Skip to main content

Computational Chemical Dynamics of Complex Systems


EMSL Project ID
20893

Abstract

The goal of this project is to apply powerful new simulation techniques to tackle computationally challenging problems in chemical dynamics, with special emphasis on electrochemistry, heterogeneous catalysis, nanoparticles, solid-state dynamics, and photochemistry. These calculations will be carried out with new high-throughput integrated software that we are developing. New research capabilities in computational chemical dynamics are expected to play a significant role in enabling environmental scientists worldwide to address environmental challenges facing DOE and the nation. Recent advances in computer power and algorithms have made possible accurate calculations of many chemical properties for both equilibria and kinetics. Nonetheless, applications to complex chemical systems, such as reactive processes in the condensed phase, remain problematic due to the lack of a seamless integration of computational methods that allow modern quantum electronic structure calculations to be combined with state-of-the-art methods for chemical thermodynamics and reactive dynamics. These problems are often exacerbated by unvalidated methods and limited software reliability. Our consortium is developing an integrated software suite that combines electronic structure packages with dynamics codes and efficient sampling algorithms for the following kinds of condensed-phase modeling problems that we propose to tackle in various parts of the present Grand Challenge project: thermochemical kinetics and rate constants, photochemistry and spectroscopy, chemical and phase equilibria, electrochemistry, and heterogeneous catalysis. These fundamental areas of research are important for solar energy, fuel-cell technology, environmental remediation, weather modeling, pollution modeling, and atmospheric chemistry. Photochemical creation of excited states offers a means to control chemical transformations because different wavelengths of light can be used to create different vibronic states, thereby directing chemical reactions along different pathways. It is crucial to understand how energy deposited into the system is used; this is particularly complicated in condensed phase systems where there are many ways to dissipate excess energy. Similar opportunities and challenges present themselves in the areas of electrochemistry and catalysis. We therefore propose to carry out prototype large-scale applications on environmental problems as well as other applications to complex chemical dynamics processes, focusing on three high-impact areas. In the computational electrochemistry area, we will be especially concerned with processes that enhance the design of fuel cell technology and with the calculation of in situ reduction potentials. For heterogeneous, nanoparticle, and solid-state dynamics, we will develop an array of methods for multi-time-scale simulation of nucleation of crystals in solution, reactions of radicals at solution-phase interfaces and in ice, zeolite catalysis, structure and dynamics of gallazane precursors to gallium nitride nanocrystals, the regulatory role of metal ions in the reactivity of inorganic phosphates, nanoparticles structure and dynamics, and ice dynamics. In the computational photochemistry area, we will construct potential energy surfaces for a number of photochemical reactions and employ them for dynamics calculations based on the new decay of mixing with coherent switches algorithm. We will also consider solvatochromic shifts on conical intersections that govern selected photo chemical processes.


Project Details

Project type
Capability Research
Start Date
2006-10-01
End Date
2009-09-30
Status
Closed

Team

Principal Investigator

Donald Truhlar
Institution
University of Minnesota

Team Members

Boris Averkiev
Institution
University of Minnesota

Brian White
Institution
University of Minnesota

Ke Yang
Institution
Yale University

Manjeera Mantina
Institution
University of Minnesota

Ewa Papajak
Institution
University of Minnesota

Bo Wang
Institution
University of Minnesota

Lucas Fiedler
Institution
University of Minnesota

Hannah Leverentz
Institution
University of Minnesota

Ryan Olson
Institution
University of Minnesota

Aleksandr Marenich
Institution
University of Minnesota

Yao Fan
Institution
University of Minnesota

Jingjing Zheng
Institution
University of Minnesota

Kelly Anderson
Institution
University of Minnesota

Christopher Mundy
Institution
Pacific Northwest National Laboratory

Ashley Jay
Institution
University of Minnesota

Karol Kowalski
Institution
Pacific Northwest National Laboratory

Kwangho Nam
Institution
University of Minnesota

Jake Rafferty
Institution
University of Minnesota

Shuhua Ma
Institution
University of Minnesota

Alessandro Cembran
Institution
University of Minnesota

Yan Zhou
Institution
University of Minnesota

Wangshen Xie
Institution
University of Minnesota

Kiniu Wong
Institution
University of Minnesota

Joseph Scanlon
Institution
University of Minnesota

Oksana Tishchenko
Institution
University of Minnesota

Anastassia Sorkin
Institution
University of Minnesota

Rosendo Valero Montero
Institution
University of Minnesota

Zhen Li
Institution
University of Minnesota

Pablo Jaque
Institution
University of Minnesota

Mark Iron
Institution
Weizmann Institute

Andreas Heyden
Institution
University of South Carolina

Ming-kang Tsai
Institution
Brookhaven National Laboratory

Peng-Dong Fan
Institution
Pacific Northwest National Laboratory

Bojana Ginovska
Institution
Pacific Northwest National Laboratory

Elizabeth Amin
Institution
University of Minnesota

Erin Dahlke
Institution
University of Minnesota

Vassiliki-Alexandra Glezakou
Institution
Pacific Northwest National Laboratory

Ben Ellingson
Institution
University of Minnesota

Yan Zhao
Institution
University of Minnesota

Steven Mielke
Institution
University of Minnesota

Mark Cunningham
Institution
University of Texas-Pan American

Arindam Chakraborty
Institution
Syracuse University

Benjamin Lynch
Institution
University of Minnesota

Michel Dupuis
Institution
University at Albany, State University of New York

Joern Siepmann
Institution
University of Minnesota

Christopher Cramer
Institution
University of Minnesota

Gregory Schenter
Institution
Pacific Northwest National Laboratory

Shawn Kathmann
Institution
Pacific Northwest National Laboratory

Marat Valiev
Institution
Environmental Molecular Sciences Laboratory

Jiali Gao
Institution
University of Minnesota

Darrin York
Institution
University of Minnesota