In situ measurements of the ClO/HCl ratio: Heterogeneous processing on sulfate aerosols and polar stratospheric clouds

1993 ◽  
Vol 20 (22) ◽  
pp. 2523-2526 ◽  
Author(s):  
C. R. Webster ◽  
R. D. May ◽  
D. W. Trohey ◽  
L. M. Avallone ◽  
J. G. Anderson ◽  
...  
2005 ◽  
Vol 5 (5) ◽  
pp. 1371-1380 ◽  
Author(s):  
C. Voigt ◽  
H. Schlager ◽  
B. P. Luo ◽  
A. Dörnbrack ◽  
A. Roiger ◽  
...  

Abstract. A PSC was detected on 6 February 2003 in the Arctic stratosphere by in-situ measurements onboard the high-altitude research aircraft Geophysica. Low number densities (~10-4cm-3) of small nitric acid (HNO3) containing particles (d<6µm) were observed at altitudes between 18 and 20km. Provided the temperatures remain below the NAT equilibrium temperature TNAT, these NAT particles have the potential to grow further and to remove HNO3 from the stratosphere, thereby enhancing polar ozone loss. Interestingly, the NAT particles formed in less than a day at temperatures just slightly below TNAT (T>TNAT-3.1K). This unique measurement of PSC formation at extremely low NAT saturation ratios (SNAT≤10) constrains current NAT nucleation theories. We suggest, that the NAT particles have formed heterogeneously, but for certain not on ice. Conversely, meteoritic particles may be favorable candidates for triggering NAT nucleation at the observed low number densities.


1996 ◽  
Vol 14 (3) ◽  
pp. 315-328 ◽  
Author(s):  
D. Fonteyn ◽  
N. Larsen

Abstract. A new two-dimensional zonal model of the stratosphere, based on a formulation in an isentropic framework, with complete chemistry has been coupled with a high resolution detailed microphysical model for polar stratospheric clouds (PSCs). The 2D model chemistry includes all presently known heterogeneous processes on sulfate aerosols and PSCs. The coupling of these two models, with inherently different time scales, is discussed. It is demonstrated that in order to obtain a realistic interrelationship between NOy and N2O an accurate simulation of the sedimentation by PSC particles is necessary. A good agreement of model PSC presence and observations is found for the Antarctic polar winter without the need to impose additional artificial temperature variations in the model. The calculated occurrence of polar stratospheric clouds and resulting heterogeneous chemistry during the Antarctic winter are discussed. Sensitivity of the polar stratospheric chemical composition and cloud formation for different perturbations is investigated by studying the effects of transport across the polar vortex boundary and heterogeneous processing by an enhanced sulfate aerosol load. The importance of including sedimentation for all cases is also discussed.


2019 ◽  
Vol 19 (9) ◽  
pp. 6235-6250 ◽  
Author(s):  
Camelia Talianu ◽  
Petra Seibert

Abstract. An increase in the sulfate aerosols observed in the period 1–6 April 2014 over Austria is analyzed using in situ measurements at an Austrian air quality background station, lidar measurements at the closest EARLINET stations around Austria, CAMS near-real-time data, and particle dispersion modeling using FLEXPART, a Lagrangian transport model. In situ measurements of SO2, PM2.5, PM10, and O3 were performed at the air quality background station Pillersdorf, Austria (EMEP station AT30, 48∘43′ N, 15∘55′ E). A CAMS aerosol mixing ratio analysis for Pillersdorf and the lidar stations Leipzig, Munich, Garmisch, and Bucharest indicates the presence of an event of aerosol transport, with sulfate and dust as principal components. For the sulfate layers identified at Pillersdorf from the CAMS analysis, backward- and forward-trajectory analyses were performed, associating lidar stations with the trajectories. The lidar measurements for the period corresponding to trajectory overpass of associated stations were analyzed, obtaining the aerosol layers, the optical properties, and the aerosol types. The potential sources of transported aerosols were determined for Pillersdorf and the lidar stations using the source–receptor sensitivity computed with FLEXPART, combined with the MACCity source inventory. A comparative analysis for Pillersdorf and the trajectory-associated lidar stations showed consistent aerosol layers, optical properties and types, and potential sources. A complex pattern of contributions to sulfate over Austria was found in this paper. For the lower layers (below 2000 m) of sulfate, it was found that central Europe was the main source of sulfate. Medium to smaller contributions come from sources in eastern Europe, northwest Africa, and the eastern US. For the middle-altitude layers (between 2000 and 5000 m), sources from central Europe (northern Italy, Serbia, Hungary) contribute with similar emissions. Northwest Africa and the eastern US also have important contributions. For the high-altitude layers (above 5000 m), the main contributions come from northwest Africa, but sources from the southern and eastern US also contribute significantly. No contributions from Europe are seen for these layers. The methodology used in this paper can be used as a general tool to correlate measurements at in situ stations and EARLINET lidar stations around these in situ stations.


2019 ◽  
Author(s):  
Michael Stukel ◽  
Thomas Kelly

Thorium-234 (234Th) is a powerful tracer of particle dynamics and the biological pump in the surface ocean; however, variability in carbon:thorium ratios of sinking particles adds substantial uncertainty to estimates of organic carbon export. We coupled a mechanistic thorium sorption and desorption model to a one-dimensional particle sinking model that uses realistic particle settling velocity spectra. The model generates estimates of 238U-234Th disequilibrium, particulate organic carbon concentration, and the C:234Th ratio of sinking particles, which are then compared to in situ measurements from quasi-Lagrangian studies conducted on six cruises in the California Current Ecosystem. Broad patterns observed in in situ measurements, including decreasing C:234Th ratios with depth and a strong correlation between sinking C:234Th and the ratio of vertically-integrated particulate organic carbon (POC) to vertically-integrated total water column 234Th, were accurately recovered by models assuming either a power law distribution of sinking speeds or a double log normal distribution of sinking speeds. Simulations suggested that the observed decrease in C:234Th with depth may be driven by preferential remineralization of carbon by particle-attached microbes. However, an alternate model structure featuring complete consumption and/or disaggregation of particles by mesozooplankton (e.g. no preferential remineralization of carbon) was also able to simulate decreasing C:234Th with depth (although the decrease was weaker), driven by 234Th adsorption onto slowly sinking particles. Model results also suggest that during bloom decays C:234Th ratios of sinking particles should be higher than expected (based on contemporaneous water column POC), because high settling velocities minimize carbon remineralization during sinking.


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