arXiv subjects

Herschel Rabitz

Publications and source records attributed to Herschel Rabitz.

At least 91 records · Page 5Linked to original sources

arXiv2013

Exploring Quantum Control Landscape Structure

A common goal of quantum control is to maximize a physical observable through the application of a tailored field. The observable value as a function of the field constitutes a quantum control landscape. Previous works have shown, under specified conditions, that the quantum control landscape should be free of suboptimal critical points. This favorable landscape topology is one factor contributing to the efficiency of climbing the landscape. An additional, complementary factor is the landscape \textit{structure}, which constitutes all non-topological features. If the landscape's structure is too complex, then climbs may be forced to take inefficient convoluted routes to finding optimal controls. This paper provides a foundation for understanding control landscape structure by examining the linearity of gradient-based optimization trajectories through the space of control fields. For this assessment, a metric $R\geq 1$ is defined as the ratio of the path length of the optimization trajectory to the Euclidean distance between the initial control field and the resultant optimal control field that takes an observable from the bottom to the top of the landscape. Computational analyses for simple model quantum systems are performed to ascertain the relative abundance of nearly straight control trajectories encountered when optimizing a state-to-state transition probability. The collected results indicate that quantum control landscapes have very simple structural features. The favorable topology and the complementary simple structure of the control landscape provide a basis for understanding the generally observed ease of optimizing a state-to-state transition probability.

quant-ph↗

arXiv2013

Topology of Classical Molecular Optimal Control Landscapes in Phase Space

Optimal control of molecular dynamics is commonly expressed from a quantum mechanical perspective. However, in most contexts the preponderance of molecular dynamics studies utilize classical mechanical models. This paper treats laser-driven optimal control of molecular dynamics in a classical framework. We consider the objective of steering a molecular system from an initial point in phase space to a target point, subject to the dynamic constraint of Hamilton's equations. The classical control landscape corresponding to this objective is a functional of the control field, and the topology of the landscape is analyzed through its gradient and Hessian with respect to the control. Under specific assumptions on the regularity of the control fields, the classical control landscape is found to be free of traps that could hinder reaching the objective. The Hessian associated with an optimal control field is shown to have finite rank, indicating the presence of an inherent degree of robustness to control noise. Extensive numerical simulations are performed to illustrate the theoretical principles on a) a model diatomic molecule, b) two coupled Morse oscillators, and c) a chaotic system with a coupled quartic oscillator, confirming the absence of traps in the classical control landscape. We compare the classical formulation with the mathematically analogous state-to-state transition probability control landscape of N-level quantum systems. The absence of traps in both circumstances provides a broader basis to understand the growing number of successful control experiments with complex molecules, which can have dynamics that transcend the classical and quantum regimes.

physics.chem-ph↗

arXiv2013

Sampled-data design for robust control of a single qubit

This paper presents a sampled-data approach for the robust control of a single qubit (quantum bit). The required robustness is defined using a sliding mode domain and the control law is designed offline and then utilized online with a single qubit having bounded uncertainties. Two classes of uncertainties are considered involving the system Hamiltonian and the coupling strength of the system-environment interaction. Four cases are analyzed in detail including without decoherence, with amplitude damping decoherence, phase damping decoherence and depolarizing decoherence. Sampling periods are specifically designed for these cases to guarantee the required robustness. Two sufficient conditions are presented for guiding the design of unitary control for the cases without decoherence and with amplitude damping decoherence. The proposed approach has potential applications in quantum error-correction and in constructing robust quantum gates.

quant-ph↗

arXiv2012

Energy-scales convergence for optimal and robust quantum transport in photosynthetic complexes

Underlying physical principles for the high efficiency of excitation energy transfer in light-harvesting complexes are not fully understood. Notably, the degree of robustness of these systems for transporting energy is not known considering their realistic interactions with vibrational and radiative environments within the surrounding solvent and scaffold proteins. In this work, we employ an efficient technique to estimate energy transfer efficiency of such complex excitonic systems. We observe that the dynamics of the Fenna-Matthews-Olson (FMO) complex leads to optimal and robust energy transport due to a convergence of energy scales among all important internal and external parameters. In particular, we show that the FMO energy transfer efficiency is optimum and stable with respect to the relevant parameters of environmental interactions and Frenkel-exciton Hamiltonian including reorganization energy $λ$, bath frequency cutoff $γ$, temperature $T$, bath spatial correlations, initial excitations, dissipation rate, trapping rate, disorders, and dipole moments orientations. We identify the ratio of $λT/γ\*g$ as a single key parameter governing quantum transport efficiency, where g is the average excitonic energy gap.

quant-ph↗

arXiv2012

Exploring the trade-off between fidelity- and time-optimal control of quantum unitary transformations

Generating a unitary transformation in the shortest possible time is of practical importance to quantum information processing because it helps to reduce decoherence effects and improve robustness to additive control field noise. Many analytical and numerical studies have identified the minimum time necessary to implement a variety of quantum gates on coupled-spin qubit systems. This work focuses on exploring the Pareto front that quantifies the trade-off between the competitive objectives of maximizing the gate fidelity $\mathcal{F}$ and minimizing the control time $T$. In order to identify the critical time $T^{\ast}$, below which the target transformation is not reachable, as well as to determine the associated Pareto front, we introduce a numerical method of Pareto front tracking (PFT). We consider closed two- and multi-qubit systems with constant inter-qubit coupling strengths and each individual qubit controlled by a separate time-dependent external field. Our analysis demonstrates that unit fidelity (to a desired numerical accuracy) can be achieved at any $T \geq T^{\ast}$ in most cases. However, the optimization search effort rises superexponentially as $T$ decreases and approaches $T^{\ast}$. Furthermore, a small decrease in control time incurs a significant penalty in fidelity for $T < T^{\ast}$, indicating that it is generally undesirable to operate below the critical time. We investigate the dependence of the critical time $T^{\ast}$ on the coupling strength between qubits and the target gate transformation. Practical consequences of these findings for laboratory implementation of quantum gates are discussed.

quant-ph↗

arXiv2012

Control through operators for quantum chemistry

We consider the problem of operator identification in quantum control. The free Hamiltonian and the dipole moment are searched such that a given target state is reached at a given time. A local existence result is obtained. As a by-product, our works reveals necessary conditions on the laser field to make the identification feasible. In the last part of this work, some algorithms are proposed to compute effectively these operators.

math.OC↗

arXiv2012

Dynamic Homotopy and Landscape Dynamical Set Topology in Quantum Control

We examine the topology of the subset of controls taking a given initial state to a given final state in quantum control, where "state" may mean a pure state |ψ>, an ensemble density matrix ρ, or a unitary propagator U(0,T). The analysis consists in showing that the endpoint map acting on control space is a Hurewicz fibration for a large class of affine control systems with vector controls. Exploiting the resulting fibration sequence and the long exact sequence of basepoint-preserving homotopy classes of maps, we show that the indicated subset of controls is homotopy equivalent to the loopspace of the state manifold. This not only allows us to understand the connectedness of "dynamical sets" realized as preimages of subsets of the state space through this endpoint map, but also provides a wealth of additional topological information about such subsets of control space.

quant-ph↗

arXiv2012

Exploring constrained quantum control landscapes

The broad success of optimally controlling quantum systems with external fields has been attributed to the favorable topology of the underlying control landscape, where the landscape is the physical observable as a function of the controls. The control landscape can be shown to contain no suboptimal trapping extrema upon satisfaction of reasonable physical assumptions, but this topological analysis does not hold when significant constraints are placed on the control resources. This work employs simulations to explore the topology and features of the control landscape for pure-state population transfer with a constrained class of control fields. The fields are parameterized in terms of a set of uniformly spaced spectral frequencies, with the associated phases acting as the controls. Optimization results reveal that the minimum number of phase controls necessary to assure a high yield in the target state has a special dependence on the number of accessible energy levels in the quantum system, revealed from an analysis of the first- and second-order variation of the yield with respect to the controls. When an insufficient number of controls and/or a weak control fluence are employed, trapping extrema and saddle points are observed on the landscape. When the control resources are sufficiently flexible, solutions producing the globally maximal yield are found to form connected `level sets' of continuously variable control fields that preserve the yield. These optimal yield level sets are found to shrink to isolated points on the top of the landscape as the control field fluence is decreased, and further reduction of the fluence turns these points into suboptimal trapping extrema on the landscape. Although constrained control fields can come in many forms beyond the cases explored here, the behavior found in this paper is illustrative of the impacts that constraints can introduce.

quant-ph↗

arXiv2012

Comment on "Are There Traps in Quantum Control Landscapes?"

Many quantum control problems are formulated as a search for an optimal field that maximizes a physical objective. This search is performed over a landscape defined as the objective as a function of the control field. A recent Letter [A. N. Pechen and D. J. Tannor, Phys. Rev. Lett. 106, 120402 (2011)] asserts that the existence of special landscape critical points (CPs) with trapping characteristics is "contrary to recent claims in the literature" and "can have profound implications for both theoretical and experimental quantum control studies." We show here that these assertions are inaccurate and misleading.

quant-ph↗

arXiv2012

Efficient estimation of energy transfer efficiency in light-harvesting complexes

The fundamental physical mechanisms of energy transfer in photosynthetic complexes is not yet fully understood. In particular, the degree of efficiency or sensitivity of these systems for energy transfer is not known given their non-perturbative and non-Markovian interactions with proteins backbone and surrounding photonic and phononic environments. One major problem in studying light-harvesting complexes has been the lack of an efficient method for simulation of their dynamics in biological environments. To this end, here we revisit the second-order time-convolution (TC2) master equation and examine its reliability beyond extreme Markovian and perturbative limits. In particular, we present a derivation of TC2 without making the usual weak system-bath coupling assumption. Using this equation, we explore the long time behaviour of exciton dynamics of Fenna-Matthews-Olson (FMO) protein complex. Moreover, we introduce a constructive error analysis to estimate the accuracy of TC2 equation in calculating energy transfer efficiency, exhibiting reliable performance for environments with weak and intermediate memory and strength. Furthermore, we numerically show that energy transfer efficiency is optimal and robust for the FMO protein complex of green sulphur bacteria with respect to variations in reorganization energy and bath correlation time-scales.

quant-ph↗

arXiv2012

Optimal coherent control of CARS: signal enhancement and background elimination

The ability to enhance resonant signals and eliminate the non-resonant background is analyzed for Coherent Anti-Stokes Raman Scattering (CARS). The analysis is done at a specific frequency as well as for broadband excitation using femtosecond pulse-shaping techniques. An appropriate objective functional is employed to balance resonant signal enhancement against non-resonant background suppression. Optimal enhancement of the signal and minimization of the background can be achieved by shaping the probe pulse alone while keeping the pump and Stokes pulses in transform-limited-form (TLF). In some cases analytical forms for the probe pulse can be found, and numerical simulations are carried out for other circumstances. It is found that a good approximate solution for the optimal pulse in the two-pulse CARS is a superposition of linear and arctangent type phases for the pump. The well-known probe delay method is shown to be a quasi-optimal scheme for background suppression. The results should provide a basis to improve the performance of CARS spectroscopy and microscopy.

quant-ph↗

arXiv2012

Critical points of the optimal quantum control landscape: a propagator approach

Numerical and experimental realizations of quantum control are closely connected to the properties of the mapping from the control to the unitary propagator. For bilinear quantum control problems, no general results are available to fully determine when this mapping is singular or not. In this paper we give suffcient conditions, in terms of elements of the evolution semigroup, for a trajectory to be non-singular. We identify two lists of "way-points" that, when reached, ensure the non-singularity of the control trajectory. It is found that under appropriate hypotheses one of those lists does not depend on the values of the coupling operator matrix.

math.NA↗

arXiv2011

Quantum Control Experiments as a Testbed for Evolutionary Multi-Objective Algorithms

Experimental multi-objective Quantum Control is an emerging topic within the broad physics and chemistry applications domain of controlling quantum phenomena. This realm offers cutting edge ultrafast laser laboratory applications, which pose multiple objectives, noise, and possibly constraints on the high-dimensional search. In this study we introduce the topic of Multi-Observable Quantum Control (MOQC), and consider specific systems to be Pareto optimized subject to uncertainty, either experimentally or by means of simulated systems. The latter include a family of mathematical test-functions with a practical link to MOQC experiments, which are introduced here for the first time. We investigate the behavior of the multi-objective version of the Covariance Matrix Adaptation Evolution Strategy (MO-CMA-ES) and assess its performance on computer simulations as well as on laboratory closed-loop experiments. Overall, we propose a comprehensive study on experimental evolutionary Pareto optimization in high-dimensional continuous domains, draw some practical conclusions concerning the impact of fitness disturbance on algorithmic behavior, and raise several theoretical issues in the broad evolutionary multi-objective context.

cs.NE↗

arXiv2011

Evolutionary Hessian Learning: Forced Optimal Covariance Adaptive Learning (FOCAL)

The Covariance Matrix Adaptation Evolution Strategy (CMA-ES) has been the most successful Evolution Strategy at exploiting covariance information; it uses a form of Principle Component Analysis which, under certain conditions, is suggested to converge to the correct covariance matrix, formulated as the inverse of the mathematically well-defined Hessian matrix. However, in practice, there exist conditions where CMA-ES converges to the global optimum (accomplishing its primary goal) while it does not learn the true covariance matrix (missing an auxiliary objective), likely due to step-size deficiency. These circumstances can involve high-dimensional landscapes with large condition numbers. This paper introduces a novel technique entitled Forced Optimal Covariance Adaptive Learning (FOCAL), with the explicit goal of determining the Hessian at the global basin of attraction. It begins by introducing theoretical foundations to the inverse relationship between the learned covariance and the Hessian matrices. FOCAL is then introduced and demonstrated to retrieve the Hessian matrix with high fidelity on both model landscapes and experimental Quantum Control systems, which are observed to possess a non-separable, non-quadratic search landscape. The recovered Hessian forms are corroborated by physical knowledge of the systems. This study constitutes an example for Natural Computing successfully serving other branches of natural sciences, and introducing at the same time a powerful generic method for any high-dimensional continuous search seeking landscape information.

cs.NE↗

arXiv2011

The quantum Goldilocks effect: on the convergence of timescales in quantum transport

Excitonic transport in photosynthesis exhibits a wide range of time scales. Absorption and initial relaxation takes place over tens of femtoseconds. Excitonic lifetimes are on the order of a nanosecond. Hopping rates, energy differences between chromophores, reorganization energies, and decoherence rates correspond to time scales on the order of picoseconds. The functional nature of the divergence of time scales is easily understood: strong coupling to the electromagnetic field over a broad band of frequencies yields rapid absorption, while long excitonic lifetimes increase the amount of energy that makes its way to the reaction center to be converted to chemical energy. The convergence of the remaining time scales to the centerpoint of the overall temporal range is harder to understand. In this paper we argue that the convergence of timescales in photosynthesis can be understood as an example of the `quantum Goldilocks effect': natural selection tends to drive quantum systems to the degree of quantum coherence that is `just right' for attaining maximum efficiency. We provide a general theory of optimal and robust, efficient transport in quantum systems, and show that it is governed by a single parameter.

quant-ph↗

arXiv2011

Gradient flow for controlling quantum ensemble

We propose in this paper a gradient-type dynamical system to solve the problem of maximizing quantum observables for finite dimensional closed quantum ensembles governed by the controlled Liouville-von Neumann equation. The asymptotic behavior is analyzed: we show that under the regularity assumption on the controls the dynamical system almost always converges to a solution of the maximization problem; we also detail the difficulties related to the occurrence of singular controls.

math.OC↗

arXiv2011

Non-equilibrium local pair potential enhancement

We propose a new mechanism for the local pair potential enhancement with the help of electromagnetic control fields. The mechanism is based on the creation of non-equilibrium, spatially localized Bogoliubov quasiparticle excitations, which result in a significant enhancement of the local pair potential and the local transition temperature T_c.

cond-mat.supr-con↗

arXiv2011

Exploring Quantum Control Landscapes: Topology, Features, and Optimization Scaling

Quantum optimal control experiments and simulations have successfully manipulated the dynamics of systems ranging from atoms to biomolecules. Surprisingly, these collective works indicate that the effort (i.e., the number of algorithmic iterations) required to find an optimal control field appears to be essentially invariant to the complexity of the system. The present work explores this matter in a series of systematic optimizations of the state-to-state transition probability on model quantum systems with the number of states $N$ ranging from 5 through 100. The optimizations occur over a landscape defined by the transition probability as a function of the control field. Previous theoretical studies on the topology of quantum control landscapes established that they should be free of sub-optimal traps under reasonable physical conditions. The simulations in this work include nearly 5000 individual optimization test cases, all of which confirm this prediction by fully achieving optimal population transfer of at least 99.9% upon careful attention to numerical procedures to ensure that the controls are free of constraints. Collectively, the simulation results additionally show invariance of required search effort to system dimension $N$. This behavior is rationalized in terms of the structural features of the underlying control landscape. The very attractive observed scaling with system complexity may be understood by considering the distance traveled on the control landscape during a search and the magnitude of the control landscape slope. Exceptions to this favorable scaling behavior can arise when the initial control field fluence is too large or when the target final state recedes from the initial state as $N$ increases.

quant-ph↗