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This book assembles both theory and application in this field, to interest experimentalists and theoreticians alike. Part 1 is concerned with the theory and computing of non-linear optical (NLO) properties while Part 2 reviews the latest developments in experimentation. This book will be invaluable to researchers and students in academia and industry, particularlrly to anyone involved in materials science, theoretical and computational chemistry, chemical physics, and molecular physics.
The field of nonlinear optics has expanded rapidly over the last 50 years as these nonlinear optical (NLO) effects are increasing utilised in devices. NLO involves the manipulation of light by as it travels through a material, which has the potential to be used in all optical data processing as well as intensity dependent imaging. These applications demand new materials with large nonlinear optical properties, of which organometallics and metal coordination complexes have a good reputation. Organometallics, especially ruthenium alkynyl complexes permit many different structural alterations which result in linear and nonlinear optical property tuning allowing for precise design of materials, however understanding of the structure-property relationships is imperative for such design. In this work, complexes with a systematically varied structure have been had their third order nonlinear optical properties analysed utilising the Z-scan technique covering a broad wavelength range; the nonlinear absorptive properties being of particular interest. Comparison of these results allows for determination of structural moieties that give high NLO response. Ruthenium alkynyl dendrimers have considerable nonlinear absorptive properties and the second part of this work covers the modification of the core structure to assess its potential for inclusion into larger systems. The level of core substitution (the number of arms branching from the core) and even the core symmetry influences the electronic properties of the molecule and therefore the nonlinear optical properties. The design limitations and synthesis of ruthenium alkynyl complexes with twelve different core substitutions is detailed and the optical and nonlinear optical properties discussed.
High power laser pulses can be a threat to optical sensors, including the human eye. Traditionally this threat has been alleviated by colour filters that block radiation in chosen wavelength ranges. Colour filters’ main drawback is that they block radiation regardless of it being useful or damaging, information is lost for wavelengths at which the filter is active. Protecting the entire wavelength range of a sensor would block or strongly attenuate the radiation needed for the operation of the sensor. Sol-gel glasses highly doped with optically non-linear chromophores have previously shown high optical quality in combination with efficient optical power limiting (OPL) through reverse saturable absorption (RSA). These filters transmit visible light unless the light fluence is above a certain threshold. A key design consideration of laser protection filters is linear absorption in relation to the threshold level. A high linear absorption means that the user’s view is degraded by the filter. To model the photokinetics of RSA chromophores, the five-level population model is widely used. It consists of three singlet and two triplet levels. Model parameters relevant for OPL performance include linear absorption cross-sections, two-photon absorption (2PA) cross-sections, lifetimes, quantum yields and inter-system-crossing (ISC) times. The dominant design paradigm is to have a highly absorbing and long-lived triplet state that is quickly populated by ISC during the beginning of a laser pulse. To simultaneously achieve a lower threshold and linear absorption a vast number of materials for self-activated filters were evaluated, either as bulk glasses or solutions. An f/5 setup was used to evaluate their OPL performance while several photophysical measurements were performed to gain an understanding of system behaviour. The first three series of methyltriethoxysilane (MTEOS) Sol-Gel glasses were doped with gold nanoparticles either solely, or with one of two Pt-acetylide chromophores. One with shorter conjugated ligands, the second with similar but longer conjugated ligands. Finally, a series of multi-branched fluorene chromophores were evaluated in solution. Their central moiety was either an organic benzene unit or an ISC promoter in the form of para-dibromobenzene or a platinum(II)-alkynyl unit. For the gold nanoparticle doped glasses, the lower performance Pt-acetylide with short ligands had its OPL threshold lowered at 600nm while the glasses doped with only gold nanoparticles showed no OPL at all. Secondly, the enhancement was most pronounced for very low gold nanoparticle concentrations. While gold nanoparticles alone showed good OPL performance at 532 nm, at this wavelength neither Pt-acetylide showed an obvious OPL enhancement beyond linear absorption losses from codoping with gold nanoparticles. The improved OPL performance at 600 nm was attributed to stronger 2PA, by electric field enhancement from the gold nanoparticles. The lack of detectable OPL improvement for 532 nm and for the higher performance Pt-Acetylide chromophore with long ligands were qualitatively explained by a lower sensitivity to 2PA on system performance. A degraded performance from linear absorption by excess nanoparticles in front of the focus explained the weakening of the enhancement at higher gold nanoparticle concentrations. All three fluorene chromophores, including the chromophore without a central ISC promoter, showed broadband OPL through the visible spectrum. The OPL performance of the two chromophores with ISC promoters was expected considering their transient absorption at microsecond time-scales. For the fluorene chromophore without an ISC-promoter, ultra-fast transient absorption was used to identify singlet excited state absorption as the source of the OPL performance. Both of these series of experiments demonstrate how a simplistic view of simply increasing desired photophysical parameters, e.g. effective 2PA cross-section or ISC quantum yield, do not always result in a noticeable increase in system performance. By employing numerical population models it was possible to identify which parameters had the highest impact on OPL performance. Laserpulser med hög effekt kan vara ett hot mot optiska sensorer, inklusive det oskyddade ögat. Traditionellt har detta hot hanterats med färgfilter som stoppar strålning inom valda våglängdsband. Färgfilters huvudsakliga begränsning ligger i att de tar bort strålning oberoende av om den är användbar eller skadlig, att information försvinner för de våglängder filtret skyddar för. Skydd över hela det våglängdsband en sensor verkar i skulle stoppa eller kraftigt försvaga strålningen som sensorn behöver för att fungera. Sol-gel glas högdopade med optiskt icke-linjära molekyler har tidigare visat hög optisk kvalité i kombination med en effektiv optisk effektbegränsning (OPL) via omvänd blekning (RSA). Dessa filter transmitterar synligt ljus så länge ljusets fluens (pulsenergi per area [J cm-2]) inte ligger över en viss begränsningsnivå. En nyckelfaktor i designen av laserskyddsfilter är linjärabsorption kontra begränsningsnivå. Genom att öka kromoforkoncentrationen så kan begränsningsnivån sänkas till kostnad av ökad linjärabsorption. Detta betyder dock att användarens omvärldsuppfattning genom filtret riskerar att minska. För att modellera fotokinetiken av RSA-molekyler har femnivåpopulationsmodellen varit vida använd. Den består av tre singlet-nivåer och två tripletnivåer. Modellparametrar relevanta för OPL-prestanda innefattar kvantverkningsgrader, olika övergångars linjärabsorptionstvärsnitt, tvåfotonsabsorptionstvärsnitt och livstider samt halveringstider för överföring mellan singlet och triplettillstånd. Den dominanta designparadigmen är att ha ett hög- absorberande och långlivat tripletläge som snabbt populeras i början av en laserpuls. För att samtidigt uppnå en lägre begränsningsnivå och lägre linjärabsorption utvärderades ett flertal självaktiverade filter, antingen i form av glas eller i vätskelösning. En f/5-uppställning användes för att utvärdera deras OPLprestanda medan en mängd fotofysiska mätningar utfördes för att få en förståelse för deras systembeteende. De tre första serierna av MTEOS Sol-Gel glas var dopade med guldnanopartiklar antingen enbart, eller med en av två Pt(II)-acetylidmolekyler. Den första hade kortare konjugerade ligandarmar, den andra var liknande men hade längre ligandarmar. Slutligen utvärderades en serie av flerarmade flourenmolekyler i vätskelösning. Deras centrala enhet bestod antingen av en organisk bensenring eller en ISC-gynnare i form av para-dibromobensen eller en Pt(II)-acetylidenhet. Guldnanopartiklarna kunde förstärka OPL-prestandan för enbart den mindre effektiva korta Pt(II)-acetylidmolekylen på 600nm men ej 532nm. Filtren dopade med enbart guldnanopartiklar visade god prestanda på 532nm men ingen på 600nm. Alla tre fluorenmolekyler visade OPL genom det synliga spektrat, även den molekylen utan ISC-gynnare. Både dessa serier experiment demonstrerar hur ett förenklat angreppsätt med att enbart öka eftertraktade fotofysiska parametrar, t.ex. effektivt 2PA-tvärsnitt eller ISC-kvantverkningsgrad, inte alltid resulterar i märkbart ökad systemprestanda. Genom att använda numeriska populationsmodeller visas hur det är möjligt att identifiera vilka parametrar som har den största inverkan på OPL-prestanda.
Organometallic chemistry is based on the reactions and use of a class of compounds (R-M) that contain a covalent bond between carbon and metal. They are prepared either by direct reaction of the metal with an organic compound or by replacement of a metal from another organometallic substance. This book presents research in this field.
Edited and authored by top international experts, this first book on conjugated polymers with a focus on synthesis provides a detailed overview of all modern synthetic methods for these highly interesting compounds. As such, it describes every important compound class, including polysilanes, organoboron compounds, and ferrocene-containing conjugated polymers. An indispensable source for every synthetic polymer chemist.
The cutting edge of scientific reporting . . . PROGRESS in Inorganic Chemistry Nowhere is creative scientific talent busier than in the world of inorganic chemistry experimentation. Progress in Inorganic Chemistry continues in its tradition of being the most respected avenue for exchanging innovative research. This series provides inorganic chemists and materials scientists with a forum for critical, authoritative evaluations of advances in every area of the discipline. With contributions from internationally renowned chemists, this latest volume offers an in-depth, far-ranging examination of the changing face of the field, providing a tantalizing glimpse of the emerging state of the science. "This series is distinguished not only by its scope and breadth, but also by the depth and quality of the reviews." —Journal of the American Chemical Society "[This series] has won a deservedly honored place on the bookshelf of the chemist attempting to keep afloat in the torrent of original papers on inorganic chemistry." —Chemistry in Britain CONTENTS OF VOLUME 54: Atomlike Building Units of Adjustable Character: Solid-State and Solution Routes to Manipulating Hexanuclear Transition Metal Chalcohalide Clusters (Eric J. Welch and Jeffrey R. Long) Doped Semiconductor Nanocrystals: Synthesis, Characterization, Physical Properties, and Applications (J. Daniel Bryan and Daniel R. Gamelin) Stereochemical Aspects of Metal Xanthane Complexes: Molecular Structures and Supramolecular Self-Assembly (Edward R. T. Tiekink and Ionel Haiduc) Trivalent Uranium: A Versatile Species for Molecular Activation (Ilia Korobkov and Sandro Gambarotta) Comparison of the Chemical Biology of NO and HNO: An Inorganic Perspective (Katrina M. Miranda and David A. Wink) Alterations of Nucleobase pKa Values upon Metal Coordination: Origins and Consequences (Bernhard Lippert) Functionalization of Myoglobin (Yoshihito Watanabe and Takashi Hayashi)
S. Di Bella, C. Dragonetti, M. Pizzotti, D. Roberto, F. Tessore, R. Ugo: Coordination and Organometallic Complexes as Second-Order Nonlinear Optical Molecular Materials.- M. G. Humphrey, M.P. Cifuentes, M. Samoc: NLO Molecules and Materials Based on Organometallics: Cubic NLO Properties.- L. Murphy, J. A. G. Williams: Luminescent Platinum Compounds: From Molecules to OLEDs. - Z. Liu, Z. Bian, C. Huang: Luminescent Iridium Complexes and Their Applications.- N. C. Fletcher, M. C. Lagunas: Chromo- and Fluorogenic Organometallic Sensors.- V. Guerchais, H. Le Bozec: Metal Complexes Featuring Photochromic Ligands.
The handbook comprehensively covers the field of inorganic photochemistry from the fundamentals to the main applications. The first section of the book describes the historical development of inorganic photochemistry, along with the fundamentals related to this multidisciplinary scientific field. The main experimental techniques employed in state-of-art studies are described in detail in the second section followed by a third section including theoretical investigations in the field. In the next three sections, the photophysical and photochemical properties of coordination compounds, supramolecular systems and inorganic semiconductors are summarized by experts on these materials. Finally, the application of photoactive inorganic compounds in key sectors of our society is highlighted. The sections cover applications in bioimaging and sensing, drug delivery and cancer therapy, solar energy conversion to electricity and fuels, organic synthesis, environmental remediation and optoelectronics among others. The chapters provide a concise overview of the main achievements in the recent years and highlight the challenges for future research. This handbook offers a unique compilation for practitioners of inorganic photochemistry in both industry and academia.
This work brings together a selection of papers dealing with various aspects of organic nonlinear optical materials.