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The importance of vertical velocity variability for estimates of the indirect aerosol effects

The activation of aerosols to form cloud droplets is dependent upon vertical velocities whose local variability is not typically resolved at the GCM grid scale. Consequently, it is necessary to represent the subgrid-scale variability of vertical velocity in the calculation of cloud droplet number concentration. This study uses the UK Chemistry and Aerosols community model (UKCA) within the Hadley Centre Global Environmental Model (HadGEM3), coupled for the first time to an explicit aerosol activation parameterisation, and hence known as UKCA-Activate. We explore the range of uncertainty in estimates of the indirect aerosol effects attributable to the choice of parameterisation of the subgrid-scale variability of vertical velocity in HadGEM-UKCA. Results of simulations demonstrate that the use of a characteristic vertical velocity cannot replicate results derived with a distribution of vertical velocities, and is to be discouraged in GCMs. This study focuses on the effect of the variance (σw2) of a Gaussian pdf (probability density function) of vertical velocity. Fixed values of σw (spanning the range measured in situ by nine flight campaigns found in the literature) and a configuration in which σw depends on turbulent kinetic energy are tested. Results from the mid-range fixed σw and TKE-based configurations both compare well with observed vertical velocity distributions and cloud droplet number concentrations. The radiative flux perturbation due to the total effects of anthropogenic aerosol is estimated at −1.9 W m−2 with σw = 0.1 m s−1, −2.1 W m−2 with σw derived from TKE, −2.25 W m−2 with σw = 0.4 m s−1, and −2.3 W m−2 with σw = 0.7 m s−1. The breadth of this range is 0.4 W m−2, which is comparable to a substantial fraction of the total diversity of current aerosol forcing estimates. Reducing the uncertainty in the parameterisation of σw would therefore be an important step towards reducing the uncertainty in estimates of the indirect aerosol effects. Detailed examination of regional radiative flux perturbations reveals that aerosol microphysics can be responsible for some climate-relevant radiative effects, highlighting the importance of including microphysical aerosol processes in GCMs.
Corrigendum to "Spectro-microscopic measurements of carbonaceous aerosol aging in Central California" published in Atmos. Chem. Phys., 13, 10445–10459, 2013
A study of aerosol liquid water content based on hygroscopicity measurements at high relative humidity in the North China Plain

Water can be a major component of aerosol particles, also serving as a medium for aqueous-phase reactions. In this study, a novel method is presented to calculate the aerosol liquid water content at high relative humidity based on measurements of aerosol hygroscopic growth factor, particle number size distribution and relative humidity in the Haze in China (HaChi) summer field campaign (July–August 2009) in the North China Plain. The aerosol liquid water content calculated using this method agreed well with that calculated using a thermodynamic equilibrium model (ISORROPIA II) at high relative humidity (>60%) with a correlation coefficient of 0.96. At low relative humidity (<60%), an underestimation was found in the calculated aerosol liquid water content by the thermodynamic equilibrium model. This discrepancy mainly resulted from the ISORROPIA II model, which only considered limited aerosol chemical compositions. The mean and maximum values of aerosol liquid water content during the HaChi campaign reached 1.69 × 10−4 g m−3 and 9.71 × 10−4 g m−3, respectively. A distinct diurnal variation of the aerosol liquid water content was found, with lower values during daytime and higher ones at night. The aerosol liquid water content depended strongly on the relative humidity. The aerosol liquid water content in the accumulation mode dominated the total aerosol liquid water content.
Extensive spatiotemporal analyses of surface ozone and related meteorological variables in South Korea for the period 1999–2010

Spatiotemporal characteristics of surface ozone (O3) variations over South Korea are investigated with consideration of meteorological factors and timescales based on the Kolmogorov–Zurbenko filter (KZ filter), using measurement data at 124 air quality monitoring sites and 72 weather stations for the 12 yr period of 1999–2010. In general, O3 levels at coastal cities are high due to dynamic effects of the sea breeze while those at the inland and Seoul Metropolitan Area (SMA) cities are low due to the NOx titration by local precursor emissions. We examine the meteorological influences on O3 using a combined analysis of the KZ filter and linear regressions between O3 and meteorological variables. We decomposed O3 time series at each site into short-term, seasonal, and long-term components by the KZ filter and regressed on meteorological variables. Impact of temperature on the O3 levels is significantly high in the highly populated SMA and inland region, but low in the coastal region. In particular, the probability of high O3 occurrence doubles with 4 °C of temperature increase in the SMA during high O3 months (May–October). This implies that those regions will experience frequent high O3 events in a future warming climate. In terms of short-term variation, the distribution of high O3 probability classified by wind direction shows the effect of both local precursor emissions and long-range transport from China. In terms of long-term variation, the O3 concentrations have increased by +0.26 ppbv yr−1 (parts per billion by volume) on nationwide average, but their trends show large spatial variability. Singular value decomposition analyses further reveal that the long-term temporal evolution of O3 is similar to that of nitrogen dioxide, although the spatial distribution of their trends is different. This study will be helpful as a reference for diagnostics and evaluation of regional- and local-scale O3 and climate simulations, and as a guide to appropriate O3 control policy in South Korea.
Overview of the Manitou Experimental Forest Observatory: site description and selected science results from 2008 to 2013

The Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen (BEACHON) project seeks to understand the feedbacks and inter-relationships between hydrology, biogenic emissions, carbon assimilation, aerosol properties, clouds and associated feedbacks within water-limited ecosystems. The Manitou Experimental Forest Observatory (MEFO) was established in 2008 by the National Center for Atmospheric Research to address many of the BEACHON research objectives, and it now provides a fixed field site with significant infrastructure. MEFO is a mountainous, semi-arid ponderosa pine-dominated forest site that is normally dominated by clean continental air but is periodically influenced by anthropogenic sources from Colorado Front Range cities. This article summarizes the past and ongoing research activities at the site, and highlights some of the significant findings that have resulted from these measurements. These activities include - soil property measurements; - hydrological studies; - measurements of high-frequency turbulence parameters; - eddy covariance flux measurements of water, energy, aerosols and carbon dioxide through the canopy; - determination of biogenic and anthropogenic volatile organic compound emissions and their influence on regional atmospheric chemistry; - aerosol number and mass distributions; - chemical speciation of aerosol particles; - characterization of ice and cloud condensation nuclei; - trace gas measurements; and - model simulations using coupled chemistry and meteorology. In addition to various long-term continuous measurements, three focused measurement campaigns with state-of-the-art instrumentation have taken place since the site was established, and two of these studies are the subjects of this special issue: BEACHON-ROCS (Rocky Mountain Organic Carbon Study, 2010) and BEACHON-RoMBAS (Rocky Mountain Biogenic Aerosol Study, 2011).
Quantifying black carbon from biomass burning by means of levoglucosan – a one-year time series at the Arctic observatory Zeppelin

Levoglucosan, a highly specific tracer of particulate matter from biomass burning, has been used to study the influence of residential wood burning, agricultural waste burning and Boreal forest fire emissions on the Arctic atmosphere black carbon (BC) concentration. A one-year time series from March 2008 to March 2009 of levoglucosan has been established at the Zeppelin observatory in the European Arctic. Elevated concentrations of levoglucosan in winter (mean: 1.02 ng m−3) compared to summer (mean: 0.13 ng m−3) were observed, resembling the seasonal variation seen for e.g. sulfate and BC. The mean concentration in the winter period was 2–3 orders of magnitude lower than typical values reported for European urban areas in winter, and 1–2 orders of magnitude lower than European rural background concentrations. Episodes of elevated levoglucosan concentration lasting from 1 to 6 days were more frequent in winter than in summer and peak values were higher, exceeding 10 ng m−3 at the most. Concentrations of elemental carbon from biomass burning (ECbb) were obtained by combining measured concentrations of levoglucosan and emission ratios of levoglucosan and EC for wildfires/agricultural fires and for residential wood burning. Neglecting chemical degradation by OH provides minimum levoglucosan concentrations, corresponding to a mean ECbb concentration of 3.7 ± 1.2 ng m−3 in winter (October–April) and 0.8 ± 0.3 ng m−3 in summer (May–September), or 8.8 ± 4.5% of the measured equivalent black carbon (EBC) concentration in winter and 6.1 ± 3.4% in summer. When accounting for chemical degradation of levoglucosan by OH, an upper estimate of 31–45% of EBC could be attributed to ECbb* (ECbb adjusted for chemical degradation) in winter, whereas no reliable (<100%) upper estimate could be provided for summer for the degradation rates applied. Hence, fossil fuel sources appear to dominate the European Arctic BC concentrations in winter, whereas the very wide range obtained for summer does not allow us to conclude upon this for the warm season. Calculations using the Lagrangian particle dispersion model FLEXPART show that the seasonal variation of the modeled ECbb (ECbb,m) concentration compared relatively well with observationally derived ECbb from agricultural fires/wildfires during summer, and residential wood burning in winter. The model overestimates by a factor of 2.2 in winter and 4.4 in summer when compared to the observationally derived mean ECbb concentration, which provides the minimum estimate, whereas it underestimates by a factor of 2.3–3.3 in winter and a factor of 4.5 in summer when compared to ECbb*, which provides the upper estimate. There are indications of too-low emissions of residential wood burning in northern Russia, a region of great importance with respect to observed concentrations of BC in the European Arctic.
Growth of sulphuric acid nanoparticles under wet and dry conditions

New particle formation, which greatly influences the number concentrations and size distributions of an atmospheric aerosol, is often followed by a rapid growth of freshly formed particles. The initial growth of newly formed aerosol is the crucial process determining the fraction of nucleated particles growing to cloud condensation nuclei sizes, which have a significant influence on climate. In this study, we report the laboratory observations of the growth of nanoparticles produced by nucleation of H2SO4 and water in a laminar flow tube at temperatures of 283, 293 and 303 K, under dry (a relative humidity of 1%) and wet conditions (relative humidity of 30%) and residence times of 30, 45, 60 and 90 s. The initial H2SO4 concentration spans the range from 2 × 108 to 1.4 × 1010 molecule cm−3 and the calculated wall losses of H2SO4 were assumed to be diffusion limited. The detected particle number concentrations, measured by the Ultrafine Condensation Particle Counter (UCPC) and Differential Mobility Particle Sizer (DMPS), were found to depend strongly on the residence time. Hygroscopic particle growth, presented by growth factors, was found to be in good agreement with the previously reported studies. The experimental growth rates ranged from 20 nm h−1 to 890 nm h−1 at relative humidity (RH) 1% and from 7 nm h−1 to 980 nm h−1 at RH 30% and were found to increase significantly with the increasing concentration of H2SO4. Increases in the nucleation temperature had a slight enhancing effect on the growth rates under dry conditions. The influence of relative humidity on growth was not consistent – at lower H2SO4 concentrations, the growth rates were higher under dry conditions while at H2SO4 concentrations greater than 1 × 1010 molecule cm−3, the growth rates were higher under wet conditions. The growth rates show only a weak dependence on the residence time. The experimental observations were compared with predictions made using a numerical model, which investigates the growth of particles with three different extents of neutralization by ammonia, NH3: (1) pure H2SO4 – H2O particles; (2) particles formed by ammonium bisulphate, (NH4)HSO4; (3) particles formed by ammonium sulphate, (NH4)2SO4. The highest growth rates were found for ammonium sulphate particles. Since the model accounting for the initial H2SO4 concentration predicted the experimental growth rates correctly, our results suggest that the commonly presumed diffusional wall losses of H2SO4 in case of long-lasting experiments are not so significant. We therefore assume that there are not only losses of H2SO4 on the wall, but also a flux of H2SO4 molecules from the wall into the flow tube, the effect being more profound under dry conditions and at higher temperatures of the tube wall. Based on a comparison with the atmospheric observations, our results indicate that sulphuric acid alone cannot explain the growth rates of particles formed in the atmosphere.
From emissions to ambient mixing ratios: online seasonal field measurements of volatile organic compounds over a Norway spruce-dominated forest in central Germany

Biogenic volatile organic compounds (BVOCs) are substantial contributors to atmospheric chemistry and physics and demonstrate the close relationship between biosphere and atmosphere. Their emission rates are highly sensitive to meteorological and environmental changes with concomitant impacts on atmospheric chemistry. We have investigated seasonal isoprenoid and oxygenated VOC (oxVOC) fluxes from a Norway spruce (Picea abies) tree in central Germany and explored the emission responses under various atmospheric conditions. Emission rates were quantified by using dynamic branch enclosure and proton-transfer-reaction mass spectrometry (PTR-MS) techniques. Additionally, ambient mixing ratios were derived through application of a new box model treatment on the dynamic chamber measurements. These are compared in terms of abundance and origin with the corresponding emissions. Isoprenoids dominate the BVOC emissions from Norway spruce, with monoterpenes and sesquiterpenes accounting for 50.8 ± 7.2% and 19.8 ± 8.1% respectively of the total emissions. Normalizing the VOC emission rates, we have observed a trend of reduction of carbon-containing emissions from April to November, with an enhancement of oxVOC. Highest emission rates were observed in June for all measured species, with the exception of sesquiterpenes, which were emitted most strongly in April. Finally, we evaluate the temperature-dependent algorithm that seems to describe the temperature-dependent emissions of methanol, acetaldehyde and monoterpenes but only with the use of the monthly derived values for emission potential, Es, and temperature dependency, β factor.
The quasi 16-day wave in mesospheric water vapor during boreal winter 2011/2012

This study investigates the characteristics of the quasi 16-day wave in the mesosphere during boreal winter 2011/2012 using observations of water vapor from ground-based microwave radiometers and satellite data. The ground-based microwave radiometers are located in Seoul (South Korea, 37° N), Bern (Switzerland, 47° N) and Sodankylä (Finland, 67° N). The quasi 16-day wave is observed in the mesosphere at all three locations, while the dominant period increases with latitude from 15 days at Seoul to 20 days at Sodankylä. The observed evolution of the quasi 16-day wave confirms that the wave activity is strongly decreased during a sudden stratospheric warming that occurred in mid-January 2012. Using satellite data from the Microwave Limb Sounder on the Aura satellite, we examine the zonal characteristics of the quasi 16-day wave and conclude that the observed waves above the midlatitudinal stations Seoul and Bern are eastward-propagating s = −1 planetary waves with periods of 15 to 16 days, while the observed oscillation above the polar station Sodankylä is a standing wave with a period of approximately 20 days. The strongest relative wave amplitudes in water vapor during the investigated time period are approximately 15%. The wave activity varies strongly along a latitude circle. The activity of the quasi 16-day wave in mesospheric water vapor during boreal winter 2011/2012 is strongest over northern Europe, the North Atlantic Ocean and northwestern Canada. The region of highest wave activity seems to be related to the position of the polar vortex. We conclude that the classic approach to characterize planetary waves zonally averaged along a latitude circle is not sufficient to explain the local observations because of the strong longitudinal dependence of the wave activity.
Comparison of Eulerian and Lagrangian moisture source diagnostics – the flood event in eastern Europe in May 2010

Moisture convergence from different sources is an important prerequisite for a heavy-precipitation event. The contributions from different source regions can, however, hardly be quantified from observations, and their assessment based on model results is complex. Two conceptually different numerical methods are widely used for the quantification of moisture sources: Lagrangian approaches based on the analysis of humidity variations along backward trajectories and Eulerian methods based on the implementation of moisture tracers into a numerical model. In this study the moisture sources for a high-impact, heavy-precipitation event that affected eastern Europe in May 2010 are studied with both Eulerian and Lagrangian moisture source diagnostics. The precipitation event was connected to a cyclone that developed over northern Africa, moved over the Mediterranean towards eastern Europe and induced transport of moist air towards the Carpathian Mountains. Heavy precipitation and major flooding occurred in Poland, the Czech Republic and Slovakia between 16 and 18 May 2010. The Lagrangian and Eulerian diagnostics consistently indicate a wide spatial and temporal range of moisture sources contributing to the event. The source with the largest share is local evapotranspiration from the European land surface, followed by moisture from the North Atlantic. Further contributions come from tropical western Africa (10–20° N) and the Mediterranean Sea. Contrary to what could be expected, the Mediterranean contribution of about 10% is relatively small. A detailed analysis of exemplary trajectories corroborates the general consistency of the two approaches, and underlines their complementarity. The Lagrangian method allows for mapping out moisture source regions with computational efficiency, whereas the more elaborate Eulerian model requires predefined moisture sources, but includes also processes such as precipitation, evaporation and turbulent mixing. However, in the Eulerian model, uncertainty concerning the relative importance of remote versus local moisture sources arises from different options to parameterise moisture tagging at the surface. Ultimately a more sophisticated parameterisation scheme will be required to reduce this uncertainty.