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Chemical Structure and Dynamics PNL-12154 UC-400 Annual Report 1998 Chemical Structure and Dynamics Steven D. Colson, Associate Director Robin S. McDowell, Program Manager and the Staff of the Chemical Structure and Dynamics Program March 1999 Prepared for the U.S. Department of Energy under Contract DE-AC06-76RLO 1830 Pacific Northwest National Laboratory Operated by Battelle for the U.S. Department of Energy DISCLAIMER This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor Battelle Memorial Institute, nor any of their employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof, or Battelle Memorial Institute. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. PACIFIC NORTHWEST NATIONAL LABORATORY operated by BATTELLE for the UNITED STATES DEPARTMENT OF ENERGY under Contract DE-AC06-76RL01830 Printed in the United States of America Available to DOE and DOE contractors from the Office of Scientific and Technical Information, P.O. Box 62, Oak Ridge, TN 37831-0062; ph: (865) 576-8401 fax: (865) 576-5728 email: [email protected] Available to the public from the National Technical Information Service, U.S. Department of Commerce, 5285 Port Royal Rd., Springfield, VA 22161 ph: (800) 553-6847 fax: (703) 605-6900 email: [email protected] online ordering: http://www.ntis.gov/ordering.htm This document was printed on recycled paper. (8/00) Chemical Structure and Dynamics 1998 Annual Report Contents Femtosecond Laser-Induced Desorption of Positive Ions from Ionic Solidsa R. M. Williams, K. M. Beck, A. G. Joly, 1. Introduction........................................... 1-1 J. T. Dickinson, and W. P. Hess..................... 3-4 Photochemistry and Product Structures 2. Reaction Mechanisms at Interfaces of Matrix-Isolated Acetyl Chloridea J. B. Rowland, P. R. Winter, Structure and Reactivity G. B. Ellison, and W. P. Hess........................ 3-6 of Ice Surfaces and Interfacesa K. P. Stevenson, Z. Dohnalek, The UV Photodissociation of a R. L. Ciolli, G. A. Kimmel, Matrix-Isolated Propionyl Chloride R. S. Smith, and B. D. Kay ........................... 2-1 P. R. Winter, J. B. Rowland, W. P. Hess, J. G. Radziszewski, Ozone Decomposition M. R. Nimlos, and G. B. Ellison .................... 3-9 in Soot Aerosolsb R. S. Disselkamp, M. A. Carpenter, Experimental and Theoretical and J. P. Cowin .......................................... 2-7 Investigations of Electron Diffraction in Stimulated Desorptiona c The Structure of Iron Oxides Surfaces M. T. Sieger, G. K. Schenter, S. A. Joyce and S. A. Chambers...................... 2-9 and T. M. Orlando .....................................3-11 Photoionization of Liquid Water Electron-Stimulated Desorption Using a Newly-Constructed and Reactive Scattering a Liquid Beam Source in Nanoscale Ice Filmsa R. G. Tonkyn, N. Petrik, M. T. Sieger, W. C. Simpson, S. E. Barlow, and T. M. Orlando...................2-11 K. A. Briggman, and T. M. Orlando..............3-13 A Soft-Landing Ion Beam Vehicle Exhaust Treatment a for Re-Creating Ionic Interfaces Using Electrical Discharge Methodsf J. P. Cowin and M. J. Iedema........................2-12 R. G. Tonkyn, S. E. Barlow, Soft-Landed Ion Study of Watera T. M. Orlando, I. S. Yoon, A. C. Kolwaite, J. P. Cowin, M. J. Iedema, M. L. Balmer, and J. Hoard..........................3-15 A. A. Tsekouras, et al..................................2-14 Production of Molecular Oxygen Phase Transfer of Hydrated Ionsa on Icy Satellites via Electronic Excitationa K. Wu, J. P. Cowin, T. M. Orlando, M. T. Sieger, M. J. Iedema, and A. A. Tsekouras ................2-18 and W. C. Simpson ....................................3-16 Low-Energy Electron Impact of Sodium Nitrate Crystals 3. High-Energy Processes at and Adsorbed Methanol Overlayersc Environmental Interfaces N. G. Petrik, D. Camaioni, and T. M. Orlando .....................................3-18 Characterization of Nanocomposite Materials Prepared via Laser Ablation Stimulated Luminescence of a,d,e c of Pt/TiO2 Bi-Combinant Targets Yttria-Stabilized Cubic Zirconia Crystals K. M. Beck, T. Sasaki, and N. Koshizaki .......... 3-1 N. G. Petrik, D. P. Taylor, and T. M. Orlando .....................................3-20 iii Chemical Structure and Dynamics 1998 Annual Report 4. Cluster Models of the Three Dimensional Vibrational Condensed Phase Imaging by Coherent g Cluster Model Studies of the Structure Anti-Stokes Raman Scattering and Bonding of Environmentally- A. Zumbusch, G. R. Holtom, Important Materialsa and X. S. Xie.............................................5-13 L. S. Wang, J. B. Nicholas, S. D. Colson, Single-Molecule Enzymatic Dynamicsa H. Wu, X. B. Wang, C. F. Ding, H. P. Lu, L. Xun, and X. S. Xie....................5-14 and X. Li................................................... 4-1 Fluorescence Spectroscopy Photodetachment Photoelectron Spectroscopy and Exciton Dynamics of a of Multiply Charged anionsa Single Allophycocyanin Trimers L. S. Wang, X. B. Wang, and C. F. Ding......... 4-2 L. Ying and X. S. Xie..................................5-17 Photoelectron Spectroscopy and 6. Appendix Electronic Structure of Metal Clusters and Chemisorbed Metal–Cluster Complexesd CS&D Staff..................................................... 6-1 L. S. Wang, H. Wu, X. B. Wang Publications and Presentations C. F. Ding, X. Li, and W. Chen ..................... 4-5 Publications ............................................. 6-6 Study of Transition Metal– In Press and Submitted ............................. 6-8 Carbon Mixed Clustersd Patents....................................................6-10 L. S. Wang, X. B. Wang, H. Wu, Presentations...........................................6-10 W. Chen, X. Li, and H. S. Cheng ................... 4-7 Honors and Recognition.................................6-15 Time-Resolved Spectroscopy Visitors .........................................................6-16 of Solute/Solvent Clustersa Collaborations D. M. Laman, A. G. Joly, and D. Ray ............. 4-9 External Collaborations............................6-17 Collaborations within PNNL .....................6-19 5. Miscellaneous Acronyms and Abbreviations .........................6-21 Where CS&D Fits in PNNL ..............................6-21 High-Resolution Infrared Spectroscopy: Basic and Applied Researchg,h S. W. Sharpe, T. A. Blake, and R. L. Sams ....... 5-1 Characterization of Funding Support Quantum-Cascade Lasersg,h a S. W. Sharpe, J. F. Kelly, J. S. Hartman, DOE Office of Basic Energy Sciences, Chemical C. Gmachl, F. Capasso, D. L. Sivco, Sciences Division, Fundamental Interactions J. N. Baillargeon, and A. Y. Cho .................... 5-3 Branch. bPacific Northwest National Laboratory (PNNL) Demonstration of the Laboratory Directed Research and Development Asymmetric Ion Trapg (LDRD). S. E. Barlow and M. L. Alexander.................. 5-6 cDOE Environmental Management Science Pro- + Radiative Association of Cs gram (EMSP). a,g with 12-crown-4 Ether at 288 K dNational Science Foundation. S. E. Barlow and M. D. Tinkle ....................... 5-9 eAgency of Industrial Science and Technology, A New Approach to Near-Field Japan. Fluorescence Microscopy: fCooperative Research and Development Agree- g Two-Photon Excitation with Metal Tips ment (CRADA) with the Low Emissions Technol- E. J. Sánchez, L. Novotny, and X. S. Xie ........5-11 ogy Research and Development Partnership. gEMSL Operations, supported by DOE Office of Biological and Environmental Research. hDepartment of Energy. iv Chemical Structure and Dynamics 1998 Annual Report The CS&D group has particular expertise in the 1. Introduction preparation and spectroscopic analysis of molecu- lar clusters (S. D. Colson, D. Ray, S. W. Sharpe, Purpose and L. S. Wang); ultrafast and nonlinear optical spectroscopies (D. Ray, G. R. Holtom, and X. Xie); The Chemical Structure and Dynamics (CS&D) ultrahigh resolution spectroscopy for measure- program is a major component of the William R. ments of electronic and geometric structures and Wiley Environmental Molecular Sciences Labo- dynamics (S. W. Sharpe and R. S. McDowell); sur- ratory (EMSL), developed by Pacific Northwest face and interface structure, chemical reaction National Laboratory (PNNL) to provide a state-of- dynamics, and kinetics (J. P. Cowin, W. P. Hess, S. the-art collaborative facility for studies of chemical A. Joyce, B. D. Kay, and T. M. Orlando); ion-mole- structure and dynamics. We respond to the need cule traps and storage technology (S. E. Barlow); for a fundamental, molecular-level understanding and specialized chambers and instruments for of chemistry at a wide variety of environmentally chemical reactivity and analysis of atmospheric important interfaces by (1) extending the aerosols (S. E. Barlow and R. S. Disselkamp). experimental characterization and theoretical description of chemical reactions to encompass the effects of condensed media and interfaces; (2) Environmental
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