Heiko Bozem

A quantitative analysis of stratospheric HCl, HNO3, and O3 in the tropopause region near the subtropical jet

The effects of chemical two-way mixing on the Extratropical Transition Layer (ExTL) near the subtropical jet are investigated by stratospheric tracer-tracer correlations. To this end, in situ measurements were performed west of Africa (25-32 ◦ N) during the Transport and Composition of the Upper Troposphere Lower Stratosphere (UTLS)/Earth System Model Validation (TACTS/ESMVal) mission in August/September 2012. The Atmospheric chemical Ionization Mass Spectrometer sampling HCl and HNO3 was for the first time deployed on the new German High Altitude and Long range research aircraft (HALO). Measurements of O3, CO, European Centre for Medium-Range Weather Forecasts (ECMWF) analysis, and the tight correlation of the unambiguous tracer HCl to O3 and HNO3 in the lower stratosphere were used to quantify the stratospheric content of these species in the ExTL. With increasing distance from the tropopause, the stratospheric content increased from 10% to 100% with differing profiles for HNO 3 and O 3 . Tropospheric fractions of 20% HNO 3 and 40% O 3 were detected up to a distance of 30 K above the tropopause.

In situ detection of stratosphere-troposphere exchange of cirrus particles in the midlatitudes

Airborne trace gas, microphysical, and radiation measurements were performed during the AIRcraft TOwed Sensor Shuttle - Inhomogeneous Cirrus Experiment over northern Germany in 2013. Based on high-precision nitrous oxide (N2O) and carbon monoxide (CO) in situ data, stratospheric air could be identified, which contained cirrus cloud particles. Consistent with the stratospheric N2O data, backward trajectories indicate that the sampled air masses crossed the dynamical tropopause in the last 3 h before the measurement. These air masses contained cirrus particles, which were formed during slow ascent in the troposphere and subsequently mixed with stratospheric air. From the CO-N2O correlation the irreversibility of this transport is deduced. To our knowledge, this is the first in situ detection of cirrus particles mixed with stratospheric air in the midlatitudes.

Evidence for marine biogenic influence on summertime Arctic aerosol

We present vertically-resolved observations of aerosol composition during pristine summertime Arctic background conditions. The methansulfonic acid (MSA)-to-sulfate ratio peaked near the surface (mean 0.10), indicating a contribution from ocean-derived biogenic sulfur. Similarly, the organic aerosol (OA)-to-sulfate ratio increased towards the surface (mean 2.0). Both MSA-to-sulfate and OA-to-sulfate ratios were significantly correlated with FLEXPART-WRF-predicted airmass residence time over open water, indicating marine influenced OA. External mixing of sea salt aerosol from a larger number fraction of organic, sulfate and amine-containing particles, together with low wind speeds (median 4.7 m s−1), suggests a role for secondary organic aerosol formation. Cloud condensation nuclei concentrations were nearly constant (∼120 cm−3) when the OA fraction was <60% and increased to 350 cm−3 when the organic fraction was larger and residence times over open water were longer. Our observations illustrate the importance of marine-influenced OA under Arctic background conditions, which are likely to change as the Arctic transitions to larger areas of open water.

Aircraft measurements of High Arctic springtime aerosol show evidence for vertically varying sources, transport and composition

The sources, chemical transformations and removal mechanisms of aerosol transported to the Arctic are key factors that control Arctic aerosol-climate interactions. Our understanding of sources and processes is limited by a lack of vertically resolved observations in remote Arctic regions. We present vertically resolved observations of trace gases and aerosol composition in High Arctic springtime, made largely north of 80◦N, during the NETCARE campaign. Trace gas gradients observed on these flights defined the polar dome as north of 66 – 68.5◦N and below potential temperatures of 283.5 – 287.5 K (Bozem et al., 5 2018). In the polar dome, we observe evidence for vertically varying source regions and chemical processing. These vertical changes in sources and chemistry lead to systematic variation in aerosol composition as a function of potential temperature. We show evidence for sources of aerosol with higher organic aerosol (OA), ammonium (NH4) and refractory black carbon (rBC) content in the upper polar dome. Based on FLEXPART-ECMWF calculations, air masses sampled at all levels inside the polar dome (i.e., potential temperature < 280.5 K, altitude < ∼3.5 km) subsided during transport over transport times of at 10 least 10 days. Air masses at the lowest potential temperatures, in the lower polar dome, had spent long times (>10 days) in the Arctic, while air masses in the upper polar dome had entered the Arctic more recently. These differences in transport history were closely related to aerosol composition. In the lower polar dome, the measured sub-micron aerosol mass was dominated by sulphate (mean 74%), with lesser contributions from rBC (1%), NH4 (4%) and OA (20%). At higher altitudes and warmer potential temperatures, OA, NH4 and rBC contributed 42%, 8% and 2% of aerosol mass, respectively. A qualitative indication 15 for the presence of sea salt showed that sodium chloride contributed to sub-micron aerosol in the lower polar dome, but was not detectable in the upper polar dome. Our observations suggest that long-term, surface-based measurements underestimate the contribution of OA, rBC and NH4 to aerosol transported to the Arctic troposphere in spring. 1 Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-628 Manuscript under review for journal Atmos. Chem. Phys. Discussion started: 24 August 2018 c

Modelling Regional Air Quality in the Canadian Arctic: Simulation of an Arctic Summer Field Campaign

Model simulations of an Arctic summer field campaign were carried out. The model results were compared with observational data from both ground-based monitoring and in situ measurements on-board multiple mobile platforms. The model was able to well capture regional sources and transport affecting the Arctic air quality. It is shown that the study area was impacted by North American (NA) regional biomass burning emissions. The model-observation comparison also corroborates previous findings on possible roles of marine-biogenic sources in aerosol production in the Arctic MBL during summertime.