arXiv subjects

Jianshu Cao

Publications and source records attributed to Jianshu Cao.

At least 55 records · Page 3Linked to original sources

arXiv2017

Unifying quantum heat transfer in a nonequilibrium spin-boson model with full counting statistics

To study the full counting statistics of quantum heat transfer in a driven nonequilibrium spin-boson model, we develop a generalized nonequilibrium polaron-transformed Redfield equation with an auxiliary counting field. This enables us to study the impact of qubit-bath coupling ranging from weak to strong regimes. Without external modulations, we observe maximal values of both steady state heat flux and noise power at moderate coupling regimes, below which we find those two transport quantities are enhanced by the finite qubit energy bias. With external modulations, the geometric-phase-induced heat flux shows monotonic decrease as increasing the qubit-bath coupling at zero qubit energy bias (without bias). While under finite qubit energy bias (with bias), the geometric-phase-induced heat flux exhibits an interesting reversal behavior in strong coupling regime. Our results unify the seemingly contradictory results in weak and strong qubit-bath coupling regimes, and provide detailed dissections for the quantum fluctuation of nonequilibrium heat transfer.

cond-mat.mes-hall↗

arXiv2017

A Unified Stochastic Formulation of Dissipative Quantum Dynamics. I. Generalized Hierarchical Equations

We extend a standard stochastic theory to study open quantum systems coupled to generic quantum environments including the three fundamental classes of noninteracting particles: bosons, fermions and spins. In this unified stochastic approach, the generalized stochastic Liouville equation (SLE) formally captures the exact quantum dissipations when noise variables with appropriate statistics for different bath models are applied. Anharmonic effects of a non-Gaussian bath are precisely encoded in the bath multi-time correlation functions that noise variables have to satisfy. Staring from the SLE, we devise a family of generalized hierarchical equations by averaging out the noise variables and expand bath multi-time correlation functions in a complete basis of orthonormal functions. The general hiearchical equations constitute systems of linear equations that provide numerically exact simulations of quantum dynamics. For bosonic bath models, our general hierarchical equation of motion reduces exactly to an extended version of hierarchical equation of motion which allows efficient simulation for arbitrary spectral densities and temperature regimes. Similar efficiency and exibility can be achieved for the fermionic bath models within our formalism. The spin bath models can be simulated with two complementary approaches in the presetn formalism. (I) They can be viewed as an example of non-Gaussian bath models and be directly handled with the general hierarchical equation approach given their multi-time correlation functions. (II) Alterantively, each bath spin can be first mapped onto a pair of fermions and be treated as fermionic environments within the present formalism.

physics.chem-ph↗

arXiv2017

A Unified Stochastic Formulation of Dissipative Quantum Dynamics. II. Beyond Linear Response of Spin Baths

We use the "generalized hierarchical equation of motion" proposed in Paper I to study decoherence in a system coupled to a spin bath. The present methodology allows a systematic incorporation of higher order anharmonic effects of the bath in dynamical calculations. We investigate the leading order corrections to the linear response approximations for spin bath models. Two types of spin-based environments are considered: (1) a bath of spins discretized from a continuous spectral density and (2) a bath of physical spins such as nuclear or electron spins. The main difference resides with how the bath frequency and the system-bath coupling parameters are chosen to represent an environment. When discretized from a continuous spectral density, the system-bath coupling typically scales as $\sim 1/\sqrt{N_B}$ where $N_B$ is the number of bath spins. This scaling suppresses the non-Gaussian characteristics of the spin bath and justify the linear response approximations in the thermodynamic limit. For the physical spin bath models, system-bath couplings are directly deduced from spin-spin interactions with no reason to obey the $1/\sqrt{N_B}$ scaling. It is not always possible to justify the linear response approximations. Furthermore, if the spin-spin Hamiltonian and/or the bath parameters are highly symmetrical, these additional constraints generate non-Markovian and persistent dynamics that is beyond the linear response treatments.

physics.chem-ph↗

arXiv2017

Construction of Multi-Chromophoric Spectra from Monomer Data: Applications to Resonant Energy Transfer

We develop a model that establishes a quantitative link between the physical properties of molecular aggregates and their constituent building blocks. The relation is built on the coherent potential approximation, calibrated against exact results, and proven reliable for a wide range of parameters. It provides a practical method to compute spectra and transfer rates in multi-chromophoric systems from experimentally accessible monomer data. Applications to Förster energy transfer reveal optimal transfer rates as functions of both the system-bath coupling and intra-aggregate coherence.

physics.chem-ph↗

arXiv2016

Dynamical signatures of molecular symmetries in nonequilibrium quantum transport

Symmetries play a crucial role in ubiquitous systems found in Nature. In this work, we propose an elegant approach to detect symmetries by measuring quantum currents. Our detection scheme relies on initiating the system in an anti-symmetric initial condition, with respect to the symmetric sites, and using a probe that acts like a local noise. Depending on the position of the probe the currents exhibit unique signatures such as a quasi-stationary plateau indicating the presence of meta-stability and multi-exponential decays in case of multiple symmetries. The signatures are sensitive to the probe and vanish completely when the timescale of the coherent system dynamics is much longer than the timescale of the probe. These results are demonstrated using a $4$-site model and an archetypal example of the para-benzene ring and are shown to be robust under a weak disorder.

cond-mat.stat-mech↗

arXiv2016

Quantum transport in d-dimensional lattices

We prove analytically that both fermionic and bosonic uniform d-dimensional lattices can be reduced to a set of independent one-dimensional modes. This reduction leads to the conclusion that the dynamics in uniform fermionic and bosonic lattices is always ballistic. By the use of the Jordan-Wigner transformation we extend our analysis to spin lattices, proving the existence of both ballistic and non-ballistic subspaces in any dimension and for any system size. We then relate the nature of transport with the number of excitations in the spin lattice, indicating that a single excitation propagates always ballistically and that the non-ballistic behavior of uniform spin lattices is a consequence of the interaction between different excitations.

quant-ph↗

arXiv2016

How two-dimensional brick layer J-aggregates differ from linear ones: excitonic properties and line broadening mechanisms

We study the excitonic coupling and homogeneous spectral line width of brick layer J-aggregate films. We begin by analysing the structural information revealed by the two-exciton states probed in two-dimensional spectra. Our first main result is that the relation between the excitonic couplings and the spectral shift in a two-dimensional structure is different (larger shift for the same nearest neighbour coupling) from that in a one-dimensional structure, which leads to an estimation of dipolar coupling in two-dimensional lattices. We next investigate the mechanisms of homogeneous broadening - population relaxation and pure dephasing - and evaluate their relative importance in linear and two-dimensional aggregates. Our second main result is that pure dephasing dominates the line width in two-dimensional systems up to a crossover temperature, which explains the linear temperature dependence of the homogeneous line width. This is directly related to the decreased density of states at the band edge when compared with linear aggregates, thus reducing the contribution of population relaxation to dephasing. Pump-probe experiments are suggested to directly measure the lifetime of the bright state and can therefore support the proposed model.

physics.chem-ph↗

arXiv2016

Efficient simulation of non-Markovian system-environment interaction

In this work, we combine an established method for open quantum systems -- the time evolving density matrix using orthogonal polynomials algorithm (TEDOPA) -- with the transfer tensors formalism (TTM), a new tool for the analysis, compression and propagation of non-Markovian processes. This enables the investigation of previously inaccessible long-time dynamics, such as those ensuing from low temperature regimes with arbitrary, possibly highly structured, spectral densities. We briefly introduce both methods, followed by a benchmark to prove viability and combination synergies. Subsequently we illustrate the capabilities of this approach at the hand of specific examples and conclude our analysis by highlighting possible further applications of our method.

quant-ph↗

arXiv2016

Quantum Diffusion on Molecular Tubes: Universal Scaling of the 1D to 2D Transition

The transport properties of disordered systems are known to depend critically on dimensionality. We study the diffusion coefficient of a quantum particle confined to a lattice on the surface of a tube, where it scales between the 1D and 2D limits. It is found that the scaling relation is universal and independent of the disorder and noise parameters, and the essential order parameter is the ratio between the localization length in 2D and the circumference of the tube. Phenomenological and quantitative expressions for transport properties as functions of disorder and noise are obtained and applied to real systems: In the natural chlorosomes found in light-harvesting bacteria the exciton transfer dynamics is predicted to be in the 2D limit, whereas a family of synthetic molecular aggregates is found to be in the homogeneous limit and is independent of dimensionality.

cond-mat.mes-hall↗

arXiv2015

Non-Markovian Dynamical Maps: Numerical Processing of Open Quantum Trajectories

The initial stages of the evolution of an open quantum system encode the key information of its underlying dynamical correlations, which in turn can predict the trajectory at later stages. We propose a general approach based on non-Markovian dynamical maps to extract this information from the initial trajectories and compress it into non-Markovian transfer tensors. Assuming time-translational invariance, the tensors can be used to accurately and efficiently propagate the state of the system to arbitrarily long timescales. The non-Markovian Transfer Tensor Method (TTM) demonstrates the coherent-to-incoherent transition as a function of the strength of quantum dissipation and predicts the non-canonical equilibrium distribution due to the system-bath entanglement. TTM is equivalent to solving the Nakajima-Zwanzig equation, and therefore can be used to reconstruct the dynamical operators (the system Hamiltonian and memory kernel) from quantum trajectories obtained in simulations or experiments. The concept underlying the approach can be generalized to physical observables with the goal of learning and manipulating the trajectories of an open quantum system.

quant-ph↗

arXiv2015

Effects of system-bath entanglement on the performance of light-harvesting systems: A quantum heat engine perspective

We explore energy transfer in a generic three-level system, which is coupled to three non-equilibrium baths. Built on the concept of quantum heat engine, our three-level model describes non-equilibrium quantum processes including light-harvesting energy transfer, nano-scale heat transfer, photo-induced isomerization, and photovoltaics in double quantum-dots. In the context of light-harvesting, the excitation energy is first pumped up by sunlight, then is transferred via two excited states which are coupled to a phonon bath, and finally decays to the ground state. The efficiency of this process is evaluated by steady state analysis via a polaron-transformed master equation; thus a wide range of the system-phonon coupling strength can be covered. We show that the coupling with the phonon bath not only modifies the steady state, resulting in population inversion, but also introduces a finite steady state coherence which optimizes the energy transfer flux and efficiency. In the strong coupling limit, the steady state coherence disappears and the efficiency approaches the heat engine limit given by Scovil and Schultz-Dubois in Phys. Rew. Lett. 2, 262 (1959).

quant-ph↗

arXiv2015

Stiffening of Red Blood Cells Induced by Disordered Cytoskeleton Structures: A Joint Theory-experiment Study

The functions and elasticities of the cell are largely related to the structures of the cytoskeletons underlying the lipid bi-layer. Among various cell types, the Red Blood Cell (RBC) possesses a relatively simple cytoskeletal structure. Underneath the membrane, the RBC cytoskeleton takes the form of a two dimensional triangular network, consisting of nodes of actins (and other proteins) and edges of spectrins. Recent experiments focusing on the malaria infected RBCs (iRBCs) showed that there is a correlation between the elongation of spectrins in the cytoskeletal network and the stiffening of the iRBCs. Here we rationalize the correlation between these two observations by combining the worm-like chain (WLC) model for single spectrins and the Effective Medium Theory (EMT) for the network elasticity. We specifically focus on how the disorders in the cytoskeletal network affect its macroscopic elasticity. Analytical and numerical solutions from our model reveal that the stiffness of the membrane increases with increasing end-to-end distances of spectrins, but has a non-monotonic dependence on the variance of the end-to-end distance distributions. These predictions are verified quantitively by our AFM and micropipette aspiration measurements of iRBCs. The model may, from a molecular level, provide guidelines for future identification of new treatment methods for RBC related diseases, such as malaria infection.

physics.bio-ph↗

arXiv2015

A Continued Fraction Resummation Form of Bath Relaxation Effect in the Spin-Boson Model

In the spin-boson model, a continued fraction form is proposed to systematically resum high-order quantum kinetic expansion (QKE) rate kernels, accounting for the bath relaxation effect beyond the second-order perturbation. In particular, the analytical expression of the sixth-order QKE rate kernel is derived for resummation. With higher-order correction terms systematically extracted from higher-order rate kernels, the resummed quantum kinetic expansion (RQKE) approach in the continued fraction form extends the Pade approximation and can fully recover the exact quantum dynamics as the expansion order increases.

quant-ph↗

arXiv2015

Forster resonance energy transfer, absorption and emission spectra in multichromophoric systems: III. Exact stochastic path integral evaluation

A numerically exact path integral treatment of the absorption and emission spectra of open quantum systems is presented that requires only the straightforward solution of a stochastic differential equation. The approach converges rapidly enabling the calculation of spectra of large excitonic systems across the complete range of system parameters and for arbitrary bath spectral densities. With the numerically exact absorption and emission operators one can also immediately compute energy transfer rates using the multi-chromophoric Forster resonant energy transfer formalism. Benchmark calculations on the emission spectra of two level systems are presented demonstrating the efficacy of the stochastic approach. This is followed by calculations of the energy transfer rates between two weakly coupled dimer systems as a function of temperature and system-bath coupling strength. It is shown that the recently developed hybrid cumulant expansion is the only perturbative method capable of generating uniformly reliable energy transfer rates and spectra across a broad range of system parameters.

physics.chem-ph↗

arXiv2014

Coherent exciton dynamics in the presence of underdamped vibrations

Recent ultrafast optical experiments show that excitons in large biological light-harvesting complexes are coupled to molecular vibration modes. These high-frequency vibrations will not only affect the optical response, but also drive the exciton transport. Here, using a model dimer system, the frequency of the underdamped vibration is shown to have a strong effect on the exciton dynamics such that quantum coherent oscillations in the system can be present even in the case of strong noise. Two mechanisms are identified to be responsible for the enhanced transport efficiency: critical damping due to the tunable effective strength of the coupling to the bath, and resonance coupling where the vibrational frequency coincides with the energy gap in the system. The interplay of these two mechanisms determines parameters responsible for the most efficient transport, and these optimal control parameters are comparable to those in realistic light-harvesting complexes. Interestingly, oscillations in the excitonic coherence at resonance are suppressed in comparison to the case of an off-resonant vibration.

quant-ph↗

arXiv2014

Coherent quantum transport in disordered systems: A unified polaron treatment of hopping and band-like transport

Quantum transport in disordered systems is studied using a polaron-based master equation. The polaron approach is capable of bridging the results from the coherent band-like transport regime governed by the Redfield equation to incoherent hopping transport in the classical regime. A non-monotonic dependence of the diffusion coefficient is observed both as a function of temperature and system-phonon coupling strength. In the band-like transport regime, the diffusion coefficient is shown to be linearly proportional to the system-phonon coupling strength, and vanishes at zero coupling due to Anderson localization. In the opposite classical hopping regime, we correctly recover that the dynamics are described by the Fermi's Golden Rule (FGR) and establish that the scaling of the diffusion coefficient depends on the phonon bath relaxation time. In both the hopping and band-like transport regimes, it is demonstrated that at low temperature the zero-point fluctuations of the bath lead to non-zero transport rates, and hence a finite diffusion constant. Application to rubrene and other organic semiconductor materials shows a good agreement with experimental mobility data.

cond-mat.mes-hall↗

arXiv2014

Nonequilibrium Energy Transfer at Nanoscale: A Unified Theory from Weak to Strong Coupling

We investigate the microscopic mechanism of quantum energy transfer in the nonequilibrium spin-boson model. By developing a nonequilibrium polaron-transformed Redfield equation based on fluctuation decoupling, we dissect the energy transfer into multi-boson associated processes with even or odd parity. Based on this, we analytically evaluate the energy flux, which smoothly bridges the transfer dynamics from the weak spin-boson coupling regime to the strong-coupling one. Our analysis explains previous limiting predictions and provides a unified interpretation of several observations, including coherence-enhanced heat flux and absence of negative differential thermal conductance in the nonequilibrium spin-boson model. The results may find wide applications for the energy and information control in nanodevices.

cond-mat.mes-hall↗

arXiv2014

Can Natural Sunlight Induce Coherent Exciton Dynamics?

Excitation of a model photosynthetic molecular aggregate by incoherent sunlight is systematically examined. For a closed system, the excited state coherence induced by the sunlight oscillates with an average amplitude that is inversely proportional to the excitonic gap, and reaches a stationary amplitude that depends on the temperature and coherence time of the radiation field. For an open system, the light-induced dynamical coherence relaxes to a static coherence determined by the non-canonical thermal distribution resulting from the entanglement with the phonon bath. The decay of the excited state population to the common ground state establishes a non-equilibrium steady-state flux driven by the sunlight, and it defines a time window to observe the transition from dynamical to static coherence. For the parameters relevant to photosynthetic systems, the exciton dynamics initiated by the sunlight exhibits a non-negligible amount of dynamical coherence (quantum beats) on the sub-picosecond timescale; however, this sub-picosecond time-scale is long enough for light-harvesting systems to establish static coherence, which plays a crucial role in efficient energy transfer. Further, a relationship is established between the non-equilibrium steady-state induced by the sunlight and the coherent dynamics initiated from the ground state by a laser $δ$-pulse, thereby making a direct connection between incoherent sunlight excitation and ultrafast spectroscopy.

physics.chem-ph↗