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Biomolecular Modification of Inorganic Crystal Growth

Description: The fascinating shapes and hierarchical designs of biomineralized structures are an inspiration to materials scientists because of the potential they suggest for biomolecular control over materials synthesis. Conversely, the failure to prevent or limit tissue mineralization in the vascular, skeletal, and urinary systems is a common source of disease. Understanding the mechanisms by which organisms direct or limit crystallization has long been a central challenge to the biomineralization community. One prevailing view is that mineral-associated macromolecules are responsible for either inhibiting crystallization or initiating and stabilizing non-equilibrium crystal polymorphs and morphologies through interactions between anionic moieties and cations in solution or at mineralizing surfaces. In particular, biomolecules that present carboxyl groups to the growing crystal have been implicated as primary modulators of growth. Here we review the results from a combination of in situ atomic force microscopy (AFM) and molecular modeling (MM) studies to investigate the effect of specific interactions between carboxylate-rich biomolecules and atomic steps on crystal surfaces during the growth of carbonates, oxalates and phosphates of calcium. Specifically, we how the growth kinetics and morphology depend on the concentration of additives that include citrate, simple amino acids, synthetic Asp-rich polypeptides, and naturally occurring Asp-rich proteins found in both functional and pathological mineral tissues. The results reveal a consistent picture of shape modification in which stereochemical matching of modifiers to specific atomic steps drives shape modification. Inhibition and other changes in growth kinetics are shown to be due to a range of mechanisms that depend on chemistry and molecular size. Some effects are well described by classic crystal growth theories, but others, such as step acceleration due to peptide charge and hydrophylicity, were previously unrealized. Finally, we show that the molecular scale observations are well correlated with macroscopic growth rate data.
Date: April 27, 2007
Creator: De Yoreo, J. J.

Carbon Capture and Storage

Description: Carbon capture and sequestration (CCS) is the long-term isolation of carbon dioxide from the atmosphere through physical, chemical, biological, or engineered processes. This includes a range of approaches including soil carbon sequestration (e.g., through no-till farming), terrestrial biomass sequestration (e.g., through planting forests), direct ocean injection of CO{sub 2} either onto the deep seafloor or into the intermediate depths, injection into deep geological formations, or even direct conversion of CO{sub 2} to carbonate minerals. Some of these approaches are considered geoengineering (see the appropriate chapter herein). All are considered in the 2005 special report by the Intergovernmental Panel on Climate Change (IPCC 2005). Of the range of options available, geological carbon sequestration (GCS) appears to be the most actionable and economic option for major greenhouse gas reduction in the next 10-30 years. The basis for this interest includes several factors: (1) The potential capacities are large based on initial estimates. Formal estimates for global storage potential vary substantially, but are likely to be between 800 and 3300 Gt of C (3000 and 10,000 Gt of CO{sub 2}), with significant capacity located reasonably near large point sources of the CO{sub 2}. (2) GCS can begin operations with demonstrated technology. Carbon dioxide has been separated from large point sources for nearly 100 years, and has been injected underground for over 30 years (below). (3) Testing of GCS at intermediate scale is feasible. In the US, Canada, and many industrial countries, large CO{sub 2} sources like power plants and refineries lie near prospective storage sites. These plants could be retrofit today and injection begun (while bearing in mind scientific uncertainties and unknowns). Indeed, some have, and three projects described here provide a great deal of information on the operational needs and field implementation of CCS. Part of this interest comes from several key ...
Date: October 3, 2007
Creator: Friedmann, S.

Cases Adjudged in The Supreme Court at October Term, 2004

Description: Volume of the United States Reports containing the final decisions and opinions of the Supreme Court justices regarding cases between October 4, 2004, and March 1, 2005. Also includes notes regarding the members of the Supreme Court, orders, and other relevant materials. Index starts on page 1307.
Date: 2007
Creator: Wagner, Frank D.

Cases Adjudged in The Supreme Court at October Term, 2004

Description: Volume of the United States Reports containing the final decisions and opinions of the Supreme Court justices regarding cases between March 2 and May 31, 2005. Also includes notes regarding the members of the Supreme Court, orders, and other relevant materials. Index starts on page 1307.
Date: 2007
Creator: Wagner, Frank D.

Cavity Microwave Searches for Cosmological Axions

Description: This chapter will cover the search for dark matter axions based on microwave cavity experiments proposed by Pierre Sikivie. We will start with a brief overview of halo dark matter and the axion as a candidate. The principle of resonant conversion of axions in an external magnetic field will be described as well as practical considerations in optimizing the experiment as a signal-to-noise problem. A major focus of this chapter will be the two complementary strategies for ultra-low noise detection of the microwave photons--the 'photon-as-wave' approach (i.e. conventional heterojunction amplifiers and soon to be quantum-limited SQUID devices), and 'photon-as-particle' (i.e. Rydberg-atom single-quantum detection). Experimental results will be presented; these experiments have already reached well into the range of sensitivity to exclude plausible axion models, for limited ranges of mass. The section will conclude with a discussion of future plans and challenges for the microwave cavity experiment.
Date: January 22, 2007
Creator: Carosi, G. & van Bibber, K.

Chapter 3: Evaluating the impacts of carbonaceous aerosols on clouds and climate

Description: Any attempt to reconcile observed surface temperature changes within the last 150 years to changes simulated by climate models that include various atmospheric forcings is sensitive to the changes attributed to aerosols and aerosol-cloud-climate interactions, which are the main contributors that may well balance the positive forcings associated with greenhouse gases, absorbing aerosols, ozone related changes, etc. These aerosol effects on climate, from various modeling studies discussed in Menon (2004), range from +0.8 to -2.4 W m{sup -2}, with an implied value of -1.0 W m{sup -2} (range from -0.5 to -4.5 W m{sup -2}) for the aerosol indirect effects. Quantifying the contribution of aerosols and aerosol-cloud interactions remain complicated for several reasons some of which are related to aerosol distributions and some to the processes used to represent their effects on clouds. Aerosol effects on low lying marine stratocumulus clouds that cover much of the Earth's surface (about 70%) have been the focus of most of prior aerosol-cloud interaction effect simulations. Since cumulus clouds (shallow and deep convective) are short lived and cover about 15 to 20% of the Earth's surface, they are not usually considered as radiatively important. However, the large amount of latent heat released from convective towers, and corresponding changes in precipitation, especially in biomass regions due to convective heating effects (Graf et al. 2004), suggest that these cloud systems and aerosol effects on them, must be examined more closely. The radiative heating effects for mature deep convective systems can account for 10-30% of maximum latent heating effects and thus cannot be ignored (Jensen and Del Genio 2003). The first study that isolated the sensitivity of cumulus clouds to aerosols was from Nober et al. (2003) who found a reduction in precipitation in biomass burning regions and shifts in circulation patterns. Aerosol effects on convection have ...
Date: September 3, 2007
Creator: Menon, Surabi & Del Genio, Anthony D.

Chapter 8: Selective Stoichiometric and Catalytic Reactivity in the Confines of a Chiral Supramolecular Assembly

Description: Nature uses enzymes to activate otherwise unreactive compounds in remarkable ways. For example, DNases are capable of hydrolyzing phosphate diester bonds in DNA within seconds,[1-3]--a reaction with an estimated half-life of 200 million years without an enzyme.[4] The fundamental features of enzyme catalysis have been much discussed over the last sixty years in an effort to explain the dramatic rate increases and high selectivities of enzymes. As early as 1946, Linus Pauling suggested that enzymes must preferentially recognize and stabilize the transition state over the ground state of a substrate.[5] Despite the intense study of enzymatic selectivity and ability to catalyze chemical reactions, the entire nature of enzyme-based catalysis is still poorly understood. For example, Houk and co-workers recently reported a survey of binding affinities in a wide variety of enzyme-ligand, enzyme-transition-state, and synthetic host-guest complexes and found that the average binding affinities were insufficient to generate many of the rate accelerations observed in biological systems.[6] Therefore, transition-state stabilization cannot be the sole contributor to the high reactivity and selectivity of enzymes, but rather, other forces must contribute to the activation of substrate molecules. Inspired by the efficiency and selectivity of Nature, synthetic chemists have admired the ability of enzymes to activate otherwise unreactive molecules in the confines of an active site. Although much less complex than the evolved active sites of enzymes, synthetic host molecules have been developed that can carry out complex reactions with their cavities. While progress has been made toward highly efficient and selective reactivity inside of synthetic hosts, the lofty goal of duplicating enzymes specificity remains.[7-9] Pioneered by Lehn, Cram, Pedersen, and Breslow, supramolecular chemistry has evolved well beyond the crown ethers and cryptands originally studied.[10-12] Despite the increased complexity of synthetic host molecules, most assembly conditions utilize self-assembly to form complex highly-symmetric structures from ...
Date: September 27, 2007
Creator: University of California, Berkeley; Laboratory, Lawrence Berkeley National; Raymond, Kenneth; Pluth, Michael D.; Bergman, Robert G. & Raymond, Kenneth N.

Couplings between changes in the climate system and biogeochemistry

Description: The Earth's climate is determined by a number of complex connected physical, chemical and biological processes occurring in the atmosphere, land and ocean. The radiative properties of the atmosphere, a major controlling factor of the Earth's climate, are strongly affected by the biophysical state of the Earth's surface and by the atmospheric abundance of a variety of trace constituents. These constituents include long-lived greenhouse gases (LLGHGs) such as carbon dioxide (CO{sub 2}), methane (CH{sub 4}) and nitrous oxide (N{sub 2}O), as well as other radiatively active constituents such as ozone and different types of aerosol particles. The composition of the atmosphere is determined by processes such as natural and anthropogenic emissions of gases and aerosols, transport at a variety of scales, chemical and microphysical transformations, wet scavenging and surface uptake by the land and terrestrial ecosystems, and by the ocean and its ecosystems. These processes and, more generally the rates of biogeochemical cycling, are affected by climate change, and involve interactions between and within the different components of the Earth system. These interactions are generally nonlinear and may produce negative or positive feedbacks to the climate system. An important aspect of climate research is to identify potential feedbacks and assess if such feedbacks could produce large and undesired responses to perturbations resulting from human activities. Studies of past climate evolution on different time scales can elucidate mechanisms that could trigger nonlinear responses to external forcing. The purpose of this chapter is to identify the major biogeochemical feedbacks of significance to the climate system, and to assess current knowledge of their magnitudes and trends. Specifically, this chapter will examine the relationships between the physical climate system and the land surface, the carbon cycle, chemically reactive atmospheric gases and aerosol particles. It also presents the current state of knowledge on budgets of ...
Date: October 1, 2007
Creator: Menon, Surabi; Denman, Kenneth L.; Brasseur , Guy; Chidthaisong, Amnat; Ciais, Philippe; Cox, Peter M. et al.

Deformation Behavior of Nanoporous Metals

Description: Nanoporous open-cell foams are a rapidly growing class of high-porosity materials (porosity {ge} 70%). The research in this field is driven by the desire to create functional materials with unique physical, chemical and mechanical properties where the material properties emerge from both morphology and the material itself. An example is the development of nanoporous metallic materials for photonic and plasmonic applications which has recently attracted much interest. The general strategy is to take advantage of various size effects to introduce novel properties. These size effects arise from confinement of the material by pores and ligaments, and can range from electromagnetic resonances to length scale effects in plasticity. In this chapter we will focus on the mechanical properties of low density nanoporous metals and how these properties are affected by length scale effects and bonding characteristics. A thorough understanding of the mechanical behavior will open the door to further improve and fine-tune the mechanical properties of these sometimes very delicate materials, and thus will be crucial for integrating nanoporous metals into products. Cellular solids with pore sizes above 1 micron have been the subject of intense research for many years, and various scaling relations describing the mechanical properties have been developed.[4] In general, it has been found that the most important parameter in controlling their mechanical properties is the relative density, that is, the density of the foam divided by that of solid from which the foam is made. Other factors include the mechanical properties of the solid material and the foam morphology such as ligament shape and connectivity. The characteristic internal length scale of the structure as determined by pores and ligaments, on the other hand, usually has only little effect on the mechanical properties. This changes at the submicron length scale where the surface-to-volume ratio becomes large and the ...
Date: November 28, 2007
Creator: Biener, J.; Hodge, A. M. & Hamza, A. V.

Electron Holography of Electromagnetic Fields - Recent Theoretical Advances.

Description: It has been shown in this work that the Fourier space approach can be fruitfully applied to the calculation of the fields and the associated electron optical phase shift of several magnetic and electrostatic structures, like superconducting vortices in conventional and high-T{sub c} superconductors, reverse biased p-n junctions, magnetic domains and nanoparticles. In all these cases, this novel approach has led to unexpected but extremely interesting results, very often expressed in analytical form, which allow the quantitative and reliable interpretation of the experimental data collected by means of electron holography or of more conventional Lorentz microscopy techniques. Moreover, it is worth recalling that whenever long-range electromagnetic fields are involved, a physical model of the object under investigation is necessary in order to take into account correctly the perturbation of the reference wave induced by the tail of the field protruding into the vacuum. For these reasons, we believe that the Fourier space approach for phase computations we have introduced and discussed in this chapter will represent an invaluable tool for the investigation of electromagnetic fields at the meso- and nano-scale.
Date: January 1, 2007
Creator: Beleggia, M.; Pozzi, G. & Tonomura, A.