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  • Articles  (12)
  • Arctic
  • Electronic structure and strongly correlated systems
  • Chemistry and Pharmacology  (12)
  • 1
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 23 (1996), S. 301-332 
    ISSN: 1573-0662
    Keywords: tropospheric ozone ; Arctic ; hydrocarbons ; halogens
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Several years of measurements of ozone, hydrocarbons, sulphate and meteorological parameters from Spitsbergen in the Norwegian Arctic are presented. Most of the measurements were taken on the Zeppelin Mountain at an altitude of 474 m a.s.l. The focus is the episodes of ozone depletion in the lower troposphere in spring, which are studied in a climatological way. Episodes of very low ozone concentrations are a common feature on the Zeppelin Mountain in spring. The low ozone episodes were observed from late March to the beginning of June. When the effect of transport direction was subtracted, the frequenty of the low ozone episodes was found to peak in the beginning of May, possibly reflecting the seasonal cycle in the actual depletion process. Analyses based on trajectory calculations show that most of the episodes occurred when the air masses were transported from W-N. Ozone soundings show that the ozone depletion may extend from the surface and up to 3–4 km altitude. The episodes were associated with a cold boundary layer beneath a thermally stable layer, suppressing mixing with the free troposphere. The concentration of several individual hydrocarbons was much lower during episodes of low ozone than for the average conditions. The change in concentration ratio between the hydrocarbons was in qualitative agreement with oxidation of hydrocarbons by Br and Cl atoms rather than by OH radicals.
    Type of Medium: Electronic Resource
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  • 2
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 9 (1989), S. 81-99 
    ISSN: 1573-0662
    Keywords: Arctic ; atmosphere ; methane ; carbon dioxide ; haze ; correlation ; AGASP
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Fifty flask air samples were taken during April 1986 from a NOAA WP-3D Orion aircraft which flew missions across a broad region of the Arctic as part of the second Arctic Gas and Aerosol Sampling Program (AGASP II). The samples were subsequently analyzed for both carbon dioxide (CO2) and methane (CH4). The samples were taken in well-defined layers of Arctic haze, in the background troposphere where no haze was detected, and from near the surface to the lower stratosphere. Vertical profiles were specifically measured in the vicinity of Barrow, Alaska to enable comparisons with routine surface measurements made at the NOAA/GMCC observatory. Elevated levels of both methane and carbon dioxide were found in haze layers. For samples taken in the background troposphere we found negative vertical gradients (lower concentrations aloft) for both gases. For the entire data set (including samples collected in the haze layers) we found a strong positive correlation between the methane and carbon dioxide concentrations, with a linear regression slope of 17.5 ppb CH4/ppm CO2, a standard error of 0.6, and a correlation coefficient (r2) of 0.95. This correlation between the two gases seen in the aircraft samples was corroborated by in situ surface measurements of these gases made at the Barrow observatory during March and April 1986. We also find a similar relationship between methane and carbon dioxide measured concurrenty for a short period in the moderately polluted urban atmosphere of Boulder, Colorado. We suggest that the strong correlation between methane and carbon dioxide concentrations reflects a common source region for both, with subsequent long-range transport of the polluted air to the Arctic.
    Type of Medium: Electronic Resource
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  • 3
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 9 (1989), S. 213-224 
    ISSN: 1573-0662
    Keywords: Aerosols ; Barrow ; Arctic ; extinction coefficient ; condensation nuclei ; nephelometer ; aethalometer
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Measurements at Barrow during the second Arctic Gas and Aerosol Sampling Program (AGASP-II), conducted in April 1986, showed no rapid long-range transport from lower-latitude source regions to Barrow, and only limited vertical transport from above the boundary layer to the surface. New aerosol size distribution measurements in the 0.005–0.1 μm diameter size range using a Nuclepore-filter diffusion battery apparatus showed a median diameter of about 0.01 μm during times of high condensation nucleus (CN) concentrations. Aerosol black carbon concentrations exceeding 400 ng m−3 were detected at the surface and were more strongly correlated with CN concentrations than with aerosol scattering extinction (σsp), suggesting that aerosol carbon was generally associated with small particles rather than large particles. Measurements at Barrow during AGASP-I, conducted in March–April 1983, showed a series of aerosol events detected at the ground that were caused by rapid long-range transport paths to the vicinity of Barrow from Eurasia. These events were strongly correlated with aerosol loading in the vertical column (optical depth).
    Type of Medium: Electronic Resource
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  • 4
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 9 (1989), S. 225-244 
    ISSN: 1573-0662
    Keywords: Arctic ; Arotic haze ; Absorption of radiation ; Acrosol ; Opcical depth ; Total-diffuse radiation ; Heating rate ; Solar ; Infrared ; Radiation
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract 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.
    Type of Medium: Electronic Resource
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  • 5
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 11 (1990), S. 211-226 
    ISSN: 1573-0662
    Keywords: Lower troposphere ; aerosols ; Arctic ; air pollution ; principal component analysis
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Six years of observations (1980 to 1986) of the composition of lower tropospheric aerosols at Alert on northern Ellesmere Island in the Canadian high Arctic yield insight into the seasonal variation of Arctic air pollutants as well as of substances of natural origin. A principal component analysis of 138 observations of 21 aerosol constituents (major ions, metals, nonmetallic trace elements) for the most polluted period of December to April identified not only a soil, sea salt and anthropogenic aerosol component, but also one associated with photochemical reactions in the atmosphere that occur at polar sunrise. Depending on the source of their gaseous precursors, elements in the photochemical component can be natural or anthropogenic in origin. For instance, SO4 2-, existing mostly as H2SO4, originates probably from both anthropogenic and natural sources while Br− is likely of marine origin. In contrast, SO4 2- in the anthropogenic component has the stoichiometry of NH4HSO4. In the winter months, over 90% of Arctic SO4 2- is in the anthropogenic and photochemical components. In winter, a substantial portion (11 to 35%) of Na+ is associated with the anthropogenic aerosol component suggesting either that marine aerosols have been physically or chemically modified by interactions with air pollution or that there are anthropogenic sources of Na+. The aerosol soil component is controlled by both local and distant dust sources. During a year, it has two peaks at Alert, one in April/May coinciding with the Asian dust storm season and one in September. There is a marked difference in the seasonal variation of particulate Br− and iodine concentrations in the air. Both have a peak in April/May associated with polar sunrise and, hence, photochemical reactions in the atmosphere. However, iodine also peaks in early fall. This may be a product of biogenic iodine emissions to the atmosphere during secondary blooms in northern oceans in late summer.
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  • 6
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 4 (1986), S. 157-171 
    ISSN: 1573-0662
    Keywords: Arctic ; Aerosol ; Aitken Particle ; Arctic Haze ; Polar Chemistry
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Results from measurements of the composition and size distribution of aerosol particles advected into central Alaska are reported. It is argued that the aerosol predominant in number, but not necessarily in mass, consists of submicron droplets of sulfuric acid. The major aerosol by mass in arctic air is a removal-resistant accumulation mode (radius ∼0.3 μm) probably to large extent originating from pollution sources ∼103 km upstream (mostly in central Eurasia) from the site in Alaska. The accumulation mode aerosol disappears when arctic air masses are replaced with relatively warmer air masses flowing in from the northern Pacific. The latter air mass systems have been strongly scavenged by clouds and precipitation associated with the Aleutian low pressure system and with forced orographic uplifting over the Alaska Mountain Range; nevertheless the Pacific air masses contain substantial (i.e., 500–1000 cm-3) quantities of small (several hundredths of a micron in radius) particles. Arctic-derived air masses are enriched in large (i.e, ∼0.3 μ) particles compared to Pacific Marine air masses, whereas the opposite trend is found for smaller, Aitken, particles. The smaller particles are found in greatest abundance in warmer air mass systems, presumably because of the relatively brief time since such air masses were last exposed to sunlight with attendant production of small particles from the gas phase.
    Type of Medium: Electronic Resource
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  • 7
    ISSN: 1573-0662
    Keywords: Carbon monoxide ; methane ; latitudinal distribution ; spectroscopic measurements ; Arctic ; Antarctic
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract The results of spectroscopic total column measurements of CO and CH4 at different points of the Northern and Southern Hemispheres in 1970–1985, are reported. Seasonal cycles of CO are evident for all the sites. The Northern Hemispheric long-term positive trend of CO seems to be 1.5–2% per year. In the Southern Hemisphere, temporal increasing was not detected and a possible upper limit for it is about 0.6% per year. Methane concentration in the Northern Hemisphere increases at a rate of 1.2% per year.
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  • 8
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 34 (1999), S. 9-20 
    ISSN: 1573-0662
    Keywords: Arctic ; analytical method ; boundary layer ; bromine oxide ; chemical amplification ; chlorine oxide ; field measurement ; halogens ; ozone depletion
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Chemical amplification, CA, a method commonly used for the detection of peroxy radicals, HO2 and RO2, was found to be sensitive towards ClOx (Cl+ClO+OClO) as well. ClOx is reduced by NO to Cl atoms which react with carbon monoxide in the presence of O2. The reaction sequence thus initiated oxidizes CO to CO2 and NO to NO2, with a chain length of 300 ± 60. This allows the atmospheric ClOx content to be measured under ambient conditions with a detection limit of better than 1 ppt. In parallel peroxy radicals are indicated with a chain length of 160 ± 15. Chemical amplification is not specific and does not indicate which radical chain it is seeing. Identification relies solely on plausibility. During the ARCtic Tropospheric Ozone Chemistry (ARCTOC) campaign in spring 1995 and 1996 the CA technique was used at Ny-Ålesund. ClOx at mixing ratios of up to 2 ppt were found in the boundary layer under certain conditions. The low concentrations of ClOx indicate that the arctic boundary ozone depletion is mainly driven by bromine.
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  • 9
    ISSN: 1573-0662
    Keywords: Br2 ; HOBr ; BrOx ; Arctic ; ozone depletion ; troposphere
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract As part of the Polar Sunrise Experiment (PSE) 1997, concentrations of halogen species thought to be involved in ground level Arctic ozone depletion were made at Alert, NWT, Canada (82.5°N, 62.3°W) during the months of March and April, 1997. Measurements were made of photolyzable chlorine (Cl2 and HOCl) and bromine (Br2 and HOBr) using the Photoactive Halogen Detector (PHD), and bromine radicals (BrOx) using a modified radical amplifier. During the sampling period between Julian Day 86 (March 27) and Day 102 (April 12), two ozone depletion episodes occurred, the most notable being on days 96-99, when ozone levels were below detectable limits (≈1 ppbv). Concentrations of BrOx above the 4 pptv detection limit were found for a significant part of the study, both during and outside of depletion events. The highest BrOx concentrations were observed at the end of the depletion event, when the concentration reached 15 pptv. We found substantial amounts of Br2 in the absence of O3, indicating that O3 is not a necessary requirement for production of Br2. There is also Br2 present when winds are from the south, implying local scale (e.g. from the snowpack) production. During the principal O3 depletion event, the HOBr concentration rose to ≈260 pptv, coincident with the BrOx maximum. This implies a steady state HO2 concentration of 6 pptv. During a partial O3 depletion event, we estimate that the flux of Br2 from the surface is about 10 times greater than that for Cl2.
    Type of Medium: Electronic Resource
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  • 10
    ISSN: 1573-0662
    Keywords: hydrocarbon measurements ; interstitial air ; snow pack ; Arctic ; active bromine
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Samples of interstitial air from within the snow pack on an ice floe on the Arctic Ocean were collected during the April 1994 Polar Sunrise Experiment. The concentrations of C2-C7 hydrocarbons are reported for the first time in the snow pack interstitial air. Alkane concentrations tended to be higher than concentrations in free air samples above the snow but very similar to winter measurements at various locations in the Arctic archipelago. However, ethyne concentrations in both interstitial and free air were highly correlated with ozone mixing ratios, consistent with previous demonstrations of the effects of Br atom chemistry. The analysis of total bromine within the snow pack indicate an enrichment in total Br at the interface layer between snow and free troposphere. The mixing ratios of some brominated compounds, such as CHBr3 and CHBr2Cl, are found to be higher in this top layer of snow relative to the boundary layer. Results were inconclusive due to the limited number of samples, but suggest the possible presence of active bromine in the snow pack and also that some differences exist between chemical reactions occurring in interstitial air compared to air in the boundary layer.
    Type of Medium: Electronic Resource
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