2003
DOI: 10.1103/physrevlett.90.117601
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Femtosecond Photodesorption of Small Molecules from Surfaces: A Theoretical Investigation from First Principles

Abstract: A microscopic model for the excitation and relaxation processes in photochemistry at surfaces is developed. Our study is based on ab initio calculations and the surrogate Hamiltonian method treating surface electron-hole pairs as a bath of two-level systems. Desorption probabilities and velocities in the experimentally observed range are obtained. The excited state lifetime is calculated, and a dependence of observables on pulse length is predicted. DOI: 10.1103/PhysRevLett.90.117601 PACS numbers: 79.20.La, 6… Show more

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Cited by 41 publications
(54 citation statements)
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“…A common feature of these methods is their ability to correctly describe thermalization of the system. Slightly different in philosophy are methods which attempt to solve the dynamics of both system and environment [66,67]. Key is to account only for that part of the environment that is relevant for the system's dynamics, i.e., for the 'effective modes', which can be spins or harmonic oscillators.…”
Section: A Markovian Vs Non-markovian Dynamicsmentioning
confidence: 99%
“…A common feature of these methods is their ability to correctly describe thermalization of the system. Slightly different in philosophy are methods which attempt to solve the dynamics of both system and environment [66,67]. Key is to account only for that part of the environment that is relevant for the system's dynamics, i.e., for the 'effective modes', which can be spins or harmonic oscillators.…”
Section: A Markovian Vs Non-markovian Dynamicsmentioning
confidence: 99%
“…However, considering all 2 N possibilities of combining the bath modes might not be necessary in a weak coupling limit. In this case, for short time dynamics, it is possible to restrict the number of simultaneous bath excitations [21]. with N exc the number of simultaneous excitations.…”
Section: Theorymentioning
confidence: 99%
“…The standard approaches fall into two classes: quantum master equations and path integral simulations. The first class of approaches is based on formally exact equations of motion, such as the Nakajima-Zwanzig formalism [1][2][3] or others, but restricted to either weak damping, high-temperature, short memory time or short simulation time [4][5][6][7][8][9][10]. The second class of approaches adopts the harmonic bath assumption which renders the use of stochastic Gaussian sampling or influence functional possible [11,12], but does not converge well with the system size, the length of the memory time or the strength of the dissipation.…”
mentioning
confidence: 99%