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Journal of Physics B Atomic Molecular and Optical Physics

Coherent excitation of N=3 Stark states of hydrogen atoms

V. Lorent, P Antoine

Published Jan 14, 1991• 7 citations
Publisher

Abstract

The authors describe a method for producing a fast atomic hydrogen beam with a large amount of population selected in 3l j, mod mj mod levels. This is realized by a one-step tunable laser excitation of the metastable component of the atomic beam inside a nonhomogeneous static electric field. The linear laser polarization is taken either parallel or perpendicular with respect to the external field. It allows the selective excitation of all the states of the n=3 Stark manifold (with the exception of the mod mj mod =5/2 state). The electric field strength vanishes immediately after the laser excitation. At this point the population of the excited states are better referred to the atomic basis. The shapes of the resonant lines show that two transient effects are leading the excitation process. The first is of an optical kind (i.e. Rabi oscillation and rapid adiabatic passage) and the second is the intra Stark manifold state mixing due to the nonadiabatic time evolution of the external field strength. The internal state of the atoms crossing these fields is completely described by the density matrix evolution calculated independently on two bases (the atomic basis and the Stark instantaneous basis).

DOI
10.1088/0953-4075/24/1/024

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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}}$${\mathrm{H}}^{\mathrm{*}}$ 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 (${n}_{1}$,${n}_{2}$,\ensuremath{\Vert}${m}_{l}$\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{}${10}^{11}$ ${\mathrm{sec}}^{\mathrm{\ensuremath{-}}1}$. 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 ${F}^{3/4}$, with slight but definite deviations. Theoretical analysis of the oscillations yields quantitative agreement with the experiment.

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We derive a set of density matrix equations describing laser photo-excitation and ionization of atomic hydrogen in the presence of an external electric field. The equations are relevant as a description of multiphoton ionization of hydrogen (or deuterium) atoms in laser-produced transient plasmas. The laser wavelength is 243 nm, so that the photoionization is resonant with the 2 s 1/2 level. The electric field causes Stark mixing of the 2 s 1/2 level with the 2 p 1/2 and 2 p 3/2 levels. Because the electric field is taken in the same direction as the linear polarization of the laser, only states with equal m j are coupled, and the atom can be described with a four-level density matrix. The laser bandwidth is taken into account by using the stochastic model of a chaotic laser field introduced by Zoller [1]. We present a few calculations of the probabilities for ionization and excitation of a single hydrogen atom as a function of laser intensity and wavelength.

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H(3s) beam production by laser excitation of metastable hydrogen atoms in an electric field. II. Theoretical approach

D. Fussen, W. Claeys, A Cornet +1 more

For pt.I see ibid., vol.18, no.18, p.3557-37 (1985). A quantitative description of H(3s) atoms produced by laser excitation of a metastable hydrogen beam in an electric field is performed and compared with the recent experimental results of Claeys et al. (1985). The Stark effect for n=3 is calculated to obtain the relative intensities of the five Stark transitions as a function of the field strength. Good agreement with the experimental values is found. The dynamical behaviour of the 3s and 3p Stark states when the atoms leave the field is then analysed. Due to the adiabatic evolution we found that only one Stark state can produce H(3s) atoms.

Journal of Physics B Atomic and Molecular Physics•Sep 28, 1985•7 citations
The authors describe a method for producing a fast atomic hydrogen beam with a large amount of population selected in 3l j, mod mj mod levels. This is realized by a one-step tunable laser excitation of the metastable component of the atomic beam inside a nonhomogeneous static electric field. The linear laser polarization is taken either parallel or perpendicular with respect to the external field. It allows the selective excitation of all the states of the n=3 Stark manifold (with the exception of the mod mj mod =5/2 state). The electric field strength vanishes immediately after the laser excitation. At this point the population of the excited states are better referred to the atomic basis. The shapes of the resonant lines show that two transient effects are leading the excitation process. The first is of an optical kind (i.e. Rabi oscillation and rapid adiabatic passage) and the second is the intra Stark manifold state mixing due to the nonadiabatic time evolution of the external field strength. The internal state of the atoms crossing these fields is completely described by the density matrix evolution calculated independently on two bases (the atomic basis and the Stark instantaneous basis).
The authors studied in an earlier paper (1985) the production of a fast beam of H(3s) atoms. They investigated the particular problem of a coherent laser excitation of the 3s 1/2 and 3p 1/2 Stark states from the 2s 1/2 metastable Stark state. They measured the 3s 1/2 fluorescence outside the electric field and quantal interference effects have been observed as a function of the electric field strength. A simple theoretical interpretation is proposed which takes into account the quasi-adiabatic evolution of the atom in the electric field under the authors' experimental conditions.
The excitation of metastable hydrogen towards the n = 4 Stark manifold is investigated both theoretically and experimentally. The Stark Hamiltonian is diagonalized to obtain the energy levels, oscillator strengths and relaxation rates of the n = 2 and n = 4 Stark states. In a fast beam experiment, the transitions are excited by the blue line of a CW argon ion laser with appropriate Doppler detuning, and the measured transition frequencies agree well with the calculated values. The population of the 4s state, as measured by its fluorescence, is maximum for an electric field strength between 50 and 100 V cm/sup -1 /, and a laser polarization perpendicular to the static field.
Two synchronised pulsed single-mode tunable laser systems are used to excite atomic hydrogen in an atomic beam. A vacuum ultraviolet (VUV) laser populates first the 2p 2 P 3/2 sublevel from the ground 1s 2 S 1/2 state. A second-step UV laser selects substates of the n=33 manifold in the presence of a weak electric field (23.6 V cm -1 ). Stark patterns of this manifold are recorded for different polarisation configurations of the exciting light beams. The n=44 substates are detected by the standard field ionisation technique. The measured relative intensities of the Stark components agree with the theoretical excitation probabilities in the two-step process, calculated to the first order of perturbation theory.
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.
We derive a set of density matrix equations describing laser photo-excitation and ionization of atomic hydrogen in the presence of an external electric field. The equations are relevant as a description of multiphoton ionization of hydrogen (or deuterium) atoms in laser-produced transient plasmas. The laser wavelength is 243 nm, so that the photoionization is resonant with the 2 s 1/2 level. The electric field causes Stark mixing of the 2 s 1/2 level with the 2 p 1/2 and 2 p 3/2 levels. Because the electric field is taken in the same direction as the linear polarization of the laser, only states with equal m j are coupled, and the atom can be described with a four-level density matrix. The laser bandwidth is taken into account by using the stochastic model of a chaotic laser field introduced by Zoller [1]. We present a few calculations of the probabilities for ionization and excitation of a single hydrogen atom as a function of laser intensity and wavelength.
For pt.I see ibid., vol.18, no.18, p.3557-37 (1985). A quantitative description of H(3s) atoms produced by laser excitation of a metastable hydrogen beam in an electric field is performed and compared with the recent experimental results of Claeys et al. (1985). The Stark effect for n=3 is calculated to obtain the relative intensities of the five Stark transitions as a function of the field strength. Good agreement with the experimental values is found. The dynamical behaviour of the 3s and 3p Stark states when the atoms leave the field is then analysed. Due to the adiabatic evolution we found that only one Stark state can produce H(3s) atoms.