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Physical Review Letters

Saturated Two-Photon Resonance Ionization of He(2S1)

G. S. Hurst, M. G. Payne, Munir Hasan Nayfeh, J. P. Judish, E. B. Wagner

Published Jul 14, 1975• 80 citations
Publisher

Abstract

We have developed a photoionization method for complete conversion of a quantum-selected population to ionization, making possible sensitive and absolute measurement of the selected populations in a gas. Each photoionization involves the absorption of two photons (from a pulsed dye laser), one of which is resonant with an intermediate state. In this demonstration we measured the absolute number of $\mathrm{He}(2^{1}S)$ states per ion pair following interaction of pulses of 2-MeV protons with He.

DOI
10.1103/physrevlett.35.82

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Journal de Physique IV (Proceedings)•Mar 1, 2000•0 citations
We have developed a photoionization method for complete conversion of a quantum-selected population to ionization, making possible sensitive and absolute measurement of the selected populations in a gas. Each photoionization involves the absorption of two photons (from a pulsed dye laser), one of which is resonant with an intermediate state. In this demonstration we measured the absolute number of He(21S)\mathrm{He}(2^{1}S)He(21S) states per ion pair following interaction of pulses of 2-MeV protons with He.
We have studied two-photon resonant three-photon ionization of atomic sodium vapor. A dye laser tuned to either the 4d or 5s two-photon allowed transition was used to excite the atom and a second more intense laser (λ = 7000 Å) was used for ionization. The ion yield was measured as a function of resonant laser intensity and detuning, the nonresonant laser intensity, and the temporal overlap of the exciting and ionizing laser pulses. We have found1 that at high laser intensities the photoionization yield decreases as the nonresonant laser intensity is increased. When tuned to the 5s level a value of ~−0.6 was obtained for the exponential index even with the resonant laser tuned to maximize the ion yield. A theoretical model including the effects of Stark shift of the ground state, power broadening of the intermediate level due to saturation of the two-photon transition and by rapid transitions to the ionization continuum was used to predict the experimental results. Good agreement between theory and experiment required the use of a photoionization cross section for the 5s level which was ~20 times greater than the accepted value. Results for photoionization from the 4d level are also presented.
Resonance ionization spectroscopy, RIS, is a multistep photon absorption process in which the final state is the ionization continuum of an atom. The RIS process can be saturated with available pulsed lasers, so that one electron can be removed from each atom of the selected type. This method was first applied to the determination of the absolute number of He(21S2^{1}S21S) excited states produced when pulsed beams of protons interacted with helium gas. Laser schemes for RIS are classified into five basic types; with these, nearly all of the elements can be detected with commercially available lasers. A periodic table is included showing schemes applicable to all of the elements except He, Ne, F, and Ar. A compact theory of the RIS process is presented which delineates the conditions under which rate equations apply. Questions on the effects of collisional line broadening, laser coherence time, and nonresonant multiphoton ionization processes are discussed. The initial demonstration of one-atom detection of Cs is described. By using laser beams to saturate the RIS process and by using proportional counters as single-electron detectors, one-atom detection is made possible. With RIS, one-atom detection is highly selective, has the ultimate in sensitivity, and has excellent space and time resolution. Furthermore, a modification of the technique in which single electrons (or single ions) are detected with a channel electron multiplier permits single-atom detection in a vacuum. Resonance ionization spectroscopy has application to classical phenomena such as the diffusion of free atoms, the chemical reaction of free atoms with a gas, the measurement of concentration fluctuations in a dilute vapor, and a variety of other atomic fluctuation phenomena. The authors describe how RIS can be used for photophysics measurements such as far wing collisional line broadening, measurements of photoionization cross sections for excited states, and collisional redistribution among excited states. Modern applications include the detection of single atoms in individual ionization tracks, such as those created by the binary fission of a parent atom, and the extension of this technique to the detection of stable or unstable daughter atoms in time coincidence with the decay of a parent atom. These methods are beig developed for use in low-level counting to determine, for example, the flux of solar neutrinos on the earth.
There have been relatively few investigations of multiphoton ionization from metastable helium. Of particular interest has been the work of Haberland et al. 1987 and Haberland and Oschwald 1988. In both the 1987 and 1988 papers they have described the two photon ionization of metastable helium. In each of these studies they have reported the occurrence of unexplained structure along the wings of their resonance profiles. Upon the performance of similar measurements by this study, the unexplained structure is not seen and the agreement of the experiment's measurements with the theoretical shape of the resonance curves has been good. To experimentally verify these resonance effects, we have used a tunable dye laser in conjunction with a time of flight mass spectrometer to create and detect ions from metastable helium by two-photon absorption. The use of a metastable state instead of the ground state is advantageous because of its proximity to the ionization continuum and its extended lifetime. Using a metastable state as a starting point for multiphoton absorption requires fewer photons to reach the ionization threshold. The extended lifetime of the state also makes it easy to access experimentally. For helium the singlet metastable state 2$\sp1$S lies at 20.61 eV above the ground level with a natural lifetime of close to a millisecond. Two photons of 501.7 nm and 504.35 nm are required for the ionization processes in resonance with the 3$\sp1$P and the 3$\sp1$D states. This thesis is the accounting of the experimental process involved in the measurement of the dipole and quadrupole resonances of two photon ionization from singlet metastable helium. The study includes the description of the laser, electron gun assembly for metastable helium creation, and the time of flight mass spectrometer. A discussion of the theory of multiphoton processes is included along with the discussion of the data, its reduction and analysis, and a comparison with theoretical prediction. This study has not only involved the acquisition of definitive atomic spectra data sets, but has also established a facility for resonant ionization spectroscopy at The American University.
Stimulated by a recent measurement of coherent control in photoionization of atomic barium, we have calculated one- and two-photon ionization cross sections of the aligned 6s6p 1P16s6p\text{ }{^{1}P}_{1}6s6p 1P1​ state of barium in the energy range between the 5d3/25{d}_{3/2}5d3/2​ and 5d5/25{d}_{5/2}5d5/2​ states of Ba+{\text{Ba}}^{+}Ba+. We have also measured these photoionization spectra in the same energy region, driving the one- or two-photon processes with the second or first harmonic of a tunable dye laser, respectively. Our calculations employ the eigenchannel RRR-matrix method and multichannel quantum defect theory to calculate the rich array of autoionizing resonances in this energy range. The nonresonant two-photon process is described using lowest-order perturbation theory for the photon-atom interactions, with a discretized intermediate-state one-electron continuum. The calculations provide an absolute normalization for the experiment, and they accurately reproduce the rich resonance structures in both the one- and two-photon cross sections, and confirm other aspects of the experimental observations. These results demonstrate the ability of these computationally inexpensive methods to reproduce experimental observables in one- and two-photon ionization of heavy alkaline earths, and they lay the groundwork for future studies of the phase-controlled interference between one- and two-photon ionization processes.
Possible schemes of resonance-enhanced two-photon selective ionization of indium atoms by using a dye laser were theoretically investigated. Ionization and excitation were performed by a dye laser [BPO, (395-415)x10-9 m] which was pumped with a pulse nitrogen laser. An optimal value of the focusing spot diameter within the interaction region that provides the maximal ions to be created for a given radiant power. We registered of about 100 ions for one laser pulse and a concentration of indium atoms of about 1014 m-3 for a trapping time of 100 periods of a rf field. Ion-atom scattering and electrode system imperfection cause the number of trapped ions to decrease by a factor of 2.71 for 10-2 c and a pressure of 4x10-6 Torr.