Optimal control theory with continuously distributed target states: An application to NaK

Abstract Laser pulse control of molecular dynamics is studied theoretically by using optimal control theory. The control theory is extended to target states which are distributed in time as well as in a space of parameters which are responsible for a change of individual molecular properties. This generalized treatment of a control task is first applied to wave packet formation in randomly oriented diatomic systems. Concentrating on an ensemble of NaK molecules which are not aligned the control yield decreases drastically when compared with an aligned ensemble. Second, we demonstrate for NaK the maximization of the probe pulse transient absorption in a pump–probe scheme with an optimized pump pulse. These computations suggest an overall optical control scheme, whereby a flexible technique is suggested to form particular wave packets in the excited state potential energy surface. In particular, it is shown that considerable wave packet localization at the turning points of the first-excited Σ-state potential energy surfaces of NaK may be achieved. The dependency of the control yield on the probe pulse parameters is also discussed.

[1]  Rabitz,et al.  Optimally controlled quantum molecular dynamics: A perturbation formulation and the existence of multiple solutions. , 1993, Physical review. A, Atomic, molecular, and optical physics.

[2]  Samuel H. Tersigni,et al.  On using shaped light pulses to control the selectivity of product formation in a chemical reaction: An application to a multiple level system , 1990 .

[3]  Marcus Motzkus,et al.  Quantum control of energy flow in light harvesting , 2002, Nature.

[4]  D. Zeidler,et al.  Optimal control of ground-state dynamics in polymers , 2002 .

[5]  G Gerber,et al.  Optimal control of photoisomerization. , 2005, Physical review letters.

[6]  An application of minimax analysis to robust optimal control of molecular dynamics , 1994 .

[7]  Andreas Kaiser,et al.  Optimal control theory for a target state distributed in time: optimizing the probe-pulse signal of a pump-probe-scheme. , 2004, The Journal of chemical physics.

[8]  Stuart A. Rice,et al.  Optical Control of Molecular Dynamics , 2000 .

[9]  Herschel Rabitz,et al.  A RAPID MONOTONICALLY CONVERGENT ITERATION ALGORITHM FOR QUANTUM OPTIMAL CONTROL OVER THE EXPECTATION VALUE OF A POSITIVE DEFINITE OPERATOR , 1998 .

[10]  H. Rabitz,et al.  The influence of laser field noise on controlled quantum dynamics. , 2004, The Journal of chemical physics.

[11]  H. Rabitz,et al.  RAPIDLY CONVERGENT ITERATION METHODS FOR QUANTUM OPTIMAL CONTROL OF POPULATION , 1998 .

[12]  Volkhard May,et al.  Optimizing frequency dispersed transient absorption signals: A computational study , 2005 .

[13]  H. Rabitz,et al.  Optimal control of quantum-mechanical systems: Existence, numerical approximation, and applications. , 1988, Physical review. A, General physics.

[14]  Volkhard May,et al.  Ultrafast Laser Pulse Control of Exciton Dynamics: A Computational Study on the FMO Complex† , 2004 .

[15]  H. Rabitz,et al.  Quantum mechanical optimal control of physical observables in microsystems , 1990 .

[16]  G. Gerber,et al.  Liquid-phase adaptive femtosecond quantum control: Removing intrinsic intensity dependencies , 2003 .

[17]  T. Mančal,et al.  Optimal control theory of ultrafast molecular dynamics: are the results of interest for the experiment? , 2002 .

[18]  R. Vivie-Riedle,et al.  Adapting optimal control theory and using learning loops to provide experimentally feasible shaping mask patterns , 2001 .

[19]  Volkhard May,et al.  Charge and Energy Transfer Dynamics in Molecular Systems, 2nd, Revised and Enlarged Edition , 2004 .

[20]  李幼升,et al.  Ph , 1989 .

[21]  Paul Brumer,et al.  Principles of the Quantum Control of Molecular Processes , 2003 .

[22]  Magnier,et al.  Potential Energies, Permanent and Transition Dipole Moments for Numerous Electronic Excited States of NaK. , 2000, Journal of molecular spectroscopy.

[23]  Gabriel Turinici,et al.  Generalized monotonically convergent algorithms for solving quantum optimal control problems. , 2004, The Journal of chemical physics.

[24]  Herschel Rabitz,et al.  Quantum optimal control of multiple targets: Development of a monotonically convergent algorithm and application to intramolecular vibrational energy redistribution control , 2001 .

[25]  L. González,et al.  Deciphering the Reaction Dynamics Underlying Optimal Control Laser Fields , 2003, Science.

[26]  Stefan M. Weber,et al.  Optimal control of ionization processes in NaK: Comparison between theory and experiment , 2004 .