In situ measurements of tropospheric volcanic plumes in Ecuador and Colombia during TC^4

A NASA DC-8 research aircraft penetrated tropospheric gas and aerosol plumes sourced from active volcanoes in Ecuador and Colombia during the Tropical Composition, Cloud and Climate Coupling (TC^4) mission in July–August 2007. The likely source volcanoes were Tungurahua (Ecuador) and Nevado del Huila (Colombia). The TC^4 data provide rare insight into the chemistry of volcanic plumes in the tropical troposphere and permit a comparison of SO_2 column amounts measured by the Ozone Monitoring Instrument (OMI) on the Aura satellite with in situ SO_2 measurements. Elevated concentrations of SO_2, sulfate aerosol, and particles were measured by DC-8 instrumentation in volcanic outflow at altitudes of 3–6 km. Estimated plume ages range from ~2 h at Huila to ~22–48 h downwind of Ecuador. The plumes contained sulfate-rich accumulation mode particles that were variably neutralized and often highly acidic. A significant fraction of supermicron volcanic ash was evident in one plume. In-plume O_3 concentrations were ~70%–80% of ambient levels downwind of Ecuador, but data are insufficient to ascribe this to O_3 depletion via reactive halogen chemistry. The TC^4 data record rapid cloud processing of the Huila volcanic plume involving aqueous-phase oxidation of SO_2 by H_2O_2, but overall the data suggest average in-plume SO_2 to sulfate conversion rates of ~1%–2% h^(−1). SO_2 column amounts measured in the Tungurahua plume (~0.1–0.2 Dobson units) are commensurate with average SO_2 columns retrieved from OMI measurements in the volcanic outflow region in July 2007. The TC^4 data set provides further evidence of the impact of volcanic emissions on tropospheric acidity and oxidizing capacity

Boreal forest fire emissions in fresh Canadian smoke plumes: C_1-C_(10) volatile organic compounds (VOCs), CO_2, CO, NO_2, NO, HCN and CH_3CN

Boreal regions comprise about 17% of the global land area, and they both affect and are influenced by climate change. To better understand boreal forest fire emissions and plume evolution, 947 whole air samples were collected aboard the NASA DC-8 research aircraft in summer 2008 as part of the ARCTAS-B field mission, and analyzed for 79 non-methane volatile organic compounds (NMVOCs) using gas chromatography. Together with simultaneous measurements of CO_2, CO, CH_4, CH_2O, NO_2, NO, HCN and CH_3CN, these measurements represent the most comprehensive assessment of trace gas emissions from boreal forest fires to date. Based on 105 air samples collected in fresh Canadian smoke plumes, 57 of the 80 measured NMVOCs (including CH_2O) were emitted from the fires, including 45 species that were quantified from boreal forest fires for the first time. After CO_2, CO and CH_4, the largest emission factors (EFs) for individual species were formaldehyde (2.1 ± 0.2 g kg^(−1)), followed by methanol, NO_2, HCN, ethene, α-pinene, β-pinene, ethane, benzene, propene, acetone and CH_3CN. Globally, we estimate that boreal forest fires release 2.4 ± 0.6 Tg C yr^(−1) in the form of NMVOCs, with approximately 41% of the carbon released as C_1-C_2 NMVOCs and 21% as pinenes. These are the first reported field measurements of monoterpene emissions from boreal forest fires, and we speculate that the pinenes, which are relatively heavy molecules, were detected in the fire plumes as the result of distillation of stored terpenes as the vegetation is heated. Their inclusion in smoke chemistry models is expected to improve model predictions of secondary organic aerosol (SOA) formation. The fire-averaged EF of dichloromethane or CH_2Cl_2, (6.9 ± 8.6) × 10^(−4)gkg^(−1), was not significantly different from zero and supports recent findings that its global biomass burning source appears to have been overestimated. Similarly, we found no evidence for emissions of chloroform (CHCl_3) or methyl chloroform (CH_3CCl_3) from boreal forest fires. The speciated hydrocarbon measurements presented here show the importance of carbon released by short-chain NMVOCs, the strong contribution of pinene emissions from boreal forest fires, and the wide range of compound classes in the most abundantly emitted NMVOCs, all of which can be used to improve biomass burning inventories in local/global models and reduce uncertainties in model estimates of trace gas emissions and their impact on the atmosphere

Improved quantification of Chinese carbon fluxes using CO2/CO correlations in Asian outflow

[1] We use observed CO2:CO correlations in Asian outflow from the TRACE-P aircraft campaign (February–April 2001), together with a three-dimensional global chemical transport model (GEOS-CHEM), to constrain specific components of the east Asian CO2 budget including, in particular, Chinese emissions. The CO2/CO emission ratio varies with the source of CO2 (different combustion types versus the terrestrial biosphere) and provides a characteristic signature of source regions and source type. Observed CO2/CO correlation slopes in east Asian boundary layer outflow display distinct regional signatures ranging from 10–20 mol/mol (outflow from northeast China) to 80 mol/mol (over Japan). Model simulations using best a priori estimates of regional CO2 and CO sources from Streets et al. [2003] (anthropogenic), the CASA model (biospheric), and Duncan et al. [2003] (biomass burning) overestimate CO2 concentrations and CO2/CO slopes in the boundary layer outflow. Constraints from the CO2/CO slopes indicate that this must arise from an overestimate of the modeled regional net biospheric CO2 flux. Our corrected best estimate of the net biospheric source of CO2 from China for March–April 2001 is 3200 Gg C/d, which represents a 45 % reduction of the net flux from the CASA model. Previous analyses of the TRACE-P data had found that anthropogenic Chinese C

Carbonyl sulfide (OCS): Large-scale distributions over North America during INTEX-NA and relationship to CO2

An extensive set of carbonyl sulfide (OCS) observations were made as part of the NASA Intercontinental Chemical Transport Experiment-North America (INTEX-NA) study, flown from 1 July to 14 August 2004 mostly over the eastern United States and Canada. These data show that summertime OCS mixing ratios at low altitude were dominated by surface drawdown and were highly correlated with CO2. Although local plumes were observed on some low-altitude flight legs, anthropogenic OCS sources were small compared to this sink. These INTEX-NA observations were in marked contrast to the early springtime 2001 Transport and Chemical Evolution over the Pacific experiment, which sampled Asian outflow dominated by anthropogenic OCS emissions. To test the gridded OCS fluxes used in past models, the INTEX-NA observations were combined with the sulfur transport Eulerian model (STEM) regional atmospheric chemistry model for a top-down assessment of bottom-up OCS surface fluxes for North America. Initial STEM results suggest that the modeled fluxes underestimate the OCS plant sink by more than 200%. Copyright 2008 by the American Geophysical Union

Genomics helps to decipher the resistance mechanisms present in a Pseudomonas chlororaphis strain recovered in an HIV patient

Fil: Montaña, Sabrina Daiana. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Houssay. Instituto de Investigaciones en Microbiología y Parasitología Médica. Universidad de Buenos Aires. Facultad de Medicina. Instituto de Investigaciones en Microbiología y Parasitología Médica; ArgentinaFil: Lazzaro, T.. California State University; Estados UnidosFil: Uong, S.. California State University; Estados UnidosFil: Place, K.. California State University; Estados UnidosFil: Iriarte, A.. Universidad de la República; UruguayFil: Ocampo, C. V.. Sanatorio Mater Dei; ArgentinaFil: Vay, C.. Sanatorio Mater Dei; Argentina. Universidad de Buenos Aires. Facultad de Medicina. Hospital de Clínicas General San Martín; ArgentinaFil: Ramírez, M. S.. California State University; Estados Unido

Size-resolved aerosol emission factors and new particle formation/growth activity occurring in Mexico City during the MILAGRO 2006 Campaign

Measurements of the aerosol size distribution from 11 nm to 2.5 microns were made in Mexico City in March 2006, during the MILAGRO (Megacity Initiative: Local and Global Research Observations) field campaign. Observations at the urban supersite, referred to as T0, could often be characterized by morning conditions with high particle mass concentrations, low mixing heights, and highly correlated particle number and CO<sub>2</sub> concentrations, indicative that particle number is controlled by primary emissions. Average size-resolved and total number- and volume-based emission factors for combustion sources impacting T0 have been determined using a comparison of peak sizes in particle number and CO<sub>2</sub> concentration. Peaks are determined by subtracting the measured concentration from a calculated baseline concentration time series. The number emission and volume emission factors for particles from 11 nm to 494 nm are 1.56 × 10<sup>15</sup> particles, and 9.48 × 10<sup>11</sup> cubic microns per kg of carbon, respectively. The uncertainty of the number emission factor is approximately plus or minus 50 %. The mode of the number emission factor was between 25 and 32 nm, while the mode of the volume factor was between 0.25 and 0.32 microns. These emission factors are reported as log normal model parameters and are compared with multiple emission factors from the literature. In Mexico City in the afternoon, the CO<sub>2</sub> concentration drops during ventilation of the polluted layer, and the coupling between CO<sub>2</sub> and particle number breaks down, especially during new particle formation events when particle number is no longer controlled by primary emissions. Using measurements of particle number and CO<sub>2</sub> taken aboard the NASA DC-8, the determined primary emission factor was applied to the Mexico City Metropolitan Area (MCMA) plume to quantify the degree of secondary particle formation in the plume; the primary emission factor accounts for less than 50 % of the total particle number and the surplus particle count is not correlated with photochemical age. Primary particle volume and number in the size range 0.1–2 μm are similarly too low to explain the observed volume distribution. Contrary to the case for number, the apparent secondary volume increases with photochemical age. The size distribution of the apparent increase, with a mode at ~250 nm, is reported

Comparison of chemical characteristics of 495 biomass burning plumes intercepted by the NASA DC-8 aircraft during the ARCTAS/CARB-2008 field campaign

This paper compares measurements of gaseous and particulate emissions from a wide range of biomass-burning plumes intercepted by the NASA DC-8 research aircraft during the three phases of the ARCTAS-2008 experiment: ARCTAS-A, based out of Fairbanks, Alaska, USA (3 April to 19 April 2008); ARCTAS-B based out of Cold Lake, Alberta, Canada (29 June to 13 July 2008); and ARCTAS-CARB, based out of Palmdale, California, USA (18 June to 24 June 2008). Approximately 500 smoke plumes from biomass burning emissions that varied in age from minutes to days were segregated by fire source region and urban emission influences. The normalized excess mixing ratios (NEMR) of gaseous (carbon dioxide, acetonitrile, hydrogen cyanide, toluene, benzene, methane, oxides of nitrogen and ozone) and fine aerosol particulate components (nitrate, sulfate, ammonium, chloride, organic aerosols and water soluble organic carbon) of these plumes were compared. A detailed statistical analysis of the different plume categories for different gaseous and aerosol species is presented in this paper. The comparison of NEMR values showed that CH4 concentrations were higher in air-masses that were influenced by urban emissions. Fresh biomass burning plumes mixed with urban emissions showed a higher degree of oxidative processing in comparison with fresh biomass burning only plumes. This was evident in higher concentrations of inorganic aerosol components such as sulfate, nitrate and ammonium, but not reflected in the organic components. Lower NOx NEMRs combined with high sulfate, nitrate and ammonium NEMRs in aerosols of plumes subject to long-range transport, when comparing all plume categories, provided evidence of advanced processing of these plumes

Bayesian optimization of laser-plasma accelerators assisted by reduced physical models

Particle-in-cell simulations are among the most essential tools for the modeling and optimization of laser-plasma accelerators, since they reproduce the physics from first principles. However, the high computational cost associated with them can severely limit the scope of parameter and design optimization studies. Here, we show that a multitask Bayesian optimization algorithm can be used to mitigate the need for such high-fidelity simulations by incorporating information from inexpensive evaluations of reduced physical models. In a proof-of-principle study, where a high-fidelity optimization with FBPIC is assisted by reduced-model simulations with Wake-T, the algorithm demonstrates an order-of-magnitude speedup. This opens a path for the cost-effective optimization of laser-plasma accelerators in large parameter spaces, an important step towards fulfilling the high beam quality requirements of future applications