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Physical Review A

Two-photon transitions in atomic hydrogen: An alternative approach

R. B. Thayyullathil, K. J. Prasanna

Published Apr 1, 1994• 7 citations
Publisher

Abstract

We present an efficient analytic approach for the evaluation of two-photon transition rates in a hydrogen atom. The method is a variation of the Dalgarno and Lewis method [Proc. R. Soc. London Ser. A 233, 70 (1955)] for the evaluation of the second-order Stark effect in a hydrogen atom.
DOI
10.1103/physreva.49.2432

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In the present thesis we have formulated the Dalgarno-Lewis procedure\nfor two-and three-photon processes and an elegant alternate expressions\nare derived. Starting from a brief review on various multiphoton processes\nwe have discussed the difficulties coming in the perturbative treatment\nof multiphoton processes. A small discussion on various available methods\nfor studying multiphoton processes are presented in chapter 2. These\ntheoretical treatments mainly concentrate on the evaluation of the higher\norder matrix elements coming in the perturbation theory. In chapter 3 we\nhave described the use of Dalgarno-Lewis procedure and its implimentation on second order matrix elements. The analytical expressions for twophoton\ntransition amplitude, two-photon ionization cross section, dipole\ndynamic polarizability and Kramers-Heiseberg are obtained in a unified\nmanner. Fourth chapter is an extension of the implicit summation technique\npresented in chapter 3. We have clearly mentioned the advantage of\nour method, especially the analytical continuation of the relevant expressions\nsuited for various values of radiation frequency which is also used for\nefficient numerical analysis.\nA possible extension of the work is to study various multiphoton processcs\nfrom the stark shifted first excited states of hydrogen atom. We\ncan also extend this procedure for studying multiphoton processes in alkali\natoms as well as Rydberg atoms. Also, instead of going for analytical expressions,\none can try a complete numerical evaluation of the higher order\nmatrix elements using this procedure.

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Journal of Physics B Atomic Molecular and Optical Physics•Jan 25, 2005•6 citations
In this paper, we present an efficient alternative method for the evaluation of the three-photon transition matrix element in the dipole approximation from the ground state to bound states in atomic hydrogen. This method is a variation of the Dalgarno–Lewis method for the treatment of the second-order Stark effect in the hydrogen atom. In this approach, the infinite double sum over the complete set of states including the continuum states present in the third-order perturbation theory result is treated exactly. The closed analytical expression obtained for the matrix element, as a function of incident photon energy, clearly displays all singularities present in the original third-order perturbation theory result.
In the present thesis we have formulated the Dalgarno-Lewis procedure\nfor two-and three-photon processes and an elegant alternate expressions\nare derived. Starting from a brief review on various multiphoton processes\nwe have discussed the difficulties coming in the perturbative treatment\nof multiphoton processes. A small discussion on various available methods\nfor studying multiphoton processes are presented in chapter 2. These\ntheoretical treatments mainly concentrate on the evaluation of the higher\norder matrix elements coming in the perturbation theory. In chapter 3 we\nhave described the use of Dalgarno-Lewis procedure and its implimentation on second order matrix elements. The analytical expressions for twophoton\ntransition amplitude, two-photon ionization cross section, dipole\ndynamic polarizability and Kramers-Heiseberg are obtained in a unified\nmanner. Fourth chapter is an extension of the implicit summation technique\npresented in chapter 3. We have clearly mentioned the advantage of\nour method, especially the analytical continuation of the relevant expressions\nsuited for various values of radiation frequency which is also used for\nefficient numerical analysis.\nA possible extension of the work is to study various multiphoton processcs\nfrom the stark shifted first excited states of hydrogen atom. We\ncan also extend this procedure for studying multiphoton processes in alkali\natoms as well as Rydberg atoms. Also, instead of going for analytical expressions,\none can try a complete numerical evaluation of the higher order\nmatrix elements using this procedure.
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.
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 infinite summations over the complete set of unperturbed atomic states appearing in the NNNth-order perturbation theory for multiphoton ionization are performed using the Dalgarno-Lewis method. The relevant transition matrix elements are written in a closed integral form exhibiting all the analytic properties of the amplitude as a function of incident photon energy. The cross sections for two- and three-photon ionization for atomic hydrogen are calculated for both linearly and circularly polarized light with a wide range of photon energy spectrum including the near resonance, and numerical comparison is made with the values obtained by different methods.