Quantum-classical Liouville dynamics of nonadiabatic proton transfer
Quantum-classical Liouville dynamics of nonadiabatic proton transfer
Publication Type:
Journal ArticleSource:
Journal of Chemical Physics, Volume 122, Number 24 (2005)URL:
https://www.scopus.com/inward/record.uri?eid=2-s2.0-22544447079&doi=10.1063%2f1.1940051&partnerID=40&md5=0fd2f7914e8637e80433bdeb34f4d9f8Keywords:
Algorithms, Approximation theory, Correlation methods, Degrees of freedom (mechanics), Functions, Hydrogen bonds, Mass transfer, Mathematical models, Molecular dynamics, Newton's equations, Proton transfer, Protons, Quantum Theory, Quantum-classical Liouville dynamics, Rate coefficients, TrajectoriesAbstract:
A proton transfer reaction in a linear hydrogen-bonded complex dissolved in a polar solvent is studied using mixed quantum-classical Liouville dynamics. In this system, the proton is treated quantum mechanically and the remainder of the degrees of freedom is treated classically. The rates and mechanisms of the reaction are investigated using both adiabatic and nonadiabatic molecular dynamics. We use a nonadiabatic dynamics algorithm which allows the system to evolve on single adiabatic surfaces and on coherently coupled pairs of adiabatic surfaces. Reactive-flux correlation function expressions are used to compute the rate coefficients and the role of the dynamics on the coherently coupled surfaces is elucidated. © 2005 American Institute of Physics.
