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Investigation of the frequency dependence of processes of multiphoton ionization of helium atoms excited in the 2s state

I.Sh. Bakosh, M. L. Nagaeva, V.G. Ovchinnikov, David M. Rubin

Published Sep 1, 1973• 0 citations
OpenAlex

Abstract

The three-photon ionization of He atoms, excited in the metastable state, is experimentally studied as a function of the radiation frequency of the ruby laser. The sizes of the cross section for the three-photon ionization and the ratio of the ionization cross section of the singlet and triplet multistable atoms are evaluated. (tr-auth)

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Three Photon Ionization of a Helium Atom in the Excited 2S Metastable State

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The purpose of the work is to observe three photon ionization of the helium atom in the 2S metastable state. The metastable helium atoms were produced in a cylindrical glass tube by low-current gas discharge. Ruby laser emission was used for ionization. (Author)

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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.

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Theoretical calculations for the 1S → 2S two- photon transition rate in atomic hydrogen are reviewed. They are compared with two experiments via the saturation effects that are observed when three-photon ionization is enhanced by two- photon resonance with the metastable 2S state. There is a significant disagreement between theoretical and experimental results. The disagreement is illustrated by determining the transition rate as a function of intensity for experimental laser profiles: (1) using parameters that give rates in agreement with experimental data, and (2) using theoretical values for the parameters. Finally, experiments that would involve direct observation of the 2S metastable state are considered. It is shown that single-longitudinal-mode laser experiments would provide an accurate measurement of the Rabi frequency for this transition and yield a definitive value for the rate. A Monte Carlo simulation method is used to consider practical effects associated with such an experiment, for example, chirp and ASE noise in the laser. Also, simulations of the multiphoton ionization process in multimode and wide band laser fields are presented.

Annual Meeting Optical Society of America•Jan 1, 1991•0 citations
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.
A joint experimental and theoretical study of three-photon ionization of the 1s2p3Po1s2p{\phantom{\rule{0.16em}{0ex}}}^{3}{P}^{o}1s2p3Po(${M}_{L}=0,\ifmmode\pm\else\textpm\fi{}1$) states of helium is presented. The ion yield is recorded in the 690--730 nm wavelength range for different laser pulse energies, using an excited helium beam produced by photodetachment of helium negative ions. Two series of asymmetric peaks due to two-photon resonances with 1snp1snp1snp and 1snf1snf1snf Rydberg states are observed. In one series, the peaks have tails towards higher frequencies, while in the other series the tails change direction for higher Rydberg states. An effective Hamiltonian is built in the dressed state picture, and a numerical model simulating the traversal of the helium atom across the laser pulse is developed. The simulated and observed ion yields are in good qualitative agreement. The observed behavior is shown to result from the contributions of two different resonantly enhanced multiphoton ionization processes, depending on the magnetic quantum number ML{M}_{L}ML​ of the initial state. The asymmetry reversal is explained by the strong 1s2p1s2p1s2p--1s3s1s3s1s3s dynamic Stark mixing for ML=0{M}_{L}=0ML​=0.
Calculations of the two-photon ionization of metastable levels of helium and the first three s levels of cesium are presented. The calculations are carried out to second order in a perturbation expansion and are valid for low laser intensities. The behavior of the ionization cross section at high photon frequencies ω is studied, and it is found that the N-photon ionization cross section behaves as σ(N) ∝ ω−(2N+1/2). This analytic asymptotic behavior is verified numerically in the case of two-photon ionization.
Multipole interference effects are predicted in the generalized cross sections, and in the ratio $\frac{{\stackrel{^}{\ensuremath{\sigma}}}_{C}}{{\stackrel{^}{\ensuremath{\sigma}}}_{L}}$ of the cross sections for circularly and linearly polarized laser light for the case of the two-photon ionization of the n=2n=2n=2 singlet metastable helium atoms in the wavelength range 5036-5050 \AA{}.
Theoretical calculations for the 1S → 2S two- photon transition rate in atomic hydrogen are reviewed. They are compared with two experiments via the saturation effects that are observed when three-photon ionization is enhanced by two- photon resonance with the metastable 2S state. There is a significant disagreement between theoretical and experimental results. The disagreement is illustrated by determining the transition rate as a function of intensity for experimental laser profiles: (1) using parameters that give rates in agreement with experimental data, and (2) using theoretical values for the parameters. Finally, experiments that would involve direct observation of the 2S metastable state are considered. It is shown that single-longitudinal-mode laser experiments would provide an accurate measurement of the Rabi frequency for this transition and yield a definitive value for the rate. A Monte Carlo simulation method is used to consider practical effects associated with such an experiment, for example, chirp and ASE noise in the laser. Also, simulations of the multiphoton ionization process in multimode and wide band laser fields are presented.