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1 Topics in Applied Physics Volume 82 ~ Available online h ttp :/ / lin k.springer de link.springer-ny.corn Available Online Topics in Applied Physics is part of the Springer LINK service. For all customers with standing orders for Topics in Applied Physics we offer the full text in electronic form via LINK free of charge. Please contact your librarian who can receive a password for free access to the full articles by registration at: If you do not have a standing order you can nevertheless browse through the table of contents of the volumes and the abstracts of each article at: There you will also find more information about the series. Springer Berlin Heidelberg New York Barcelona Hong Kong London Milan Paris Tokyo PhysicsandAstronomy[]~ ONLINE LIBRARY htt p:// e/phys/

2 Topics in Applied Physics Topics in Applied Physics is a well-established series of review books, each of which presents a comprehensive survey of a selected topic within the broad area of applied physics. Edited and written by leading research scientists in the field concerned, each volume contains review contributions covering the various aspects of the topic. Together these provide an overview of the state of the art in the respective field, extending from an introduction to the subject right up to the frontiers of contemporary research. Topics in Applied Physics is addressed to all scientists at universities and in industry who wish to obtain an overview and to keep abreast of advances in applied physics. The series also provides easy but comprehensive access to the fields for newcomers starting research. Contributions are specially commissioned. The Managing Editors are open to any suggestions for topics coming from the community of applied physicists no matter what the field and encourage prospective editors to approach them with ideas. See also: Managing Editors Dr. Claus E. Ascheron Springer-Verlag Heidelberg Topics in Applied Physics Tiergartenstr Heidelberg Germany ascheron@springer.de Dr. Hans J. K61sch Springer-Verlag Heidelberg Topics in Applied Physics Tiergartenstr. ~ Heidelberg Germany koelsch@springer.de Assistant Editor Dr. Werner Skolaut Springer-Verlag Heidelberg Topics in Applied Physics Tiergartenstr. t Heidelberg Germany skolaut@springer.de

3 Vladimir M. Shalaev (Ed.) Optical Properties of Nanostructured Random Media With 18 5 Figures ~ Springer

4 Prof. Vladimir M. Shalaev School of Electronical and Computer Engineering Purdue University West Lafayette, IN 479o USA edu Library of Congress Cataloging-in-Publication Data Optical properties of nanostructured random media / Vladimir M. Shalaev (ed.). p. cm. -- (Topics in applied physics, ISSN ; v. 82) Includes bibliographical references and index. ISBN (alk. paper) 1. Nanostructure materials. 2. Nonlinear optics. I. Shalaev, Vladimir M., 195% II. Series. TA418.9.N '1--dc Physics and Astronomy Classification Scheme (PACS): k, 42.7o.-a, 73.zo.Mf, 78.3o.Ly, w, 81.o5.-t ISSN print edition: o3o ISSN electronic edition: 1437-o859 ISBN 3-54o-4zo31-z Springer-Verlag Berlin Heidelberg New York This work is subiect to copyright. All rights are reserved, whether the whole or part of the material is concerned, specifically the rights of translation, reprinting, reuse of illustrations, recitation, broadcasting, reproduction on microfilm or in any other way, and storage in data banks. Duplication of this publication or parts thereof is permitted only under the provisions of the German Copyright Law of September 9,1965, in its current version, and permission for use must always be obtained from Springer-Verlag. Violations are liable for prosecution under the German Copyright Law. Springer-Verlag Berlin Heidelberg New York a member of BertelsmannSpringer Science+Business Media GmbH Springer-Verlag Berlin Heidelberg zooz Printed in Germany The use of general descriptive names, 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. Typesetting: DA-TEX Gerd Blumenstein, Leipzig Cover design: design e~ production GmbH, Heidelberg Printed on acid-free paper SPIN: /31411mf o

5 Preface The search for new materials is one of the defining characteristics of modern science and technology. Novel mechanical, electrical, magnetic, chemical, biological, and optical devices are often the result of the fabrication of new materials. Of specific interest to this book, recent advances in optical science and technology, such as the development of new lasers, detectors, and photonic devices, have relied heavily on advances in materials research. This book is the result of collective efforts of leading experts in the field of nonlinear optics of nanostructured materials. The authors try to address, in particular, the fundamental problem of the way the symmetry of nanostructured materials affects their physical properties. In other words, given nanometer-size particles, what geometrical structure should be chosen for fabricating a material with desired properties. Typically, different symmetries are best suited for different applications. For some properties a periodic structure is ideal, whereas for others different types of symmetries, often random ones, would result in better performance of a material. Modern nanotechnology allows one to fabricate materials with almost any structure; this opens new avenues in engineering nanomaterials with desired properties. Much of science is dominated by questions of symmetry. This is especially obvious in condensed matter physics where translational symmetry dominates both concept and language. And with justification; the elegance of symmetry arguments is so appealing that it tends to push aside many other issues. Yet there is a host of phenomena whose symmetries, if they exist at all, are hidden: the dynamics of a pile of sand; the growth through accretion of clusters such as soot particles and algal colonies; thin film growth and surface etching; the structures of cermets, porous media, globular polymers and proteins, randomly branched objects, and so on. These have always been items of fascination. However, their complexity had, in the past, forestalled the same level of deep dynamic and structural understanding as for crystals. All that is changing; interest in "disordered" systems is growing rapidly owing to the advent of powerful and plentiful computational resources which have dragged in their wake the theoretical innovations needed to truly understand these phenomena. Among the resulting insights are, ironically, the discovery of new symmetries: a seemingly unsymmetrical cluster, tbr example, might, possess dilation symmetry -- when portions of it are magnified or reduced

6 VI Preface they look structurally similar to the whole. The fascination with nonlinear systems has even led to the insight that order is often a parametric accident of chaos. The symmetry of a nanostructured material plays a key role in its properties. For example, periodically arranged dielectric nanoparticles in photonic band crystals, with certain types of defects, can be used for fabricating waveguides and microcavities with superb properties. On the other hand, in a number of applications, disordered nanomaterials may surpass their geometrically ordered counterparts. For example, random but statistically scale-invariant structures of metal nanoparticles, such as fractal aggregates of colloidal particles and percolation metal dielectric fihns, permit achieving the largest local-field enhancements in a broad spectral range. This property is crucial for designing optical materials with the broadband amplification of nonlinear responses and for various types of spectroscopy. Thus, although in many cases geometrically ordered nanostructured materials have superb performance, in some other cases, their disordered counterparts, or materials combining both ordered and disordered components, may have better properties. The optics of disordered nanomaterials displays a rich variety of effects some of which are hardly intuitive. Field localization of various sorts occur and recur in a wide gamut of disordered systems, most strikingly in those possessing dilation symmetry, leading to the enhancement of many optical phenomena, especially nonlinear processes. Making judicious use of these enhancement effects and of other aspects of the many complex resonances that distinguish these systems can lead to new and unexpected physics and to such applications as very low threshold lasers (whose cavities are self-organizing loops of coherently scattered events in highly unconventional media), superspectroseopy of single molecules and nanocrystals, and new classes of optical amplifiers and switchers. When developed, in the fullness of time, these disordered materials may attain a level of practical importance and versatility surpassing their geometrically ordered counterparts in certain areas of applications. I need to say a few words as a guide to the contents of the book. The first four chapters (Sipe and Boyd; Bergman and Stroud; Ma et al.; Sibilia et al.) describe recent theoretical and experimental studies on optical nonlinearities of various composite materials. The most important message here is that nonlinear optical responses of a nanocomposite comprising several materials can significantly exceed the individual nonlinearities of the materials. The resultant enhancement of optical nonlinearities depends strongly on the symrnetry of nanostructured composites. As mentioned, the dilation symmetry of fractal aggregates (Shalaev; Draehev et al.; Kim et al.) and percolation metal dielectric composites (Sarychev and Shalaev; Gadenne and Rivoal) may result in particularly large optical nonlinearities in a very broad spectral range, from the near ultraviolet to the midinfrared. The enhanced local responses of randora nanocomposites can be used for various types of spectroscopy, including

7 Preface VII Raman and hyper-raman spectroscopy of single molecules (Moskovits et al.; Kneipp et al.). Magneto-optical phenomena in ferromagnetic cermets are discussed in the chapter by Gadenne. Several chapters of this book address the problem of multiple light scattering in random media. The role of magnetic field in light scattering and propagation is considered in the chapter by van Tiggelen and Rikken. Random lasers with coherent feedback provided by multiple scattering are discussed in the Chapter by Cao. The Chapter by Bozhevolnyi describes scattering and localization of surface plasmon polaritons studied by scanning near-field optical microscopy. Multiple scattering phenomena in linear and nonlinear optical processes on rough metal films are reviewed in the Chapter by Leskova et al.. Altogether, tile chapters review important recent advances in nonlinear optics of random media. Finally, I would like to express my deep appreciation for the time and effort that the authors invested in writing their excellent chapters. I thank all the authors for their genuine interest in this publication and for their cooperation. I am also grateful to Viktor Podolskiy at New Mexico State University who helped with the editorial work. West Lafayette, Indiana, USA September 2001 Vladimir M. Shalaev

8 Contents Nanocomposite Materials for Nonlinear Optics Based on Local Field Effects John E. Sipe and Robert W. Boyd Introduction Linear Optical Properties Nonlinear Optical Properties Recent Advances References Response of Composite Media Made of Weakly Nonlinear Constituents David J. Bergman and David G. Stroud Introduction Perturbation Theory Limiting Cases and Exactly Solvable Microstructures Parallel Cylinders and Parallel Slabs Dilute Regime and Clausius Mossotti Approximation Self-Consistent Effective Medium Approximation and Its Breakdown Quasi-static Resonances: Enhancement of Nonlinearity and Intrinsic Optical Bistability Solvable Microstructures The Principle of "Zero Virtual Work" and Its Application Harmonic Generation and Induced Nonlinearity References Third-Order Nonlinear Properties of Au Clusters Containing Dielectric Thin Films Hongru Ma, Ping Sheng, and George K. L. Wong Introduction Experimental Preparation and Characterization of Samples Nonlinear Optical Measurements... 45

9 X Contents 3. Theoretical General Theory Application of the Theory to Four Effective Medium Theories Illustrations and Comparison of Theory with Experiments References Linear and Nonlinear Optical Properties of Quasi-Periodic One-Dimensional Structures Concita Sibilia, Mario Bertolotti, Marco Centini, Giuseppe D'Aguanno, Michael Scalora, Mark J. Bloemer, and Charles M. Bowden Introduction Something about Fractals Optical Properties of Filters Based on a Fractal Code Dispersive Properties of One-Dimensional Filters Metal Dielectric Quasi-Periodic Filters Nonlinear Model of the Filter Mesoscopic Layered Structures Conclusions References Optical Nonlinearities of Fractal Composites Vladimir M. Shalaev Introduction Local-Field Enhancement in Nanospheres and Nanospheroids Local-Field Enhanced Optical Responses in Fractal Aggregates Enhanced Optical Nonlinearities in Fractals References Nonlinear Optical Effects and Selective Photomodification of Colloidal Silver Aggregates Vladimir P. Drachev, Sergey V. Perminov~ Sergey G. Rautian, and Vladimir P. Safonov Spectral Dependenceof Selective Photomodification in Colloidal Silver Aggregates Local Optical Nonlinearities in Silver Colloids Nonlocal Optical Nonlinearities in Silver Colloids Chirality of Plasmon Modes Experiments on Nonlinear Gyrotropy in a Macroscopic Sample Conclusion References

10 Contents XI Fractal-Microcavity Composites: Giant Optical Responses Won-Tae Kim, Vladimir P. Safonov, Vladimir P. Drachev, Viktor A. Podolskiy, Vladimir M. Shalaev, and Robert L. Armstrong Introduction Optical Properties of the Composites Fractal Silver Aggregates Microcavities Composites Lasing in Fractal-Microcavity Composites Ultra-Broadband nm Light Emission References Theory of Nonlinear Optical Responses in Metal-Dielectric Composites Andrey K. Sarychev and Vladimir M. Shalaev Introduction Percolation and Anderson Transition Problem Scaling in LocM-Field Distribution Enhanced Optical Nonlinearities References S ur face-plasmon-enhanced Nonlinearities in Percolating 2-D Metal-Dielectric Films: Calculation of the Localized Giant Field and Their Observation in SNOM Patrice Gadenne and Jean C. Rivoal Introduction Semicontinuous FractM Metallic Films Thin Film Deposition Nonoptical Characterizations Linear Optical Measurements Linear Optical Properties in the Percolation Regime Enhancement of Optical Processes in Semicontinuous Metallic Films Plasmon Resonance Shalaev-Sarychev Approach Anderson Localization The Percolation Regime Experimental Observation of "Hot Spots" Using a Scanning Near-Field Optical Microscope Near-Field Versus Far-Field Imaging Fibers or Tips? The Setup Experimental Observation of "Hot Spots"

11 XII Contents 5. Conclusion References SERS and the Single Molecule Martin Moskovits, Li-Lin Tay, Jody Yang and Thomas Haslett Introduction Results and Discussion Interpretation Conclusion References Nonlinear Raman Probe of Single Molecules Attached to Colloidal Silver and Gold Clusters Katrin Kneit)p, Harald Kneipp, Irving Itzkan, Ramachandra R. Dasari, Michael S. Feld and Mildred S. Dresselhaus Introduction Surface-Enhanced Linear and Nonlinear Raman Scattering Experimental Surface-Enhanced Linear Raman Scattering Surface-Enhanced Raman Scattering from Single Wall Carbon Nanotubes Pumped Anti-Stokes Raman Scattering Surface-Enhanced Hyper-Raman Scattering (SEHRS) Discussion References Electromagnetic Response of Ferromagnetic Cermet: Superparamagnetic Transition Mireille Gadenne Introduction Description of tile Materials Studied Cermet Definition of a Ferromagnetic Mono-Domain Particle Magnetic Anisotropy Relaxation Time Magnetization and Coercive Field Relation between Measuring Time, Critical Volume, and Blocking Temperature Tb Interaction with an Electromagnetic Wave: Theoretical Approach Study of the Effective Dielectric Function Study of Effective Magnetic Permeability of a Cermet

12 Contents XIII 5. Numerical Results and Influence of Various Parameters Superparamagnetism Influence of the Filling Factor Variations of Magnetic Permeability versus Frequency Influence of the Particle Size Influence of Temperature on the Variation in # versus Frequency Consequences on Optical Absorption Expression of Reflectance and Transmittance of a Thin Magnetic Fihn Application to Cermet: Curves in the Spectral Range Corresponding to the Relaxation Time To Conclusion References Manipulating Light with a Magnetic Field Bart A. van Tiggelen and Geert L. J. A. Rikken Introduction Magneto-Optics of Homogeneous Media Magnetodeflection of Light Bending of Light by Magnetic Fields Magneto-Optics of Heterogeneous Media Single Magneto-Mie Scattering Multiple Magnetoscattering of Light Theory of Magnetodiffusion Experiments on Magnetodiffusion Note Added in Proof References Random Lasers with Coherent Feedback Hui Cao Introduction Two Kinds of Random Lasers Random Lasers with Resonant Feedback Microlasers Made of Disordered Media Theoretical Modeling Conclusion References

13 XIV Contents Localization Phenomena in Elastic Surface Plasmon Polariton Scattering Sergey I. Bozhevolnyi Introduction Near-Field Mapping of Surface Plasmon Polaritons Elastic and Inelastic Scattering Topographical Artifacts Influence of a Probe Image Formation Localization of Surface Plasmon Polaritons Single and Multiple Scattering Observation of Localized Surface Polaritons Statistics of Surface Polariton Intensity Distributions Conclusions References Multiple-Scattering Phenomena in the Second-Harmonic Generation of Light Reflected from and Transmitted Through Randomly Rough Metal Surfaces Tamara A. Leskova, Alexei A. Maradudin and Eugenio R. MSndez Introduction Characterization of a Random Surface Clean Metal Surfaces Linear and Nonlinear Boundary Conditions Strongly Rough Surfaces Weakly Rough Surfaces The Kretschmann Geometry Linear and Nonlinear Boundary Conditions Strongly Rough Surfaces Weakly Rough Surfaces Conclusions References Index