Abstract. In April-July 2008, intensive measurements were made of atmospheric composition and chemistry in Sabah, Malaysia, as part of the "Oxidant and particle photochemical processes above a South-East Asian tropical rainforCorrespondence to: C. N. Hewitt (n.hewitt@lancaster.ac.uk) est" (OP3) project. Fluxes and concentrations of trace gases and particles were made from and above the rainforest canopy at the Bukit Atur Global Atmosphere Watch station and at the nearby Sabahmas oil palm plantation, using both ground-based and airborne measurements. Here, the measurement and modelling strategies used, the characteristics of the sites and an overview of data obtained are described. Composition measurements show that the rainforest Published by Copernicus Publications on behalf of the European Geosciences Union. 170 C. N. Hewitt et al.: The OP3 project: introduction, rationale, location characteristics and tools site was not significantly impacted by anthropogenic pollution, and this is confirmed by satellite retrievals of NO 2 and HCHO. The dominant modulators of atmospheric chemistry at the rainforest site were therefore emissions of BVOCs and soil emissions of reactive nitrogen oxides. At the observed BVOC:NO x volume mixing ratio (∼100 pptv/pptv), current chemical models suggest that daytime maximum OH concentrations should be ca. 10 5 radicals cm −3 , but observed OH concentrations were an order of magnitude greater than this. We confirm, therefore, previous measurements that suggest that an unexplained source of OH must exist above tropical rainforest and we continue to interrogate the data to find explanations for this.
Abstract.Results from a measurement study performed in the Tropical Atlantic on board the RHaMBLe Discovery Cruise D319 are presented. Measurements of aerosol composition, hygroscopicity and CCN activity were used to test the ability of a single parameter model to describe water uptake in sub-and supersaturated conditions. It was found that the magnitude and temporal variability of the sub-saturated water uptake could be well represented using the non-refractory composition to derive the model input for 2 periods when the large majority of the aerosol mass was non-refractory. As may be expected, when a significant fraction of the aerosol volume is refractory the sub-saturated water uptake is not well predicted by the non-refractory composition. When predicting the cloud activation potential from the composition and the hygroscopicity there is a consistent under-prediction of the CCN activity. The prediction of CCN activity from the sub-saturated water uptake gives a better prediction of the CCN activity than the composition when the non-refractory components are not fully representative of the aerosol composition.Based on these observations it appears that a single parameter cannot always capture the behavior fully across the sub-and supersaturated regimes. Measurements made at relative humidities (RHs) up to 94% showed that the water activity appears satisfactorily represented by a single parameter Correspondence to: G. McFiggans (g.mcfiggans@manchester.ac.uk) derived at 90% RH. It therefore appears that the change in the observed hygroscopicity take place between 94 %RH and the point of activation. This change may be due in part to a change solution non-ideality, surface tension effects or the presence of sparingly soluble compounds for example, but cannot be reconciled without measurements at higher RHs.
Abstract. Aerosol physical, chemical and hygroscopic properties were measured in a range of airmasses during COPS (Convective and Orographically-induced Precipitation Study) ground-based in June and July of 2007 at the Hornisgrinde mountain site in the Black Forest, Southwest Germany. Non-refractory aerosol composition was measured with an Aerosol Mass Spectrometer, simultaneous to hygroscopic growth factors at 86% relative humidity and CCN activity measurements for particles of dry (< 20%) diameters 27 to 217 nm, with particle water uptake exhibiting substantial variability with time and with particle size.Variability in the measurements of hygroscopic growth factor and critical supersaturation for particles of similar sizes indicates significant compositional impact on particle water affinity. Critical supersaturation prediction using a single parameter hygroscopicity approximation derived from measured HTDMA mean growth factors deviate, beyond measurement uncertainties, from critical supersaturations derived from CCN measurements. These led to differences averaging around 35% in the number of CCN (N CCN ) for the most reliable measurements depending on averaging methodology, often very much larger for individual time periods. This indicates aspects of water uptake behaviour unresolved in this experiment by the single parameter representation which, depending on its origin, may have important consequences on its generalised use.
Long‐term measurements of the light absorption coefficient (babs) obtained with a particle soot absorption photometer (PSAP), babs (PSAP), have been previously reported for Barrow, Alaska, and Ny‐Ålesund, Spitsbergen, in the Arctic. However, the effects on babs of other aerosol chemical species coexisting with black carbon (BC) have not been critically evaluated. Furthermore, different mass absorption cross section (MAC) values have been used to convert babs to BC mass concentration (MBC = babs/MAC). We used a continuous soot monitoring system (COSMOS), which uses a heated inlet to remove volatile aerosol compounds, to measure babs (babs (COSMOS)) at these sites during 2012–2015. Field measurements and laboratory experiments have suggested that babs (COSMOS) is affected by about 9% on average by sea‐salt aerosols. MBC values derived by COSMOS (MBC (COSMOS)) using a MAC value obtained by our previous studies agreed to within 9% with elemental carbon concentrations at Barrow measured over 11 months. babs (PSAP) was higher than babs (COSMOS), by 22% at Barrow (PM1) and by 43% at Ny‐Ålesund (PM10), presumably due to the contribution of volatile aerosol species to babs (PSAP). Using babs (COSMOS) as a reference, we derived MBC (PSAP) from babs (PSAP) measured since 1998. We also established the seasonal variations of MBC at these sites. Seasonally averaged MBC (PSAP) decreased at a rate of about 0.55 ± 0.30 ng m−3 yr−1. We also compared MBC (COSMOS) and scaled MBC (PSAP) values with previously reported data and evaluated the degree of inconsistency in the previous data.
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