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Physical Review A

Nonvanishing J=1↔0 equal-frequency two-photon decay: E1M2 decay of the He-like 2S13 state

R. W. Dunford

Published Jun 3, 2004• 15 citations
Publisher

Abstract

The selection rule which forbids $J=1\ensuremath{\leftrightarrow}0$ two-photon decay when the energies of the two photons are equal is shown to apply only when the multipolarities of the two photons are the same (i.e., $2E1$, $2M1$, etc.) and does not generally apply to mixed multipolarity amplitudes such as $E1M2$. A calculation of the two-photon decay rate for He-like ions in the $2\phantom{\rule{0.2em}{0ex}}^{3}S_{1}$ state including both $2E1$ and $E1M2$ two-photon decay amplitudes is presented. It shows a significant contribution for the case of equal-energy photons. The ratio of the $E1M2$ contribution to the $2E1$ contribution is found to be surprisingly large. For example, it is 0.27 for two-photon decay of the $2\phantom{\rule{0.2em}{0ex}}^{3}S_{1}$state in He-like uranium.

DOI
10.1103/physreva.69.062502

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The selection rule which forbids J=1\ensuremath↔0J=1\ensuremath{\leftrightarrow}0J=1\ensuremath↔0 two-photon decay when the energies of the two photons are equal is shown to apply only when the multipolarities of the two photons are the same (i.e., 2E12E12E1, 2M12M12M1, etc.) and does not generally apply to mixed multipolarity amplitudes such as E1M2E1M2E1M2. A calculation of the two-photon decay rate for He-like ions in the 23S12\phantom{\rule{0.2em}{0ex}}^{3}S_{1}23S1​ state including both 2E12E12E1 and E1M2E1M2E1M2 two-photon decay amplitudes is presented. It shows a significant contribution for the case of equal-energy photons. The ratio of the E1M2E1M2E1M2 contribution to the 2E12E12E1 contribution is found to be surprisingly large. For example, it is 0.27 for two-photon decay of the 23S12\phantom{\rule{0.2em}{0ex}}^{3}S_{1}23S1​state in He-like uranium.
We have applied the density matrix and second-order perturbation theory in order to re-analyze the two-photon decay of hydrogen-like ions for the polarization of emitted light. Special attention is paid to the linear polarization of one of the photons, while the spin state of the second photon is supposed to be unobserved. For such an “angle-polarization” correlation of the two photons we investigate the contributions that arise from non electric-dipole terms in the expansion of the electron-photon interaction. Detailed calculations are performed for the 2s 1/2 →1s 1/2 and 3d 5/2 →1s 1/2 transitions in neutral hydrogen as well as in hydrogen-like uranium.
The amplitude of two-photon transitions between hyperfine states in hydrogenlike ions is derived based on the relativistic Dirac equation and second-order perturbation theory. We study angular and linear polarization properties of the photon pair emitted in the decay of 2s2s2s states, where spin-flip and non-spin-flip transitions are highlighted. We pay particular attention to hydrogenlike uranium, since it is an ideal candidate for investigating relativistic and high-multipole effects, such as spin-flip transitions. Two types of emission patterns are identified: (i) non-spin-flip transitions are found to be characterized by an angular distribution of the type $W(\ensuremath{\theta})\ensuremath{\sim}1+{cos}^{2}\ensuremath{\theta}$ while the polarizations of the emitted photons are parallel; and (ii) spin-flip transitions have somewhat smaller decay rates and are found to be characterized by an angular distribution of the type $W(\ensuremath{\theta})\ensuremath{\sim}1\ensuremath{-}1/3{cos}^{2}\ensuremath{\theta}$ while the polarizations of the emitted photons are orthogonal, where $\ensuremath{\theta}$ is the angle between photons directions. Deviations due to nondipole and relativistic contributions are evaluated for both types of transitions. This work is the first step toward exploring the effect of the nucleus over the angular and polarization properties of the photon pairs emitted by two-photon transitions.
Detailed descriptions of one- and two-photon ionization are presented. We go beyond conventional perturbation theory to investigate the dynamics of both processes for a broad range of field intensities. The general theory of unstable decaying states is applied to the problem of one-photon ionization (the photoeffect). It is found that a non-trivial dependence of the transition dipole moment on the continuum state energy can lead to corrections to exponential decay, and even oscillations in the bound state population. As examples we consider the photoionization of hydrogen and atoms with autoionizing states. Only in the absence of autoionizing states corrections to exponential decay remain inconsequential for any experimentally relevant intensity. Our description of two-photon ionization is formulated in the Heisenberg picture. Besides the usual two-level atom projection operators we introduce explicitly the operators referring to the atomic continuum. By eliminating from the equations of motion the terms related to the electromagnetic self field as well as the terms referring to the continuum, transverse and longitudinal damping corresponding to spontaneous emission and photoionization is obtained. The use of field correlation functions allows us to account for the partial coherence of the applied field. We develop a technique to extract from the equations of motion a unique two-photon ionization rate. Such a characterization of the ionization process is not only instructive because of its simplicity, it is also in many cases completely satisfactory. The resulting general expression for the two-photon ionization rate is the central result of our treatment. From it we recover several familiar results in different limiting cases. In addition, our general rate expression provides the first description of the complete hierarchy of saturation effects that one should expect. We present a number of examples where we calculate the two-photon ionization rate as a function of the detuning, and where we emphasize the saturation and field correlation effects.
Two-photon decay of hydrogenlike ions is studied within the framework of second-order perturbation theory, based on the relativistic Dirac's equation. Special attention is paid to the effects arising from the summation over the negative-energy (intermediate virtual) states that occur in such a framework. In order to investigate the role of these states, detailed calculations have been carried out for the $2{s}_{1/2}\ensuremath{\rightarrow}1{s}_{1/2}$ and $2{p}_{1/2}\ensuremath{\rightarrow}1{s}_{1/2}$ transitions in neutral hydrogen H as well as for hydrogenlike xenon Xe53+{\text{Xe}}^{53+}Xe53+ and uranium U91+{\text{U}}^{91+}U91+ ions. We found that for a correct evaluation of the total and energy-differential decay rates, summation over the negative-energy part of Dirac's spectrum should be properly taken into account both for high-ZZZ and low-ZZZ atomic systems.
Two-photon transitions between atomic states of total electronic angular-momentum Ja=0{J}_{a}=0Ja​=0 and Jb=1{J}_{b}=1Jb​=1 are forbidden when the photons are of the same energy. This selection rule is analogous to the Landau-Yang theorem in particle physics that forbids decays of vector particle into two photons. It arises because it is impossible to construct a total angular-momentum ${J}_{2\ensuremath{\gamma}}=1$ quantum-mechanical state of two photons that is permutation symmetric, as required by Bose-Einstein statistics. In atoms with nonzero nuclear spin, the selection rule can be violated due to hyperfine interactions. Two distinct mechanisms responsible for the hyperfine-induced two-photon transitions are identified, and the hyperfine structure of the induced transitions is evaluated. The selection rule is also relaxed, even for zero-nuclear-spin atoms, by application of an external magnetic field. Once again, there are two similar mechanisms at play: Zeeman splitting of the intermediate-state sublevels, and off-diagonal mixing of states with different total electronic angular momentum in the final state. The present theoretical treatment is relevant to the ongoing experimental search for a possible Bose-Einstein-statistics violation using two-photon transitions in barium, where the hyperfine-induced transitions have been recently observed, and the magnetic-field-induced transitions are being considered both as a possible systematic effect, and as a way to calibrate the measurement.
The angular correlations in the two-photon decay of hydrogenlike ions are studied within the framework of second-order perturbation theory, based on Dirac's equation. Particular attention has been paid to the effects which arise from the higher (nondipole) terms in the expansion of the electron-photon interaction. It is shown that the photon-photon angular correlation function, which is found symmetric with respect to the angle $\ensuremath{\theta}=90\ifmmode^\circ\else\textdegree\fi{}$ in the electric dipole approximation, becomes asymmetric because of the nondipole contributions, and that this effect is enhanced as the nuclear charge ZZZ increases. Detailed computations on the photon-photon angular distribution have been carried out for the $2{s}_{1∕2}\ensuremath{\rightarrow}1{s}_{1∕2}$ and $3{d}_{5∕2}\ensuremath{\rightarrow}1{s}_{1∕2}$ transitions in neutral hydrogen (H) as well as for hydrogenlike xenon (Xe53+)({\mathrm{Xe}}^{53+})(Xe53+) and uranium (U91+)({\mathrm{U}}^{91+})(U91+) ions, and are compared with previous nonrelativistic results by Au [Phys. Rev. A 14, 531 (1976)]).