We explore the properties of steady-state Fano coherences generated in a three-level V-system continuously pumped by polarized incoherent light in the absence of coherent driving. The ratio of the stationary coherences to excited-state populations $\mathcal{C} = (1+\frac{Δ^2}{γ(r+γ)} )^{-1}$ is maximized when the excited-state splitting $Δ$ is small compared to either the spontaneous decay rate $γ$ or the incoherent pumping rate $r$. We demonstrate that an intriguing regime exists where the $\mathcal{C}$ 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 identify the imaginary Fano coherence with the non-equilibrium flux across a pair of qubits coupled to two independent thermal baths, unraveling a direct connection between the seemingly unrelated phenomena of incoherent driving of multilevel quantum systems and non-equilibrium quantum transport in qubit networks. 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. 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 vs. isotropic incoherent light. Our analysis paves the way toward further theoretical and experimental studies of non-equilibrium coherent steady states in thermally driven atomic and molecular systems, and for the exploration of their potential role in biological processes.
Two different Master Equation approaches have been formally derived to address the dynamics of open quantum systems interacting with a thermal environment (such as sunlight). They have led to two different physical results: non-secular equations that show noise-induced (Fano) coherences and secular equations that do not. An experimental test for the appearance of non-secular terms is proposed using Ca atoms in magnetic fields excited by broadband incoherent radiation. Significantly different patterns of fluorescence are predicted, allowing for a clear test for the validity of the secular and n…
Experimental challenges and prospects for quantum-enhanced energy conversion: Stationary Fano coherence in V-type qutrits interacting with polarized incoherent radiation
Istituto Nazionale di Ottica, Consiglio Nazionale delle Ricerche (CNR-INO)（意大利国家光学研究所）；European Laboratory for Non-linear Spectroscopy (LENS), Università degli Studi di Firenze（佛罗伦萨大学非线性光谱学欧洲实验室）；Dipartimento di Fisica e Astronomia, Università degli Studi di Firenze（佛罗伦萨大学物理与天文学系）；Istituto dei Sistemi Complessi, Consiglio Nazionale delle Ricerche (CNR-ISC)（意大利复杂系统研究所）
The question of how quantum coherence facilitates energy transfer has been intensively debated in the scientific community. Since natural and artificial light-harvesting units operate under the stationary condition, we address this question via a non-equilibrium steady-state analysis of a molecular dimer irradiated by incoherent sunlight and then generalize the key predictions to arbitrarily-complex exciton networks. The central result of the steady-state analysis is the coherence-flux-efficiency relation:$η=c\sum_{i\neq j}F_{ij}κ_j=2c\sum_{i\neq j}J_{ij}{\rm Im}[ρ_{ij}]κ_j$ with $c$ the norma…
We present 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. 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 $ζ=\frac{1}{2}(γ_1+γ_2)/Δ_p$, where $γ_i$ are the radiative decay rates of the excited levels $i=1,2$, and $Δ_p=\sqrt{Δ^2 + (1-p^2)γ_1γ_2}$ depends on the excited-st…
We investigate steady-state properties of a two-dimensional incoherent-pumped dissipative Bose-Hubbard model, which describes a photon square lattice. This incoherent pumping exhibits an important environment-induced higher-order fluctuation effect, which induces a strong competition between the driven-dissipative channel, the photon-photon interaction, and the photon hopping in multi-photon processes. This new competition gives rise to a spontaneous breaking of the U(1) symmetry of system. As a result, we predict a many-body steady-state localized-delocalized phase transition and an anti-bloc…
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-…
In the case of quantum systems interacting with multiple environments, the time-evolution of the reduced density matrix is described by the Liouvillian. For a variety of physical observables, the long-time limit or steady state solution is needed for the computation of desired physical observables. For inverse design or optimal control of such systems, the common approaches are based on brute-force search strategies. Here, we present a novel methodology, based on automatic differentiation, capable of differentiating the steady state solution with respect to any parameter of the Liouvillian. Ou…
We investigate the collective interaction of a multi-atom three-level ladder system with an environmental incoherent reservoir. The exact solution of the master equation that describes such a system of atoms emitting distinguishable or indistinguishable photons on interaction with an incoherent reservoir is obtained. The quantum decay interference effects have no influences over steady-state distribution of population among the energy levels. However, the photon statistics of the collectively emitted photons are different in this case. In particular, the normalized second-order photon correlat…
Following the method of Victor V. Kozlov et al.[PhysRevA. 74. 063829],we inspect the coherence induced by incoherent pump and spontaneous decay process in $Λ$ type three-level atomic system with degenerated lower duplicate levels. The system shows a coherent population trapping state and multi-steady states characteristic in different conditions. Interestingly, two kinds of steady states generated by the system in different sets of pumping and decaying parameters, the "singlet" state and the "triplet" state, exhibit stable or unstable characteristics under the action of pumping field and vacuu…
Oscillations in time-dependent 2D electronic spectra appear as evidence of quantum coherence in light-harvesting systems related to electronic-vibrational resonant interactions. Nature, however, takes place in a non-equilibrium steady-state, so the relevance of these arguments to the natural process is unclear. Here we examine the role of intramolecular vibrations in the non-equilibrium steady-state of photosynthetic dimers in the natural scenario of incoherent light excitation. It is found that vibrations resonant with the energy difference between exciton states do not increase the quantum y…
Electromagnetically induced slow-light medium is a promising system for quantum memory devices, but controlling its noise level remains a major challenge to overcome. This work considers the simplest model for such medium, comprised of three-level $Λ$-systems interacting with bosonic bath, and provides a new fundamental trade-off relation in light-matter interaction between the group velocity of light and the Fano factor of photon current due to radiative transitions. Considering the steady state limits of a newly derived Lindblad-type equation, we find that the Fano factor of the photon curre…
We present a systematic approach for constructing steady state density operators of Markovian dissipative evolution for open quantum chain models with integrable bulk interaction and boundary incoherent driving. The construction is based on fundamental solutions of the quantum Yang-Baxter equation pertaining to quantum algebra symmetries and their quantizations (q-deformations). In particular, we facilitate a matrix-product state description, by resorting to generic spin-s infinite-dimensional solutions associated with non-compact spins, serving as ancillary degrees of freedom. After formally …
The nonequilibrium steady state (NESS) of a quantum network is central to a host of physical and biological scenarios. Examples include natural processes such as vision and photosynthesis, as well as technical devices such as photocells, both activated by incoherent light (e.g. sunlight) and leading to quantum transport. Here, a completely general approach to defining components of a quantum network in the NESS, and obtaining rates of processes between these components is provided. Quantum effects are explicitly included throughout, both in (a) defining network components via projection operat…
One of the most pertinent problems in the debate on non-trivial quantum effects in biology concerns natural photosynthesis. Since sunlight is composed of thermal photons, it was argued to be unable to induce quantum coherence in matter, and that quantum mechanics is therefore irrelevant for the dynamical processes following photoabsorption. Our present analysis of a toy ``molecular aggregate" -- composed of two dipole-dipole interacting two-level atoms treated as an open quantum system -- however shows that incoherent excitations indeed can trigger coherent dynamics that persist: We demonstrat…
We discuss current carrying non-equilibrium steady state of an open fermionic Hubbard chain that is strongly driven by markovian incoherent processes localized at the chain ends. An explicit form of exact many-body density operator for any value of the coupling parameter is presented. The structure of a matrix product form of the solution is encoded in terms of a novel diagrammatic technique which should allow for generalization to other integrable non-equillibrium models.
We experimentally study a driven-dissipative Josephson junction array, realized with a weakly interacting Bose Einstein condensate residing in a one-dimensional optical lattice. Engineered losses on one site act as a local dissipative process, while tunneling from the neighboring sites constitutes the driving force. We characterize the emerging steady-states of this atomtronic device. With increasing dissipation strength $γ$ the system crosses from a superfluid state, characterized by a coherent Josephson current into the lossy site to a resistive state, characterized by an incoherent hopping …
There has recently been some interest in the prospect of detecting ionized intergalactic baryons by examining the properties of incoherent light from background cosmological sources, namely quasars. Although the paper by \cite{lieu13} proposed a way forward, it was refuted by the later theoretical work of \cite{hir14} and observational study of \cite{hal16}. In this paper we investigated in detail the manner in which incoherent radiation passes through a dispersive medium both from the frameworks of classical and quantum electrodynamics, which led us to conclude that the premise of \cite{lieu1…
Excitation of molecules by incident incoherent electromagnetic radiation, such as sunlight, is described in detail and contrasted with the effect of coherent (e.g. laser) light. The nature of the quantum coherences induced by the former, relevant to transport processes in nature and in technology, is emphasized. Both equilibrium and steady state scenarios are discussed, Three examples: simple models, calcium excitation in polarized light, and the isomerization of retinal in rhodopsin are used to expose the underlying qualitative nature of the established coherences.
We identify sufficient conditions on the structure of the interaction Hamiltonian between a two-level quantum system and a thermal bath which, without any external drive or coherent measurement, guarantee the generation of steady-state coherences (SSC). The SSC this way obtained remarkably turn out to be independent on the initial state of the system, which therefore could be even taken initially incoherent. We characterize in detail this phenomenon first analytically in the weak coupling regime for two paradigmatic models, and then numerically in more complex systems without any assumption on…
We investigate experimentally the number statistics of a mesoscopic ensemble of cold atoms in a microscopic dipole trap loaded from a magneto-optical trap, and find that the atom number fluctuations are reduced with respect to a Poisson distribution due to light-assisted two-body collisions. For numbers of atoms N>2, we measure a reduction factor (Fano factor) of 0.72+/-0.07, which differs from 1 by more than 4 standard deviations. We analyze this fact by a general stochastic model describing the competition between the loading of the trap from a reservoir of cold atoms and multi-atom losses, …
Recent observations of coherence in photosynthetic complexes have led to the question of whether quantum effects can occur in vivo, not under femtosecond laser pulses but in incoherent sunlight and at steady state, and, if so, whether the coherence explains the high exciton transfer efficiency. We distinguish several types of coherence and show that although some photosynthetic pathways are partially coherent processes, photosynthesis in nature proceeds through stationary states. This distinction allows us to rule out several mechanisms of transport enhancement in sunlight. In particular, alth…
We provide a quantitative description of the nonequilibriumness based on the model of coupled oscillators interacting with multiple energy sources. This can be applied to the study of vibrational energy transport in molecules. The curl quantum flux quantifying the nonequilibriumness and time-irreversibility is quantified in the coherent representation and we find the geometric description of the shape and polarization of the flux which provides the connection between the microscopic description of quantum nonequilibriumness and the macroscopic observables, i.e., correlation function. We use th…
We show that short-range correlations have a dramatic impact on the steady-state phase diagram of quantum driven-dissipative systems. This effect, never observed in equilibrium, follows from the fact that ordering in the steady state is of dynamical origin, and is established only at very long times, whereas in thermodynamic equilibrium it arises from the properties of the (free) energy. To this end, by combining the cluster methods extensively used in equilibrium phase transitions to quantum trajectories and tensor-network techniques, we extend them to nonequilibrium phase transitions in diss…
We study an open Heisenberg XXZ spin chain with long-range Ising-type interaction, which is incoherently driven at its boundaries and therefore a far-from-equilibrium steady state current is induced. Quantum Monte Carlo techniques make a regime accessible, where the system size is large enough to examine the transition from a diffusive to a ballistic transport regime. We find that the chain lengths for this transition are increasing with decreasing range of the Ising-type interactions between distant spins, while the strength of the incoherent driving does not have a relevant effect on the tra…
We study a driven-dissipative Bose-Hubbard model in presence of two-particle losses and an incoherent single-particle drive on each lattice site, leading to a finite-density stationary state. Using dynamical mean-field theory (DMFT) and an impurity solver based on exact diagonalization of the associated Lindbladian, we investigate the regime of strong two-particle losses. Here, a stationary-state quantum Zeno effect emerges, as can be seen in the on-site occupation and spectral function. We show that DMFT captures this effect through its self-consistent bath. We show that, in the deep Zeno reg…
We consider three- and four-level atomic lasers that are either incoherently (unidirectionally) or coherently (bidirectionally) pumped, the single-mode cavity being resonant with the laser transition. The intra-cavity Fano factor and the photo-current spectral density are evaluated on the basis of rate equations. According to that approach, fluctuations are caused by jumps in active and detecting atoms. The algebra is considerably simpler than the one required by Quantum-Optics treatments. Whenever a comparison can be made, the expressions obtained coincide. The conditions under which the outp…
We give a semiclassical analysis of the average photon number as well as photon number variance (Fano factor $F$) for a Josephson-junction (JJ) embedded microwave cavity system, where the JJ is subject to a fluctuating (i.e. noisy) bias voltage with finite dc average. Through the ac Josephson effect, the dc voltage bias drives the effectively nonlinear microwave cavity mode into an amplitude squeezed state ($F<1$), as has been established previously [A. D. Armour, et al., Phys. Rev. Lett. 111, 247001 (2013)], but bias noise acts to degrade this squeezing. We find that the sensitivity of the Fa…
The appearance of steady-state coherence (SSC) from system-bath interaction proves that quantum effects can appear without an external drive. Such SSC could become a resource to demonstrate quantum advantage in the applications. We predict the generation of SSC if the target system repeatedly interacts with independent and non-correlated bath elements. To describe their behavior, we use the collision model approach of system-bath interaction, where the system interacts with one bath element (initially in an incoherent state) at a time, asymptotically (in the fast-collision regime) mimicking a …
We develop a Gutzwiller theory for the non-equilibrium steady states of a strongly-interacting photon fluid driven by a non-Markovian incoherent pump. In particular, we explore the collective excitation modes across the out-of-equilibrium Mott/superfluid transition, characterizing the diffusive Goldstone mode in the superfluid phase and the particle/hole excitations in the insulating one. Observable features in the pump-and-probe optical response of the system are highlighted. Our results appear as experimentally accessible to state-of-the-art circuit-QED devices and open the way for driven-di…
