Kenneth A. Jung

Bio: Kenneth A. Jung is an academic researcher from University of Toronto. The author has contributed to research in topics: Dephasing & Automatic differentiation. The author has an hindex of 2, co-authored 4 publications receiving 13 citations.

Energy transfer under natural incoherent light: Effects of asymmetry on efficiency.

Abstract: The non-equilibrium stationary coherences that form in donor–acceptor systems are investigated to determine their relationship to the efficiency of energy transfer to a neighboring reaction center. It is found that the effects of asymmetry in the dimer are generally detrimental to the transfer of energy. Four types of systems are examined, arising from combinations of localized trapping, delocalized (Forster) trapping, eigenstate dephasing, and site basis dephasing. In the cases of site basis dephasing, the interplay between the energy gap of the excited dimer states and the environment is shown to give rise to a turnover effect in the efficiency under weak dimer coupling conditions. Furthermore, the nature of the coherences and associated flux is interpreted in terms of pathway interference effects. In addition, regardless of the cases considered, the ratio of the real part and the imaginary part of the coherences in the energy-eigenbasis tends to a constant value in the steady state limit.

Inverse design of dissipative quantum steady-states with implicit differentiation

Abstract: Inverse design of a property that depends on the steady-state of an open quantum system is commonly done by grid-search type of methods. In this paper we present a new methodology that allows us to compute the gradient of the steady-state of an open quantum system with respect to any parameter of the Hamiltonian using the implicit differentiation theorem. As an example, we present a simulation of a spin-boson model where the steady-state solution is obtained using Redfield theory.

Energy transfer under natural incoherent light: Effects of asymmetry on efficiency

Abstract: The non-equilibrium stationary coherences that form in donor-acceptor systems are investigated to determine their relationship to the efficiency of energy transfer to a neighboring reaction center. It is found that the effects of asymmetry in the dimer are generally detrimental to the transfer of energy. Four types of systems are examined, arising from combinations of localized trapping, delocalized (Forster) trapping, eigenstate dephasing and site basis dephasing. In the cases of site basis dephasing the interplay between the energy gap of the excited dimer states and the environment is shown to give rise to a turnover effect in the efficiency under weak dimer coupling conditions. Furthermore, the nature of the coherences and associated flux are interpreted in terms of pathway interference effects. In addition, regardless of the cases considered, the ratio of the real part and the imaginary part of the coherences in the energy-eigenbasis tends to a constant value in the steady state limit.

Fully differentiable optimization protocols for non-equilibrium steady states

Abstract: The time-evolution or equations of motions for many systems are usually described by a set of first-order ordinary differential equations, and for a variety of physical observables, the long-time limit or steady state solution is desired. In the case of open quantum systems, the time-evolution of the reduced density matrix is described by the Liouvillian. 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. Our approach has a low memory cost, and is agnostic to the exact algorithm for computing the steady state. We illustrate the advantage of this method by inverse designing the parameters of a quantum heat transfer device that maximizes the heat current and the rectification coefficient. We also optimize the parameters of various Lindblad operators used in the simulation of energy transfer under natural incoherent light.

Quantum optimal control in quantum technologies. Strategic report on current status, visions and goals for research in Europe

Abstract: Quantum optimal control, a toolbox for devising and implementing the shapes of external fields that accomplish given tasks in the operation of a quantum device in the best way possible, has evolved into one of the cornerstones for enabling quantum technologies. The last few years have seen a rapid evolution and expansion of the field. We review here recent progress in our understanding of the controllability of open quantum systems and in the development and application of quantum control techniques to quantum technologies. We also address key challenges and sketch a roadmap for future developments.

Steady-State Analysis of Light-Harvesting Energy Transfer Driven by Incoherent Light: From Dimers to Networks.

Abstract: 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 sta...

Steady-state Fano coherences in a V-type system driven by polarized incoherent light

Abstract: 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 $\mathcal{C} = (1+\frac{\Delta^2}{\gamma(r+\gamma)} )^{-1}$ is maximized when the excited-state splitting $\Delta$ is small compared to either the spontaneous decay rate $\gamma$ 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 $\gamma_d$. 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.

Steady-State Analysis of Light-harvesting Energy Transfer Driven by Incoherent Light: From Dimers to Networks

Abstract: 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:$\eta=c\sum_{i eq j}F_{ij}\kappa_j=2c\sum_{i eq j}J_{ij}{\rm Im}[{\rho}_{ij}]\kappa_j$ with $c$ the normalization constant. In this relation, the first equality indicates that energy transfer efficiency $\eta$ is uniquely determined by the trapping flux, which is the product of flux $F$ and branching ratio $\kappa$ for trapping at the reaction centers, and the second equality indicates that the energy transfer flux $F$ is equivalent to quantum coherence measured by the imaginary part of the off-diagonal density matrix, i.e., $F_{ij}=2J_{ij}{\rm Im}[{\rho}_{ij}]$. Consequently, maximal steady-state coherence gives rise to optimal efficiency. The coherence-flux-efficiency relation holds rigorously and generally for any exciton networks of arbitrary connectivity under the stationary condition and is not limited to incoherent radiation or incoherent pumping. For light-harvesting systems under incoherent light, non-equilibrium energy transfer flux (i.e. steady-state coherence) is driven by the breakdown of detailed balance and by the quantum interference of light-excitations and leads to the optimization of energy transfer efficiency. It should be noted that the steady-state coherence or, equivalently, efficiency is the combined result of light-induced transient coherence, inhomogeneous depletion, and system-bath correlation, and is thus not necessarily correlated with quantum beatings.

Nonequilibrium steady-state picture of incoherent light-induced excitation harvesting.

Abstract: We formulate a comprehensive theoretical description of excitation harvesting in molecular aggregates photoexcited by weak incoherent radiation. An efficient numerical scheme that respects the continuity equation for excitation fluxes is developed to compute the nonequilibrium steady state (NESS) arising from the interplay between excitation generation, excitation relaxation, dephasing, trapping at the load, and recombination. The NESS is most conveniently described in the so-called preferred basis in which the steady-state excitonic density matrix is diagonal. The NESS properties are examined by relating the preferred-basis description to the descriptions in the site or excitonic bases. Focusing on a model photosynthetic dimer, we find that the NESS in the limit of long trapping time is quite similar to the excited-state equilibrium in which the stationary coherences originate from the excitation–environment entanglement. For shorter trapping times, we demonstrate how the properties of the NESS can be extracted from the time-dependent description of an incoherently driven but unloaded dimer. This relation between stationary and time-dependent pictures is valid, provided that the trapping time is longer than the decay time of dynamic coherences accessible in femtosecond spectroscopy experiments.