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Laser-Induced Processes in Molecules: Physics and Chemistry Proceedings of the European Physical Society, Divisional Conference at Heriot-Watt University Edinburgh, Scotland, September 20–22, 1978 PDF

374 Pages·1979·9.368 MB·English
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Preview Laser-Induced Processes in Molecules: Physics and Chemistry Proceedings of the European Physical Society, Divisional Conference at Heriot-Watt University Edinburgh, Scotland, September 20–22, 1978

6 Springer Series in Chemical Physics Edited by Fritz Peter Schafer "-------------' Springer Series in Chemical Physics Editors: V. I. Goldanskii R. Gomer F. P. Schafer 1. P. Toennies Volume 1 Atomic Spectra and Radiative Transitions By I. I. Sobelman Volume 2 Surface Crystallography by LEED Theory, Computation and Structural Results By M. A. Van Hove, S. Y. Tong Volume 3 Advances in Laser Chemistry Editor: A. H. Zewail Volume 4 Picosecond Phenomena Editors: C. V. Shank, E. P. Ippen, S. L. Shapiro Volume 5 Laser Spectroscopy Fundamentals and Techniques By W. Demtroder Volume 6 Laser-Induced Processes in Molecules Physics and Chemistry Editors: K. L. Kompa, S. D. Smith Volume 7 Excitation of Atoms and Broadening of Spectral Lines By I. I. Sobelman, L. A. Vainshtein, E. A. Yukov Laser-Induced Processes in Molecules Physics and Chemistry Proceedings of the European Physical Society Divisional Conference at Heriot -Watt University Edinburgh, Scotland, September 20-22, 1978 Editors K.L.Kompa and S.D. Smith With 196 Figures Springer-Verlag Berlin Heidelberg New York 1979 Professor Dr. Karl Ludwig Kompa Projektgruppeflir Laserforschung, Max-Planck-GeseIlschaft zur Forderung der Wissenschaften e.V. D-8046 Garching bei Miinchen, Fed. Rep. of Germany Professor Stanley Desmond Smith, Ph.D. D.Sc. FRS Department of Physics, Heriot-Watt University, Riccarton, Edinburgh EH14 4AS, Scotland Series Editors: Professor Vitalii I. Goldanskii Professor Dr. Fritz Peter Schafer Institute of Chemical Physics, Academy Max-Planck-Institut flir Biophysikalische of Sciences, Vorobyevskoye Chaussee 2-b Chemie, D-3400 Gottingen-Nikolausberg Moscow V-334, USSR Fed. Rep. of Germany Professor Robert Gomer Professor Dr. J. Peter Toennies The James Franck Institute Max-Planck-Institut flir Stromungsforschung The University of Chicago, 5640 Ellis Av enue BottingerstraBe 6-8 Chicago, IL 60637, USA D-3400 Gottingen, Fed. Rep. of Germany Conference Chairmen: Professor S. D. Smith FRS and Professor K. L. Kompa Conference Organizer: Dr. R.G. Harrison, Heriot-Watt University Conference Treasurer: H.A. MacKenzie, Heriot-Watt University Sponsors: Imperial Chemical Industries Ltd.; Spectra Physics Inc.; Edinburgh Instruments Ltd. Programme and Advisory Committee: M.J. Berry, B. Bolger, B. Burlamacchi, J. Ernest, S. Kimel, K.L. Kompa, S. Leach, V.S. Letokhov, S.D. Smith, I.J. Spalding, O. Svelto, J.J. Turner, H. Walther, R.N. Zare ISBN-I3: 978-3-642-67256-9 e-ISBN-I3: 978-3-642-67254-5 DOl: 10.1007/978-3-642-67254-5 This work is subject to copyright. All rights are reserved, whether the whole or part of the material is concerned, specifically those of translation, reprinting, reuse of illustrations, broadcasting, reproduction by photocopying machine or similar means, and storage in data banks. Under § 54 of the German Copyright Law where copies are made for other than private use, a fee is payable to the publisher, the amount of the fee to be determined by agreement with the publisher. © by Springer-Verlag Berlin Heidelberg 1979 Softcover reprint of the harcover I st edition 1979 The use of registered names, trademarks, etc. in this publication does not imply, even in the absence of a specific statement, that such names are exempt from the relevant protective laws and regulations and therefore free for general use. Preface This conference on both the physics and chemistry of laser-induced processes in molecules was organized by the Quantum Electronics Divisional Board of the European Physical Society whose membership is given on p.367. The confer ence aim, to mix physicists and chemists interested in this exciting field both from Europe and further afield, was well fulfilled by the attendance of around 250 participants and the submission of about 100 papers, which dre presented here. Numerous people at both the Physics Department, Heriot-Watt University, Edinburgh, and at the Projektgruppe fUr Laserforschung, MPI, Garching, con tributed hard work to the organization; in addition to Dr. Bob Harrison, who bore the biggest burden with conspicuous success, we particularly thank Hugh MacKenzie, Richard Dennis and last but not least Miss Joanne Askham and the secretaries in Edinburgh together with Frau Doris Maischberger and the secretaries in Garching. December 1978 K.L. Kompa S.D. Smith Conren~ Part I. Study of Lasers and Related Techniques Suitable for Applications in Chemistry and Spectroscopy Rare Gas Halogen Lasers and Photochemical Applications. By S.D. Rockwood................................................... 3 Group VI Molecular Photolytic Dissociation Studies Using Rare Gas Halide Lasers. By M.C. Gower, A.J. Kearsley, and C.E. Webb ......... 8 Broadly Tunable UV Source Based on Stimulated Raman Scattering. By V. Wi 1k e and W. Schmi dt ......................................... 12 Laser-Induced Intermolecular and Intramolecular Energy Transfer Processes. By S. Spei ser ........................................... 15 A New Method for Exposing Mammalian Cells to Intense Laser Radiation Using the Evanescent Fields Created in Optical Waveguides. By H.L. Cox, Jr. .................................................. 19 Time-Dependent Kinetic-Thermodynamic Description of a Nonequilibrium Molecular System: The HF Chemical Laser. By A. Ben-Shaul, O. Kafri, and R.D. Levine.................................................... 22 Low-Temperature Performance of Roto-Vibrational Molecular Lasers. By J.M. Green...................................................... 26 HBr Laser Emission at 4 Based on the Chemical Generation of ~m Bromine Atoms. By S.J. Arnold and K.D. Foster " .................... 29 Tunable Infrared Generation from Four-Wave Mixing in Room-Temperature Germanium. By S.R. Butcher, R.G. Harrison, and R.A. Wood ........... 32 Part II. Spectroscopic Studies with and Related to Lasers High-Resolution Double-Resonance Spectroscopy of SF6. By P.F. Moulton and A. Mooradian ................................... 37 VII High-Resolution Coherent Raman Spectroscopy of Methane and Intensity of CARS vs Pressure in Gases. By J. -P. Boqui 11 on ................... 43 Molecular Spectroscopy of NO and C2H4 Using Step-Tunable IR Lasers and the External Resonator Controlled Spin-Flip Raman Laser. By G. Crowder, R.B. Dennis, H.A. MacKenzie, M.H. Mozolowski, and M. Sioudi ...................................................... 46 Photophysics of Gaseous UF6 in the UV: Energy Ba'lance Through Quantum Efficiency Measurements. By O. de Witte, R. Dumanchin, J.P. Gauyacq, and M. Michon ........................................ 49 Optical Dephasing in Molecular Iodine. By R.G. Brewer and S.S. Kano .......................................................... 54 An Efficient Algorithm for the Study of Nonlinear Resonant Propagation of Two Concomitant Optical Pulses Interacting with a Three-Level Atomic System. By F.P. Mattar and J.H. Eberly ........ 61 The Influence of Hyperfine Coherence and of Elastic Collisions on the Circular Polarisation of Emission from Li2. By M.D. Rowe and A.J. McCaffery..................................................... 66 Collisional Depolarization and Rotational Energy Transfer of the 7Li2B1rru - Li2S1/2 System Using Laser-Induced Fluorescene. By C.R. Vidal ...................................................... 69 Saturated Absorption Experiments on a Molecule Dressed by a Radio- frequency Fi e 1d . By E. Ari mondo and P. Glori eux .................... 71 dc Magnetic Field Effects on Polarized Monochromatic Laser Radiation Absorption in Electronic Transitions: A Simple Model. By M. Bernardini, A. Fubini, and G. Sacerdoti ...................... 74 Effect of Two-Photon Saturation on Ordinary Raman Scattering. By A.D. Wilson-Gordon and H. Friedmann 78 Predissociation in the A'A" State of HNO. By R.N. Dixon and M. Noble......................................... 81 Photoassociation of Heavy Metal Excimers: Spectroscopic, Kinetic, and Laser Applications. By D.J. Ehrlich and R. M. Osgood, Jr. ................................................... 85 Dye-Laser-Induced Emission from the KXe Molecule. By C.R. Webster and F. Rostas .......................................................... 89 VIII Laser-Induced Emission from the NaK Molecule in a Supersonic Beam. By E.-J. Breford and F. Engelke .................................... 92 The Singlet-Triplet Energy Separation of CH2 and Spectroscopy of the alAI State. By D. Feldmann, K. Meier, R. Schmiedl, H. Zacharias, and K.H. Welge..................................................... 95 Time-Resolved Fluorescence Spectroscopy Using Pulsed Laser Excitation. By K.P. Ghiggino, A.J. Roberts, and D. Phillips .................... 98 Ultrafast Spectroscopy with a Streak Camera: Excited State Spectros- copy and Kinetics of Coumarin Derivatives. By J. Schulz-Hennig and A. MUller ...................................................... 101 Laser-Induced Processes in Phthalocyanines. By J. McVie, R.S. Sinclair, and T. G. Truscott .................................................. 104 Fluorescence Decay-Time Measurement of Rhodamine 6G and Rhodamine B in Different Solutions. By H. Alobaidi, F. Alberkdar, Z. Hafidh, and S. Alalkawy .................................................... 108 Laser Flash Spectroscopy of 4-Nitrostilbenes and Thioindigo Dyes; Configuration of the Triplet State in Solution. By H. Garner and D. Schulte-Frohl inde ............................................... 111 Part III. Multiphoton Excitation, Dissociation and Ionization Laser-Induced Unimolecular Reactions. By N. Bloembergen and E. Yablonovitch .................................................... 117 Time and Intensity Dependence of the Infrared Absorption of SF6: Measurements with an Injection-Locked Single Mode TEA CO2 Laser. By S.D. Smith, W.E. Schmid, F.M.G. Tablas, and K.L. Kompa .......... 121 IR Absorption of Highly Excited SF6. By W. Fui3 and J. Hartmann .......................................... 128 Absorption of Intense Laser Radiation by SF6 and S2F10' By J.L. Lyman ...................................................... 131 Collisional Effects in the Multiple-Photon Infrared Laser Pumping of Polyatomic Molecules. By G.P. Quigley .............................. 134 Coherent Pulse Propagation Effects in Multilevel Molecular Systems. By C.D. Cantrell, W.H. Louisell, and J.F. Lam ...................... 138 IX The Influence of Intensity and Laser-Energy Fluence in Unimolecular Reactions Induced by Monochromatic Infrared Radiation (URIMIR). By M. Quack ........................................................ 142 On the Dynamics of Multiphoton Dissociation of Polyatomic Molecules II. Application to 03. By K.D. Hansel .................... 145 Nonthermal Theory of Threshold Behaviour of Collisionless Multiphoton Dissociation. By H. Friedmann .......................... 149 An Anharmonic Model for Molecular Photo-Excitation. By P.G. Harper ..................................................... 152 Dynamic Stark Splitting of Multiphoton Absorption Resonances. By P.L. Knight ..................................................... 155 Polarization Selection Rules for Two-Photon Processes. By B.R. Marx and L. Allen 158 Doppler-Free Raman Spectroscopy and Suppression of Molecular Doppler-Broadened Transitions Induced by Laser Field. By A.K. Popov and L.N. Talashkevich ................................ 161 Laser-Controlled Unimolecular and Bimolecular Processes: Field-Dependent Rate "Constants". By A.M.F. Lau .................... 163 Laser-Induced Predissociation of Diatomic and Polyatomic Molecules by the Photo-Cata lyti c Effect. By A. M. F. Lau ....................... 167 Possibility of Hole Burning in Single Quantum Power Spectrum Due to Autler-Townes Splitting. By J.V. Moloney and F.H.M. Faisal ......... 171 Computation of Rovibrational Multiphoton Spectra: Application to CO. By J.V. Moloney and F.H.M. Faisal .................................. 173 Crossed Laser and Molecular Beam Study of Multiphoton Dissociation of C2F5Cl. By D.J. Krajnovich, A. Giardini-Guidoni, Aa.S. Sudb~, P.A. Schulz, Y.R. Shen, and Y.T. Lee ............................... 176 Study of Primary Characteristics of Multiple IR Photon Excitation and Dissociation of CF3I. By V.N. Bagratashvili, V.S. Doljikov, V.S. Letokhov, and E.A. Ryabov ..................................... 179 Photofragment Spectroscopy of Multiple Photon Dissociation by Laser Induced Fluorescence. By R. Schmiedl, R. Bottner, H. Zacharias, U. Meier, D. Feldmann, and K.H. Welge .............................. 186 x Laser-Excited Fluorescence Studies of IR Multiple Photon Dissociation Fragments: NH2(2B1) from CH3NH2 and NH3. By G. Hancock, R.J. Hennessy, and T. Villis ....................................... 190 Time Behavior of CN Radicals in Laser-Initiated Thermal Isomeriza.tion of CH3NC. By D.S. Bethune, J.R. Lankard, M.M.T. Loy, J. Ors, and P.P. Sorokin ........................................... 193 Laser-Induced Decomposition of Methanol: A Comparative Study Using Pulsed HF and CO2 Lasers. By R. Bhatnagar, P.E. Dyer, and G.A. Oldershaw ................................................. 195 IR Laser Sensitised Chemical Reactions of Polyatomic Molecules. By C. Steel, V. Starov, P. John, R.G. Harrison, and R. Leo ......... 198 Excitation of Ammonia in the Megawatt Region Using a CO2 Laser. By V. Starov, C. Steel, S. Butcher, R.G. Harrison, P. John, and R. Leo ......................................................... 201 Reaction Between CH3N02 and H2 Induced by CO2 Laser Pulses. By M. Neve de Mevergni es and P. Fettwei s ........................... 205 Multiphoton Dissociation in Formaldehyde. By G. Koren and U. P. Oppenhei m ..................................... 209 Multiphoton Vacuum UV Photodissociation of Simple Polyatomic Molecules. By A.P. Baronavski, V.M. Donnelly, and J.R. McDonald .... 213 Mass Selective Two-Photon Ionization of a Polyatomic Molecule. By U. Boesl, H.J. Neusser, and E.W. Schlag ......................... 219 Part IV. Laser Control of Chemical Reactions Laser-Induced Chemical Processes: Reactions with Oriented Reagents. By R.N. Zare ....................................................... 225 Laser-Induced Fluorescence Study of the Reactions of F Atoms with CH3I, CF3I and IC1. By L. Stein, J. Wanner, H. Figger, and H. Walther ..................................................... 232 A Laser-Induced Fluorescence Study of the Reaction Ca + CC14-+ CaCl + CC13. By A. Schultz and W. Schmidt .............. 236 cw Laser-Induced Fluorescence Study of BA + S02: Vibronic Distribution of BaO as a Function of Collisional Energy. By R. Dirscherl and H.U. Lee ....................................................... 239 XI

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