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Physical Review A

Spectrum of quasistable states in a strong infrared field

Changchun Zhong, F. Robicheaux

Published Jul 13, 2015• 1 citation
Publisher

Abstract

The quasi-stability of highly-exicited H and He atoms in a strong infrared (IR) field is studied based on three-dimensional quantum calculations.The spectra of atoms that survive the IR field show a series of IR-frequency-modulated peaks which extend from deeply bound states all the way to the ionization threshold and above.The atoms that survive mainly consist of highly-excited Rydberg states, even after hundreds of the intense IR cycles.Also they tend to have initial energies which allow emission or absorption of an integer number of IR photons to reach these quasi-stable states.Peaks above the ionization threshold in the survival spectra indicate the existence of multi-photon assisted recombination in the intense IR field.

DOI
10.1103/physreva.92.013406

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The quasi-stability of highly-exicited H and He atoms in a strong infrared (IR) field is studied based on three-dimensional quantum calculations.The spectra of atoms that survive the IR field show a series of IR-frequency-modulated peaks which extend from deeply bound states all the way to the ionization threshold and above.The atoms that survive mainly consist of highly-excited Rydberg states, even after hundreds of the intense IR cycles.Also they tend to have initial energies which allow emission or absorption of an integer number of IR photons to reach these quasi-stable states.Peaks above the ionization threshold in the survival spectra indicate the existence of multi-photon assisted recombination in the intense IR field.
When atoms are exposed to intense laser or microwave pulses, $\ensuremath{\sim}10%$ of the atoms are found in Rydberg states subsequent to the pulse, even if it is far more intense than required for static field ionization. The optical spectra of the surviving Li atoms in the presence of a 38-GHz microwave field suggest how atoms survive an intense pulse. The spectra exhibit a periodic train of peaks 38 GHz apart. One peak is just below the limit, and with a 90-V/cm field amplitude the train extends from 300 GHz above the limit to 3000 GHz below it. The spectra and quantum-mechanical calculations imply that the atoms survive in quasistable states in which the Rydberg electron is in a weakly bound orbit infrequently returning to the ionic core during the intense pulse.
We study the quasistability of UV-pulse-train-excited H atoms in a strong infrared (IR) laser as a function of the phase delay of the UV pulse train relative to the IR laser. The UV pulse train contains two frequency components. When the two components have frequencies separated by two IR photons, the population of surviving electrons is modulated by up to ten percent. When electrons are excited to right above or below the threshold, the survival probabilities have inverted phase delay dependence, which can be explained classically. When the two frequencies are one IR photon apart, the angular symmetry of the quasistable electrons is broken, and the asymmetry is also controlled by the phase delay. The asymmetrical distribution can be observed while the IR is on and smoothly evolves to a nonzero asymmetry that only weakly depends on the duration of the IR field.
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.
We have studied ionization and excitation of Rydberg atoms by intense sub‐picosecond electromagnetic field pulses of less than one cycle duration. The ionization threshold electric field scales as the binding energy (i.e., n*−2, rather than the n*−4 threshold scaling characteristic of static field ionization and high order multiphoton ionization. This altered behavior is due to the short duration and the subcycle nature of the field. We also find a wide distribution of final states produced by these pulses, which are effectively ‘‘in resonance’’ for dozens of transitions simultaneously.
The Stark spectroscopy of the hydrogen atom has been investigated near the ionization threshold in static homogeneous external electric fields from \ensuremath{\sim}1000 to \ensuremath{\sim}8000 V/cm with use of a two-step excitation H(n=1)+\ensuremath{\Elzxh}${\ensuremath{\omega}}_{\mathrm{vuv}\ensuremath{\rightarrow}}$H(n=2)+\ensuremath{\Elzxh}\ensuremath{\omega} $_{\mathrm{uv}\ensuremath{\rightarrow}}$H∗{\mathrm{H}}^{\mathrm{*}}H∗ with vuv and uv laser radiation, independently tunable and linearly polarized either parallel (\ensuremath{\pi}) or perpendicular (\ensuremath{\sigma}) with respect to the external field. Different from other, nonhydrogenic atoms, the hydrogen atom is a peculiar case insofar as the initial states of H(n=2), from which excitation takes place, are essentially of parabolic character at the field strengths employed in this study.Individual sublevels (n1{n}_{1}n1​,n2{n}_{2}n2​,\ensuremath{\Vert}ml{m}_{l}ml​\ensuremath{\Vert}) have been prepared in the n=2 state with sub-Doppler resolution. Photoionization spectra have been obtained with \ensuremath{\pi}- and \ensuremath{\sigma}-polarized uv radiation from the four possible sublevels of the n=2 Stark manifold: \ensuremath{\Vert}1,0,0〉 \ensuremath{\Vert}\ifmmode\pm\else\textpm\fi{}1/2〉, \ensuremath{\Vert}0,1,0〉 \ensuremath{\Vert}\ifmmode\pm\else\textpm\fi{}1/2〉, \ensuremath{\Vert}0,0,\ifmmode\pm\else\textpm\fi{}1〉 \ensuremath{\Vert}\ifmmode\pm\else\textpm\fi{}1/2〉, and \ensuremath{\Vert}0,0,\ensuremath{\mp}1〉 \ensuremath{\Vert}\ifmmode\pm\else\textpm\fi{}1/2〉. All spectra show sharp line structures of quasistable field-ionizing states superimposed on continua in the energy region between the classical saddle point, ${E}_{\mathrm{SP}=\mathrm{\ensuremath{-}}2\phantom{\rule{0ex}{0ex}}\mathrm{\ensuremath{\surd}}\mathrm{F}}$ a.u., and the zero-field ionization threshold E=0 a.u. Employing existing theoretical treatments, the quasistable spectral structures are quantitatively completely analyzed and accounted for, as long as their field ionization rate is less than \ensuremath{\sim}5\ifmmode\times\else\texttimes\fi{}1011{10}^{11}1011 ${\mathrm{sec}}^{\mathrm{\ensuremath{-}}1}$. Field-ionization rates of quasistable states have been measured and are compared with theory. Oscillatory resonance structures of the ionization cross section near the zero-field threshold are observed with pronounced modulation degree only in the spectrum from the \ensuremath{\Vert}1,0,0〉 \ensuremath{\Vert}\ifmmode\pm\else\textpm\fi{}1/2〉 sublevel excited with the uv \ensuremath{\pi}-polarized. The energy spacing of the oscillations has been measured as a function of the electric field strength F and found to be nearly proportional to F3/4{F}^{3/4}F3/4, with slight but definite deviations. Theoretical analysis of the oscillations yields quantitative agreement with the experiment.