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Emissions from biomass burning in the Yucatan

In March 2006 two instrumented aircraft made the first detailed field measurements of biomass burning (BB) emissions in the Northern Hemisphere tropics as part of the MILAGRO project. The aircraft were the National Center for Atmospheric Research C-130 and a University of Montana/US Forest Service Twin Otter. The initial emissions of up to 49 trace gas or particle species were measured from 20 deforestation and crop residue fires on the Yucatan peninsula. This included two trace gases useful as indicators of BB (HCN and acetonitrile) and several rarely, or never before, measured species: OH, peroxyacetic acid, propanoic acid, hydrogen peroxide, methane sulfonic acid, and sulfuric acid. Crop residue fires emitted more organic acids and ammonia than deforestation fires, but the emissions from the main fire types were otherwise fairly similar. The Yucatan fires emitted unusually high amounts of SO2 and particle chloride, likely due to a strong marine influence on this peninsula. As smoke from one fire aged, the ratio ΔO3/ΔCO increased to ~15% in <~1 h similar to the fast net production of O3 in BB plumes observed earlier in Africa. The rapid change in O3 occurs at a finer spatial scale than is employed in global models and is also faster than predicted by micro-scale models. Fast increases in PAN, H2O2, and two organic acids were also observed. The amount of secondary organic acid is larger than the amount of known precursors. Rapid secondary formation of organic and inorganic aerosol was observed with the ratio ΔPM2.5/ΔCO more than doubling in ~1.4±0.7 h. The OH measurements revealed high initial levels (>1×107 molecules/cm3) that were likely caused in part by high initial HONO (~10% of NOy). Thus, more research is needed to understand critical post emission processes for the second-largest trace gas source on Earth. It is estimated that ~44 Tg of biomass burned in the Yucatan in the spring of 2006. Mexican BB (including Yucatan BB) and urban emissions from the Mexico City area can both influence the March-May air quality in much of Mexico and the US.
Retrieval of aerosol single scattering albedo at ultraviolet wavelengths at the T1 site during MILAGRO

Surface measurements of direct and diffuse voltages at UV wavelengths were made at the T1 site during the MILAGRO (Megacity Initiative: Local and Global Research Observations) field campaign in March 2006, using a multifilter rotating shadowband radiometer (UV-MFRSR). We used the MFRSR data, together with measurements from a co-located CIMEL Sun photometer at the site operating as part of the AERONET network, to deduce aerosol single scattering albedo (ω) at 368 and 332 nm for four cloud-free days during the study. Our retrievals suggest that T1 aerosols with aerosol extinction optical depth τ368>0.1 that are influenced by Mexico City emissions, blowing dust, and biomass burning, are characterized by low ω368=0.73–0.85 and ω332=0.70–0.86, with small or no spectral variation of ω between 368 and 332 nm. Our findings are consistent with other published estimates of ω for Mexico City aerosols, including those that suggest that the absorption attributable to these aerosols is enhanced at UV wavelengths relative to visible wavelengths. We also demonstrate, via sensitivity tests, the importance of accurate τ and surface albedo measurements in ω retrievals at UV wavelengths.
A statistical analysis of the influence of deep convection on water vapor variability in the tropical upper troposphere

The factors that control the influence of deep convective detrainment on water vapor in the tropical upper troposphere are examined using observations from multiple satellites in conjunction with a trajectory model. Deep convection is confirmed to act primarily as a moisture source to the upper troposphere, modulated by the ambient relative humidity (RH). Convective detrainment provides strong moistening at low RH and offsets drying due to subsidence across a wide range of RH. Strong day-to-day moistening and drying takes place most frequently in relatively dry transition zones, where between 0.01% and 0.1% of Tropical Rainfall Measuring Mission Precipitation Radar observations indicate active convection. Many of these strong moistening events in the tropics can be directly attributed to detrainment from recent tropical convection, while others in the subtropics appear to be related to stratosphere-troposphere exchange. The temporal and spatial limits of the convective source are estimated to be about 36–48 h and 600–1500 km, respectively, consistent with the lifetimes of detrainment cirrus clouds. Larger amounts of detrained ice are associated with enhanced upper tropospheric moistening in both absolute and relative terms. In particular, an increase in ice water content of approximately 400% corresponds to a 10–90% increase in the likelihood of moistening and a 30–50% increase in the magnitude of moistening.
The shortwave radiative forcing bias of liquid and ice clouds from MODIS observations

We present an assessment of the plane-parallel bias of the shortwave cloud radiative forcing (SWCRF) of liquid and ice clouds at 1 deg scales using global MODIS (Terra and Aqua) cloud optical property retrievals for four months of the year 2005 representative of the meteorological seasons. The (negative) bias is estimated as the difference of SWCRF calculated using the Plane-Parallel Homogeneous (PPH) approximation and the Independent Column Approximation (ICA). PPH calculations use MODIS-derived gridpoint means while ICA calculations use distributions of cloud optical thickness and effective radius. Assisted by a broadband solar radiative transfer algorithm, we find that the absolute value of global SWCRF bias of liquid clouds at the top of the atmosphere is about 6 W m−2 for MODIS overpass times while the SWCRF bias for ice clouds is smaller in absolute terms by about 0.7 W m−2, but with stronger spatial variability. If effective radius variability is neglected and only optical thickness horizontal variations are accounted for, the absolute SWCRF biases increase by about 0.3–0.4 W m−2 on average. Marine clouds of both phases exhibit greater (more negative) SWCRF biases than continental clouds. Finally, morning (Terra)–afternoon (Aqua) differences in SWCRF bias are much more pronounced for ice clouds, up to about 15% (Aqua producing stronger negative bias) on global scales, with virtually all contribution to the difference coming from land areas. The substantial magnitude of the global SWCRF bias, which for clouds of both phases is collectively about 4 W m−2 for diurnal averages, should be considered a strong motivation for global climate modelers to accelerate efforts linking cloud schemes capable of subgrid condensate variability with appropriate radiative transfer schemes.
Inverse modeling and mapping US air quality influences of inorganic PM2.5 precursor emissions using the adjoint of GEOS-Chem

Influences of specific sources of inorganic PM2.5 on peak and ambient aerosol concentrations in the US are evaluated using a combination of inverse modeling and sensitivity analysis. First, sulfate and nitrate aerosol measurements from the IMPROVE network are assimilated using the four-dimensional variational (4D-Var) method into the GEOS-Chem chemical transport model in order to constrain emissions estimates in four separate month-long inversions (one per season). Of the precursor emissions, these observations primarily constrain ammonia (NH3). While the net result is a decrease in estimated US~NH3 emissions relative to the original inventory, there is considerable variability in adjustments made to NH3 emissions in different locations, seasons and source sectors, such as focused decreases in the midwest during July, broad decreases throughout the US~in January, increases in eastern coastal areas in April, and an effective redistribution of emissions from natural to anthropogenic sources. Implementing these constrained emissions, the adjoint model is applied to quantify the influences of emissions on representative PM2.5 air quality metrics within the US. The resulting sensitivity maps display a wide range of spatial, sectoral and seasonal variability in the susceptibility of the air quality metrics to absolute emissions changes and the effectiveness of incremental emissions controls of specific source sectors. NH3 emissions near sources of sulfur oxides (SOx) are estimated to most influence peak inorganic PM2.5 levels in the East; thus, the most effective controls of NH3 emissions are often disjoint from locations of peak NH3 emissions. Controls of emissions from industrial sectors of SOx and NOx are estimated to be more effective than surface emissions, and changes to NH3 emissions in regions dominated by natural sources are disproportionately more effective than regions dominated by anthropogenic sources. NOx controls are most effective in northern states in October; in January, SOx controls may be counterproductive. When considering ambient inorganic PM2.5 concentrations, intercontinental influences are small, though transboundary influences within North America are significant, with SOx emissions from surface sources in Mexico contributing almost a fourth of the total influence from this sector.
Recent trends in atmospheric methyl bromide: analysis of post-Montreal Protocol variability

The atmospheric methyl bromide (CH3Br) burden has declined in recent years, in response to the phaseout of agricultural and structural fumigation consumption under the amendments to the Montreal Protocol. The timing and magnitude of this decrease represents an opportunity to examine our current understanding of atmospheric CH3Br and its budget, response to the phaseout, and response to interannual variability in biomass burning and global OH. In this study, simulations obtained from a time-dependent global model of atmospheric CH3Br emissions and uptake are compared to observations from the NOAA flask network. The model includes a detailed gridded ocean model coupled to a time-dependant atmospheric 2-box model. The phaseout of CH3Br production for agricultural uses began in 1998, concurrent with the pulse in biomass burning associated with the 1998 El Niño. The combined effects of three factors (biomass burning, global OH, and anthropogenic phaseout) appear to explain most of the observed atmospheric methyl bromide variability over the 1997–2008 period. The global budget remains imbalanced, with a large missing source indicated. The missing source does not exhibit a systematic decline during the phaseout period, and therefore, is not the result of significantly underestimating non-QPS agricultural CH3Br emissions. The model results suggest that the oceans should be less undersaturated than before the phaseout began.
Comparison of analytical methods for Humic Like Substances (HULIS) measurements in atmospheric particles

Humic-Like Substances (HULIS) are a major contributor to the organic carbon in atmospheric aerosol. It would be necessary to standardize an analytical method that could be easily and routinely used for HULIS measurements. We present one of the first comparisons of two of the main methods in use to extract HULIS, using I) a weak anion exchanger (DEAE) and II) the combination of two separation steps, one according to polarity (on C18) and the second according to acidity (with a strong anion exchanger SAX). The quantification is performed with a TOC analyzer, complemented by an investigation of the chemical structure of the extracted fractions by UV-Visible spectroscopy. The analytical performances of each method are determined and compared for humic substances standards. These methods are further applied to determine the water extractable HULIS (HULISWS) and the 0.1 M NaOH alkaline extractable HULIS (HULIS T) in atmospheric aerosol collected in an Alpine Valley during winter time. This comparison, although on a limited batch of samples shows that the simpler DEAE isolation procedure leads to higher recoveries and better reproducibility than the C18-SAX procedure, and might therefore be preferable.
Parameterizing the competition between homogeneous and heterogeneous freezing in ice cloud formation – polydisperse ice nuclei

This study presents a comprehensive ice cloud formation parameterization that computes the ice crystal number, size distribution, and maximum supersaturation from precursor aerosol and ice nuclei. The parameterization provides an analytical solution of the cloud parcel model equations and accounts for the competition effects between homogeneous and heterogeneous freezing, and, between heterogeneous freezing in different modes. The diversity of heterogeneous nuclei is described through a nucleation spectrum function which is allowed to follow any form (i.e., derived from classical nucleation theory or from observations). The parameterization reproduces the predictions of a detailed numerical parcel model over a wide range of conditions, and several expressions for the nucleation spectrum. The average error in ice crystal number concentration was −2.0±8.5% for conditions of pure heterogeneous freezing, and, 4.7±21% when both homogeneous and heterogeneous freezing were active. The formulation presented is fast and free from requirements of numerical integration.
Measurements of particle masses of inorganic salt particles for calibration of cloud condensation nuclei counters

We measured the mobility equivalent critical dry diameter for cloud condensation nuclei (CCN) activation (dc_me) and the particle mass of size-selected (NH4)2SO4 and NaCl particles to calibrate a CCN counter (CCNC) precisely. The CCNC was operated downstream of a differential mobility analyzer (DMA) for the measurement of dc_me. The particle mass was measured using an aerosol particle mass analyzer (APM) operated downstream of the DMA. The measurement of particle mass was conducted for 50–150-nm particles. Effective densities (ρeff) of (NH4)2SO4 particles were 1.67–1.75 g cm−3, which correspond to dynamic shape factors (χ) of 1.01–1.04. This shows that (NH4)2SO4 particles are not completely spherical. In the case of NaCl particles, ρeff was 1.75–1.99 g cm−3 and χ was 1.05–1.14, demonstrating that the particle shape was non-spherical. Using these experimental data, the volume equivalent critical dry diameter (dc_ve) was calculated, and it was used as an input parameter for calculations of critical supersaturation (S). Several thermodynamics models were used for the calculation of water activity. When the Pitzer model was employed for the calculations, the critical S calculated for (NH4)2SO4 and NaCl agreed to well within the uncertainty of 2% (relative). This result demonstrates that the use of the Pitzer model for the calibration of CCNCs gives the most accurate value of S.
Tropospheric water vapour above Switzerland over the last 12 years

Integrated Water vapour (IWV) has been measured since 1994 by the TROWARA microwave radiometer in Bern, Switzerland. Homogenization techniques were used to identify and correct step changes in IWV related to instrument problems. IWV from radiosonde, GPS and sun photometer (SPM) was used in the homogenisation process as well as partial IWV columns between valley and mountain weather stations. The average IWV of the homogenised TROWARA time series was 14.4 mm over the 1996–2007 period, with maximum and minimum monthly average values of 22.4 mm and 8 mm occurring in August and January, respectively. A weak diurnal cycle in TROWARA IWV was detected with an amplitude of 0.32 mm, a maximum at 21:00 UT and a minimum at 11:00 UT. For 1996–2007, TROWARA trends were compared with those calculated from the Payerne radiosonde and the closest ECMWF grid point to Bern. Using least squares analysis, the IWV time series of radiosondes at Payerne, ECMWF, and TROWARA showed consistent positive trends from 1996 to 2007. The radiosondes measured an IWV trend of 0.45±0.29%/y, the TROWARA radiometer observed a trend of 0.39±0.44%/y, and ECMWF operational analysis gave a trend of 0.25±0.34%/y. Since IWV has a strong and variable annual cycle, a seasonal trend analysis (Mann-Kendall analysis) was also performed. The seasonal trends are stronger by a factor 10 or so compared to the full year trends above. The positive IWV trends of the summer months are partly compensated by the negative trends of the winter months. The strong seasonal trends of IWV on regional scale underline the necessity of long-term monitoring of IWV for detection,understanding, and forecast of climate change effects in the Alpine region.