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Estimating trajectory uncertainties due to flow dependent errors in the atmospheric analysis

The uncertainty of a calculated trajectory is dependent on the uncertainty in the atmospheric analysis. Using the Ensemble Transform method (originally adapted for ensemble forecasting) we sample the analysis uncertainty in order to create an ensemble of analyses where a trajectory is started from each perturbed analysis. This method, called the Ensemble analysis method (EA), is compared to the Initial spread method (IS), where the trajectory receptor point is perturbed in the horizontal and vertical direction to create a set of trajectories used to estimate the trajectory uncertainty. The deviation growth is examined for one summer and one winter month and for 15 different geographical locations. We find up to a 40% increase in trajectory deviation in the mid-latitudes using the EA method. A simple model for trajectory deviation growth speed is set up and validated. It is shown that the EA method result in a faster error growth compared to the IS method. In addition, two case studies are examined to qualitatively illustrate how the flow dependent analysis uncertainty can impact the trajectory calculations. We find a more irregular behavior for the EA trajectories compared to the IS trajectories and a significantly increased uncertainty in the trajectory origin. We conclude that by perturbing the analysis in agreement with the analysis uncertainties the error in backward trajectory calculations can be more consistently estimated.
Size-distributions of n-alkanes, PAHs and hopanes and their sources in the urban, mountain and marine atmospheres over East Asia

Size-segregated (9 stages) n-alkanes, polycyclic aromatic hydrocarbons (PAHs) and hopanes in the urban (Baoji city in inland China), mountain (Mt. Tai in east coastal China) and marine (Okinawa Island, Japan) atmospheres over East Asia were studied using a GC/MS technique. Ambient concentrations of n-alkanes (1698±568 ng m−3 in winter and 487±145 ng m−3 in spring), PAHs (536±80 and 161±39 ng m−3), and hopanes (65±24 and 20±2.4 ng m−3) in the urban air are 1–2 orders of magnitude higher than those in the mountain aerosols and 2–3 orders of magnitude higher than those in the marine samples. Mass ratios of n-alkanes, PAHs and hopanes clearly demonstrate coal-burning emissions as their major source. Size distributions of fossil fuel derived n-alkane, PAHs and hopanes were found to be unimodal in most cases, peaking at 0.7–1.1 μm size. In contrast, plant wax derived n-alkanes presented a bimodal distribution with two peaks at the sizes of 0.7–1.1 μm and >4.7 μm in the summer mountain and spring marine samples. Among the three types of samples, geometric mean diameter (GMD) of the organics in fine mode (<2.1 μm) was found to be smallest (av. 0.63 μm in spring) for the urban samples and largest (1.01 μm) for the marine samples, whereas the GMD in coarse mode (≥2.1 μm) was found to be smallest (3.48 μm) for the marine aerosols and largest (4.04 μm) for the urban aerosols. The fine mode GMDs of the urban and mountain samples were larger in winter than in spring and summer. Moreover, GMDs of 3- and 4-ring PAHs were larger than those of 5- and 6-ring PAHs in the three types of atmospheres. Such differences in GMDs can be interpreted by the repartitioning of organic compounds and the coagulation and hygroscopic growth of particles during a long-range transport from the inland continent to the marine area, as well as the difference in their sources among the three regions.
Can gravity waves significantly impact PSC occurrence in the Antarctic?

A combination of POAM III aerosol extinction and CHAMP RO temperature measurements are used to examine the role of atmospheric gravity waves in the formation of Antarctic Polar Stratospheric Clouds (PSCs). POAM III aerosol extinction observations and quality flag information are used to identify Polar Stratospheric Clouds using an unsupervised clustering algorithm. A PSC proxy, derived by thresholding Met Office temperature analyses with the PSC Type Ia formation temperature (TNAT), shows general agreement with the results of the POAM III analysis. However, in June the POAM III observations of PSC are more abundant than expected from temperature threshold crossings in five out of the eight years examined. In addition, September and October PSC identified using temperature thresholding is often significantly higher than that derived from POAM III; this observation probably being due to dehydration and denitrification. Comparison of the Met Office temperature analyses with corresponding CHAMP observations also suggests a small warm bias in the Met Office data in June. However, this bias cannot fully explain the differences observed. Analysis of CHAMP data indicates that temperature perturbations associated with gravity waves may partially explain the enhanced PSC incidence observed in June (relative to the Met Office analyses). For this month, approximately 40% of the temperature threshold crossings observed using CHAMP RO data are associated with small-scale perturbations. Examination of the distribution of temperatures relative to TNAT shows a large proportion of June data to be close to this threshold, potentially enhancing the importance of gravity wave induced temperature perturbations. Inspection of the longitudinal structure of PSC occurrence in June 2005 also shows that regions of enhancement are geographically associated with the Antarctic Peninsula; a known mountain wave "hotspot". The latitudinal variation of POAM III observations means that we only observe this region in June–July, and thus the true pattern of enhanced PSC production may continue operating into later months. The analysis has shown that early in the Antarctic winter stratospheric background temperatures are close to the TNAT threshold (and PSC formation), and are thus sensitive to temperature perturbations associated with mountain wave activity near the Antarctic peninsula (40% of PSC formation). Later in the season, and at latitudes away from the peninsula, temperature perturbations associated with gravity waves contribute to about 15% of the observed PSC (a value which corresponds well to several previous studies). This lower value is likely to be due to colder background temperatures already achieving the TNAT threshold unaided. Additionally, there is a reduction in the magnitude of gravity waves perturbations observed as POAM III samples poleward of the peninsula.
Decadal trends in aerosol chemical composition at Barrow, Alaska: 1976–2008

Aerosol measurements at Barrow, Alaska during the past 30 years have identified the long range transport of pollution associated with Arctic Haze as well as ocean-derived aerosols of more local origin. Here, we focus on measurements of aerosol chemical composition to assess (1) trends in Arctic Haze aerosol and implications for source regions, (2) the interaction between pollution-derived and ocean-derived aerosols and the resulting impacts on the chemistry of the Arctic boundary layer, and (3) the response of aerosols to a changing climate. Aerosol chemical composition measured at Barrow, AK during the Arctic haze season is compared for the years 1976–1977 and 1997–2008. Based on these two data sets, concentrations of non-sea salt (nss) sulfate (SO4=) and non-crustal (nc) vanadium (V) have decreased by about 60% over this 30 year period. Consistency in the ratios of nss SO4=/ncV and nc manganese (Mn)/ncV between the two data sets indicates that, although emissions have decreased in the source regions, the source regions have remained the same over this time period. The measurements from 1997–2008 indicate that, during the haze season, the nss SO4= aerosol at Barrow is becoming less neutralized by ammonium (NH4+) yielding an increasing sea salt aerosol chloride (Cl−) deficit. The expected consequence is an increase in the release of Cl atoms to the atmosphere and a change in the lifetime of volatile organic compounds (VOCs) including methane. In addition, summertime concentrations of biogenically-derived methanesulfonate (MSA−) and nss SO4= are increasing at a rate of 12 and 8% per year, respectively. Further research is required to assess the environmental factors behind the increasing concentrations of biogenic aerosol.
Effect of biomass burning on marine stratocumulus clouds off the California coast

Aerosol-cloud interactions are considered to be one of the most important and least known forcings in the climate system. Biomass burning aerosols are of special interest due to their radiative impact (direct and indirect effect) and their potential to increase in the future due to climate change. Combining data from Geostationary Operational Environmental Satellite (GOES) and MODerate-resolution Imaging Spectroradiometer (MODIS) with passive tracers from the FLEXPART Lagrangian Particle Dispersion Model, the impact of biomass burning aerosols on marine stratocumulus clouds has been examined in June and July of 2006–2008 off the California coast. Using a continental tracer, the indirect effect of biomass burning aerosols has been isolated by comparing the average cloud fraction and cloud albedo for different meteorological situations, and for clean versus polluted (in terms of biomass burning) continental air masses at 14:00 local time. Within a 500 km-wide band along the coast of California, biomass burning aerosols, which tend to reside above the marine boundary layer, increased the cloud fraction by 0.143, and the cloud albedo by 0.038. Absorbing aerosols located above the marine boundary layer lead to an increase of the lower tropospheric stability and a reduction in the vertical entrainment of dry air from above, leading to increased cloud formation. The combined effect was an indirect radiative forcing of −7.5% ±1.7% (cooling effect) of the outgoing radiative flux at the top of the atmosphere on average, with a bias due to meteorology of +0.9%. Further away from the coast, the biomass burning aerosols, which were located within the boundary layer, reduced the cloud fraction by 0.023 and the cloud albedo by 0.006, resulting in an indirect radiative forcing of +1.3% ±0.3% (warming effect) with a bias of +0.5%. These results underscore the dual role that absorbing aerosols play in cloud radiative forcing.
On the relationship of polar mesospheric cloud ice water content, particle radius and mesospheric temperature and its use in multi-dimensional models

The distribution of ice layers in the polar summer mesosphere (called polar mesospheric clouds or PMCs) is sensitive to background atmospheric conditions and therefore affected by global-scale dynamics. To investigate this coupling it is necessary to simulate the global distribution of PMCs within a 3-dimensional (3-D) model that couples large-scale dynamics with cloud microphysics. However, modeling PMC microphysics within 3-D global chemistry climate models (GCCM) is a challenge due to the high computational cost associated with particle following (Lagrangian) or sectional microphysical calculations. By characterizing the relationship between the PMC effective radius, ice water content (iwc), and local temperature (T) from an ensemble of simulations from the sectional microphysical model, the Community Aerosol and Radiation Model for Atmospheres (CARMA), we determined that these variables can be described by a robust empirical formula. The characterized relationship allows an estimate of an altitude distribution of PMC effective radius in terms of local temperature and iwc. For our purposes we use this formula to predict an effective radius as part of a bulk parameterization of PMC microphysics in a 3-D GCCM to simulate growth, sublimation and sedimentation of ice particles without keeping track of the time history of each ice particle size or particle size bin. This allows cost effective decadal scale PMC simulations in a 3-D GCCM to be performed. This approach produces realistic PMC simulations including estimates of the optical properties of PMCs. We validate the relationship with PMC data from the Solar Occultation for Ice Experiment (SOFIE).
Heavy ozone enrichments from MIPAS limb emission spectra

Vertical enrichment profiles of stratospheric heavy ozone (asymmetric and symmetric 50O3 isotopomers) have been derived from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). As a continuously operating satellite instrument, MIPAS has an advantage over previous measurements in providing global coverage over an extended time period, allowing the variations in enrichment to be determined. However, since the spectral features of the isotopomers are comparable with the magnitude of the instrument noise, a sequential estimation retrieval scheme has been used to average the measurements zonally. The magnitude of observed enrichments is ~10% in stratosphere, a value consistent with previous observations and lab measurements. The data indicate that asymmetric heavy ozone is significantly more enriched than the symmetric isotopomer and show latitudinal and vertical variations in both the asymmetric and symmetric 50O3 enrichments. Enrichments decrease with decreasing temperature, as previously noted, at midlatidudes and polar regions, while they increase with decreasing temperature in equatorial regions. MIPAS measurements contain also information on the asymmetric and symmetric 49O3 isotopomers. The enrichments of 49O3, obtained with the same sequential estimator approach, are much larger than the enrichments of 50O3, in contraddictions with previous results which predict larger enrichments for heavier isotopomers.
Sensitivity studies of different aerosol indirect effects in mixed-phase clouds

Aerosols affect the climate system by changing cloud characteristics. Using the global climate model ECHAM5-HAM, we investigate different aerosol effects on mixed-phase clouds: The glaciation effect, which refers to a more frequent glaciation due to anthropogenic aerosols, versus the de-activation effect, which suggests that ice nuclei become less effective because of an anthropogenic sulfate coating. The glaciation effect can partly offset the indirect aerosol effect on warm clouds and thus causes the total anthropogenic aerosol effect to be smaller. It is investigated by varying the parameterization for the Bergeron-Findeisen process and the threshold coating thickness of sulfate (SO4-crit), which is required to convert an externally mixed aerosol particle into an internally mixed particle. Differences in the net radiation at the top-of-the-atmosphere due to anthropogenic aerosols between the different sensitivity studies amount up to 0.5 W m−2. This suggests that the investigated mixed-phase processes have a major effect on the total anthropogenic aerosol effect.
Northern winter stratospheric temperature and ozone responses to ENSO inferred from an ensemble of Chemistry Climate Models

The connection between the El Niño Southern Oscillation (ENSO) and the Northern polar stratosphere has been established from observations and atmospheric modeling. Here a systematic inter-comparison of the sensitivity of the modeled stratosphere to ENSO in Chemistry Climate Models (CCMs) is reported. This work uses results from a number of the CCMs included in the 2006 ozone assessment. In the lower stratosphere, the mean of all model simulations reports a warming of the polar vortex during strong ENSO events in February–March, consistent with but smaller than the estimate from satellite observations and ERA40 reanalysis. The anomalous warming is associated with an anomalous dynamical increase of column ozone north of 70° N that is accompanied by coherent column ozone decrease in the Tropics, in agreement with that deduced from the NIWA column ozone database, implying an increased residual circulation in the mean of all model simulations during ENSO. The spread in the model responses is partly due to the large internal stratospheric variability and it is shown that it crucially depends on the representation of the tropospheric ENSO teleconnection in the models.
Reduction in biomass burning aerosol light absorption upon humidification: roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer

Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used were Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients revealed a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: (1) shielding of inner monomers after particle consolidation or collapse with water uptake; (2) the lower case contribution of mass transfer through evaporation and condensation at high relative humidity (RH) to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.