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arXiv:0810.0073 · Physical Review A

Virtual resonant states in two-photon decay processes: Lower-order terms, subtractions, and physical interpretations

Ulrich D. Jentschura

Published Feb 19, 2009• 25 citations
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Abstract

We investigate the two-photon decay rate of a highly excited atomic state which can decay to bound states of lower energy via cascade processes. We show that a na\"{\i}ve treatment of the process, based on the introduction of phenomenological decay rates for the intermediate, resonant states, leads to lower-order terms which need to be subtracted in order to obtain the coherent two-photon correction to the decay rate. The sum of the lower-order terms is exactly equal to the one-photon decay rate of the initial state, provided the na\"{\i}ve two-photon decay rates are summed over all available two-photon channels. A quantum electrodynamics treatment of the problem leads to an ``automatic'' subtraction of the lower-order terms.

DOI
10.1103/physreva.79.022510

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We investigate the two-photon decay rate of a highly excited atomic state which can decay to bound states of lower energy via cascade processes. We show that a na"{\i}ve treatment of the process, based on the introduction of phenomenological decay rates for the intermediate, resonant states, leads to lower-order terms which need to be subtracted in order to obtain the coherent two-photon correction to the decay rate. The sum of the lower-order terms is exactly equal to the one-photon decay rate of the initial state, provided the na"{\i}ve two-photon decay rates are summed over all available two-photon channels. A quantum electrodynamics treatment of the problem leads to an ``automatic'' subtraction of the lower-order terms.
We consider the general scenario of an excited level $|i\ensuremath{\rangle}$ of a quantum system that can decay via two channels: (i) via a single-quantum jump to an intermediate, resonant level $|\overline{m}\ensuremath{\rangle}$, followed by a second single-quantum jump to a final level $|f\ensuremath{\rangle}$, and (ii) via a two-quantum transition to a final level $|f\ensuremath{\rangle}$. Cascade processes $|i\ensuremath{\rangle}\ensuremath{\rightarrow}|\overline{m}\ensuremath{\rangle}\ensuremath{\rightarrow}|f\ensuremath{\rangle}$ and two-quantum transitions $|i\ensuremath{\rangle}\ensuremath{\rightarrow}|m\ensuremath{\rangle}\ensuremath{\rightarrow}|f\ensuremath{\rangle}$ compete (in the latter case, $|m\ensuremath{\rangle}$ can be both a nonresonant as well as a resonant level). General expressions are derived within second-order time-dependent perturbation theory, and the cascade contribution is identified. When the one-quantum decay rates of the virtual states are included into the complex resonance energies that enter the propagator denominator, it is found that the second-order decay rate contains the one-quantum decay rate of the initial state as a lower-order term. For atomic transitions, this implies that the differential-in-energy two-photon transition rate with complex resonance energies in the propagator denominators can be used to good accuracy even in the vicinity of resonance poles.
Two-photon decay rates in simple atoms such as hydrogenlike systems represent rather interesting fundamental problems in atomic physics. The sum of the energies of the two emitted photons has to fulfill an energy conservation condition, the decay takes place via intermediate virtual states, and the total decay rate is obtained after an integration over the energy of one of the emitted photons. Here, we investigate cases with a virtual state having an energy intermediate between the initial and the final state of the decay process, and we show that due to non-uniform convergence, only a careful treatment of the singularities infinitesimally displaced from the photon integration contour leads to consistent and convergent results.
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.
It is well known that energy-time entanglement can enhance two-photon absorption (TPA) by simultaneously optimizing the two-photon resonance and the coincidence rate of photons at the absorber. However, the precise relation between entanglement and the TPA rate depends on the coherences of intermediate states involved in the transition, making it a rather challenging task to identify universal features of TPA processes. In the present paper, we show that the theory can be simplified greatly by separating the two-photon resonance from the temporal dynamics of the intermediate levels. The result is a description of the role of entanglement in the TPA process by a one-dimensional coherence in the Hilbert space defined by the arrival-time difference of the two photons. Transformation into the frequency-difference basis results in Kramers-Kronig relations for the TPA process, separating off-resonant contributions of virtual levels from resonant contributions. In particular, it can be shown that off-resonant contributions are insensitive to the frequencies of the associated virtual states, indicating that virtual-state spectroscopy of levels above the final two-photon excited state is not possible.
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.
We consider two separate atoms interacting with a single-mode optical resonator. When the frequency of the resonator field is twice the atomic transition frequency, we show that there exists a resonant coupling between one photon and two atoms, via intermediate virtual states connected by counter-rotating processes. If the resonator is prepared in its one-photon state, the photon can be jointly absorbed by the two atoms in their ground state which will both reach their excited state with probability close to one. Like ordinary quantum Rabi oscillations, this process is coherent and reversible, so that two atoms in their excited state will undergo a downward transition jointly emitting a single cavity photon. This joint absorption and emission processes can also occur with three atoms. The parameters used to investigate this process correspond to experimentally demonstrated values in circuit quantum electrodynamics systems.