Abstract:Activated chlorine compounds in the polar winter stratosphere drive catalytic cycles that deplete ozone and methane, whose abundances are highly relevant to the evolution of global climate. The present work introduces a novel dataset of in situ measurements of relevant chlorine species in the lowermost Arctic stratosphere from the aircraft mission POLSTRACC-GW-LCYCLE-SALSA during winter 2015/2016. The major stages of chemical evolution of the lower polar vortex are presented in a consistent series of high-reso… Show more
“…For this situation, the sum of observed HCl and ClONO 2 , however, is substantially smaller than inferred Cl y , suggesting a significant contribution from active chlorine, ClO x (defined here as the difference between Cl y and the sum of HCl and ClONO 2 ) of up to 1.2 ppbv ( Fig. 15; see also Marsing et al 2019). In fact, the Cl y and ClO x concentrations derived from the in situ observations agree very well with calculations from the CLaMS model.…”
Section: E N I T R I F I C a T I O N O F T H E Stratosphere And Extmentioning
The Polar Stratosphere in a Changing Climate (POLSTRACC) mission employed the German High Altitude and Long Range Research Aircraft (HALO). The payload comprised an innovative combination of remote sensing and in situ instruments. The in situ instruments provided high-resolution observations of cirrus and polar stratospheric clouds (PSCs), a large number of reactive and long-lived trace gases, and temperature at the aircraft level. Information above and underneath the aircraft level was achieved by remote sensing instruments as well as dropsondes. The mission took place from 8 December 2015 to 18 March 2016, covering the extremely cold late December to early February period and the time around the major warming in the beginning of March. In 18 scientific deployments, 156 flight hours were conducted, covering latitudes from 25° to 87°N and maximum altitudes of almost 15 km, and reaching potential temperature levels of up to 410 K. Highlights of results include 1) new aspects of transport and mixing in the Arctic upper troposphere–lower stratosphere (UTLS), 2) detailed analyses of special dynamical features such as tropopause folds, 3) observations of extended PSCs reaching sometimes down to HALO flight levels at 13–14 km, 4) observations of particulate NOy and vertical redistribution of gas-phase NOy in the lowermost stratosphere (LMS), 5) significant chlorine activation and deactivation in the LMS along with halogen source gas observations, and 6) the partitioning and budgets of reactive chlorine and bromine along with a detailed study of the efficiency of ClOx/BrOx ozone loss cycle. Finally, we quantify—based on our results—the ozone loss in the 2015/16 winter and address the question of how extraordinary this Arctic winter was.
“…For this situation, the sum of observed HCl and ClONO 2 , however, is substantially smaller than inferred Cl y , suggesting a significant contribution from active chlorine, ClO x (defined here as the difference between Cl y and the sum of HCl and ClONO 2 ) of up to 1.2 ppbv ( Fig. 15; see also Marsing et al 2019). In fact, the Cl y and ClO x concentrations derived from the in situ observations agree very well with calculations from the CLaMS model.…”
Section: E N I T R I F I C a T I O N O F T H E Stratosphere And Extmentioning
The Polar Stratosphere in a Changing Climate (POLSTRACC) mission employed the German High Altitude and Long Range Research Aircraft (HALO). The payload comprised an innovative combination of remote sensing and in situ instruments. The in situ instruments provided high-resolution observations of cirrus and polar stratospheric clouds (PSCs), a large number of reactive and long-lived trace gases, and temperature at the aircraft level. Information above and underneath the aircraft level was achieved by remote sensing instruments as well as dropsondes. The mission took place from 8 December 2015 to 18 March 2016, covering the extremely cold late December to early February period and the time around the major warming in the beginning of March. In 18 scientific deployments, 156 flight hours were conducted, covering latitudes from 25° to 87°N and maximum altitudes of almost 15 km, and reaching potential temperature levels of up to 410 K. Highlights of results include 1) new aspects of transport and mixing in the Arctic upper troposphere–lower stratosphere (UTLS), 2) detailed analyses of special dynamical features such as tropopause folds, 3) observations of extended PSCs reaching sometimes down to HALO flight levels at 13–14 km, 4) observations of particulate NOy and vertical redistribution of gas-phase NOy in the lowermost stratosphere (LMS), 5) significant chlorine activation and deactivation in the LMS along with halogen source gas observations, and 6) the partitioning and budgets of reactive chlorine and bromine along with a detailed study of the efficiency of ClOx/BrOx ozone loss cycle. Finally, we quantify—based on our results—the ozone loss in the 2015/16 winter and address the question of how extraordinary this Arctic winter was.
“…The accuracies of the measurements are 15% for NO y and CO, 5% for O 3 , 0.1% for CH 4 , and 0.02% for CO 2 . The atmospheric chemical ionization mass spectrometer (AIMS) uses SF 5 − reagent ions for the detection of upper tropospheric and stratospheric concentrations of gaseous SO 2 , hydrogen chloride (HCl), nitric acid (HNO 3 ), and chlorine nitrate (ClONO 2 ) (Voigt et al 2014;Jurkat et al 2016Jurkat et al , 2017Marsing et al 2019).…”
During spring 2020, the COVID-19 pandemic caused massive reductions in emissions from industry, ground and airborne transportation. To explore the resulting atmospheric composition changes, we conducted the BLUESKY campaign with two research aircraft and measured trace gases, aerosols, and cloud properties from the boundary layer to the lower stratosphere. From 16 May to 9 June 2020, we performed 20 flights in the early COVID-19 lockdown phase over Europe and the Atlantic Ocean. We found up to 50% reductions in boundary layer nitrogen dioxide concentrations in urban areas from GOME-2B satellite data, along with carbon monoxide reductions in the pollution hot spots. We measured 20 to 70% reductions in total reactive nitrogen, carbon monoxide and fine mode aerosol concentration in profiles over German cities compared to a 10-year data set from passenger aircraft. The total aerosol mass was significantly reduced below 5 km altitude, and the organic aerosol fraction also aloft, indicative of decreased organic precursor gas emissions. The reduced aerosol optical thickness caused a perceptible shift in sky color towards the blue part of the spectrum (hence BLUESKY) and increased shortwave radiation at the surface. We find that the 80% decline in air traffic led to substantial reductions in nitrogen oxides at cruise altitudes, in contrail cover, and in resulting radiative forcing. The light extinction and depolarization by cirrus were also reduced in regions with substantially decreased air traffic. General circulation-chemistry model simulations indicate good agreement with the measurements when applying a reduced emission scenario. The comprehensive BLUESKY dataset documents the major impact of anthropogenic emissions on the atmospheric composition.
“…An additional in-situ data set is provided by the atmospheric chemical ionization mass spectrometer (AIMS) deployed on DLR-Falcon and includes information on gaseous SO 2 and HNO 3 . For the detection of upper tropospheric and lower stratospheric SO 2 and HNO 3 mixing ratios the AIMS uses SF 5 − reagent ions (Voigt et al, 2014;Jurkat et al, 2016;Marsing et al, 2019;Tomsche et al, 2022). The one sigma detection limit is 0.0006 to 0.0017 ppbv and 0.005 to 0.009 ppbv for SO 2 and HNO 3 , respectively.…”
The composition of the upper troposphere/lower stratosphere region (UTLS) is influenced by long-range or regional transport in the troposphere and stratosphere, vertical transport within convective systems and warm conveyor belts, rapid turbulent mixing, as well as photochemical production or loss of species. This results in the formation of the extratropical transition layer, which has been defined by the vertical structure of CO profiles and studied by now mostly by means of trace gas correlations. Here, we extend the analysis to aerosol particles and derive the ozone to sulfate aerosol correlation in Central Europe from aircraft in-situ measurements during the CAFE-EU/BLUESKY mission in May and June 2020. During the campaign two research aircraft, i.e., DLR-HALO (High Altitude and Long Range Research Aircraft) and DLR-Falcon, were deployed covering an altitude range from the planetary boundary layer up to 14 km altitude and thus probing the UTLS during the COVID-19 period with significant reduced anthropogenic emissions. We operated a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) to measure the chemical composition of non-refractory aerosol particles in the size range from about 40 to 800 nm. In addition to the C-ToF-AMS data, we use trace gas measurements from both HALO and DLR-Falcon.
In our study, we find a correlation between the ozone mixing ratio (O3) and the sulfate mass concentration in the lower stratosphere, between 10 and 14 km for all flights. The correlation is not constant with time but exhibits some variability over the two-week period of the campaign exceeding the background sulfate to ozone correlation. Especially during one flight, we observed enhanced mixing ratios of sulfate aerosol in the lowermost stratosphere, where the analysis of trace gases, such as CO, SO2, H2O, O3 and HNO3 show tropospheric influence during this time. Also, back trajectories indicate, that no recent mixing with tropospheric air occurred within the last 10 days. In addition, we analyzed satellite SO2 retrievals from TROPOMI for volcanic plumes and eruptions. These satellite observations show enhanced volcanic activities in April 2020 on Kamchatka, Russia, with at least one explosive eruption of the Sheveluch volcano reaching the tropopause region and some minor eruptions of different volcanoes into the free troposphere. From these findings, we conclude that gas-to-particle conversion of volcanic SO2 leads to the observed enhanced sulfate aerosol mixing ratios.
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