Selectivity in Chemical Reactions
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1 Selectivity in Chemical Reactions
2 NATO ASI Series Advanced Science Institutes Series A Series presenting the results of activities sponsored by the NA TO Science Committee, which aims at the dissemination of advanced scientific and technological knowledge, with a view to strengthening links between scientific communities. The Series is published by an international board of publishers in conjunction with the NATO Scientific Affairs Division A Life Sciences B Physics C Mathematical and Physical Sciences D Behavioural and Social Sciences E Applied Sciences F Computer and Systems Sciences G Ecological Sciences H Cell Biology Plenum Publishing Corporation London and New York Kluwer Academic Publishers Dordrecht, Boston and London Springer-Verlag Berlin, Heidelberg, New York, London, Paris and Tokyo Series C: Mathematical and Physical Sciences - Vol. 245
3 Selectivity in Chemical Reactions edited by J. C. Whitehead Department of Chemistry, University of Manchester, Manchester, U.K.... " Kluwer Academic Publishers Dordrecht / Boston / London Published in cooperation with NATO Scientific Affairs Division
4 Proceedings of the NATO Advanced Research Workshop on Selectivity in Chemical Reactions Bowness-on-Windermere, U.K September 1987 Library of Congress Cataloging in Publication Data NATO Advanced Research Workshop on Selectivity iq Chemical Reactions (1987 : Windermere, England) Selectivity in chemical reactions. (NATO ASI series. Series C, Mathematical and physical sciences ; vol. 245) "Published in cooperation with NATO Scientific Affairs Division." Includes index. 1. Chemical reaction, Rate of--congresses. 2. Chemical reaction, Conditions and law of--congresses. I. Whitehead, J. C., II. North Atlantic Treaty Organization. Scientific Affairs Division. III. Title. IV. Series: NATO ASl series. Series C, Mathematics and physical sciences no QD502.N ' ISBN-13: e-isbn-13: DOl: / Published by Kluwer Academic Publishers, P.O. Box 17, 3300 AA Dordrecht, The Netherlands. Kluwer Academic Publishers incorporates the publishing programmes of D. Reidel, Martinus Nijhoff, Dr W. Junk, and MTP Press. Sold and distributed in the U.S.A. and Canada by Kluwer Academic Publishers, 101 Philip Drive, Norwell, MA 02061, U.S.A. In all other countries, sold and distributed by Kluwer Academic Publishers Group, P.O. Box 322, 3300 AH Dordrecht, The Netherlands. All Rights Reserved 1988 by Kluwer Academic Publishers. Softcover reprint of the hardcover 1 sl edition 1988 No part of the material protected by this copyright notice may be reproduced or utilized in any form or by any means, electronic or mechanical, including photocopying, recording or by any information storage and retrieval system, without written permission from the copyright owner.
5 This book contains the proceedings of a NATO Advanced Research Workshop held within the programme of activities of the NATO Special Programme on Selective Activation of Molecules running from 1983 to 1988 as part of the activities of the NATO Science Committee. Other books previously published as a result of the activities of the Special Programme are BOSNICH, B. (Ed.) - Asymmetric Catalysis (E103), 1986 PELIZZE'ITI, E. and SERPONE, N. (Eds.) - Homogeneous and Heterogeneous Photocatalysis (C174) 1986 SCHNEIDER, M. P. (Ed.) - Enzymes as Catalysts in Organic Synthesis (C178) 1986 SETION, R. (Ed.) - Chemical Reactions in Organic and Inorganic Constrained Systems (C165) 1986 VIEHE, H. G., JANOUSEK, Z. and MERENYI, R. (Eds.) - Substituent Effects in Radical Chemistry (C189) 1986 BALZANI, V. (Ed.) - Supramolecular Photochemistry (C214) 1987 FONTANILLE, M. and GUYOT, A.(Eds.) - Recent Advances in Mechanistic and Synthetic Aspects of Polymerization (C215) 1987 LAINE, R. M. (Ed.) - Transformation of Organometallics into Common and Exotic Materials: Design and Activation (E141) 1988 BASSET, J.-M., et al. (Eds.) - Surface Organometallic Chemistry: Molecular Approaches to Surface Catalysis (C231) 1988
6 CONTENTS Preface... xi Introduction Selectivity in Elementary Chemical Reactions.... RB. Bernstein Specijicty of Reagent States in Chemical Reactions Laser Studies on the Selectivity of Elementary Chemical Reactions: Products, Energy, Orientation J. Wolfrum Rotational and Steric Effects in Three Centre Reactions W. Grote, M. Hoffmeister, R Schleysing, H. zerhau-dreihofer and HJ. Loesch Selectivity of Translational Excitation in Reactive Collisions. The Alkaline plus Alkyl Halide Reaction Family A. Gonzalez Urefia The Effect of Changing Reagent Translation on Reaction Dynamics: F + CF 31 ~ IF + CF M. Trautmann, K. Wagemann, J. Wanner and X.K. zeng Internal Energy Distributions in AlO given by the Reactions of Aluminium Atoms with Several Oxidant Molecules M. Costes, C. Naulin, G. Dorthe and G. Nouchi The Effect of Electronic Excitation in the Reactions of Oxygen Atoms with Simple Hydride Molecules Sloan, E.I. Kruus and B.I. Niefer Laser Studies of Reaction Dynamics: The Ca* + HF ~ CaF(X2~,v) + H and Ca* + SFs ~ CaF(X2~,V) + SFs Reactions F. Engelke and K.H. Meiwes-Broer Spin-Orbit Effects in Chemical Reactions Spin-Orbit Effects in Chemical Reactions PJ. Dagdigian Open Shell Atomic Beam Scattering and the Spin Orbit Dependence of Potential Energy Surfaces v. Aquilanti, R Candori, G. Liuti and F. Pirani vii
7 viii Orientation and Alignment in Chemical Reactions Reactive Scattering with Oriented Molecules: Selectivity in the Ba + N 20 ~ BaO + N 2 Reaction H. Jalink, M.H.M. Janssen, M. Geijsberts, S. Stolte, D.H. Parker and J.Z.W. Wang Product Alignment in Reactive, Inelastic and Half-Collisions J.P. Simons Alignment Effects in Electronic Energy Transfer and Reactive Events S.R. Leone Fundamental Considerations in the Study of Inelastic and Reactive Collisions Involving Atoms in 1 P Electronic States M.H. Alexander and B. Pouilly Ionizing Collisions of Fast K Atoms with Oriented Symmetric Top Molecules: Preliminary Results H.S. Carman, L.F. Phillips and P.R. Brooks Saturation in Laser-Induced Fluorescence: Detection of Nascent Product Rotational Angular Momentum Alignment M.H.M. Janssen, M.A. Quesada, D.H. Parker and S.Stolte Investigation of the Orientation Dependence of the F + H2 Reaction Using Scaled Barrier Functions in the Angle-Dependent Line-of-Centres Model J.N.L. Connor and W. Jakubetz Reactions of van der Waals Complexes and Clusters Chemistry and van der Waals Complexes C. Jouvet and M. Boivineau A Theoretical Study of the Oriented Reaction HBr CO 2 + hv ~ OH + CO + Br G.C. Schatz and M.S. Fitzcharles Reactions of Molecular Ions in Association with Inert Gas Clusters AJ. Stace and D.M. Bernard Accuracy and Availability of Potential Energy Surfaces Accuracy and Availability of Potential Energy Surfaces J.N. Murrell The Calculation of Potential Energy Surfaces for Reactive Systems D.M. Hirst Electronic Deexcitation of OH(. L+) with CO(X1 L+): An Ab Initio Study A. Vegiri, S.C. Farantos, P. Papagiannakopoulos and C. Fotakis
8 Direct US of the Diatomics-in-Molecules Method in Large Systems and in Dynamical Calculations P.l Kuntz Spin-Orbit Interaction on Potential Energy Surfaces Involving Halogen Atoms N.C. Firth and R Grice Multiple Pathways in Chemical Reactions Branching Ratios in Chemical Reactions Ch. Ottinger The M + X 2 Reactions: Paradigms of Selectivity and Specificity in Electronic Multi-Channel Reactions M. Menzinger Applied Aspects of Chemical Selectivity The Role of Selective Chemical Reactions in Laser Technology J.J. Ewing State Selective Chemiluminescent Reactions for Chemical Laser Applications... '" S.l Davis and A.M. Woodward The Characterisation of the Mechanism of IF(B) Production in Fluorine I Iodide Systems D. Raybone, T.M. Watkinson and le. Whitehead IF(A-X,B-X) Chemiluminescence of Fluorine-Iodide Systems in a Crossed Molecular Beam Experiment M. Trautmann, T. Trickl and 1 Wanner Unexpected Properties of Atmospheric Reactions B.A. Thrush State Selectivity in Light Emission from Flames D.R Crosley, K.l Rensberger and RA. Copeland Conclusion Concluding Remarks Rl Donovan Organising Committee List of Participants Index ix
9 PREFACE The aim of this Workshop on "Selectivity in Chemical Reactions" was to examine the specific preferences exhibited by simple chemical reactions with regards to reagents having particular energy states, symmetries, alignment and orientation and the resulting formation of certain products with their corresponding energies, states, alignment and polarisation. Such problems come close to the ultimate goal of reaction dynamics of being able to determine experimentally and theoretically state-to-state cross sections and stereochemical effects under well defined and characterised conditions. There are many examples of highly selective and specific processes to be found in atmospheric and combustion chemistry and the production of population inversions amongst vibrational and electronic states lies at the heart of the development of chemical laser systems. Only when we can understand the fundamental processes that underlie the selectivity in the formation of products in a chemical reaction and the specific requirements of initial states of the reagents, can we expect to be able to develop the explanatory and predictive tools necessary to apply the subject to the development of new laser systems, efficient combustion schemes and specific methods of chemical synthesis, to the control of atmospheric pollution and to all problems in which it is necessary to direct the outcome of a chemical reaction in a specific way. The brief given to the Workshop was to critically review the field, to discuss the present limitations and difficulties and to identify new directions. This was achieved by having a small group of 34 participants and a mixture of nine review lectures, three panel discussions and a poster session. The topics that were covered were grouped under the headings of "Specificity of Reagent States in Chemical Reactions", "Spin-Orbit Effects in Chemical Reactions", "Orientation and Alignment in Chemical Reactions", "Reactions of van der Waals Complexes and Clusters",, "Accuracy and Availability of Potential Energy Surfaces", "Multiple Pathways in Chemical Reactions" and "Applied Aspects of Chemical Selectivity". As far as is possible, the various contributions to this book have been grouped in the same way. Inevitably, this book cannot record the discussion that took place at the Workshop or the collaborations and future projects that have originated from it. There were many themes which ran through the Workshop that connected various contributions in a way that is restricted by the above categorisations and could not have been predicted in advance. One example is the ROCO system that was discussed in the context of the photo-initiated reaction R + CO 2 within the van der Waals complex RBr-C0 2, the kinetics of the atmospheric and combustion reaction OR + CO and the relaxation of OR by CO in flames and the associated potential energy surfaces. The success of the Workshop and its ultimate record in this book is due to many people. Firstly, Dr. e. Sinclair of the NATO Scientific Affairs Division for his help in the organisation of the Workshop and Prof. J.P. Simons who was the member of the NATO "Selective Activation of Molecules" Panel who suggested this Workshop. I was greatly assisted in the scientific organisation and choice of the participants by the organising committee, Jonathan Connor, Paul Dagdigian and Steven Stolte. All the manuscripts were retyped with speed and efficiency by Debra Acton and proof-read by Tim Watkinson. To all these people and all the authors and participants, I express my grateful thanks. J.e. Whitehead, Manchester, March xi
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