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Jianshu Cao

Publications and source records attributed to Jianshu Cao.

At least 19 recordsLinked to original sources

The Transfer Tensor Method: an Analytical Study Case

The transfer tensor method is a versatile tool for analyzing and propagating general open quantum systems. It captures in a compact manner all memory effects in a non-Markovian system through a straightforward transformation of a set of dynamical maps. Transfer tensors provide the exact convolutional propagator associated with a given time discretization over the past evolution of an open quantum system. Here we show that, for any finite time discretization, the memory kernel of the Nakajima Zwanzig equation deviates from the exact transfer tensors, although both converge in the continuous-time limit, as expected. We examine this behaviour in the context of an analytically solvable model: a two level atom resonant with a lossy cavity in the Jaynes Cummings limit. The atomic dynamics separate into two decoupled degrees of freedom -- the coherence and the population inversion. We derive exact expressions for the dynamical map, the transfer tensors and the memory kernel governing the coherence, and we relate them to their counterparts for the population inversion. As a function of the ratio between the cavity loss rate and the atom-cavity coupling strength, we identify regions of enhanced non-Markovianity in which the system can be described as fully Markovian for certain time-step choices.

quant-ph

First-Passage Time Fluctuation Theorem and Thermodynamic Bound in Cooperative Biomolecular Networks

Using a pathway analysis technique, a dynamic fluctuation relation is derived for a kinetically cooperative biomolecular machine (e.g., an enzyme or a motor protein). This new relation indicates that, in the absence of hidden current, a fluctuation theorem can be established for the first-passage time of the observable process, and we show that this dramatic reduction is a general feature applicable to a wide variety of cooperative networks. This first-passage time fluctuation theorem can be experimentally tested, with its violation serving as a unique signature of hidden detailed balance breaking. Additionally, we obtain a remarkably compact exact expression for the integrated correction to this fluctuation theorem, as well as the general form, revealing a thermodynamic bound on the kinetic branching ratio (i.e., the forward-to-backward observable process probability ratio). These results provide detailed insight into the rich connections between dynamic measurements and the underlying nonequilibrium thermodynamics for cooperative biomolecular machines.

physics.bio-ph

Relation between structure and functionality in photosynthetic antenna complex of green sulfur bacteria: efficiency under natural sunlight pumping

Large-scale simulations of light-matter interaction in natural photosynthetic antenna complexes of the Chlorobium Tepidum green sulfur bacteria (GSB) containing more than one hundred thousand chlorophyll molecules, comparable with natural size, have been performed. Here we have modeled the entire process of the exciton energy transfer, from sunlight absorption to exciton trapping in the reaction centers (RCs) in presence of a thermal bath. The energy transfer has been analyzed using the radiative non-Hermitian Hamiltonian and solving the rate equations for the populations. Sunlight pumping has been modeled as black-body radiation with an attenuation factor that takes the Sun-Earth distance into account. Cylindrical structures typical of GSB antenna complexes, and the dimeric baseplate comparable to natural size have been considered. Our analysis shows that under natural sunlight, in photosynthetic antennae of GSB the number of excitations reaching the RC per unit time matches the RC closure rate and the internal efficiency shows values close to 80%. We also considered cylindrical structures where the orientation of the dipoles does not reflect the natural one. Specifically, we vary continuously the angle of the transition dipole with respect to the cylinder main axis, focusing on the case where all dipoles are parallel to the cylinder axis. We also consider the important case where the dipoles are randomly oriented. In all cases the light-harvesting efficiency is lower than in the natural structure, showing the high sensitivity of light harvesting to the specific orientation of the dipole moments. Our results allow for a better understanding of the relationship between structure and functionality in photosynthetic antennae of GSB and could drive the design of efficient light-harvesting devices.

cond-mat.mes-hall

Noise-enhanced Ballistic Expansion of Polariton Wave-packets in a Multimode Cavity

Advances in optical measurements enable precise tracking of cavity polariton wave-packets across broad spatial and temporal ranges, but how dephasing reshapes their real-space dynamics over multiple time scales remains unclear. Here we show, using a stochastic multimode Tavis-Cummings model, that dephasing noise leads to a robust hierarchy of dynamical regimes comprising Rabi oscillation damping, center-of-mass slowdown, population relaxation, and ballistic-to-diffusive crossover, in the order of increasing time scales. We further predict that dephasing can enhance ballistic spreading and sustain it far beyond the microscopic dephasing time by two orders of magnitude. These predictions agree with recent microscopy measurements and provide experimentally testable guidance for engineering energy transport in polaritonic platforms.

physics.optics

Stochastic Thermodynamics of Cooperative Biomolecular Machines: Fluctuation Relations and Hidden Detailed Balance Breaking

We examine a biomolecular machine involving a driven, observable process coupled to a hidden process in a kinetically cooperative manner. A stochastic thermodynamics framework is employed to analyze a fluctuation theorem for the first-passage time of the observable process under nonequilibrium steady-state conditions. Based on a generic kinetic model, we demonstrate that, along first-passage trajectories, entropy production remains constant when the changes in stochastic entropy and free energy of the machine are balanced, which corresponds to zero net hidden flux through the initial state manifold. Under this condition, which we define quite generally, this first-passage time fluctuation theorem can be established, with its violation serving as an experimentally detectable signature of hidden detailed balance breaking (which we subsequently characterize). In addition, using an enzymatic model, we show that the violation of our first-passage time fluctuation theorem can be thought of as a consequence of the breakdown of local detailed balance in the steps linking coarse-grained states that correspond to the initial and intermediate state manifolds. In the absence of hidden current, the fluctuation theorem is restored, and a mesoscopic local detailed balance condition can be established, which has implications for the thermodynamic analysis of driven, coarse-grained systems. This work sheds significant light on the unique connections between stochastic thermodynamic quantities and kinetic measurements in complex cooperative networks.

cond-mat.stat-mech

Quantum Beatings in Optical Cavities

Cavity polaritons, quasiparticles formed by coherent light-matter coupling, are at the heart of fundamental concepts of quantum optics. The quintessential signature of this coherent coupling is the Rabi oscillation, which results from the neglect of the counter-rotating-wave (CRW) effect in the weak-coupling regime. The goal of this letter is to predict resonant beatings that envelop the Rabi oscillation on the second or higher excitation manifold. These polariton beatings arise from the CRW term in the Dicke or Pauli-Fierz model and are directly correlated with the asymmetry in polariton eigenenergies. Our findings highlight the relevance of the CRW effect even in the weak-coupling regime, offer novel perspectives about coherent polariton dynamics, and shed new light on experiments of coupled quantum systems.

quant-ph

Characterization of Polariton Dynamics in a Multimode Cavity (II): Coherent-Incoherent Transition Driven by Photon Loss

Motivated by the recent advances in optical imaging and tracking of wave-packet propagation in optical cavities, we systematically explore the non-Hermitian polariton dynamics within a decay-tunable multimode cavity model. The complex eigen-spectrum of the model Hamiltonian allows us to predict the incoherent-coherent transition induced by photon losses, which defines an exceptional point at resonance and evolves analytically as the wavevector shifts off-resonantly. The resulting dispersion relation, group velocity, and relaxation rate exhibit striking signatures, such as curve crossing, level repulsion, turnover, bifurcation, and coalescence, as the decay rate crosses the critical transition or the wavevector crosses the resonance. The spectral characterization leads to surprising features in the non-Hermitian wave packet dynamics: (i) maximal population relaxation rate at the critical transition; (ii) reversed propagation in the center-of-mass motion; (iii) ballistic-to-diffusion transition; (iv) contraction in the displacement and width of the polariton wave-packet. These dynamical features have complementary symmetry between the upper-polariton (UP) branch and lower-polariton (LP) branch in the two-dimensional phase diagram spanned by the photon decay rate and wavevector. Thus, the combination of complex spectral characterization and non-Hermitian wave packet propagation establishes the photon decay rate as a powerful control parameter for polariton transport, reveals the underlying symmetry in lossy cavities, and presents a starting point to incorporate other dissipative mechanisms.

quant-ph

Dynamical generation and transfer of nonclassical states in strongly interacting light-matter systems in cavities

We propose leveraging strong and ultrastrong light-matter coupling to efficiently generate and exchange nonclassical light and quantum matter states. Two initial conditions are considered: (a) a displaced quadrature-squeezed matter state, and (b) a coherent state in a cavity. In both scenarios, polaritons mediate the dynamical generation and transfer of nonclassical states between light and matter. By monitoring the dynamics of both subsystems, we uncover the emergence of beatings in the collective matter oscillations. The beating period depends on the particle density through the vacuum Rabi splitting and peaks sharply under light-matter resonance conditions. For initial condition (a), nonclassicality is efficiently transferred from matter to photons under strong and ultrastrong coupling. However, for initial condition (b), nonclassical photonic states are generated only in the ultrastrong coupling regime due to the counter-rotating terms, highlighting the advantages of ultrastrong coupling. Furthermore, in the ultrastrong coupling regime, distinctive asymmetries relative to cavity detuning emerge in dynamical observables of both light and matter. The nonclassical photons can be extracted through a semi-transparent cavity mirror, while nonclassical matter states can be detected via time-resolved spectroscopy. This work highlights that hybrid polariton states can be utilized for dynamically generating nonclassical states, with potential applications in quantum state transfer.

quant-ph

Unusual Diffusivity in Strongly Disordered Quantum Lattices: Random Dimer Model

Recent advances in transport properties measurements of disordered materials and lattice simulations, using superconducting qubits, have rekindled interest in Anderson localization, motivating our study of highly disordered quantum lattices. Initially, our statistical analysis of localized eigenstates reveals a distinct transition between weak and strong disorder regimes, suggesting a random distribution of dimers in highly disordered systems. Subsequently, the random dimer model predicts an oscillating diffusivity that decays as $t^{-1/2}$, is inversely proportional to the disorder strength, and maintains a constant frequency with an initial phase shift of $π/4$. The first peak exhibits a universal scaling of $σ^{-1}$ both in peak time and amplitude. Finally, we find that stochastic noise suppresses these oscillations and induces hopping between localized eigenstates, resulting in constant diffusion over long times. Our predictions challenge the conventional understanding of incoherent hopping under strong disorder. This offers new insights to optimize disordered systems for optoelectrical and quantum information technologies.

quant-ph

Extracting Kinetic Information from Short-Time Trajectories: Relaxation and Disorder of Lossy Cavity Polaritons

The emerging field of molecular cavity polaritons has stimulated a surge of experimental and theoretical activities and presents a unique opportunity to develop the many-body simulation methodology. This paper presents a numerical scheme for the extraction of key kinetic information of lossy cavity polaritons based on the transfer tensor method (TTM). Steady state, relaxation timescales and oscillatory phenomena can all be deduced directly from a set of transfer tensors without the need for long-time simulation. Moreover, we generalize TTM to disordered systems by sampling dynamical maps and achieve fast convergence to disordered-averaged dynamics using a small set of realizations. Together, these techniques provide a toolbox for characterizing the interplay of cavity loss, disorder, and cooperativity in polariton relaxation and allow us to predict unusual dependences on the initial excitation state, photon decay rate, strength of disorder, and the type of cavity models. Thus, we have demonstrated significant potential in the use of the TTM towards both the efficient computation of long-time polariton dynamics and the extraction of crucial kinetic information about polariton relaxation from a small set of short-time trajectories.

quant-ph

Coherent spatial control of wave packet dynamics on quantum lattices

Quantum lattices are pivotal in the burgeoning fields of quantum materials and information science. Rapid developments in microscopy and quantum engineering allow for preparing and monitoring wave-packet dynamics on quantum lattices with increasing spatial and temporal resolution. Motivated by these emerging research interests, we present an analytical study of wave packet diffusivity and diffusion length on tight-binding quantum lattices subject to stochastic noise. Our analysis points to the crucial role of spatial coherence and predicts a set of novel phenomena: noise can enhance the transient diffusivity and diffusion length of sufficiently extended initial states; A smooth Gaussian initial state spreads slower than a localized initial state; A standing or traveling initial state with large momentum spreads faster than a localized initial state and exhibits a noise-induced peak in the transient diffusivity; The change in the time-dependent diffusivity and diffusion length relative to a localized initial state follows a universal dependence on the Gaussian width. These theoretical predictions and the underlying mechanism of spatial coherence suggest the possibility of controlling the wave packet dynamics on quantum lattices by spatial manipulations, which will have implications for materials science and quantum technologies.

quant-ph

Cavity-Induced Quantum Interference and Collective Interactions in van der Waals Systems

The central topic of this letter is to show that light-matter hybridization not only gives rise to novel dynamic responses but can also modify intermolecular interactions and induce new structural order. Using the van der Waals (vdW) system in an optical cavity as an example, we predict the effects of interference and collectivity in cavity-induced many-body dispersion interactions. Specifically, the leading order correction due to cavity-induced quantum fluctuations leads to 3-body and 4-body vdW interactions, which can align intermolecular vectors and are not pairwise additive. In addition, the cavity-induced dipole leads to a single-molecule energy shift that aligns individual molecules, and a pair-wise interaction that scales as $R^{-3}$ instead of the standard $R^{-6}$ distance scaling. The coefficients of all these cavity-induced corrections depend on the cavity frequency and are renormalized by the effective Rabi frequency, which in turn depends on the particle density. Finally, we study the interaction of the vdW system in a cavity with an external object and find a significant enhancement in the interaction range due to modified distance scaling laws. These theoretical predictions suggest the possibility of cavity-induced nematic or smectic order and may provide an essential clue to understanding intriguing phenomena observed in optical cavities, such as strongly-modified ground-state reactivity, ion transport and solvent polarity.

quant-ph

Polariton Localization and Dispersion Properties of Disordered Quantum Emitters in Multimode Microcavities

Experiments have demonstrated that the strong light-matter coupling in polaritonic microcavities significantly enhances transport. Motivated by these experiments, we have solved the disordered multimode Tavis-Cummings model in the thermodynamic limit and used this solution to analyze its dispersion and localization properties. The solution implies that wave-vector-resolved spectroscopic quantities can be described by single-mode models, but spatially resolved quantities require the multimode solution. Nondiagonal elements of the Green's function decay exponentially with distance, which defines the coherence length. The coherence length is strongly correlated with the photon weight and exhibits inverse scaling with respect to the Rabi frequency and an unusual dependence on disorder. For energies away from the average molecular energy $E_{\text{M}}$ and above the confinement energy $E_C$, the coherence length rapidly diverges such that it exceeds the photon resonance wavelength $λ_0$. The rapid divergence allows us to differentiate the localized and delocalized regimes and identify the transition from diffusive to ballistic transport.

physics.optics

Dynamical symmetries of periodically-driven quantum systems and their spectroscopic signatures

Spatial symmetries of quantum systems leads to important effects in spectroscopy, such as selection rules and dark states. Motivated by the increasing strength of light-matter interaction achieved in recent experiments, we investigate a set of dynamically-generalized symmetries for quantum systems, which are subject to a strong periodic driving. Based on Floquet response theory, we study rotational, particle-hole, chiral and time-reversal symmetries and their signatures in spectroscopy, including symmetry-protected dark states (spDS), a Floquet band selection rule (FBSR), and symmetry-induced transparency (siT). Specifically, a dynamical rotational symmetry establishes dark state conditions, as well as selection rules for inelastic light scattering processes; a particle-hole symmetry introduces dark states for symmetry related Floquet states and also a transparency effect at quasienergy crossings; chiral symmetry and time-reversal symmetry alone do not imply dark state conditions, but can be combined to the particle-hole symmetry. Our predictions reveal new physical phenomena when a quantum system reaches the strong light-matter coupling regime, important for superconducting qubits, atoms and molecules in optical or plasmonic field cavities, and optomechanical systems.

quant-ph

Higher-Order Photon Statistics as a New Tool to Reveal Hidden Excited States in a Plasmonic Cavity

Among the best known quantities obtainable from photon correlation measurements are the $g^{(m)}$~correlation functions. Here, we introduce a new procedure to evaluate these correlation functions based on higher-order factorial cumulants $C_{\text{F},m}$ which integrate over the time dependence of the correlation functions, i.e., summarize the available information at different time spans. In a systematic manner, the information content of higher-order correlation functions as well as the distribution of photon waiting times is taken into account. Our procedure greatly enhances the sensitivity for probing correlations and, moreover, is robust against a limited counting efficiency and time resolution in experiment. It can be applied even in case $g^{(m)}$ is not accessible at short time spans. We use the new evaluation scheme to analyze the photon emission of a plasmonic cavity coupled to a single quantum dot. We derive criteria which must hold if the system can be described by a generic Jaynes-Cummings model. A violation of the criteria can be explained by the presence of an additional excited quantum dot state.

cond-mat.mes-hall

Long-Range Non-Equilibrium Coherent Tunneling Induced by Fractional Vibronic Resonances

We study the influence of a linear energy bias on a non-equilibrium excitation on a chain of molecules coupled to local phonons (a tilted Holstein model) using both a random-walk rate kernel theory and a nonperturbative, massively parallelized adaptive-basis algorithm. We uncover structured and discrete vibronic resonance behavior fundamentally different from both linear response theory and homogeneous polaron dynamics. Remarkably, resonance between the phonon energy $\hbarω$ and the bias $δ_ε$ occurs not only at integer but also fractional ratios $δ_ε/(\hbarω) = \frac{m}{n}$, which effect long-range $n$-bond $m$-phonon tunneling. These observations are also reproduced in a model calculation of a recently demonstrated Cy3 system. Potential applications range from molecular electronics to optical lattices and artificial light harvesting via vibronic engineering of coherent quantum transport.

quant-ph

Unusual Dynamical Properties of Disordered Polaritons in Micocavities

The strong light-matter interaction in microcavities gives rise to intriguing phenomena, such as cavity-mediated transport that can potentially overcome the Anderson localization. Yet, an accurate theoretical treatment is challenging as the matter (e.g.,molecules) are subject to large energetic disorder. In this article, we develop the Green's function solution to the Fano-Anderson model and use the exact analytical solution to quantify the effects of energetic disorder on the spectral and transport properties in microcavities. Starting from microscopic equation of motions, we derive an effective non-Hermitian Hamiltonian and predict a set of scaling laws: (i) The complex eigen-energies of the effective Hamiltonian exhibit an exceptional point, which leads to underdamped coherent dynamics in the weak disorder regime, where the decay rate increases with disorder, and overdamped incoherent dynamics in the strong disorder regime, where the slow decay rate decreases with disorder. (ii) The total density of states of disordered ensembles can be exactly partitioned into the cavity, bright-state and dark-state local density of states, which are determined by the complex eigen solutions and can be measured via spectroscopy. (iii) The cavity-mediated relaxation and transport dynamics are intimately related such that the energy-resolved relaxation and transport rates are proportional to the cavity local density of states. The ratio of the disorder averaged relaxation and transport rates equals the molecule number, which can be interpreted as a result of a quantum random walk. (iv) A turnover in the rates as a function of disorder or molecule density can be explained in terms of the overlap of the disorder distribution function and the cavity local density of states. These findings reveal the significant impact of the dark states on the transport properties of disordered ensembles in cavities.

quant-ph

Generalized resonance energy transfer theory: Applications to vibrational energy flow in optical cavities

A general rate theory for resonance energy transfer is formulated to incorporate any degrees of freedom (e.g., rotation, vibration, exciton, and polariton) as well as coherently-coupled composite states. The compact rate expression allows us to establish useful relationships: (i) detailed balance condition when the donor and acceptor are at the same temperature; (ii) proportionality to the overlap between donor's emission and acceptor's absorption spectra; (iii) scaling with the effective coherent size, i.e., the number of coherently coupled molecules; (iv) spatial and orientational dependences as derived from the interaction potential. When applied to cavity-assisted vibrational energy transfer, the rate formalism provides an intuitive and quantitative explanation of intriguing phenomena such as cooperativity, resonance, and nonlinearity in the collective vibrational strong coupling regime, as demonstrated in recent simulations.

physics.chem-ph