Stimulated electronic Raman scattering, SERS, is a simple method of efficiently generating widely tunable infrared radiation. This work describes techniques by which the tuning capability of this process may be extended. To this end several schemes in Caesium and Barium vapours have been investigated. In Barium vapour two Raman transitions were studied using fixed frequency lasers. Poor performance of one of these transitions led to the application of biharmonic pumping or 'coherent Raman mixing' to enable generation of infrared light, and was the first observation of this process in an atomic vapour. This technique was subsequently used to generate infrared light from tunable dye laser light, which gave continuous tuning from 1.16µm to 1.5µm. The process was found to be limited by atomic saturation. The effect which saturation has on the generation efficiency is considered theoretically, and predicts quite accurately the observed tuning behaviour. Two methods aimed at reducing molecular absorption effects in SERS in alkali vapours were investigated. The techniques employed either laser excitation and dissociation of the molecules or a reduction in their ground state concentration by superheating of the vapour. Some degree of success was achieved in improving the available tuning from the 6s-7s transition in Caesium. However, the inclusion of the effect of collision broadening of atomic transitions into a calculation of the Raman threshold suggests that little further improvement can be obtained on this transition. A direct measurement of the Raman threshold power on the 6s-5d5/2 transition in Caesium gave excellent agreement with theoretical predictions based on collision broadening of this Raman transition. In addition, this work gave an insight into the role photoionization plays in increasing the threshold under certain circumstances. The analysis suggests that laser pulse duration and vapour column length are important in determining whether Raman threshold can be exceeded.
We present in this paper results of a nonlinear optical spectroscopy approach to measurement of excited-state transition matrix elements. Recent advances in the quality of excited-state transition matrix elements have permitted renormalization of earlier measurements of transition amplitudes associated with the 5s 2 S 1/2 → 5p 2 P j → 5d 2 D 3/2 two-photon transitions in atomic 87 Rb. Previous measurements were made to high precision, but further improvement of the accuracy was limited by uncertainties in data describing the influence of energetically distant transitions. Availability of more reliable matrix elements, including relativistic all-order calculations of transition matrix elements in alkali atoms, has since significantly improved the situation. In the present paper, we show that theoretical relative transition amplitudes for the excited state 5p 2 P j → 5d 2 D 3/2 doublet (ratio = 1.098(9)) are now in excellent agreement with experiment (ratio = 1.090(6)). This result, combined with our recent work on caesium, shows that it is possible to determine relative line strengths, for transitions connecting atomic excited states, with precision previously found only in state-of-the-art measurements of alkali resonance doublets. Detailed discussion of the experimental technique and supporting data, including polarization measurements on the 5s 2 S 1/2 → 5p 2 P j → 5d 2 D 5/2 transitions, is also presented.
The main properties of infrared stimulated electronic Raman scattering (SERS) at the 6 2 S 1/2 -7 2 S 1/2, 3/2 transitions in cesium atoms are studied theoretically and experimentally as functions of the atomic concentration, which was varied from 10 11 to 10 16 cm −3 . It is found that the efficiency of generation of Stokes radiation strongly depends on one-photon absorption of the pump radiation tuned near frequencies of the 6 2 S 1/2 -7 2 P 1/2, 3/2 transitions. By using the equation for the density matrix, which describes the evolution of a three-level system, the theory of resonance excitation of IR radiation upon one-photon absorption at an adjacent transition is developed. The theory describes well the main features of IR SERS in alkali-metal vapors.
We report here the first observation and measurement of the transition magnetic moment for a strongly forbidden S-S transition of an alkali atom. By using single-photon excitation of the 6S1/2-7S1/2 caesium transition in a quasi-static electric field, we have detected an electronic polarization of the excited state, specific to an interference effect occurring in mixed electric magnetic dipole transitions. Our measurements, independent of the vapour density, indicate that the magnetic dipole amplitude M 1 has the same size as the electric dipole amplitude E1 , induced by an electric field, parallel to the light wave polarization, and equal to 2.62 ± 0.21 V/cm. We also obtain the relative sign of M 1 and E1. Using a theoretical value of E 1 and a well-defined phase convention, we deduce for the magnetic moment of the transition < 7S, 1/ 2 | μ z | 6S, 1/ 2 > = - (4.24 ± 0.34) 10-5 |μB|, in good agreement with a theoretical estimate. This result can also be expressed in terms of the oscillator strength in zero electric field f6S-7S = 4.05 × 10-15, or of the single-photon M1 decay rate Γ 7S-6S = 0.93 x 10-6 s-1.
Magic wavelengths (${\ensuremath{\lambda}}_{\mathrm{magic}}$) for the $7{S}_{1/2}\ensuremath{-}7{P}_{1/2,3/2}$ transitions (D lines) in Fr were reported by Dammalapati et al. [U. Dammalapati, K. Harada, and Y. Sakemi, Phys. Rev. A 93, 043407 (2016)]. These ${\ensuremath{\lambda}}_{\mathrm{magic}}$ were determined by plotting dynamic polarizabilities ($\ensuremath{\alpha}$) of the involved states with the above transitions against a desired range of wavelengths. Electric dipole (E1) matrix elements listed in [J. E. Sansonetti, J. Phys. Chem. Ref. Data 36, 497 (2007)], from the measured lifetimes of the
7P1/2,3/2 states and from the calculations considering core-polarization effects in the relativistic Hartree-Fock (HFR) method, were used to determine $\ensuremath{\alpha}$. However, contributions from core correlation effects and from the E1 matrix elements of the $7P\ensuremath{-}7S, 7P\ensuremath{-}8S$, and $7P\ensuremath{-}6D$ transitions to $\ensuremath{\alpha}$ of the
7P states were ignored. In this work, we demonstrate importance of these contributions and improve accuracies of $\ensuremath{\alpha}$ further by replacing the E1 matrix elements taken from the HFR method by the values obtained employing relativistic coupled-cluster theory. Our static $\ensuremath{\alpha}$ are found to be in excellent agreement with the other available theoretical results, whereas substituting the E1 matrix elements used by Dammalapati et al. gives very small $\ensuremath{\alpha}$ values for the
7P states. Owing to this, we find disagreement in ${\ensuremath{\lambda}}_{\mathrm{magic}}$ reported by Dammalapati et al. for linearly polarized light, especially at wavelengths close to the D lines and in the infrared region. As a consequence, a ${\ensuremath{\lambda}}_{\mathrm{magic}}$ reported at 797.75 nm which was seen supporting a blue detuned trap in their work is now estimated at 771.03 nm and is supporting a red detuned trap. Also, none of our results match with the earlier results for circularly polarized light. Moreover, our static values of $\ensuremath{\alpha}$ will be very useful for guiding experiments to carry out their measurements.