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Model intercomparison of indirect aerosol effects

Modeled differences in predicted effects are increasingly used to help quantify the uncertainty of these effects. Here, we examine modeled differences in the aerosol indirect effect in a series of experiments that help to quantify how and why model-predicted aerosol indirect forcing varies between models. The experiments start with an experiment in which aerosol concentrations, the parameterization of droplet concentrations and the autoconversion scheme are all specified and end with an experiment that examines the predicted aerosol indirect forcing when only aerosol sources are specified. Although there are large differences in the predicted liquid water path among the models, the predicted aerosol first indirect effect for the first experiment is rather similar, about −0.6 Wm−2 to −0.7 Wm−2. Changes to the autoconversion scheme can lead to large changes in the liquid water path of the models and to the response of the liquid water path to changes in aerosols. Adding an autoconversion scheme that depends on the droplet concentration caused a larger (negative) change in net outgoing shortwave radiation compared to the 1st indirect effect, and the increase varied from only 22% to more than a factor of three. The change in net shortwave forcing in the models due to varying the autoconversion scheme depends on the liquid water content of the clouds as well as their predicted droplet concentrations, and both increases and decreases in the net shortwave forcing can occur when autoconversion schemes are changed. The parameterization of cloud fraction within models is not sensitive to the aerosol concentration, and, therefore, the response of the modeled cloud fraction within the present models appears to be smaller than that which would be associated with model "noise". The prediction of aerosol concentrations, given a fixed set of sources, leads to some of the largest differences in the predicted aerosol indirect radiative forcing among the models, with values of cloud forcing ranging from −0.3 Wm−2 to −1.4 Wm−2. Thus, this aspect of modeling requires significant improvement in order to improve the prediction of aerosol indirect effects.
Spectral light absorption by ambient aerosols influenced by biomass burning in the Amazon Basin. I: Comparison and field calibration of absorption measurement techniques

Spectral aerosol light absorption is an important parameter for the assessment of the radiation budget of the atmosphere. Although on-line measurement techniques for aerosol light absorption, such as the Aethalometer and the Particle Soot Absorption Photometer (PSAP), have been available for two decades, they are limited in accuracy and spectral resolution because of the need to deposit the aerosol on a filter substrate before measurement. Recently, a 7-wavelength (λ) Aethalometer became commercially available, which covers the visible (VIS) to near-infrared (NIR) spectral range (λ=450–950 nm), and laboratory calibration studies improved the degree of confidence in these measurement techniques. However, the applicability of the laboratory calibration factors to ambient conditions has not been investigated thoroughly yet. As part of the LBA-SMOCC (Large scale Biosphere atmosphere experiment in Amazonia – SMOke aerosols, Clouds, rainfall and Climate) campaign from September to November 2002 in the Amazon basin we performed an extensive field calibration of a 1-λ PSAP and a 7-λ Aethalometer utilizing a photoacoustic spectrometer (PAS, 532 nm) as reference device. Especially during the dry period of the campaign, the aerosol population was dominated by pyrogenic emissions. The most pronounced artifact of integrating-plate type attenuation techniques (e.g. Aethalometer, PSAP) is due to multiple scattering effects within the filter matrix. For the PSAP, we essentially confirmed the laboratory calibration factor by Bond et al. (1999). On the other hand, for the Aethalometer we found a multiple scattering enhancement of 5.23 (or 4.55, if corrected for aerosol scattering), which is significantly larger than the factors previously reported (~2) for laboratory calibrations. While the exact reason for this discrepancy is unknown, the available data from the present and previous studies suggest aerosol mixing (internal versus external) as a likely cause. For Amazonian aerosol, we found no absorption enhancement due to hygroscopic particle growth in the relative humidity (RH) range between 40% and 80%. However, a substantial bias in PSAP sensitivity that correlated with both RH and temperature (T) was observed for 20%<RH<30% and 24°C<T<26°C, respectively. In addition, both PSAP and Aethalometer demonstrated no sensitivity to gaseous adsorption. Although very similar in measurement principle, the PSAP and Aethalometer require markedly different correction factors, which is probably due to the different filter media used. Although on-site calibration of the PSAP and Aethalometer is advisable for best data quality, we recommend a set of "best practice" correction factors for ambient sampling based on the data from the present and previous studies. For this study, the estimated accuracies of the absorption coefficients determined by the PAS, PSAP and Aethalometer were 10, 15 and 20% (95% confidence level), respectively.
Factors of air ion balance in a coniferous forest according to measurements in Hyytiälä, Finland

A new mathematical model describing air ion balance was developed and tested. It has improved approximations and includes dry deposition of ions onto the forest canopy. The model leads to an explicit algebraic solution of the balance equations. This allows simple calculation of both the ionization rate and the average charge of aerosol particles from measurements of air ions and aerosol particles, with some parameters of the forest. Charged aerosol particles are distinguished from cluster ions by their size, which exceeds 1.6 nm diameter. The relative uncertainty of the ionization rate is about the same or less than the relative uncertainties of the measurements. The model was tested with specific air ion measurements carried out simultaneously at two heights at the Hyytiälä forest station, Finland. Earlier studies have shown a difference in the predictions of the ionization rate in the Hyytiälä forest when calculated in two different ways: based on the measurements of the environmental radioactivity and based on the air ion and aerosol measurements. The new model explains the difference as a consequence of neglecting dry deposition of ions in the earlier models. The ionization rate during the 16 h campaign was 5.6±0.8 cm−3 s−1 at the height of 2 m and 3.9±0.2 cm−3 s−1 at the height of 14 m, between the tops of the trees. The difference points out the necessity to consider the height variation when the ionization rate is used as a parameter in studies of ion-induced nucleation. Additional results are some estimates of the parameters of air ion balance. The recombination sink of cluster ions on the ions of opposite polarity made up 9–13%, the sink on aerosol particles 65–69%, and the sink on forest canopy 18–26% of the total sink of cluster ions. The average lifetime of cluster ions was about 130 s for positive and about 110 s for negative ions. At the height of 2 m, about 70% of the space charge of air was carried by aerosol particles, and at the height of 14 m, about 84%.
First space-borne measurements of methanol inside aged southern tropical to mid-latitude biomass burning plumes using the ACE-FTS instrument

First measurements from space of upper tropospheric and lower stratospheric methanol profiles within aged fire plumes are reported. Elevated levels of methanol at 0–45° S from 30 September to 3 November 2004 have been measured by the high resolution infrared spectrometer ACE-FTS onboard the SCISAT satellite. Methanol volume mixing ratios higher than 4000 pptv are detected and are strongly correlated with other fire products such as CO, C2H6, and HCN. A sensitivity study of the methanol retrieval, accounting for random and systematic contributions, shows that the retrieved methanol profile for a single occultation exceeds 100% error above 16.5 km, with an accuracy of about 20% for measurements inside polluted air masses. The upper tropospheric enhancement ratio of methanol with respect to CO is estimated from the correlation plot between methanol and CO for aged tropical biomass burning plumes. This ratio is in good agreement with the ratio measured in the free troposphere (up to 12 km) by recent aircraft studies and does not suggest any secondary production of methanol by oxidation in aged biomass burning plumes.
Interannual variability in global biomass burning emissions from 1997 to 2004

Biomass burning represents an important source of atmospheric aerosols and greenhouse gases, yet little is known about its interannual variability or the underlying mechanisms regulating this variability at continental to global scales. Here we investigated fire emissions during the 8 year period from 1997 to 2004 using satellite data and the CASA biogeochemical model. Burned area from 2001–2004 was derived using newly available active fire and 500 m. burned area datasets from MODIS following the approach described by Giglio et al. (2006). ATSR and VIRS satellite data were used to extend the burned area time series back in time through 1997. In our analysis we estimated fuel loads, including organic soil layer and peatland fuels, and the net flux from terrestrial ecosystems as the balance between net primary production (NPP), heterotrophic respiration (Rh), and biomass burning, using time varying inputs of precipitation (PPT), temperature, solar radiation, and satellite-derived fractional absorbed photosynthetically active radiation (fAPAR). For the 1997–2004 period, we found that on average approximately 58 Pg C year−1 was fixed by plants as NPP, and approximately 95% of this was returned back to the atmosphere via Rh. Another 4%, or 2.5 Pg C year−1 was emitted by biomass burning; the remainder consisted of losses from fuel wood collection and subsequent burning. At a global scale, burned area and total fire emissions were largely decoupled from year to year. Total carbon emissions tracked burning in forested areas (including deforestation fires in the tropics), whereas burned area was largely controlled by savanna fires that responded to different environmental and human factors. Biomass burning emissions showed large interannual variability with a range of more than 1 Pg C year−1, with a maximum in 1998 (3.2 Pg C year−1) and a minimum in 2000 (2.0 Pg C year−1).
Application of thermal-dissociation laser induced fluorescence (TD-LIF) to measurement of HNO3, Σalkyl nitrates, Σperoxy nitrates, and NO2 fluxes using eddy covariance

Nitrogen exchange between the atmosphere and biosphere directly influences atmospheric composition. While much is known about mechanisms of NO and N2O emissions, instrumentation for the study of mechanisms contributing to exchange of other major nitrogen species is quite limited. Here we describe the application of a new technique, thermal dissociation-laser induced fluorescence (TD-LIF), to eddy covariance measurements of the fluxes of NO2, total peroxy acyl and peroxy nitrates, total alkyl and multifunctional alkyl nitrates, and nitric acid. The technique offers the potential for investigating mechanisms of exchange of these species at the canopy scale over timescales from days to years. Examples of flux measurements at a ponderosa pine plantation in the mid-elevation Sierra Nevada Mountains in California are reported and used to evaluate instrument performance.
Intraseasonal variations of upper tropospheric water vapor in Asian monsoon region

This study investigates intraseasonal oscillations (ISOs) of upper tropospheric water vapor (UTWV) in the Asian monsoon region in boreal summer by using data with high spatial and temporal resolution from the AIRS instrument. There are robust intraseasonal cycles with periods of 30–60 days and 10–20 days in the UTWV field over both South Asia and East Asia. The 30–60-day oscillation accounts for more than 60 percent of the total variance. For the 30–60-day mode, the source and propagating signature of the UTWV disturbances are distinct in two monsoon sub-systems. Two patterns in the 30–60 day oscillation are seen: a South Asian pattern that originates on the western side of the Arabian Sea and moves eastward, and an East Asian pattern that develops over West Pacific and moves westward. The 10–20-day mode exhibits a uniform westward propagating signature from West Pacific to the Arabian Sea. The Asian summer monsoon region is identified as a main source for UTWV, so another special interest in this study is the relationship between monsoon activity and the 30–60-day oscillation of UTWV. The data show that the upper troposphere is moistened following intense monsoon convection with lags about 5–10 days. An examination of the low level circulation reveals that wet and dry periods in UTWV are closely related to active and break (inactive) periods in monsoon convection, suggesting that the Asian summer monsoon plays an important role in the intraseasonal variations of UTWV. Similar variability is seen in water vapor from European Center for Medium-Range Weather Forecasts (ECMWF) analyses.
A Lagrangian analysis of the impact of transport and transformation on the ozone stratification observed in the free troposphere during the ESCOMPTE campaign

The ozone variability observed by tropospheric ozone lidars during the ESCOMPTE campaign is analyzed by means of a hybrid-Lagrangian modeling study. Transport processes responsible for the formation of ozone-rich layers are identified using a semi-Lagrangian analysis of mesoscale simulations to identify the planetary boundary layer (PBL) footprint in the free troposphere. High ozone concentrations are related to polluted air masses exported from the Iberian PBL. The chemical composition of air masses coming from the PBL and transported in the free troposphere is evaluated using a Lagrangian chemistry model. The initial concentrations are provided by a model of chemistry and transport. Different scenarios are tested for the initial conditions and for the impact of mixing with background air in order to perform a quantitative comparison with the lidar observations. For this meteorological situation, the characteristic mixing time is of the order of 2 to 6 days depending on the initial conditions. Ozone is produced in the free troposphere within most air masses exported from the Iberian PBL at an average rate of 0.2 ppbv h−1, with a maximum ozone production of 0.4 ppbv h−1. Transport processes from the PBL are responsible for an increase of 13.3 ppbv of ozone concentrations in the free troposphere compared to background levels; about 45% of this increase is attributed to in situ production during the transport rather than direct export of ozone.
Diel and seasonal variations in the chemical composition of biomass burning aerosol

Fine aerosol particles were collected separately during daytime and nighttime at a tropical pasture site in Rondônia, Brazil, during the burning and dry-to-wet transition period in 2002. Total carbon (TC) and water-soluble organic carbon (WSOC) were measured by evolved gas analysis (EGA). Based on the thermochemical properties of the fine aerosol, the relative amounts of the volatile and refractory compounds were estimated. It was found that the thermally refractory (possibly higher molecular weight) compounds dominated the TC composition. Their contribution to TC was higher in the daytime than in the nighttime samples. The relative share of WSOC also showed a statistically significant diel variation as did its refractory fraction. Anhydrosugars and phenolic acids were determined by GC-MS and their diel variation was studied. Based on the decrease of their relative concentrations between the biomass burning and transition periods and their distinctly different diel variations, we suggest that the phenolic acids may undergo chemical transformations in the aerosol phase, possibly towards more refractory compounds (humic-like substances, HULIS), as has been suggested previously. These conclusions are supported by the results of the thermally assisted hydrolysis and methylation gas chromatography-mass spectrometry of the same filter samples.
Probing stratospheric transport and chemistry with new balloon and aircraft observations of the meridional and vertical N2O isotope distribution

A comprehensive set of stratospheric balloon and aircraft samples was analyzed for the position-dependent isotopic composition of nitrous oxide (N2O). Results for a total of 220 samples from between 1987 and 2003 are presented, nearly tripling the number of mass-spectrometric N2O isotope measurements in the stratosphere published to date. Cryogenic balloon samples were obtained at polar (Kiruna/Sweden, 68° N), mid-latitude (southern France, 44° N) and tropical sites (Hyderabad/India, 18° N). Aircraft samples were collected with a newly-developed whole air sampler on board of the high-altitude aircraft M55 Geophysica during the EUPLEX 2003 campaign. For mixing ratios above 200 nmol mol−1, relative isotope enrichments (δ values) and mixing ratios display a compact relationship, which is nearly independent of latitude and season and which can be explained equally well by Rayleigh fractionation or mixing. However, for mixing ratios below 200 nmol mol−1 this compact relationship gives way to meridional, seasonal and interannual variations. A comparison to a previously published mid-latitude balloon profile even shows large zonal variations, justifying the use of three-dimensional (3-D) models for further data interpretation. In general, the magnitude of the apparent fractionation constants (i.e., apparent isotope effects) increases continuously with altitude and decreases from the equator to the North Pole. Only the latter observation can be understood qualitatively by the interplay between the time-scales of N2O photochemistry and transport in a Rayleigh fractionation framework. Deviations from Rayleigh fractionation behavior also occur where polar vortex air mixes with nearly N2O-free upper stratospheric/mesospheric air (e.g., during the boreal winters of 2003 and possibly 1992). Aircraft observations in the polar vortex at mixing ratios below 200 nmol mol−1 deviate from isotope variations expected for both Rayleigh fractionation and two-end-member mixing, but could be explained by continuous weak mixing between intravortex and extravortex air (Plumb et al., 2000). However, it appears that none of the simple approaches described here can capture all features of the stratospheric N2O isotope distribution, again justifying the use of 3-D models. Finally, correlations between 18O/16O and average 15N/14N isotope ratios or between the position-dependent 15N/14N isotope ratios show that photo-oxidation makes a large contribution to the total N2O sink in the lower stratosphere (possibly up to 100% for N2O mixing ratios above 300 nmol mol−1). Towards higher altitudes, the temperature dependence of these isotope correlations becomes visible in the stratospheric observations.