0000000000131880
AUTHOR
J. Lelieveld
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…
Impact of Manaus City on the Amazon Green Ocean atmosphere: ozone production, precursor sensitivity and aerosol load
As a contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia – Cooperative LBA Airborne Regional Experiment (LBA-CLAIRE-2001) field campaign in the heart of the Amazon Basin, we analyzed the temporal and spatial dynamics of the urban plume of Manaus City during the wet-to-dry season transition period in July 2001. During the flights, we performed vertical stacks of crosswind transects in the urban outflow downwind of Manaus City, measuring a comprehensive set of trace constituents including O<sub>3</sub>, NO, NO<sub>2</sub>, CO, VOC, CO<sub>2</sub>, and H<sub>2</sub>O. Aerosol loads were characterized by concentrations of t…
The summertime Boreal forest field measurement intensive (HUMPPA-COPEC-2010): an overview of meteorological and chemical influences
This paper describes the background, instrumentation, goals, and the regional influences on the HUMPPACOPEC intensive field measurement campaign, conducted at the Boreal forest research station SMEAR II (Station for Measuring Ecosystem-Atmosphere Relation) in Hyyti¨al¨a, Finland from 12 July–12 August 2010. The prevailing meteorological conditions during the campaign are examined and contrasted with those of the past six years. Back trajectory analyses show that meteorological conditions at the site in 2010 were characterized by a higher proportion of southerly flow than in the other years studied. As a result the summer of 2010 was anomalously warm and high in ozone making the campaign rel…
Implementation of a comprehensive ice crystal formation parameterization for cirrus and mixed-phase clouds in the EMAC model (based on MESSy 2.53)
A comprehensive ice nucleation parameterization has been implemented in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations (ICNCs). The parameterization of Barahona and Nenes (2009, hereafter BN09) allows for the treatment of ice nucleation taking into account the competition for water vapour between homogeneous and heterogeneous nucleation in cirrus clouds. Furthermore, the influence of chemically heterogeneous, polydisperse aerosols is considered by applying one of the multiple ice nucleating particle parameterizations which are included in BN09 to compute the heterogeneously formed ice crystals. BN09 has been modified in order to co…
The summertime Boreal forest field measurement intensive (HUMPPA-COPEC-2010): an overview of meteorological and chemical influences
This paper describes the background, instrumentation, goals, and the regional influences on the HUMPPACOPEC intensive field measurement campaign, conducted at the Boreal forest research station SMEAR II (Station for Measuring Ecosystem-Atmosphere Relation) in Hyyti¨al¨a, Finland from 12 July–12 August 2010. The prevailing meteorological conditions during the campaign are examined and contrasted with those of the past six years. Back trajectory analyses show that meteorological conditions at the site in 2010 were characterized by a higher proportion of southerly flow than in the other years studied. As a result the summer of 2010 was anomalously warm and high in ozone making the campaign rel…
Sensitivity of transatlantic dust transport to chemical aging and related atmospheric processes
We present a sensitivity study on transatlantic dust transport, a process which has many implications for the atmosphere, the ocean and the climate. We investigate the impact of key processes that control the dust outflow, i.e., the emission flux, convection schemes and the chemical aging of mineral dust, by using the EMAC model following Abdelkader et al. (2015). To characterize the dust outflow over the Atlantic Ocean, we distinguish two geographic zones: (i) dust interactions within the Intertropical Convergence Zone (ITCZ), or the dust–ITCZ interaction zone (DIZ), and (ii) the adjacent dust transport over the Atlantic Ocean (DTA) zone. In the latter zone, the dust loading shows a steep …
Emission of nitrous acid from soil and biological soil crusts represents an important source of HONO in the remote atmosphere in Cyprus
Abstract. Soil and biological soil crusts can emit nitrous acid (HONO) and nitric oxide (NO). The terrestrial ground surface in arid and semiarid regions is anticipated to play an important role in the local atmospheric HONO budget, deemed to represent one of the unaccounted-for HONO sources frequently observed in field studies. In this study HONO and NO emissions from a representative variety of soil and biological soil crust samples from the Mediterranean island Cyprus were investigated under controlled laboratory conditions. A wide range of fluxes was observed, ranging from 0.6 to 264 ng m−2 s−1 HONO-N at optimal soil water content (20–30 % of water holding capacity, WHC). Maximum NO-N f…
Hydroxyl radicals in the tropical troposphere over the Suriname rainforest: comparison of measurements with the box model MECCA
As a major source region of the hydroxyl radical OH, the Tropics largely control the oxidation capacity of the atmosphere on a global scale. However, emissions of hydrocarbons from the tropical rainforest that react rapidly with OH can potentially deplete the amount of OH and thereby reduce the oxidation capacity. The airborne GABRIEL field campaign in equatorial South America (Suriname) in October 2005 investigated the influence of the tropical rainforest on the HO<sub>x</sub> budget (HO<sub>x</sub> = OH + HO<sub>2</sub>). The first observations of OH and HO<sub>2</sub> over a tropical rainforest are compared to steady state concentrations ca…
Including vegetation dynamics in an atmospheric chemistry-enabled general circulation model: linking LPJ-GUESS (v4.0) with the EMAC modelling system (v2.53)
Central to the development of Earth system models (ESMs) has been the coupling of previously separate model types, such as ocean, atmospheric, and vegetation models, to address interactive feedbacks between the system components. A modelling framework which combines a detailed representation of these components, including vegetation and other land surface processes, enables the study of land–atmosphere feedbacks under global climate change. Here we present the initial steps of coupling LPJ-GUESS, a dynamic global vegetation model, to the atmospheric chemistry-enabled atmosphere–ocean general circulation model EMAC. The LPJ-GUESS framework is based on ecophysiological processes, such as phot…
Diurnal variability, photochemical production and loss processes of hydrogen peroxide in the boundary layer over Europe
Hydrogen peroxide (H2O2) plays a significant role in the oxidizing capacity of the atmosphere. It is an efficient oxidant in the liquid phase and serves as a temporary reservoir for the hydroxyl radical (OH), the most important oxidizing agent in the gas phase. Due to its high solubility, removal of H2O2 due to wet and dry deposition is efficient, being a sink of HOx (OH+HO2) radicals. In the continental boundary layer, the H2O2 budget is controlled by photochemistry, transport and deposition processes. Here we use in situ observations of H2O2 and account for chemical source and removal mechanisms to study the interplay between these processes. The data were obtained during five ground-base…
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…
Summertime total OH reactivity measurements from boreal forest during HUMPPA-COPEC 2010
Ambient total OH reactivity was measured at the Finnish boreal forest station SMEAR II in Hyytiälä (Latitude 61&deg;51' N; Longitude 24&deg;17' E) in July and August 2010 using the Comparative Reactivity Method (CRM). The CRM – total OH reactivity method – is a direct, in-situ determination of the total loss rate of hydroxyl radicals (OH) caused by all reactive species in air. During the intensive field campaign HUMPPA-COPEC 2010 (<b>H</b>yytiälä <b>U</b>nited <b>M</b>easurements of <b>P</b>hotochemistry and <b>P</b>articles in <b>A</b>ir – <b>C</b>omprehensive <b>O</b>rganic <b>P&l…
Daytime formation of nitrous acid at a coastal remote site in Cyprus indicating a common ground source of atmospheric HONO and NO
Characterization of daytime sources of nitrous acid (HONO) is crucial to understand atmospheric oxidation and radical cycling in the planetary boundary layer. HONO and numerous other atmospheric trace constituents were measured on the Mediterranean island of Cyprus during the CYPHEX (CYprus PHotochemical EXperiment) campaign in summer 2014. Average volume mixing ratios of HONO were 35 pptv (±25 pptv) with a HONO ∕ NOx ratio of 0.33, which was considerably higher than reported for most other rural and urban regions. Diel profiles of HONO showed peak values in the late morning (60 ± 28 pptv around 09:00 local time) and persistently high mixing ratios during daytime (45 ± 18 pptv), indicating …
Light-induced protein nitration and degradation with HONO emission
Proteins can be nitrated by air pollutants (NO2), enhancing their allergenic potential. This work provides insight into protein nitration and subsequent decomposition in the presence of solar radiation. We also investigated light-induced formation of nitrous acid (HONO) from protein surfaces that were nitrated either online with instantaneous gas-phase exposure to NO2 or offline by an efficient nitration agent (tetranitromethane, TNM). Bovine serum albumin (BSA) and ovalbumin (OVA) were used as model substances for proteins. Nitration degrees of about 1 % were derived applying NO2 concentrations of 100 ppb under VIS∕UV illuminated conditions, while simultaneous decomposition of (nitrated) p…