In Li-FCH3 and Li-FH

Total Page:16

File Type:pdf, Size:1020Kb

In Li-FCH3 and Li-FH Alkali-Metal Harpooning Reactions in Li-FCH3 and Li-FH A thesis submitted in conformity with the requirements for the degree of Doctor of Philosophy, Graduate Department of Chemistry, University of Toronto. @Copyright by HanBin Oh National Library Bib1iothèq.de nationaie du Canada Acquisitions and Acquisitions et Bibliographie Services services bibliographiques 395 Wellington Street 395, rue Wellington OttawaON K1AON4 Ottawa ON 'K1A ON4 Canada Canada The author has granted a non- L'auteur a accordé une licence non exclusive licence allowing the exc1wive pennettant à la National Lhrary of Canada to Bibliothèque nationale du Canada de reproduce, loan, distribute or sell reproduire, prêter, distribuer ou copies of this thesis in microfoxm, vendre des copies de cette thèse sous paper or electronic formats. la forme de microfichelfilm, de reproduction sur papier ou sur format électronique. The author retains ownership of the L'auteur conserve la propriété du copyright in this thesis. Neither the droit d'auteur qui protège cette thèse. thesis nor substantial extracts fkom it Ni la thèse ni des extraits substantiels may be printed or otherwise de celle-ci ne doivent être imprimés reproduced without the author's ou autrement reproduits sans son permission. autonsation. Thesis Abstract Alkali-Metal Harpooning Reactions in Li-FCH l3 and LieeFH HanE3in Oh For the degree of Doctor of Philosophy, Department of Chemisftry, University of Toronto 2ao 1 The van der Waals complexes, Lib4FCH3and Li..FH, have been forrned for the first time. using a laser-ablation method. The complexes were identified by photoionization tirne-of-fiight mass spectrometry. The excitation of the complexes accessed selected configura'tions of the Transition State (TS) of the electronically-excited reaction, ~i'(2p~~)+ XR -, LiX + R, leading thereafter to depletion of the complexes. Depletion oif complexes was obser~edacross a broad range of excitation wavelengths. 'The experimentally observed depletion spectrum was compared to the results oTf ab initio calculations, perfomed by others. These ab inifio calculations permitted identification of the electronically- excited states reached by photoexcitatiorn of the Li..XR complex and assisted in the interpretation of the depletion spectra. Reaction proceeds by surface- hopping from the TS to the ground state; the TS lifetime was obtained by an optical saturation method, and was founai to be 5 1.3ns for both Li reactions. To Boln, SuMin, and JiHye Acknowledgements I sincerely thank John Polanyi for his guidance and support during my stay in Toronto. I have gained a lot of confidence while working under his guidance. I have learned from him that the physical insight and the understanding of nature are far more important than any technical details. I am indebted to Andrew Hudson for teaching me experimental techniques. I have enjoyed working companionship with him for last 4 years. I would like to thank TaeGeol, Javier, Jiaxi, and Sergei for providing a cozy environment in the laboratotyloffice and for their wam welcome-smile every morning. Duncan has always been kind to me whenever I needed his heip. Maria and Anastasia have patiently listened to my complaints and silly stories. Fedor Naumkin explained his theoretical results to me in a very understandable language. Especially his calculations for Li..FCH3 were so great than even 1 were able to appreciate it irnrnediately! Prof. Piotr Piecuch was a good mentor to me and showed me the beauty of ab initio calculations. Serguei Raspopov patiently followed al1 the algebra and corrected the wrong equation for TS lifetime. I think that I could not finish rny Ph.D without Boln's sacrifice and her endless love. Boln spent the whole summer parenting SuMin and JiHye while I was struggling with writing my poor thesis. I sincerely thank my parents, parents- in-law, BoAe, SungHan, and HanJong for being supportive and encouraging me al1 the time. iii Table of Contents Chapter 1- Introduction 1-1. Chernical Dynamics of the reaction event 2 History of TSS Line broadening in non-reactive system Line broadening in the reactive system Continuum resonance Raman Scattering (Bound-free transition) TSS in van der Waals complexes Negativeion photoelectron spectroscopy Femtosecond Tmnsition Spectroscopy (FTS) TSS performed previously in thiJ labaratory 1-3. Alkali metal reaction with halide molecule M + X2 reaction M + CHgreaction M + HX reaction 4. Thesis preview Chapter 2. Experiments 24. Apparatus 2-1 Vacuum system 2-1-2. Laser-ablation method Motivation for use of laser-ablation method Formation of van der Waals complexes from the laser-ablation source Pulsed valves Description of the mechanical part of the ablation assembly Procedures for making the Li sample-rod 2-1-3. Laser system Excitation laser, LI lonization laser, L2 2-1-4. Timeof-flight mass spectrometer (TOFMS) TOFMS Data acquisition & timing circuitry 2-2. Data analysis Mass spectra Measurernents of the photodepletion cross-section 2-3. Summary Chapter 3. Transition State Spectroscopy for the reaction of Li'(2p 'P) + CHjF -+ LiF + CH3 3 Introduction Experiments 3-2. Identification of the LLFCH3 vdW complex 3-3. Measurements of the photodepletion cross-section 62 for Li..FCH3 34. Assignments of the depletion peaks 65 Theoretical results and Discussion 3-5. Po tenfial-en ergy-surfaces 69 3-6. Simulation of the photoabsorption spectrum 76 3-7. Measurements of fhe TS lifetlme by optical 80 'saturation method' 3-8. Summary 85 Chapter 4. Transition State Spectroscopy for the reaction of 87 Li'(2p 'P) + HF + LiF + H 4- 1. Introduction -4-2. Experiments Results 4-3. Identification of the Li-FH complexes 4-4. Photodepletion spectrum for the LLoFH complex Discussion 4-5. Assignment of peaks in the photodepletion spectrum 1O4 4-6. Dynamics of harpooning 107 4-7. Summary 910 Chapter 5. Thesis summary and future directions 5-1. Thesis summary 5-2 Future directions Conclusions Appendix A References vii List of Figures Figure 2-1 : Side view of the vacuum system Figure 2-2: Schematic diagrarn of the laser-ablation assembly Figure 2-3: Schematic diagram of the pulsed valve Figure 24: Schematic drawing of the laser-ablation source assembly Figure 25: (a) The procedure for rnolding the Li support-rod (b) The procedure for molding the Li support-rod Figure 2-6: Depletion-signal versus delay between two lasers Figure 2-7: Schematic drawing of the experimental setup Figure 2-8: Depletion-signal versus excitation-laser fluence Figure 3-1: TOF mass spectrurn for the Li-FCH3 complexes. The ion Signal was measured following photoionization by laser La (h2 =248nm). The dotted line represents ion-signals before photoexcitation and the solid line is the ion-signal after photoexcitation. Figure 3-2: Power dependence of the ionization signal ((A2 =248nm) for Li-FCH3. The straight line is a linear least-square fit to the date points. The slope of the line is 1.02. Figure 3-3: Action spectra for (a) LLFCH3 and (b) NammFCH3 Complexes, showing the depletion cross-section in A2 vs. the wavelength hl of Li in nm. Figure 34: Potential-energy curves for the ground and the electronicallv-excited states of LimoFCH3.alona an a~~roxirnateminirnum- viii energy path for the collinear PES. The observed spectrum is shown, aginst the appropriate energies, inset at the top left. Figure 3-5: Potential-energy contour polts (a) for the ground 2s and (b) (c) (d) for the electronically-excited states 2px, Zp,, 2pz of LieeFCH3. Figure 3-6: Minimumenergy structure for the LieeFCH3complex. Figure 3-7: Sirnulated photoabsorption spectrum of LieeFCH3for T=250K. V~brationallevels up to v=10 on the ground and excited States were included. Figure 3-8: Laserexcitation and rate processes initiated in the complex. Figure 3-9: Simulation of the TS lifetime for LiaeFCH3at II =640nm, using Eq. 3-7 (see text). The heave dashed-line gives comparable data for NaeaFCH3at hl = 690nm. Figure 4-1 : Crossed-beam assembly for formation of the Li-FH Complexes. Figure 4-2: TOF spectrurn illustrating the formation of the Li-FH VdW Complexes. Figure 43: Action spectra for LFH(above) and NaaeFH(below) Complexes (the latter being from Ref. 24), showing the depletion Cross-section in A2 VS. the wavelength of laser Li in nrn. The heavy Vertical Iine is the atomic D-line (2p t 2s for Li, and 3p t 3s for Na). Vibrational spacing indicative of anhannonicity is identified for a series viii of four vibrational levels (see text). Figure 4-4: Ab initio calculation of the vertical-transition energies for 106 excitation from the minimum-energy geometry of the LLFH and Na-FH complexes (the latter being from Ref. 40) on the ground-state PES, q2A',to the lowest-lying excited states. z2A',32A', 12A". Figure 45: Potential-energy curves for the ground and the Electronically-excited states of LiFH. along an approximate minimum- Energy path for the collinear PES. The equilibrium values for the Li-F and H-F bond lengths are indicated on their respective axes by downward pointing arrows at r~=ro (Li-F) = 1.564A and at r2 =ro (H-F) = 0.917A. Vibration in the ground electronic state LLFH (tentatively identified with the vibrational progression of Fig. 4-3) is indicated for v = 0-3. List of Tables Table 2-1: Voltages on the plates and the flight tube in the TOFMS Table 3-1 : Calculated electronic-vibrational transitions in Li-FCH3 (wavelength in nm, integrated absorption coefficient in cnilmole). Chapter 1. Introduction 11 Chernical Dynamics of the reacüon event Understanding the dynamics of the reaction event is a goal of chemical dynamics. The reaction event includes processes occurring during the collision. The reaction event involves breaking of old chernical bonds and sirnultaneous formation of new chemical bonds. The co~certednessof this event is evident in that average collision energies for successful reactions are typically less than 10% of the dissociation energies of the old bonds.
Recommended publications
  • Arxiv:2011.07125V1 [Physics.Comp-Ph] 13 Nov 2020 Θ Hψθ I Θ Dx1
    Better, Faster Fermionic Neural Networks James Spencery, David Pfauy, Aleksandar Botevy, W. M. C. Foulkes∗ yDeepMind, ∗Imperial College London London, UK {jamessspencer, pfau, botev}@google.com, [email protected] Abstract The Fermionic Neural Network (FermiNet) [12] is a recently-developed neural network architecture that can be used as a wavefunction Ansatz for many-electron systems, and has already demonstrated high accuracy on small systems. Here we present several improvements to the FermiNet that allow us to set new records for speed and accuracy on challenging systems. We find that increasing the size of the network is sufficient to reach chemical accuracy on atoms as large as argon. Through a combination of implementing FermiNet in JAX and simplifying several parts of the network, we are able to reduce the number of GPU hours needed to train the FermiNet on large systems by an order of magnitude. This enables us to run the FermiNet on the challenging transition of bicyclobutane to butadiene and compare against the PauliNet on the automerization of cyclobutadiene, and we achieve results near the state of the art for both. 1 Introduction Accurate computational solutions to the Schrödinger equation are critical for quantum chemistry and condensed matter physics. The time-independent form of the equation tries to solve for a wavefunction (x1; x2;:::; xn), which is an eigenfunction of the Hamiltonian, H^ of the system: H^ (x1;:::; xn) = E (x1;:::; xn) (1) H^ = − 1 P r2 + P 1 − P ZI + P ZI ZJ (2) 2 i i i>j jri−rj j iI jri−RI j I>J jRI −RJ j Here E is the real-valued energy of the wavefunction, xi (ri) is the position and spin (position) of the ith electron, RI is the position of the Ith nucleus and ZI is the charge of the Ith nucleus.
    [Show full text]
  • This Manuscript Has Been Reproduced from the Microfilm Master
    This manuscript has been reproduced from the microfilm master. UMI fi!ms the text directly from the original or copy submitted. Thus, some thesis and dissertation copies are in typewriter face, while others may be from any type of computer printer. The quality of this reproduction is dependent upon the quality of the copy submitted. Broken or indistinct print, colored or poor quality illustrations and photographs, print bleedthrough, substandard margins, and improper alignment can adversely affect reproduction. In the unlikely event that the author did not send UMI a complete manuscript and there are missing pages, these will be noted. Also, if unauthorized copyright material had to be removed, a note will indicate the deletion. Oversize materials (e.g., maps, drawings, charts) are reproduced by sectiaoning the original, beginning at the upper left-hand comer and continuing from left to right in equal sections with small overlaps. Photographs included in the original manuscript have been reproduced xerographically in this copy. Higher quality 6" x 9" black and white photographic prints are available for any photographs or illustrations appearing in this copy for an additional charge. Contact UMI directly to order. BeH & Howell Information and Learning 300 North Zeeb Road, Ann Arbor, MI 48106-1346 USA Dynamics of Harpooning Studied by Transition State Spectroscopy Andrew J. Hudson A thesis submitted in conformity with the requirements for the degree of Doctor of Philosophy. Graduate Department of Chemistry, in the University of Toronto.
    [Show full text]
  • Better, Faster Fermionic Neural Networks
    Better, Faster Fermionic Neural Networks James Spencery, David Pfauy, Aleksandar Botevy, W. M. C. Foulkes∗ yDeepMind, ∗Imperial College London London, UK {jamessspencer, pfau, botev}@google.com, [email protected] Abstract The Fermionic Neural Network (FermiNet) [12] is a recently-developed neural network architecture that can be used as a wavefunction Ansatz for many-electron systems, and has already demonstrated high accuracy on small systems. Here we present several improvements to the FermiNet that allow us to set new records for speed and accuracy on challenging systems. We find that increasing the size of the network is sufficient to reach chemical accuracy on atoms as large as argon. Through a combination of implementing FermiNet in JAX and simplifying several parts of the network, we are able to reduce the number of GPU hours needed to train the FermiNet on large systems by an order of magnitude. This enables us to run the FermiNet on the challenging transition of bicyclobutane to butadiene and compare against the PauliNet on the automerization of cyclobutadiene, and we achieve results near the state of the art for both. 1 Introduction Accurate computational solutions to the Schrödinger equation are critical for quantum chemistry and condensed matter physics. The time-independent form of the equation tries to solve for a wavefunction (x1; x2;:::; xn), which is an eigenfunction of the Hamiltonian, H^ of the system: H^ (x1;:::; xn) = E (x1;:::; xn) (1) H^ = − 1 P r2 + P 1 − P ZI + P ZI ZJ (2) 2 i i i>j jri−rj j iI jri−RI j I>J jRI −RJ j Here E is the real-valued energy of the wavefunction, xi (ri) is the position and spin (position) of the ith electron, RI is the position of the Ith nucleus and ZI is the charge of the Ith nucleus.
    [Show full text]
  • Photoluminescence, Photophysics, and Photochemistry of the ${{\Rm{V}} {\Rm{B}}}^ -$ Defect in Hexagonal Boron Nitride
    PHYSICAL REVIEW B 102, 144105 (2020) − Photoluminescence, photophysics, and photochemistry of the VB defect in hexagonal boron nitride Jeffrey R. Reimers ,1,2,* Jun Shen ,3,† Mehran Kianinia,2 Carlo Bradac ,2,4,‡ Igor Aharonovich,2 Michael J. Ford ,2,§ and Piotr Piecuch 3,5, 1International Centre for Quantum and Molecular Structures and Department of Physics, Shanghai University, Shanghai 200444, China 2University of Technology Sydney, School of Mathematical and Physical Sciences, Ultimo, New South Wales 2007, Australia 3Department of Chemistry, Michigan State University, East Lansing, Michigan 48824, USA 4Department of Physics and Astronomy, Trent University, 1600 West Bank Dr., Peterborough, Ontario, Canada K9J 0G2 5Department of Physics and Astronomy, Michigan State University, East Lansing, Michigan 48824, USA (Received 14 July 2020; revised 11 September 2020; accepted 15 September 2020; published 12 October 2020) − Extensive photochemical and spectroscopic properties of the VB defect in hexagonal boron nitride are calculated, concluding that the observed photoemission associated with recently observed optically detected 3 → 3 magnetic resonance is most likely of (1) E (1) A2 origin. Rapid intersystem crossing from the defect’s triplet to singlet manifolds explains the observed short excited-state lifetime and very low quantum yield. New experimental results reveal smaller intrinsic spectral bandwidths than previously recognized, interpreted in terms of spectral narrowing and zero-phonon-line shifting induced by the Jahn-Teller effect. Different types of computational methods are applied to map out the complex triplet and singlet defect manifolds, including the doubly ionized formulation of the equation-of-motion coupled-cluster theory that is designed to deal with the open-shell nature of defect states, and mixed quantum-mechanics/molecular-mechanics schemes enabling 5763-atom simulations.
    [Show full text]
  • Piotr Piecuch Department of Chemistry, Michigan State
    NEW COUPLED-CLUSTER METHODS FOR MOLECULAR POTENTIAL ENERGY SURFACES: I. GROUND-STATE APPROACHES Piotr Piecuch Department of Chemistry, Michigan State University, East Lansing, Michigan 48824 P. Piecuch and K. Kowalski, in: Computational Chemistry: Reviews of Current Trends, edited by J. Leszczynski´ (World Scientific, Singapore, 2000), Vol. 5, pp. 1-104; K. Kowalski and P. Piecuch, J. Chem. Phys. 113, 18-35 (2000); 113, 5644-5652 (2000); J. Molec. Struct.: THEOCHEM 547, 191-208 (2001); Chem. Phys. Lett. 344, 165-175 (2001); P. Piecuch, S.A. Kucharski, and K. Kowalski, Chem. Phys. Lett. 344, 176-184 (2001); P. Piecuch, S.A. Kucharski, V. Spirkˇ o, and K. Kowalski, J. Chem. Phys. 115, 5796-5804 (2001); P. Piecuch, K. Kowalski, and I.S.O. Pimienta, Int. J. Mol. Sci., submitted (2001); P. Piecuch and K. Kowalski, Int. J. Mol. Sci., submitted (2001); K. Kowalski and P. Piecuch, J. Chem. Phys. 115, 2966-2978 (2001); P. Piecuch, K. Kowalski, I.S.O. Pimienta, and S.A. Kucharski, in: Accurate Description of Low-Lying Electronic States and Potential Energy Surfaces, ACS Symposium Series, Vol. XXX, edited by M.R. Hoffmann and K.G. Dyall (ACS, Washington, D.C., 2002), pp. XXX-XXXX; K. Kowalski and P. Piecuch, J. Chem. Phys., submitted (2001); P. Piecuch, S.A. Kucharski, and V. Spirkˇ o, J. Chem. Phys. 111, 6679-6692 (1999); K. Kowalski and P. Piecuch, J. Chem. Phys. 113, 8490-8502 (2000); 115, 643-651 (2001); K. Kowalski and P. Piecuch, Chem. Phys. Lett. 347, 237-246 (2001). 1 The \holy grail" of the ab initio electronic structure theory: The development of simple, \black-box," and affordable methods that can pro- vide highly accurate ( spectroscopic) description of ENTIRE GROUND- AND ∼ EXCITED-STATE POTENTIAL ENERGY SURFACES 14000 12000 10 NaF+H 10000 8 8000 V/cm-1 6000 6 Na *+ FH 4000 Energy/eV 4 2000 Na .
    [Show full text]
  • Piotr Piecuch Department of Chemistry, Michigan State
    NEW COUPLED-CLUSTER METHODS FOR MOLECULAR POTENTIAL ENERGY SURFACES: II. EXCITED-STATE APPROACHES Piotr Piecuch Department of Chemistry, Michigan State University, East Lansing, Michigan 48824 P. Piecuch and K. Kowalski, in: Computational Chemistry: Reviews of Current Trends, edited by J. Leszczynski´ (World Scientific, Singapore, 2000), Vol. 5, pp. 1-104; K. Kowalski and P. Piecuch, J. Chem. Phys. 113, 18-35 (2000); 113, 5644-5652 (2000); J. Molec. Struct.: THEOCHEM 547, 191-208 (2001); Chem. Phys. Lett. 344, 165-175 (2001); P. Piecuch, S.A. Kucharski, and K. Kowalski, Chem. Phys. Lett. 344, 176-184 (2001); P. Piecuch, S.A. Kucharski, V. Spirkˇ o, and K. Kowalski, J. Chem. Phys. 115, 5796-5804 (2001); P. Piecuch, K. Kowalski, and I.S.O. Pimienta, Int. J. Mol. Sci., submitted (2001); P. Piecuch and K. Kowalski, Int. J. Mol. Sci., submitted (2001); K. Kowalski and P. Piecuch, J. Chem. Phys. 115, 2966-2978 (2001); P. Piecuch, K. Kowalski, I.S.O. Pimienta, and S.A. Kucharski, in: Accurate Description of Low-Lying Electronic States and Potential Energy Surfaces, ACS Symposium Series, Vol. XXX, edited by M.R. Hoffmann and K.G. Dyall (ACS, Washington, D.C., 2002), pp. XXX-XXXX; K. Kowalski and P. Piecuch, J. Chem. Phys., submitted (2001); P. Piecuch, S.A. Kucharski, and V. Spirkˇ o, J. Chem. Phys. 111, 6679-6692 (1999); K. Kowalski and P. Piecuch, J. Chem. Phys. 113, 8490-8502 (2000); 115, 643-651 (2001); K. Kowalski and P. Piecuch, Chem. Phys. Lett. 347, 237-246 (2001). 1 The \holy grail" of the ab initio electronic structure theory: The development of simple, \black-box," and affordable methods that can pro- vide highly accurate ( spectroscopic) description of ENTIRE GROUND- AND ∼ EXCITED-STATE POTENTIAL ENERGY SURFACES 14000 12000 10 NaF+H 10000 8 8000 V/cm-1 6000 6 Na *+ FH 4000 Energy/eV 4 2000 Na .
    [Show full text]
  • Symposium Program
    “A little insight goes a long way: a transformative role of theory in spectroscopy and chemical dynamics.” A symposium in honor of Prof. Benny Gerber “The purpose of computing is insight, not numbers” !!!!!!!R.W. Hamming The symposium will highlight a transformative role that theory plays in modern research by making bold predictions, guiding the design of new experiments, and enabling insightful interpretation of experimental observations. The focus of the symposium will be on the theories and computational approaches connecting experimental observations to the underlying interactions between atoms and molecules developed by Prof. Benny Gerber and his colleagues, collaborators, students, and post docs. The topics will cover a broad range of experimental and theoretical physical chemistry including atmospheric processes, novel rare gas containing compound, new spectroscopic approaches, and more. Symposium sponsors: Fritz Haber Center (The Hebrew University of Jerusalem) University of California, Irvine University of Southern California Q-Chem, Inc Preliminary program: The symposium is a part of ACS National Meeting in Dallas, March 16-20, 2014. We are scheduled for Sunday, Monday, and Wednesday (Tuesday is reserved for ACS award symposia). On Monday evening, a hosted symposium reception and dinner is planned. Session I: Biology and condensed phase (Sunday AM) Chair: Anna Krylov 810-815 Welcome remarks 815-845! Doug Tobias, “Making sense of transmembrane voltage sensing by voltage-gated ion channels: concerted simulation and experimental
    [Show full text]
  • Accurate Potential Energy Surfaces and Beyond: Chemical Reactivity, Binding, Long-Range Interactions, and Spectroscopy
    Advances in Physical Chemistry Accurate Potential Energy Surfaces and Beyond: Chemical Reactivity, Binding, Long-Range Interactions, and Spectroscopy Guest Editors: Laimutis Bytautas, Joel M. Bowman, Xinchuan Huang, and António J. C. Varandas Accurate Potential Energy Surfaces and Beyond: Chemical Reactivity, Binding, Long-Range Interactions, and Spectroscopy Advances in Physical Chemistry Accurate Potential Energy Surfaces and Beyond: Chemical Reactivity, Binding, Long-Range Interactions, and Spectroscopy Guest Editors: Laimutis Bytautas, Joel M. Bowman, Xinchuan Huang, and Antonio´ J. C. Varandas Copyright © 2012 Hindawi Publishing Corporation. All rights reserved. This is a special issue published in “Advances in Physical Chemistry.” All articles are open access articles distributed under the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. Editorial Board Janos´ G. Angy´ an,´ France F. Illas, Spain Eli Ruckenstein, USA M. Sabry Abdel-Mottaleb, Egypt KwangS.Kim,RepublicofKorea Gnther Rupprechter, Austria Taicheng An, China Bernard Kirtman, USA Kenneth Ruud, Norway J. A. Anderson, UK Lowell D. Kispert, USA Viktor A. Safonov, Russia Panos Argyrakis, Greece Marc Koper, The Netherlands Dennis Salahub, Canada Ricardo Aroca, Canada Alexei A. Kornyshev, UK Anunay Samanta, USA Stephen H. Ashworth, UK Yuan Kou, China Dipankar Das Sarma, India Biman Bagchi, India David Logan, UK Joop Schoonman, The Netherlands Hans Bettermann, Germany Clare M. McCabe, USA Stefan Seeger, Switzerland Vasudevanpillai Biju, Japan James K. McCusker, USA Tamar Seideman, USA Joel Bowman, USA MichaelL.McKee,USA Hiroshi Sekiya, Japan Wybren J. Buma, The Netherlands Robert M. Metzger, USA Luis Serrano-Andres,´ Spain Sylvio Canuto, Brazil Michael V.
    [Show full text]
  • 9789400720763.Pdf
    ADVANCES IN THE THEORY OF QUANTUM SYSTEMS IN CHEMISTRY AND PHYSICS Progress in Theoretical Chemistry and Physics VOLUME 22 Honorary Editors: Sir Harold W. Kroto (Florida State University, Tallahassee, FL, U.S.A.) Pr Yves Chauvin (Institut Franc¸ais du P´etrole, Tours, France) Editors-in-Chief: J. Maruani (formerly Laboratoire de Chimie Physique, Paris, France) S. Wilson (formerly Rutherford Appleton Laboratory, Oxfordshire, U.K.) Editorial Board: V. Aquilanti (Universit`a di Perugia, Italy) E. Brandas¨ (University of Uppsala, Sweden) L. Cederbaum (Physikalisch-Chemisches Institut, Heidelberg, Germany) G. Delgado-Barrio (Instituto de Matem´aticas y F´ısica Fundamental, Madrid, Spain) E.K.U. Gross (Freie Universit¨at, Berlin, Germany) K. Hirao (University of Tokyo, Japan) E. Kryachko (Bogolyubov Institute for Theoretical Physics, Kiev, Ukraine) R. Lefebvre (Universit´e Pierre-et-Marie-Curie, Paris, France) R. Levine (Hebrew University of Jerusalem, Israel) K. Lindenberg (University of California at San Diego, CA, U.S.A.) R. McWeeny (Universit`a di Pisa, Italy) M.A.C. Nascimento (Instituto de Qu´ımica, Rio de Janeiro, Brazil) P. Piecuch (Michigan State University, East Lansing, MI, U.S.A.) M. Quack (ETH Z¨urich, Switzerland) S.D. Schwartz (Yeshiva University, Bronx, NY, U.S.A.) A. Wang (University of British Columbia, Vancouver, BC, Canada) Former Editors and Editorial Board Members: I. Prigogine (†) H. Hubac(*)ˇ J. Rychlewski (†)M.P.Levy(*) Y. G . S m ey e r s ( †) G.L. Malli (*) R. Daudel (†) P.G. Mezey (*) M. Mateev (†)N.Rahman(*) W.N. Lipscomb (†) S. Suhai (*) H. Agren˚ (*) O. Tapia (*) D. Avnir (*) P.R. Taylor (*) J. Cioslowski (*) R.G.
    [Show full text]
  • Q Frontiers in Uantum Systems in Chemistry And
    FRONTIERS IN QUANTUM SYSTEMS IN CHEMISTRY AND PHYSICS Progress in Theoretical Chemistry and Physics VOLUME 18 Honorary Editors: W.N. Lipscomb (Harvard University, Cambridge, MA, U.S.A.) Yves Chauvin (Institut Français du Pétrole, Tours, France ) Editors-in-Chief: J. Maruani (formerly Laboratoire de Chimie Physique, Paris, France) S. Wilson (formerly Rutherford Appleton Laboratory, Oxfordshire, U.K.) Editorial Board: V. Aquilanti (Università di Perugia, Italy) E. Brändas (University of Uppsala, Sweden) L. Cederbaum (Physikalisch-Chemisches Institut, Heidelberg, Germany) G. Delgado-Barrio (Instituto de Matemáticas y Física Fundamental, Madrid, Spain) E.K.U. Gross (Freie Universität, Berlin, Germany) K. Hirao (University of Tokyo, Japan) R. Lefebvre (Université Pierre-et-Marie-Curie, Paris, France) R. Levine (Hebrew University of Jerusalem, Israel) K. Lindenberg (University of California at San Diego, CA, U.S.A.) M. Mateev (Bulgarian Academy of Sciences and University of Sofia, Bulgaria) R. McWeeny (Università di Pisa, Italy) M.A.C. Nascimento (Instituto de Química, Rio de Janeiro, Brazil) P. Piecuch (Michigan State University, East Lansing, MI, U.S.A.) S.D. Schwartz (Yeshiva University, Bronx, NY, U.S.A.) A. Wang (University of British Columbia, Vancouver, BC, Canada) R.G. Woolley (Nottingham Trent University, U.K.) Former Editors and Editorial Board Members: ˆ I. Prigogine (†) I. Hubac ()* J. Rychlewski (†) M.P. Levy ()* Y.G. Smeyers (†) G.L. Malli ()* R. Daudel (†) P.G. Mezey ()* H. Ågren ()* N. Rahman ()* D. Avnir (*) S. Suhai ()* J. Cioslowski ()* O. Tapia ()* W.F. van Gunsteren ()* P.R. Taylor ()* † : deceased; * : end of term For other titles published in this series, go to www.springer.com/series/6464 Frontiers in Quantum Systems in Chemistry and Physics Edited by STEPHEN WILSON University of Oxford, UK PETER J.
    [Show full text]
  • Curriculum Vitae
    The University of Arizona, Department of Chemistry and Biochemistry, Tucson, AZ 85721 E-mail: [email protected]; Tel: 520-621-6607; FAX: 520-621-8407 WWW Site: http://www.chem..Arizona.edu/faculty/adam/Adamowicz.html Curriculum Vitae Ludwik Adamowicz Education: MS, Warsaw University MS thesis "Mulliken Population Analysis of Water Complexes with Li+, Na+, F- and Cl-", 1973, Advisor Professor W. Kolos. Ph.D., Institute of Physical Chemistry of the Polish Academy of Sciences. Ph.D. Thesis "Gaussian Geminals Used to Calculate Electronic Correction Energy of Small Molecules", 1977, Advisor Professor A.J. Sadlej. Employment: Aug. 1998-present: Professor of Chemistry, University of Arizona. (Primary appointment) June 2003-present: Professor of Physics, University of Arizona Sum. 2010, 2011, 2012 Visiting Professor, University of Oslo, Norway Feb. 2004- July 2004: Visiting Professor, University of Pisa, Italy Dec. 2001-Aug. 2002: Visiting Professor, Laboratoire de Physique Quantique, Universite Paul Sabatier, Toulouse, France. Aug. 2001-Dec. 2001: Visiting Professor, Nagoya University and The Institute for Molecular Science, Okazaki, Japan. Feb. 1995–Aug.1995: Visiting Researcher, Laboratoire de Physique Quantique, Universite Paul Sabatier, Toulouse, France. (Sabbatical leave from The University of Arizona) Aug. 1994-Feb.-1995: Visiting Professor, University of Lund, Lund, Sweden. (Sabbatical leave from The University of Arizona) 1993-1998: Associate Professor of Chemistry (with tenure), The University of Arizona. 1987-1993: Assistant Professor of Chemistry, The University of Arizona. 1983-1987: Research Associate (with R. J. Bartlett), Quantum Theory Project, University of Florida. 1980-1983: Research Associate (with E. A. McCullough), Department of Chemistry and Biochemistry, Utah State University.
    [Show full text]
  • Diffusion of Atomic Oxygen on the Si(100) Surface Pooja Arora Iowa State University
    Chemistry Publications Chemistry 7-2010 Diffusion of Atomic Oxygen on the Si(100) Surface Pooja Arora Iowa State University Wei Li Michigan State University Piotr Piecuch Michigan State University James W. Evans Iowa State University, [email protected] Marvin Argulla Albao Iowa State University SeFoe nelloxtw pa thige fors aaddndition addal aitutionhorsal works at: http://lib.dr.iastate.edu/chem_pubs Part of the Applied Mathematics Commons, Astrophysics and Astronomy Commons, and the Chemistry Commons The ompc lete bibliographic information for this item can be found at http://lib.dr.iastate.edu/ chem_pubs/534. For information on how to cite this item, please visit http://lib.dr.iastate.edu/ howtocite.html. This Article is brought to you for free and open access by the Chemistry at Iowa State University Digital Repository. It has been accepted for inclusion in Chemistry Publications by an authorized administrator of Iowa State University Digital Repository. For more information, please contact [email protected]. Diffusion of Atomic Oxygen on the Si(100) Surface Abstract The processes of etching and diffusion of atomic oxygen on the reconstructed Si(100)-2 × 1 surface are investigated using an embedded cluster QM/MM (Quantum Mechanics/Molecular Mechanics) method, called SIMOMM (Surface Integrated Molecular Orbital Molecular Mechanics). Hopping of an oxygen atom along the silicon dimer rows on a Si15H16 cluster embedded in an Si136H92 MM cluster model is studied using the SIMOMM/UB3LYP (unrestricted density functional theory (UDFT) with the Becke three- parameter Lee−Yang−Parr (B3LYP) hybrid functional) approach, the Hay−Wadt effective core potential, and its associated double-ζ plus polarization basis set.
    [Show full text]