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arXiv:1602.03705 · The Journal of Chemical Physics

Non-Hermitian wave packet approximation for coupled two-level systems in weak and intense fields

Raiju Puthumpally-Joseph, Maxim Sukharev, Éric Charron

Published Apr 20, 2016• 4 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1063/1.4947140

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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.
We introduce a non-Hermitian approximation of Bloch optical equations. This approximation provides a complete description of the excitation, relaxation, and decoherence dynamics of ensembles of coupled quantum systems in weak laser fields, taking into account collective effects and dephasing. In the proposed method, one propagates the wave function of the system instead of a complete density matrix. Relaxation and dephasing are taken into account via automatically adjusted time-dependent gain and decay rates. As an application, we compute the numerical wave packet solution of a time-dependent non-Hermitian Schrödinger equation describing the interaction of electromagnetic radiation with a quantum nano-structure, and compare the calculated transmission, reflection, and absorption spectra with those obtained from the numerical solution of the Liouville-von Neumann equation. It is shown that the proposed wave packet scheme is significantly faster than the propagation of the full density matrix while maintaining small error. We provide the key ingredients for easy-to-use implementation of the proposed scheme and identify the limits and error scaling of this approximation.
We study the Maxwell–Bloch model, which describes the propagation of a laser through a material and the associated interaction between laser and matter (polarization of the atoms through light propagation, photon emission and absorption, etc.). The laser field is described through Maxwell's equations, a classical equation, while matter is represented at a quantum level and satisfies a quantum Liouville equation known as the Bloch model. Coupling between laser and matter is described through a quadratic source term in both equations. The model also takes into account partial relaxation effects, namely the trend of matter to return to its natural thermodynamic equilibrium. The whole system involves 6 + N(N + 1)/2 unknowns, the six-dimensional electromagnetic field plus the N(N + 1)/2 unknowns describing the state of matter, where N is the number of atomic energy levels of the considered material. We consider at once a high frequency and weak coupling situation, in the general case of anisotropic electromagnetic fields that are subject to diffraction. Degenerate energy levels are allowed. The whole system is stiff and involves strong nonlinearities. We show the convergence to a nonstiff, nonlinear, coupled Schrödinger-rate model, involving 3 + N unknowns. The electromagnetic field is eventually described through its envelope, one unknown vector in ℂ3. It satisfies a Schrödinger equation that takes into account propagation and diffraction of light inside the material. Matter on the other hand is described through a N-dimensional vector describing the occupation numbers of each atomic level. It satisfies Einstein's rate equation that describes the jumps of the electrons between the various atomic energy levels, as induced by the interaction with light. The rate of exchange between the atomic levels is proportional to the intensity of the laser field. The whole system is the physically natural nonlinear model. In order to provide an important and explicit example, we completely analyze the specific (two-dimensional) Transverse Magnetic case, for which formulae turn out to be simpler. Technically speaking, our analysis does not enter the usual mathematical framework of geometric optics: it is more singular, and requires an ad hoc Ansatz.
It is our aim to study the dynamics of a two-level atom immersed in the modified radiation field of a photonic band-gap material using non-Markovian stochastic Schr\"odinger equations. Up to now, such methodology has only been applied to toy models and not to physically realistic systems as the one presented here. In order to check its validity, we shall study several of the physical phenomena already described in the literature within non-Markovian master equations, such as the long-time-limit residual population in the excited level of the atom and the population inversion which occurs in the atomic system when applying an external laser field. In addition to the stochastic equation, we propose a non-Markovian master equation derived from the stochastic formalism, which in contrast to the current models of master equation preserves positivity. We propose a correlation function for the radiation field (environment) that captures many of the physically relevant aspects of the problem and describes the short-time behavior in a more accurate way than previously proposed ones. This characteristic permits a correct description of the fluctuations of the electromagnetic field, which in the stochastic formalism are represented by the noise, and a better description of the non-Markovian effects in the atomic dynamics. The methodology presented in this paper to apply stochastic Schr\"odinger equations can be followed to study more complex systems, like many-level atoms embedded in more complicated photonic band-gap structures.
Time-dependent density functional theory (TDDFT) has developed into an efficient and versatile description of realistic extended many-electron systems driven, e.g., by strong laser fields. It accounts for the fully coherent evolution of the NNN-electron wave packet representing an isolated system. Decoherence as encountered in open systems by coupling to external degrees of freedom of a bath of, e.g., phonons or defects, is, by construction, absent. In this work we present an open-quantum system (OQS) extension of TDDFT accounting for dephasing and decoherence due to electron-phonon or defect scattering. We test the OQS-TDDFT for high-harmonic generation and irreversible changes of dielectric properties in solids driven by strong ir and mid-ir laser pulses. We present applications to diamond as a prototypical wide band-gap dielectric. For weak pulses we demonstrate the equivalence of OQS-TDDFT with the solution of the Bloch equations for the reduced one-particle density matrix while differences appear at high excitation densities. Our study highlights the importance of the accurate representation of the band structure in simulations of the harmonic spectrum. Narrow avoided crossings within the Brillouin zone can give rise to Bloch-type oscillations.
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.
A V-type three level system with two closely spaced upper levels interacting with a single mode of the electromagnetic field is studied for the absorptive and dispersive lineshapes. A semiclassical description for the atom-field interaction is being adopted to obtain the usual optical Bloch equations. The approximate analytical solutions for the density matrix elements are obtained by solving coupled optical Bloch equations. Through the off-diagonal density matrix elements, the introduction of phase angles between the levels participating in dipole allowed transitions are automatic. It is shown that these phases are appreciable if the applied electromagnetic field is strong. These field dependent phases (coherence) are responsible for the reduction of the inversionless gain and the absorptionless dispersion. For large decay constants, it is found that the energy gap between the upper two levels has no role to play on the laser without inversion and on the absorptionless dispersion. However, for large population per unit decay, a significant increase of the absorptionless dispersion and the inversionless gain is obtained. The condition for large population decay and a possible experimental realization of the field dependent phases are discussed.