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The objectives of this research are threefold: (1) to develop methods for the study electron transfer processes at the single molecule level, (2) to develop a series of modifiable and structurally well defined molecular and nanoparticle systems suitable for detailed single molecule/particle and bulk spectroscopic investigation, (3) to relate experiment to theory in order to elucidate the dependence of electron transfer processes on molecular and electronic structure, coupling and reorganization energies. We have begun the systematic development of single molecule spectroscopy (SMS) of electron transfer and summaries of recent studies are shown. There is a tremendous need for experiments designed to probe the discrete electronic and molecular dynamic fluctuations of single molecules near electrodes and at nanoparticle surfaces. Single molecule spectroscopy (SMS) has emerged as a powerful method to measure properties of individual molecules which would normally be obscured in ensemble-averaged measurement. Fluctuations in the fluorescence time trajectories contain detailed molecular level statistical and dynamical information of the system. The full distribution of a molecular property is revealed in the stochastic fluctuations, giving information about the range of possible behaviors that lead to the ensemble average. In the case of electron transfer, this level of understanding is particularly important to the field of molecular and nanoscale electronics: from a device-design standpoint, understanding and controlling this picture of the overall range of possible behaviors will likely prove to be as important as designing ia the ideal behavior of any given molecule.
The goal of the current proposal is to obtain partial support for an upcoming symposium planned for the Fall 2011 American Chemical Society national meeting. The symposium is designed to honor the deceased senior physical chemist and Department of Energy Principle Investigator, Professor Paul Barbara. The primary use of support from DOE's Basic Energy Sciences division would be to fund registration for postdoctoral and junior scientists, as well as registration and travel support for principle investigators from Primarily Undergraduate Institutions (PUIs). Professor Barbara was particularly adept at mentoring postdoctoral scholars in their transition to independent researchers. DOE support would help to promote the participation of these early career scientists in this symposium. Professor Barbara undertook many projects of considerable importance to the Nation's energy program; it is hoped that the symposium, beyond honoring him, will also provide an opportunity to discuss the best ways to move forward the unfinished science he initiated with his collaborators.
In this thesis, several problems regarding dynamics and spectra in condensed phases are theoretically analyzed via analytical models. The thesis consists of four main topics. First, a theoretical description of single molecule spectroscopy is presented in order to study time-dependent fluctuations of single molecule spectra in a dynamic environment. In particular, the photon counting statistics is investigated for a single molecule undergoing a generic type of spectral diffusion process. An exact analytical solution is found for this case, and various physical limits are analyzed. Second, motivated by recent experimental observations of anomalous spectral fluctuations in quantum dot systems, both the lineshape phenomenon and the photon counting statistics are explored when spectral fluctuations are characterized by power-law statistics, for which there is no finite timescale. Unique features of the power-law statistics are demonstrated in spectral properties of those systems. Third, a spectral analysis method is developed for the non-adiabatic electron transfer reactions, which allows a unified treatment of diverse kinetic regimes in the electron transfer process. The method is applied to electron transfer reactions in mixed-valence systems in order to explore the possibility of electronic coherence. Finally, effects of the nonequilibrium bath relaxation on the excitation energy transfer process are investigated by generalizing the Forster-Dexter theory of excitation energy transfer to the case of the nonstationary bath relaxation.
The topics range from single molecule experiments in quantum optics and solid-state physics to analogous investigations in physical chemistry and biophysics.
With this collection of short review papers we would like to present a broad overview of research on poly?uorenes and related heteroanalogues over the last two decades. The collection begins with papers on the synthesis of po- ?uorenesandrelatedpolyheteroarenes, thenreportsphotophysicalproperties of this class of conjugated polymers both at the ensemble and the single chain level, continues with a discussion of the rich solid state structures of poly?uorenes, and ?nally switches to device applications (e.g. in OLEDs). In addition, two chapters are devoted to de?ned oligo?uorenesas lowmolecular weight model systems forpoly?uorenes and also to degradation studies. We feel that this up-to-date collection will be very helpful to all polymer chemists and physicists, and will also aid graduate students interested in this fascinating and still growing area of research, since such a compact overview is only now available. All articles are presented by leading scientists in their ?elds, insuring state-of-the-art coverage of all relevant aspects. Together with the body of references this volume is meant to assist researchers in the daily lab routine. Moreover, Advances in Polymer Science, as an established series of high quality review papers, represents a very appropriate platform for our project.Wehopethatthisshortcollectionwillbeofgreatvaluebothforbeg- ners and established researchscientists inthe?eldofpoly?uorene research.
Closing a gap in the literature, this handbook gathers all the information on single particle tracking and single molecule energy transfer. It covers all aspects of this hot and modern topic, from detecting virus entry to membrane diffusion, and from protein folding using spFRET to coupled dye systems, as well recent achievements in the field. Throughout, the first-class editors and top international authors present content of the highest quality, making this a must-have for physical chemists, spectroscopists, molecular physicists and biochemists.
The availability of the photosynthetic reaction center's structure at an atomic resolution of less than three angstroms has revolutionized research. This protein is the first integral membrane protein whose structure has been determined with such precision. Each volume of the Photosynthetic Reaction Center contains original research, methods, and reviews. Together, these volumes cover our current understanding of how photosynthesis converts light energy into stored chemical energy.Volume I describes the chemistry and biochemistry of photosynthesis, including green plant photosynthesis; it is devoted to the overall features and implications of the bacterial reaction center for green plant research. It features a new description of the structure of the reaction center, followed by coverage of the antenna and light functions. Volume I also details new manipulations of the reaction center including chemical and genetic modifications. It describes how the reaction center provides reducing power via electron transfer chemistry coupled to proton uptake and release; coupling of electron transport between the oxidized reaction center and the aqueous periplasm; and the general operation of membrane-bound proteins. Additionally, this volume contains five chapters detailing facets of green plant photosynthesis important for future research.