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CHEMICAL SCIENCES DIVISION Annual Report 1992 September 1993

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CHEMICAL SCIENCES DIVISION Annual Report 1992 September 1993 LBL-34259 UC-401 CHEMICAL SCIENCES DIVISION Annual Report 1992 September 1993 Lawrence Berkeley Laboratory University of California Berkeley, California 94720 & Prepared for the U.S. Department of Energy under Contract No. DE-AC03-76SF00098 -y3 Contents REMARKS BY THE DIVISION DIRECTOR Charles B. Harris v CHEMICAL SCIENCES Fundamental Interactions Photochemical and Radiation Sciences Photochemistry of Materials in the Stratosphere Harold S. Johnston, Investigator 1 Chemical Physics Energy Transfer and Structural Studies of Molecules on Surfaces Charles B. Harris, Investigator 2 Laser Sources and Techniques Andrew H. Kung, Investigator 6 Crossed Molecular Beams Yuan T. Lee, Investigator 8 Molecular Interactions William A. Lester, Jr., Investigator. 14 Theory of Atomic and Molecular Collision Processes William H. Miller, Investigator 17 Selective Photochemistry C. Bradley Moore, Investigator 20 Photodissociation of Free Radicals Daniel M. Neumark, Investigator 24 Physical Chemistry with Emphasis on Thermodynamic Properties Kenneths. Pitzer, Investigator 27 Chemical Physics at High Photon Energies David'A. Shirley, Investigator 31 Atomic Physics Experimental Search for the Electron Electric Dipole Moment Eugene D. Commins, Investigator 36 High Energy Atomic Physics Harvey Could, Investigator 38 Atomic Physics Michael H. Prior, Investigator 40 Processes and Techniques Chemical Energy High-Energy Oxidizers and Delocalized-Electron Solids NeilBanletl, Investigator 44 Catalytic Hydrogenation of CO AlexT. Bell, Investigator 48 Transition Metal Catalyzed Conversion of CO, NO, H2 and Organic Molecules to Fuels and Petrochemicals Robert C. Bergman, Investigator 51 Formation of Oxyacids of Sulfur from SO2 Robert E. Connick, Investigator 56 Potentially Catalytic and Conducting Polyorganometallics K. Peter C. Vollhardt, Investigator 57 Heavy-Element Chemistry Actinide Chemistry Norman M. Edelstein, Richard A. Andersen, and Kenneth N. Raymond, Investigators 62 Chemical Engineering Sciences Molecular Thermodynamics for Phase Equilibria in Mixtures John M. Prausnitz, Investigator 72 WORK FOR OTHERS United States Office of Naval Research Normal and Superconducting Properties of High-Tc Systems Vladimir Z Kresin, Investigator 77 APPENDICES Appendix A: Division Personnel 79 Appendix B: Index of Investigators 83 REMARKS BY THE DIVISION DIRECTOR The Chemical Sciences Division (CSD) is one of This year, the Division also continued to place a strong twelve research Divisions of the Lawrence Berkeley emphasis on full compliance with environmental health and Laboratory, a Department of Energy National Laboratory. safety guidelines and regulations. In the coming years we The CSD is composed of individual groups and research will be looking at ways in which Chemical Sciences programs that are organized into five scientific areas: Division research can help strengthen United States' Chemical Physics, Inorganic/Organometallic Chemistry, industrial competitiveness both here and abroad, and how Actinide Chemistry, Atomic Physics, and Physical our research can better assist our nation's environmental Chemistry. The CSD is unique in that a good deal of our remediation efforts. Division's research activity occurs in laboratories located Awards and honors received by CSD investigators in on the campus of the University of California at Berkeley, FY 1992 include: involving students and faculty in the Department of Chemistry. Several large programs, notably the Actinide • Neil Bartlett received the American Chemical Chemistry Program and the Atomic Physics Program, are Society Award for Creative Work in Fluorine based at the Lawrence Berkeley Laboratory (LBL) site just Chemistry and received an Honorary Doctor of east of and above the University campus. The two sites, the Science degree from McMaster University, campus and the Laboratory, are linked by an efficient Hamilton, Ontario, Canada. minibus system that transports students, faculty, staff, and • Ali Belkacem received an LBL Outstanding visitors between the two institutions. Service Award. The benefits of close ties with the campus are broad • Alexis T. Bell received the 1992 R.H. Wilhelm and numerous. One of the most important of these is the Award in Chemical Reaction Engineering and was vigor, dedication, and high productivity that graduate an Irving Langmuir Lecturer at the Division of student research assistants bring to our various research Colloid and Surface Chemistry. projects. In addition, the Laboratory has a staff of highly • Y.T. Lee received the Faraday Medal, Royal skilled engineers and crafts technicians who support the Society of Chemistry, Great Britain, and received scientific mission, and it is the site of several major, world- an Honorary Doctor of Science degree from class user facilities such as the Advanced Light Source University of Rome, Italy; he was an Alstadt- (ALS). Combined, the two institutions represent a highly Lord-Mark Chair Lecturer, Polytechnic enriched research environment, attracting a large number of University, a Gooch-Stephens Lecturer at Baylor eminent scientists and leaders from all over the world— University, and a Hill Lecturer at Duke University. many of whom have close associations with the Chemical • William Lester, Jr. was elected as a Fellow of the Sciences research programs. American Association for the Advancement of In FY 1992 the Division continued to advance the Science and elected to the national board of Combustion Dynamics Initiative in support of DOE's AAAS, appointed to the Federal Networking national role in combustion research and chemical science. Council Advisory Committee, and appointed to The intent of the initiative is to achieve fundamental NSF's Blue Ribbon Panel on High Performance advances in understanding the structure and reactivity of Computing. critical reaction intermediates and transients and the • K.P.C. Vollhardt was selected as an Humboldt dynamics of elementary chemical reactions. The initiative Senior Scientist Awardee. envisions both experimental and theoretical efforts that would lead to accurate and reliable models for predicting combustion properties to improve the design of engines, Charles B. Harris burners, and other combustion devices. Division Director Chemical Sciences Division Chemical Sciences FUNDAMENTAL INTERACTIONS PHOTOCHEMICAL AND RADIATION SCIENCES Photochemistry of Materials in the appear to have caused global ozone reduction at mid- Stratosphere* latitudes. These reactions convert inactive chlorine species (HO and C1N03) to active forms (CI, CIO) and alter the concentration of hydroxy] radicals. Work here indicates Harolds. Johnston, Investigator that nitrosyl sulfuric acid (NOHSO4) may also convert inactive HC1 to active C1NO, and nitrosyl sulfuric acid hydrolyses under certain conditions to release HONO(g), which directly leads to ozone loss. INTRODUCTION This research is concerned with global change in the FY 1992 PUBLICATIONS AND REPORTS chemistry of the atmosphere, including theoretical and interpretative gas-phase and heterogeneous photochemistry. Work continues on writing up former graduate student Refereed Journals theses for publication. 1. B. Kim, P.L. Hunter, and H.S. Johnston, "N03 Radical Studied by Laser Induced Fluorescence," J. Chem. Phys., The principal investigator is (1) an advisor to the 96,4057 (1992); LBL-30869. Upper Atmosphere Research Program, Atmospheric Effects 2. J.D. Burley and H.S. Johnston, "Photoabsorption Cross of Stratospheric Aircraft, of the National Aeronautics and Sections of (FS03)2 and FSO3," J. Photochem. PhotobioI. Space Administration (NASA), (2) Trustee for the National A: Chem.«, 141 (1992); LBL-31547. Institute for Global Environmental Change, administered 3. J.D. Burley and H.S. Johnston, "Ionic Mechanisms for by the University of California, and (3) Member of the Heterogeneous Stratospheric Reactions and Ultraviolet + National Needs Task Force of the Lawrence Berkeley Photoabsorption Cross Sections for N02 , HNO3, and N03~ Laboratory. in Sulfuric Acid," Geophys. Res. Lett. 19, 1359 (1992); LBL-31660. 4. J.D. Burley and H.S. Johnston, "Nitrosyl Sulfuric Acid and Stratospheric Aerosols," Geophys. Res. Lett. 19, 1363 1. Heterogeneous Chemical Reactions in the (1992);LBL-32177. Stratosphere (Publications 3 and 4) For a few years, it has been known that heterogeneous Other Publications chemical catalysis, 5. H.S. Johnston, "Atmospheric Ozone," Annual Rev. Phys. Chem. 43,1 (1992); LBL-33576. HCl(g) + CIN03(g) - (cat.) -> Cl2(g) + HN03(s) , where the catalyst is ice or nitric acid trihydrate ice, and other heterogeneous reactions are an essential component Invited Talks of the Antarctic "ozone hole." In 1991, NASA scientists 6. H.S. Johnston, "Stratospheric Aircraft: Impact on Ozone?" found that heterogeneous hydrolysis reactions on aqueous The Chemistry of the Atmosphere: Its Impact on Global sulfuric acid aerosols Change, CHEMRAWN VII, A World Conference, Baltimore, MD, December 2-6,1991. N205(g) + H20 - (H2S04,'.) -» 2HN03(g) 7. H.S. Johnston, "Collisions! Deactivation of Highly Excited Nitriogen Dioxide," Physical Chemistry Colloquium, ClN03(g) + H20 - (H2S04,1)) -> HOCl(g) + HN03(g) University of Colorado, Boulder, CO, April 17,1992. This work was supported by the Director, Office of Energy Research. Office of Basic Energy Sciences, Chemical Sciences Division of the U. S. Department of Energy under Contract No. DE-ACO3-76SFO0O98. 1 CHEMICAL PHYSICS Energy Transfer and Structural Studies metal-insulator interface and of the dynamics of electrons in atomically
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