We use observations from the April 2008 NASA ARCTAS aircraft campaign to the North American Arctic, interpreted with a global 3-D chemical transport model (GEOS-Chem), to better understand the ...sources and cycling of hydrogen oxide radicals (HOx≡H+OH+peroxy radicals) and their reservoirs (HOy≡HOx+peroxides) in the springtime Arctic atmosphere. We find that a standard gas-phase chemical mechanism overestimates the observed HO2 and H2O2 concentrations. Computation of HOx and HOy gas-phase chemical budgets on the basis of the aircraft observations also indicates a large missing sink for both. We hypothesize that this could reflect HO2 uptake by aerosols, favored by low temperatures and relatively high aerosol loadings, through a mechanism that does not produce H2O2. We implemented such an uptake of HO2 by aerosol in the model using a standard reactive uptake coefficient parameterization with γ(HO2) values ranging from 0.02 at 275 K to 0.5 at 220 K. This successfully reproduces the concentrations and vertical distributions of the different HOx species and HOy reservoirs. HO2 uptake by aerosol is then a major HOx and HOy sink, decreasing mean OH and HO2 concentrations in the Arctic troposphere by 32% and 31% respectively. Better rate and product data for HO2 uptake by aerosol are needed to understand this role of aerosols in limiting the oxidizing power of the Arctic atmosphere.
The INTEX‐A field mission was conducted in the summer of 2004 (1 July to 15 August 2004) over North America (NA) and the Atlantic in cooperation with multiple national and international partners as ...part of a consortium called ICARTT. The main goals of INTEX‐A were to (1) characterize the composition of the troposphere over NA, (2) characterize the outflow of pollution from NA and determine its chemical evolution during transatlantic transport, (3) validate satellite observations of tropospheric composition, (4) quantitatively relate atmospheric concentrations of gases and aerosols with their sources and sinks, and (5) investigate aerosol properties and their radiative effects. INTEX‐A primarily relied on instrumented DC‐8 and J‐31 aircraft platforms to achieve its objectives. The DC‐8 was equipped to measure detailed gas and aerosol composition and provided sufficient range and altitude capability to coordinate activities with distant partners and to sample the entire midlatitude troposphere. The J‐31 was specifically focused on radiative effects of clouds and aerosols and operated largely in the Gulf of Maine. Satellite products along with meteorological and 3‐D chemical transport model forecasts were integrated into the flight planning process. Intercomparisons were performed to quantify the accuracy of data and to create a unified data set. Satellite validation activities principally focused on Terra (MOPITT, MODIS, and MISR), Aqua (AIRS and MODIS) and Envisat (SCIAMACHY) to validate observations of CO, NO2, HCHO, H2O, and aerosol. Persistent fires in Alaska and NW Canada offered opportunities to quantify emissions from fires and study the transport and evolution of biomass burning plumes. Contrary to expectations, several pollution plumes of Asian origin, frequently mixed with stratospheric air, were sampled over NA. Quasi‐Lagrangian sampling was successfully carried out to study chemical aging of plumes during transport over the Atlantic. Lightning NOx source was found to be far larger than anticipated and provided a major source of error in model simulations. The composition of the upper troposphere was significantly perturbed by influences from surface pollution and lightning. Drawdown of CO2 was characterized over NA and its atmospheric abundance related to terrestrial sources and sinks. INTEX‐A observations provide a comprehensive data set to test models and evaluate major pathways of pollution transport over NA and the Atlantic. This overview provides a context within which the present and future INTEX‐A/ICARTT publications can be understood.
Airborne measurements of a large number of oxygenated volatile organic chemicals (OVOC) were carried out in the Pacific troposphere (0.1-12 km) in winter/spring of 2001 (24 February to 10 April). ...Specifically, these measurements included acetone (CH3COCH3), methylethyl ketone (CH3COC2H5, MEK), methanol (CH3OH), ethanol (C2H5OH), acetaldehyde (CH3CHO), propionaldehyde (C2H5CHO), peroxyacylnitrates (PANs) (C(sub n)H(sub 2n+1)COO2NO2), and organic nitrates (C(sub n)H(sub 2n+1)ONO2). Complementary measurements of formaldehyde (HCHO), methyl hydroperoxide (CH3OOH), and selected tracers were also available. OVOC were abundant in the clean troposphere and were greatly enhanced in the outflow regions from Asia. Background mixing ratios were typically highest in the lower troposphere and declined toward the upper troposphere and the lowermost stratosphere. Their total abundance (Summation of OVOC) was nearly twice that of nonmethane hydrocarbons (Summation of C2-C8 NMHC). Throughout the troposphere, the OH reactivity of OVOC is comparable to that of methane and far exceeds that of NMHC. A comparison of these data with western Pacific observations collected some 7 years earlier (February-March 1994) did not reveal significant differences. Mixing ratios of OVOC were strongly correlated with each other as well as with tracers of fossil and biomass/biofuel combustion. Analysis of the relative enhancement of selected OVOC with respect to CH3Cl and CO in 12 plumes originating from fires and sampled in the free troposphere (3-11 km) is used to assess their primary and secondary emissions from biomass combustion. The composition of these plumes also indicates a large shift of reactive nitrogen into the PAN reservoir thereby limiting ozone formation. A three-dimensional global model that uses state of the art chemistry and source information is used to compare measured and simulated mixing ratios of selected OVOC. While there is reasonable agreement in many cases, measured aldehyde concentrations are significantly larger than predicted. At their observed levels, acetaldehyde mixing ratios are shown to be an important source of HCHO (and HO x ) and PAN in the troposphere. On the basis of presently known chemistry, measured mixing ratios of aldehydes and PANs are mutually incompatible. We provide rough estimates of the global sources of several OVOC and conclude that collectively these are extremely large (150-500 Tg C / yr) but remain poorly quantified.
Rapidity-odd directed flow (v1) measurements for charged pions, protons, and antiprotons near midrapidity (y=0) are reported in sNN=7.7, 11.5, 19.6, 27, 39, 62.4, and 200 GeV Au+Au collisions as ...recorded by the STAR detector at the Relativistic Heavy Ion Collider. At intermediate impact parameters, the proton and net-proton slope parameter dv1/dy|y=0 shows a minimum between 11.5 and 19.6 GeV. In addition, the net-proton dv1/dy|y=0 changes sign twice between 7.7 and 39 GeV. The proton and net-proton results qualitatively resemble predictions of a hydrodynamic model with a first-order phase transition from hadronic matter to deconfined matter, and differ from hadronic transport calculations.
We analyze detailed atmospheric gas/aerosol composition data acquired during the 2008 NASA ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) airborne ...campaign performed at high northern latitudes in spring (ARCTAS-A) and summer (ARCTAS-B) and in California in summer (ARCTAS-CARB). Biomass burning influences were widespread throughout the ARCTAS campaign. MODIS data from 2000 to 2009 indicated that 2008 had the second largest fire counts over Siberia and a more normal Canadian boreal forest fire season. Near surface arctic air in spring contained strong anthropogenic signatures indicated by high sulfate. In both spring and summer most of the pollution plumes transported to the Arctic region were from Europe and Asia and were present in the mid to upper troposphere and contained a mix of forest fire and urban influences. The gas/aerosol composition of the high latitude troposphere was strongly perturbed at all altitudes in both spring and summer. The reactive nitrogen budget was balanced with PAN as the dominant component. Mean ozone concentrations in the high latitude troposphere were only minimally perturbed (<5
ppb), although many individual pollution plumes sampled in the mid to upper troposphere, and mixed with urban influences, contained elevated ozone (ΔO
3/ΔCO
=
0.11
±
0.09
v/v). Emission and optical characteristics of boreal and California wild fires were quantified and found to be broadly comparable. Greenhouse gas emission estimates derived from ARCTAS-CARB data for the South Coast Air Basin of California show good agreement with state inventories for CO
2 and N
2O but indicate substantially larger emissions of CH
4. Simulations by multiple models of transport and chemistry were found to be broadly consistent with observations with a tendency towards under prediction at high latitudes.
In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction ...measured by satellites) and mass measurements of aerosol loading (PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type – such as composition, size, and hygroscopicity – and to the surrounding atmosphere, such as temperature, relative humidity (RH), and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project, extensive in situ atmospheric profiling in the Baltimore, MD–Washington, D.C. region was performed during 14 flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties, and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 %) and organics (57 %). A distinct difference in composition was observed, with high-loading days having a proportionally larger percentage of sulfate due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity) such that higher relative contributions of inorganics increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity, causing an increase in the water content of the aerosol. Conversely, low-aerosol-loading days had lower sulfate and higher black carbon contributions, causing lower single-scattering albedos (SSAs). The average black carbon concentrations were 240 ng m−3 in the lowest 1 km, decreasing to 35 ng m−3 in the free troposphere (above 3 km). Routine airborne sampling over six locations was used to evaluate the relative contributions of aerosol loading, composition, and relative humidity (the amount of water available for uptake onto aerosols) to variability in mixed-layer aerosol extinction. Aerosol loading (dry extinction) was found to be the predominant source, accounting for 88 % on average of the measured spatial variability in ambient extinction, with lesser contributions from variability in relative humidity (10 %) and aerosol composition (1.3 %). On average, changes in aerosol loading also caused 82 % of the diurnal variability in ambient aerosol extinction. However on days with relative humidity above 60 %, variability in RH was found to cause up to 62 % of the spatial variability and 95 % of the diurnal variability in ambient extinction. This work shows that extinction is driven to first order by aerosol mass loadings; however, humidity-driven hydration effects play an important secondary role. This motivates combined satellite–modeling assimilation products that are able to capture these components of the aerosol optical depth (AOD)–PM2.5 link. Conversely, aerosol hygroscopicity and SSA play a minor role in driving variations both spatially and throughout the day in aerosol extinction and therefore AOD. However, changes in aerosol hygroscopicity from day to day were large and could cause a bias of up to 27 % if not accounted for. Thus it appears that a single daily measurement of aerosol hygroscopicity can be used for AOD-to-PM2.5 conversions over the study region (on the order of 1400 km2). This is complimentary to the results of Chu et al. (2015), who determined that the aerosol vertical distribution from "a single lidar is feasible to cover the range of 100 km" in the same region.
Intercontinental Chemical Transport Experiment-B (INTEX-B) was a major NASA (Acronyms are provided in Appendix A.) led multi-partner atmospheric field campaign completed in the spring of 2006 ...(http://cloud1.arc.nasa.gov/intex-b/). Its major objectives aimed at (i) investigating the extent and persistence of the outflow of pollution from Mexico; (ii) understanding transport and evolution of Asian pollution and implications for air quality and climate across western North America; and (iii) validating space-borne observations of tropospheric composition. INTEX-B was performed in two phases. In its first phase (1–21 March), INTEX-B operated as part of the MILAGRO campaign with a focus on observations over Mexico and the Gulf of Mexico. In the second phase (17 April–15 May), the main INTEX-B focus was on trans-Pacific Asian pollution transport. Multiple airborne platforms carrying state of the art chemistry and radiation payloads were flown in concert with satellites and ground stations during the two phases of INTEX-B. Validation of Aura satellite instruments (TES, OMI, MLS, HIRDLS) was a key objective within INTEX-B. Satellite products along with meteorological and 3-D chemical transport model forecasts were integrated into the flight planning process to allow targeted sampling of air parcels. Inter-comparisons were performed among and between aircraft payloads to quantify the accuracy of data and to create a unified data set. Pollution plumes were sampled over the Gulf of Mexico and the Pacific several days after downwind transport from source regions. Signatures of Asian pollution were routinely detected by INTEX-B aircraft, providing a valuable data set on gas and aerosol composition to test models and evaluate pathways of pollution transport and their impact on air quality and climate. This overview provides details about campaign implementation and a context within which the present and future INTEX-B/MILAGRO publications can be understood.
We present the discovery of eight new radio pulsars located in the Large Magellanic Cloud (LMC). Five of these pulsars were found from reprocessing the Parkes Multibeam Survey of the Magellanic ...Clouds, while the remaining three were from an ongoing new survey at Parkes with a high-resolution data acquisition system. It is possible that these pulsars were missed in the earlier processing due to radio frequency interference, visual judgment or the large number of candidates that must be analysed. One of these new pulsars has a dispersion measure of 273 pc cm−3, almost twice the highest previously known value, making it possibly the most distant LMC pulsar. In addition, we present the null result of a radio pulse search of an X-ray point source located in SNR J0047.2−7308 in the Small Magellanic Cloud (SMC). Although no millisecond pulsars have been found, these discoveries have increased the known rotation-powered pulsar population in the LMC by more than 50 per cent. Using the current sample of LMC pulsars, we used a Bayesian analysis to constrain the number of potentially observable pulsars in the LMC to within a 95 per cent credible interval of 57 000+70000
−30000. The new survey at Parkes is ∼20 per cent complete, and it is expected to yield at most six millisecond pulsars in the LMC and SMC. Although it is very sensitive to short period pulsars, this new survey provides only a marginal increase in sensitivity to long periods. The limiting luminosity for this survey is 125 mJy kpc2 for the LMC which covers the upper 10 per cent of all known radio pulsars. The luminosity function for normal pulsars in the LMC is consistent with their counterparts in the Galactic disc. The maximum 1400 MHz radio luminosity for LMC pulsars is ∼1000 mJy kpc2.
High levels of fine particulate matter (PM2.5) pollution in East Asia often exceed local air quality standards. Observations from the Korea–United States Air Quality (KORUS-AQ) field campaign in May ...and June 2016 showed that development of extreme pollution (haze) occurred through a combination of long-range transport and favorable meteorological conditions that enhanced local production of PM2.5. Atmospheric models often have difficulty simulating PM2.5 chemical composition during haze, which is of concern for the development of successful control measures. We use observations from KORUS-AQ to examine the ability of the GEOS-Chem chemical transport model to simulate PM2.5 composition throughout the campaign and identify the mechanisms driving the pollution event. At the surface, the model underestimates sulfate by -64 % but overestimates nitrate by +36 %. The largest underestimate in sulfate occurs during the pollution event, for which models typically struggle to generate elevated sulfate concentrations due to missing heterogeneous chemistry in aerosol liquid water in the polluted boundary layer. Hourly surface observations show that the model nitrate bias is driven by an overestimation of the nighttime peak. In the model, nitrate formation is limited by the supply of nitric acid, which is biased by +100 % against aircraft observations. We hypothesize that this is due to a large missing sink, which we implement here as a factor of 5 increase in dry deposition. We show that the resulting increased deposition velocity is consistent with observations of total nitrate as a function of photochemical age. The model does not account for factors such as the urban heat island effect or the heterogeneity of the built-up urban landscape, resulting in insufficient model turbulence and surface area over the study area that likely results in insufficient dry deposition. Other species such as NH3 could be similarly affected but were not measured during the campaign. Nighttime production of nitrate is driven by NO2 hydrolysis in the model, while observations show that unexpectedly elevated nighttime ozone (not present in the model) should result in N2O5 hydrolysis as the primary pathway. The model is unable to represent nighttime ozone due to an overly rapid collapse of the afternoon mixed layer and excessive titration by NO. We attribute this to missing nighttime heating driving deeper nocturnal mixing that would be expected to occur in a city like Seoul. This urban heating is not considered in air quality models run at large enough scales to treat both local chemistry and long-range transport. Key model failures in simulating nitrate, mainly overestimated daytime nitric acid, incorrect representation of nighttime chemistry, and an overly shallow and insufficiently turbulent nighttime mixed layer, exacerbate the model's inability to simulate the buildup of PM2.5 during haze pollution. To address the underestimate in sulfate most evident during the haze event, heterogeneous aerosol uptake of SO2 is added to the model, which previously only considered aqueous production of sulfate from SO2 in cloud water. Implementing a simple parameterization of this chemistry improves the model abundance of sulfate but degrades the SO2 simulation, implying that emissions are underestimated. We find that improving model simulations of sulfate has direct relevance to determining local vs. transboundary contributions to PM2.5. During the haze pollution event, the inclusion of heterogeneous aerosol uptake of SO2 decreases the fraction of PM2.5 attributable to long-range transport from 66 % to 54 %. Locally produced sulfate increased from 1 % to 25 % of locally produced PM2.5, implying that local emissions controls could have a larger effect than previously thought. However, this additional uptake of SO2 is coupled to the model nitrate prediction, which affects the aerosol liquid water abundance and chemistry driving sulfate–nitrate–ammonium partitioning. An additional simulation of the haze pollution with heterogeneous uptake of SO2 to aerosol and simple improvements to the model nitrate simulation results in 30 % less sulfate due to 40 % less nitrate and aerosol water, and this results in an underestimate of sulfate during the haze event. Future studies need to better consider the impact of model physical processes such as dry deposition and nighttime boundary layer mixing on the simulation of nitrate and the effect of improved nitrate simulations on the overall simulation of secondary inorganic aerosol (sulfate + nitrate + ammonium) in East Asia. Foreign emissions are rapidly changing, increasing the need to understand the impact of local emissions on PM2.5 in South Korea to ensure continued air quality improvements.
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