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arXiv:2006.02477 · Physical Review A

Perturbative theory of statistically averaged atomic dynamics in fluctuating laser fields

Tejaswi Katravulapally, Lampros A. A. Nikolopoulos

Published Nov 16, 2020• 3 citations
arXivHTMLPDF

Abstract

We have developed a perturbative method to model the resonant ionization of atomic systems in fluctuating laser fields. The perturbative method is based on an expansion in terms of the multitime cumulants, a suitable combination of moments (field's coherence functions), used to represent the field's statistical properties. The second-order truncated expansion is expressed in terms of the radiation's power spectrum and the intensity autocorrelation function. We investigate the range of validity of the model in terms of the field's coherence temporal length and peak intensity and have compared the results with conventional Monte Carlo calculations. We apply the theory in the case of a near-resonant ionization of the helium $2s2p$ autoionizing state with a self-amplified spontaneous emission free-electron laser pulse with square-exponentially dependent first-order coherence function. The ionization lineshape profile acquires a Voight profile; the degree of the Gaussian or Lorentzian character of the lineshape will depend crucially on the field's coherence time.

DOI
10.1103/physreva.102.053111

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We have developed a perturbative method to model the resonant ionization of atomic systems in fluctuating laser fields. The perturbative method is based on an expansion in terms of the multitime cumulants, a suitable combination of moments (field's coherence functions), used to represent the field's statistical properties. The second-order truncated expansion is expressed in terms of the radiation's power spectrum and the intensity autocorrelation function. We investigate the range of validity of the model in terms of the field's coherence temporal length and peak intensity and have compared the results with conventional Monte Carlo calculations. We apply the theory in the case of a near-resonant ionization of the helium 2s2p2s2p2s2p autoionizing state with a self-amplified spontaneous emission free-electron laser pulse with square-exponentially dependent first-order coherence function. The ionization lineshape profile acquires a Voight profile; the degree of the Gaussian or Lorentzian character of the lineshape will depend crucially on the field's coherence time.
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.
A method of calculation of multiple-time correlation functions of the resonance fluorescence light from a two-level atom driven by a realistic laser field with phase and amplitude fluctuations is developed. Both kinds of fluctuations are assumed to be Gaussian. The phase fluctuations are treated in the phase-diffusion model. The averaging over the amplitude fluctuations can be performed in a closed way when the relative mean-square amplitude fluctuation is small compared with the ratio of the amplitude correlation decay rate to the characteristic atomic relaxation rate. There is no restriction to Markovian amplitude fluctuations. Arbitrary values for the mean Rabi frequency are allowed. Results are presented for the intensity, the intensity correlation function, and the spectrum of the fluorescent light. It is shown that even in the case when the relative strength of the amplitude fluctuations is small, significant effects can occur due to the finite correlation length of the fluctuations. The results for fast amplitude correlation decay correspond to the situation without amplitude fluctuations. When the correlation time of the amplitude fluctuations becomes comparable with the atomic relaxation times, the Rabi oscillations of the intensity and the intensity correlation function are nearly washed out, and non-Lorentzian line shapes for the side peaks in the spectrum are observed. It is found that the ratio of the heights of the central peak to the side peak increases with increasing correlation time.
When an atom is driven by a laser field with a photon energy that is nearly resonant with an atomic transition, it can undergo periodic population transfers between the ground and excited state, known as Rabi oscillations [1], [2]. The aim of this work is to study photoionization from atoms for parameters accessible to a free-electron laser (FEL) [3]. Using time dependent perturbation theory to model photoionization from a Rabi oscillating atom, we have shown that in addition to the expected pathway of ionization from the excited state, non-resonant two-photon ionization will have a comparable amplitude at intensities on the order of 1013W/cm2[3].
We analyze theoretically the high intensity photoionization dynamics of a system with two atomic states resonantly coupled by coherent extreme ultraviolet laser radiation that also gives rise to the ionization. The ground state occupation of such a system is shown to exhibit damped Rabi oscillations. The corresponding ionization, which is responsible for the damping, scales almost linearly with the field intensity when the pulse length exceeds the Rabi period. For shorter pulses a quadratic scaling is found. The Rabi frequency is shifted compared to its value for an isolated two-level system. The shift increases with excitation intensity and can acquire a high percentage of the unrenormalized frequency at high intensities. Analytical results obtained within a simplified solvable model demonstrate that the damping and the shift both result from the coupling of the discrete states to the ionization continuum and are therefore closely related. Numerical simulations for a two-electron system reveal at high intensities the importance of off-resonant ionization channels.
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.
We formulate a computationally feasible method for calculating multiphoton ionization rates for atoms exposed to intense fields in the intensity regime where perturbation theory ceases to apply. The method is based on the time-independent picture of ionization, which starts with the Floquet ansatz. The question of the gauge of the radiation field is discussed in some detail. Various expressions for the ionization amplitude are derived from a variational principle, with the radiation field expressed in the velocity gauge. We consider in particular an approximation in which the wave vector developing from the initial state is replaced by a trial vector that is the Floquet expansion truncated just below the threshold for ionization, and in which the wave vector developing into the final state is replaced by a trial vector that is just the wave vector appearing in the Kroll-Watson low-frequency approximation in scattering theory. We have applied this approximation to hydrogen and we present some results for both nonresonant and resonant multiphoton ionization. We argue that the experimentally observed resonance structure in the above-threshold peaks of the ionization signal occurs through the electron jumping from one dressed-state energy-eigenvalue curve to another.