附註:Includes bibliographical references and index.
Cover -- Table of Contents -- Preface -- 1. Using Quantum Calculations of NMR Properties to Elucidate Local and Mid-Range Structures in Amorphous Oxides, Nitrides and Aluminosilicates -- 1 Introduction -- 2 Computational methods -- 3 Results -- 4 Conclusions -- 2. Molecular Modeling of Poly(ethylylene oxide) Melts and Poly(ethylene oxide) Based Polymer Electrolytes -- 1 Introduction -- 2 Technological importance of poly(ethylene oxide) -- 3 Molecular modeling of PEO oligomers and PEO melts -- 4 Molecular modeling of poly(ethylene oxide)/LiBF4 polymer electrolytes -- 5 Conclusions -- Appendix -- 3. Nanostructure Formation and Relaxation in Metal(100) Homoepitaxial Thin Films: Atomistic and Continuum Modeling -- 1 Introduction -- 2 General features of atomistic lattice-gas models for metal(100) homoepitaxy -- 3 Details of tailored atomistic lattice-gas modeling for Ag/Ag(100) -- 4 Atomistic and continuum modeling of Ag/Ag(100) film growth -- 5 Atomistic and continuum modeling of post-deposition relaxation for Ag/Ag(100) -- 6 Effect of a chemical additive (oxygen) on Ag/Ag(100) film evolution -- 7 Conclusions -- Appendix -- 4. Theoretical Studies of Silicon Surface Reactions with Main Group Absorbates -- 1 Introduction -- 2 Theoretical methods and surface models -- 3 2x1 reconstruction of a clean silicon surface -- 4 Hydrogenation of the reconstructed Si(100) surface -- 5 Adsorbates containing the Group 3 element boron -- 6 Adsorbates containing Group 4 elements -- 7 Adsorbates containing Group 5 elements -- 8 Adsorbates containing Group 6 elements -- 9 Adsorption and etching of Si(100) with halogen, adsorbates containing Group 7 elements -- 10 Summary and outlook -- 5. Quantum-Chemical Studies of Molecular Reactivity in Nanoporous Materials -- 1 Introduction -- 2 Structural models and computational methods -- 3 Survey of reactivity studies -- 4 Conclusions -- 6. Theoretical Methods for Modeling Chemical Processes on Semiconductor -- 1 Introduction -- 2 Geometrical
摘要:As a result of the advancements in algorithms and the huge increase in speed of computers over the past decade, electronic structure calculations have evolved into a valuable tool for characterizing surface species and for elucidating the pathways for their formation and reactivity. It is also now possible to calculate, including electric field effects, STM images for surface structures. To date the calculation of such images has been dominated by density functional methods, primarily because the computational cost of - curate wave-function based calculations using either realistic cluster or slab models would be prohibitive. DFT calculations have proven especially valuable for elucidating chemical processes on silicon and other semiconductor surfaces. However, it is also clear that some of the systems to which DFT methods have been applied have large non-dynamical correlation effects, which may not be properly handled by the current generation of Kohn-Sham-based density functionals. For example, our CASSCF calculations on the Si(001)/acetylene system reveal that at some geometries there is extensive 86 configuration mixing. This, in turn, could signal problems for DFT cal- lations on these systems. Some of these problem systems can be addressed using ONIOM or other "layering" methods, treating the primary region of interest with a CASMP2 or other multireference-based method, and treating the secondary region by a lower level of electronic structure theory or by use of a molecular mechanics method. ACKNOWLEDGEMENTS We wish to thank H. Jónsson, C. Sosa, D. Sorescu, P. Nachtigall, and T.-C.
