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Register a new userNonlinear Light Absorption in Many-Electron Systems Excited by an Instantaneous Electric Field: A Non-Perturbative Approach
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We study light absorption in many-electron interacting systems beyond the linear regime by using a {em single} broadband impulse of an electric field in the instantaneous limit. We determine non-pertubatively the absorption cross section from the Fourier transform of the time-dependent induced dipole moment, which can be obtained from the time evolution of the wavefunction. We discuss the dependence of the resulting cross section on the magnitude of the impulse and we highlight the advantages of this method in comparison with perturbation theory working on a one-dimensional model system for which numerically exact solutions are accessible. Thus we demonstrate that the considered non pertubative approach provides us with an effective tool for investigating fluence-dependent nonlinear optical excitations.
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Perturbation theory (PT) is a powerful and commonly used tool in the investigation of closed quantum systems. In the context of open quantum systems, PT based on the Markovian quantum master equation is much less developed. The investigation of open systems mostly relies on exact diagonalization of the Liouville superoperator or quantum trajectories. In this approach, the system size is rather limited by current computational capabilities. Analogous to closed-system PT, we develop a PT suitable for open quantum systems. This proposed method is useful in the analytical understanding of open systems as well as in the numerical calculation of system properties, which would otherwise be impractical.
If one-electron observables of a many-electron system are of interest, a many-electron dynamics can be represented exactly by a one-electron dynamics with effective potentials. The formalism for this reduction is provided by the Exact Electron Factorization (EEF). We study the time-dependent features of the EEF effective potentials for a model of an atom ionized by an ultrastrong and ultrashort laser pulse, with the aim of understanding what is needed to develop computationally feasible approximations. It is found that the simplest approximation, the so-called time-independent conditional amplitude (TICA) approximation, is complementary to single-active electron (SAE) approaches as it reproduced the exact dynamics well for high photon frequencies of the laser field or large Keldysh parameter. For relatively low frequencies of the laser field or for smaller Keldysh parameters, we find that excited state dynamics in the core region of the atom leads to a time-dependent ionization barrier in the EEF potential. The time-dependence of the barrier needs to be described accurately to correctly model many-electron effects, and we conclude that a multi-state extension of the TICA approximation is a possible route how this can be achieved. In general, our study sheds a different light on one-electron pictures of strong-field ionization and shows that many-electron effects for such processes may be included by solving a one-electron Schrodinger equation, provided the core dynamics can be modeled successfully.
We combine experimental and theoretical approaches to explore excited rotational states of molecules embedded in helium nanodroplets using CS$_2$ and I$_2$ as examples. Laser-induced nonadiabatic molecular alignment is employed to measure spectral lines for rotational states extending beyond those initially populated at the 0.37 K droplet temperature. We construct a simple quantum mechanical model, based on a linear rotor coupled to a single-mode bosonic bath, to determine the rotational energy structure in its entirety. The calculated and measured spectral lines are in good agreement. We show that the effect of the surrounding superfluid on molecular rotation can be rationalized by a single quantity -- the angular momentum, transferred from the molecule to the droplet.
We study the interaction between two neutral atoms or molecules subject to a uniform static electric field, using quantum mechanics (QM) and quantum electrodynamics (QED) applied to coupled harmonic Drude oscillators. Our focus is to understand the interplay between dispersion interactions and field-induced electrostatics and polarization in both retarded and non-retarded regimes. We present an exact solution for two coupled oscillators using QM and Rayleigh-Schrodinger perturbation theory, demonstrating that the external field controls the strength of different intermolecular interactions and relative orientations of the molecules. In the retarded regime described by QED and rationalized by stochastic electrodynamics, our analysis shows that field-induced electrostatics and polarization terms remain unchanged (in isotropic and homogeneous vacuum) compared to the non-retarded QM description, in contrast to a recent work. Our framework combining four complementary theoretical approaches paves the way to a systematic description and enhanced understanding of molecular interactions under the combined action of external and vacuum fields.
A number of physical processes occurring in a flat one-dimensional graphene structure under the action of strong time-dependent electric fields are considered. It is assumed that the Dirac model can be applied to the graphene as a subsystem of the general system under consideration, which includes an interaction with quantized electromagnetic field. The Dirac model itself in the external electromagnetic field (in particular, the behavior of charged carriers) is treated nonperturbatively with respect to this field within the framework of strong-field QED with unstable vacuum. This treatment is combined with a kinetic description of the radiation of photons from the electron-hole plasma created from the vacuum under the action of the electric field. An interaction with quantized electromagnetic field is described perturbatively. A significant development of the kinetic equation formalism is presented. A number of specific results are derived in course of analytical and numerical study of the equations. We believe that some of predicted effects and properties of considered processes may be verified experimentally. Among these effects, it should be noted a characteristic spectral composition anisotropy of the quantum radiation and a possible presence of even harmonics of the external field in the latter radiation.
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