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Journal of Physics B Atomic and Molecular Physics

AC Stark effect and fluorescence using modulated laser beams. I. Effect of laser fluctuations and arbitrary relaxation parameters

Ragini Saxena, G. S. Agarwal

Published Jun 28, 1979• 16 citations
Publisher

Abstract

The influence of relaxation parameters, as well as temporal fluctuations in the laser field on the modulation rate and phaseshift of the fluorescence from a two-level atom excited by a weakly modulated source is studied in detail. It is shown that, for intense resonant laser fields, the resonance in the modulation rate occurs at the modulation frequency Omega =2 due to the dynamical Stark splitting and has a width equal to 1 / 2 (T 1 -1 +T 2 -1 ). When temporal fluctuations of the exciting laser field are taken into account, the phaseshift of the scattered light is found to be strongly dependent on the bandwidth of the exciting source, as well as the frequency of modulation; hence experimental results on the determination of the lifetime by the phaseshift method have to be interpreted carefully. Numerical results for the modulation rates and phaseshift at different field strengths and various values of T 1 -1 , T 2 -1 , Delta laser bandwidth and Doppler broadening are presented.

DOI
10.1088/0022-3700/12/12/013

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Acta Optica Sinica•Jan 1, 1988•0 citations
The influence of relaxation parameters, as well as temporal fluctuations in the laser field on the modulation rate and phaseshift of the fluorescence from a two-level atom excited by a weakly modulated source is studied in detail. It is shown that, for intense resonant laser fields, the resonance in the modulation rate occurs at the modulation frequency Omega =2 due to the dynamical Stark splitting and has a width equal to 1 / 2 (T 1 -1 +T 2 -1 ). When temporal fluctuations of the exciting laser field are taken into account, the phaseshift of the scattered light is found to be strongly dependent on the bandwidth of the exciting source, as well as the frequency of modulation; hence experimental results on the determination of the lifetime by the phaseshift method have to be interpreted carefully. Numerical results for the modulation rates and phaseshift at different field strengths and various values of T 1 -1 , T 2 -1 , Delta laser bandwidth and Doppler broadening are presented.
For pt.I see ibid., vol.12, no.12, p.1939 (1979). The modulated fluorescence in an optical double resonance experiment, i.e. when an atom interacts with two intense monochromatic laser beams each of which is weakly modulated in amplitude at frequency Omega , is studied in detail. The modulation rate corresponding to the steady-state population of the highest atomic level exhibits resonant structures at the modulation frequencies Omega =0, +or- alpha 0 , +or-2 alpha 0 due to the dynamical Stark splitting of the various energy levels; alpha 0 being related to the Rabi frequencies alpha 1 and alpha 2 associated with the two lasers and the two atomic transitions, by alpha 0 2 = mod alpha 1 mod 2 + mod alpha 2 mod 2 . The peak at Omega =+or- alpha 0 is the most intense and exhibits splitting when the applied fields are detuned from exact resonance with the respective atomic frequencies. Resonances are observed in the modulation rate of the intermediate-level population at the modulation frequencies Omega =0, +or-2 alpha 0 . In the presence of detunings of the applied fields, additional resonant structures occur at Omega =+or- alpha 0 which increase in magnitude with higher detunings and split. Explicit expressions for the positions, widths and weights of these resonant components are obtained analytically for intense, resonant fields. Numerical results for general values of the laser field strengths and the detunings are given.
The fluorescence emitted by atoms whose excited states have Zeeman structure is studied for the case of excitation by partially coherent optical sources whose amplitudes are weakly modulated at a low frequency $\ensuremath{\Omega}$. The temporal fluctuations in lasers are taken into account exactly by using the phase-diffusion model of the laser. Analytical results for the modulated fluorescence are presented for the case of weak fields. It is shown that the shape of the fluorescent signal is extremely sensitive to the bandwidth of the field; for example, one gets resonances at a Larmor frequency equal to $\mathcal{s}=\frac{\ifmmode\pm\else\textpm\fi{}\ensuremath{\Omega}}{2}(0,\ifmmode\pm\else\textpm\fi{}\ensuremath{\Omega})$ for broadband (monochromatic) fields. Various limiting cases are treated, and in the limit of very broadband fields, results reduce to those of Corney and Series. The fluorescence is studied both as a function of the modulation frequency and as a function of the magnetic field. Numerical studies of the modulated Hanle signals in intense fields reveal resonant structures in the modulation-frequency scan at $\ensuremath{\Omega}=0,\ifmmode\pm\else\textpm\fi{}{\ensuremath{\alpha}}_{0}$, $\ifmmode\pm\else\textpm\fi{}2{\ensuremath{\alpha}}_{0}({\ensuremath{\alpha}}_{0}^{2}={\mathcal{s}}^{2}+2{\ensuremath{\alpha}}^{2})$ due to the dynamical Stark splitting of the various energy levels, with the strength of the resonances depending on the direction of detection.
Attention is focused on the dynamic evolution of the emission spectrum following abrupt excitation of a near-resonant two-level absorber by a strong laser field. The multiphoton character of the absorption-emission process is evident in the AC Stark splitting of the spectrum, which begins approximately half an atomic lifetime after excitation, if the laser field is strong enough. Analytic expressions for the spectra are given of arbitrary laser field strength, atomic lifetime, laser-atom detuning, and the bandwidth of the spectrometer used to analyse the spectrum. Selected graphs are included to illustrate various time-dependent features of the spectrum. The influence on the transient spectrum of three different states of atomic excitation prior to laser irradiation and the effect on the spectrum of irradiation by a phase-noisy laser are also considered. Comparison of the transient spectra from atoms initially prepared in ' pi /2' and '3 pi /2' states show clearly that phase relationships between the irradiating field and the emitting dipole are important even in fluorescence.
An experiment was performed recently [Y. Zhu, A. Lezama, Q. Wu, and T. W. Mossberg (unpublished)] in which a two-level atom of transition frequency \ensuremath{\Omega} was placed in a bichromatic laser field with frequencies \ensuremath{\Omega}\ifmmode\pm\else\textpm\fi{}\ensuremath{\delta}, of sufficient intensity to produce dynamic Stark splitting. The observed fluorescence spectrum differed qualitatively in almost all its details from the well-known Mollow triplet [B. R. Mollow, Phys. Rev. 188, 1969 (1969)]. In this article, we use a dressed-atom model to explain the observed results.
A quantum statistical theory of resonant optical phenomena is developed for the case when the fluctuations of the laser, used for exciting transitions, are important. The general equations describing the dynamics of a relaxing two-level atom (TLA) are solved exactly for different types of mean values and the two-time amplitude and intensity correlations. The phase-diffusion model is adopted for laser fluctuations. The exact results are used to analyze the effect of laser fluctuations on a number of optical effects-optical free-induction decay, adiabatic following, the spectrum of the scattered light from a relaxing TLA, the energy-absorption spectrum from a weak field, Hanle resonances, etc. In each case, the laser fluctuations are found to affect in an important way the characteristics of the above optical-resonance phenomena. For example, the spectrum of scattered radiation from a TLA has the usual three-peak structure for fields at resonance and with strengths $\ensuremath{\alpha}$ above the threshold and for $\ensuremath{\alpha}\ensuremath{\gg}{\ensuremath{\gamma}}_{c}$; however, now the peak heights (widths) are in the ratio 3x3x3x (23x\frac{2}{3x}3x2​), $x=\frac{[{\ensuremath{\gamma}}_{c}+\frac{({T}_{1}^{\ensuremath{-}1}+{T}_{2}^{\ensuremath{-}1})}{3}]}{[2{\ensuremath{\gamma}}_{c}+{T}_{2}^{\ensuremath{-}1}]}$, where ${\ensuremath{\gamma}}_{c}^{\ensuremath{-}1}$ is the correlation time for laser phase fluctuations. For ${\ensuremath{\gamma}}_{c}\ensuremath{\gg}\ensuremath{\alpha}$, one gets a single-peak spectrum. The laser field is treated as a second-quantized field with excitation in either a coherent state or a Fock state. The results, obtained by straightforward perturbation theory, but valid for arbitrary values of the relaxation parameters, detuning, and the laser correlation time, are also presented.
The lifetime of atoms and molecules can be measured by using modulated resonant single-mode laser field. A theoretical mode for this method is presented. It is shown that the laser induced fluorescence, a resonance flourescence is modulated at the same frequency, but phase shift from the exciting laser. The phase shift is mainly due to three processes (1) coherent excitation process characterized by transverse relaxation rate and line width of the laser, (2) population damping process characterized by the decay time of excited levels and other populated levels, (3) collision process characterized by the relaxation time by which the system to be in equilibrium state. The effect of these processes on measurement result is discussed. The Doppler broading is considered also.