The objective of this study is to analyze the pollution inflow into California during summertime and how it impacts surface air quality through combined analysis of a suite of observations and global ...and regional models. The focus is on the transpacific pollution transport investigated by the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission in June 2008. Additional observations include satellite retrievals of carbon monoxide and ozone by the EOS Aura Tropospheric Emissions Spectrometer (TES), aircraft measurements from the MOZAIC program and ozonesondes. We compare chemical boundary conditions (BC) from the MOZART-4 global model, which are commonly used in regional simulations, with measured concentrations to quantify both the accuracy of the model results and the variability in pollution inflow. Both observations and model reflect a large variability in pollution inflow on temporal and spatial scales, but the global model captures only about half of the observed free tropospheric variability. Model tracer contributions show a large contribution from Asian emissions in the inflow. Recirculation of local US pollution can impact chemical BC, emphasizing the importance of consistency between the global model simulations used for BC and the regional model in terms of emissions, chemistry and transport. Aircraft measurements in the free troposphere over California show similar concentration ranges, variability and source contributions as free tropospheric air masses over ocean, but caution has to be taken that local pollution aloft is not misinterpreted as inflow. A flight route specifically designed to sample boundary conditions during ARCTAS-CARB showed a prevalence of plumes transported from Asia and thus may not be fully representative for average inflow conditions. Sensitivity simulations with a regional model with altered BCs show that the temporal variability in the pollution inflow does impact modeled surface concentrations in California. We suggest that time and space varying chemical boundary conditions from global models provide useful input to regional models, but likely still lead to an underestimate of peak surface concentrations and the variability associated with long-range pollution transport.
Evaluation of a regional air quality forecasting system for the Pacific Northwest was carried out using a suite of surface and satellite observations. Wildfire events for the 2007 and 2008 fire ...seasons were simulated using the Air Information Report for Public Access and Community Tracking v.3 (AIRPACT-3) framework utilizing the Community Multi-scale Air Quality (CMAQ) model. Fire emissions were simulated using the BlueSky framework with fire locations determined by the Satellite Mapping Automated Reanalysis Tool for Fire Incident Reconciliation (SMARTFIRE). Plume rise was simulated using two different methods: the Fire Emission Production Simulator (FEPS) and the Sparse Matrix Operator Kernel Emissions (SMOKE) model. Predicted plume top heights were compared to the Cloud-Aerosol LIDAR with Orthogonal Polarization (CALIOP) instrument aboard the Cloud Aerosol LIDAR and Infrared Pathfinder Satellite Observation (CALIPSO) satellite. Carbon monoxide predictions were compared to the Atmospheric InfraRed Sounder (AIRS) instrument aboard the Aqua satellite. Horizontal distributions of column aerosol optical depth (AOD) were compared to retrievals by the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument aboard the Aqua satellite. Model tropospheric nitrogen dioxide distributions were compared to retrievals from the Ozone Monitoring Instrument (OMI) aboard the Aura satellite. Surface ozone and PM2.5 predictions were compared to surface observations. The AIRPACT-3 model captured the location and transport direction of fire events well, but sometimes missed the timing of fire events and overall underestimated the PM2.5 impact of wildfire events at surface monitor locations. During the 2007 (2008) fire period, the fractional biases (FBs) of AIRPACT-3 for various pollutant observations included: average 24 h PM2.5 FB = −33% (−27%); maximum daily average 8 h ozone FB = −8% (+1%); AOD FB = −61% (−53%); total column CO FB = −10% (−5%); and tropospheric column NO2 FB = −39% (−28%). The bias in total column CO is within the range of expected error. Fractional biases of AIRPACT-3 plume tops were found to be −46% when compared in terms of above mean sea level, but only −28% when compared in terms of above ground level, partly due to the under-estimation of AIRPACT-3 ground height in complex terrain that results from the 12 km grid-cell smoothing. We conclude that aerosol predictions were too low for locations greater than ~100–300 km downwind from wildfire sources and that model predictions are likely under-predicting secondary organic aerosol (SOA) production, due to a combination of very low volatile organic compound (VOC) emission factors used in the United States Forest Service Consume model, an incomplete speciation of VOC to SOA precursors in SMOKE, and under-prediction by the SOA parameterization within CMAQ.
Measurements from the Terra satellite launched in December of 1999 provide a global record of the recent interannual variability of tropospheric air quality: carbon monoxide (CO) from the Measurement ...of Pollution in the Troposphere (MOPITT) instrument and aerosol optical depth (AOD) from the Moderate‐Resolution Imaging Spectroradiometer (MODIS). This paper compares and contrasts these data sets with a view to understanding the general features of the overall pollutant loading of the Northern Hemisphere (NH). We present a detailed examination of the seasonal and recent interannual variability of the fine mode AOD and CO column, first considering the variation of the global zonal average for both quantities, and then concentrating on several geographical regions with the aim of isolating different emissions. In a zonal sense, the principal NH sources are related to anthropogenic urban and industrial activity. We show that both the CO and the AOD zonal seasonal variations reflect the atmospheric oxidant concentration, which determines the primary sink of CO and the production of sulfate aerosol. As a consequence, the seasonal cycles are several months out of phase, with perturbations resulting from sporadic wildfire or biomass‐burning emissions. In these cases, carbonaceous particles dominate the AOD, and this results in the best correlation with the CO column. Of the 4 years of data available from the Terra satellite, the winter and spring of 2002–2003 showed anomalously high NH pollution compared to the previous years. This was a result of fires in western Russia in the late summer and fall of 2002 and intense fires in the southeast of Russia in the spring and summer of 2003. We examine these events using fire counts from MODIS to indicate the burning regions and investigate how the timing of the fires in relation to atmospheric oxidant concentrations affects the resultant seasonal pollutant loadings. Finally, we trace the emissions from these fires to indicate how intense local pollution sources can impact continental‐ and global‐scale air quality.
A procedure for tagging ozone produced from NO sources through updates to an existing chemical mechanism is described, and results from its implementation in the Model for Ozone and Related chemical ...Tracers (MOZART-4), a global chemical transport model, are presented. Artificial tracers are added to the mechanism, thus, not affecting the standard chemistry. The results are linear in the troposphere, i.e., the sum of ozone from individual tagged sources equals the ozone from all sources to within 3% in zonal mean monthly averages. In addition, the tagged ozone is shown to equal the standard ozone, when all tropospheric sources are tagged and stratospheric input is turned off. The stratospheric ozone contribution to the troposphere determined from the difference between total ozone and ozone from all tagged sources is significantly less than estimates using a traditional stratospheric ozone tracer (8 vs. 20 ppbv at the surface). The commonly used technique of perturbing NO emissions by 20% in a region to determine its ozone contribution is compared to the tagging technique, showing that the tagged ozone is 2-4 times the ozone contribution that was deduced from perturbing emissions. The ozone tagging described here is useful for identifying source contributions based on NO emissions in a given state of the atmosphere, such as for quantifying the ozone budget.
The combination of low anthropogenic emissions and large biogenic sources that characterizes the Southern Hemisphere (SH) leads to significant differences in atmospheric composition relative to the ...better studied Northern Hemisphere. This unique balance of sources poses significant challenges for global models. Carbon monoxide (CO) in particular is difficult to simulate in the SH due to the increased importance of secondary chemical production associated with the much more limited primary emissions. Here, we use aircraft observations from the 1991–2000 Cape Grim Overflight Program (CGOP) and the 2009–2011 HIAPER (High-performance Instrumented Airborne Platform for Environmental Research) Pole-to-Pole Observations (HIPPO), together with model output from the SH Model Intercomparison Project, to elucidate the drivers of CO vertical structure in the remote SH. Observed CO vertical profiles from Cape Grim are remarkably consistent with those observed over the southern mid-latitudes Pacific 10–20 years later, despite major differences in time periods, flight locations, and sampling strategies between the two data sets. These similarities suggest the processes driving observed vertical gradients are coherent across much of the remote SH and have not changed significantly over the past 2 decades. Model ability to simulate CO profiles reflects the interplay between biogenic emission sources, the chemical mechanisms that drive CO production from these sources, and the transport that redistributes this CO throughout the SH. The four chemistry-climate and chemical transport models included in the intercomparison show large variability in their abilities to reproduce the observed CO profiles. In particular, two of the four models significantly underestimate vertical gradients in austral summer and autumn, which we find are driven by long-range transport of CO produced from oxidation of biogenic compounds. Comparisons between the models show that more complex chemical mechanisms do not necessarily provide more accurate simulation of CO vertical gradients due to the convolved impacts of emissions, chemistry, and transport. Our results imply a large sensitivity of the remote SH troposphere to biogenic emissions and chemistry, both of which remain key uncertainties in global modeling. We suggest that the CO vertical gradient can be used as a metric for future model evaluation as it provides a sensitive test of the processes that define the chemical state of the background atmosphere.
A comprehensive group of reactive nitrogen species (NO, NOz, HN03, HOzN02, PANs, alkyl nitrates, and aerosol-NO3) were measured over North America during July/August 2004 from the NASA DC-8 platform ...(0.1 - 12 km). Nitrogen containing tracers of biomass combustion (HCN and CH3CN) were also measured along with a host of other gaseous (CO, VOC, OVOC, halocarbon) and aerosol tracers. Clean background air as well as air with influences from biogenic emissions, anthropogenic pollution, biomass combustion, convection, lightning, and the stratosphere was sampled over the continental United States, the Atlantic, and the Pacific. The North American upper troposphere (UT) was found to be greatly influenced by both lightning NO, and surface pollution lofted via convection and contained elevated concentrations of PAN, ozone, hydrocarbons, and NO,. Observational data suggest that lightning was a far greater contributor to NO, in the UT than previously believed. PAN provided a dominant reservoir of reactive nitrogen in the UT while nitric acid dominated in the lower troposphere (LT). Peroxynitric acid (H02N02) was present in sizable concentrations peaking at around 8 km. Aerosol nitrate appeared to be mostly contained in large soil based particles in the LT. Plumes from Alaskan fires contained large amounts of PAN and aerosol nitrate but little enhancement in ozone. A comparison of observed data with simulations from four 3-D models shows significant differences between observations and models as well as among models. We investigate the partitioning and interplay of the reactive nitrogen species within characteristic air masses and further examine their role in ozone formation.
Validation results are reported for the MOPITT (Measurements of Pollution in the Troposphere) “Version 5” (V5) product for tropospheric carbon monoxide (CO) and are compared to results for the ...“Version 4” product. The V5 retrieval algorithm introduces (1) a method for reducing retrieval bias drift associated with long‐term instrumental degradation, (2) a more exact representation of the effects of random errors in the radiances and, for the first time, (3) the use of MOPITT's near‐infrared (NIR) radiances to complement the thermal‐infrared (TIR) radiances. Exploiting TIR and NIR radiances together facilitates retrievals of CO in the lowermost troposphere. V5 retrieval products based (1) solely on TIR measurements, (2) solely on NIR measurements and (3) on both TIR and NIR measurements are separately validated and analyzed. Actual retrieved CO profiles and total columns are compared with equivalent retrievals based on in situ measurements from (1) routine NOAA aircraft sampling mainly over North America and (2) the “HIAPER Pole to Pole Observations” (HIPPO) field campaign. Particular attention is focused on the long‐term stability and geographical uniformity of the retrieval errors. Results for the retrieved total column clearly indicate reduced temporal bias drift in the V5 products compared to the V4 product, and do not exhibit a positive bias in the Southern Hemisphere, which is evident in the V4 product.
Key Points
New MOPITT products exhibit enhanced sensitivity to CO in the lower troposphere.
V5 products are rigorously validated using a large database of in-situ profiles.
V5 validation results indicate reduced bias drift compared to V4 products.
This study quantifies future changes in tropospheric ozone (O3) using
a simple parameterisation of source–receptor relationships based on
simulations from a range of models participating in the Task ...Force on
Hemispheric Transport of Air Pollutants (TF-HTAP) experiments. Surface and
tropospheric O3 changes are calculated globally and across 16 regions
from perturbations in precursor emissions (NOx, CO, volatile organic compounds – VOCs)
and methane (CH4) abundance only, neglecting any impact from climate
change. A source attribution is provided for each source region along with an
estimate of uncertainty based on the spread of the results from the models.
Tests against model simulations using the Hadley Centre Global Environment
Model version 2 – Earth system configuration (HadGEM2-ES) confirm that the approaches
used within the parameterisation perform well for most regions. The
O3 response to changes in CH4 abundance is slightly larger in
the TF-HTAP Phase 2 than in the TF-HTAP Phase 1 assessment (2010) and provides
further evidence that controlling CH4 is important for limiting
future O3 concentrations. Different treatments of chemistry and
meteorology in models remain one of the largest uncertainties in calculating
the O3 response to perturbations in CH4 abundance and
precursor emissions, particularly over the Middle East and south Asia
regions. Emission changes for the future Evaluating the CLimate and Air Quality
ImPacts of Short-livEd Pollutants (ECLIPSE) scenarios and a subset of
preliminary Shared Socioeconomic Pathways (SSPs) indicate that surface
O3 concentrations will increase regionally by 1 to 8 ppbv in 2050.
Source attribution analysis highlights the growing importance of CH4
in the future under current legislation. A change in the global tropospheric
O3 radiative forcing of +0.07 W m−2 from 2010 to 2050 is
predicted using the ECLIPSE scenarios and SSPs, based solely on changes in
CH4 abundance and tropospheric O3 precursor emissions and
neglecting any influence of climate change. Current legislation is shown to
be inadequate in limiting the future degradation of surface ozone air quality
and enhancement of near-term climate warming. More stringent future emission
controls provide a large reduction in both surface O3 concentrations
and O3 radiative forcing. The parameterisation provides a simple tool
to highlight the different impacts and associated uncertainties of local and
hemispheric emission control strategies on both surface air quality and the
near-term climate forcing by tropospheric O3.
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