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arXiv:2309.17126 · The Journal of Physical Chemistry Letters

Population Oscillations and Ubiquitous Coherences in Multilevel Quantum Systems Driven by Incoherent Radiation

Amro Dodin, Timur V. Tscherbul, Paul W. Brumer

Published Jul 22, 2024• 6 citations
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Abstract

We consider incoherent excitation of multilevel quantum systems, e.g., molecules with multiple vibronic states. We show that (1) the geometric constraints of the matter-field coupling operator guarantee that noise-induced coherences will be generated in all systems with four or more incoherent transitions between energy eigenstates and (2) noise-induced coherences can lead to population oscillations due to quantum interference via coherence transfer between pairs of states in the ground and excited manifolds. Our findings facilitate the experimental detection of noise-induced coherent dynamics in complex quantum systems.

DOI
10.1021/acs.jpclett.4c01621

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We consider incoherent excitation of multilevel quantum systems, e.g., molecules with multiple vibronic states. We show that (1) the geometric constraints of the matter-field coupling operator guarantee that noise-induced coherences will be generated in all systems with four or more incoherent transitions between energy eigenstates and (2) noise-induced coherences can lead to population oscillations due to quantum interference via coherence transfer between pairs of states in the ground and excited manifolds. Our findings facilitate the experimental detection of noise-induced coherent dynamics in complex quantum systems.
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.
We show that radiative coupling between two multilevel atoms having near-degenerate states can produce new interference effects in spontaneous emission. We explicitly demonstrate this possibility by considering two identical V systems each having a pair of transition dipole matrix elements that are orthogonal to each other. We discuss in detail the origin of the new interference terms and their consequences. Such terms lead to the evolution of certain coherences and excitations that would not occur otherwise. The special choice of the orientation of the transition dipole matrix elements enables us to illustrate the significance of vacuum-induced coherence in multiatom multilevel systems. These coherences can be significant in energy transfer studies.
We explore the properties of steady-state noise-induced (Fano) coherences generated in a three-level V-system continuously pumped by polarized incoherent light in the absence of coherent driving.By solving the nonsecular Bloch-Redfield quantum master equation, we obtain the ratio of the stationary coherences to excited-state populations, C = 1, which quantifies the impact of steady-state coherences on excited-state dynamical observables of the V-system.The ratio is maximized when the excited-state splitting is small compared to either the spontaneous decay rate γ or the incoherent pumping rate r.We demonstrate that while the detrimental effects of a strongly decohering environment generally suppress the coherence-to-population ratio by the factor γ d /γ , an intriguing regime exists where the C ratio displays a maximum as a function of the dephasing rate γ d .We attribute the surprising dephasing-induced enhancement of stationary Fano coherences to the environmental suppression of destructive interference of individual incoherent excitations generated at different times.We clarify the physical basis for the steady-state Fano coherence, whose imaginary part is identified with the nonequilibrium flux across a pair of qubits coupled to two independent thermal baths or, equivalently, the spontaneous emission flux from the right qubit to the right bath, unraveling a direct connection between the seemingly unrelated phenomena of incoherent driving of multilevel quantum systems and nonequilibrium quantum transport in qubit networks.We further establish the equivalence between the two-qubit system and a V-system, each of whose transitions is driven simultaneously by both baths.The real part of the steady-state Fano coherence is found to be proportional to the deviation of excited-state populations from their values in thermodynamic equilibrium, making it possible to observe signatures of steady-state Fano coherences in excited-state populations.Finally, we put forward an experimental proposal for observing steady-state Fano coherences by detecting the total fluorescence signal emitted by Calcium atoms excited by polarized versus isotropic incoherent light.Our analysis paves the way toward further theoretical and experimental studies of nonequilibrium coherent steady states in thermally driven atomic and molecular systems and for the exploration of their potential role in quantum thermodynamics and in biological processes.
We present a theoretical study of noise-induced quantum coherences in a model three-level VVV-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.
The noise-induced coherence created via the quantum interference of incoherent radiation in atomic three-level systems of V and \ensuremath{\Lambda} types driven by a pair of weak laser pulses is shown to result in exchange of optical vortices. In the three- level V-type atom-light coupling the system is populated in its ground level, while in the \ensuremath{\Lambda} model the system is initially prepared in an electromagnetically induced transparency state. By solving the quantum optical Maxwell-Bloch equations and with quantum interference of incoherent radiation present, we show that the orbital angular momentum (OAM) of the vortex probe beam can be transferred to a generated signal field. While the exchange efficiency in the V configuration is higher, the losses are less in the \ensuremath{\Lambda} scheme when we consider such a noise-induced coherence. We further discuss the effects of phase mismatching and inhomogeneous broadening on the energy conversion between light beams carrying OAM.
Coherent generation of indistinguishable single photons is crucial for many quantum communication and processing protocols. Solid-state realizations of two-level atomic transitions or three-level spin-Λ systems offer significant advantages over their atomic counterparts for this purpose, albeit decoherence can arise due to environmental couplings. One popular approach to mitigate dephasing is to operate in the weak-excitation limit, where the excited-state population is minimal and coherently scattered photons dominate over incoherent emission. Here we probe the coherence of photons produced using two-level and spin-Λ solid-state systems. We observe that the coupling of the atomiclike transitions to the vibronic transitions of the crystal lattice is independent of the driving strength, even for detuned excitation using the spin-Λ configuration. We apply a polaron master equation to capture the non-Markovian dynamics of the vibrational manifolds. These results provide insight into the fundamental limitations to photon coherence from solid-state quantum emitters.