Meteorology and haze structure during AGASP-II,Part 1: Alaskan Arctic flights, 2–10 April 1986

The second Arctic Gas and Aerosol Sampling Program (AGASP-II) was conducted across the Alaskan and Canadian Arctic in April 1986, to study the in situ aerosol, and the chemical and optical properties of Arctic haze. The NOAA WP-3D aircraft, with special instrumentation added, made six flights during AGASP-II. Measurements of wind, pressure, temperature, ozone, water vapor, condensation nuclei (CN) concentration, and aerosol scattering extinction (b_sp) were used to determine the location of significant haze layers. The measurements made on the first three flights, over the Arctic Ocean north of Barrow and over the Beaufort Sea north of Barter Island, Alaska are discussed in detail in this report of the first phase of AGASP II. In the Alaskan Arctic the WP-3D detected a large and persistent region of haze between 960 and 750 mb, in a thermally stable layer, on 2, 8, and 9 April 1986. At its most dense, the haze contained CN concentrations >10,000 cm^–3 and b_sp of 80×10^–6 m^–1 suggesting active SO₂ to H₂SO₄ gas-to-particle conversion. Calculations based upon observed SO₂ concentrations and ambient relative humidities suggest that 10⁴–10⁵ small H₂SO₄ droplets could have been produced in the haze layers. High concentrations of sub-micron H₂SO₄ droplets were collected in haze. Ozone concentrations were 5–10 ppb higher in the haze layers than in the surrounding troposphere. Outside the regions of haze, CN concentrations ranged from 100 to 400 cm^–3 and b_sp values were about (20–40)×10^–6 m^–1. Air mass trajectories were computed to depict the air flow upwind of regions in which haze was observed. In two cases the back trajectories and ground measurements suggested the source to be in central Europe.     

NOAA WP-3D instrumentation and flight operations on AGASP-II

The second Arctic Gas and Aerosol Sampling Program (AGASP-II) was conducted across the non-Soviet Arctic in March and April 1986, to study the aerosol, gaseous, chemical, and optical properties of Arctic haze. One component of the program was supported with an instrumented NOAA WP-3D atmospheric research aircraft. Measurements of wind, temperature, ozone, water vapor, condensation nucleus concentration, and aerosol scattering extinction coefficient were used to determine the locations and properties of haze layers. The first three NOAA WP-3D research flights were conducted north of Barrow, Alaska, and over the Beaufort Sea northeast of Barter Island, Alaska. The next three sampled conditions in the high Arctic near Alert, Northwest Territories, Canada. All basic meteorological, gas, and aerosol systems are described. The WP-3D flight tracks and operations are presented.     

Correlations among combustion effluent species at Barrow,Alaska: Aerosol black carbon,carbon dioxide,and methane

As part of the second Arctic Gas and Aerosol Sampling Program (AGASP II) continuous measurements of atmospheric aerosol black carbon (BC) were made at the NOAA/GMCC observatory at Barrow, Alaska (71°19N, 156°36W) during the period March 21–April 22, 1986. Black carbon is produced only by incomplete combustion of carbonaceous materials and so is a particularly useful atmospheric indicator of anthropogenic activities. The BC data have been analyzed together with the concurrent measurements of carbon dioxide (CO₂), methane (CH₄), and condensation nuclei (CN) that are routinely made at the observatory. All four species showed elevated and highly variable concentrations due to local human activities, principally in the township of Barrow, 7 km to the southwest, and at the DEW Line radar installation 1 km to the northwest. We distinguish between those periods of the record that are affected by local activities and those that are not, on the basis of the short-term (periods of up to 1 hour) variability of the continuous CO₂ and CN records, with large short-term variabilities indicating local sources. We identified seven periods of time (events) with durations ranging from 13 to 37 hours when the BC, CO₂, and CH₄ concentrations changed smoothly over time, were highly correlated with each other, and were not influenced by local activities. These events had BC/CO₂ ratios in the range (50–103)×10^–6. These ratios are dimensionless since we convert the CO₂ concentrations to units of ng m^–3 of carbon. Such values of BC/CO₂ are characteristic of the combustion effluent from large installations burning heavy fuel oil or coal, automobiles, and domestic-scale natural gas usage. We conclude that these events are indicative of air masses that have been polluted with combustion emissions in a distant location and then transported to the Arctic. In the absence of species-selective loss mechanisms, these air masses will maintain their combustion effluent signatures during the transport. The BC/CO₂ ratios found for the local combustion activities are consistent with those expected from known combustion processes.     

Meteorology and haze structure during AGASP-II,Part 2: Canadian Arctic flights, 13–16 April 1986

In April 1986, a well-instrumented NOAA WP-3D research aircraft conducted three flights in the Canadian Arctic tied to the Canadian Atmospheric Environment Service baseline station in Alert, Northwest Territories. Two of the flights were coordinated with the National Aeronautical Establishment of Canada Twin Otter and the University of Washington C-131 research aircraft. The haze observed in the Canadian Arctic was well-aged and mixed throughout the troposphere in concentrations well below those observed during the previous weeks in the Alaskan Arctic. Over the ice, beneath the surface temperature inversion, ozone was generally depleted to near zero. Over the coast at Alert, there is evidence that topography and downslope winds reduce the strength of the inversion, thus allowing lower tropospheric gases and aerosols to mix down to the surface. At the top of the troposphere, an aerosol-depleted region was observed. In the lower stratosphere, aerosol concentrations were elevated above those observed in the troposphere.     

Pan over the Arctic; Observations during AGASP-2 in April 1986

During three of the flights with the NOAA P3 Orion over the Arctic icecap in April 1986, the atmospheric concentration of PAN (peroxyacetyl nitrate) was measured. Due to major experimental problems, the uncertainty in the data is large (+/–50%), but, nevertheless, some important trends can be resolved. More than 600 (+/–300) ppt(v) of PAN was present in a moderately dense arctic haze layer, confirming conclusions reached from surface observations at Alert, N.W.T., Canada, that PAN is a major odd nitrogen species in Arctic polluted air masses. In relatively clean air off Barrow, Alaska, PAN levels were well below 100 (+/–50) ppt(v), increasing with altitude, in agreement with theoretical predictions concerning the occurrence of PAN in clean air. PAN mixing ratios in the upper troposphere or lower stratosphere were variable (from ca. 30 (+/–15) ppt(v) on April 13 up to 140 (+/–70) ppt(v) on April 8), suggesting involvement in the tropospheric-stratospheric exchange of odd nitrogen. To place the PAN data in a broader context, measurements of other NO_y compounds as well as integrated SO_x data are also reported.     

Relative radiative forcing consequences of global emissions of hydrocarbons, carbon monoxide and NOx from human activities estimated with a zonally-averaged two-dimensional model

A global two-dimensional (altitude-latitude) chemistry transport model is used to follow the changes in the tropospheric distribution of the two major radiatively active trace gases, methane and ozone, following step changes to the sustained emissions of the short-lived trace gases methane, carbon monoxide and non-methane hydrocarbons. The radiative impacts were dependent on the latitude chosen for the applied change in emissions. Step change global warming potentials (GWPs) were derived for a range of short-lived trace gases to describe their time-integrated radiative forcing impacts for unit emissions relative to that of carbon dioxide. The GWPs show that the tropospheric chemistry of the hydrocarbons can produce significant indirect radiative impacts through changing the tropospheric distributions of hydroxyl radicals, methane and ozone. For aircraft, the indirect radiative forcing impact of the NO _x emissions appears to be greater than that from their carbon dioxide emissions. Quantitative results from this two-dimensional model study must, however, be viewed against the known inadequacies of zonally-averaged models and their poor representation of many important tropospheric processes.     

Concentrations of atmospheric constituents observed at Alert,Canada, in relation to air trajectories and synoptic systems

A meteorological analysis is presented for environmental data set obtained from the Canadian Arctic haze study, which is part of AGASP-II. Results of the study indicated that atmospheric carbon dioxide (CO₂), methane (CH₄), sulphate (SO₄ ⁼), ozone (O₃) and other air pollutants observed at Alert, N.W.T. underwent periodical fluctuations. It was found that high concentrations of these atmospheric constituents were associated with a deep (1430–2074 m) inversion and with a major anticyclone. In contrast, relatively low values of these constituents were associated with a cyclonic disturbance near Alert. High concentrations of these constituents occurred with air trajectories coming from the N-W direction, while low values occurred with S trajectories. In addition, examinations of satellite imagery with other meteorological data suggested that volcanic inputs of ash and gases from Augustine Island, Alaska were negligible for the observed high values of these constituents at the ground level at Alert.     

Studies of ice nucleation by Arctic aerosol on AGASP-II

Aerosol particles were collected on filters for studies of their ability to nucleate ice during the second Arctic Gas and Aerosol Sampling Program (AGASP-II) in April, 1986. The ice nuclei (IN) samples were collected from an aircraft at altitudes ranging from the surface to the vicinity of the tropopause in Arctic locations over Alaska, northern Canada and Greenland. Samples of other components of the aerosol were collected and measurements were made of other properties of the aerosol coincident in time with the IN samples. The IN filters were exposed to water saturation in a dynamic developing chamber at –15° C and –25° C. Ice crystals grew on the IN and were counted on the filters at discrete time intervals during the exposure period to determine the rate of ice nucleation and the final concentration of (IN). Results show that Arctic haze aerosol, identified by pollutant signatures, had lower IN concentrations, a lower IN to total aerosol fraction and slower ice nucleation rates than aerosol which had a chemical signature more indicative of the remote unpolluted troposphere. These observations suggest that the Arctic haze aerosol does not efficiently form ice in the arctic troposphere. This may be a factor contributing to the long-range transport of Arctic haze.     

Arctic hazes in summer over Greenland and the North American Arctic. I: Incidence and origins

Airborne observations during August 1985 over Greenland and the North American Arctic revealed that dense, discrete haze layers were common above 850 mb. No such hazes were found near the surface in areas remote from local sources of particles. The haze layers aloft were characterized by large light-scattering coefficients due to dry particles (maximum value 1.24 × 10^–4m^–1) and relatively high total particle concentrations (maximum value 3100 cm^–3). Sulfate was the dominant ionic component of the aerosol (0.06 – 1.9 g m^–3); carbon soot was also present. Evidence for relatively fresh aerosols, accompanied by NO₂ and O₃ depletion, was found near, but not within, the haze layers. The hazes probably derived from anthropogenic sources and/or biomass burning at midlatitudes.It is hypothesized that the scavenging of particles by stratus clouds plays an important role in reducing the frequency and intensity of hazes at the surface in the Arctic in summer. Since the detection of haze layers aloft through measurements of column-integrated parameters from the surface (e.g., by lidar) cannot be carried out reliably when clouds are present, such measurements have likely underestimated the occurrence of haze layers in the Arctic, particularly in summer.     

Greenhouse Gas Emissions from Hydroelectric Reservoirs in Tropical Regions

This paper discusses emissions by power-dams in the tropics. Greenhouse gas emissions from tropical power-dams are produced underwater through biomass decomposition by bacteria. The gases produced in these dams are mainly nitrogen, carbon dioxide and methane. A methodology was established for measuring greenhouse gases emitted by various power-dams in Brazil. Experimental measurements of gas emissions by dams were made to determine accurately their emissions of methane (CH₄) and carbon dioxide (CO₂) gases through bubbles formed on the lake bottom by decomposing organic matter, as well as rising up the lake gradient by molecular diffusion.The main source of gas in power-dams reservoirs is the bacterial decomposition (aerobic and anaerobic) of autochthonous and allochthonous organic matter that basically produces CO₂ and CH₄. The types and modes of gas production and release in the tropics are reviewed.     

Sulfur dioxide in the North American Arctic

Determinations of atmospheric sulfur dioxide were made across the North American Aretic using gas chromatography with a detection limit of 25 parts per trillion by volume and a precision of 25% or better. The vertical distribution of sulfur dioxide in the Arctic atmosphere in April, 1986 was highly variable, with concentrations ranging from the detection limit to 15 parts-per-billion by volume (ppbv). While SO₂ exceeded 10 ppbv in an exceptional haze layer in the Alaskan Arctic, sulfur dioxide was sometimes in the 1 – 5 ppbv range when the haze was absent. This was particularly true for the Canadian Arctic in the vicinity of Alert. In the lower stratosphere over Ellesmere Island, sulfur dioxide was 0.85 ppbv.     

In-situ measurements of the aerosol size distributions,physicochemistry and light absorption properties of Arctic haze

Thermal and optical techniques were used at Barrow, Alaska during AGASP II (3/20/86–4/7/86) to measure in-situ variability of major aerosol components present in Arctic Haze. The experiment provided continuous data on the concentration, size distribution and relative proportions of sulfate species and refractory aerosol for particle diameters of 0.15 to 5 m. Filter samples were also taken for determination of aerosol optical absorption due to soot (EC-elemental carbon). Although pronounced haze events were absence during this period the haze aerosol present varied in concentration between 2 and 6 g/m³ but showed little change in relative constituents. Apart from local influences, the optical data indicated a persistent fine-mode sulfate aerosol with a NH₄ ⁺/SO₄ ^– molar ratio of about 0.4 and a refractory component of somewhat less than 10% by mass. A preliminary comparison of soot estimates determined from the light absorption data with the size distributions of refractory aerosol observed independently by the optical particle counter showed good agreement during the sample period. In the absence of local pollution, values of single scatter albedo derived from light scattering and light absorption showed similar variation about the average value of 0.86 found by us during flights north of Barrow three years earlier during AGASP I.     

The effects of the Arctic haze as determined from airborne radiometric measurements during AGASP II

The interaction of the Aretic winter aerosol (Arctic haze) with solar radiation produces changes in the radiation field that result in the enhancement of scattering and absorption processes which alter the energy balance and solar energy distribution in the Arctic atmosphere-surface system. During the second Arctic Gas and Aerosols Sampling Project (AGASP II) field experiment, we measured radiation parameters using the NOAA WP-3D research aircraft as a platform. State-of-the-art instrumentation was used to measure in situ the absorption of solar radiation by the Arctic atmosphere during severe haze events. Simultaneously with the absorption measurements, we determined optical depths, and total, direct, and scattered radiation fields. All optical measurements were made at spectral bands centered at 412, 500, 675, and 778 nm and with a bandpass of 10 nm. With this selection of spectral regions we concentrated on the measurement of the radiative effects of the aerosol excluding most of the contributions by the gaseous components of the atmosphere. An additional measurement performed during these experiments was the determination of total solar spectrum fluxes. The experimentally determined parameters were used to define an aerosol model that was employed to deduce the absorption by the aerosols over the full solar spectrum and to calculate atmospheric heating rate profiles. The analyses summarized above allowed us to deduce the magnitude of the change in some important parameters. For example, we found changes in instantaneous heating rate of up to about 0.6 K/day. Besides the increased absorption (30 to 40%) and scattering of radiation by the atmosphere, the haze reduces the surface absorption of solar energy by 6 to 10% and the effective planetary albedo over ice surfaces by 3 to 6%. The vertical distribution of the absorbing aerosol is inferred from the flux measurements. Values for the specific absorption of carbon are found to be around 6 m²/g for externally mixed aerosol and about 11.7 m²/g for internally mixed aerosol. A complete study of the radiative effects of the Arctic haze should include infrared measurements and calculations as well as physics of the ice, snow, and water surfaces.     

Arctic haze: Perturbation to the radiation field

Summary A model of the polluted arctic troposphere is constructed to estimate the magnitude and seasonal variation of the climate forcing function of arctic haze. Using a pill-box bathtub model for the Arctic and envisioning it to be filled with pollution from industrial sources in Eurasia, we estimate that maximum climate perturbation from arctic contamination occurs in the spring months. The major perturbation to the radiation budget is a lowering of the albedo (heating) of the earth-atmosphere system around the vernal equinox and is due to a trace amount (about 5% by mass) of black carbon associated with the removal-resistant submicron mode of aerosols. The black carbon over the reflecting polar ice/snow introduces a heating of about 1.5 degree per day into the haze layer.With 8 Figures     

Emissions, Concentrations, & Temperature: A Time Series Analysis

We use recent advances in time series econometrics to estimate the relation among emissions of CO₂ and CH₄, the concentration of these gases, and global surface temperature. These models are estimated and specified to answer two questions; (1) does human activity affect global surface temperature and; (2) does global surface temperature affect the atmospheric concentration of carbon dioxide and/or methane. Regression results provide direct evidence for a statistically meaningful relation between radiative forcing and global surface temperature. A simple model based on these results indicates that greenhouse gases and anthropogenic sulfur emissions are largely responsible for the change in temperature over the last 130 years. The regression results also indicate that increases in surface temperature since 1870 have changed the flow of carbon dioxide to and from the atmosphere in a way that increases its atmospheric concentration. Finally, the regression results for methane hint that higher temperatures may increase its atmospheric concentration, but this effect is not estimated precisely.     

Transient Behaviour of Tropospheric Ozone Precursors in a Global 3-D CTM and Their Indirect Greenhouse Effects

The global three-dimensional Lagrangian chemistry-transport model STOCHEM has been used to follow the changes in the tropospheric distributions of the two major radiatively-active trace gases, methane and tropospheric ozone, following the emission of pulses of the short-lived tropospheric ozone precursor species, methane, carbon monoxide, NO_x and hydrogen. The radiative impacts of NO_x emissionswere dependent on the location chosen for the emission pulse, whether at the surface or in the upper troposphere or whether in the northern or southern hemispheres. Global warming potentials were derived for each of the short-lived tropospheric ozone precursor species by integrating the methane and tropospheric ozone responses over a 100 year time horizon. Indirect radiative forcing due to methane and tropospheric ozone changes appear to be significant for all of the tropospheric ozone precursor species studied. Whereas the radiative forcing from methane changes is likely to be dominated by methane emissions, that from tropospheric ozone changes is controlled by all the tropospheric ozone precursor gases, particularly NO_xemissions. The indirect radiative forcing impacts of tropospheric ozone changes may be large enough such that ozone precursors should be considered in the basket of trace gases through which policy-makers aim to combat global climate change.     

Emissions from Russian domestic civil aviation in 2000–2012 and integrated assessment of their impact on the climate system

Emissions from Russian domestic civil aviation for the period of 2000–2012 are assessed for the following gases: carbon dioxide, methane, nitrous oxide, carbon monoxide, nitrogen oxides, and sulfur dioxide. The integrated assessment of their impact on the climate system is performed using the values of the global warming potential. The CO₂ equivalent was used as a common measure of emissions. It is established that the modern impact of Russian civil aviation on the Earth climate is insignificant.     

Remote and in situ measurements of aerosol concentration in the Arctic troposphere from the Yak-42D “Roshydromet” research aircraft

The results are presented of measurements of aerosol content at different heights in the Arctic troposphere in the area of Naryan-Mar city and the Yamal Peninsula on June 24, 2014 using in situ and remote instruments installed on the Yak-42D "Roshydromet" research aircraft. The maximum aerosol content was detected in the layer up to 3000 m, and the aerosol concentration in the troposphere over the Yamal Peninsula is higher than that in the area of Naryan-Mar by 100 times. The in situ aircraft instrument measured the number concentration of black carbon particles in the tropospheric aerosol. To identify the sources of aerosol in the Arctic troposphere during airborne measurements the air mass trajectory analysis was performed. Simulations were conducted using the TRACAO trajectory model and FLEXPART particle dispersion model. The possible contribution of long-range and local transport of industrial pollutants to the Arctic troposphere was analyzed. The air mass transport was simulated using the trajectory model. Model computations of aerosol concentration in the troposphere using the satellite data on the gas flaring incite that the high content of black carbon in the lower troposphere over the Yamal Peninsula was caused by its transfer from the oil-producing areas located on the adjoining territory of Russia. The contribution of long-range transport of pollutants from industrial enterprises in Western Europe to the Arctic area under study was insignificant in the period under consideration.     

Analytical electron microscope studies of size-segregated particles collected during AGASP-II,flights 201–203

Cascade impactor samples were collected over the Alaskan Arctic during the first three research flights of AGASP-II. These samples were analyzed using analytical electron microscopy to determine the morphology, mineralogy and elemental composition of individual particles. For analytical considerations, a typical impactor sample was run for approximately 20 min, thus giving excellent time resolution of discrete events.Samples collected during flights 201 and 202 consisted of stratospheric aerosol and lower-altitude haze samples. Stratospheric samples were characterized by moderate loadings of H₂SO₄ droplets with relatively few particles of other types. Samples collected in tropospheric haze layers generally exhibited light-to-moderate particle loadings. H₂SO₄ was again the most prevalent species, with crustal and anthropogenic particles also observed. One sample taken over south-central Alaska near the end of flight 203 showed high concentrations of solid crustal particles, with relatively little associated H₂SO₄. Giant particles larger than 5 m were occasionally observed in this aerosol. The composition of this material closely matches that of bulk ash from the Mt. Augustine volcano, which erupted 9–13 days before collection of this sample. This brings forth the possibility that pockets of ash-rich aerosol existed over parts of south and central Alska during the AGASP-II field mission. There is no evidence that these volcanic aerosols were present in the AGASP study area north of the Brooks Range.     

Elemental composition of particulate material sampled from the Arctic haze aerosol

Thirty-six aerosol filter samples collected in tropospheric Arctic haze layers, in the stratosphere, and in the marine boundary layer during the 1983 Arctic Gas and Aerosol Sampling Program were analyzed for trace elements using instrumental neutron activation analysis. Average crustal dust concentrations were 540 ng/m³ and 330 ng/m³ for samples collected in Arctic haze over the North American and Norwegian Arctic, respectively. An average marine salt concentration of 120 ng/m³ was obtained for haze samples collected above the marine boundary layer on both sides of the Arctic.Meteorological and wind trajectory information were used to identify specific haze transport pathways, which brought relatively unmixed aerosol from the central Soviet Union into the AGASP sampling areas. Results from individual filters collected within these transport zones are discussed, with emphasis on certain trace metal ratos which have been proposed by other researchers as discriminators of aerosols from different source regions. Our aircraft-collected data are compared with previously-collected ground-based measurements, and show reasonably good agreement for most tracer elements and ratios. Specifically, we have determined the As/Sb ratio tracer, named by other researchers as the most effective elemental discriminator of aerosol from the central Soviet Union, to be approximately 5–6. This relatively high tracer value is consistent with previous ground-based findings. A significantly lower V/Sb ratio was observed throughout this study, possibly indicating a change in the source signature.