Optimal control of open quantum systems: A combined surrogate Hamiltonian optimal control theory approach applied to photochemistry on surfaces

Asplund, Erik; Klüner, Thorsten

doi:10.1063/1.3698289

Cited by 3 publications

(1 citation statement)

References 52 publications

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“…The influence of the surface temperature on the desorption yield and velocity distributions is also a possible route for future studies [54]. Another extension would be to apply the Optimal Control Theory in order to artificially prolong the lifetime on the electronically excited state, which has been done for the NO/NiO system [55,56]. This, in combination with experimental studies could shed new light on the desorption mechanism and prove the validity of the calculated potential energy surfaces and the microscopic model of the bath and the interaction in the Surrogate Hamiltonian approach.…”

Section: Discussionmentioning

confidence: 98%

A Surrogate Hamiltonian study of femtosecond photodesorption of CO from NiO(100)

Asplund

Klüner

2013

Molecular Physics

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In this paper, the Surrogate Hamiltonian approach is employed in order to study electronic relaxation in femtosecond laserinduced desorption experiments of CO from NiO(100). The study is based on ab initio calculations and a microscopic description of the NiO(100)-surface and the relaxation mechanism developed by Koch et al. The relaxation mechanism is assumed to be of dipole-dipole interaction nature, where the transition dipole moment of the adsorbate interacts with surface electron-hole pairs. In the Surrogate Hamiltonian approach the electron-hole pairs are treated as two-level systems and are described by excitation energy and a dipole charge. The Surrogate Hamiltonian parameters and potential energy surfaces used are obtained from ab initio calculations. The desorption probability and the velocity distributions of the desorbing molecules are calculated and an excited state lifetime is predicted. Throughout this paper atomic units, i.e. = m e = e = a 0 = 1, have been used unless otherwise stated.

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Section: Discussionmentioning

confidence: 98%

A Surrogate Hamiltonian study of femtosecond photodesorption of CO from NiO(100)

Asplund

Klüner

2013

Molecular Physics

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Quantum dynamical study of femtosecond photodesorption of CO from TiO2(110)

Asplund

Klüner

2014

The Journal of Chemical Physics

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The photodesorption of CO from TiO2(110) by femtosecond pulses is investigated with the Surrogate Hamiltonian approach. The aim of the study is to resolve the relaxation mechanism and forecast the lifetime of the exited state based on a microscopic description of the excitation and relaxation processes. The parameters characterizing the system are obtained from ab initio and Density Functional Theory-calculations with one parameter estimated from physical considerations and convergence studies. Two electronic states are considered and the relaxation is assumed to be due to the interaction of the excited adsorbate with electron hole pairs in the surface. Desorption probabilities and velocity distributions of the desorbing molecules are calculated and an exited state lifetime is predicted. Throughout this paper atomic units, i.e., ℏ = me = e = a0 = 1, have been used unless otherwise stated.

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Quantum thermodynamics and open-systems modeling

Kosloff

2019

The Journal of Chemical Physics

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A comprehensive approach to modeling open quantum systems consistent with thermodynamics is presented. The theory of open quantum systems is employed to define system bath partitions. The Markovian master equation defines an isothermal partition between the system and bath. Two methods to derive the quantum master equation are described: the weak coupling limit and the repeated collision model. The role of the eigenoperators of the free system dynamics is highlighted, in particular, for driven systems. The thermodynamical relations are pointed out. Models that lead to loss of coherence, i.e., dephasing are described. The implication of the laws of thermodynamics to simulating transport and spectroscopy is described. The indications for self-averaging in large quantum systems and thus its importance in modeling are described. Basic modeling by the surrogate Hamiltonian is described, as well as thermal boundary conditions using the repeated collision model and their use in the stochastic surrogate Hamiltonian. The problem of modeling with explicitly time dependent driving is analyzed. Finally, the use of the stochastic surrogate Hamiltonian for modeling ultrafast spectroscopy and quantum control is reviewed.

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Optimal control of open quantum systems: A combined surrogate Hamiltonian optimal control theory approach applied to photochemistry on surfaces

Cited by 3 publications

References 52 publications

A Surrogate Hamiltonian study of femtosecond photodesorption of CO from NiO(100)

A Surrogate Hamiltonian study of femtosecond photodesorption of CO from NiO(100)

Quantum dynamical study of femtosecond photodesorption of CO from TiO2(110)

Quantum thermodynamics and open-systems modeling

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