Quantifying O₃ Impacts in Urban Areas Due to Wildfires Using a Generalized Additive Model

Wildfires emit O₃ precursors but there are large variations in emissions, plume heights, and photochemical processing. These factors make it challenging to model O₃ production from wildfires using Eulerian models. Here we describe a statistical approach to characterize the maximum daily 8-h average O₃ (MDA8) for 8 cities in the U.S. for typical, nonfire, conditions. The statistical model represents between 35% and 81% of the variance in MDA8 for each city. We then examine the residual from the model under conditions with elevated particulate matter (PM) and satellite observed smoke (“smoke days”). For these days, the residuals are elevated by an average of 3–8 ppb (MDA8) compared to nonsmoke days. We found that while smoke days are only 4.1% of all days (May–Sept) they are 19% of days with an MDA8 greater than 75 ppb. We also show that a published method that does not account for transport patterns gives rise to large overestimates in the amount of O₃ from fires, particularly for coastal cities. Finally, we apply this method to a case study from August 2015, and show that the method gives results that are directly applicable to the EPA guidance on excluding data due to an uncontrollable source

Interannual Variability in Baseline Ozone and Its Relationship to Surface Ozone in the Western U.S.

Baseline ozone refers to observed concentrations of tropospheric ozone at sites that have a negligible influence from local emissions. The Mount Bachelor Observatory (MBO) was established in 2004 to examine baseline air masses as they arrive to North America from the west. In May 2012, we observed an O₃ increase of 2.0–8.5 ppbv in monthly average maximum daily 8-hour average O₃ mixing ratio (MDA8 O₃) at MBO and numerous other sites in the western U.S. compared to previous years. This shift in the O₃ distribution had an impact on the number of exceedance days. We also observed a good correlation between daily MDA8 variations at MBO and at downwind sites. This suggests that under specific meteorological conditions, synoptic variation in O₃ at MBO can be observed at other surface sites in the western U.S. At MBO, the elevated O₃ concentrations in May 2012 are associated with low CO values and low water vapor values, consistent with transport from the upper troposphere/lower stratosphere (UT/LS). Furthermore, the Real-time Air Quality Modeling System (RAQMS) analyses indicate that a large flux of O₃ from the UT/LS in May 2012 contributed to the observed enhanced O₃ across the western U.S. Our results suggest that a network of mountaintop observations, LiDAR and satellite observations of O₃ could provide key data on daily and interannual variations in baseline O₃

Global Atmospheric Transport and Source-Receptor Relationships for Arsenic

Arsenic and many of its compounds are toxic pollutants in the global environment. They can be transported long distances in the atmosphere before depositing to the surface, but the global source-receptor relationships between various regions have not yet been assessed. We develop the first global model for atmospheric arsenic to better understand and quantify its intercontinental transport. Our model reproduces the observed arsenic concentrations in surface air over various sites around the world. Arsenic emissions from Asia and South America are found to be the dominant sources for atmospheric arsenic in the Northern and Southern Hemispheres, respectively. Asian emissions are found to contribute 39% and 38% of the total arsenic deposition over the Arctic and Northern America, respectively. Another 14% of the arsenic deposition to the Arctic region is attributed to European emissions. Our results indicate that the reduction of anthropogenic arsenic emissions in Asia and South America can significantly reduce arsenic pollution not only locally but also globally

Fast Time Resolution Oxidized Mercury Measurements during the Reno Atmospheric Mercury Intercomparison Experiment (RAMIX)

The Reno Atmospheric Mercury Intercomparison Experiment (RAMIX) was carried out from 22 August to 16 September, 2011 in Reno, NV to evaluate the performance of new and existing methods to measure atmospheric mercury (Hg). Measurements were made using a common sampling manifold to which controlled concentrations of Hg species, including gaseous elemental mercury (GEM) and HgBr₂ (a surrogate gaseous oxidized mercury (GOM) compound), and potential interferents were added. We present an analysis of Hg measurements made using the University of Washington’s Detector for Oxidized Hg Species (DOHGS), focusing on tests of GEM and HgBr₂ spike recovery, the potential for interference from ozone (O₃) and water vapor (WV), and temporal variability of ambient reactive mercury (RM). The mean GEM and HgBr₂ spike recoveries measured with the DOHGS were 95% and 66%, respectively. The DOHGS responded linearly to HgBr₂. We found no evidence that elevated O₃ interfered in the DOHGS RM measurements. A reduction in RM collection and retention efficiencies at very high ambient WV mixing ratios is possible. Comparisons between the DOHGS and participating Hg instruments demonstrate good agreement for GEM and large discrepancies for RM. The results suggest that existing GOM measurements are biased low

Impact of Wildfires on Ozone Exceptional Events in the Western U.S.

Wildfires generate substantial emissions of nitrogen oxides (NO_<i>x</i>) and volatile organic compounds (VOCs). As such, wildfires contribute to elevated ozone (O₃) in the atmosphere. However, there is a large amount of variability in the emissions of O₃ precursors and the amount of O₃ produced between fires. There is also significant interannual variability as seen in median O₃, organic carbon and satellite derived carbon monoxide mixing ratios in the western U.S. To better understand O₃ produced from wildfires, we developed a statistical model that estimates the maximum daily 8 h average (MDA8) O₃ as a function of several meteorological and temporal variables for three urban areas in the western U.S.: Salt Lake City, UT; Boise, ID; and Reno, NV. The model is developed using data from June-September 2000–2012. For these three locations, the statistical model can explain 60, 52, and 27% of the variability in daily MDA8. The Statistical Model Residual (SMR) can give information on additional sources of O₃ that are not explained by the usual meteorological pattern. Several possible O₃ sources can explain high SMR values on any given day. We examine several cases with high SMR that are due to wildfire influence. The first case considered is for Reno in June 2008 when the MDA8 reached 82 ppbv. The wildfire influence for this episode is supported by PM concentrations, the known location of wildfires at the time and simulations with the Weather and Research Forecasting Model with Chemistry (WRF-Chem) which indicates transport to Reno from large fires burning in California. The contribution to the MDA8 in Reno from the California wildfires is estimated to be 26 ppbv, based on the SMR, and 60 ppbv, based on WRF-Chem. The WRF-Chem model also indicates an important role for peroxyacetyl nitrate (PAN) in producing O₃ during transport from the California wildfires. We hypothesize that enhancements in PAN due to wildfire emissions may lead to regional enhancements in O₃ during high fire years. The second case is for the Salt Lake City (SLC) region for August 2012. During this period the MDA8 reached 83 ppbv and the SMR suggests a wildfire contribution of 19 ppbv to the MDA8. The wildfire influence is supported by PM_2.5 data, the known location of wildfires at the time, HYSPLIT dispersion modeling that indicates transport from fires in Idaho, and results from the CMAQ model that confirm the fire impacts. Concentrations of PM_2.5 and O₃ are enhanced during this period, but overall there is a poor relationship between them, which is consistent with the complexities in the secondary production of O₃. A third case looks at high MDA8 in Boise, ID, during July 2012 and reaches similar conclusions. These results support the use of statistical modeling as a tool to quantify the influence from wildfires on urban O₃ concentrations

Sequence data

MBO_mapping_file_impingers_controls_figshare.txt - A tab-delimited text file with sample information. The columns of the text file include a sample identifier ("SampleID"), barcode sequences ("BarcodeSequence"), forward primer sequence ("LinkerPrimerSequence"), date of sample collection ("Sample_date"), sample type (rDNA or rRNA, "Sample_type"), barcode, and sample description (samples versus controls, "Description").<div><br></div><div>seqs_figshare.fastq - Raw 16S sequence data in FASTQ format, produced by a sequencing run using Illumina MiSeq 300 bp single-end sequencing technology. </div

Do We Understand What the Mercury Speciation Instruments Are Actually Measuring? Results of RAMIX

From August 22 to September 16, 2012, atmospheric mercury (Hg) was measured from a common manifold in the field during the Reno Atmospheric Mercury Intercomparison eXperiment. Data were collected using Tekran systems, laser induced fluorescence, and evolving new methods. The latter included the University of Washington-Detector for Oxidized Mercury, the University of Houston Mercury instrument, and a filter-based system under development by the University of Nevada-Reno. Good transmission of total Hg was found for the manifold. However, despite application of standard protocols and rigorous quality control, systematic differences in operationally defined forms of Hg were measured by the sampling systems. Concentrations of reactive Hg (RM) measured with new methods were at times 2-to-3-fold higher than that measured by Tekran system. The low RM recovery by the latter can be attributed to lack of collection as the system is currently configured. Concentrations measured by all instruments were influenced by their sampling location in-the-manifold and the instrument analytical configuration. On the basis of collective assessment of the data, we hypothesize that reactions forming RM were occurring in the manifold. Results provide a new framework for improved understanding of the atmospheric chemistry of Hg

Regional Influence of Aerosol Emissions from Wildfires Driven by Combustion Efficiency: Insights from the BBOP Campaign

Wildfires are important contributors to atmospheric aerosols and a large source of emissions that impact regional air quality and global climate. In this study, the regional and nearfield influences of wildfire emissions on ambient aerosol concentration and chemical properties in the Pacific Northwest region of the United States were studied using real-time measurements from a fixed ground site located in Central Oregon at the Mt. Bachelor Observatory (∼2700 m a.s.l.) as well as near their sources using an aircraft. The regional characteristics of biomass burning aerosols were found to depend strongly on the modified combustion efficiency (MCE), an index of the combustion processes of a fire. Organic aerosol emissions had negative correlations with MCE, whereas the oxidation state of organic aerosol increased with MCE and plume aging. The relationships between the aerosol properties and MCE were consistent between fresh emissions (∼1 h old) and emissions sampled after atmospheric transport (6–45 h), suggesting that biomass burning organic aerosol concentration and chemical properties were strongly influenced by combustion processes at the source and conserved to a significant extent during regional transport. These results suggest that MCE can be a useful metric for describing aerosol properties of wildfire emissions and their impacts on regional air quality and global climate