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arXiv:2406.16559 · Proceedings of the Royal Society A Mathematical Physical and Engineering Sciences

Non-Hermitian Floquet dynamics in absorption spectroscopy

R. M. Potvliege

Published Apr 1, 2025• 0 citations
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Abstract

A theory of the absorption of a laser field by an atomic or condensed matter medium is presented for the case where the medium is also interacting with a strong electromagnetic field. The rotating wave approximation is not assumed for the latter. It is shown that in the weak probe limit the Lindblad master equation reduces to a smaller system of linear equations for the relevant steady-state coherences. In this limit, the complex susceptibility of the medium can be expressed in terms of individual contributions of decaying dressed states, the latter being eigenstates of a non-Hermitian Floquet Hamiltonian.

DOI
10.1098/rspa.2024.0484

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A theory of the absorption of a laser field by an atomic or condensed matter medium is presented for the case where the medium is also interacting with a strong electromagnetic field. The rotating wave approximation is not assumed for the latter. It is shown that in the weak probe limit the Lindblad master equation reduces to a smaller system of linear equations for the relevant steady-state coherences. In this limit, the complex susceptibility of the medium can be expressed in terms of individual contributions of decaying dressed states, the latter being eigenstates of a non-Hermitian Floquet Hamiltonian.
In this chapter,we shall analyze the particular case of an atom interacting with a laser pulse whose duration is sufficiently long, so that the evolution of the atom in the laser field is adiabatic. When this condition is fulfilled, the atom can be considered to interact with a monochromatic laser field. As a consequence, the Hamiltonian of the system is periodic in time, and the Floquet theory [1] can be used to solve the time-dependent Schrödinger equation (TDSE) non-perturbatively. We begin in Section 4.1 by considering the Hermitian Floquet theory. We first derive the Floquet theorem for a monochromatic, spatially homogeneous laser field and show that the solutions of the TDSE correspond to dressed states having real quasi-energies , which can be obtained by solving an infinite system of time-independent coupled equations. We then generalize the Floquet theory to multicolor laser fields and to “non-dipole” laser fields which are not spatially homogeneous. In Section 4.2, the Floquet theory is applied to study the dynamics of a model atom having M discrete levels interacting with a monochromatic laser field. In this case, the coupling between the bound and continuum atomic states is neglected.We analyze the relationship between the Floquet theory and the rotating wave approximation, and examine the perturbative limit of the Floquet theory. We also consider the population transfer between Floquet dressed states.
An analysis is made of the spectrum of absorption of a weak probe electromagnetic by two-level atoms in a strong resonant laser field, undergoing collision with buffer gas atoms. The analysis is made using an approach that allows for the direct influence of a strong electromagnetic on the dynamics of an elastic collision between an active atom and a buffer gas atom. Rate equations are analyzed for a combined atom–strong electromagnetic field system (an atom dressed by the field) allowing for spontaneous and optical collisional transitions, and also for the interaction with the probe field. In the steady-state case, an expression is derived for the electric susceptibility of the medium at the small-signal frequency. This expression contains the rates of the optical collisional transitions that depend nontrivially on the parameters of the strong electromagnetic field. The phenomenological characteristics of optical collisional transitions generally used are only valid at low intensities and for small frequency detunings of the strong electromagnetic field, i.e., in the impact limit.
We introduce a non-Hermitian Schrödinger-type approximation of optical Bloch equations for two-level systems. This approximation provides a complete and accurate description of the coherence and decoherence dynamics in both weak and strong laser fields at the cost of losing accuracy in the description of populations. In this approach, it is sufficient to propagate the wave function of the quantum system instead of the density matrix, providing that relaxation and dephasing are taken into account via automatically adjusted time-dependent gain and decay rates. The developed formalism is applied to the problem of scattering and absorption of electromagnetic radiation by a thin layer comprised of interacting two-level emitters.
The many-mode Floquet theory (MMFT) recently developed by authors is extended to incorporate the irreversible damping mechanisms for the nonperturbative treatment of the dynamical evolution of dissipative three-level systems at two-photon or multiphoton coherent resonance trapping conditions induced by two strong linearly polarized monochromatic fields. It has been recently shown by several workers that under the rotating-wave approximation (RWA), population may be permanently trapped in the three-level system if the coherent monochromatic fields are exactly two-photon resonant with the initial and final states, decoupled from the intermediate decaying level. In practice, the inclusion of the non-RWA terms necessarily modifies the resonant trapping conditions and behavior. In this paper we extend the generalized Van Vleck (GVV) nearly degenerate perturbation theory to an analytical treatment of the non-Hermitian two-mode Floquet Hamiltonian. This reduces the infinite-dimensional time-independent non-Hermitian Floquet Hamiltonian to a 3\ifmmode\times\else\texttimes\fi{}3 effective Hamiltonian, from which essential properties of the coherent population-trapping behavior as well as the dynamical evolution of the dissipative SU(3) coherence vector S\ensuremath{\rightarrow}(t) can be readily obtained and expressed in terms of only three complex quasienergy eigenvalues and eigenvectors. The MMFT-GVV studies show that the RWA two-photon resonant trapping condition is substantially modified by the effects of non-RWA terms, and that the system can be ``quasitrapped'' for only a finite amount of time characterized by a small imaginary energy (width) associated with a coherent superposition state of the initial and final levels. Furthermore, it is found that the initially eight-dimensional coherence vector S\ensuremath{\rightarrow}(t) evolves predominantly to a one-dimensional scalar at the two-photon or multiphoton resonant quasitrapping conditions. Detailed results and pictorial representations of the population trapping and SU(3) dissipative dynamical evolution are presented.
Recent developments on intense laser sources is opening a new field of optical sciences. An intense coherent light beam strongly interacting with the matter causes a coherent motion of a particle, forming a strongly dressed excited particle. A photon emission from this dressed excited particle is a strong nonlinear process causing high-harmonic generation (HHG), where the perturbation analysis is broken down. In this work, we study a coherent photon emission from a strongly dressed excited atom in terms of complex spectral analysis in the extended Floquet-Hilbert-space. We have obtained the eigenstates of the total Hamiltonian with use of Feshbach-Brilloiun-Wigner projection method. In this extended space, the eigenstates of the total Hamiltonian consisting of the radiation field and the atom system have complex eigenvalues whose imaginary part represents the decay rate. Time evolution of the system is represented by the complex eigenvector expansion so that the correlation dynamics between the photon and the atom is fully taken into account. The HHG is interpreted as the irreversible spontaneous photon emission due to the resonance singularity in terms of the multiple Floquet states that are generated by periodic external field. We have found that the interference between the emitted photons over the different Floquet states causes spatial pulse emission correlated with the decay process of the excited atom.
The dressed atom approach provides a tool to investigate the dynamics of an atom-laser system by fully retaining the quantum nature of the coherent mode. In its standard derivation, the internal atom-laser evolution is described within the rotating-wave approximation, which determines a doublet structure of the spectrum and the peculiar fluorescence triplet in the steady state. However, the rotating wave approximation may fail to apply to atomic systems subject to femtosecond light pulses, light-matter systems in the strong-coupling regime or sustaining permanent dipole moments. This work aims to demonstrate how the general features of the steady-state radiative cascade are affected by the interaction of the dressed atom with propagating radiation modes. Rather than focusing on a specific model, we analyze how these features depend on the parameters characterizing the dressed eigenstates in arbitrary atom-laser dynamics, given that a set of general hypotheses is satisfied. Our findings clarify the general conditions in which a description of the radiative cascade in terms of transition between dressed states is self-consistent. We provide a guideline to determine the properties of photon emission for any atom-laser interaction model, which can be particularly relevant when the model should be tailored to enhance a specific line. We apply the general results to the case in which a permanent dipole moment is a source of low-energy emission, whose frequency is of the order of the Rabi coupling.