Airlie Conference Center Warrenton, Virginia October 24-27, 2004 Chemical Sciences, Geosciences & Biosciences Division Cover Top Structure and Dynamics of Chemical Processes in Water Clusters K. D. Jordan Dept. of Chemistry, University of Pittsburgh, Pittsburgh, PA. 15260 and M. A. Johnson, Dept. of Chemistry, Yale University, New Haven CT 06520 Comparison of the experimental (lower) and theoretical (upper) spectra for the water - tetramer anion. Spectra A and C refer to (H2O)4 in the water bending region, while B and - D correspond to the (D2O)4 isotopomer in the OD stretching region. Bottom Optical Manipulation of Ultrafast Electron and Nuclear Motion on Metal Surfaces Hrvoje Petek, Department of Physics and Astronomy, University of Pittsburgh, Pittsburgh, PA 15260 a) 3D plot of 2 photon photoemission spectra of Cs/Cu(111) at 300 K as a function of Cs coverage. The dotted line indicates approximate shift in the energy of the antibonding state A with coverage. b) detail of the photoemission spectra in a) showing the tuning of A through the resonance with surface state. Foreword This volume summarizes the scientific content of the 2004 Research Meeting on Condensed Phase and Interfacial Molecular Science (CPIMS) sponsored by the U. S. Department of Energy (DOE), Office of Basic Energy Sciences (BES). This meeting marks the initiation of a new BES Contractor's Research meeting that will focus on the molecular-level understanding of complex physical and chemical processes in condensed phases and at interfaces. The meeting features the participation of 71 principal investigators from the following core research activities and nanoscale science initiative programs: Chemical Physics Program (36), Photochemical and Radiation Sciences Program (21), Atomic, Molecular and Optical Sciences Program (3), Nanoscale Science, Engineering and Technology/Theory, Modeling and Simulation in Nanoscience (11). The research described here is supported by the Chemical Sciences, Geosciences and Biosciences Division of BES, through the Fundamental Interactions Team, with an approximate annual funding level of $16.6 M. The agenda reflects some of the research topics covered within the broad CPIMS theme, including: structure and dynamics of liquid water, chemistry of metal clusters, physical and chemical processes induced by low-energy electrons in aqueous solutions, dynamics and reactions on surfaces, optical and electronic responses in nanoscale materials, and probing or manipulation of single molecules at interfaces. Theory and experiment is well integrated throughout, indicative of the need for both in understanding these complex systems. Contractor Research meetings are intended to facilitate an understanding of BES programmatic goals, enhance the alignment of fundamental research efforts with those goals, and foster new ideas and collaborations among the participants. The three Contractors' meetings currently sponsored by our Team (Combustion, AMOS and Solar Photochemistry) are passing the quarter-century mark in longevity and are very highly regarded by their participants. I sincerely hope that CPIMS will become another successful Contractors’ meeting in our long-standing tradition. CPIMS differs in one important respect from the others in that it includes participation from all of the core research areas within our Team. Thus, it does not coincide with a single box on our organizational chart. However, from the PIs’ perspective, a “program” is defined more by the annual Contractors’ Meeting than by boxes on a BES organizational chart. I urge the participants to provide feedback to us on how well CPIMS has succeeded (or failed) in this regard and on ways it can be improved in future years. I am delighted that the program managers from our Team, Mary Gress, Frank Tully and Dick Hilderbrandt, and our Division director, Walt Stevens, will be attending the meeting. I gratefully acknowledge the contributions of this year’s speakers for their investment of time and for their willingness to share their ideas with the meeting participants. Thanks also go to Dick Hilderbrandt for assembling the book of abstracts, and to Diane Marceau from BES, Sophia Kitts and Kellye Sliger from Oak Ridge Institute of Science and Education, and the staff of the Airlie Conference Center for taking care of the logistical aspects of the meeting. Eric Rohlfing Team Leader, Fundamental Interactions Chemical Sciences, Geosciences and Biosciences Division Office of Basic Energy Sciences September 2004 Agenda U. S. Department of Energy Office of Basic Energy Sciences 2004 Meeting on Condensed Phase and Interfacial Molecular Sciences Sunday, October 24 3:00-6:00 pm **** Registration **** 6:00 pm **** Reception (No Host) **** 7:00 pm **** Dinner **** Monday, October 25 7:00 am **** Breakfast **** 8:00 am Introductory Remarks Walter Stevens and Eric Rohlfing, BES/DOE Session I Chair: Eric Rohlfing 8:30 am Dynamics of Nanoscopic Water: Ultrafast Vibrational Echo Experiments on Reverse Micelles Michael Fayer, Stanford University 9:00 am Probing Water Confined in Reverse Micelles through Quasielastic Neutron Scattering and Molecular Dynamics Simulations Nancy Levinger, Colorado State University 9:30 am The Dynamics and Kinetics of Hydrogen Bonds in Water Andrei Tokmakoff, MIT 10:00 am **** Break **** 10:30 am Development of a New Polarizable, Flexible Interaction Potential for Water: From Clusters to Liquid Water and Ice Sotiris Xantheas, PNNL 11:00 am Optical Spectroscopy at the Spatial Limit Wilson Ho, UC Irvine 11:30 am Semiempirical Representations of Molecular Interaction for Statistical Mechanical Simulation Greg Schenter, PNNL 12:00 pm **** Lunch **** 5:00 pm **** Reception (No Host) **** 6:00 pm **** Dinner **** Session II Chair: Scott Anderson 7:00 pm Clusters: Unraveling Fundamental Oxygen-Transfer Reaction Mechanisms Effected by Heterogeneous Catalysts Will Castleman, Penn State 7:30 pm Structure and Dynamics in Metal-Molecular Complexes via IR Spectroscopy Michael Duncan, University of Georgia 8:00 pm Computational Electron Spectroscopy: A Powerful Tool for Studies of Size-, Structure-, Charge State-, and Composition-Specific Properties of Finite Systems Julius Jellinek, Argonne National Laboratory 8:30 pm Gas-Phase Transition Metal Containing Molecules: Electronic Structure and Bonding Tim Steimle, Arizona State University Tuesday, October 26 7:30 am **** Breakfast **** Session III Chair: Bruce Garrett 8:30 am Dynamics of Low Energy Electrons in Ion Radiolysis of Aqueous Systems Simon Pimblott, Notre Dame Radiation Laboratory 9:00 am Electron-Driven Chemistry: The Challenge to Theory Bill McCurdy, LBNL 9:30 am Low Energy Electron Interactions with Complex Targets Thom Orlando, Georgia Tech 10:00 am **** Break **** 10:30 am Electron-Stimulated Reactions at the Interfaces of Thin Water Films Greg Kimmel, PNNL 11:00 am Delocalized Charges and Excitations in Molecular Materials Paul Barbara, University of Texas 11:30 am How Water Networks Accommodate an Excess Electron: Structure and Dynamics of the Binding Site through Cluster Spectroscopy Mark Johnson, Yale University and Ken Jordan, Univ. of Pittsburgh 12:10 pm **** Lunch **** Session IV Chair: Ian Harrison 4:00 pm Dynamics of Electrons at Interfaces on the Femtosecond Timescale Charles Harris, LBNL 4:30 pm Eley-Rideal and Hot Atom Reactions between H Atoms on Metal and Graphite Surfaces Bret Jackson, University of Massachusetts 5:00 pm Self-Organization and Oxidative Surface Reaction Dynamics of Condensed Phase Systems Steve Sibener, University of Chicago 5:30 pm A Combined QM/MM and Kinetic Monte Carlo Approach to Surface Science Mark Gordon, Ames National Laboratory 6:00 pm **** Reception (No Host) **** 7:00 pm **** Dinner **** Wednesday, October 27 7:00 am **** Breakfast **** Session V Chair: Frank Tully 8:00 am Recent Progress Understanding Slow Dynamics and Aging David Chandler, LBNL 8:30 am Computational Nanophotonics Steve Gray, Argonne National Laboratory 9:00 am Scalable Methods for Electronic Excitations and Optical Responses of Nanostructures Steven Louie, LBNL 9:30 am **** Break **** 10:00 am Single Molecule Conformational and Enzymatic Dynamics Sunney Xie, Harvard University 10:30 am Beakers Without Walls: Formation of Deeply-Supercooled Solutions from Nanoscale Amorphous Solid Films Bruce Kay, PNNL 11:00 am Single-Molecule Spectroscopy and Dynamics of Nanoscale Interfacial Rate Processes Peter Lu, PNNL 11:30 pm Closing Remarks Eric Rohlfing, BES/DOE 11:45 am **** Lunch **** (Optional boxed lunches available) Table of Contents Invited Presentations (Ordered by Agenda) Solvent Dynamics and Photoinduced Electron Transfer in Complex Molecular Systems Michael D. Fayer....................................................................................................1 “Fundamental Properties of Solvent Pools of Reverse Micelles Used in Nanoparticle Synthesis” Nancy E. Levinger and Branka M. Ladanyi .......................................................5 Structural Dynamics in Complex Liquids Studied with Multidimensional Vibrational Spectroscopy Andrei Tokmakoff .................................................................................................8 Molecular Theory & Modeling: Development of a new polarizable, flexible interaction potential for water: From clusters to liquid water and ice Sotiris S. Xantheas ...............................................................................................10 Optical Spectroscopy at the Spatial Limit Wilson Ho .............................................................................................................15