0000000000131878
AUTHOR
P. Hoor
Chemical and meteorological influences on the lifetime of NO<sub>3</sub> at a semirural mountain site during "PARADE"
Abstract. Through measurements of NO2, O3, and NO3 during the PARADE campaign (PArticles and RAdicals, Diel observations of mEchanisms of oxidation) in the German Taunus mountains we derive nighttime, steady state lifetimes (τss) of NO3 and N2O5. During some nights, high NO3 (~ 200 pptv) and N2O5 (~ 1 ppbv) mixing ratios are associated with values of τss that exceeded one hour for NO3 and three hours for N2O5 near the ground. Such long boundary layer lifetimes for NO3 and N2O5 are usually only encountered in very clean/unreactive air masses whereas the PARADE measurement site is impacted by both biogenic emissions from the surrounding forest and anthropogenic emissions from the nearby urban…
The novel HALO mini-DOAS instrument: inferring trace gas concentrations from airborne UV/visible limb spectroscopy under all skies using the scaling method
Abstract. We report on a novel six-channel optical spectrometer (further on called mini-DOAS instrument) for airborne nadir and limb measurements of atmospheric trace gases, liquid and solid water, and spectral radiances in the UV/vis and NIR spectral ranges. The spectrometer was developed for measurements from aboard the German High-Altitude and Long-Range (HALO) research aircraft during dedicated research missions. Here we report on the relevant instrumental details and the novel scaling method used to infer the mixing ratios of UV/vis absorbing trace gases from their absorption measured in limb geometry. The uncertainties of the scaling method are assessed in more detail than before for …
In situ observations of CH2Cl2 and CHCl3 show efficient transport pathways for very short-lived species into the lower stratosphere via the Asian and the North American summer monsoon
Efficient transport pathways for ozone-depleting very short-lived substances (VSLSs) from their source regions into the stratosphere are a matter of current scientific debate; however they have yet to be fully identified on an observational basis. Understanding the increasing impact of chlorine-containing VSLSs (Cl-VSLSs) on stratospheric ozone depletion is important in order to validate and improve model simulations and future predictions. We report on a transport study using airborne in situ measurements of the Cl-VSLSs dichloromethane (CH2Cl2) and trichloromethane (chloroform, CHCl3) to derive a detailed description of two transport pathways from (sub)tropical source regions into the ext…
Chlorine partitioning in the lowermost Arctic vortex during the cold winter 2015/2016
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-resolution mass spectrometric observations of HCl and ClONO2. Simultaneous measurements of CFC-12 are used to derive total inorganic chlorine (Cly) and active chlorine (ClOx). The new data…
Vertical profiles of light absorption and scattering associated with black carbon particle fractions in the springtime Arctic above 79° N
Despite the potential importance of black carbon (BC) for radiative forcing of the Arctic atmosphere, vertically resolved measurements of the particle light scattering coefficient (σsp) and light absorption coefficient (σap) in the springtime Arctic atmosphere are infrequent, especially measurements at latitudes at or above 80∘ N. Here, relationships among vertically distributed aerosol optical properties (σap, σsp and single scattering albedo or SSA), particle microphysics and particle chemistry are examined for a region of the Canadian archipelago between 79.9 and 83.4∘ N from near the surface to 500 hPa. Airborne data collected during April 2015 are combined with gro…
Particulate trimethylamine in the summertime Canadian high Arctic lower troposphere
Size-resolved and vertical profile measurements of single particle chemical composition (sampling altitude range 50–3000 m) were conducted in July 2014 in the Canadian high Arctic during an aircraft-based measurement campaign (NETCARE 2014). We deployed the single particle laser ablation aerosol mass spectrometer ALABAMA (vacuum aerodynamic diameter range approximately 200–1000 nm) to identify different particle types and their mixing states. On the basis of the single particle analysis, we found that a significant fraction (23 %) of all analyzed particles (in total: 7412) contained trimethylamine (TMA). Two main pieces of evidence suggest that these TMA-containing particles originated from…
A tandem approach for collocated measurements of microphysical and radiative cirrus properties
Microphysical and radiation measurements were collected with the novel AIRcraft TOwed Sensor Shuttle (AIRTOSS) – Learjet tandem platform. The platform is a combination of an instrumented Learjet 35A research aircraft and an aerodynamic bird, which is detached from and retracted back to the aircraft during flight via a steel wire with a length of 4000 m. Both platforms are equipped with radiative, cloud microphysical, trace gas, and meteorological instruments. The purpose of the development of this tandem set-up is to study the inhomogeneity of cirrus as well as other stratiform clouds. Sophisticated numerical flow simulations were conducted in order to optimally integrate an axially asymmet…
Chemical and meteorological influences on the lifetime of NO3 at a semi-rural mountain site during PARADE
Through measurements of NO2, O3 and NO3 during the PARADE campaign (PArticles and RAdicals, Diel observations of mEchanisms of oxidation) in the German Taunus mountains we derive nighttime steady-state lifetimes (τss) of NO3 and N2O5. During some nights, high NO3 (∼ 200 pptv) and N2O5 (∼ 1 ppbv) mixing ratios were associated with values of τss that exceeded 1 h for NO3 and 3 h for N2O5 near the ground. Such long boundary-layer lifetimes for NO3 and N2O5 are usually only encountered in very clean/unreactive air masses, whereas the PARADE measurement site is impacted by both biogenic emissions from the surrounding forest and anthropogenic emissions from the nearby urbanised/industrialised cen…
Overview paper: New insights into aerosol and climate in the Arctic
Motivated by the need to predict how the Arctic atmosphere will change in a warming world, this article summarizes recent advances made by the research consortium NETCARE (Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments) that contribute to our fundamental understanding of Arctic aerosol particles as they relate to climate forcing. The overall goal of NETCARE research has been to use an interdisciplinary approach encompassing extensive field observations and a range of chemical transport, earth system, and biogeochemical models. Several major findings and advances have emerged from NETCARE since its formation in 2013. (1) Unexpectedly high summer…
Organic and inorganic bromine measurements around the extratropical tropopause and lowermost stratosphere: insights into the transport pathways and total bromine
We report on measurements of total bromine (Brtot) in the upper troposphere and lower stratosphere taken during 15 flights with the German High Altitude and LOng range research aircraft (HALO). The research campaign WISE (Wave-driven ISentropic Exchange) included regions over the North Atlantic, Norwegian Sea, and northwestern Europe in fall 2017. Brtot is calculated from measured total organic bromine (Brorg) added to inorganic bromine (Bryinorg), evaluated from measured BrO and photochemical modeling. Combining these data, the weighted mean [Brtot] is 19.2±1.2 ppt in the northern hemispheric lower stratosphere (LS), in agreement with expectations for Brtot in the middle stratosphere (Enge…