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Physical Review A

Two-photon decay of hydrogenic atoms

J. H. Tung, X. M. Salamo, F. T. Chan

Published Sep 1, 1984• 72 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.30.1175

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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 n1s\ensuremath→n2s{n}_{1}s\ensuremath{\rightarrow}{n}_{2}sn1​s\ensuremath→n2​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, 1\ensuremathτ=8.2284\frac{1}{\ensuremath{\tau}}=8.2284\ensuremathτ1​=8.2284 sec\ensuremath−1{\mathrm{sec}}^{\ensuremath{-}1}sec\ensuremath−1, agrees with Klarsfeld. For transitions of n1s\ensuremath→1s{n}_{1}s\ensuremath{\rightarrow}1sn1​s\ensuremath→1s and n1d\ensuremath→1s(n1\ensuremath≥3){n}_{1}d\ensuremath{\rightarrow}1s ({n}_{1}\ensuremath{\ge}3)n1​d\ensuremath→1s(n1​\ensuremath≥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 n1d\ensuremath→1s{n}_{1}d\ensuremath{\rightarrow}1sn1​d\ensuremath→1s transitions is shown to be significantly different from the n1s\ensuremath→1s{n}_{1}s\ensuremath{\rightarrow}1sn1​s\ensuremath→1s transitions. Finally, a possible experiment is suggested to test the results presented in this paper.
Within the framework of nonrelativistic quantum mechanics, the analysis of the two-photon absorption by atomic hydrogen is generalized to the case of two incident beams with arbitrary direction and polarization (including circular polarization). In the dipole approximation, the second-order matrix elements responsible for two-photon absorption are transformed into a finite sum consisting of the product of a radial part and an angular part. Exact calculation of the angular part predicts that, for the s–s transition only, transparency is obtained regardless of the frequencies of the two beams with perpendicular polarizations. In addition, circularly polarized light is found to be more efficient (up to a factor of 1.5) for the s–d two-photon transition. The radial parts of the matrix elements are accurately evaluated by using the Coulomb Green’s function technique and an implicit technique of Dalgarno and Lewis. Their calculation indicates that “zeros” exist in the two-photon absorption spectrum, thereby predicting that absorption is not possible at certain frequencies. It should be noted that in the calculated spectrum, near or at resonance points, the linewidths of the intermediate levels must be included in order to obtain accurate results.
The hyperfine levels for the ground state of hydrogen are normally connected by magnetic dipole transitions. However, for astrophysical applications, it may be that two-photon electric dipole processes are also important over cosmological distances. This thesis sets up a general mathematical formalism for the calculation of two-photon processes within the hyperfine structure of an atom with spin 1/21/21/2, and applies it to the ground state of hydrogen. Rates are calculated for both spontaneous emission and absorption of radiation. Due to an extraordinary degree of cancellation in the matrix elements, the rates turn out to be too small to have a significant impact on astrophysical processes involving the absorption and emission of radiation. The results are nevertheless important in reducing the uncertainty due to possible contributions from these processes. Other two-photon processes involving Raman scattering are also considered and the relevant cross sections calculated. The calculations of the decay rate, absorption coefficient and Raman scattering cross section are extended to heavier hydrogenic ions as a function of the nuclear charge ZZZ, using an approximate interpolation formula for the hyperfine splitting in the ground state. Results are presented for the hydrogenlike ions from He+^++ to Pb81+^{81+}81+. Modifications for the case of isotopes with a nuclear spin greater than 1/21/21/2 are briefly considered
Two-photon transitions for hydrogen and hydrogenlike ions in arbitrary magnetic fields are investigated using currently available nonrelativistic energy levels and one-photon dipole transition probabilities. For hydrogen, the 2s-1s two-photon spontaneous-decay rate is shown to increase rapidly with the strength of the applied field from its field-free value of 8.2284 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ to a maximum of 1.537\ifmmode\times\else\texttimes\fi{}108{10}^{8}108 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ at 1.41\ifmmode\times\else\texttimes\fi{}106{10}^{6}106 T, approaching that of the 2p-1s one-photon rate, and to drop slightly to 1.055\ifmmode\times\else\texttimes\fi{}108{10}^{8}108 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ at 4.7\ifmmode\times\else\texttimes\fi{}108{10}^{8}108 T. The transition rate is shown to scale as Z4{\mathit{Z}}^{4}Z4 for hydrogenic ions with nuclear charge Z in fields \ensuremath{\ge}3300Z2{\mathit{Z}}^{2}Z2 T. The spectral distribution of the photons for the 2s-1s transition in a large field reveals interesting features including resonances due to migration of the 2p0{\mathit{p}}_{0}p0​ and 2${\mathit{p}}_{\mathrm{\ensuremath{-}}1}$ energy levels between the 1s and 2s levels and the appearance of minima resulting from destructive interference between the intermediate-state dipole terms. In the field-free case, these spectral features are only present for high-lying-state transitions, i.e., 3s-1s, 4s-1s, etc.
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{}${10}^{\ensuremath{-}29}$ cm4{\mathrm{cm}}^{4}cm4 ${\mathrm{W}}^{\ensuremath{-}1}$. The lowest order damping corrections to the perturbation-theory results are worked out.
The general theory of multiphoton ionization of hydrogen atoms by simultaneous absorption of several photons is discussed. In the nonrelativistic dipole approximation, the calculations lead to a recursion relationship concerning angular functions and involve radial matrix elements containing many summations over intermediate states. A general method for exactly evaluating several sums is described in detail and applied to the photo-ionization of atomic hydrogen in the ground state. Numerical results are presented as dispersion curves of the transition rate $\frac{{\ensuremath{\sigma}}_{n}}{{I}^{N\ensuremath{-}1}}$ for a range of wavelengths from 1000 up to 7200 \AA{}.