Collision- and Interaction-Induced Spectroscopy PDF
Preview Collision- and Interaction-Induced Spectroscopy
Collision- and Interaction-Induced Spectroscopy 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 Plenum Publishing Corporation B Physics London and New York C Mathematical Kluwer Academic Publishers and Physical Sciences Dordrecht, Boston and London D Behavioural and Social Sciences E Applied Sciences F Computer and Systems Sciences Springer-Verlag G Ecological Sciences Berlin, Heidelberg, New York, London, H Cell Biology Paris and Tokyo I Global Environmental Change NATO-PCO-DATA BASE The electronic index to the NATO ASI Series provides full bibliographical references (with keywords and/or abstracts) to more than 30000 contributions from international scientists published in all sections of the NATO ASI Series. Access to the NATO-PCO-DATA BASE is possible in two ways: - via online FILE 128 (NATO-PCO-DATA BASE) hosted by ESRIN, Via Galileo Galilei, 1-00044 Frascati, Italy. - via CD-ROM "NATO-PCO-DATA BASE" with user-friendly retrieval software in English, French and German (© WTV GmbH and DATAWARE Technologies Inc. 1989). The CD-ROM can be ordered through any member of the Board of Publishers or through NATO-PCO, Overijse, Belgium. Series C: Mathematical and Physical Sciences -Vol. 452 Collision- and Interaction-Induced Spectroscopy edited by G.C. Tabisz Department of Physics, University of Manitoba, Winnipeg, Manitoba, Canada and M.N. Neuman Department of Physics, Okanagan University College, Kelowna, British Columbia, Canada Springer-Science+Business Media, B.V. Proceedings of the NArD Advanced Research Workshop on Induced Spectroscopy: Advances and Applications Banff, Alberta, Canada 30 August -3 September 1993 A C.I.P. Catalogue record for this book is available from the Ubrary of Congress. ISBN 978-94-010-4082-2 ISBN 978-94-011-0183-7 (eBook) DOI 10.1007/978-94-011-0183-7 Printed an acid-free paper AII Rights Reserved © 1995 Springer Science+Business Media Dordrecht Originally published by Kluwer Academic Publishers in 1995 Softcover reprint of the hardcover 1s t edition 1995 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 photo copying, recording or by any information storage and retrieval system, without written permission from the copyright owner. CONTENTS Preface Acknowledgements SECTION A - INTERACTIONS Cancellation Effects in Collision-Induced Phenomena ......................... . G. Birnbaum and B. Guillot Three-Body CILS Spectra of Gases: Experimental ........................... 31 U. Bafile, S. Pestelli, L. Ulivi, and M. Zoppi Irreducible Three-Body Dipole Moments in Hydrogen ........................ 41 M. Moraldi and L. Frommhold Ternary Effects in Far IR Absorption in the Gas Phase ........................ 51 S. Weiss Collision-Induced Dipoles and Polarizabilities for S State Atoms or Diatomic Molecules ........................................................ 61 K. L. C. Hunt and X. Li Dielectric Properties of Dense Fluids .................................... 77 T. K. Bose SECTION B - FLUIDS AT LIQUID AND NEAR-LIQUID DENSITIES Depolarized Light Scattering: The Influence of Induced Scattering on Allowed Raman and Rayleigh Bands .................................................... 87 M. Keller, A. Mueller, M. Reh, M. Roder, W. A. Steele, and H. Versmold Moments: Simulation and Theory for Rayleigh and Raman Spectra 107 A. Mueller, H. Versmold, and W. Steele Interaction-Induced Spectral Properties of Small Molecule Dense Fluids by Raman Scattering ... . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 119 F. G. Baglin vi Simulation of the Far Infrared Spectrum of Liquid Water and Steam Along the Coexistence Curve from the Triple Point to the Critical Point . . . . . . . . . . . . . . . . .. 129 B. Guillot and Y. Guissani Interaction-Induced Contributions to Spectra of Polar Liquids . . . . . . . . . . . . . . . . .. 143 B. M. Ladanyi, M. F. Skaf and Y. Q. Liang Kinetic Theory Approach to Interaction Induced Light Scattering ............... 159 J. Piasecki SECTION C - COMPLEX LIQUIDS The Characterisation of Interaction-Induced Vibrational Spectra in Complex Liquids . 169 J. Yarwood Far Infrared Spectroscopic Investigations of Liquid Mixtures .................. 201 M. Besnard, Y. Danten, T. Tassaing Theory of Infrared Bandshapes in Hydrogen-Bonded Crystals .................. 215 D. B. Murray, M. N. Neuman, and M. Falk Rayleigh-Brillouin Light Scattering in Supercooled Liquids 227 C. Dreyfus, M. J. Lebon, A. Bykhovskii, and R. M. Pick Interaction-Induced Spectra as a Tool for the Study of Structure in Supercooled Liquids and Glasses . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 235 D. Kivelson, X-C. Zeng, H. Sakai, and G. Tarjus Composition Induced Dynamic Depolarized Light Scattering from Diblock Copolymer Systems Near the Ordering Transition . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 249 G.Fytas SECTION D -SOLIDS AND INCLUSION COMPLEXES Interaction-Induced Spectra of Endohedral Complexes of Buckminsterfullerene ..... 261 C. G. Joslin, C. G. Gray, J. D. Poll, S. Goldman, and A. D. Buckingham Electric Field Effects Observed on the Infrared Spectra of Molecules Adsorbed in Zeolites ........................................................ 287 E. Cohen de Lara Atoms in Irradiated Solid Deuterium: Charge-Induced Spectra ................. 297 R. L. Brooks, 1. A. Forrest, and J. L. Hunt Induced Light Scattering from Electrically Disordered Solids .................. 307 P. Benassi, P. Gallo, G. Ruocco, G. Signorelli, and V. Mazzacurati vii On the Spectroscopy of Solid Hydrogen 323 J. D. Poll and P. H. Lim SECTION E -ELECTRONIC SPECTRA Collisional Redistribution of Light 333 M. Belsley Depolarization in Collisionally-Induced Electronic Transitions ................. 343 F. Rebentrost The Depolarized Interaction-Induced Light Scattering Spectrum of Mercury Vapor at Low Density . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 357 F. Barocchi, M. Sampoli, F. Hensel, J. Rathenow, and R. Winter SECTION F -LINE SHAPES IN GASES Calculation of Far Wings of Allowed Spectra: The Water Continuum ............ 369 R. H. Tipping and Q. Ma Calculation of High-Frequency Wings of Interaction-Induced Spectra ............ 383 C. G. Gray, C. G. Joslin, and J. D. Poll Collision-Induced and Allowed Raman Spectra in Hydrogen Gas ............... 395 A. Borysow and M. Moraldi Interference of Allowed and Collision-Induced Transitions in HD: Experiment ...... 407 L. Ulivi, Z. Lu, and G. C. Tabisz Interference of Allowed and Collision-Induced Transitions in HD: Calculation ...... 417 G. C. Tabisz, B. Gao, and 1. Cooper High-Frequency Interaction-Induced Rototranslational Wings of Molecular Spectra ... 423 Y. Le Duff, T. Bancewicz, and W. Glaz Ab Initio Interaction-Induced Dipoles and Related Absorption Spectra ............ 441 W. Meyer and L. Frommhold Far Infrared Absorption Spectra of CO with He, Ar and Xe: Experiment and 2 Calculations ..................................................... 457 M. V. Tonkov SECTION G - DIMERS Infrared Studies of van der Waals Complexes: The Low Temperature Limit of Collision- Induced Spectra . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 467 A. R. W. McKellar viii Dimer Features of H2-H2 and Isotopomers at Low Temperatures ................ 485 J. Schaefer The Pure Translational Spectrum of Low Temperature Hydrogen Gas ............ 495 E. H. Wishnow, I. Ozier, and H. P. Gush Semiclassical Calculations of Profiles of Induced Spectra . . . . . . . . . . . . . . . . . . . .. 507 N. Meinander SECTION H - ASTROPHYSICS Induced Spectra in Planetary Atmospheres . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 517 L. M. Trafton Collision-Induced Molecular Absorption in Stellar Atmospheres ..... . . . . . . . . . .. 529 A. Borysow SECTION I - ASSESSMENT Workshop Report: Gases 541 J. L. Hunt Workshop Report on Liquids ......................................... 545 C. J. Montrose Some Reflections at the End of the Workshop . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 551 L. Frommhold AUTHOR INDEX .................................................... 571 CHEMICAL INDEX . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 573 SUBJECT INDEX . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. 581 PREFACE Collision-or interaction-induced spectroscopy refers to radiative transitions, which are forbidden in free atoms or molecules, but which occur in clusters of interacting atoms or molecules. The most common phenomena are induced absorption, in the infrared region, and induced light scattering, which involves inelastic scattering of visible laser light. The particle interactions giving rise to the necessary induced dipole moments and polarizabilities are modelled at long range by multipole expansions; at short range, electron overlap and exchange mechanisms come into play. Information on atomic and molecular interactions and dynamics in dense media on a picosecond timescale may be drawn from the spectra. Collision-induced absorption in the infrared was discovered at the University of Toronto in 1949 by Crawford, Welsh and Locke who studied liquid O2 and N2. Through the 1950s and 1960s, experimental elucidation of the phenomenon, particularly in gases, continued and theoretical underpinnings were established. In the late 1960s, the related phenomenon of collision-induced light scattering was first observed in compressed inert gases. In 1978, an 'Enrico Fermi' Summer School was held at Varenna, Italy, under the directorship of J. Van Kranendonk. The lectures, there, reviewed activity from the previous two decades, during which the approach to the subject had not changed greatly. In 1983, a highly successful NATO Advanced Research Workshop was held at Bonas, France, under the directorship of G. Birnbaum. An important outcome of that meeting was the demonstration of the maturity and sophistication of current experimental and theoretical techniques. At the time of Bonas, activity was largely centred on fundamental aspects of the problem through spectra of gas, liquids and solids, composed of small, highly symmetric molecules. Since then studies in this area have continued. For example, reliable information on irreducible three body interactions is now being obtained, providing surprising insights into the induction mechanism. There is increased interest in induced electronic transitions in atoms which extend the frequency range of interest from the infrared to the visible and ultraviolet. Equally striking, however, has been the progress in the alllllication of induced spectroscopy to the elucidation of more general scientific problems. Thus it is being used to unravel the dynamics of complex fluids and of molecular dimers. Data from induced spectra are employed to help specify semi-empirical intermolecular potentials. Ab initio computational techniques are profoundly tested in calculating induced spectra or in providing parameters necessary to derive information from the spectra. The modelling of atmospheres of the heavy planets and their satellites involves the effects of induced transitions. The opacities of certain cool stars may be controlled by induced absorption in H2 and H2-He mixtures. From August 29 to September 3, 1993, a NATO Advanced Workshop was held at the Banff Centre for Conferences, Banff, Alberta, Canada. It was attended by 48 physicists, chemists and astrophysicists who reviewed and consolidated the progress made over the past ten years. This volume records the papers delivered at that meeting in a review and tutorial format designed hopefully to make them accessible to the expert and neophyte alike. They are grouped to correspond to broad subsets of the field. ix x The subject of the basic molecular interactions responsible for induced phenomena is discussed in Section A. Striking advances have been made in the treatment of multibody effects, particularly three-body interactions. In the past, interactions had been considered almost exclusively to be pairwise additive. Liquids constitute a complicated physical system. It is frequently the practice to employ relatively simple models in order to include induced phenomena in a situation already difficult to analyze. For example, in light scattering, often only the first-order dipole-induced-dipole contribution to the induced polarizability is taken. The spectra of liquids show features due to allowed and induced transitions and to important interference effects between them. The relation between hydrogen bond dynamics and spectroscopic observations received close attention at the Workshop. Two papers addressed supercooled glass-forming liquids and the connection between the mode coupling theory of vitreous transitions and induced phenomena. Liquids and complex liquids are discussed in sections B and C. Section D contains papers on solids and inclusion complexes. Well studied systems such as KCl-KBr (alkali halides) show spectral features which, it is now realized, may be due to induced transitions. The recently discovered novel molecular structures known as fullerenes can provide environments for trapped impurity atoms and give rise to induced absorption and scattering spectra. Solid hydrogen continues to be a rich source of information on intermolecular interactions and induced transitions. The gas is a relatively well-understood physical system and here much insight can be gained into the nature of the interactions responsible for the induction process. The spectral lineshape may be studied in great detail. Far wing spectra provide severe tests for theories of line broadening and can contain contributions from induction mechanisms involving high-order multipole moments and polarizabilities. These gas phase spectra, and perhaps especially those of van der Waals dimers, lead to the specification of accurate intermolecular potentials. The astrophysical applications arise through induced transitions in gases. Much of the highly quantitative work on gases is made possible by the availability of accurate ab initio calculations of pair dipole moments and polarizabilities. These topics are treated in sections E through H. The volume closes with a final section containing three papers which attempt to identify the major themes of the workshop, assess progress and speculate about the future. It is hoped that this melding of new information on the fundamental physics of induced phenomena with the growing diversity of applications will initiate a new round of advances in a subject whose importance and influence continues to grow. References Here are listed some review articles and bibliographies appearing elsewhere which the reader may find helpful. Welsh, H. L. (1972) 'Pressure-induced absorption spectra of hydrogen', in D. A. Ramsay (ed.), MTP International Review of Science, Vol. 3, Spectroscopy, Butterworths, London, pp. 33-71. Tabisz, G. C. (1979) 'Collision-induced Rayleigh and Raman Scattering', in A Specialist Periodical Report, Molecular Spectroscopy, Vol. 6, The Chemical Society, London, pp. 136-173. Birnbaum, G., Guillot, B., and Bratos, S. (1982) 'Theory of collision-induced lineshapes - absorption and light scattering at low density', Adv. Chern. Phys. 51,49-112.
The list of books you might like
