90 research outputs found
Photoelectron diffraction: from phenomenological demonstration to practical tool
The potential of photoelectron diffraction—exploiting the coherent interference of directly-emitted and elastically scattered components of the photoelectron wavefield emitted from a core level of a surface atom to obtain structural information—was first appreciated in the 1970s. The first demonstrations of the effect were published towards the end of that decade, but the method has now entered the mainstream armoury of surface structure determination. This short review has two objectives: First, to outline the way that the idea emerged and the way this evolved in my own collaboration with Neville Smith and his colleagues at Bell Labs in the early years: Second, to provide some insight into the current state-of-the art in application of (scanned-energy mode) photoelectron diffraction to address two key issue in quantitative surface structure determination, namely, complexity and precision. In this regard a particularly powerful aspect of photoelectron diffraction is its elemental and chemical-state specificity
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Time-resolved infrared studies of the dynamics of ligand binding to cytochrome c oxidase
Time-resolved infrared spectroscopy (TRIRS) has been employed to study the reactions of small molecules with the cytochrome a{sub 3}-Cu{sub B} site of cytochrome c oxidase (CcO). All phases of these reactions have been investigated, from ultrafast phenomena (hundreds of femtoseconds) to relatively slow processes (milliseconds). The ligation dynamics immediately following photodissociation have been studied using a TRIR technique with time resolution of less than 1 ps. The rate of photoinitiated transfer of CO from Fe{sub a3}{sup 2+} to Cu{sub B}{sup +} was measured directly by monitoring the development of the transient Cu{sub B}{sup +}-CO absorption. The development of a stationary Cu{sub B}{sup +}-CO spectrum which is constant until the CO dissociates from Cu{sub B}{sup +} occurs in less than 1 ps, indicating that the photoinitiated transfer of CO is remarkably fast. This unprecedented ligand transfer rate has profound implications with regard to the structure and dynamics of the cytochrome a{sub 3}-Cu{sub B} site, the functional architecture of the protein and coordination dynamics in general. The photodissociation and recombination of Cn{sup {minus}} has also been studied using a real-time TRIR technique. The CN{sup {minus}} recombination rate of 430 s{sup {minus}1} is consistent with a recombination pathway similar to the one they have previously proposed for CO. The authors suggest the rate determining step for CN{sup {minus}} recombination is the thermal dissociation of the Fe{sub a3}{sup 2+}-L bond. 25 refs., 7 figs
Examining Contextual Factors and Individual Value Dimensions of Healthcare Providers Intention to Adopt Electronic Health Technologies in Developing Countries
Part 5: Research in ProgressInternational audienceDespite substantial research on electronic health (e-Health) adoption, there still exist vast differences between resource-rich and resource-poor populations regarding Information Technology adoption. To help bridge the technological gulf between developed and developing countries, this research-in-progress paper examines healthcare providers’ intention to adopt e-health technologies from two perspectives 1) contextual factors (i.e. specific to developing world settings) and 2) individual value dimensions (i.e. cultural, utilitarian, social and personal). The primary output of this paper is a theoretical model merging both the contextual factors and value dimensions; this forms a strong baseline to examine and help ensure the successful adoption of e-Health technologies within developing countries. Future research will be performed to validate the model developed in this paper, with a specific focus on mobile Health in Malawi, Africa
History of clinical transplantation
How transplantation came to be a clinical discipline can be pieced together by perusing two volumes of reminiscences collected by Paul I. Terasaki in 1991-1992 from many of the persons who were directly involved. One volume was devoted to the discovery of the major histocompatibility complex (MHC), with particular reference to the human leukocyte antigens (HLAs) that are widely used today for tissue matching.1 The other focused on milestones in the development of clinical transplantation.2 All the contributions described in both volumes can be traced back in one way or other to the demonstration in the mid-1940s by Peter Brian Medawar that the rejection of allografts is an immunological phenomenon.3,4 © 2008 Springer New York
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Photoredox reactions: Energy storage and halocarbon degradation
This is the final report of a three-year, Laboratory Directed Research and Development (LDRD) project at the Los Alamos National Laboratory (LANL). The objectives of this project were the following: (1) To characterize the structures and the structural dynamics of the singlet and triplet states of selected metal-metal bonded systems; (2) To characterize the post-excitation intramolecular electron transfer reactions of these complexes; (3) To investigate strongly adiabatic photo-oxidative addition reactions, including the addition of halocarbons to the electronically excited complexes and their hydrogen-evolving reactions; (4) To seek effective reductant systems that will function in catalytic cycles and regenerate the original, reduced dimer; and (5) To explore the chemistry of metals less expensive than iridium or platinum with regard to their potential for photochemical reactivity. The results include studies of W and Mo clusters with potential multielectron excited state redox reactivity, metal-metal bonded dimers sequestered in liquid crystal environments, d{sup 7} dimers with long-lived photocycles, and photochemically produced oxygen-fluorine systems
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Ultrafast studies of solution dynamics
This is the final report of a one-year, Laboratory Directed Research and Development (LDRD) project at Los Alamos National Laboratory (LANL). Fast chemical dynamics generally must be initiated photochemically. This limits the applicability of modern laser methods for following the structural changes that occur during chemical and biological reactions to those systems that have an electronic chromophore that has a significant yield of photoproduct when excited. This project has developed a new and entirely general approach to ultrafast initiation of reactions in solution: laser-induced temperature jump (T-jump). The results open entire new fields of study of ultrafast molecular dynamics in solution. The authors have demonstrated the T-jump technique on time scales of 50 ps and longer, and have applied it to study of the fast events in protein folding. They find that a general lifetime of alpha-helix formation is ca 100 ns, and that tertiary folds (in apomyoglobin) form in ca 100 {mu}s
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