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Physical Review

Two-Photon Ionization of Atomic Hydrogen

Wolfgang Zernik

Published Jul 6, 1964• 164 citations
Publisher

Abstract

This paper discusses the general theory of two-photon ionization of a hydrogenic state in the nonrelativistic dipole approximation. An application is made to the photoionization of the metastable $2S$ state of atomic hydrogen by optical radiation, for example, by the light from a ruby laser. The sum over intermediate states is carried out exactly by means of an implicit technique. The results are given for a range of wave-lengths from the threshold at 7290 down to 4556 \AA{}. At 6943 \AA{}, the total cross section per unit intensity is found to be 5.35\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}29}$ ${\mathrm{cm}}^{4}$ ${\mathrm{W}}^{\ensuremath{-}1}$. The lowest order damping corrections to the perturbation-theory results are worked out.

DOI
10.1103/physrev.135.a51

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The two-photon decay mode of hydrogenic atoms from an arbitrary state (${n}_{1}$, ${l}_{1}$, ${m}_{1}$) to an arbitrary state (${n}_{2}$, ${l}_{2}$, ${m}_{2}$) is studied within the framework of nonrelativistic quantum mechanics. In the dipole approximation, these decay rates, which involve infinite summation over intermediate states, are derived exactly via a general second-order matrix element obtained by Kelsey and Macek and an implicit technique introduced by Dalgarno and Lewis. The results are expressed in terms of hypergeometric functions. For transitions ${n}_{1}s\ensuremath{\rightarrow}{n}_{2}s$, our results reduce to those of Klarsfeld whose starting point is the Coulomb Green's function. For transitions to the ground state, an alternative expression involving a simple one-dimensional integral is presented. The decay rate of the $2s$ metastable state of atomic hydrogen is calculated as an illustration of the method. The result, $\frac{1}{\ensuremath{\tau}}=8.2284$ ${\mathrm{sec}}^{\ensuremath{-}1}$, agrees with Klarsfeld. For transitions of ${n}_{1}s\ensuremath{\rightarrow}1s$ and ${n}_{1}d\ensuremath{\rightarrow}1s ({n}_{1}\ensuremath{\ge}3)$, the transition rates exhibit interesting and unexpected structures. In particular, "zeros" are found in the two-photon emission spectrum indicating that two-photon emission is not possible at certain frequencies. Physically, these "zeros" are the result of destructive interference between the radiating dipole terms associated with the sum over intermediate states. In addition to the emission spectrum the expected coincidence signal between two detectors monitoring the two photons simultaneously emitted during a two-photon transition is calculated as a function of the angle between the detectors. The angular distribution for the ${n}_{1}d\ensuremath{\rightarrow}1s$ transitions is shown to be significantly different from the ${n}_{1}s\ensuremath{\rightarrow}1s$ transitions. Finally, a possible experiment is suggested to test the results presented in this paper.

Physical Review A•Sep 1, 1984•72 citations
This paper discusses the general theory of two-photon ionization of a hydrogenic state in the nonrelativistic dipole approximation. An application is made to the photoionization of the metastable 2S2S2S state of atomic hydrogen by optical radiation, for example, by the light from a ruby laser. The sum over intermediate states is carried out exactly by means of an implicit technique. The results are given for a range of wave-lengths from the threshold at 7290 down to 4556 \AA{}. At 6943 \AA{}, the total cross section per unit intensity is found to be 5.35\ifmmode\times\else\texttimes\fi{}10\ensuremath−29{10}^{\ensuremath{-}29}10\ensuremath−29 cm4{\mathrm{cm}}^{4}cm4 W\ensuremath−1{\mathrm{W}}^{\ensuremath{-}1}W\ensuremath−1. The lowest order damping corrections to the perturbation-theory results are worked out.
The theory of two-photon ionization of a hydrogenic state in the nonrelativistic dipole approximation is generalized for elliptically polarized light. An application to the metastable 2S state of atomic hydrogen is made. Significant differences in the angular distribution of the outgoing electrons are found depending upon the polarization of the photons. It is claimed that two-photon ionization employing elliptically polarized photons from lasers may provide an additional test for the theories of multiphoton ionization.
This paper is an extension of a previous one and discusses the theory of the quenching of the metastable 2S2S2S state of atomic hydrogen by means of optical radiation, for example by the light from a ruby laser. The case discussed is that for which the incident intensity is sufficiently weak for the usual quantum-electrodynamical perturbation theory to be valid. A procedure developed by Schwartz and others is used to carry out the sum over intermediate states without explicit enumeration. The results are given for a range of incident wavelengths from 5000 \AA{} to 5\ensuremath{\mu}. For unpolarized light from a ruby laser (6934 \AA{}), the total cross section for quenching is found to be ${\ensuremath{\sigma}}_{Q}=1.27\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}22}$ cm2{\mathrm{cm}}^{2}cm2. The cross section for coherent scattering has also been calculated for the same range of wavelengths; for ruby laser light, the total cross section for scattering is found to be ${\ensuremath{\sigma}}_{S}=1.03\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}23}$ cm2{\mathrm{cm}}^{2}cm2.
We investigate the absorption of two identical photons from the ground state of hydrogen-like atoms over an energy range that extends beyond that explored up to now. Our approach is based on a hybrid formula, valid in second-order perturbation theory, in which the A2{\mathbf{A}}^{2}A2 contribution from the nonrelativistic Hamiltonian is treated exactly, while the $\mathbf{A}\ifmmode\cdot\else\textperiodcentered\fi{}\mathbf{P}$ contribution is calculated in dipole approximation. We find that, at least up to 50 keV, the nonrelativistic dipole approximation, based only on the $\mathbf{A}\ifmmode\cdot\else\textperiodcentered\fi{}\mathbf{P}$ contribution, determines the values of the total cross section. Our numerical results, covering photon energies from 90 nm (13.7 eV) to 0.0248 nm (50 keV) are in very good agreement with most previous theoretical works. Differences with recent results are discussed.
This paper contains a generalization of results described in previous work. A general formula is given for the total cross section for two-photon ionization of a hydrogenic state. An implicit method for evaluating the second-order radial matrix elements that occur in this expression is described in detail. Numerical results were obtained for the states with principal quantum numbers n = 1 through 5. It is concluded that, when both one-photon and two-photon ionization are energetically possible, the effect of the latter may be expressed as an intensity-dependent correction to the Gaunt factor which may therefore be written as G = g1 + ζIλ3g2. Here g1 is the usual Gaunt factor, I is the intensity of the light in W cm−2, λ is the wavelength in cm, g2 is a dimensionless factor of order unity, and ζ is a constant given by ζ = 0.1504 W−1 cm−1. Graphs of g2 are given as a function of electron energy. These results do not include the effect of three-photon processes, which can also contribute to the first-order intensity-dependent correction to the Gaunt factor as a result of interference between the first- and third-order amplitudes.
The two-photon decay mode of hydrogenic atoms from an arbitrary state (n1{n}_{1}n1​, l1{l}_{1}l1​, m1{m}_{1}m1​) to an arbitrary state (n2{n}_{2}n2​, l2{l}_{2}l2​, m2{m}_{2}m2​) is studied within the framework of nonrelativistic quantum mechanics. In the dipole approximation, these decay rates, which involve infinite summation over intermediate states, are derived exactly via a general second-order matrix element obtained by Kelsey and Macek and an implicit technique introduced by Dalgarno and Lewis. The results are expressed in terms of hypergeometric functions. For transitions ${n}_{1}s\ensuremath{\rightarrow}{n}_{2}s$, our results reduce to those of Klarsfeld whose starting point is the Coulomb Green's function. For transitions to the ground state, an alternative expression involving a simple one-dimensional integral is presented. The decay rate of the 2s2s2s metastable state of atomic hydrogen is calculated as an illustration of the method. The result, $\frac{1}{\ensuremath{\tau}}=8.2284$ ${\mathrm{sec}}^{\ensuremath{-}1}$, agrees with Klarsfeld. For transitions of ${n}_{1}s\ensuremath{\rightarrow}1s$ and ${n}_{1}d\ensuremath{\rightarrow}1s ({n}_{1}\ensuremath{\ge}3)$, the transition rates exhibit interesting and unexpected structures. In particular, "zeros" are found in the two-photon emission spectrum indicating that two-photon emission is not possible at certain frequencies. Physically, these "zeros" are the result of destructive interference between the radiating dipole terms associated with the sum over intermediate states. In addition to the emission spectrum the expected coincidence signal between two detectors monitoring the two photons simultaneously emitted during a two-photon transition is calculated as a function of the angle between the detectors. The angular distribution for the ${n}_{1}d\ensuremath{\rightarrow}1s$ transitions is shown to be significantly different from the ${n}_{1}s\ensuremath{\rightarrow}1s$ transitions. Finally, a possible experiment is suggested to test the results presented in this paper.