Preface
Downloaded by 80.82.77.83 on October 12, 2017 | http://pubs.acs.org Publication Date: May 5, 1996 | doi: 10.1021/bk-1996-0628.pr001
SlNCE
T H E FIRST
THEORETICAL DESCRIPTION
of
nonlinear
optical
phenomena was published in 1962, many people have worked to improve our fundamental understanding of the microscopic mechanism and origin of these processes. These efforts extend from the development of simple phenomenological models for explaining experimental observations in terms of a few physical quantities to the development and application of increasingly sophisticated quantum chemical techniques to correctly predict structure-nonlinear optical property relationship information that can be used to design and develop new materials in an efficient and costeffective manner. Despite the contributions of many individuals, we felt the field lacked a single central source of information for new researchers to get a good overview of the theoretical aspects of nonlinear optical materials design. T h e symposium o n which this book is based provided a useful exchange of information. W e convinced several of the leading authorities in the field to contribute chapters describing the history and state of the art from their individual perspectives in the design and understanding of n o n linear optical materials. This book is the culmination of our efforts. T h e interest in quantum mechanical modeling of nonlinear optical materials has, fortunately, coincided with the availability of low-cost c o m puters with fast central processing units, so that it is becoming possible to address more basic and fundamental problems for increasingly complex and realistic model systems. It might even be argued that the increased demand for the computational modeling of nonlinear optical and other materials is largely responsible for the rapid pace of high-performance computer development. In addition, these demands have also made the development of software systems that can be used to model nonlinear optical materials o n these machines a profitable and competitive business. W i t h increased access to modeling tools and a spiraling cost of materials and waste disposal, computational modeling probably will acquire a more significant status and make valuable contributions to the development of new nonlinear optical materials. W e hope that this book will serve as an important and useful resource for practicing scientists as well as newcomers in the field of computational nonlinear optical materials development. W e also hope that experimentally oriented scientists may find this book useful as an aid to understanding the promise, and the limitations, of computational modeling for nonlinear optical design. ix Karna and Yeates; Nonlinear Optical Materials ACS Symposium Series; American Chemical Society: Washington, DC, 1996.
Downloaded by 80.82.77.83 on October 12, 2017 | http://pubs.acs.org Publication Date: May 5, 1996 | doi: 10.1021/bk-1996-0628.pr001
T h e chapters are grouped together by general technique(s) used for the modeling and their applications. After an introduction, graciously contributed by N . Bloembergen, one of the founders of the field, and the overview chapter, the next three chapters (2-4) focus o n the ab initio time-dependent H a r t r e e - F o c k and p o s t - H a r t r e e - F o c k techniques and their application for the calculation of molecular nonlinear optical materials. T h e n Chapters 5 - 7 discuss the H a r t r e e - F o c k - b a s e d semiempirical techniques and their applications to modeling the second- and third-order organic nonlinear optical materials. Chapters 8 and 9 focus on the development of density-functional techniques and their application to predict molecular nonlinear optical coefficients. Chapter 10 discusses a time-dependent perturbation theory for determining nonlinear optical properties of polymers. Chapters 11 and 12, also devoted to the n o n linear optical properties of polymers, discuss model Hamiltonian methods and their applications. W e conclude with an experimental chapter devoted to one of the most recent applications of nonlinear optical materials—the resonant nonlinear optical phenomenon, which presents a major challenge to theoretical modeling. Acknowledgments W e are grateful to the following people whose contributions made this book possible. First we thank all the authors for contributing their time and expertise to create authoritative and stimulating chapters. W e also thank J o h n Kester, Robert J . Hildreth, and John Wilkes of the F r a n k J . Seiler Laboratory, and Bruce Reinhardt and D o u g Dudis of Wright Laboratory for their help and valuable discussions throughout the p r o gress of this book. W e owe a special thank you to Sylvia Miles at Seiler Laboratory for organizing the chapter contributions and reviews. Finally, we gratefully acknowledge financial support for this research from the A i r F o r c e Office of Scientific Research, the Wright Laboratory Materials Directorate, and Biosym, Inc. SHASHI P. KARNA
Space Electronics Division U . S . A i r Force Phillips Laboratory 3550 Aberdeen Avenue, Southeast Kirtland Air Force Base, NM 87117-5776 ALAN T. YEATES
Polymer Branch Wright Laboratory Wright-Patterson Air Force Base, OH 45433-7750 December 20,
1995
x
Karna and Yeates; Nonlinear Optical Materials ACS Symposium Series; American Chemical Society: Washington, DC, 1996.
Introduction
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T H E H E L D O F ORGANIC NONLINEAR OPTICAL
materials has been the subject of intense research efforts during the past two decades. Several important applications in nonlinear optical devices appear close to reali zation. They have been demonstrated in principle, but the economic and engineering considerations require further developments. It is timely to have a collection of the various theoretical approaches to describe the nonlinear optical properties of large organic molecules and of polymers. The results are compared with the ever-increasing body of experimental results. They include diverse nonlinear optical phenomena such as third-harmonic generation, two-photon absorption, electric field induced second-harmonic generation, intensity-dependent index of refraction, stimulated Raman scattering, and others. This book provides an up-to-date account and critical discussion that emphasize the issues of theoretical modeling of nonlinear optical proper ties of organic materials. It is a welcome addition to the ever-growing literature in nonlinear optics. N. BLOEMBERGEN
Division of Applied Science Harvard University Pierce Hall Cambridge, MA 02138 October 29, 1995
xi Karna and Yeates; Nonlinear Optical Materials ACS Symposium Series; American Chemical Society: Washington, DC, 1996.
