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  • 11
    Publication Date: 2019-07-12
    Description: A number of techniques have been proposed for detecting atmospheric OH radicals. Of these, the laser-induced fluorescence (LIF) technique has been used by the largest number of investigators. One of the problems arising in connection with the implementation of this technique is related to the perturbing effect of the UV (lambda approximately 282 nm) laser beam used for OH monitoring, while another problem relates to signal extraction. Several new LIF approaches have been or are currently under development with the objective to bring both problems under control. The present paper deals with the experimental features of one of these new approaches. The considered approach is referred to as 2-lambda laser-induced fluorescence (2-lambda LIF). It is shown that the 2-lambda LIF system provides significant advantages over earlier 1-lambda LIF OH measurement instruments operating at ambient pressure.
    Keywords: INSTRUMENTATION AND PHOTOGRAPHY
    Type: Journal of Geophysical Research (ISSN 0148-0227); 90; 12
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  • 12
    Publication Date: 2019-08-28
    Description: Aircraft measurements of key reactive nitrogen species (NO, NO2, HNO3, PAN, PPN, NO3(-), NO(y)), C1 to C6 hydrocarbons, acetone, O3, chemical tracers (C2Cl4, CO), and important meteorological parameters were performed over eastern Canada during July to August 1990 at altitudes between 0 and 6 km as part of an Arctic Boundary Layer Expedition (ABLE3B). In the free troposphere, PAN was found to be the single most abundant reactive nitrogen species constituting a major fraction of NO(y) and was significantly more abundant than NO(x) and HNO3. PAN and O3 were well correlated both in their fine and gross structures. Compared to data previously collected in the Arctic/subarctic atmosphere over Alaska (ABLE3A), the lower troposphere (0-4 km) over eastern Canada was found to contain larger reactive nitrogen and anthropogenic tracer concentrations. At higher altitudes (4-6 km) the atmospheric composition was in many ways similar to what was seen over Alaska and supports the view that a large-scale reservoir of PAN (and NO(y)) is present in the upper troposphere over the entire Arctic/subarctic region. The reactive nitrogen budget based on missions conducted from the North Bay site (missions 2-10) showed a small shortfall, whereas the budget for data collected from the Goose Bay operation (missions 11-19) showed essential balance. It is calculated that 15-20 ppt of the observed NO(x) may find its source from the available PAN reservoir. Meteorological considerations as well as relationships between reactive nitrogen and tracer species suggest that the atmosphere over eastern Canada during summer is greatly influenced by forest fires and transported industrial pollution.
    Keywords: METEOROLOGY AND CLIMATOLOGY
    Type: Journal of Geophysical Research (ISSN 0148-0227); 99; D1; p. 1821-1835
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  • 13
    Publication Date: 2019-08-28
    Description: Biomass-burning impacted air masses sampled over central and eastern Canada during the summer of 1990 as part of ABLE 3B contained enhanced mixing ratios of gaseous HNO3, HCOOH, CH3COOH, and what appears to be (COOH)2. These aircraft-based samples were collected from a variety of fresh burning plumes and more aged haze layers from different source regions. Values of the enhancement factor, delta X/delta CO, where X represents an acidic gas, for combustion-impacted air masses sampled both near and farther away from the fires, were relatively uniform. However, comparison of carboxylic acid emission ratios measured in laboratory fires to field plume enhancement factors indicates significant in-plume production of HCOOH. Biomass-burning appears to be an important source of HNO3, HCOOH, and CH3COOH to the troposphere over subarctic Canada.
    Keywords: METEOROLOGY AND CLIMATOLOGY
    Type: Journal of Geophysical Research (ISSN 0148-0227); 99; D1; p. 1721-1737
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  • 14
    Publication Date: 2019-08-28
    Description: Measurements of NO, NO2, PAN and NO(y) are presented for the summertime middle/lower troposphere over northern high latitudes. Chemical signatures from concurrent measurements of O3, CO, C2H2, C2H6, C3H8, C2Cl4, and H2O are used to characterize factors affecting the budget and distribution of N(x)O(y) in the Arctic and Sub-Arctic tropospheric air masses sampled over Alaska during the NASA Arctic Boundary Layer Expedition (ABLE 3A). The results implicate biomass burning in Siberia as the probable source of about one-third of the NO(y) abundance within the middle lower troposphere over Alaska and the downward transport of air from altitude in the vicinity of the tropopause as a major contributor to the abundance of NO(y) within the lower 6 km column over Alaska.
    Keywords: GEOPHYSICS
    Type: Journal of Geophysical Research (ISSN 0148-0227); 97; D15; p. 16,481-16,509.
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  • 15
    Publication Date: 2019-08-28
    Description: Budgets of O3, NO(x), and NO(y), and acetic acid in the Arctic Boundary Layer Expedition (ABLE 3A) flight region are constructed using photochemical model statistics based on aircraft observations. A Lagrangian model is used to reconstruct the photochemical history of two aged biomass fire plumes sampled by the ABLE 3A aircraft. It is shown that anthropogenic influence on O3 levels in the Arctic may manifest itself not by long-range transport of pollution-derived O3, but rather by a decrease of the regional photochemical sink due to the presence of small amounts of NO(x). The low concentrations of NO(x) measured in ABLE 3A were sufficient to reduce the rate of photochemical loss appreciably relative to a NO(x)-free atmosphere, thus increasing the O3 lifetime. It is shown that decomposition of PAN can account for most of the NO(x) measured below 4-km altitude, but for only 20 percent at 6-km altitude. A lifetime of 29 days is estimated for NO(y) in the ABLE 23A flight region.
    Keywords: GEOPHYSICS
    Type: Journal of Geophysical Research (ISSN 0148-0227); 97; D15; p. 16,421-16,431.
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  • 16
    Publication Date: 2019-08-28
    Description: We report here large-scale features of the distribution of NO(x), HNO3, PAN, particle NO3, and NO(y) in the troposphere from 0.15 to 6 km altitude over central Canada. These measurements were conducted in July - August 1990 from the NASA Wallops Electra aircraft as part of the joint United States-Canadian Arctic Boundary Layer Expedition (ABLE) 3B-Northern Wetlands Study. Our findings show that this region is generally NO(x) limited, with NO(x) mixing ratios typically 20-30 parts per trillion by volume (pptv). We found little direct evidence for anthropogenic enhancement of mixing ratios of reactive odd nitrogen species and NO(y) above those in 'background' air. Instead, it appears that enhancements in the mixing ratios of these species were primarily due to emissions from several day old or CO-rich-NO(x)-poor smoldering local biomass-burning fires. NO(x) mixing ratios in biomass-burning impacted air masses were usually less than 50 pptv, but those of HNO3 and PAN were typically 100-300 pptv representing a twofold-threefold enhancement over 'background' air. During our study period, inputs of what appeared to be aged tropical air were a major factor influencing the distribution of reactive odd nitrogen in the midtroposphere over northeastern North America. These air masses were quite depleted in NO(y) (generally less than 150 pptv), and a frequent summertime occurrence of such air masses over this region would imply a significant influence on the reactive odd nitrogen budget. Our findings show that the chemical composition of aged air masses over subarctic Canada and those documented in the Arctic during ABLE 3A have strikingly similar chemistries, suggesting large-scale connection between the air masses influencing these regions.
    Keywords: METEOROLOGY AND CLIMATOLOGY
    Type: Journal of Geophysical Research (ISSN 0148-0227); 99; D1; p. 1863-1885
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  • 17
    Publication Date: 2019-07-12
    Description: The operating principle, design, and performance of a two-photon LIF (TP-LIF) sensor for simultaneous measurements of NO, NO(x) (NO + NO2), and NO2 are described. In this instrument, NO is first measured by direct spectroscopic TP-LIF detection; NO2 is converted to NO by photofragmentation using an XeF excimer laser operating at 353 nm; and the resulting NO is then detected quantitatively by TP-LIF. The detection limits of the instrument are found to be 3.5 parts per trillion by volume (pptv) of NO and 10 pptv for NO2, with integration times of 2 and 6 min, respectively. The in-flight performance of the instrument was evaluated during the NASA Global Tropospheric Experiment Chemical Instrumentation Test and Evaluation 2 program in summer 1986, as reported by Gregory et al. (1990).
    Keywords: AIRCRAFT INSTRUMENTATION
    Type: Journal of Geophysical Research (ISSN 0148-0227); 95; 10155-10
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  • 18
    Publication Date: 2019-07-12
    Description: Reported in this paper are the Georgia Institute of Technology NO results from the fall 1983 NASA GTE/CITE 1 Airborne Field Sampling Program. These data were predominantly collected over a geographical area defined by the eastern and central North Pacific Ocean, spanning the latitude range of 15-42 deg N. These NO measurements were taken using the two-photon laser-induced fluorescence technique. The data show a general trend of increasing levels of NO from the boundary layer up to altitudes of nearly 10 km. The average midday value of NO at altitudes of less than or equal to 1.8 km was 4 parts per trillion by volume (pptv), and at about 6 km, 20 pptv, whereas that at about 9 km was 25-35 pptv, the higher value reflecting the inclusion of NO data collected from the outflow region of two electrically active cumulonimbus clouds. The high-altitude NO data strongly suggest that at least during the time of the GTE flight operation, the major sources of NO for remote regions of the Pacific Ocean were those resulting from lightning and the downward transport of stratospheric air.
    Keywords: GEOPHYSICS
    Type: Journal of Geophysical Research (ISSN 0148-0227); 92; 2049-207
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  • 19
    Publication Date: 2019-07-13
    Description: Aerosol sampling for the determination of the concentrations of soluble ionic species and the natural radionuclides Be-7 and Pb-210 was conducted from the NASA DC-8 over the western Pacific as part of GTE/PEM-West B during February - March 1994. Concentrations of most soluble ionic species in the free troposphere were higher in samples collected on flights originating from Hong Kong and Japan than those collected further east over the open ocean. In both regions the measured concentrations were higher than those found during PEM-West A (fall 1991). Activities of Pb-210 tracer of air masses influenced by sources on the Asian continent, showed the same patterns. These data indicate the effect of stronger continental outflow from Asia over the western Pacific during the spring compared to fall season. For readily scavenged aerosol-associated species and soluble acidic gases the strongest indications of Asian outflow were restricted to altitudes below 6 km. The distribution of the continental tracer Pb-210 was also compared to those of a large number of gas phase species measured on the DC-8. Relatively strong correlations were found with O3 and peroxyacetylnitrate (PAN), but only during the flights over the remote Pacific. During PEM-West A, similar correlations were seen, but they were stronger near Asia. We believe that these correlations are a signature of continental air that has been processed by deep wet convection over land before being advected over the ocean. One flight over the Sea of Japan provided the opportunity to sample upper troposphere/lower stratosphere air in and around a tropopause fold. Concentrations of Be-7 reached 7 pCi/cu m STP, and peak O3, mixing ratios of 480 ppb were encountered at 10.7 km. The Be-7 data are used to estimate the fraction of stratospheric air mixed down into the troposphere by circulation in the fold.
    Keywords: Environment Pollution
    Type: Paper-96JD02981 , Journal of Geophysical Research (ISSN 0148-0227); 102; D23; 28,287-28,302
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  • 20
    Publication Date: 2019-07-13
    Description: The chemical characteristics of air parcels over the tropical South Atlantic during September - October 1992 are summarized by analysis of aged marine and continental outflow classifications. Positive correlations between CO and CH3CL and minimal enhancements of C2CL40, and various ChloroFluoroCarbon (CFC) species in air parcels recently advected over the South Atlantic basin strongly suggest an impact on tropospheric chemistry from biomass burning on adjacent continental areas of Brazil and Africa. Comparison of the composition of aged Pacific air with aged marine air over the South Atlantic basin from 0.3 to 12.5 km altitude indicates potential accumulation of long-lived species during the local dry season. This may amount to enhancements of up to two-fold for C2H6, 30% for CO, and 10% for CH3Cl. Nitric oxide and NO(x) were significantly enhanced (up to approx. 1 part per billion by volume (ppbv)) above 10 km altitude and poorly correlated with CO and CH3Cl. In addition, median mixing ratios of NO and NO(x) were essentially identical in aged marine and continental outflow air masses. It appears that in addition to biomass burning, lightning or recycled reactive nitrogen may be an important source of NO(x) to the upper troposphere. Methane exhibited a monotonic increase with altitude from approx. 1690 to 1720 ppbv in both aged marine and continental outflow air masses. The largest mixing ratios in the upper troposphere were often anticorrelated with CO, CH3Cl, and CO2, suggesting CH, contributions from natural sources. We also argue, based on CH4/CO ratios and relationships with various hydrocarbon and CFC species, that inputs from biomass burning and the northern hemisphere are unlikely to be the dominant sources of CO, CH4 and C2H6 in aged marine air. Emissions from urban areas would seem to be necessary to account for the distribution of at least CH4 and C2H6. Over the African and South American continents an efficient mechanism of convective vertical transport coupled with large-scale circulations conveys biomass burning, urban, and natural emissions to the upper troposphere over the South Atlantic basin. Slow subsidence over the eastern South Atlantic basin may play an important role in establishing and maintaining the rather uniform vertical distribution of long-lived species over this region. The common occurrence of values greater than 1 for the ratio CH3OOH/H2O2 in the upper troposphere suggests that precipitation scavenging effectively removed highly water soluble gases (H2O2, HNO3, HCOOH, and CH3COOH) and aerosols during vertical convective transport over the continents. However, horizontal injection of biomass burning products over the South Atlantic, particularly water soluble species and aerosol particles, was frequent below 6 km altitude.
    Keywords: Environment Pollution
    Type: NASA/CR-96-207359 , NAS 1.26:207359 , Paper-95JDO3630 , Journal of Geophysical Research (ISSN 0148-0227); 101; D19; 24,187-24,202
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