ALBERT

Description: We use the GEOS-Chem global 3-D chemistry transport model to investigate the relative importance of chemical and physical processes that determine observed variability of hydrogen cyanide (HCN) in the troposphere and lower stratosphere. Consequently, we reconcile ground-based FTIR column measurements of HCN, which show annual and semi-annual variations, with recent space-borne measurements of HCN mixing ratio in the tropical lower stratosphere, which show a large two-year variation. We find that the observed column variability over the ground-based stations is determined by a superposition of HCN from several regional burning sources, with GEOS-Chem reproducing these column data with a positive bias of 5%. GEOS-Chem reproduces the observed tropical HCN variability from the Microwave Limb Sounder and the Atmospheric Chemistry Experiment satellite instruments with a negative bias of 7%. We show the tropical biomass burning emissions explain mostly the observed HCN variations in the upper troposphere and lower stratosphere (UTLS), with the remainder due to atmospheric transport and HCN chemistry. In the mid and upper stratosphere, atmospheric dynamics progressively exerts more influences on HCN variations. The extent of temporal overlap between African and other continental burning seasons is key in establishing the apparent bienniel cycle in the UTLS. Similar analysis of other, shorter-lived trace gases have not observed the transition between annual and bienniel cycles in the UTLS probably because the signal of inter-annual variations from surface emission has vanished before arriving at the lower stratosphere (LS), due to shorter atmospheric lifetimes.

Description: The characteristics of planetary wave energy propagation are being compared based on NCEP reanalysis data from 1958 to 2002 between boreal winters after strong volcanic eruptions, non-volcanic winters and episodes of strong polar vortex lasting at least 30 days. It shows that in the volcanically disturbed winters much more planetary wave energy is produced in the troposphere, passes through the lowermost stratosphere and enters the upper stratosphere than in any other times. This is contradicting earlier interpretations and model simulations. Possibly the observed El Ninos coinciding with the three significant eruptions in the second half of the 20th century contributed to the planetary wave energy. In order to produce the observed robust climate anomaly patterns in the lower troposphere, these planetary waves are suggested to be reflected near the stratopause instead of breaking. While a strong polar vortex is observed after volcanic eruptions in the stratosphere and in the troposphere, specific episodes of strong polar vortex regime exhibit much stronger anomalies and different dynamics. Hence it is suggested that the climate effects of volcanic eruptions are not being explained by the excitation of inherent zonal mean variability modes such as Strong Polar Vortex or Northern Annular Mode, but rather is another mode that possibly reflects upon the North Atlantic Oscillation.

Description: The probability density on a height-meridional plane of negative refractive index squared f(nk2

Description: Observations from the 2007 Border Air Quality and Meteorology Study (BAQS-Met 2007) in Southern Ontario, Canada, were used to evaluate predictions of primary organic aerosol (POA) and two other carbonaceous species, black carbon (BC) and carbon monoxide (CO), made for this summertime period by Environment Canada's AURAMS regional chemical transport model. Particle component-based factor analysis was applied to aerosol mass spectrometer measurements made at one urban site (Windsor, ON) and two rural sites (Harrow and Bear Creek, ON) to derive hydrocarbon-like organic aerosol (HOA) factors. A novel diagnostic model evaluation was performed by investigating model POA bias as a function of HOA mass concentration and indicator ratios (e.g. BC/HOA). Eight case studies were selected based on factor analysis and back trajectories to help classify model bias for certain POA source types. By considering model POA bias in relation to co-located BC and CO biases, a plausible story is developed that explains the model biases for all three species. At the rural sites, daytime mean PM1 POA mass concentrations were under-predicted compared to observed HOA concentrations. POA under-predictions were accentuated when the transport arriving at the rural sites was from the Detroit/Windsor urban complex and for short-term periods of biomass burning influence. Interestingly, the daytime CO concentrations were only slightly under-predicted at both rural sites, whereas CO was over-predicted at the urban Windsor site with a normalized mean bias of 134%, while good agreement was observed at Windsor for the comparison of daytime PM1 POA and HOA mean values, 1.1 μg m−3 and 1.2 μg m−3, respectively. Biases in model POA predictions also trended from positive to negative with increasing HOA values. Periods of POA over-prediction were most evident at the urban site on calm nights due to an overly-stable model surface layer. This model behaviour can be explained by a combination of model under-estimation of vertical mixing at the urban location, under-representation of PM emissions for on-road traffic exhaust along major urban roads and highways, and a more structured allocation of area POA sources such as food cooking and dust emissions to urban locations. A downward trend in POA bias was also observed at the urban site as a function of the BC/HOA indicator ratio, suggesting a possible association of POA under-prediction with under-representation of diesel combustion sources. An investigation of the emission inventories for the province of Ontario and the nearby US state of Indiana also suggested that the top POA area emission sources (food cooking, organic-bound to dust, waste disposal burning) dominated over mobile and point sources, again consistent with a mobile under-estimation. We conclude that more effort should be placed at reducing uncertainties in the treatment of several large POA emission sources, in particular food cooking, fugitive dust, waste disposal burning, and on-road traffic sources, and especially their spatial surrogates and temporal profiles. This includes using higher spatial resolution model grids to better resolve the urban road network and urban food cooking locations. We also recommend that additional sources of urban-scale vertical mixing in the model, such as a stronger urban heat island effect and vehicle-induced turbulence, would help model predictions at urban locations, especially at night time.

Description: We investigate the relative impacts of biomass burning emissions and dynamics on tropical upper tropospheric carbon monoxide (CO) and ozone (O3) over western and central Indonesia during the August–November 2006 fires in equatorial Asia by using a global three-dimensional model of tropospheric chemistry (GEOS-Chem) and by comparing model results with Microwave Limb Sounder (MLS) observations of upper tropospheric CO and O3. GEOS-Chem CO and O3 show similarities with MLS observed enhancements from convective lifting of fire emissions. In the tropical upper troposphere (UT), fire effluents from equatorial Asia are primarily transported southwestward to the eastern tropical Indian Ocean, driven by the high-pressure systems along 10° N–15° N and 10° S–15° S latitudes, and northeastward to southeast Asia and beyond, driven by the western North Pacific subtropical high. A characteristic feature of these CO enhancements is that they lag behind biomass burning emissions (by 2–3 weeks) at the three pressure levels 215, 147 and 100 hPa, resulting from the decreasing influence of deep convective lifting with altitude in the tropical UT. Inclusion of biomass burning injection height significantly improves model comparison with observations. We estimate the fire influences by contrasting one model simulation with year-specific and another with climatological biomass burning emissions. Biomass burning accounts for about 50–150 ppbv of CO and 5–15 ppbv of O3 in the tropical UT below 100 hPa during October and November, with temporal variations driven by biomass burning and deep convection. We estimate the dynamic impacts by examining the difference between a model simulation for 2006 (El Niño) and another for 2005 (neutral). The dynamic impacts are far more complex and account for up to 100 ppbv of CO and 30 ppbv of O3 in the tropical UT below 100 hPa. The temporal variation of the dynamic impact on CO is driven by deep convection. The variation of the dynamic impact on O3 depends on deep convection as well as the associated lightning NOx emissions and also reflects non-linearity of O3 chemistry.

Description: Forest fires are an important source to carbonaceous aerosols in the Western United States (WUS). We quantify the relative contribution of biomass burning to black carbon (BC) in the WUS mountain ranges by analyzing surface BC observations for 2006 from the Interagency Monitoring of PROtected Visual Environment (IMPROVE) network using the GEOS-Chem global chemical transport model. Observed surface BC concentrations show broad maxima during late June to early November. Enhanced potassium concentrations and potassium/sulfur ratios observed during the high-BC events indicate a dominant biomass burning influence during the peak fire season. Model surface BC reproduces the observed day-to day and synoptic variabilities in regions downwind of but near urban centers. Major discrepancies are found at elevated mountainous sites during the July-October fire season when simulated BC concentrations are biased low by a factor of two. We attribute these low biases largely to the underestimated (by more than a factor of two) and temporally misplaced biomass burning emissions of BC in the model. Additionally, we find that the biomass burning contribution to surface BC concentrations in the USA likely was underestimated in a previous study using GEOS-Chem (Park et al., 2003), because of the unusually low planetary boundary layer (PBL) heights in the GEOS-3 meteorological reanalysis data used to drive the model. PBL heights from GEOS-4 and GEOS-5 reanalysis data are comparable to those from the North American Regional Reanalysis (NARR). Model simulations show slightly improved agreements with the observations when driven by GEOS-5 reanalysis data, but model results are still biased low. The use of biomass burning emissions with diurnal cycle, synoptic variability, and plume injection has relatively small impact on the simulated surface BC concentrations in the WUS.

Description: Forest fires in Alaska and western Canada represent important sources of aerosols and trace gases in North America. Among the largest uncertainties when modeling forest fire effects are the timing and injection height of biomass burning emissions. Here we simulate CO and aerosols over North America during the 2004 fire season, using the GEOS-Chem chemical transport model. We apply different temporal distributions and injection height profiles to the biomass burning emissions, and compare model results with satellite-, aircraft-, and ground-based measurements. We find that averaged over the fire season, the use of finer temporal resolved biomass burning emissions usually decreases CO and aerosol concentrations near the fire source region, and often enhances long-range transport. Among the individual temporal constraints, switching from monthly to 8-day time intervals for emissions has the largest effect on CO and aerosol distributions, and shows better agreement with measured day-to-day variability. Injection height substantially modifies the surface concentrations and vertical profiles of pollutants near the source region. Compared with CO, the simulation of black carbon aerosol is more sensitive to the temporal and injection height distribution of emissions. The use of MISR-derived injection heights improves agreement with surface aerosol measurements near the fire source. Our results indicate that the discrepancies between model simulations and MOPITT CO measurements near the Hudson Bay can not be attributed solely to the representation of injection height within the model. Frequent occurrence of strong convection in North America during summer tends to limit the influence of injection height parameterizations of fire emissions in Alaska and western Canada with respect to CO and aerosol distributions over eastern North America.

Description: Particle size distribution from biomass combustion is an important parameter as it affects air quality, climate modelling and health effects. To date, particle size distributions reported from prior studies vary not only due to difference in fuels but also difference in experimental conditions. This study aims to report characteristics of particle size distributions in well controlled repeatable lab scale biomass fires for southwestern United States fuels with focus on chaparral. The combustion laboratory at the United States Department of Agriculture-Forest Service's Fire Science Laboratory (USDA-FSL), Missoula, MT provided a repeatable combustion and dilution environment ideal for measurements. For a variety of fuels tested the major mode of particle size distribution was in the range of 29 to 52 nm, which is attributable to dilution of the fresh smoke. Comparing mass size distribution from FMPS and APS measurement 51–68% of particle mass was attributable to the particles ranging from 0.5 to 10 μm for PM10. Geometric mean diameter rapidly increased during flaming and gradually decreased during mixed and smoldering phase combustion. Most fuels produced a unimodal distribution during flaming phase and strong biomodal distribution during smoldering phase. The mode of combustion (flaming, mixed and smoldering) could be better distinguished using the slopes in MCE (Modified Combustion Efficiency) vs. geometric mean diameter than only using MCE values.

Description: We use the GEOS-Chem global 3-D chemistry transport model to investigate the relative importance of chemical and physical processes that determine observed variability of hydrogen cyanide (HCN) in the troposphere and lower stratosphere. Consequently, we reconcile ground-based FTIR column measurements of HCN, which show annual and semi-annual variations, with recent space-borne measurements of HCN mixing ratio in the tropical lower stratosphere, which show a large two-year variation. We find that the observed column variability over the ground-based stations is determined by a superposition of HCN from several regional burning sources, with GEOS-Chem reproducing these column data with a positive bias of 5%. GEOS-Chem reproduces the observed HCN mixing ratio from the Microwave Limb Sounder and the Atmospheric Chemistry Experiment satellite instruments with a mean negative bias of 20%, and the observed HCN variability with a mean negative bias of 7%. We show that tropical biomass burning emissions explain most of the observed HCN variations in the upper troposphere and lower stratosphere (UTLS), with the remainder due to atmospheric transport and HCN chemistry. In the mid and upper stratosphere, atmospheric dynamics progressively exerts more influence on HCN variations. The extent of temporal overlap between African and other continental burning seasons is key in establishing the apparent bienniel cycle in the UTLS. Similar analysis of other, shorter-lived trace gases have not observed the transition between annual and bienniel cycles in the UTLS probably because the signal of inter-annual variations from surface emission has been diluted before arriving at the lower stratosphere (LS), due to shorter atmospheric lifetimes.