This workshop will bring together mathematicans, chemists, physicists, biologists and researchers from other disciplines whose work pertains to statistical mechanics and molecular dynamics used in simulations of biomolecular, chemical, and liquid or solid state systems. We will consider key aspects of molecular simulations--numerical algorithms, mathematical analysis and applications--paying special attention to problems that call for new methodologies or mathematics. Relevant topics include sampling methods, methods for free energy calculation, reaction pathways and reaction rates, long-time integration, geometric integrators, trajectory analysis, stochastic and Monte Carlo methods, and Car-Parrinello dynamics. Numerical methodologies, mathematical theory, and applications will be discussed.