Quantum transport theory of vibrons in a molecular monolayer

Citation
V. Pouthier et al., Quantum transport theory of vibrons in a molecular monolayer, J CHEM PHYS, 114(11), 2001, pp. 4955-4967
Citations number
67
Categorie Soggetti
Physical Chemistry/Chemical Physics
Journal title
JOURNAL OF CHEMICAL PHYSICS
ISSN journal
00219606 → ACNP
Volume
114
Issue
11
Year of publication
2001
Pages
4955 - 4967
Database
ISI
SICI code
0021-9606(20010315)114:11<4955:QTTOVI>2.0.ZU;2-D
Abstract
We establish a quantum kinetic equation describing the transport properties of the vibrons in a molecular monolayer adsorbed on a dielectric substrate . A renormalization procedure is applied to the Hamiltonian of the system w hich is then separated in a vibron Hamiltonian, a bath Hamiltonian connecte d the external motions and a coupling Hamiltonian between the vibrons and t he external modes. A perturbative analysis based on the projector method al lows us to eliminate the irrelevant information related to the bath dynamic s. The use of conventional approximations (Markov limit and Wick theorem) l eads us to write the kinetic equation in a form exhibiting linear and nonli near contributions. The linear term characterizes irreversible processes co nnected to the bath fluctuations whereas the nonlinear term represents a se lf-modulation of the dynamical matrix with respect to the vibron distributi on. An application of the transport of CO vibrons on NaCl(100) illustrates the method. (C) 2001 American Institute of Physics.