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Emissions of biogenic volatile organic compounds and subsequent formation of secondary organic aerosols in a Larix kaempferi forest

We conducted simultaneous measurements of concentrations and above-canopy fluxes of isoprene and α-pinene, along with their oxidation products in aerosols in a Larix kaempferi (Japanese larch) forest in summer 2012. Vertical profiles of isoprene showed the maximum concentration near the forest floor with a peak around noon, whereas oxidation products of isoprene, i.e., methacrolein (MACR) and methyl vinyl ketone (MVK), showed higher concentrations near the canopy level of the forest. The vertical profile suggests large emissions of isoprene near the forest floor, likely due to Dryopteris crassirhizoma (a fern species), and the subsequent reaction within the canopy. The concentrations of α-pinene also showed highest values near the forest floor, with maximums in the early morning and late afternoon. The vertical profiles of α-pinene suggest its large emissions from soil and litter in addition to emissions from L. kaempferi leaves at the forest site. Isoprene and its oxidation products in aerosols exhibited similar diurnal variations within the forest canopy, providing evidence of secondary organic aerosol (SOA) formation via oxidation of isoprene most likely emitted from the forest floor. Although high abundance of α-pinene was observed in the morning, its oxidation products in aerosols showed peaks in daytime, due to a time lag between the emission and atmospheric reactions of α-pinene to form SOA. Positive matrix factorization (PMF) analysis indicated that anthropogenic influence is the most important factor contributing to the elevated concentrations of molecular oxidation products of isoprene- (> 64 %) and α-pinene-derived SOA (> 57 %). The combination of the measured fluxes and vertical profiles of biogenic volatile organic compounds (BVOCs) suggests that the inflow of anthropogenic precursors/aerosols likely enhanced the formation of both isoprene SOA and α-pinene SOA within the forest canopy even when the BVOC flux was relatively low. This study highlights the importance of intra-canopy processes that promote biogenic SOA formation in the presence of significant inflow of oxidants together with anthropogenic aerosols and their precursors.
The regional distribution characteristics of aerosol optical depth over the Tibetan Plateau

The Tibetan Plateau (TP) is representative of typical clean atmospheric conditions. Aerosol optical depth (AOD) retrieved by the Multi-angle Imaging SpectroRadiometer (MISR) is higher over Qaidam Basin than the rest of the TP throughout the year. Different monthly variation patterns of AOD are observed over the southern and northern TP, whereby the aerosol load is usually higher in the northern TP than in the southern part. The aerosol load over the northern part increases from April to June, peaking in May. The maximum concentration of aerosols over the southern TP occurs in July. Aerosols appear to be more easily transported to the main body of the TP across the northern edge rather than the southern edge. This is maybe partly because the altitude is lower at the northern edge than that of the Himalayas located along the southern edge of the TP. Three-dimensional distributions of dust, polluted dust, polluted continental aerosol and smoke are also investigated, based on Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) data. Dust is found to be the most prominent aerosol type on the TP, and other types of aerosols affect the atmospheric environment slightly. A dividing line of higher dust occurrence in the northern TP and lower dust occurrence in the southern TP can be observed clearly at an altitude of 6–8 km above sea level, especially in spring and summer. This demarcation appears around 33–35° N in the middle of the plateau, and it is possibly associated with the high-altitude terrain in the same geographic location. Comparisons of CALIPSO and MISR data show that the vertical dust occurrences are consistent with the spatial patterns of AOD. The different seasonal variation patterns between the northern and southern TP are primarily driven by atmospheric circulation, and are also related to the emission characteristics over the surrounding regions.
Impact of atmospheric circulations on aerosol distributions in autumn over eastern China: observational evidence

Regional heavy pollution events in eastern China (110–122° E, 28–40° N) are causing serious environmental problems. In this study, the relationship between the degree of regional pollution and the patterns of large-scale atmospheric circulation over eastern China in October is investigated using 10-year (2001–2010) Terra/MODIS aerosol optical depth and NCEP reanalysis data by both case study and composite analysis. Eighteen polluted and 10 clean episodes are selected and categorised into six polluted types and three clean types respectively. Generally speaking, weather patterns such as a uniform surface pressure field in eastern China or a steady straight westerly in the middle troposphere, particularly when being at the rear of the anticyclone at 850 hPa, are typically responsible for heavy pollution events. Meanwhile, clean episodes occur when strong southeastward cold air advection prevails below the middle troposphere or air masses are transported from sea to land. Uniform descending motion prevails over the study region, trapping pollutants in the lower atmosphere. Therefore, the value of vertical velocity averaged from 1000 to 100 hPa and divergence of wind field in the lower troposphere are used in this study to quantify the diffusion conditions in each circulation type. The results reveal that it is often a clean episode when both the mean downward motion (larger than 2.56 × 10−2 Pa s−1) and the divergence of low-level winds (larger than 1.79 × 10−2 s−1) are strong. Otherwise, it is more likely to be a polluted episode.
What is the real role of iron oxides in the optical properties of dust aerosols?

Iron oxide compounds constitute an important component of mineral dust aerosols. Several previous studies have shown that these minerals are strong absorbers at visible wavelengths and thus that they play a critical role in the overall climate perturbation caused by dust aerosols. When compiling a database of complex refractive indices of possible mineral species of iron oxides to study their optical properties, we found that uniformly continuous optical constants for a single type of iron oxide in the wavelength range between 0.2 and 50 μm are very scarce, and that the use of hematite to represent all molecular or mineral iron-oxides types is a popular hypothesis. However, the crucial problem is that three continuous data sets for complex refractive indices of hematite are employed in climate models, but there are significant differences between them. Thus, the real role of iron oxides in the optical properties of dust aerosols becomes a key scientific question, and we address this problem by considering different refractive indices, size distributions and more logical weight fractions and mixing states of hematite. Based on the microscopic observations, a semi-external mixture that employs an external mixture between Fe aggregates and other minerals and partly internal mixing between iron oxides and aluminosilicate particles is advised as the optimal approximation. The simulations demonstrate that hematite with a spectral refractive index from Longtin et al. (1988) shows approximately equal absorbing capacity to the mineral illite over the whole wavelength region from 0.55 to 2.5 μm, and only enhances the optical absorption of aerosol mixture at λ < 0.55 μm. Using the data set from Querry (1985) may overestimate the optical absorption of hematite at both visible and near-infrared wavelengths. More laboratory measurements of the refractive index of iron oxides, especially for hematite and goethite in the visible spectrum, should therefore be taken into account when assessing the effect of mineral dust on climate forcing.
Assessment of long-term WRF–CMAQ simulations for understanding direct aerosol effects on radiation "brightening" in the United States

Long-term simulations with the coupled WRF–CMAQ (Weather Research and Forecasting–Community Multi-scale Air Quality) model have been conducted to systematically investigate the changes in anthropogenic emissions of SO2 and NOx over the past 16 years (1995–2010) across the United States (US), their impacts on anthropogenic aerosol loading over North America, and subsequent impacts on regional radiation budgets. In particular, this study attempts to determine the consequences of the changes in tropospheric aerosol burden arising from substantial reductions in emissions of SO2 and NOx associated with control measures under the Clean Air Act (CAA) especially on trends in solar radiation. Extensive analyses conducted by Gan et al. (2014a) utilizing observations (e.g., SURFRAD, CASTNET, IMPROVE, and ARM) over the past 16 years (1995–2010) indicate a shortwave (SW) radiation (both all-sky and clear-sky) "brightening" in the US. The relationship of the radiation brightening trend with decreases in the aerosol burden is less apparent in the western US. One of the main reasons for this is that the emission controls under the CAA were aimed primarily at reducing pollutants in areas violating national air quality standards, most of which were located in the eastern US, while the relatively less populated areas in the western US were less polluted at the beginning of this study period. Comparisons of model results with observations of aerosol optical depth (AOD), aerosol concentration, and radiation demonstrate that the coupled WRF–CMAQ model is capable of replicating the trends well even though it tends to underestimate the AOD. In particular, the sulfate concentration predictions were well matched with the observations. The discrepancies found in the clear-sky diffuse SW radiation are likely due to several factors such as the potential increase of ice particles associated with increasing air traffic, the definition of "clear-sky" in the radiation retrieval methodology, and aerosol semi-direct and/or indirect effects which cannot be readily isolated from the observed data.
The radiative impact of desert dust on orographic rain in the Cévennes–Vivarais area: a case study from HyMeX

The study is focused on Intensive Observation Period (IOP) 14 of the Hydrological Cycle in the Mediterranean Experiment first Special Observing Period (HyMeX SOP 1) that took place from 17 to 19 October 2012 and was dedicated to the study of orographic rain in the Cévennes–Vivarais (CV) target area. During this IOP a dense dust plume originating from northern Africa (the Maghreb and Sahara) was observed to be transported over the Balearic Islands towards the south of France. The plume was characterized by an aerosol optical depth between 0.2 and 0.8 at 550 nm, highly variable in time and space over the western Mediterranean Basin. The impact of this dust plume, the biggest event observed during the 2-month-long HyMeX SOP 1, on the precipitation over the CV area has been analyzed using high-resolution simulations from the convection permitting mesoscale model Meso-NH (mesoscale non-hydrostatic model) validated against measurements obtained from numerous instruments deployed specifically during SOP 1 (ground-based/airborne water vapor and aerosol lidars, airborne microphysics probes) as well as space-borne aerosol products. The 4-day simulation reproduced realistically the temporal and spatial variability (including the vertical distribution) of the dust. The dust radiative impact led to an average 0.6 K heating at the altitude of the dust layer in the CV area (and up to +3 K locally) and an average 100 J kg−1 increase of most unstable convective available potential energy (and up to +900 J kg−1 locally) with respect to a simulation without prescribed dust aerosols. The rainfall amounts and location were only marginally affected by the dust radiative effect, even after 4 days of simulation. The transient nature of this radiative effect in dynamical environments such as those found in the vicinity of heavy precipitation events in the Mediterranean is not sufficient to impact 24 h of accumulated rainfall in the dust simulation.
Impacts of Amazonia biomass burning aerosols assessed from short-range weather forecasts

The direct radiative impacts of biomass burning aerosols (BBA) on meteorology are investigated using short-range forecasts from the Met Office Unified Model (MetUM) over South America during the South American Biomass Burning Analysis (SAMBBA). The impacts are evaluated using a set of three simulations: (i) no aerosols, (ii) with monthly mean aerosol climatologies and (iii) with prognostic aerosols modelled using the Coupled Large-scale Aerosol Simulator for Studies In Climate (CLASSIC) scheme. Comparison with observations show that the prognostic CLASSIC scheme provides the best representation of BBA. The impacts of BBA are quantified over central and southern Amazonia from the first and second day of 2-day forecasts during 14 September–3 October 2012. On average, during the first day of the forecast, including prognostic BBA reduces the clear-sky net radiation at the surface by 15 ± 1 W m−2 and reduces net top-of-atmosphere (TOA) radiation by 8 ± 1 W m−2, with a direct atmospheric warming of 7 ± 1 W m−2. BBA-induced reductions in all-sky radiation are smaller in magnitude: 9.0 ± 1 W m−2 at the surface and 4.0 ± 1 W m−2 at TOA. In this modelling study the BBA therefore exert an overall cooling influence on the Earth–atmosphere system, although some levels of the atmosphere are directly warmed by the absorption of solar radiation. Due to the reduction of net radiative flux at the surface, the mean 2 m air temperature is reduced by around 0.1 ± 0.02 °C. The BBA also cools the boundary layer (BL) but warms air above by around 0.2 °C due to the absorption of shortwave radiation. The overall impact is to reduce the BL depth by around 19 ± 8 m. These differences in heating lead to a more anticyclonic circulation at 700 hPa, with winds changing by around 0.6 m s−1. Inclusion of climatological or prognostic BBA in the MetUM makes a small but significant improvement in forecasts of temperature and relative humidity, but improvements were small compare with model error and the relative increase in forecast skill from the prognostic aerosol simulation over the aerosol climatology was also small. Locally, on a 150 km scale, changes in precipitation reach around 4 mm day−1 due to changes in the location of convection. Over Amazonia, including BBA in the simulation led to fewer rain events that were more intense. This change may be linked to the BBA changing the vertical profile of stability in the lower atmosphere. The localised changes in rainfall tend to average out to give a 5 % (0.06 mm day−1) decrease in total precipitation over the Amazonian region (except on day 2 with prognostic BBA). The change in water budget from BBA is, however, dominated by decreased evapotranspiration from the reduced net surface fluxes (0.2 to 0.3 mm day−1), since this term is larger than the corresponding changes in precipitation and water vapour convergence.
An algorithm for the numerical solution of the multivariate master equation for stochastic coalescence

In cloud modeling studies, the time evolution of droplet size distributions due to collision–coalescence events is usually modeled with the Smoluchowski coagulation equation, also known as the kinetic collection equation (KCE). However, the KCE is a deterministic equation with no stochastic fluctuations or correlations. Therefore, the full stochastic description of cloud droplet growth in a coalescing system must be obtained from the solution of the multivariate master equation, which models the evolution of the state vector for the number of droplets of a given mass. Unfortunately, due to its complexity, only limited results were obtained for certain types of kernels and monodisperse initial conditions. In this work, a novel numerical algorithm for the solution of the multivariate master equation for stochastic coalescence that works for any type of kernels, multivariate initial conditions and small system sizes is introduced. The performance of the method was seen by comparing the numerically calculated particle mass spectrum with analytical solutions of the master equation obtained for the constant and sum kernels. Correlation coefficients were calculated for the turbulent hydrodynamic kernel, and true stochastic averages were compared with numerical solutions of the kinetic collection equation for that case. The results for collection kernels depending on droplet mass demonstrates that the magnitudes of correlations are significant and must be taken into account when modeling the evolution of a finite volume coalescing system.
Modeling particle nucleation and growth over northern California during the 2010 CARES campaign

Accurate representation of the aerosol lifecycle requires adequate modeling of the particle number concentration and size distribution in addition to their mass, which is often the focus of aerosol modeling studies. This paper compares particle number concentrations and size distributions as predicted by three empirical nucleation parameterizations in the Weather Research and Forecast coupled with chemistry (WRF-Chem) regional model using 20 discrete size bins ranging from 1 nm to 10 μm. Two of the parameterizations are based on H2SO4, while one is based on both H2SO4 and organic vapors. Budget diagnostic terms for transport, dry deposition, emissions, condensational growth, nucleation, and coagulation of aerosol particles have been added to the model and are used to analyze the differences in how the new particle formation parameterizations influence the evolving aerosol size distribution. The simulations are evaluated using measurements collected at surface sites and from a research aircraft during the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted in the vicinity of Sacramento, California. While all three parameterizations captured the temporal variation of the size distribution during observed nucleation events as well as the spatial variability in aerosol number, all overestimated by up to a factor of 2.5 the total particle number concentration for particle diameters greater than 10 nm. Using the budget diagnostic terms, we demonstrate that the combined H2SO4 and low-volatility organic vapor parameterization leads to a different diurnal variability of new particle formation and growth to larger sizes compared to the parameterizations based on only H2SO4. At the CARES urban ground site, peak nucleation rates are predicted to occur around 12:00 Pacific (local) standard time (PST) for the H2SO4 parameterizations, whereas the highest rates were predicted at 08:00 and 16:00 PST when low-volatility organic gases are included in the parameterization. This can be explained by higher anthropogenic emissions of organic vapors at these times as well as lower boundary-layer heights that reduce vertical mixing. The higher nucleation rates in the H2SO4-organic parameterization at these times were largely offset by losses due to coagulation. Despite the different budget terms for ultrafine particles, the 10–40 nm diameter particle number concentrations from all three parameterizations increased from 10:00 to 14:00 PST and then decreased later in the afternoon, consistent with changes in the observed size and number distribution. We found that newly formed particles could explain up to 20–30 % of predicted cloud condensation nuclei at 0.5 % supersaturation, depending on location and the specific nucleation parameterization. A sensitivity simulation using 12 discrete size bins ranging from 1 nm to 10 μm diameter gave a reasonable estimate of particle number and size distribution compared to the 20 size bin simulation, while reducing the associated computational cost by ~ 36 %.
Ice water content vertical profiles of high-level clouds: classification and impact on radiative fluxes

In this article, we discuss the shape of ice water content (IWC) vertical profiles in high ice clouds and its effect on their radiative properties, both in short- and in long-wave bands (SW and LW). Based on the analysis of collocated satellite data, we propose a minimal set of primitive shapes (rectangular, isosceles trapezoid, lower and upper triangle), which represents the IWC profiles sufficiently well. About 75 % of all high-level ice clouds (P < 440 hPa) have an ice water path (IWP) smaller than 100 g m−2, with a 10 % smaller contribution from single layer clouds. Most IWC profiles (80 %) can be represented by a rectangular or isosceles trapezoid shape. However, with increasing IWP, the number of lower triangle profiles (IWC rises towards cloud base) increases, reaching up to 40 % for IWP values greater than 300 g m−2. The number of upper triangle profiles (IWC rises towards cloud top) is in general small and decreases with IWP, with the maximum occurrence of 15 % in cases of IWP less than 10 g m−2. We propose a statistical classification of the IWC shapes using IWP as a single parameter. We have estimated the radiative effects of clouds with the same IWP and with different IWC profile shapes for five typical atmospheric scenarios and over a broad range of IWP, cloud height, cloud vertical extent, and effective ice crystal diameter (De). We explain changes in outgoing LW fluxes at the top of the atmosphere (TOA) by the cloud thermal radiance while differences in TOA SW fluxes relate to the De vertical profile within the cloud. Absolute differences in net TOA and surface fluxes associated with these parameterized IWC profiles instead of assuming constant IWC profiles are in general of the order of 1–2 W m−2: they are negligible for clouds with IWP < 30 g m−2, but may reach 2 W m−2 for clouds with IWP > 300 W m−2.