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Topical Meeting on Laser Techniques in the Extreme Ultraviolet

Non-Linear Mixing

K. H. Welge

Published Jan 1, 1982• 0 citations
Publisher

Abstract

We report investigations with tunable VUV radiation, employing VUV generation in regions down to the cut-off wavelength of lithium fluorid crystal (~ 110 nm) by frequency tripling of tunable UV from dye laser. -Experiments on multiphoton excitation and ionization of atomic hydrogen with tunable VUV light at Lyman-α, have been carried out with the following objectives: (1) sensitive H and D atom detection by two-photon ionization i. e. 1s ω Lyα → 2 p ω uv → ion , (2) two-photon ionization of H with high resolution at Lyman-α to resolve the hyperfine groundstate doublet, aiming at the production of polarized protons, (3) state selective production of high Rydberg states ( 1 s ω Lyα → 2p ω uv → ns, nd ) , and their ionization, (4) Doppler line shape spectroscopy at Lyman-α applied to recoil energy and momentum distribution measurements of H and D atoms in dissociation processes. -Depending on the objective, different experimental conditions and systems have been employed, for instance atomic beam configuration, mass-spectroscopic ion detection, field ionization in cryogenetic environment, and for Doppler measurements laser induced fluorescence.

DOI
10.1364/euvs.1982.wa1

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We report investigations with tunable VUV radiation, employing VUV generation in regions down to the cut-off wavelength of lithium fluorid crystal (~ 110 nm) by frequency tripling of tunable UV from dye laser. -Experiments on multiphoton excitation and ionization of atomic hydrogen with tunable VUV light at Lyman-α, have been carried out with the following objectives: (1) sensitive H and D atom detection by two-photon ionization i. e. 1s ω Lyα → 2 p ω uv → ion , (2) two-photon ionization of H with high resolution at Lyman-α to resolve the hyperfine groundstate doublet, aiming at the production of polarized protons, (3) state selective production of high Rydberg states ( 1 s ω Lyα → 2p ω uv → ns, nd ) , and their ionization, (4) Doppler line shape spectroscopy at Lyman-α applied to recoil energy and momentum distribution measurements of H and D atoms in dissociation processes. -Depending on the objective, different experimental conditions and systems have been employed, for instance atomic beam configuration, mass-spectroscopic ion detection, field ionization in cryogenetic environment, and for Doppler measurements laser induced fluorescence.
Two kinds of experiments with tunable VUV laser light have been carried out with H atoms: (1) High resolution resonant two‐photon ionization, H(1 2S1/2)+hνα→H(2 2P1/2,3/2)+ hνuv→H++e with tunable Lyman‐α light and (2) resonant tow photon excitation of high Rydberg states. H(1 2S1/2)+hνα→H(2 2P)+hνuv →H(n 2S, n 2D)→H++e followed by ionization through collisions. In both cases an atomic beam configuration has been employed and H+ ions were detected with a mass filter. The smallest bandwidth of tunable Lyman‐α radiation achieved was ∼1.0 Ghz, enough for partial resolution of the hyperfine structure doublet of the 1 2S1/2 ground state. The application to produce polarized protons by high resolution two photon ionization is discussed. Rydberg states have been excited up to n∼48 and detected by collisional ionization under the given experimental conditons.
We have observed second-harmonic generation in atomic hydrogen in the Lyman-α region, with and without an applied dc electric field, Ea. Experiments with a continuous atomic beam were carried out by using a pulsed dye laser tuned to 243 nm for excitation of the n = 2-1 transition. The laser beam was focused 0.4 mm below the H-source nozzle, where the H-atom density was estimated to be 5 × 1013 cm-3. Measurements of second-harmonic generation (SHG) at ~122 nm were made at various electric fields up to ~27 kV/cm. It was shown that the SH signal produced at E a = 0 occurs because of a charge-separation field of ~800 V/cm that is caused by three-photon ionization. Measurements of the SHG and ion current were found to vary as I2 L and I3 L , respectively. At high fields (E a > 10 kV/cm) the SH signal at the center of the Stark-split components decreased somewhat from the peak value, but the ion current (corresponding to photon absorption) approached zero. This observation is a clear demonstration of a similar effect, predicted by Harris et al.1 of efficient nonlinear conversion with induced transparency, and it suggests the possibility of obtaining intense Lyman-a radiation.
Multiphoton ionization (MPI) of alkali atoms has played a pivotal role in our understanding of the interaction of intense electromagnetic radiation with matter. The "hydrogen-like" energy levels and absence of low-lying autoionizing states make the alkali atom theoretically tractable. The low ionization potential of these atomic species and the ease with which one can produce atomic beams of alkali atoms facilitate the experimental studies. Many of the early MPI studies involved high-powered fixed-frequency lasers. Presently, the availability of tunable dye lasers with wavelength extension (i.e., frequency doubling, Raman shifting, etc.) makes it possible to study one- to six-photon ionization of the alkali atom with continuously tunable radiation. Also, harmonic generation in these systems which may be present during ionization can be recorded more easily than in other systems since the radiation generated is in the visible or near ultraviolet spectral region. The ability to tune the laser to high Rydberg states with even or odd numbers of photons accesses electronic states of both parities. Stepwise excitation is capable of selectively producing states of high orbital angular momentum. Experiments in which highly excited states are produced in external electric or magnetic fields allow one to test fundamental ideas about the electron–Coulomb system in the quasi–continuum.3
High-power tunable VUV light pulses with energies up to 0.7 μJ were generated in the 115.7–116.9-nm region by use of a two-photon resonant four-wave mixing scheme in a Xe–Ar gas mixture. This is the highest reported pulse energy that has been produced in this wavelength region using a four-wave mixing process. Efficient detection of krypton isotopes at densities as low as 10 atoms/cm3 was demonstrated by resonantly ionizing the atom through its one-photon allowed state at the vacuum wavelength of 116.49 nm.