Electron Transfer in Hydrogenated Nanocrystalline Silicon Observed by Time-Resolved Terahertz Spectroscopy
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Observations show an increasing amplitude in the seasonal cycle of CO2 (ASC) north of 45°N of 56 ± 9.8% over the last 50 years and an increase in vegetation greenness of 7.5–15% in high northern latitudes since the 1980s. However, the causes of these changes remain uncertain. Historical simulations from terrestrial biosphere models in the Multiscale Synthesis and Terrestrial Model Intercomparison Project are compared to the ASC and greenness observations, using the TM3 atmospheric transport model to translate surface fluxes into CO2 concentrations. We find that the modeled change in ASC is too small but the mean greening trend is generally captured. Modeled increases in greenness are primarily driven by warming, whereas ASC changes are primarily driven by increasing CO2. We suggest that increases in ecosystem-scale light use efficiency (LUE) have contributed to the observed ASC increase but are underestimated by current models. We highlight potential mechanisms that could increase modeled LUE.
We use the spectrally invariant method to study the variability of cloud optical thickness τ and droplet effective radius reff in transition zones (between the cloudy and clear sky columns) observed from Solar Spectral Flux Radiometer (SSFR) and Shortwave Array Spectroradiometer-Zenith (SASZe) during the Marine ARM GPCI Investigation of Clouds (MAGIC) field campaign. The measurements from the SSFR and the SASZe are different, however inter-instrument differences of self-normalized measurements (divided by their own spectra at a fixed time) are small. The spectrally invariant method approximates the spectra in the cloud transition zone as a linear combination of definitely clear and cloudy spectra, where the coefficients, slope and intercept, character-ize the spectrally invariant properties of the transition zone. Simulation results from the SBDART (Santa Barbara DISORT Atmospheric Radiative Transfer) model demonstrate that (1) the slope of the visible band is positively correlated with the cloud optical thickness τ while the intercept of the near-infrared band has high negative cor-relation with the cloud drop effective radius reff even without the exact knowledge of τ; (2) the above relations hold for all Solar Zenith Angle (SZA) and for cloud-contaminated skies. In observations using redundant measure-ments from SSFR and SASZe, we find that during cloudy-to-clear transitions, (a) the slopes of the visible band de-crease, and (b) the intercepts of the near-infrared band remain almost constant near cloud edges. The findings in simulations and observations suggest that, while the optical thickness decreases during the cloudy-to-clear transition, the cloud drop effective radius does not change when cloud edges are approached. These results sup-port the hypothesis that inhomogeneous mixing dominates near cloud edges in the studied cases.
The prevalent approach to developing new nanomaterials is a trial and error process of iteratively altering synthesis procedures and then characterizing the resulting nanostructures. This is fundamentally limited in that the growth processes that occur during synthesis can only be inferred from the final synthetic structure. Directly observing real-time nanomaterial growth provides unprecedented insight into the relationship between synthesis conditions and product evolution, and facilitates a mechanistic approach to nanomaterial development. Here we use in situ liquid stage scanning transmission electron microscopy to observe the growth of mesoporous palladium in a solvated block copolymer (BCP) template under various synthesis conditions, and ultimately determine a refined synthesis procedure that yields ordered pores. We find that at low organic solvent (tetrahydrofuran, THF) content, the BCP assembles into a rigid, cylindrical micelle array with a high degree of short-range order, but poor long-range order. Upon slowing the THF evaporation rate using a solvent-vapor anneal step, the long-range order is greatly improved. The electron beam induces nucleation of small particles in the aqueous phase around the micelles. The small particles then flocculate and grow into denser structures that surround the micelles, forming an ordered mesoporous structure. The microscope observations revealed that template disorder can be addressed prior to reaction, and is not invariably induced by the growth process itself, allowing us to more quickly optimize the synthetic method. This work was conducted in the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by DOE’s Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. The Pacific Northwest National Laboratory is operated by Battelle for the U.S. Department of Energy under contract DE-AC05-76RL01830. This research was funded in part by: the Presidential Early Career Award for Scientist and Engineers for I.A., the University of California Academic Senate and the University of California Laboratory fee research grant, the Laboratory-Directed Research and Development program at Sandia National Laboratories, and the Chemical Imaging Initiative at Pacific Northwest National Laboratory. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000.
Liquid Cell Transmission Electron Microscopy (LCTEM) can provide direct observations of solution phase nanoscale materials, and holds great promise as a tool for monitoring dynamic self assembly processes. Control over particle behavior within the liquid cell, and under electron beam irradiation, is of paramount importance for this technique to contribute to our understanding of chemistry and materials science at the nanoscale. However, this type of control has not been demonstrated for complex, organic macromolecular materials, which form the basis for all biological systems, all of polymer science, and encompass important classes of advanced porous materials. Here we show that by controlling the liquid cell surface chemistry and electron beam effects, the dynamics and self-assembly of metal-organic frameworks (MOFs) can be observed. Our results demonstrate that hybrid organic/inorganic beam sensitive materials can be analyzed with LCTEM and at least in the case of Zif-8 dynamics, the results correlate with observations from bulk growth or other standard synthetic conditions. We anticipate that direct, nanoscale imaging by LCTEM of MOF nucleation and growth mechanisms, may provide insight into controlled MOF crystal morphology, domain composition, and processes influencing defect formation.
We present the results of observations of the TeV binary LS I +61{sup 0} 303 with the VERITAS telescope array between 2008 and 2010, at energies above 300 GeV. In the past, both ground-based gamma-ray telescopes VERITAS and MAGIC have reported detections of TeV emission near the apastron phases of the binary orbit. The observations presented here show no strong evidence for TeV emission during these orbital phases; however, during observations taken in late 2010, significant emission was detected from the source close to the phase of superior conjunction (much closer to periastron passage) at a 5.6 standard deviation (5.6{sigma}) post-trials significance. In total, between 2008 October and 2010 December a total exposure of 64.5 hr was accumulated with VERITAS on LS I +61{sup 0} 303, resulting in an excess at the 3.3{sigma} significance level for constant emission over the entire integrated data set. The flux upper limits derived for emission during the previously reliably active TeV phases (i.e., close to apastron) are less than 5% of the Crab Nebula flux in the same energy range. This result stands in apparent contrast to previous observations by both MAGIC and VERITAS which detected the source during these phases at 10% of the Crab Nebula flux. During the two year span of observations, a large amount of X-ray data were also accrued on LS I +61{sup 0} 303 by the Swift X-ray Telescope and the Rossi X-ray Timing Explorer Proportional Counter Array. We find no evidence for a correlation between emission in the X-ray and TeV regimes during 20 directly overlapping observations. We also comment on data obtained contemporaneously by the Fermi Large Area Telescope.
Ambipolar diffusion (AD) is believed to be a crucial process for redistributing magnetic flux in the dense molecular gas that occurs in regions of star formation. We carry out numerical simulations of this process in regions of low ionization using the heavy-ion approximation. The simulations are for regions of strong field (plasma {beta} = 0.1) and mildly supersonic turbulence (M=3, corresponding to an Alfven Mach number of 0.67). The velocity power spectrum of the neutral gas changes from an Iroshnikov-Kraichnan spectrum in the case of ideal MHD to a Burgers spectrum in the case of a shock-dominated hydrodynamic system. The magnetic power spectrum shows a similar behavior. We use a one-dimensional radiative transfer code to post-process our simulation results; the simulated emission from the CS J = 2-1 and H{sup 13}CO{sup +} J = 1-0 lines shows that the effects of AD are observable in principle. Linewidths of ions are observed to be less than those of neutrals, and we confirm previous suggestions that this is due to AD. We show that AD is unlikely to affect the Chandrasekhar-Fermi method for inferring field strengths unless the AD is stronger than generally observed. Finally, we present a study of the enhancement of AD by turbulence, finding that AD is accelerated by factor 2-4.5 for non-self-gravitating systems with the level of turbulence we consider.
We present a new method for confirming transiting planets based on the combination of transit timing variations (TTVs) and dynamical stability. Correlated TTVs provide evidence that the pair of bodies is in the same physical system. Orbital stability provides upper limits for the masses of the transiting companions that are in the planetary regime. This paper describes a non-parametric technique for quantifying the statistical significance of TTVs based on the correlation of two TTV data sets. We apply this method to an analysis of the TTVs of two stars with multiple transiting planet candidates identified by Kepler. We confirm four transiting planets in two multiple-planet systems based on their TTVs and the constraints imposed by dynamical stability. An additional three candidates in these same systems are not confirmed as planets, but are likely to be validated as real planets once further observations and analyses are possible. If all were confirmed, these systems would be near 4:6:9 and 2:4:6:9 period commensurabilities. Our results demonstrate that TTVs provide a powerful tool for confirming transiting planets, including low-mass planets and planets around faint stars for which Doppler follow-up is not practical with existing facilities. Continued Kepler observations will dramatically improve the constraints on the planet masses and orbits and provide sensitivity for detecting additional non-transiting planets. If Kepler observations were extended to eight years, then a similar analysis could likely confirm systems with multiple closely spaced, small transiting planets in or near the habitable zone of solar-type stars.
Transit timing variations provide a powerful tool for confirming and characterizing transiting planets, as well as detecting non-transiting planets. We report the results of an updated transit timing variation (TTV) analysis for 1481 planet candidates based on transit times measured during the first sixteen months of Kepler observations. We present 39 strong TTV candidates based on long-term trends (2.8% of suitable data sets). We present another 136 weaker TTV candidates (9.8% of suitable data sets) based on the excess scatter of TTV measurements about a linear ephemeris. We anticipate that several of these planet candidates could be confirmed and perhaps characterized with more detailed TTV analyses using publicly available Kepler observations. For many others, Kepler has observed a long-term TTV trend, but an extended Kepler mission will be required to characterize the system via TTVs. We find that the occurrence rate of planet candidates that show TTVs is significantly increased ({approx}68%) for planet candidates transiting stars with multiple transiting planet candidates when compared to planet candidates transiting stars with a single transiting planet candidate.
We report on VERITAS very high energy (VHE; E {>=} 100 GeV) observations of six blazars selected from the Fermi Large Area Telescope First Source Catalog (1FGL). The gamma-ray emission from 1FGL sources was extrapolated up to the VHE band, taking gamma-ray absorption by the extragalactic background light into account. This allowed the selection of six bright, hard-spectrum blazars that were good candidate TeV emitters. Spectroscopic redshift measurements were attempted with the Keck Telescope for the targets without Sloan Digital Sky Survey spectroscopic data. No VHE emission is detected during the observations of the six sources described here. Corresponding TeV upper limits are presented, along with contemporaneous Fermi observations and non-concurrent Swift UVOT and X-Ray Telescope data. The blazar broadband spectral energy distributions (SEDs) are assembled and modeled with a single-zone synchrotron self-Compton model. The SED built for each of the six blazars shows a synchrotron peak bordering between the intermediate- and high-spectrum-peak classifications, with four of the six resulting in particle-dominated emission regions.
We present the results of observations of blazar PKS 1510-089 with the Herschel Space Observatory PACS and SPIRE instruments, together with multiwavelength data from Fermi/LAT, Swift, SMARTS, and Submillimeter Array. The source was found in a quiet state, and its far-infrared spectrum is consistent with a power law with a spectral index of {alpha} {approx_equal} 0.7. Our Herschel observations were preceded by two 'orphan' gamma-ray flares. The near-infrared data reveal the high-energy cutoff in the main synchrotron component, which cannot be associated with the main gamma-ray component in a one-zone leptonic model. This is because in such a model the luminosity ratio of the external-Compton (EC) and synchrotron components is tightly related to the frequency ratio of these components, and in this particular case an unrealistically high energy density of the external radiation would be implied. Therefore, we consider a well-constrained two-zone blazar model to interpret the entire data set. In this framework, the observed infrared emission is associated with the synchrotron component produced in the hot-dust region at the supra-parsec scale, while the gamma-ray emission is associated with the EC component produced in the broad-line region at the sub-parsec scale. In addition, the optical/UV emission is associated with the accretion disk thermal emission, with the accretion disk corona likely contributing to the X-ray emission.