{"title":"Nonlinear Optical Susceptibilities; Beyond the Local Field Approximation","authors":"S. Mukamel, J. Knoester","doi":"10.1364/nlopm.1988.mb3","DOIUrl":"https://doi.org/10.1364/nlopm.1988.mb3","url":null,"abstract":"The Bloch-Maxwell equations are usually derived for isolated molecules interacting with an external electromagnetic field. This is justified in the limit of low molecular density, where intermolecular forces may be neglected. The problem which we address in this work is how to extend these equations in a systematic way to incorporate properly intermolecular forces. We thus develop a systematic microscopic basis for the calculation of nonlinear response functions and susceptibilities. Such a theory is essential for relating microscopic, single-molecule, polarizabilities to the macroscopic susceptibilities of optical materials. The local field approximation [1,2] is a mean-field procedure which is widely used in the calculation of molecular susceptibilities at finite densities, when intermolecular forces are important. The local field model provides a simple way to relate the polarizabilities of isolated molecules to the macroscopic susceptibilities. It is clear, however, that this procedure is not rigorous. It fails to take properly into account the correlated dynamics of the interacting many-body system, i.e., correlations among the molecules, as well as correlations between the molecules and the radiation field. Short-range forces (e.g., exchange) are totally neglected in this procedure. Moreover, even the dipoledipole forces are not fully taken into account. The resulting susceptibilities do not depend at all on the wavevectors (apart from the local field contribution) but just on the frequencies. This indicates that processes such as exciton migration and energy transfer and transport (e.g., the Forster transfer) are neglected in this procedure. Such processes are often added phenomelogically in order to interpret transient grating spectroscopy[3], which is a four-wave mixing technique that measures transport processes by following the wavevector dependence of the susceptibilities. The common derivation of the local field approximation cannot be extended to include these processes, since it is intrinsically a mean-field single molecule theory.","PeriodicalId":208307,"journal":{"name":"Nonlinear Optical Properties of Materials","volume":"2 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"131216737","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Twenty-Five Years of Nonlinear Optics","authors":"N. Bloembergen","doi":"10.1364/nlopm.1988.me1","DOIUrl":"https://doi.org/10.1364/nlopm.1988.me1","url":null,"abstract":"Summary not available.","PeriodicalId":208307,"journal":{"name":"Nonlinear Optical Properties of Materials","volume":"49 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"132817068","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Third-Order Optical Susceptibility in n-i-p-i GaAs Arising from Nonparabolic Electronic Subbands","authors":"K. Choquette","doi":"10.1364/nlopm.1988.md3","DOIUrl":"https://doi.org/10.1364/nlopm.1988.md3","url":null,"abstract":"Semiconductor superlattices allow the development of materials with enhanced nonlinear optical characteristics over those found in bulk semiconductors. For both doping and compositional superlattices a one-dimensional periodic potential is introduced which modifies the electronic energy band structure. This paper reports the investigation of the optimization of nonparabolic subbands in compensated short-period GaAs doping superlattices for enhancement of a nonresonant third-order optical susceptibility. This nonlinear phenomenon would be useful for nonlinear optical applications requiring long wavelengths or wavelength insensitivity.","PeriodicalId":208307,"journal":{"name":"Nonlinear Optical Properties of Materials","volume":"35 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"114485909","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
D. Hall, N. Borrelli, W. H. Dumbaugh, M. Newhouse, D. Weidman
{"title":"Nonlinear Measurements of High-Index Glasses","authors":"D. Hall, N. Borrelli, W. H. Dumbaugh, M. Newhouse, D. Weidman","doi":"10.1364/nlopm.1988.tha2","DOIUrl":"https://doi.org/10.1364/nlopm.1988.tha2","url":null,"abstract":"It has recently been emphasized [1] that transparent glasses with large and fast (< 1ps) nonresonant nonlinearites may be a viable alternative to semiconductor and organic materials for certain photo–optic switching applications, including multi–GHz demultiplexing and highly parallel ‘pipeline’ calculations. We report results of measurements of high–index glasses that exhibit large values of χ3.","PeriodicalId":208307,"journal":{"name":"Nonlinear Optical Properties of Materials","volume":"49 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"124769422","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Photorefractive Optical Nonlinearities","authors":"A. Glass","doi":"10.1364/nlopm.1988.mc1","DOIUrl":"https://doi.org/10.1364/nlopm.1988.mc1","url":null,"abstract":"The photorefractive effect is well suited to optical image processing. The talk will emphasize the optimization of the speed and sensitivity of photorefractive materials.","PeriodicalId":208307,"journal":{"name":"Nonlinear Optical Properties of Materials","volume":"1 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"129746041","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Crystals for Nonlinear Optics","authors":"C. L. Tang, L. Cheng, W. Bosenberg, H. Nakatani","doi":"10.1364/nlopm.1988.wc1","DOIUrl":"https://doi.org/10.1364/nlopm.1988.wc1","url":null,"abstract":"For a nonlinear optical crystal to be useful, optical nonlinearity is only one of many equally important properties that the material must have. In fact, large optical nonlinearity may be one of the easier material properties to predict and to have. Frequently, it is the other properties such as the mechanical, thermal, chemical, hygroscopic, linear dispersion and birefringence, optical damage, and crystal growth properties that are more difficult to predict. Yet, failure to meet some minimum requirement in any one of these properties could easily disqualify the material for a given application. Thus, in the search for new nonlinear optical materials, far more than the optical nonlinearity must be considered. Nevertheless, everything being equal, obviously the larger the optical nonlinearity the better is the material. In this talk, we will first review the basics of the nonlinear optical properties of crystalline materials.","PeriodicalId":208307,"journal":{"name":"Nonlinear Optical Properties of Materials","volume":"8 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"132473736","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Superradiative Decay and Enhanced Optical Nonlinearity of Excitons in Qunatum Wells","authors":"E. Hanamura","doi":"10.1364/nlopm.1988.tud1","DOIUrl":"https://doi.org/10.1364/nlopm.1988.tud1","url":null,"abstract":"We evaluate the exciton coherence length and discuss theoretically how it determines its superradiative decay time and its third-order optical nonlinearity in the qunatum wells and microcrystallites.","PeriodicalId":208307,"journal":{"name":"Nonlinear Optical Properties of Materials","volume":"2 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"121082571","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Second Harmonic Generation in β-Barium Borate using Elliptical Focussing","authors":"T. Freegarde, J. Coutts, A. Corney","doi":"10.1364/nlopm.1988.mf5","DOIUrl":"https://doi.org/10.1364/nlopm.1988.mf5","url":null,"abstract":"Elliptical focussing can be used to enhance SHG efficiency significantly in highly birefringent media such as β-barium borate.","PeriodicalId":208307,"journal":{"name":"Nonlinear Optical Properties of Materials","volume":"29 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"114280471","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Optical Nonlinearities in Organics","authors":"G. Meredith","doi":"10.1364/nlopm.1988.ma1","DOIUrl":"https://doi.org/10.1364/nlopm.1988.ma1","url":null,"abstract":"Major advances are being made in the science and technologies of nonlinear optics with organics. Therefore, in addition to reviewing fundamentals, a critical overview of models, calculations, experimental methods and results, and material scouting and development efforts is presented.","PeriodicalId":208307,"journal":{"name":"Nonlinear Optical Properties of Materials","volume":"255 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"132525821","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Theoretical Considerations on Second-Order Nonlinearities of Organic Molecules","authors":"G. Wagnière, J. Hutter","doi":"10.1364/nlopm.1988.ma2","DOIUrl":"https://doi.org/10.1364/nlopm.1988.ma2","url":null,"abstract":"It is now widely recognized that the long-wavelength second-order nonlinear optical properties of organic molecules which absorb in the visible or near-UV, may be reasonably well interpreted by semiempirical quantum chemical calculations. Methods such as PPP (taking into account only π electrons), CNDO or INDO (including also σ valence electrons), are generally used in conjunction with the sum-over-states expressions to obtain the tensor elements of β(ω1 + ω2; −ω1, −ω2). Such calculations may predict correct orders of magnitude, show the relative influence of donor and acceptor substituents, and enable one to identify the dominant contributions to particular tensor elements. Although these methods have a common-structure, namely a SCF part followed by some configuration interaction (CI), they also present severe limitations. They are based on a number of particular approximations, and certain intermediate quantities are calibrated on empirical data, which makes in general the results parameter-dependent1-4). This raises the question on how the situation may be improved. With the advent of large-scale vectorized computers, the possibilities of obtaining better molecular wave-functions also by ab initio methods seem promising. How will this affect the computation of nonlinear optical susceptibilities?","PeriodicalId":208307,"journal":{"name":"Nonlinear Optical Properties of Materials","volume":"16 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"134373781","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}