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Electron Transfer in Chemistry and Biology An Introduction to the Theory Alexander M. Kuznetsov Russian Academy of Sciences, Moscow, Russia Jens Ulstrup Technical University of Denmark, Lyngby, Denmark Electron transfer is perhaps the single most important physical event in chemical, electrochemical, photochemical, biochemical, and biophysical processes. The focus and ubiquity of electron transfer is intriguing and exciting but a coherent and comprehensive approach to this topic is at the same time a challenge. Electron Transfer in Chemistry and Biology provides a thorough and didactic approach to the theoretical basis of electron transfer phenomena. Not only does it offer a full introduction to this area and a discussion of its historical development, it also gives detailed explanations of difficult issues, for example, long-range electron transfers, stochastic and dynamic processes, and biological features. A wide variety of readers will find this volume of great interest, ranging from final year undergraduate students, postgraduate students and university lecturers, to research staff in numerous fields including medical companies, electronics industry, catalysis research and development, chemical industry and some hospitals.
Electron transfer reactions are vital for life: they are the essential steps in all the major biological energy conservation pathways and the rate of electron transfer sometimes determines the fate of energy flow. While the rates of electron transfer over 1-2 nanometers in proteins can largely be described by well-known theories, it is not well understood how these processes scale to microscopic distances, for example, micrometer length microbial nanowires. Electron transfer reactions are known to be highly sensitive to the chemical properties of the electron carriers and distances between carriers, yet, this information is not available for naturally occurring microbial nanowires. On the other hand, microbial nanowires have inspired the development of novel biological conductive materials and bioelectronics, although these biomimicking materials would significantly benefit from a higher degree of structural definition, which would greatly improve rational redesign.This dissertation work presents two distinct approaches for arranging electron carriers (heme) into structurally defined arrays that can facilitate electron transfer:1) A crystalline lattice of small tetraheme cytochromes that form a well-defined, three-dimensional network of closely spaced redox centers was used to demonstrate the multi-step electron hopping over a micrometer scale.2) A heme attachment strategy was developed that allows one to introduce redox active cofactor hemes into non-heme-binding proteins, while maintaining the proteins' original function. Adding hemes to a nanotube-forming self-assembling protein was used to demonstrate the potential of this strategy to form a structurally defined heme array.The first crystal approach provides detailed information about structure and electronic states which can be used as a platform for testing theories, while the second heme-attaching approach is an engineering platform that allows researchers to introduce redox properties into other well-studied proteins with minimal effort. These two approaches, from two perspectives, lay the foundation of building structurally defined architectures for the understanding of microbial nanowires and the application of biological long-range electron transfer materials.
From May 3-7,1997, the NATO Advanced Research Workshop on 'Biological Electron Transfer Chains' was organized in Tomar, Portugal. In the application for support the choice of the topic was justified as follows: "[Until recently efforts] have concentrated on the study of the structure and function of individual redox enzymes and proteins. Enough information is now available to make a start with the study of biological electron transfer (E1) at the next higher level of organization, that of the complete ET chain." The interest in the workshop was high: the majority of participants had registered before the workshop was formally announced, which illustrates the popularity of the topic within the biochemical and biophysical communities. The present volume contains a number of reports based on the lectures presented by the key speakers during the meeting. The workshop dealt with the following three themes: a) Electron transfer, which is the subject of Chapter 1. The analysis of ET at the molecular level is still fundamental for an understanding of how ET chains operate in vivo. After 40 years of research the contours of the subject are becoming clear now. b) Bacterial redox chains. This is the subject of Chapter 2. Its contents show how complicated these chains can be, often involving a number of gene clusters. Our understanding of the regulatory aspects and control mechanisms of these chains is only in its beginning.
an integrated approach to electron transfer phenomena This two-part stand-alone volume in the prestigious Advances in Chemical Physics series provides the most comprehensive overview of electron transfer science today. It draws on cutting-edge research from diverse areas of chemistry, physics, and biology-covering the most recent developments in the field, and pointing to important future trends. This initial volume includes: * A historical perspective spanning five decades * A review of concepts, problems, and ideas in current research * Electron transfer in isolated molecules and in clusters * General theory, including useful algorithms * Spectra and electron transfer kinetics in bridged compounds The second volume covers solvent control, ultrafast electron transfer and coherence effects, molecular electronics, electron transfer and chemistry, and biomolecules. Electron transfer science has seen tremendous progress in recent years. Technological innovations, most notably the advent of femtosecond lasers, now permit the real-time investigation of intramolecular and intermolecular electron transfer processes on a time scale of nuclear motion. New scientific information abounds, illuminating the processes of energy acquisition, storage, and disposal in large molecules, clusters, condensed phase, and biophysical systems. Electron Transfer: From Isolated Molecules to Biomolecules is the first book devoted to the exciting work being done in nonradiative electron transfer dynamics today. This two-part edited volume emphasizes the interdisciplinary nature of the field, bringing together the contributions of pioneers in chemistry, physics, and biology. Both theoretical and experimental topics are featured. The authors describe modern approaches to the exploration of different systems, including supersonic beam techniques, femtosecond laser spectroscopy, chemical syntheses, and methods in genetic and chemical engineering. They examine applications in such areas as supersonic jets, solvents, electrodes, semi- conductors, respiratory and enzymatic protein systems, photosynthesis, and more. They also relate electron transfer and radiationless transitions theory to pertinent physical phenomena, and provide a conceptual framework for the different processes. Complete with over two hundred illustrations, Part One reviews developments in the field since its inception fifty years ago, and discusses electron transfer phenomena in both isolated molecules and in clusters. It outlines the general theory, exploring areas of the control of kinetics, structure-function relationships, fluctuations, coherence, and coupling to solvents with complex spectral density in different types of electron transfer processes. Timely, comprehensive, and authoritative, Electron Transfer: From Isolated Molecules to Biomolecules is an essential resource for physical chemists, molecular physicists, and researchers working in nonradiative dynamics today.
Various aspects of electron and proton transfer in chemistry and biology are described in this volume. The joint presentation was chosen for two reasons. Rapid electron and proton transfer govern cellular energetics in both the most primitive and higher organisms with photosynthetic and heterotrophic lifestyles. Further, biology has become the area where the various disciplines of science, which were previously diversified, are once again converging. The book begins with a survey of physicochemical principles of electron transfer in the gas and solid phase, with thermodynamic and photochemical driving force. Inner and outer sphere mechanisms and the coupling of electron transfer to nuclear rearrangements are reviewed. These principles are applied to construct artificial photosynthesis, leading to biological electron transfer involving proteins with transition metal and/or organic redox centres. The tuning of the free energy profile on the reaction trajectory through the protein by single amino acids or by the larger ensemble that determines the electrostatic properties of the reaction path is one major issue.Another one is the transformation of one-electron to paired-electron steps with protection against hazardous radical intermediates. The diversity of electron transport systems is represented in various chapters with emphasis on photosynthesis, respiration and nitrogenases. The book will be of interest to scientists in chemistry, physics and the life sciences.
Developed from a symposium sponsored by the International Chemical Congress of Pacific Basin Societies, Honolulu, Hawaii, December 17-22, 1989.