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arXiv:1403.6816 · Physical Review Letters

Long-Lived Quasistationary Coherences in a V -type System Driven by Incoherent Light

Timur V. Tscherbul, Paul W. Brumer

Published Sep 11, 2014• 82 citations
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Abstract

We present a theoretical study of noise-induced quantum coherences in a model three-level $V$-type system interacting with incoherent radiation, an important prototype for a wide range of physical systems ranging from trapped ions to biomolecules and quantum dots. By solving the quantum optical equations of motion, we obtain analytic expressions for the noise-induced coherences and show that they exhibit an oscillating behavior in the limit of large excited level spacing $\mathrm{\ensuremath{\Delta}}$ ($\mathrm{\ensuremath{\Delta}}/\ensuremath{\gamma}\ensuremath{\gg}1$, where $\ensuremath{\gamma}$ is the radiative decay width). Most remarkably, we find that in the opposite limit of small level spacing $\mathrm{\ensuremath{\Delta}}/\ensuremath{\gamma}\ensuremath{\ll}1$, appropriate for large molecules, (a) the coherences can survive for an extremely long time $\ensuremath{\tau}=(2/\ensuremath{\gamma})(\mathrm{\ensuremath{\Delta}}/\ensuremath{\gamma}{)}^{\ensuremath{-}2}$ before eventually decaying to zero, and (b) coherences at short times can be substantial. We further show that the long-lived coherences can survive environmental relaxation and decoherence, suggesting implications to the design of quantum heat engines and to incoherent light excitation of biological systems.

DOI
10.1103/physrevlett.113.113601

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Closed-form analytic solutions to non-secular Bloch-Redfield master equations for quantum dynamics of a V-type system driven by weak coupling to a thermal bath, relevant to light harvesting processes, are obtained and discussed. We focus on noise-induced Fano coherences among the excited states induced by incoherent driving of the V-system initially in the ground state. For suddenly turned-on incoherent driving, the time evolution of the coherences is determined by the damping parameter ζ=12(γ1+γ2)/Δp, where γi are the radiative decay rates of the excited levels i = 1, 2, and Δp=Δ(2)+(1-p(2))γ1γ2 depends on the excited-state level splitting Δ > 0 and the angle between the transition dipole moments in the energy basis. The coherences oscillate as a function of time in the underdamped limit (ζ ≫ 1), approach a long-lived quasi-steady state in the overdamped limit (ζ ≪ 1), and display an intermediate behavior at critical damping (ζ = 1). The sudden incoherent turn-on is shown to generate a mixture of excited eigenstates |e1〉 and |e2〉 and their in-phase coherent superposition |ϕ+〉=1r1+r2(r1|e1〉+r2|e2〉), which is remarkably long-lived in the overdamped limit (where r1 and r2 are the incoherent pumping rates). Formation of this coherent superposition enhances the decay rate from the excited states to the ground state. In the strongly asymmetric V-system where the coupling strengths between the ground state and the excited states differ significantly, additional asymptotic quasistationary coherences are identified, which arise due to slow equilibration of one of the excited states. Finally, we demonstrate that noise-induced Fano coherences are maximized with respect to populations when r1 = r2 and the transition dipole moments are fully aligned.
Light-induced processes in nature occur by irradiation with slowly turned-on incoherent light. The general case of time-dependent incoherent excitation is solved here analytically for V-type systems using a newly developed master equation method. Clear evidence emerges for the disappearance of radiatively induced coherence as turn-on times of the radiation exceed characteristic system times. The latter is the case, in nature, for all relevant dynamical time scales for other than nearly degenerate energy levels. We estimate that, in the absence of non-radiative relaxation and decoherence, turn-on times slower than 1 ms (still short by natural standards) only induce Fano coherences between energy eigenstates that are separated by less than 0.9 cm−1.
We present a theoretical study of quantum coherent dynamics of a three-level Λ-system driven by a thermal environment (such as blackbody radiation), which serves as an essential building block of photosynthetic light-harvesting models and quantum heat engines. By solving nonsecular Bloch–Redfield master equations, we obtain analytical results for the ground-state population and coherence dynamics and classify the dynamical regimes of the incoherently driven Λ-system as underdamped and overdamped depending on whether the ratio Δ/[rf(p)] is greater or less than one, where Δ is the ground-state energy splitting, r is the incoherent pumping rate, and f(p) is a function of the transition dipole alignment parameter p. In the underdamped regime, we observe long-lived coherent dynamics that lasts for τc ≃ 1/r, even though the initial state of the Λ-system contains no coherences in the energy basis. In the overdamped regime for p = 1, we observe the emergence of coherent quasi-steady states with the lifetime τc = 1.34(r/Δ2), which have a low von Neumann entropy compared to conventional thermal states. We propose an experimental scenario for observing noise-induced coherent dynamics in metastable He* atoms driven by x-polarized incoherent light. Our results suggest that thermal excitations can generate experimentally observable long-lived quantum coherent dynamics in the ground-state subspace of atomic and molecular Λ-systems in the absence of coherent driving.
The response of an arbitrary closed quantum system to a partially coherent electric field is investigated, with a focus on the transient coherences in the system. As a model we examine, both perturbatively and numerically, the coherences induced in a three level V system. Both rapid turn-on and pulsed turn-on effects are investigated. The effect of a long and incoherent pulse is also considered, demonstrating that during the pulse the system shows a coherent response which reduces after the pulse is over. Both the pulsed scenario and the thermally broadened CW case approach a mixed state in the long time limit, with rates dictated by the adjacent level spacings and the coherence time of the light, and via a mechanism that is distinctly different from traditional decoherence. These two excitation scenarios are also explored for a minimal "toy" model of the electronic levels in pigment protein complex PC645 by both a collisionally broadened CW laser and by a noisy pulse, where unexpectedly long transient coherence times are observed and explained. The significance of environmentally induced decoherence is noted.
Quantum coherence offers potential for energy conversion technologies. It influences light absorption and emission, affecting energy conversion limits and efficiency. As a result, quantum coherence is being harnessed to boost performance in quantum heat engines, photocells, and photosynthetic-inspired platforms. Of particular interest in this context is the generation of Fano coherences, i.e., the formation of quantum coherences due to the interaction with the continuum of modes characterizing an incoherent process. We aim to formalize mathematically the possibility of achieving steady-state Fano coherence in a V-type three-level quantum system using polarized incoherent radiation, without requiring the energy difference between the excited levels to tend to zero. We perform this analysis by deriving the Bloch-Redfield equation from first-principles by quantizing the incoherent radiation. The resulting reduced dynamics of the system are analysed, so as to determine the lifetime of Fano coherence and identify the conditions under which it becomes stationary. We characterise distinct dynamical regimes, ranging from weak to strong pumping, in which steady-state Fano coherence emerges, and we quantitatively determine its magnitude. For each regime, we analyse the generation of Fano coherence as a function of both the intensity of the incoherent pumping and the energy splitting between the excited levels. We also assess how obtaining Fano coherence is modified by symmetric or asymmetric decay rates. These findings indicate that a three-level quantum system driven by polarized incoherent light can act as a robust resource for coherence-assisted energy conversion and storage. Finally, we discuss the experimental challenges associated with the implementation of the proposed model using an ensemble of Rubidium atoms.