different structures of molecular orbitals. However, distinct quantum features in the Rydberg excitation processes that are apparently beyond the semiclassical picture have been identified, i.e., the less suppressed probability of O2{\mathrm{O}}_{2}O2​ at low intensity and the oscillation behavior of the ratio between N2{\mathrm{N}}_{2}N2​ and Ar, indicating that our understanding of the relevant physics is still far from complete.
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.
This paper summarizes a long series of experiments that have been done on Rydberg states of Rb. The basic experimental technique that has been used is atomic-beam laser spectroscopy which allows both low-resolution and high-resolution studies. Excitation of Rydberg states is provided by single-photon absorption from a suitably frequency-doubled rhodamine 6G6G6G tunable laser. Detection is done by field ionization and ion counting. These techniques have allowed us to study the critical ionizing field, which has been found to follow classical, hydrogenic behavior closely. Rydberg states of Rb have been observed from n=28n=28n=28 up to n>100n>100n>100. High-resolution spectroscopic studies have led to measurement of the fine structure for np\mathrm{np}np levels located between n=28n=28n=28 and n=60n=60n=60, as well as the isotope shift of the ground state, $\ensuremath{\delta}\ensuremath{\nu}=(172\ifmmode\pm\else\textpm\fi{}15)$ MHz. Anomalies in the intensity ratio of the doublet $5s\ensuremath{-}np$ transitions have been observed and interpreted as relativistic effects. Perturbations by weak and strong dc electric field are reported. In the case of weak electric fields it is possible to evaluate the polarizability. In the case of strong dc electric fields, new phenomena have been observed and analyzed. We also find experimental evidence of selective photoionization in the presence of an appropriate dc electric field, which could have some applications in laser isotope separation. Finally, we give the preliminary results of an experiment on the effect of a strong nonresonant electromagnetic field on high-lying Rydberg states.