Two photon emission of metastable atomic hydrogen is analysed in comparison to two photon cascade emission from a three level atom. The joint count probabilities are found to be in agreement with experimental results[10].
The Paper first summarizes fundamental aspects and results of the quantum electrodynamical theory of the two-photon radiationfromthe decay of the metastable 2 2 S 1/2 atomic hydrogen state. After a brief description of the second improved Stirling two-photon coincidence experiment polarization correlations of the two-photon decay are described in which both two or three linear polarizers are applied in order to test predictions of such correlations based upon quantum mechanics and local realistic theories (i.e., Einstein-Podolsky-Rosen type experiments). It is particularly noticeable that the three-polarizer coincidence measurement provided the largest difference (about 40%) between the Bell limits of local realistic theories and quantum mechanics so far. Apart from confirming in addition the correlations of right-right and left-left circularly polarized two-photon correlations a new type of coherence analysis of the two-photon radiation has been carried out experimentally and theoretically. A result of it is the measured coherence time of τ coh = 1.2 · 10 −15 s and coherence length of l coh = c · τ coh = 350 nm of the two-photon emission. By applying a theoretical model of the two-photon radiation linked to cascade transitions the coherence length can be estimated to l coh ≈ 100 nm in agreement by order of magnitude with the experimental data.
A novel Fourier-transform spectroscopic method using two-photon polarization to determine the spectral distribution of the two photons emitted in the spontaneous decay of metastable atomic hydrogen is described. The method uses birefringent retardation plates and takes advantage of the subtle interplay between the spectral properties and the entangled polarization properties of the radiation emitted in the decay. Assuming the validity of the theoretical spectral distribution, it is shown that the experimental results agree well with theory. On the other hand, success in solving the inverse problem of determining the spectral distribution from the experimental results is limited by the small number of experimental points. However, making reasonable assumptions it is deduced that the observed spectrum is characterized by a broadband signal of width and centre angular frequency in good agreement with the predictions of and , respectively, obtained from the theoretical spectral distribution modified to take account of the absorption of the two-photon radiation in air. The values of 1.5 fs for the coherence time and 440 nm for the coherence length for single photons of the two-photon pair which are obtained from the measured bandwidth imply that, in the ideal case, these values are determined by the essentially zero lifetime of the virtual intermediate state of the decay process rather than the long lifetime of the metastable state which, it is suggested, determines the coherence time and coherence length appropriate to certain types of fourth-order interference experiments.
The problem of the evaluation of the two-photon decay width of excited states in hydrogen is considered. Two different approaches to the evaluation of the width including cascades channels are employed: the summation of the transition probabilities for various decay channels and the evaluation of the imaginary part of the Lamb shift. As application, the two-photon decay channels for the 3s level of the hydrogen atom are evaluated, including the cascade transition probability $3s\text{\ensuremath{-}}2p\text{\ensuremath{-}}1s$. An important role is assigned to the two-photon decays in astrophysics context, since processes of this kind provide a possibility for the decoupling of radiation and matter in the early universe. We demonstrate the ambiguity of separation of the ``pure'' two-photon contribution and criticize the existing methods for such a separation.
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.
The two-photon decay mode of hydrogenic atoms from an arbitrary state (n1, l1, m1) to an arbitrary state (n2, l2, 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 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.