scholarly journals Measurement of 14C Concentrations of Stratospheric CO2 by Accelerator Mass Spectrometry

Radiocarbon ◽  
1992 ◽  
Vol 34 (3) ◽  
pp. 745-752 ◽  
Author(s):  
Toshio Nakamura ◽  
Takakiyo Nakazawa ◽  
Nobuyuki Nakai ◽  
Hiroyuki Kitagawa ◽  
Hideyuki Honda ◽  
...  

In order to measure the concentrations of anthropogenically influenced gases in the stratosphere, we have collected air samples from the lower stratosphere since 1985, by a balloon-borne cryogenic sampling method, developed at the Institute of Space and Astronautical Science (ISAS). Air samples of ≃16 liters at STP were collected in the stratosphere at altitudes from 18.6 to 30.4 km, over the northeastern part of Japan (39.5°N, 139–142°E), on 1 September 1989. We conducted 14C analyses to study the vertical and horizontal air-mass movement in the stratosphere, and to investigate the air transport mechanism between troposphere and stratosphere. Carbon dioxide (containing a few mg carbon) was separated cryogenically from the air samples, and the 14C concentration of the CO2 was measured by a Tandetron accelerator mass spectrometer, using Fe-graphite targets prepared by reducing CO2 on Fe-powder with hydrogen in a Vycor tube at 650°. The 14C concentrations, expressed as Δ14C, of CO2 were 267–309‰ at altitudes of 21–30 km, and 134‰ at 19–20 km. The Δ14C values at 21–30 km were higher than those of the current tropospheric CO2, of around 80–200‰. The observed 14C concentrations, higher in the stratosphere than the troposphere, seem to be explained by large bomb-produced 14C inventories and/or high 14C production by cosmic rays, as well as weak vertical mixing of air masses in the stratosphere.

2010 ◽  
Vol 10 (22) ◽  
pp. 10753-10770 ◽  
Author(s):  
K. S. Law ◽  
F. Fierli ◽  
F. Cairo ◽  
H. Schlager ◽  
S. Borrmann ◽  
...  

Abstract. Trace gas and aerosol data collected in the tropical tropopause layer (TTL) between 12–18.5 km by the M55 Geophysica aircraft as part of the SCOUT-AMMA campaign over West Africa during the summer monsoon in August 2006 have been analysed in terms of their air mass origins. Analysis of domain filling back trajectories arriving over West Africa, and in the specific region of the flights, showed that the M55 flights were generally representative of air masses arriving over West Africa during the first 2 weeks of August, 2006. Air originating from the mid-latitude lower stratosphere was under-sampled (in the mid-upper TTL) whilst air masses uplifted from central Africa (into the lower TTL) were over-sampled in the latter part of the campaign. Signatures of recent (previous 10 days) origins were superimposed on the large-scale westward flow over West Africa. In the lower TTL, air masses were impacted by recent local deep convection over Africa at the level of main convective outflow (350 K, 200 hPa) and on certain days up to 370 K (100 hPa). Estimates of the fraction of air masses influenced by local convection vary from 10 to 50% depending on the method applied and from day to day during the campaign. The analysis shows that flights on 7, 8 and 11 August were more influenced by local convection than on 4 and 13 August allowing separation of trace gas and aerosol measurements into "convective" and "non-convective" flights. Strong signatures, particularly in species with short lifetimes (relative to CO2) like CO, NO and fine-mode aerosols were seen during flights most influenced by convection up to 350–365 K. Observed profiles were also constantly perturbed by uplift (as high as 39%) of air masses from the mid to lower troposphere over Asia, India, and oceanic regions resulting in import of clean oceanic (e.g. O3-poor) or polluted air masses from Asia (high O3, CO, CO2) into West Africa. Thus, recent uplift of CO2 over Asia may contribute to the observed positive CO2 gradients in the TTL over West Africa. This suggests a more significant fraction of younger air masses in the TTL and needs to taken into consideration in derivations of mean age of air. Transport of air masses from the mid-latitude lower stratosphere had an impact from the mid-TTL upwards (20–40% above 370 K) during the campaign period importing air masses with high O3 and NOy. Ozone profiles show a less pronounced lower TTL minimum than observed previously by regular ozonesondes at other tropical locations. Concentrations are less than 100 ppbv in the lower TTL and vertical gradients less steep than in the upper TTL. The air mass origin analysis and simulations of in-situ net photochemical O3 production, initialised with observations, suggest that the lower TTL is significantly impacted by uplift of O3 precursors (over Africa and Asia) leading to positive production rates (up to 2 ppbv per day) in the lower and mid TTL even at moderate NOx levels. Photochemical O3 production increases with higher NOx and H2O in air masses with O3 less than 150 ppbv.


2010 ◽  
Vol 10 (6) ◽  
pp. 15485-15536 ◽  
Author(s):  
K. S. Law ◽  
F. Fierli ◽  
F. Cairo ◽  
H. Schlager ◽  
S. Borrmann ◽  
...  

Abstract. Trace gas and aerosol data collected in the tropical tropopause layer (TTL) between 12–18.5 km by the M55 Geophysica aircraft as part of the SCOUT-AMMA campaign over West Africa during the summer monsoon in August 2006 have been analysed in terms of their air mass origins. Analysis of domain filling back trajectories arriving over West Africa, and in the specific region of the flights, showed that the M55 flights were generally representative of air masses arriving over West Africa during the first 2 weeks of August, 2006. Air originating from the mid-latitude lower stratosphere was under-sampled (in the mid-upper TTL) whilst air masses uplifted from central Africa (into the lower TTL) were over-sampled in the latter part of the campaign. Signatures of recent (previous 10 days) origins were superimposed on the large-scale westerly flow over West Africa. In the lower TTL, air masses were impacted by recent local deep convection over Africa at the level of main convective outflow (350 K, 200 hPa) and on certain days up to 370 K (100 hPa). Estimates of the fraction of air masses influenced by local convection vary from 10 to 50% depending on the method applied and from day to day during the campaign. The analysis shows that flights on 7, 8 and 11 August were more influenced by local convection than on 4 and 13 August allowing separation of trace gas and aerosol measurements into ''convective'' and ''non-convective'' flights. Strong signatures, particularly in short-lived species like CO, NO and fine-mode aerosols were seen during flights most influenced by convection up to 350–365 K. Observed profiles were also constantly perturbed by uplift (as high as 39%) of air masses from the mid to lower troposphere over Asia, India, and oceanic regions resulting in import of clean oceanic (e.g., O3-poor) or polluted air masses from Asia (high O3, CO, CO2) into West Africa. Thus, recent uplift of CO2 over Asia may contribute to the observed positive CO2 gradients in the TTL over West Africa. This suggests a more significant fraction of younger air masses in the TTL making it difficult to derive mean age of air from average gradients. Transport of air masses from the mid-latitude lower stratosphere had an impact from the mid-TTL upwards (20–40% above 370 K) during the campaign period importing air masses with high O3 and NOy. Ozone profiles show a less pronounced lower TTL minimum than observed previously by regular ozonesondes at other tropical locations. Concentrations are less than 100 ppbv in the lower TTL and vertical gradients less steep than in the upper TTL. The air mass origin analysis and simulations of in-situ net photochemical O3 production, initialised with observations, suggest that the lower TTL is significantly impacted by uplift of O3 precursors (over Africa and Asia) leading to positive production rates (up to 2 ppbv per day) in the lower and mid TTL even at moderate NOx levels. Photochemical O3 production increases with higher NOx and H2O in air masses with O3 less than 150 ppbv.


2020 ◽  
Vol 4 ◽  
pp. 78-95
Author(s):  
A.R. Ivanova ◽  
◽  
E.N. Skriptunova ◽  
N.I. Komasko ◽  
A.A. Zavialova ◽  
...  

A review of literature on the impact of dust and sand storms on the air transport operation is presented. Observational data on dust storms at the aerodromes of European Russia for the period of 2001-2019 are analyzed. The seasonal variations in dust transport episodes at aerodromes and its relationship with visibility changes are discussed. The characteristics of dusty air masses and advection are given. It is concluded that the frequency of dust transfer episodes for the aerodromes under study has decreased over the past five years, except for Gumrak aerodrome (Volgograd). Keywords: dust storm, sand storm, aviation, visibility, seasonal variations, aerodrome оf European Russia


2019 ◽  
Vol 19 (19) ◽  
pp. 12477-12494 ◽  
Author(s):  
Armin Sigmund ◽  
Korbinian Freier ◽  
Till Rehm ◽  
Ludwig Ries ◽  
Christian Schunk ◽  
...  

Abstract. To assist atmospheric monitoring at high-alpine sites, a statistical approach for distinguishing between the dominant air masses was developed. This approach was based on a principal component analysis using five gas-phase and two meteorological variables. The analysis focused on the Schneefernerhaus site at Zugspitze Mountain, Germany. The investigated year was divided into 2-month periods, for which the analysis was repeated. Using the 33.3 % and 66.6 % percentiles of the first two principal components, nine air mass regimes were defined. These regimes were interpreted with respect to vertical transport and assigned to the BL (recent contact with the boundary layer), UFT/SIN (undisturbed free troposphere or stratospheric intrusion), and HYBRID (influences of both the boundary layer and the free troposphere or ambiguous) air mass classes. The input data were available for 78 % of the investigated year. BL accounted for 31 % of the cases with similar frequencies in all seasons. UFT/SIN comprised 14 % of the cases but was not found from April to July. HYBRID (55 %) mostly exhibited intermediate characteristics, whereby 17 % of the HYBRID class suggested an influence from the marine boundary layer or the lower free troposphere. The statistical approach was compared to a mechanistic approach using the ceilometer-based mixing layer height from a nearby valley site and a detection scheme for thermally induced mountain winds. Due to data gaps, only 25 % of the cases could be classified using the mechanistic approach. Both approaches agreed well, except in the rare cases of thermally induced uplift. The statistical approach is a promising step towards a real-time classification of air masses. Future work is necessary to assess the uncertainty arising from the standardization of real-time data.


2011 ◽  
Vol 11 (1) ◽  
pp. 363-373 ◽  
Author(s):  
H. Bencherif ◽  
L. El Amraoui ◽  
G. Kirgis ◽  
J. Leclair De Bellevue ◽  
A. Hauchecorne ◽  
...  

Abstract. This paper reports on an increase of ozone event observed over Kerguelen (49.4° S, 70.3° E) in relationship with large-scale isentropic transport. This is evidenced by ground-based observations (co-localised radiosonde and SAOZ experiments) together with satellite global observations (Aura/MLS) assimilated into MOCAGE, a Méteo-France model. The study is based on the analyses of the first ozonesonde experiment never recorded at the Kerguelen site within the framework of a French campaign called ROCK that took place from April to August 2008. Comparisons and interpretations of the observed event are supported by co-localised SAOZ observations, by global mapping of tracers (O3, N2O and columns of O3) from Aura/MLS and Aura/OMI experiments, and by model simulations of Ertel Potential Vorticity initialised by the ECMWF (European Centre for Medium-Range Weather Forecasts) data reanalyses. Satellite and ground-based observational data revealed a consistent increase of ozone in the local stratosphere by mid-April 2008. Additionally, Ozone (O3) and nitrous oxide (N2O) profiles obtained during January–May 2008 using the Microwave Limb Sounder (MLS) aboard the Aura satellite are assimilated into MOCAGE (MOdèle de Chimie Atmosphérique à Grande Echelle), a global three-dimensional chemistry transport model of Météo-France. The assimilated total O3 values are consistent with SAOZ ground observations (within ±5%), and isentropic distributions of O3 match well with maps of advected potential vorticity (APV) derived from the MIMOSA model, a high-resolution advection transport model, and from the ECMWF reanalysis. The event studied seems to be related to the isentropic transport of air masses that took place simultaneously in the lower- and middle-stratosphere, respectively from the polar region and from the tropics to the mid-latitudes. In fact, the ozone increase observed by mid April 2008 resulted simultaneously: (1) from an equator-ward departure of polar air masses characterised with a high-ozone layer in the lower stratosphere (near the 475 K isentropic level), and (2) from a reverse isentropic transport from the tropics to mid- and high-latitudes in the upper stratosphere (nearby the 700 K level). The increase of ozone observed over Kerguelen from the 16-April ozonesonde profile is thus attributed to a concomitant isentropic transport of ozone in two stratospheric layers: the tropical air moving southward and reaching over Kerguelen in the upper stratosphere, and the polar air passing over the same area but in the lower stratosphere.


2010 ◽  
Vol 2010 ◽  
pp. 1-15 ◽  
Author(s):  
D. G. Kaskaoutis ◽  
P. G. Kosmopoulos ◽  
H. D. Kambezidis ◽  
P. T. Nastos

Aerosol optical depth at 550 nm () and fine-mode (FM) fraction data from Terra-MODIS were obtained over the Greater Athens Area covering the period February 2000–December 2005. Based on both and FM values three main aerosol types have been discriminated corresponding to urban/industrial aerosols, clean maritime conditions, and coarse-mode, probably desert dust, particles. Five main sectors were identified for the classification of the air-mass trajectories, which were further used in the analysis of the ( and FM data for the three aerosol types). The HYSPLIT model was used to compute back trajectories at three altitudes to investigate the relation between -FM and wind sector depending on the altitude. The accumulation of local pollution is favored in spring and corresponds to air masses at lower altitudes originating from Eastern Europe and the Balkan. Clean maritime conditions are rare over Athens, limited in the winter season and associated with air masses from the Western or Northwestern sector. The coarse-mode particles origin seems to be more complicated proportionally to the season. Thus, in summer the Northern sector dominates, while in the other seasons, and especially in spring, the air masses belong to the Southern sector enriched with Saharan dust aerosols.


2020 ◽  
Vol 20 (20) ◽  
pp. 12033-12045
Author(s):  
Haeyoung Lee ◽  
Edward J. Dlugokencky ◽  
Jocelyn C. Turnbull ◽  
Sepyo Lee ◽  
Scott J. Lehman ◽  
...  

Abstract. To understand the Korean Peninsula's carbon dioxide (CO2) emissions and sinks as well as those of the surrounding region, we used 70 flask-air samples collected during May 2014 to August 2016 at Anmyeondo (AMY; 36.53∘ N, 126.32∘ E; 46 m a.s.l.) World Meteorological Organization (WMO) Global Atmosphere Watch (GAW) station, located on the west coast of South Korea, for analysis of observed 14C in atmospheric CO2 as a tracer of fossil fuel CO2 contribution (Cff). Observed 14C ∕ C ratios in CO2 (reported as Δ values) at AMY varied from −59.5 ‰ to 23.1 ‰, with a measurement uncertainty of ±1.8 ‰. The derived mean value Cff of (9.7±7.8) µmol mol−1 (1σ) is greater than that found in earlier observations from Tae-Ahn Peninsula (TAP; 36.73∘ N, 126.13∘ E; 20 m a.s.l., 28 km away from AMY) of (4.4±5.7) µmol mol−1 from 2004 to 2010. The enhancement above background mole fractions of sulfur hexafluoride (Δx(SF6)) and carbon monoxide (Δx(CO)) correlate strongly with Cff (r>0.7) and appear to be good proxies for fossil fuel CO2 at regional and continental scales. Samples originating from the Asian continent had greater Δx(CO) : Cff(RCO) values, (29±8) to (36±2) nmol µmol−1, than in Korean Peninsula local air ((8±2) nmol µmol−1). Air masses originating in China showed (1.6±0.4) to (2.0±0.1) times greater RCO than a bottom-up inventory, suggesting that China's CO emissions are underestimated in the inventory, while observed RSF6 values are 2–3 times greater than inventories for both China and South Korea. However, RCO values derived from both inventories and observations have decreased relative to previous studies, indicating that combustion efficiency is increasing in both China and South Korea.


2016 ◽  
Author(s):  
Osamu Uchino ◽  
Tetsu Sakai ◽  
Toshiharu Izumi ◽  
Tomohiro Nagai ◽  
Isamu Morino ◽  
...  

Abstract. To validate products of the Greenhouse gases Observing SATellite (GOSAT), we observed vertical profiles of aerosols, thin cirrus clouds, and tropospheric ozone with a mobile lidar system that consisted of a two-wavelength (532 and 1064 nm) polarization lidar and a tropospheric ozone Differential Absorption Lidar (DIAL). We used these lidars to make continuous measurements over Saga (33.24° N, 130.29° E) during 20–31 March 2015. High ozone and high aerosol concentrations were observed almost simultaneously in the altitude range 0.5–1.5 km from 03:00 to 20:00 Japan Standard Time on 22 March 2015. The maximum ozone volume mixing ratio was ~ 110 ppbv. The maxima of the aerosol extinction coefficient and optical depth at 532 nm were 1.2 km−1 and 2.1, respectively. Backward trajectory analysis indicated that an air mass with high ozone and aerosol concentrations could have been transported from Northeast Asia. Based on the lidar data and the ground-based in-situ measurements at Saga, this air mass could have been transported to the surface by vertical mixing when the planetary boundary layer developed in the daytime. This plume, which contained high ozone and aerosol pollutant concentrations, impacted surface air quality substantially. After some modifications of its physical and chemical parameters, the Meteorological Research Institute Chemistry-Climate Model, version 2 (MRI-CCM2) approximately reproduced the high-ozone volume-mixing ratio. The Model of Aerosol Species IN the Global AtmospheRe (MASINGAR) mk-2 successfully predicted high aerosol concentrations, but the predicted peak aerosol optical thickness was about one-third of the observed value.


2018 ◽  
Vol 20 (3) ◽  
pp. 544-552 ◽  
Author(s):  
Anteneh Assefa ◽  
Mats Tysklind ◽  
Jana Klanova ◽  
Karin Wiberg

A combination of PCDD/F patterns and metal source markers in ambient air samples together with stable air mass back trajectories can reveal the most significant atmospheric sources of PCDD/Fs.


2021 ◽  
Author(s):  
Meike Rotermund ◽  
Vera Bense ◽  
Martyn Chipperfield ◽  
Andreas Engel ◽  
Jens-Uwe Grooß ◽  
...  

<p>We report on measurements of total bromine (Br<sup>tot</sup>) in the upper troposphere and lower stratosphere (UTLS) taken from the German High Altitude and LOng range research aircraft (HALO) over the North Atlantic, Norwegian Sea and north-western Europe in September/ October 2017 during the WISE (Wave-driven ISentropic Exchange) research campaign. Br<sup>tot</sup> is calculated from measured total organic bromine (Br<sup>org</sup>) (i.e., the sum of bromine contained in CH<sub>3</sub>Br, the halons and the major very short-lived brominated substances) added to inorganic bromine (Br<sub>y</sub><sup>inorg</sup>), evaluated from measured BrO and photochemical modelling. Combining these data, the weighted mean [Br<sup>tot</sup>] is 19.2 ± 1.2 ppt in the extratropical lower stratosphere (Ex-LS) of the northern hemisphere. The inferred average Br<sup>tot</sup> for the Ex-LS is slightly smaller than expected for the middle stratosphere in 2016 (~19.6 ppt (ranging from 19-20 ppt) as reported by the WMO/UNEP Assessment (2018)). However, it reflects the expected variability in Br<sup>tot</sup> in the Ex-LS due to influxes of shorter lived brominated source and product gases from different regions of entry. A closer look into Br<sup>org</sup> and Br<sub>y</sub><sup>inorg</sup> as well as simultaneously measured transport tracers (CO, N<sub>2</sub>O, ...) and an air mass lag-time tracer (SF<sub>6</sub>), suggests that a filament of air with elevated Br<sup>tot</sup> protruded into the extratropical lowermost stratosphere (Ex-LMS) from 350-385 K and between equivalent latitudes of 55-80˚N (high bromine filament – HBrF). Lagrangian transport modelling shows the multi-pathway contributions to Ex-LMS bromine. According to CLaMS air mass origin simulations, contributions to the HBrF consist of predominantly isentropic transport from the tropical troposphere (also with elevated [Br<sup>tot</sup>] = 21.6 ± 0.7 ppt) as well as a smaller contribution from an exchange across the extratropical tropopause which are mixed into the stratospheric background air. In contrast, the surrounding LS above and below the HBrF has less tropical tropospheric air, but instead additional stratospheric background air. Of the tropical tropospheric air in the HBrF, the majority is from the outflow of the Asian monsoon anticyclone and the adjacent tropical regions, which greatly influences concentrations of trace gases transported into the Ex-LMS in boreal summer and fall. The resulting increase of Br<sup>tot</sup> in the Ex-LMS and its consequences for ozone is investigated through the TOMCAT/SLIMCAT model simulations. However, more extensive monitoring of total stratospheric bromine in more aged air (i.e., in the middle stratosphere) as well as globally and seasonally is required in addition to model simulations to fully understand its impact on Ex-LMS ozone and the radiative forcing of climate.</p>


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