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Quantum coherent dynamics of a $\Lambda$-system driven by a thermal environment: Enhancing coherence lifetimes via incoherent driving

Suyesh Koyu, Timur V. Tscherbul

Published Aug 17, 2021• 0 citations
OpenAlex

Abstract

We present a theoretical study of quantum coherent dynamics in a three-level $\Lambda$ system driven by a thermal environment. By solving the 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 $\Lambda$-system as underdamped and overdamped depending on whether the ratio $\Delta/[r f(p)]$ is greater or less than one, where $\Delta$ is the ground-state energy splitting, $r$ is the incoherent pumping rate, and $f(p)$ is a dimensionless function of the transition dipole alignment parameter $p$. In the underdamped regime, we observe long-lived coherent dynamics that lasts for $\tau_c\simeq 1/r$, even though the initial state of the $\Lambda$-system contains no coherences in the energy basis. In the overdampled regime for $p = 1$, we observe the emergence of coherent quasi-steady states with the lifetime $\tau_{c} = 1.34 (r/\Delta^{2})$, which have low von Neumann entropy compared to the conventional thermal states. Our results suggest that thermal excitations can enhance the lifetimes of initially created coherent superpositions, making thermal driving a potentially useful coherence-enhancing tool for quantum information science.

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Long-lived quantum coherences in a V -type system strongly driven by a thermal environment

Suyesh Koyu, Timur V. Tscherbul

We explore the coherent dynamics of a three-level $\mathsf{V}$-type system interacting with a thermal bath in the regime where thermal excitation occurs much faster than spontaneous decay. We present analytic solutions of the Bloch-Redfield quantum master equations, which show that strong incoherent pumping can generate long-lived quantum coherences among the excited states of the $\mathsf{V}$-type system in the overdamped regime defined by the condition $\mathrm{\ensuremath{\Delta}}/(\overline{n}\ensuremath{\gamma})<f(p)$, where $\mathrm{\ensuremath{\Delta}}$ is the excited-state level splitting, $\ensuremath{\gamma}$ is the spontaneous decay rate, $\overline{n}\ensuremath{\gg}1$ is the effective photon occupation number proportional to the pumping intensity, and $f(p)$ is a universal function of the transition dipole alignment parameter $p$. In the limit of nearly parallel transition dipoles ($p\ensuremath{\rightarrow}1$) the coherence lifetime ${\ensuremath{\tau}}_{c}=1.34(\overline{n}/\ensuremath{\gamma}){(\mathrm{\ensuremath{\Delta}}/\ensuremath{\gamma})}^{\ensuremath{-}2}$ scales linearly with $\overline{n}$ and is enhanced by the factor $0.67\overline{n}$ with respect to the weak-pumping limit [Phys. Rev. Lett. 113, 113601 (2014); J. Chem. Phys. 144, 244108 (2016)]. We also establish the existence of long-lived quasistationary states, which occur in the overdamped regime and affect the process of thermalization of the $\mathsf{V}$-type system with the bath, slowing down the approach to thermal equilibrium. In the case of nonparallel transition dipole moments ($p<1$), no quasistationary states are formed and the coherence lifetime decreases sharply. The sharp transition between the different regimes of coherent dynamics is due to an interplay between coherence-generating Fano interference and various coherence-destroying processes (such as stimulated decay). Using a newly developed effective decoherence rate model, we find that in the limit $p\ensuremath{\rightarrow}1$ the rates of coherence generation and decay are almost exactly balanced and the effective decoherence rate is minimized, leading to long coherence lifetimes. Our results reveal new regimes of long-lived quantum coherent dynamics, which could be observed in thermally driven atomic and molecular systems.

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Quantum coherent dynamics of a Λ\LambdaΛ-system driven by a thermal environment: Enhancing coherence lifetimes via incoherent driving
We present a theoretical study of quantum coherent dynamics in a three-level Λ\LambdaΛ system driven by a thermal environment. By solving the 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\LambdaΛ-system as underdamped and overdamped depending on whether the ratio Δ/[rf(p)]\Delta/[r f(p)]Δ/[rf(p)] is greater or less than one, where Δ\DeltaΔ is the ground-state energy splitting, rrr is the incoherent pumping rate, and f(p)f(p)f(p) is a dimensionless function of the transition dipole alignment parameter ppp. In the underdamped regime, we observe long-lived coherent dynamics that lasts for τc≃1/r\tau_c\simeq 1/rτc​≃1/r, even though the initial state of the Λ\LambdaΛ-system contains no coherences in the energy basis. In the overdampled regime for p=1p = 1p=1, we observe the emergence of coherent quasi-steady states with the lifetime τc=1.34(r/Δ2)\tau_{c} = 1.34 (r/\Delta^{2})τc​=1.34(r/Δ2), which have low von Neumann entropy compared to the conventional thermal states. Our results suggest that thermal excitations can enhance the lifetimes of initially created coherent superpositions, making thermal driving a potentially useful coherence-enhancing tool for quantum information science.
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.
We explore the coherent dynamics of a three-level V\mathsf{V}V-type system interacting with a thermal bath in the regime where thermal excitation occurs much faster than spontaneous decay. We present analytic solutions of the Bloch-Redfield quantum master equations, which show that strong incoherent pumping can generate long-lived quantum coherences among the excited states of the V\mathsf{V}V-type system in the overdamped regime defined by the condition $\mathrm{\ensuremath{\Delta}}/(\overline{n}\ensuremath{\gamma})<f(p)$, where $\mathrm{\ensuremath{\Delta}}$ is the excited-state level splitting, $\ensuremath{\gamma}$ is the spontaneous decay rate, $\overline{n}\ensuremath{\gg}1$ is the effective photon occupation number proportional to the pumping intensity, and f(p)f(p)f(p) is a universal function of the transition dipole alignment parameter ppp. In the limit of nearly parallel transition dipoles ($p\ensuremath{\rightarrow}1$) the coherence lifetime ${\ensuremath{\tau}}_{c}=1.34(\overline{n}/\ensuremath{\gamma}){(\mathrm{\ensuremath{\Delta}}/\ensuremath{\gamma})}^{\ensuremath{-}2}$ scales linearly with n‾\overline{n}n and is enhanced by the factor 0.67n‾0.67\overline{n}0.67n with respect to the weak-pumping limit [Phys. Rev. Lett. 113, 113601 (2014); J. Chem. Phys. 144, 244108 (2016)]. We also establish the existence of long-lived quasistationary states, which occur in the overdamped regime and affect the process of thermalization of the V\mathsf{V}V-type system with the bath, slowing down the approach to thermal equilibrium. In the case of nonparallel transition dipole moments (p<1p<1p<1), no quasistationary states are formed and the coherence lifetime decreases sharply. The sharp transition between the different regimes of coherent dynamics is due to an interplay between coherence-generating Fano interference and various coherence-destroying processes (such as stimulated decay). Using a newly developed effective decoherence rate model, we find that in the limit $p\ensuremath{\rightarrow}1$ the rates of coherence generation and decay are almost exactly balanced and the effective decoherence rate is minimized, leading to long coherence lifetimes. Our results reveal new regimes of long-lived quantum coherent dynamics, which could be observed in thermally driven atomic and molecular systems.
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.
Abstract Whether genuine quantum effects, particularly quantum coherences, can offer an advantage to quantum devices is a topic of much interest. Here, we study a minimal model, the three-level V system coupled to two heat baths, and investigate the role of quantum coherences in heat transport in both the transient regime and in the nonequilibrium steady-state. In our model, energy is exchanged between the baths through two parallel pathways, which can be made distinct through the nondegeneracy of excited levels (energy splitting Δ) and a control parameter α , which adjusts the strength of one of the arms. Using a nonsecular quantum master equation of Redfield form, we succeed in deriving closed-form expressions for the quantum coherences and the heat current in the steady state limit for closely degenerate excited levels. By including three ingredients in our analysis: nonequilibrium baths, nondegeneracy of levels, and asymmetry of pathways, we show that quantum coherences are generated and sustained in the V model in the steady-state limit if three conditions, conjoining thermal and coherent effects are simultaneously met: (i) the two baths are held at different temperatures. (ii) Bath-induced pathways do not interfere destructively. (iii) Thermal rates do not mingle with the control parameter α to destroy interference through an effective local equilibrium condition. Particularly, we find that coherences are maximized when the heat current is suppressed. Although we mainly focus on analytical results in the steady state limit, numerical simulations reveal that the transient behavior of coherences contrasts the steady-state limit: large long-lived transient coherences vanish at steady state, while weak short-lived transient coherences survive, suggesting that different mechanisms are at play in these two regimes. Enhancing either the lifetime of transient coherences or their magnitude at steady state thus requires the control and optimization of different physical parameters.
We develop a perturbative technique for solving Markovian quantum dissipative dynamics, with the perturbation parameter being a small gap in the eigenspectrum. As an example, we apply the technique and straightforwardly obtain analytically the dynamics of a three-level system with quasidegenerate excited states, where quantum coherences persist for very long times, proportional to the inverse of the energy splitting squared. We then show how to bypass this long-lived coherent dynamics and accelerate the relaxation to thermal equilibration in a hyper-exponential manner, a Markovian quantum-assisted Mpemba-like effect. This hyperacceleration of the equilibration process manifests if the initial state is carefully prepared, such that its coherences precisely store the amount of population relaxing from the initial condition to the equilibrium state. Our analytical method for solving quantum dissipative dynamics readily provides equilibration timescales, and as such it reveals how coherent and incoherent effects interlace in the dynamics. It further advises on how to accelerate relaxation processes, which is desirable when long-lived quantum coherences stagnate dynamics.
We present an efficient theoretical method for calculating the time evolution of the density matrix of a multilevel quantum system weakly interacting with incoherent light. The method combines the Bloch-Redfield theory with a partial secular approximation for one-photon coherences, resulting in a master equation that explicitly exposes the reliance on transition rates and the angles between transition dipole moments in the energy basis. The partial secular Bloch-Redfield master equation allows an unambiguous distinction between the regimes of quantum coherent vs. incoherent energy transfer under incoherent light illumination. The fully incoherent regime is characterized by orthogonal transition dipole moments in the energy basis, leading to a dynamical evolution governed by a coherence-free Pauli-type master equation. The coherent regime requires non-orthogonal transition dipole moments in the energy basis and leads to the generation of noise-induced quantum coherences and population-to-coherence couplings. As a first application, we consider the dynamics of excited state coherences arising under incoherent light excitation from a single ground state and observe population-to-coherence transfer and the formation of non-equilibrium quasisteady states in the regime of small excited state splitting. Analytical expressions derived earlier for the V-type system [T. V. Tscherbul and P. Brumer, Phys. Rev. Lett. 113, 113601 (2014)] are found to provide a nearly quantitative description of multilevel excited-state populations and coherences in both the small- and large-molecule limits.