arXiv subjects

Lipeng Chen

Publications and source records attributed to Lipeng Chen.

51 records · Page 3Linked to original sources

arXiv2021

Simulation of absorption spectra of molecular aggregates: a Hierarchy of Stochastic Pure States approach

The simulation of spectroscopic observables for molecular aggregates with strong and structured coupling of electronic excitation to vibrational degrees of freedom is an important but challenging task. The hierarchy of pure states (HOPS) provides a formally exact solution based on local, stochastic trajectories. Exploiting the localization of HOPS for the simulation of absorption spectra in large aggregares requires a formulation in terms of normalized trajectories. Here we provide a normalized dyadic equation where the ket- and bra-states are propagated in different electronic Hilbert spaces. This work opens the door to apply adaptive HOPS methods for the simulation of absorption spectra and also to a formulation for non-linear spectroscopy that is perturbative with respect to interactions with the electric field.

quant-ph↗

arXiv2021

Effects of high pulse intensity and chirp in two-dimensional electronic spectroscopy of an atomic vapor

The effects of high pulse intensity and chirp on two-dimensional electronic spectroscopy signals are experimentally investigated in the highly non-perturbative regime using atomic rubidium vapor as clean model system. Data analysis is performed based on higher-order Feynman diagrams and non-perturbative numerical simulations of the system response. It is shown that higher-order contributions may lead to a fundamental change of the static appearance and beating-maps of the 2D spectra and that chirped pulses enhance or suppress distinct higher-order pathways. We further give an estimate of the threshold intensity beyond which the high-intensity effects become visible for the system under consideration.

physics.optics↗

arXiv2021

Disentangling Dynamical Quantum Coherences in the Fenna-Matthews-Olson Complex

In the primary step of light-harvesting, the energy of a photon is captured in antenna chlorophyll as an exciton. Its efficient conversion to stored chemical potential occurs in the special pair reaction center, which has to be reached by down-hill ultrafast excited state energy transport. The interaction between the chromophores leads to spatial delocalization and quantum coherence effects, the importance of which depends on the coupling between the chlorophylls in relation to the intensity of the fluctuations and reorganization dynamics of the protein matrix, or bath. The latter induce uncorrelated modulations of the site energies, and thus quantum decoherence, and localization of the exciton. Current consensus is that under physiological conditions quantum decoherence occurs on the 10 fs time scale, and quantum coherence plays little role for the observed picosecond energy transfer dynamics. In this work, we reaffirm this from a different point of view by finding that the true onset of electronic quantum coherence only occurs at extremely low temperatures of ~20 K. We have directly determined the exciton coherence times by two-dimensional electronic spectroscopy of the Fenna-Matthew-Olson complex over an extensive temperature range with a supporting theoretical modelling. At 20 K, electronic coherences persist out to 200 fs (close to the antenna) and marginally up to 500 fs at the reaction-center side. It decays markedly faster with modest increases in temperature to become irrelevant above 150 K. This temperature dependence also allows disentangling the previously reported long-lived beatings. We show that they result from mixing vibrational coherences in the electronic ground state ...

cond-mat.other↗

arXiv2020

Improving Redundancy Availability: Dynamic Subtasks Modulation for Robots with Redundancy Insufficiency

This work presents an approach for robots to suitably carry out complex applications characterized by the presence of multiple additional constraints or subtasks (e.g. obstacle and self-collision avoidance) but subject to redundancy insufficiency. The proposed approach, based on a novel subtask merging strategy, enforces all subtasks in due course by dynamically modulating a virtual secondary task, where the task status and soft priority are incorporated to improve the overall efficiency of redundancy resolution. The proposed approach greatly improves the redundancy availability by unitizing and deploying subtasks in a fine-grained and compact manner. We build up our control framework on the null space projection, which guarantees the execution of subtasks does not interfere with the primary task. Experimental results on two case studies are presented to show the performance of our approach.

cs.RO↗

arXiv2020

Variational approach to time-dependent fluorescence of a driven qubit

We employ the Dirac-Frenkel variational principle and multiple Davydov ansatz to study time-dependent fluorescence spectra of a driven qubit in the weak- to strong qubit-reservoir coupling regimes, where both the Rabi frequency and spontaneous decay rate are comparable to the transition frequency of the qubit. Our method agrees well with the time-local master-equation approach in the weak-coupling regime, and offers a flexible way to compute the spectra from the bosonic dynamics instead of two-time correlation functions. While the perturbative master equation breaks down in the strong-coupling regime, our method actually becomes more accurate due to the use of bosonic coherent states under certain conditions. We show that the counter-rotating coupling between the qubit and the reservoir has considerable contributions to the photon number dynamics and the spectra under strong driving conditions even though the coupling is moderately weak. The time-dependent spectra are found to be generally asymmetric, a feature that is derived from photon number dynamics. In addition, it is shown that the spectral profiles can be dramatically different from the Mollow triplet due to strong dissipation and/or multiphoton processes associated with the strong driving. Our formalism provides a unique perspective to interpret time-dependent spectra.

quant-ph↗

arXiv2019

Fast, accurate simulation of polaron dynamics and multidimensional spectroscopy by multiple Davydov trial states

By employing the Dirac-Frenkel time-dependent variational principle, we study the dynamical properties of the Holstein molecular crystal model with diagonal and off-diagonal exciton-phonon coupling. A linear combination of the Davydov D$_1$ (D$_2$) Anstaz, referred to as the multi-D$_1$ Ansatz (multi-D$_2$ Ansatz), is used as the trial state with enhanced accuracy but without sacrificing efficiency. The time evolution of the exciton probability is found to be in perfect agreement with that of the hierarchy equations of motion, demonstrating the promise the multiple Davydov trial states hold as an efficient, robust description of dynamics of complex quantum systems. In addition to the linear absorption spectra computed for both diagonal and off-diagonal cases, for the first time, $2$D spectra have been calculated for systems with off-diagonal exciton-phonon coupling by employing the multiple $D_2$ Ansatz to compute the nonlinear response function, testifying to the great potential of the multiple $D_2$ Ansatz for fast, accurate implementation of multidimensional spectroscopy. It is found that the signal exhibits a single peak for weak off-diagonal coupling, while a vibronic multi-peak structure appears for strong off-diagonal coupling.

cond-mat.stat-mech↗

arXiv2018

Planning for Muscular and Peripersonal-Space Comfort during Human-Robot Forceful Collaboration

This paper presents a planning algorithm designed to improve cooperative robot behavior concerning human comfort during forceful human-robot physical interaction. Particularly, we are interested in planning for object grasping and positioning ensuring not only stability against the exerted human force but also empowering the robot with capabilities to address and improve human experience and comfort. Herein, comfort is addressed as both the muscular activation level required to exert the cooperative task, and the human spatial perception during the interaction, namely, the peripersonal space. By maximizing both comfort criteria, the robotic system can plan for the task (ensuring grasp stability) and for the human (improving human comfort). We believe this to be a key element to achieve intuitive and fluid human-robot interaction in real applications. Real HRI drilling and cutting experiments illustrated the efficiency of the proposed planner in improving overall comfort and HRI experience without compromising grasp stability.

cs.RO↗

arXiv2018

Manipulation Planning under Changing External Forces

In this work, we present a manipulation planning algorithm for a robot to keep an object stable under changing external forces. We particularly focus on the case where a human may be applying forceful operations, e.g. cutting or drilling, on an object that the robot is holding. The planner produces an efficient plan by intelligently deciding when the robot should change its grasp on the object as the human applies the forces. The planner also tries to choose subsequent grasps such that they will minimize the number of regrasps that will be required in the long-term. Furthermore, as it switches from one grasp to the other, the planner solves the problem of bimanual regrasp planning, where the object is not placed on a support surface, but instead it is held by a single gripper until the second gripper moves to a new position on the object. This requires the planner to also reason about the stability of the object under gravity.We provide an implementation on a bimanual robot and present experiments to show the performance of our planner.

cs.RO↗

arXiv2017

Transient dynamics of a one-dimensional Holstein polaron under the influence of an external electric field

Following the Dirac-Frenkel time-dependent variational principle, transient dynamics of a one-dimensional Holstein polaron with diagonal and off-diagonal exciton-phonon coupling in an external electric field is studied by employing the multi-D$_2$ {\it Ansatz}, also known as a superposition of the usual Davydov D$_2$ trial states. Resultant polaron dynamics has significantly enhanced accuracy, and is in perfect agreement with that derived from the hierarchy equations of motion method. Starting from an initial broad wave packet, the exciton undergoes typical Bloch oscillations. Adding weak exciton-phonon coupling leads to a broadened exciton wave packet and a reduced current amplitude. Using a narrow wave packet as the initial state, the bare exciton oscillates in a symmetric breathing mode, but the symmetry is easily broken by weak coupling to phonons, resulting in a non-zero exciton current. For both scenarios, temporal periodicity is unchanged by exciton-phonon coupling. In particular, at variance with the case of an infinite linear chain, no steady state is found in a finite-sized ring within the anti-adiabatic regime. For strong diagonal coupling, the multi-$\rm D_2$ {\it Anstaz} is found to be highly accurate, and the phonon confinement gives rise to exciton localization and decay of the Bloch oscillations.

quant-ph↗

arXiv2017

Polaron dynamics with off-diagonal coupling: beyond the Ehrenfest approximation

Treated traditionally by the Ehrenfest approximation, dynamics of a one-dimensional molecular crystal model with off-diagonal exciton-phonon coupling is investigated in this work using the Dirac-Frenkel time-dependent variational principle with the multi-D$_2$ {\it Ansatz}. It is shown that the Ehrenfest method is equivalent to our variational method with the single D$_2$ {\it Ansatz}, and with the multi-D$_2$ {\it Ansatz}, the accuracy of our simulated dynamics is significantly enhanced in comparison with the semi-classical Ehrenfest dynamics. The multi-D$_2$ {\it Ansatz} is able to capture numerically accurate exciton momentum probability and help clarify the relation between the exciton momentum redistribution and the exciton energy relaxation. The results demonstrate that the exciton momentum distributions in the steady state are determined by a combination of the transfer integral and the off-diagonal coupling strength, independent of the excitonic initial conditions. We also probe the effect of the transfer integral and the off-diagonal coupling on exciton transport in both real and reciprocal space representations. Finally, the variational method with importance sampling is employed to investigate temperature effects on exciton transport using the multi-$\rm D_2$ {\it Ansatz}, and it is demonstrated that the variational approach is valid in both low and high temperature regimes.

physics.chem-ph↗

arXiv2017

Finite-temperature time-dependent variation with multiple Davydov states

The Dirac-Frenkel time-dependent variational approach with Davydov Ansätze is a sophisticated, yet efficient technique to obtain an acuurate solution to many-body Schrödinger equations for energy and charge transfer dy- namics in molecular aggregates and light-harvesting complexes. We extend this variational approach to finite temperatures dynamics of the spin-boson model by adopting a Monte Carlo importance sampling method. In or- der to demonstrate the applicability of this approach, we compare real-time quantum dynamics of the spin-boson model calculated with that from numerically exact iterative quasiadiabatic propagator path integral (QUAPI) technique. The comparison shows that our variational approach with the single Davydov Ansätze is in excellent agreement with the QUAPI method at high temperatures, while the two differ at low temperatures. Accuracy in dynamics calculations employing a multitude of Davydov trial states is found to improve substantially over the single Davydov Ansatz, especially at low temperatures. At a moderate computational cost, our variational approach with the multiple Davydov Ansatz is shown to provide accurate spin-boson dynamics over a wide range of temperatures and bath spectral densities.

quant-ph↗

arXiv2015

Variational dynamics of the sub-Ohmic spin-boson model on the basis of multiple Davydov $\mathrm{D}_1$ states

Dynamics of the sub-Ohmic spin-boson model is investigated by employing a multitude of the Davydov D$_1$ trial states, also known as the multi-D$_1$ Ansatz. Accuracy in dynamics simulations is improved significantly over the single D$_1$ Ansatz, especially in the weak system-bath coupling regime. The reliability of the multi-D$_1$ Ansatz for various coupling strengths and initial conditions are also systematically examined, with results compared closely with those of the hierarchy equations of motion and the path integral Monte Carlo approaches. In addition, a coherent-incoherent phase crossover in the nonequilibrium dynamics is studied through the multi-D$_1$ Ansatz. The phase diagram is obtained with a critical point $s_{c}=0.4$. For $s_{c}<s<1$, the coherent-to-incoherent crossover occurs at a certain coupling strength, while the coherent state recurs at a much larger coupling strength. For $s<s_{c}$, only the coherent phase exists.

quant-ph↗

arXiv2015

Superradiance at the localization-delocalization crossover in tubular chlorosomes

We study the effect of disorder on spectral properties of tubular chlorosomes in green sulfur bacteria Cf. aurantiacus. Employing a Frenkel-exciton Hamiltonian with diagonal and off-diagonal disorder consistent with spectral and structural studies, we analyze excitonic localization and spectral statistics of the chlorosomes. A size-dependent localization-delocalization crossover is found to occur as a function of the excitonic energy. The crossover energy region coincides with the more optically active states with maximized superradiance, and is, consequently, more conducive for energy transfer.

physics.bio-ph↗

arXiv2015

Symmetry and the critical phase of the two-bath spin-boson model: Ground-state properties

A generalized trial wave function termed as the "multi-D1 Ansatz" has been developed to study the ground state of the spin-boson model with simultaneous diagonal and off-diagonal coupling in the sub-Ohmic regime. Ground-state properties including the energy and the spin polarization are investigated, and the results are consistent with those from the exact diagonalization and density matrix renormalization group approaches for the cases involving two oscillators and two baths described by a continuous spectral density function. Breakdown of the rotational and parity symmetries along the continuous quantum phase transition separating the localized phase from the critical phase has been uncovered. Moreover, the phase boundary is determined accurately with the corresponding symmetry parameters of the rotational and parity symmetries. A critical value of the spectral exponent s* = 0.49(1) is predicted in the weak coupling limit, which is in agreement with the mean-field prediction of 1/2, but much smaller than the earlier literature estimate of 0.75(1).

cond-mat.quant-gas↗

arXiv2014

Ground state properties of sub-Ohmic spin-boson model with simultaneous diagonal and off-diagonal coupling

By employing the variational approach, density matrix renormalization group (DMRG), exact diagonalization as well as symmetry and mean-field analyses, the ground state properties of the two-bath spin boson model with simultaneous diagonal and off-diagonal coupling are systematically studied in the sub-Ohmic regime. A novel quantum phase transition from a doubly degenerate "localized phase" to the other doubly degenerate "delocalized phase" is uncovered. Via the multi-D1 ansatz as the variational wave function, transition points are determined accurately, consistent with the results from DMRG and exact diagonalization. An effective spatial dimension $d_{eff} = 2.37(6)$ is then estimated, which is found to be compatible with the mean-field prediction. Furthermore, the quantum phase transition is inferred to be of first order for the baths described by a continuous spectral density function. In the case of single mode, however, the transition is softened.

cond-mat.stat-mech↗