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Atoms-Photonic Field Interaction: Influence Functional and Perturbation Theory

Emmanouil George Thrapsaniotis

Published Jun 14, 2017• 4 citations
Publisher

Abstract

We study the dynamics of one-electron atoms interacting with a pulsed, elliptically polarized, ultrashort, and coherent state.We use path integral methods.We path integrate the photonic part and extract the corresponding influence functional describing the interaction of the pulse with the atomic electron.Then we angularly decompose it.We keep the first-order angular terms in all but the last factor as otherwise their angular integration would contribute infinites as the number of time slices tends to infinity.Further we use the perturbative expansion of the last factor in powers of the inverse volume and integrate on time.Finally, we obtain a closed angularly decomposed expression of the whole path integral.As an application we develop a scattering theory and study the two-photon ionization of hydrogen.

DOI
10.5772/67774

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We study the dynamics of one-electron atoms interacting with a pulsed, elliptically polarized, ultrashort, and coherent state.We use path integral methods.We path integrate the photonic part and extract the corresponding influence functional describing the interaction of the pulse with the atomic electron.Then we angularly decompose it.We keep the first-order angular terms in all but the last factor as otherwise their angular integration would contribute infinites as the number of time slices tends to infinity.Further we use the perturbative expansion of the last factor in powers of the inverse volume and integrate on time.Finally, we obtain a closed angularly decomposed expression of the whole path integral.As an application we develop a scattering theory and study the two-photon ionization of hydrogen.
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.
The infinite summations over the complete set of unperturbed atomic states appearing in the Nth-order time-dependent perturbation theory are performed using the Green's function formalism. In order to test the method extended calculations of the cross section for two- and three-photon ionization for atomic hydrogen are made and numerical comparison is shown with the values obtained by different methods. The resonant character of the process is made evident since the poles of the radial part of the Green's function represent the actual energy spectrum of the atom. The relevant transition matrix elements are written in closed form and then computed exactly without averaging over the intermediate states. The cross sections vanish for circularly polarized light near some energies which explains the form of the cross sections for circularly and linearly polarized light.
We present a quantum dynamical study of pulsed few-photon scattering from a single artificial atom, consisting of a two-level system (TLS) or qubit, in a waveguide QED system, directly comparing and contrasting two different quantum theoretical simulation methods: (i) an input-output scattering approach that uses frequency-dependent scattering matrices, and (ii) a matrix product states (MPS) approach, which uses quantum noise operators in time bins and a tensor network technique to solve the time-dependent waveguide function for the entire system. Beginning with pulsed excitation using one-photon and two-photon Fock state pulses, we first show how to compute time-dependent observables with the scattering matrix approach, in terms of frequency integrals that encode the pulse spectrum, including how to extract the population dynamics of the excited quantum emitter, as well as the linear and nonlinear contributions. We present solutions for both symmetric and chiral TLS coupling. We then show how to compute the qubit and field observables in a more direct way using MPS, and obtain the characteristic bird-like shape for the two-photon correlation function at two times, which has been observed in recent experiments. We compare and contrast both of these methods, for one and two-photon excitation pulses, and show excellent agreement. We also present a study of the linear and nonlinear contributions, which can easily be calculated using scattering theory, and show the important role of pulse duration. Finally, we demonstrate the clear advantages of MPS by easily going to higher N-photon excitations, and show selected example population dynamics of up to eight-photon Fock-state pulses, manifesting in clear nonlinear population oscillations during the pulse interaction, similar to classical Rabi oscillations, but with quantum input fields that have a vanishing electric field expectation value.
Until recently, the nonlinear interaction between light and matter has been restricted to only low photon energies produced by optical lasers. However, about a decade ago, the rise of free-electron laser facilities revolutionized the field of nonlinear light-matter interaction by delivering intense high-energy light pulses. Today, such lasers are used for research in materials science, chemical technology, biophysical science, solid state physics as well as fundamental research. It is the new experimental possibilities provided by free-electron lasers that motivated the work presented in this thesis. Two-photon ionization process is one of the simplest nonlinear interactions in which absorption of two photons by an atom (or a molecule) leads to promoting one of its bound electrons to continuum. This work presents studies of two-photon ionization of neutral atoms. After a brief historical introduction to the topic of nonlinear light-matter interaction, the density matrix describing the state of an atom and a photoelectron following two-photon ionization is derived. In each successive chapter, part of this density matrix is used to obtain characteristic quantities such as total two-photon ionization cross section, photoelectron angular distributions, ion polarization or degree of polarization of fluorescence photon produced by subsequent decay of the photoion. Physical properties of these quantities are studied and intriguing phenomena, such as elliptical dichroism, polarization transfer as well as relativistic and screening effects are investigated.