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Statistical properties of aerosol-cloud-precipitation interactions in South America

Given the complex interaction between aerosol, cloud, and atmospheric properties, it is difficult to extract their individual effects to observed rainfall amount. This research uses principle component analysis (PCA) that combines Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol and cloud products, NCEP Reanalysis atmospheric products, and rainrate estimates from the Tropical Rainfall Measuring Mission (TRMM) precipitation radar (PR) to assess if aerosols affect warm rain processes. Data collected during September 2006 over the Amazon basin in South America during the biomass-burning season are used. The goal of this research is to combine these observations into a smaller number of variables through PCA with each new variable having a unique physical interpretation. In particular, we are concerned with PC variables whose weightings include aerosol optical thickness (AOT), as these may be an indicator of aerosol indirect effects. If they are indeed occurring, then PC values that include AOT should change as a function of rainrate. To emphasize the advantage of PCA, changes in aerosol, cloud, and atmospheric observations are compared to rainrate. Comparing no-rain, rain, and heavy rain only (>5 mm h−1) samples, we find that cloud thicknesses, humidity, and upward motion are all greater during rain and heavy rain conditions. However, no statistically significant difference in AOT exists between each sample, indicating that atmospheric conditions are more important to rainfall than aerosol concentrations as expected. If aerosols are affecting warm process clouds, it would be expected that stratiform precipitation would decrease as a function increasing aerosol concentration through either Twomey and/or semi-direct effects. PCA extracts the latter signal in a variable labeled PC2, which explains 15% of the total variance and is second in importance the variable (PC1) containing the broad atmospheric conditions. PC2 contains weightings showing that AOT is inversely proportional to low-level humidity and cloud optical thickness. Increasing AOT is also positively correlated with increasing low-level instability due to aerosol absorption. The nature of these weightings is strongly suggestive that PC2 is an indicator of the semi-direct effect with larger values associated with lower rainfall rates. PC weightings consistent with the Twomey effect (an anti-correlation between AOT and cloud droplet effective radius) are only present in higher order PC variables that explain less than 1% of the total variance, and do not vary significantly as a function of rainrate. If the Twomey effect is occurring, it is highly non-linear and/or being overshadowed by other processes. Using the raw variables alone, these determinations could not be made; thus, we are able to show the advantage of using advanced statistical techniques such as PCA for analysis of aerosols impacts on precipitation in South America.
Measured and predicted aerosol light scattering enhancement factors at the high alpine site Jungfraujoch

Ambient relative humidity (RH) determines the water content of atmospheric aerosol particles and thus has an important influence on the amount of visible light scattered by particles. The RH dependence of the particle light scattering coefficient (σsp) is therefore an important variable for climate forcing calculations. We used a humidification system for a nephelometer which allows for the measurement of σsp at a defined RH in the range of 20–95%. In this paper we present measurements of light scattering enhancement factors f(RH)=σsp(RH)/σsp(dry) from a 1-month campaign (May 2008) at the high alpine site Jungfraujoch (3580 m a.s.l.), Switzerland. Measurements at the Jungfraujoch are representative for the lower free troposphere above Central Europe. For this aerosol type hardly any information about the f(RH) is available so far. At this site, f(RH=85%) varied between 1.2 and 3.3. Measured f(RH) agreed well with f(RH) calculated with Mie theory using measurements of the size distribution, chemical composition and hygroscopic diameter growth factors as input. Good f(RH) predictions at RH<85% were also obtained with a simplified model, which uses the Ångström exponent of σsp(dry) as input. RH influences further intensive optical aerosol properties. The backscatter fraction decreased by about 30% from 0.128 to 0.089, and the single scattering albedo increased on average by 0.05 at 85% RH compared to dry conditions. These changes in σsp, backscatter fraction and single scattering albedo have a distinct impact on the radiative forcing of the Jungfraujoch aerosol.
Depositional ice nucleation on solid ammonium sulfate and glutaric acid particles

Heterogeneous ice nucleation on solid ammonium sulfate and glutaric acid particles was studied using optical microscopy and Raman spectroscopy. Optical microscopy was used to detect selective nucleation events as water vapor was slowly introduced into an environmental sample cell. Particles that nucleated ice were dried via sublimation and examined in detail using Raman spectroscopy. Depositional ice nucleation is highly selective and occurred preferentially on just a few ammonium sulfate and glutaric acid particles in each sample. For freezing temperatures between 214 K and 235 K an average ice saturation ratio of S = 1.10±0.07 for solid ammonium sulfate was observed. Over the same temperature range, S values observed for ice nucleation on glutaric acid particles increased from 1.2 at 235 K to 1.6 at 218 K. Experiments with externally mixed particles further show that ammonium sulfate is a more potent ice nucleus than glutaric acid. Our results suggest that heterogeneous nucleation on ammonium sulfate may be an important pathway for atmospheric ice nucleation and cirrus cloud formation when solid ammonium sulfate aerosol particles are available for ice formation. This pathway for ice formation may be particularly significant near the tropical tropopause region where sulfates are abundant and other species known to be good ice nuclei are depleted.
Aerosol effects on deep convective clouds: impact of changes in aerosol size distribution and aerosol activation parameterization

A cloud-resolving model including explicit aerosol physics and chemistry is used to study the impact of aerosols on deep convective strength. More specifically, by conducting six sensitivity series we examine how the complexity of the aerosol model, the size of the aerosols and the aerosol activation parameterization influence the aerosol-induced deep convective cloud sensitivity. Only aerosol effects on liquid droplet formation are considered. We find that an increased aerosol concentration generally results in stronger convection, which for the simulated case is in agreement with the conceptual model presented by Rosenfeld et al. (2008). However, there are two sensitivity series that do not display a monotonic increase in updraft velocity with increasing aerosol concentration. These exceptions illustrate the need to: 1) account for changes in evaporation processes and subsequent cooling when assessing aerosol effects on deep convective strength, 2) better understand graupel impaction scavenging of aerosols which may limit the number of CCN at a critical stage of cloud development and thereby dampen the convection, 3) increase our knowledge of aerosol recycling due to evaporation of cloud droplets. Furthermore, we find a significant difference in the aerosol-induced deep convective cloud sensitivity when using different complexities of the aerosol model and different aerosol activation parameterizations. For the simulated case, a 100% increase in aerosol concentration results in a difference in average updraft between the various sensitivity series which is as large as the average updraft increase itself. The model simulations also show that the change in graupel and rain formation is not necessarily directly proportional to the change in updraft velocity. For example, several of the sensitivity series display a decrease of the rain amount at the lowest model level with increasing updraft velocity. Finally, an increased number of aerosols in the Aitken mode (here defined by 23 nm≤d≤100.0 nm) may result in a larger impact on the convective strength compared to an increased number of aerosols in the accumulation mode (here defined by 100 nm≤d≤900.0 nm). When accumulation mode aerosols are activated and grow at the beginning of the cloud cycle, the supersaturation near the cloud base is lowered which to some extent limits further aerosol activation.
On the transitions in marine boundary layer cloudiness

Satellite observations and meteorological reanalysis are used to examine the transition from unbroken sheets of stratocumulus to fields of scattered cumulus, and the processes controlling them, in four subtropical oceans. A Lagrangian analysis suggests that both the transition, defined as the temporal evolution in cloudiness, and the processes driving the transition, are quite similar among the subtropical oceans. The increase in sea surface temperature and the associated decrease in lower tropospheric stability appear to play a far more important role in cloud evolution than other factors including changes in large scale divergence and upper tropospheric humidity. During the summer months, the transitions in marine boundary layer cloudiness appear so systematically that their characteristics obtained by documenting the flow of thousands of individual air masses are well reproduced by the mean (or climatological) fields of the different data sets. This highlights interesting opportunities for future observational and modeling studies of these transitions.
Chemical evolution of volatile organic compounds in the outflow of the Mexico City Metropolitan area

The volatile organic compound (VOC) distribution in the Mexico City Metropolitan Area (MCMA) and its evolution as it is uplifted and transported out of the MCMA basin was studied during the 2006 MILAGRO/MIRAGE-Mex field campaign. The results show that in the morning hours in the city center, the VOC distribution is dominated by non-methane hydrocarbons (NMHCs) but with a substantial contribution from oxygenated volatile organic compounds (OVOCs), predominantly from primary emissions. Alkanes account for a large part of the NMHC distribution in terms of mixing ratios. In terms of reactivity, NMHCs also dominate overall, especially in the morning hours. However, in the afternoon, as the boundary layer lifts and air is mixed and aged within the basin, the distribution changes as secondary products are formed. The WRF-Chem (Weather Research and Forecasting with Chemistry) model and MOZART (Model for Ozone and Related chemical Tracers) were able to approximate the observed MCMA daytime patterns and absolute values of the VOC OH reactivity. The MOZART model is also in agreement with observations showing that NMHCs dominate the reactivity distribution except in the afternoon hours. The WRF-Chem and MOZART models showed higher reactivity than the experimental data during the nighttime cycle, perhaps indicating problems with the modeled nighttime boundary layer height. A northeast transport event was studied in which air originating in the MCMA was intercepted aloft with the Department of Energy (DOE) G1 on 18 March and downwind with the National Center for Atmospheric Research (NCAR) C130 one day later on 19 March. A number of identical species measured aboard each aircraft gave insight into the chemical evolution of the plume as it aged and was transported as far as 1000 km downwind; ozone was shown to be photochemically produced in the plume. The WRF-Chem and MOZART models were used to examine the spatial extent and temporal evolution of the plume and to help interpret the observed OH reactivity. The model results generally showed good agreement with experimental results for the total VOC OH reactivity downwind and gave insight into the distributions of VOC chemical classes. A box model with detailed gas phase chemistry (NCAR Master Mechanism), initialized with concentrations observed at one of the ground sites in the MCMA, was used to examine the expected evolution of specific VOCs over a 1–2 day period. The models clearly supported the experimental evidence for NMHC oxidation leading to the formation of OVOCs downwind, which then become the primary fuel for ozone production far away from the MCMA.
Estimates of biomass burning emissions in tropical Asia based on satellite-derived data

Biomass burning in tropical Asia emits large amounts of trace gases and particulate matter into the atmosphere, which has significant implications for atmospheric chemistry and climatic change. In this study, emissions from open biomass burning over tropical Asia were evaluated during seven fire years from 2000 to 2006 (1 March 2000–31 February 2007). The size of the burned areas was estimated from newly published 1-km L3JRC and 500-m MODIS burned area products (MCD45A1). Available fuel loads and emission factors were assigned to each vegetation type in a GlobCover characterisation map, and fuel moisture content was taken into account when calculating combustion factors. Over the whole period, both burned areas and fire emissions showed clear spatial and seasonal variations. The size of the L3JRC burned areas ranged from 36 031 km2 in fire year 2005 to 52 303 km2 in 2001, and the MCD45A1 burned areas ranged from 54 790 km2 in fire year 2001 to 148 967 km2 in 2004. Comparisons of L3JRC and MCD45A1 burned areas using ground-based measurements and other satellite data were made in several major burning regions, and the results suggest that MCD45A1 generally performed better than L3JRC, although with a certain degree of underestimation in forest areas. The average annual L3JRC-based emissions were 123 (102–152), 12 (9–15), 1.0 (0.7–1.3), 1.9 (1.4–2.6), 0.11 (0.09–0.12), 0.89 (0.63–1.21), 0.043 (0.036–0.053), 0.021 (0.021–0.023), 0.41 (0.34–0.52), 3.4 (2.6–4.3), and 3.6 (2.8–4.7) Tg yr−1 for CO2, CO, CH4, NMHCs, NOx, NH3, SO2, BC, OC, PM2.5, and PM10, respectively, whereas MCD45A1-based emissions were 122 (108–144), 9.3 (7.7–11.7), 0.63 (0.46–0.86), 1.1 (0.8–1.6), 0.11 (0.10–0.13), 0.54 (0.38–0.76), 0.043 (0.038–0.051), 0.033 (0.032–0.037), 0.39 (0.34–0.47), 3.0 (2.6–3.7), and 3.3 (2.8–4.0) Tg yr−1. Forest burning was identified as the major source of the fire emissions due to its high carbon density. Although agricultural burning was the second highest contributor, it is possible that some crop residue combustion was missed by satellite observations. This possibility is supported by comparisons with previously published data, and this result may be due to the small size of the field crop residue burning. Fire emissions were mainly concentrated in Indonesia, India, Myanmar, and Cambodia. Furthermore, the peak in the size of the burned area was generally found in the early fire season, whereas the maximum fire emissions often occurred in the late fire season.
Observations of OM/OC and specific attenuation coefficients (SAC) in ambient fine PM at a rural site in central Ontario, Canada

Ambient particulate matter (PM) samples were collected on quartz filters at a rural site in central Ontario during an intensive study in 2007. The concentrations of organic carbon (OC), pyrolysis organic carbon (POC), and elemental carbon (EC) were determined by thermal analysis. The concentrations are compared to the organic aerosol mass concentration (OM) measured with an Aerodyne C-ToF Aerosol Mass Spectrometer (AMS) and to the particle absorption coefficient (basp) obtained from a Radiance Research Particle Soot Absorption Photometer (PSAP). The total organic mass to organic carbon ratios (OM/OC) and specific attenuation coefficients (SAC=basp/EC) are derived. Proportionality of the POC mass with the oxygen mass in the aerosols estimated from the AMS offers a potential means to estimate OM/OC from thermal measurements only. The mean SAC for the study is 3.8±0.3 m2 g−1. It is found that the SAC is independent of or decrease with increasing particle mass loading, depending on whether or not the data are separated between aerosols dominated by more recent anthropogenic input and aerosols dominated by longer residence time or biogenic components. There is no evidence to support an enhancement of light absorption by the condensation of secondary material to particles, suggesting that present model simulations built on such an assumption may overestimate atmospheric warming by BC.
Formaldehyde and its relation to CO, PAN, and SO2 in the Houston-Galveston airshed

The Houston-Galveston Airshed (HGA) is one of the major metropolitan areas in the US that is classified as a nonattainment area of federal ozone standards. Formaldehyde (HCHO) is a key species in understanding ozone related air pollution; some of the highest HCHO concentrations in North America have been reported for the HGA. We report on HCHO measurements in the HGA from summer 2006. Among several sites, maximum HCHO mixing ratios were observed in the Houston Ship Channel (HSC), a region with a very high density of industrial/petrochemical operations. HCHO levels at the Moody Tower (MT) site close to downtown were dependent on the wind direction: southerly maritime winds brought in background levels (0.5–1 ppbv) while trajectories originating in the HSC resulted in high HCHO (up to 31.5 ppbv). Based on the best multiparametric linear regression model fit, the HCHO levels at the MT site can be accounted for as follows: 38.5±12.3% from primary vehicular emissions (using CO as an index of vehicular emission), 24.1±17.7% formed photochemically (using peroxyacetic nitric anhydride (PAN) as an index of photochemical activity) and 8.9±11.2% from industrial emissions (using SO2 as an index of industrial emissions). The balance 28.5±12.7% constituted the residual which cannot be easily ascribed to the above categories and/or which is transported into the HGA. The CO related HCHO fraction is dominant during the morning rush hour (06:00–09:00 h, all times are given in CDT); on a carbon basis, HCHO emissions are up to 0.7% of the CO emissions. The SO2 related HCHO fraction is significant between 09:00–12:00 h. After 12:00 h HCHO is largely formed through secondary processes. The HCHO/PAN ratios are dependent on the SO2 levels. The SO2 related HCHO fraction at the downtown site originates in the ship channel. Aside from traffic-related primary HCHO emissions, HCHO of industrial origin serves as an appreciable source for OH in the morning.
Isotope modeling of nitric acid formation in the atmosphere using ISO-RACM: testing the importance of NO oxidation, heterogeneous reactions, and trace gas chemistry

Here we present ISO-RACM, an isotope mass balance model that utilizes the Regional Atmospheric Chemistry Mechanism to predict Δ17O values in atmospheric nitrate. A large number of simulations were carried out that varied atmospheric parameters that are important in altering the magnitude and range of Δ17O values generated in photochemically produce nitrate. These parameters included temperature, relative humidity, actinic flux, aerosol surface area and chemical speciation, and three different N2O5 uptake parameterizations. Trace gas mixing ratios were also varied including CH4, CO, NOx, O3, volatile organic compounds and biogenic organic compounds. The model predicts that there are seasonal, latitudinal and diurnal variations in Δ17O values due to changes in actinic flux with lower values corresponding to higher actinic fluxes. There was also a minor positive correlation between higher Δ17O values and increased temperature. There were distinct differences in Δ17O depending on which N2O5 parameterization was used, mostly the result of changing relative humidity being a factor in two of the parameterization schemes. Changing CO and CH4 mixing ratios had negligible impact on Δ17O values but significant variation in magnitude and range were predicted with NOx, O3, and organic loading. High NOx and O3 generated high Δ17O with a narrow (10 &permil;) range, while high organics led to low Δ17O values and a wider range of possible values. Implications for using Δ17O to evaluate NOx-NOy chemistry and aerosol formation processes are discussed, as is needed future research.