The Stark splitting of the second excited level of atomic hydrogen (with principal quantum number
n=3) has been measured by pulsed laser spectroscopy in order to determine small electric fields by optical means. Doppler-free excitation with two counterpropagating laser beams at
205nm allows us to measure the
n=3 Stark spectra either by an optogalvanic signal after ionization by a third laser photon or by detection of the Balmer-$\ensuremath{\alpha}$ fluorescence photons emitted by the excited atoms. Three different cases of laser polarization have been investigated in order to evaluate the possibilities and limitations of this one-step laser excitation method for electric field determination, especially at field strengths below
200V∕cm. The method provides the best field sensitivity achieved with lower excited levels that can be reached directly by two-photon absorption from the ground state (in contrast to the more sensitive Rydberg levels). For this purpose, an advanced tunable pulsed uv laser with narrow bandwidth almost at the Fourier limit has been used. The high spectral resolution allowed us to deduce electric field strengths as small as
50V∕cm from the frequency shift between two selected isolated Stark components. As a main advantage, this simple analysis of the measured spectra does not rely on knowledge of the line intensities which may be strongly affected by the measuring conditions.
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∗ 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,
n2,\ensuremath{\Vert}
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 ${\mathrm{sec}}^{\mathrm{\ensuremath{-}}1}$. 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, with slight but definite deviations. Theoretical analysis of the oscillations yields quantitative agreement with the experiment.
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 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.
We have measured certain ratios of transition intensities between excited hydrogen Stark sublevels over a range of electric-field values.
CO2 lasers were used to excite a fast beam of hydrogen atoms. The \ensuremath{\pi}-polarized transitions studied were from extremal Stark sublevels of principal quantum number n=10 to extremal and next extremal sublevels of n=30 and 44, at fields from 2 to 700 V/cm. The observed ratios are compared with those obtained using a non-relativistic zero-field formula attributed to Gordon [Ann. Phys. (Leipzig 2, 1031 (1929)] and with calculations employing matrix diagonalization including fine structure. Even for those relatively high n values, we find at low field significant deviations from results from Gordon's formula due to fine structure in the lower state as well as deviations at high field due to n mixing in the upper state induced by the static electric field. The experimental results and the matrix diagonalization calculations agree to within a few percent, which is the order of magnitude of possible saturation effects.
Second harmonic generation (SHG) in free atoms is one of the unsolved problems in nonlinear optics. The most probable mechanism is due to Stark mixing between nearby excited states through an electric field caused by charge separation through the process of three-photon ionization. To test the mechanism, atomic hydrogen appears to be the best candidate because of its well-known electronic structure and large dipole moments of its excited states. In this work we report on the observation of SHG in atomic hydrogen in the Lyman-α region. Pulsed dye laser radiation was doubled and tuned to 243 nm for excitation of the 2s ← 1s transition at 121.6 nm by a two-photon resonance process. A cw atomic beam was used with hydrogen atoms generated in a dc discharge of H2 gas. The laser beam was focused ~1 mm below the nozzle where the hydrogen atom density was estimated to be 1013 cm−3. The second harmonic radiation was strongly enhanced by adding an external dc field of up to 10 kV/cm. Stark splitting was clearly observed at higher fields.