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Conducting precise electronic-vibrational dynamics simulations of molecular systems poses significant challenges when dealing with realistic environments composed of numerous vibrational modes. Here, we introduce a technique for the construction of effective phonon spectral densities that capture accurately open-system dynamics over a finite time interval of interest. When combined with existing nonperturbative simulation tools, our approach can reduce significantly the computational costs associated with many-body open-system dynamics.
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We exploit the properties of chain mapping transformations of bosonic environments to identify a finite collection of modes able to capture the characteristic features, or fingerprint, of the environment. Moreover we show that the countable infinity of residual bath modes can be replaced by a universal Markovian closure, namely, a small collection of damped modes undergoing a Lindblad-type dynamics whose parametrization is independent of the spectral density under consideration. We show that the Markovian closure provides a quadratic speedup with respect to standard chain mapping techniques and makes the memory requirement independent of the simulation time, while preserving all the information on the fingerprint modes. We illustrate the application of the Markovian closure to the computation of linear spectra but also to nonlinear spectral response, a relevant experimentally accessible many body coherence witness for which efficient numerically exact calculations in realistic environments are currently lacking.
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We investigate the quench dynamics of an open quantum system involving a quantum phase transition. In the isolated case, the quench dynamics involving the phase transition exhibits a number of scaling relations with the quench rate as predicted by the celebrated Kibble-Zurek mechanism. In contact with an environment however, these scaling laws break down and one may observe an anti-Kibble-Zurek behavior: slower ramps lead to less adiabatic dynamics, increasing thus nonadiabatic effects with the quench time. In contrast to previous works, we show here that such anti-Kibble-Zurek scaling can acquire a universal form in the sense that it is determined by the equilibrium critical exponents of the phase transition, provided the excited states of the system exhibit singular behavior, as observed in fully connected models. This demonstrates novel universal scaling laws granted by a system-environment interaction in a critical system. We illustrate these findings in two fully connected models, namely, the quantum Rabi and the Lipkin-Meshkov-Glick models. In addition, we discuss the impact of nonlinear ramps and finite-size systems.
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A nanoring-rotaxane supramolecular assembly with a Cy7 cyanine dye (hexamethylindotricarbocyanine) threaded along the axis of the nanoring was synthesized as a model for the energy transfer between the light-harvesting complex LH1 and the reaction center in purple bacteria photosynthesis. The complex displays efficient energy transfer from the central cyanine dye to the surrounding zinc porphyrin nanoring. We present a theoretical model that reproduces the absorption spectrum of the nanoring and quantifies the excitonic coupling between the nanoring and the central dye, thereby explaining the efficient energy transfer and demonstrating similarity with structurally related natural light-harvesting systems.
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Carbocianinas/metabolismo , Colorantes/metabolismo , Complejos de Proteína Captadores de Luz/metabolismo , Nanopartículas/metabolismo , Porfirinas/metabolismo , Rotaxanos/metabolismo , Carbocianinas/química , Colorantes/química , Complejos de Proteína Captadores de Luz/química , Modelos Moleculares , Nanopartículas/química , Porfirinas/química , Rotaxanos/químicaRESUMEN
Charge and energy transfer in biological and synthetic organic materials are strongly influenced by the coupling of electronic states to a highly structured dissipative environment. Nonperturbative simulations of these systems require a substantial computational effort, and current methods can only be applied to large systems if environmental structures are severely coarse grained. Time evolution methods based on tensor networks are fundamentally limited by the times that can be reached due to the buildup of entanglement in time, which quickly increases the size of the tensor representation, i.e., the bond dimension. In this Letter, we introduce a dissipation-assisted matrix product factorization (DAMPF) method that combines a tensor network representation of the vibronic state within a pseudomode description of the environment where a continuous bosonic environment is mapped into a few harmonic oscillators under Lindblad damping. This framework is particularly suitable for a tensor network representation, since damping suppresses the entanglement growth among oscillators and significantly reduces the bond dimension required to achieve a desired accuracy. We show that dissipation removes the "time-wall" limitation of existing methods, enabling the long-time simulation of large vibronic systems consisting of 10-50 sites coupled to 100-1000 underdamped modes in total and for a wide range of parameter regimes. For these reasons, we believe that our formalism will facilitate the investigation of spatially extended systems with applications to quantum biology, organic photovoltaics, and quantum thermodynamics.
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We investigate how correlated fluctuations affect oscillatory features in rephasing and non-rephasing two-dimensional (2D) electronic spectra of a model dimer system. Based on a beating map analysis, we show that non-secular environmental couplings induced by uncorrelated fluctuations lead to oscillations centered at both cross- and diagonal-peaks in rephasing spectra as well as in non-rephasing spectra. Using an analytical approach, we provide a quantitative description of the non-secular effects in terms of the Feynman diagrams and show that the environment-induced mixing of different inter-excitonic coherences leads to oscillations in the rephasing diagonal-peaks and non-rephasing cross-peaks. We demonstrate that as correlations in the noise increase, the lifetime of oscillatory 2D signals is enhanced at rephasing cross-peaks and non-rephasing diagonal-peaks, while the other non-secular oscillatory signals are suppressed. We discuss that the asymmetry of 2D lineshapes in the beating map provides information on the degree of correlations in environmental fluctuations. Finally we investigate how the oscillatory features in 2D spectra are affected by inhomogeneous broadening.
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Quantum metrology protocols allow us to surpass precision limits typical to classical statistics. However, in recent years, no-go theorems have been formulated, which state that typical forms of uncorrelated noise can constrain the quantum enhancement to a constant factor and, thus, bound the error to the standard asymptotic scaling. In particular, that is the case of time-homogeneous (Lindbladian) dephasing and, more generally, all semigroup dynamics that include phase covariant terms, which commute with the system Hamiltonian. We show that the standard scaling can be surpassed when the dynamics is no longer ruled by a semigroup and becomes time inhomogeneous. In this case, the ultimate precision is determined by the system short-time behavior, which when exhibiting the natural Zeno regime leads to a nonstandard asymptotic resolution. In particular, we demonstrate that the relevant noise feature dictating the precision is the violation of the semigroup property at short time scales, while non-Markovianity does not play any specific role.
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We discuss the use of inequalities of the Leggett-Garg type (LGtI) to witness quantum coherence and present the first experimental violation of this type of inequalities using a light-matter interfaced system. By separately benchmarking the Markovian character of the evolution and the translational invariance of the conditional probabilities, the observed violation of a LGtI is attributed to the quantum coherent character of the process. These results provide a general method to benchmark "quantumness" when the absence of memory effects can be independently certified and confirm the persistence of quantum coherent features within systems of increasing complexity.
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The prospect of coherent dynamics and excitonic delocalization across several light-harvesting structures in photosynthetic membranes is of considerable interest, but challenging to explore experimentally. Here we demonstrate theoretically that the excitonic delocalization across extended domains involving several light-harvesting complexes can lead to unambiguous signatures in the optical response, specifically, linear absorption spectra. We characterize, under experimentally established conditions of molecular assembly and protein-induced inhomogeneities, the optical absorption in these arrays from polarized and unpolarized excitation, and demonstrate that it can be used as a diagnostic tool to determine the resonance coupling between iso-energetic light-harvesting structures. The knowledge of these couplings would then provide further insight into the dynamical properties of transfer, such as facilitating the accurate determination of Förster rates.
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Membrana Celular/metabolismo , Fenómenos Ópticos , Fotosíntesis , Teoría Cuántica , Membrana Celular/química , Modelos Moleculares , Conformación MolecularRESUMEN
We challenge the misconception that Bloch-Redfield equations are a less powerful tool than phenomenological Lindblad equations for modeling exciton transport in photosynthetic complexes. This view predominantly originates from an indiscriminate use of the secular approximation. We provide a detailed description of how to model both coherent oscillations and several types of noise, giving explicit examples. All issues with non-positivity are overcome by a consistent straightforward physical noise model. Herein also lies the strength of the Bloch-Redfield approach because it facilitates the analysis of noise-effects by linking them back to physical parameters of the noise environment. This includes temporal and spatial correlations and the strength and type of interaction between the noise and the system of interest. Finally, we analyze a prototypical dimer system as well as a 7-site Fenna-Matthews-Olson complex in regards to spatial correlation length of the noise, noise strength, temperature, and their connection to the transfer time and transfer probability.
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We present a comprehensive and up-to-date review of the concept of quantum non-Markovianity, a central theme in the theory of open quantum systems. We introduce the concept of a quantum Markovian process as a generalization of the classical definition of Markovianity via the so-called divisibility property and relate this notion to the intuitive idea that links non-Markovianity with the persistence of memory effects. A detailed comparison with other definitions presented in the literature is provided. We then discuss several existing proposals to quantify the degree of non-Markovianity of quantum dynamics and to witness non-Markovian behavior, the latter providing sufficient conditions to detect deviations from strict Markovianity. Finally, we conclude by enumerating some timely open problems in the field and provide an outlook on possible research directions.
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New experimental techniques based on nonlinear ultrafast spectroscopies have been developed over the last few years, and have been demonstrated to provide powerful probes of quantum dynamics in different types of molecular aggregates, including both natural and artificial light harvesting complexes. Fourier transform-based spectroscopies have been particularly successful, yet "complete" spectral information normally necessitates the loss of all information on the temporal sequence of events in a signal. This information though is particularly important in transient or multi-stage processes, in which the spectral decomposition of the data evolves in time. By going through several examples of ultrafast quantum dynamics, we demonstrate that the use of wavelets provide an efficient and accurate way to simultaneously acquire both temporal and frequency information about a signal, and argue that this greatly aids the elucidation and interpretation of physical process responsible for non-stationary spectroscopic features, such as those encountered in coherent excitonic energy transport.
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The elucidation of the mechanisms underpinning chirality-induced spin selectivity remains an outstanding scientific challenge. Here we consider the role of delocalized phonon modes in electron transport in chiral structures and demonstrate that spin selectivity can originate from spin-dependent energy and momentum conservation in electron-phonon scattering events. While this mechanism is robust to the specific nature of the vibrational modes, the degree of spin polarization depends on environmental factors, such as the specific temperature and phonon relaxation rates, as well as the presence of external driving fields. This parametric dependence is used to present experimentally testable predictions of our model.
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We analyze precision bounds for a local phase estimation in the presence of general, non-Markovian phase noise. We demonstrate that the metrological equivalence of product and maximally entangled states that holds under strictly Markovian dephasing fails in the non-Markovian case. Using an exactly solvable model of a physically realistic finite bandwidth dephasing environment, we demonstrate that the ensuing non-Markovian dynamics enables quantum correlated states to outperform metrological strategies based on uncorrelated states using otherwise identical resources. We show that this conclusion is a direct result of the coherent dynamics of the global state of the system and environment and therefore the obtained scaling with the number of particles, which surpasses the standard quantum limit but does not achieve Heisenberg resolution, possesses general validity that goes beyond specific models. This is in marked contrast with the situation encountered under general Markovian noise, where an arbitrarily small amount of noise is enough to restore the scaling dictated by the standard quantum limit.
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We analyze the steady state entanglement generated in a coherently coupled dimer system subject to dephasing noise as a function of the degree of Markovianity of the evolution. By keeping fixed the effective noise strength while varying the memory time of the environment, we demonstrate that non-Markovianity is an essential, quantifiable resource that may support the formation of steady state entanglement whereas purely Markovian dynamics governed by Lindblad master equations lead to separable steady states. This result illustrates possible mechanisms leading to long-lived entanglement in purely decohering, possibly local, environments. We present a feasible experimental demonstration of this noise assisted phenomenon using a system of trapped ions.
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Based entirely upon actual experimental observations on electron-phonon coupling, we develop a theoretical framework to show that the lowest energy band of the Fenna-Matthews-Olson complex exhibits observable features due to the quantum nature of the vibrational manifolds present in its chromophores. The study of linear spectra provides us with the basis to understand the dynamical features arising from the vibronic structure in nonlinear spectra in a progressive fashion, starting from a microscopic model to finally performing an inhomogeneous average. We show that the discreteness of the vibronic structure can be witnessed by probing the diagonal peaks of the nonlinear spectra by means of a relative phase shift in the waiting time resolved signal. Moreover, we demonstrate that the photon-echo and non-rephasing paths are sensitive to different harmonics in the vibrational manifold when static disorder is taken into account. Supported by analytical and numerical calculations, we show that non-diagonal resonances in the 2D spectra in the waiting time, further capture the discreteness of vibrations through a modulation of the amplitude without any effect in the signal intrinsic frequency. This fact generates a signal that is highly sensitive to correlations in the static disorder of the excitonic energy albeit protected against dephasing due to inhomogeneities of the vibrational ensemble.
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Dinámicas no Lineales , Termodinámica , VibraciónRESUMEN
We study the nonequilibrium dynamics of electron transmission from a straight waveguide to a helix with spin-orbit coupling. Transmission is found to be spin-selective and can lead to large spin polarizations of the itinerant electrons. The degree of spin selectivity depends on the width of the interface region, and no polarization is found for single-point couplings. We show that this is due to momentum conservation conditions arising from extended interfaces. We therefore identify interface structure and conservation of momentum as crucial ingredients for chiral-induced spin selectivity, and we confirm that this mechanism is robust against static disorder.
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The sub-Ohmic spin-boson model possesses a quantum phase transition at zero temperature between a localized and a delocalized phase, whose properties have so far only been extracted by numerical approaches. Here we present an extension of the Silbey-Harris variational polaron ansatz which allows us to develop an analytical theory which correctly describes a continuous transition with mean-field exponents for 0
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The unavoidable presence of noise is thought to be one of the major problems to solve in order to pave the way for implementing quantum information technologies in realistic physical platforms. However, here we show a clear example in which noise, in terms of dephasing, may enhance the capability of transmitting not only classical but also quantum information, encoded in quantum systems, through communication networks. In particular, we find analytically and numerically the quantum and classical capacities for a large family of quantum channels and show that these information transmission rates can be strongly enhanced by introducing dephasing noise in the complex network dynamics.
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We address the problem of quantifying the non-markovian character of quantum time evolutions of general systems in contact with an environment. We introduce two different measures of non-markovianity that exploit the specific traits of quantum correlations and are suitable for opposite experimental contexts. When complete tomographic knowledge about the evolution is available, our measure provides a necessary and sufficient condition to quantify strictly the non-markovianity. In the opposite case, when no information whatsoever is available, we propose a sufficient condition for non-markovianity. Remarkably, no optimization procedure underlies our derivation, which greatly enhances the practical relevance of the proposed criteria.