Quantum molecular dynamic application

Finally, Sections B3.4.10. touches on the application of quantum molecular dynamics to a very exciting field laser interactions with molecules. This field presents, in principle, the opportunity to influence chemistry by lasers rather than to simply observe it. 

Zhang J Z H 1999 Theory and Application of Quantum Molecular Dynamics (River Edge, NJ World Scientific)... 

In molecular dynamics applications there is a growing interest in mixed quantum-classical models various kinds of which have been proposed in the current literature. We will concentrate on two of these models the adiabatic or time-dependent Born-Oppenheimer (BO) model, [8, 13], and the so-called QCMD model. Both models describe most atoms of the molecular system by the means of classical mechanics but an important, small portion of the system by the means of a wavefunction. In the BO model this wavefunction is adiabatically coupled to the classical motion while the QCMD model consists of a singularly perturbed Schrddinger equation nonlinearly coupled to classical Newtonian equations, 2.2. 

Garcia-Vela, A., Gerber, R. B. Hybrid quantum-semiclassical wave packet method for molecular dynamics Application to photolysis of Ar...HCl. J. Chem. Phys. 98 (1993) 427-43... 

In this paper we present a number of time integrators for various problems ranging from classical to quantum molecular dynamics. These integrators share some common features they are new, they are second-order accurate and time-reversible, they improve substantially over standard schemes in well-defined model situations — and none of them has been tested on real applications at the time of this writing. This last feature will hopefully change in the near future [20]. 

The Car-Parrinello quantum molecular dynamics technique, introduced by Car and Parrinello in 1985 [1], has been applied to a variety of problems, mainly in physics. The apparent efficiency of the technique, and the fact that it combines a description at the quantum mechanical level with explicit molecular dynamics, suggests that this technique might be ideally suited to study chemical reactions. The bond breaking and formation phenomena characteristic of chemical reactions require a quantum mechanical description, and these phenomena inherently involve molecular dynamics. In 1994 it was shown for the first time that this technique may indeed be applied efficiently to the study of, in that particular application catalytic, chemical reactions [2]. We will discuss the results from this and related studies we have performed. 

John Z. H. Zhang, Theory and Applications of Quantum Molecular Dynamics, World Scientific, Singapore, 1999. 

Latterly, increasing use has also been made of Quantum Molecular Dynamics (QMD), based on the pioneering work of Car and Parrinello (1985) (see Chapter 8). The Car-Parrinello method makes use of Density Functional Theory to calculate explicitly the energy of a system and hence the interatomic forces, which are then used to determine the atomic trajectories and related dynamic properties, in the manner of classical MD. As an ab initio technique, QMD has the advantage over classical simulation methods that it is not reliant on interatomic potentials, and should in principle lead to far more accurate results. The disadvantage is that it demands far greater computing resources, and its application has thus far been limited to relatively simple systems. 

Zhang JZH (1989) Theory and application of quantum molecular dynamics. World Scientific, Singapore, pp 333... 

Fifteen years ago Roberto Car of Princeton Uiuversity and Michele Parrinello of Max Planck Institute introduced a method that revolutionized electronic structure calculations for molecules, liquids and solids. In addition, this method called the Car-Parrinello Method also opened the field of quantum molecular dynamics for physicists. The Car-Parrinello algorithm allows for rigorous evaluation of molecular dynamics in clusters, solids and surfaces. Ursula Rothlisberger, a former member of the Parrinello s group, reviews the formations of the methods in its most common implementations in chapter two. She provides a munber of examples of applications of this powerful technique. Also, predictions of future directions of the methods are given in her chapter. 

By its nature, the application of direct dynamics requires a detailed knowledge of both molecular dynamics and quantum chemistry. This chapter is aimed more at the quantum chemist who would like to use dynamical methods to expand the tools at theh disposal for the study of photochemistry, rather than at the dynamicist who would like to learn some quantum chemishy. It hies therefore to introduce the concepts and problems of dynamics simulations, shessing that one cannot strictly think of a molecule moving along a trajectory even though this is what is being calculated. 

It seems that surface hopping (also called Molecular Dynamics with Quantum Transitions, MDQT) is a rather heavy tool to simulate proton dynamics. A recent and promising development is path integral centroid dynamics [123] that provides approximate dynamics of the centroid of the wavefunctions. Several improvements and applications have been published [123, 124, 125, 126, 127, 128). 

Bala, R, Lesyng, B., McCammon, J.A. Extended Hellmann-Feynman theorem for non-stationary states and its application in quantum-classical molecular dynamics simulations. Chem. Phys. Lett. 219 (1994) 259-266. 

P. Bala, P. Grochowski, B. Lesyng, and J. A. McCammon Quantum-classical molecular dynamics. Models and applications. In Quantum Mechanical Simulation Methods for Studying Biological Systems (M. Fields, ed.). Les Houches, France (1995)... 

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