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arXiv:cond-mat/0002312 · Physical review. B, Condensed matter

Linear and nonlinear susceptibilities of a decoherent two-level system

Gregory Levine

Published Feb 15, 2000• 7 citations
arXivHTMLPDF

Abstract

The linear and nonlinear dynamical susceptibilities of a two-level system are calculated as it undergoes a transition to a decoherent state. Analogously to the Glover-Tinkham-Ferrell sum rule of superconductivity, spectral weight in the linear susceptibility is continuously transferred from a finite frequency resonance to nearly zero frequency, corresponding to a broken symmetry in the thermodynamic limit. In this respect, the behavior of the present model (the Mermin model) differs from the spin-boson model. The third order nonlinear susceptibility, corresponding to two-photon absorption, has an unexpected nonmonotonic behavior as a function of the environmental coupling, reaching a maximum within the decoherent phase of the model. Both linear and nonlinear susceptibilities may be expressed in a universal form.

DOI
10.1103/physrevb.61.4636

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The linear and nonlinear dynamical susceptibilities of a two-level system are calculated as it undergoes a transition to a decoherent state. Analogously to the Glover-Tinkham-Ferrell sum rule of superconductivity, spectral weight in the linear susceptibility is continuously transferred from a finite frequency resonance to nearly zero frequency, corresponding to a broken symmetry in the thermodynamic limit. In this respect, the behavior of the present model (the Mermin model) differs from the spin-boson model. The third order nonlinear susceptibility, corresponding to two-photon absorption, has an unexpected nonmonotonic behavior as a function of the environmental coupling, reaching a maximum within the decoherent phase of the model. Both linear and nonlinear susceptibilities may be expressed in a universal form.
A two-level system with a transverse linear infrared singular coupling to a boson gas is treated within a mode-coupling approximation for the dynamics. Static spin susceptibilities and spin polarizations are evaluated consistently with the dynamics by exploiting sum rules. The spin energy is obtained by integration over the excitation spectrum of the boson scattering matrix. In case of a high-frequency boson cutoff large compared to the level splitting, the results demonstrate pronounced precursor phenomena for the known zero-temperature phase transition of the model. In the opposite case the results are in semiquantitative agreement with previous numerical findings for the transition to self-trapping obtained by DeRaedt and DeRaedt.
We calculate the third-order nonlinear absorption and dispersion (self-phase-modulation and cross-phase modulation) of a homogeneously broadened two-level molecular system with permanent dipole moments interacting with (1) an optical field of frequency \ensuremath{\omega}, and (2) two optical fields of frequency ${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$, i.e., the susceptibilities ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-\ensuremath{\omega};\ensuremath{\omega},-\ensuremath{\omega},\ensuremath{\omega}) and ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-${\mathrm{\ensuremath{\omega}}}_{1}$;${\mathrm{\ensuremath{\omega}}}_{1}$,-${\mathrm{\ensuremath{\omega}}}_{2}$,${\mathrm{\ensuremath{\omega}}}_{2}$). Sharp features in the nonlinear absorption and dispersion appear whenever one- or two-photon resonance conditions are met. Only features corresponding to one-photon resonance arise if the difference between the permanent dipole moments of the levels, \ensuremath{\Delta}\ensuremath{\mu}, vanishes. The ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-\ensuremath{\omega};\ensuremath{\omega},-\ensuremath{\omega},\ensuremath{\omega}) spectrum has two features, one at frequency ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$ dominated by contributions proportional to ${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}^{4}$, where ${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}$ is the transition dipole moment of the two levels with transition frequency ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$, and the other at frequency ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$/2 dominated by contributions proportional to (\ensuremath{\Delta}\ensuremath{\mu})2{)}^{2})2${\mathrm{\ensuremath{\mu}}}_{\mathit{a}\mathit{b}}^{2}$. Sharp features in ${\mathrm{\ensuremath{\chi}}}^{(3)}$(-${\mathrm{\ensuremath{\omega}}}_{1}$;${\mathrm{\ensuremath{\omega}}}_{2}$,-${\mathrm{\ensuremath{\omega}}}_{2}$,${\mathrm{\ensuremath{\omega}}}_{1}$) appear when ${\mathrm{\ensuremath{\omega}}}_{2}$ is near ${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$,${\mathrm{\ensuremath{\omega}}}_{1}$,${\mathrm{\ensuremath{\omega}}}_{1}$+${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$, and \ensuremath{\Vert}${\mathrm{\ensuremath{\omega}}}_{1}$-${\mathrm{\ensuremath{\omega}}}_{\mathit{b}\mathit{a}}$\ensuremath{\Vert}.
We consider multiple noninteracting quantum mechanical two-level systems coupled to a common bosonic bath and study its quantum phase transition with Monte Carlo simulations using a continuous imaginary time cluster algorithm. The common bath induces an effective ferromagnetic interaction between the otherwise independent two-level systems, which can be quantified by an effective interaction strength. For degenerate energy levels above a critical value of the bath coupling strength $\ensuremath{\alpha}$ all two-level systems freeze into the same state and the critical value ${\ensuremath{\alpha}}_{c}$ decreases asymptotically as 1/N1/N1/N with increasing NNN. For a finite number NNN of two-level systems the quantum phase transition (at zero temperature) is in the same universality class as the single spin-boson model; in the limit $N\ensuremath{\rightarrow}\ensuremath{\infty}$ the system shows mean-field critical behavior independent of the power of the spectral function of the bosonic bath. We also study the influence of a spatial separation of the spins in a bath of bosonic modes with linear dispersion relation on the location and characteristics of the phase transition as well as on correlations between the two-level systems.
The authors consider a system comprised of a collection of identical two-level atoms interacting with the electromagnetic field in the dipole approximation and with an externally applied steady-state coherent driving field. The atoms are considered to interact with each other only via the electromagnetic field and are assumed to be contained within a volume much smaller than a resonance wavelength. The system is treated as a quantum-statistical ensemble in the rotating frame, rotating at the carrier frequency of the externally applied coherent field. The Hamiltonian in this frame is explicitly time independent and the exact analog of a spin temperature is defined. The thermodynamic-Green's-function method is used to determine the thermodynamic equilibrium properties of the system in the rotating frame. This results in a nonlinear relation between the applied field and the field in the volume containing the atoms. The expression is a nonlinear function of the effective or "spin" temperature as well, and has the form of a first-order phase transition with the macroscopic atomic polarization as order parameter. In the low-"spin"-temperature limit, and for perfect tuning, the expression reduces to the exact form of the nonlinear relation for optical bistability derived by Bonifacio and Lugiato and relating the incident and transmitted fields for atoms in a ring cavity in the mean-field approximation. The results contain absorptive as well as dispersive contributions. These results predict essentially different behavior as a function of off tuning compared with behavior predicted by others using statistical steady-state models far from thermodynamic equilibrium. In the limit of zero value for the applied field amplitude, the results reduce to the conditions for the well-known second-order superradiant" phase transition. The condition for the existence of the second-order phase transition is shown to depend on the cavity tuning and the photon escape rate. The authors also show why, in light of the experiments in optical bistability, this second-order phase is difficult to observe.
We examine the conditions in favor and necessity of a realistic multileveled description of a decohering quantum system. Under these conditions approximate techniques to simplify a multileveled system by its first two levels is unreliable and a realistic multilevel description in the formulation of decoherence is unavoidable. In this regard, our first crucial observation is that, the validity of the two level approximation of a multileveled system is not controlled purely by {\it sufficiently low temperatures}. We demonstrate using three different environmental spectral models that the type of system-environment coupling and the environmental spectrum have a dominant role over the temperature. Particularly, zero temperature quantum fluctuations induced by the Caldeira-Leggett type linear coordinate coupling can be influential in a wide energy range in the systems allowed transitions. The second crucial observation against the validity of the two level approximation is that the decoherence times being among the system's short time scales are found to be dominated not by the resonant but {\it non-resonant} processes. We demonstrate this in three stages. Firstly, our zero temperature numerical calculations reveal that, the calculated decoherence rates including relaxation, dephasing and leakage phenomena show, a linear dependence on the spectral area for all spectral models used, independent from the spectral shape within a large environmental spectral range compared to the quantum system's energies. Secondly, within the same range, the decoherence times only have a marginal dependence on the translations of the entire frequency spectrum. Finally, the same decoherence rates show strong dependence on the number of coupled levels by the system-environment coupling.
The dynamics of a two-level system which is coupled to an environmental sea of infinitely many spin-1/2 particles is investigated by use of the resolvent operator approach. Only at zero temperature does this spin-spin-bath model exhibit identical behavior as the more familiar spin-boson model. It is found that increasing temperature favors coherent dynamics. At high temperatures, the spin-spin-bath model for an Ohmic spectral density sustains a coherent dynamics if the dissipation coefficient $\ensuremath{\alpha}$ is sufficiently small, i.e., $\ensuremath{\alpha}<1/2$; while the decoherence exhibits pure exponential decay if $\ensuremath{\alpha}>1/2$.