Selective Control of Rugged Energy Landscapes: Structural and Dynamical Studies of Encapsulated Clusters

Brown University, Providence RI

Investigators

Abstract

Jimmy Doll of Brown University and David Freeman of the University of Rhode Island are supported by the Theoretical and Computational Chemistry Program for research that addresses theoretical issues concerning the prediction, characterization, and control of the structure and dynamics of cluster-based precursors. This effort seeks to invert the logic of the minimization problem, by undertaking to reshape energy landscapes and thereby to exercise control over selected physical systems. In particular, this research aims to learn to stabilize and/or chemically trap cluster conformers that are otherwise either unstable or metastable. The project goals are to (1) identify possible approaches for achieving thermodynamic and kinetic control of selected cluster structures, (2) establish those observables that provide the most sensitive signatures of relevant cluster structure and dynamics, and (3) assist in the interpretation of experimental data relevant to those observables. To promote the interplay between experimental and theoretical observations, collaboration with experimentalists at Argonne National Laboratory is planned. Computer simulations have proved to be useful tools that aid in predicting the properties of new materials. With the development of new synthetic methods that use nanoscale clusters as fundamental building blocks, computational studies of clusters are expected to grow in importance. The outcomes of this research are expected to provide the necessary experience and background to help determine methods for controlling structures and properties of the component parts for materials composed of clusters, with likely applications in chemistry, biology, and materials science.