Optimal laser control of molecular photoassociation along with vibrational stabilization

AbstractThis work explores the optimization of laser pulses for the control of photoassociation and vibrational stabilization. Simulations are presented within a model system for the electronic ground-state collision of O+H. The goal is to drive the transition from a wavepacket representing the colliding atoms to the vibrational ground level of the diatomic molecule. The optimized fields resulting from two distinct trial pulses are analyzed and compared. Very high yields were obtained in the molecular vibrational ground-level

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 $\lambda$, bath frequency cutoff $\gamma$, temperature $T$, bath spatial correlations, initial excitations, dissipation rate, trapping rate, disorders, and dipole moments orientations. We identify the ratio of \lambda T/\gamma\*g as a single key parameter governing quantum transport efficiency, where g is the average excitonic energy gap.Comment: minor revisions, removing some figures, 19 pages, 19 figure

Volume Fractions of the Kinematic "Near-Critical" Sets of the Quantum Ensemble Control Landscape

An estimate is derived for the volume fraction of a subset $C_{\epsilon}^{P} = \{U : ||grad J(U)|\leq {\epsilon}\}\subset\mathrm{U}(N)$ in the neighborhood of the critical set $C^{P}\simeq\mathrm{U}(\mathbf{n})P\mathrm{U}(\mathbf{m})$ of the kinematic quantum ensemble control landscape J(U) = Tr(U\rho U' O), where $U$ represents the unitary time evolution operator, {\rho} is the initial density matrix of the ensemble, and O is an observable operator. This estimate is based on the Hilbert-Schmidt geometry for the unitary group and a first-order approximation of $||grad J(U)||^2$. An upper bound on these near-critical volumes is conjectured and supported by numerical simulation, leading to an asymptotic analysis as the dimension $N$ of the quantum system rises in which the volume fractions of these "near-critical" sets decrease to zero as $N$ increases. This result helps explain the apparent lack of influence exerted by the many saddles of $J$ over the gradient flow.Comment: 27 pages, 1 figur

Unified analysis of terminal-time control in classical and quantum systems

Many phenomena in physics, chemistry, and biology involve seeking an optimal control to maximize an objective for a classical or quantum system which is open and interacting with its environment. The complexity of finding an optimal control for maximizing an objective is strongly affected by the possible existence of sub-optimal maxima. Within a unified framework under specified conditions, control objectives for maximizing at a terminal time physical observables of open classical and quantum systems are shown to be inherently free of sub-optimal maxima. This attractive feature is of central importance for enabling the discovery of controls in a seamless fashion in a wide range of phenomena transcending the quantum and classical regimes.Comment: 10 page

Wigner phase space distribution as a wave function

We demonstrate that the Wigner function of a pure quantum state is a wave function in a specially tuned Dirac bra-ket formalism and argue that the Wigner function is in fact a probability amplitude for the quantum particle to be at a certain point of the classical phase space. Additionally, we establish that in the classical limit, the Wigner function transforms into a classical Koopman-von Neumann wave function rather than into a classical probability distribution. Since probability amplitude need not be positive, our findings provide an alternative outlook on the Wigner function's negativity.Comment: 6 pages and 2 figure

Calculation of the unitary part of the Bures measure for N-level quantum systems

We use the canonical coset parameterization and provide a formula with the unitary part of the Bures measure for non-degenerate systems in terms of the product of even Euclidean balls. This formula is shown to be consistent with the sampling of random states through the generation of random unitary matrices

Optimal number of pigments in photosynthetic complexes

We study excitation energy transfer in a simple model of photosynthetic complex. The model, described by Lindblad equation, consists of pigments interacting via dipole-dipole interaction. Overlapping of pigments induces an on-site energy disorder, providing a mechanism for blocking the excitation transfer. Based on the average efficiency as well as robustness of random configurations of pigments, we calculate the optimal number of pigments that should be enclosed in a pigment-protein complex of a given size. The results suggest that a large fraction of pigment configurations are efficient as well as robust if the number of pigments is properly chosen. We compare optimal results of the model to the structure of pigment-protein complexes as found in nature, finding good agreement.Comment: 20 pages, 7 figures; v2.: new appendix, published versio

Constructive control of quantum systems using factorization of unitary operators

We demonstrate how structured decompositions of unitary operators can be employed to derive control schemes for finite-level quantum systems that require only sequences of simple control pulses such as square wave pulses with finite rise and decay times or Gaussian wavepackets. To illustrate the technique it is applied to find control schemes to achieve population transfers for pure-state systems, complete inversions of the ensemble populations for mixed-state systems, create arbitrary superposition states and optimize the ensemble average of dynamic observables.Comment: 28 pages, IoP LaTeX, principal author has moved to Cambridge University ([email protected]

Optimization search effort over the control landscapes for open quantum systems with Kraus-map evolution

A quantum control landscape is defined as the expectation value of a target observable $\Theta$ as a function of the control variables. In this work control landscapes for open quantum systems governed by Kraus map evolution are analyzed. Kraus maps are used as the controls transforming an initial density matrix $\rho_{\rm i}$ into a final density matrix to maximize the expectation value of the observable $\Theta$. The absence of suboptimal local maxima for the relevant control landscapes is numerically illustrated. The dependence of the optimization search effort is analyzed in terms of the dimension of the system $N$, the initial state $\rho_{\rm i}$, and the target observable $\Theta$. It is found that if the number of nonzero eigenvalues in $\rho_{\rm i}$ remains constant, the search effort does not exhibit any significant dependence on $N$. If $\rho_{\rm i}$ has no zero eigenvalues, then the computational complexity and the required search effort rise with $N$. The dimension of the top manifold (i.e., the set of Kraus operators that maximizes the objective) is found to positively correlate with the optimization search efficiency. Under the assumption of full controllability, incoherent control modelled by Kraus maps is found to be more efficient in reaching the same value of the objective than coherent control modelled by unitary maps. Numerical simulations are also performed for control landscapes with linear constraints on the available Kraus maps, and suboptimal maxima are not revealed for these landscapes.Comment: 29 pages, 8 figure

Coherent Optimal Control of Multiphoton Molecular Excitation

We give a framework for molecular multiphoton excitation process induced by an optimally designed electric field. The molecule is initially prepared in a coherent superposition state of two of its eigenfunctions. The relative phase of the two superposed eigenfunctions has been shown to control the optimally designed electric field which triggers the multiphoton excitation in the molecule. This brings forth flexibility in desiging the optimal field in the laboratory by suitably tuning the molecular phase and hence by choosing the most favorable interfering routes that the system follows to reach the target. We follow the quantum fluid dynamical formulation for desiging the electric field with application to HBr molecule.Comment: 5 figure