Abstract Bulk aerosol composition and aerosol size distributions measured aboard the DC‐8 aircraft during the Deep Convective Clouds and Chemistry Experiment mission in May/June 2012 were used to investigate the transport of mineral dust through nine storms encountered over Colorado and Oklahoma. Measurements made at low altitudes (<5 km mean sea level (MSL)) in the storm inflow region were compared to those made in cirrus anvils (altitude > 9 km MSL). Storm mean outflow Ca 2+ mass concentrations and total coarse (1 µm < diameter < 5 µm) aerosol volume ( V c ) were comparable to mean inflow values as demonstrated by average outflow/inflow ratios greater than 0.5. A positive relationship between Ca 2+ , V c , ice water content, and large (diameter > 50 µm) ice particle number concentrations was not evident; thus, the influence of ice shatter on these measurements was assumed small. Mean inflow aerosol number concentrations calculated over a diameter range (0.5 µm < diameter < 5.0 µm) relevant for proxy ice nuclei ( N PIN ) were ~15–300 times higher than ice particle concentrations for all storms. Ratios of predicted interstitial N PIN (calculated as the difference between inflow N PIN and ice particle concentrations) and inflow N PIN were consistent with those calculated for Ca 2+ and V c and indicated that on average less than 10% of the ingested N PIN were activated as ice nuclei during anvil formation. Deep convection may therefore represent an efficient transport mechanism for dust to the upper troposphere where these particles can function as ice nuclei cirrus forming in situ.
Abstract. To recover the actual responsivity for the Ultraviolet Multi-Filter Rotating Shadowband Radiometer (UV-MFRSR), the complex (e.g., unstable, noisy, and with gaps) time series of its in situ calibration factors (V0) need to be smoothed. Many smoothing techniques require accurate input uncertainty of the time series. A new method is proposed to estimate the dynamic input uncertainty by examining overall variation and subgroup means within a moving time window. Using this calculated dynamic input uncertainty within Gaussian process (GP) regression provides the mean and uncertainty functions of the time series. This proposed GP solution was first applied to a synthetic signal and showed significantly smaller RMSEs than a Gaussian process regression performed with constant values of input uncertainty and the mean function. GP was then applied to three UV-MFRSR V0 time series at three ground sites. The method appropriately accounted for variation in slopes, noises, and gaps at all sites. The validation results at the three test sites (i.e., HI02 at Mauna Loa, Hawaii; IL02 at Bondville, Illinois; and OK02 at Billings, Oklahoma) demonstrated that the agreement among aerosol optical depths (AODs) at the 368 nm channel calculated using V0 determined by the GP mean function and the equivalent AERONET AODs were consistently better than those calculated using V0 from standard techniques (e.g., moving average). For example, the average AOD biases of the GP method (0.0036 and 0.0032) are much lower than those of the moving average method (0.0119 and 0.0119) at IL02 and OK02, respectively. The GP method's absolute differences between UV-MFRSR and AERONET AOD values are approximately 4.5 %, 21.6 %, and 16.0 % lower than those of the moving average method at HI02, IL02, and OK02, respectively. The improved accuracy of in situ UVMRP V0 values suggests the GP solution is a robust technique for accurate analysis of complex time series and may be applicable to other fields.
Abstract. Urban air pollution absorbs and scatters solar ultraviolet (UV) radiation, and thus has a potentially large effect on tropospheric photochemical rates. We present the first detailed comparison between UV actinic fluxes (AF) measured in highly polluted conditions and simulated with the Tropospheric Ultraviolet-Visible (TUV) model. Measurements were made during the MILAGRO campaign near Mexico City in March 2006, at a ground-based station near Mexico City (the T1 supersite) and from the NSF/NCAR C-130 aircraft. At the surface, measured AF values are typically smaller than the model by up to 25% in the morning, 10% at noon, and 40% in the afternoon, for pollution-free and cloud-free conditions. When measurements of PBL height, NO2 concentration and aerosols optical properties are included in the model, the agreement improves to within ±10% in the morning and afternoon, and ±3% at noon. Based on daily averages, aerosols account for 67% and NO2 for 25% of AF reductions observed at the surface. Several overpasses from the C-130 aircraft provided the opportunity to examine the AF perturbations aloft, and also show better agreement with the model when aerosol and NO2 effects are included above and below the flight altitude. TUV model simulations show that the vertical structure of the actinic flux is sensitive to the choice of the aerosol single scattering albedo (SSA) at UV wavelengths. Typically, aerosols enhance AF above the PBL and reduce AF near the surface. However, for highly scattering aerosols (SSA > 0.95), enhancements can penetrate well into the PBL, while for strongly absorbing aerosols (SSA < 0.6) reductions in AF are computed in the free troposphere as well as in the PBL. Additional measurements of the SSA at these wavelengths are needed to better constrain the effect of aerosols on the vertical structure of the AF.
Abstract East Asia is the strongest global source region for anthropogenic black carbon (BC), the most important light‐absorbing aerosol contributing to direct radiative climate forcing. To provide extended observational constraints on regional BC distributions and impacts, in situ measurements of BC were obtained with a single particle soot photometer during the May/June 2016 Korean‐United States Air Quality aircraft campaign (KORUS‐AQ) in South Korea. Unique chemical tracer relationships were associated with BC sourced from different regions. The extent and variability in vertical BC mass burden for 48 profiles over a single site near Seoul were investigated using back trajectory and chemical tracer analysis. Meteorologically driven changes in transport influenced the relative importance of different source regions, impacting observed BC loadings at all altitudes. Internal mixing and size distributions of BC further demonstrated dependence on source region: BC attributed to China had a larger mass median diameter (180 ± 13 nm) than BC attributed to South Korea (152 ± 25 nm), and BC associated with long‐range transport was less thickly coated (60 ± 4 nm) than that sourced from South Korea (75 ± 16 nm). The column BC direct radiative effect at the top of the atmosphere was estimated to be W/m 2 , with average values for different meteorological periods varying by a factor of 2 due to changes in the BC vertical profile. During the campaign, BC sourced from South Korea (≤ 31%), China (22%), and Russia (14%) were the most significant single‐region contributors to the column direct radiative effect.
Abstract. KORUS-AQ was an international cooperative air quality field study in South Korea that measured local and remote sources of air pollution affecting the Korean Peninsula during May–June 2016. Some of the largest aerosol mass concentrations were measured during a Chinese haze transport event (24 May). Air quality forecasts using the WRF-Chem model with aerosol optical depth (AOD) data assimilation captured AOD during this pollution episode but overpredicted surface particulate matter concentrations in South Korea, especially PM2.5, often by a factor of 2 or larger. Analysis revealed multiple sources of model deficiency related to the calculation of optical properties from aerosol mass that explain these discrepancies. Using in situ observations of aerosol size and composition as inputs to the optical properties calculations showed that using a low-resolution size bin representation (four bins) underestimates the efficiency with which aerosols scatter and absorb light (mass extinction efficiency). Besides using finer-resolution size bins (8–16 bins), it was also necessary to increase the refractive indices and hygroscopicity of select aerosol species within the range of values reported in the literature to achieve better consistency with measured values of the mass extinction efficiency (6.7 m2 g−1 observed average) and light-scattering enhancement factor (f(RH)) due to aerosol hygroscopic growth (2.2 observed average). Furthermore, an evaluation of the optical properties obtained using modeled aerosol properties revealed the inability of sectional and modal aerosol representations in WRF-Chem to properly reproduce the observed size distribution, with the models displaying a much wider accumulation mode. Other model deficiencies included an underestimate of organic aerosol density (1.0 g cm−3 in the model vs. observed average of 1.5 g cm−3) and an overprediction of the fractional contribution of submicron inorganic aerosols other than sulfate, ammonium, nitrate, chloride, and sodium corresponding to mostly dust (17 %–28 % modeled vs. 12 % estimated from observations). These results illustrate the complexity of achieving an accurate model representation of optical properties and provide potential solutions that are relevant to multiple disciplines and applications such as air quality forecasts, health impact assessments, climate projections, solar power forecasts, and aerosol data assimilation.
