[1] The formation of secondary organic aerosol (SOA) in an anthropogenic-influenced region in the southeastern United States is investigated by a comparison with urban plumes in the northeast. The analysis is based on measurements of fine-particle organic compounds soluble in water (WSOC) as a measure of secondary organic aerosol. Aircraft measurements over a large area of northern Georgia, including the Atlanta metropolitan region, and in plumes from New York City and surrounding urban regions in the northeast show that fine-particle WSOC are spatially correlated with vehicle emission tracers (e.g., CO), yet the measurements indicate that vehicles do not directly emit significant particulate WSOC. In addition to being correlated, WSOC concentrations were in similar proportions to anthropogenic tracers in both regions, despite biogenic volatile organic compounds (VOCs) that were on average 10-100 times higher over northern Georgia. In contrast, radiocarbon analysis on WSOC extracted from integrated filters deployed in Atlanta suggests that roughly 70-80% of the carbon in summertime WSOC is modern. If both findings are valid, the combined results indicate that in northern Georgia, fine-particle WSOC was secondary and formed through a process that involves mainly modern biogenic VOCs but which is strongly linked to an anthropogenic component that may largely control the mass of SOA formed. Independent of the radiocarbon results, a strong association between SOA and anthropogenic sources has implications for control strategies in urban regions with large biogenic VOC emissions.Citation: Weber, R. J., et al. (2007), A study of secondary organic aerosol formation in the anthropogenic-influenced southeastern United States,

Light absorption of fine particle (PM_2.5) aqueous extracts between wavelengths of 200 and 800 nm were investigated from two data sets: 24-h Federal Reference Method (FRM) filter extracts from 15 Southeastern US monitoring sites over the year of 2007 (900 filters), and online measurements from a Particle-Into-Liquid Sampler deployed from July to mid-August 2009 in Atlanta, Georgia. Three main sources of soluble chromophores were identified: biomass burning, mobile source emissions, and compounds linked to secondary organic aerosol (SOA) formation. Absorption spectra of aerosol solutions from filter extracts were similar for different sources. Angstrom exponents were ~7±1 for biomass burning and non-biomass burning-impacted 24-h filter samples (delineated by a levoglucosan concentration of 50 ng m⁻³) at both rural and urban sites. The absorption coefficient from measurements averaged between wavelength 360 and 370 nm (Abs₃₆₅, in units m⁻¹) was used as a measure of overall brown carbon light absorption. Biomass-burning-impacted samples were highest during winter months and Abs₃₆₅ was correlated with levoglucosan at all sites. During periods of little biomass burning in summer, light absorbing compounds were still ubiquitous and correlated with fine particle Water-Soluble Organic Carbon (WSOC), but comprised a much smaller fraction of the WSOC, where Abs₃₆₅/WSOC (i.e., mass absorption efficiency) was typically ~3 times higher in biomass burning-impacted samples. Factor analysis attributed 50% of the yearly average Abs₃₆₅ to biomass burning sources. Brown carbon from primary urban emissions (mobile sources) was also observed and accounted for ~10% of the regional yearly average Abs₃₆₅. Summertime diurnal profiles of Abs₃₆₅ and WSOC showed that morning to midday increases in WSOC from photochemical production were associated with a decrease in Abs₃₆₅/WSOC. After noon, this ratio substantially increased, indicating that either some fraction of the non-light absorbing fresh SOA was rapidly (within hours) converted to chromophores heterogeneously, or that SOA from gas-particle partitioning later in the day was more light-absorbing. Factor analysis on the 24-h integrated filter data associated ~20 to 30% of Abs₃₆₅ over 2007 with a secondary source that was highest in summer and also the main source for oxalate, suggesting that aqueous phase reactions may account for the light-absorbing fraction of WSOC observed throughout the Southeastern US in summer

A chemical mass balance (CMB) receptor model using particle-phase organic compounds as tracers is applied to apportion the primary source contributions to fine particulate matter and fine particulate organic carbon concentrations in the southeastern United States to determine the seasonal variability of these concentrations. Source contributions to particles with aerodynamic diameter < or =2.5 microm (PM2.5) collected from four urban and four rural/suburban sites in AL, FL, GA, and MS during April, July, and October 1999 and January 2000 are calculated and presented. Organic compounds in monthly composite samples at each site are identified and quantified by gas chromatography/mass spectrometry and are used as molecular markers in the CMB model. The major contributors to identified PM2.5 organic carbon concentrations at these sites in the southeastern United States include wood combustion (25-66%), diesel exhaust (14-30%), meat cooking (5-12%), and gasoline-powered motor vehicle exhaust (0-10%), as well as smaller but statistically significant contributions from natural gas combustion, paved road dust, and vegetative detritus. The primary sources determined in the present study when added to secondary aerosol formation account for on average 89% of PM2.5 mass concentrations, with the major contributors to PM2.5 mass as secondary sulfate (30+/-6%), wood combustion (15+/-12%), diesel exhaust (16+/-7%), secondary ammonium (8+/-2%), secondary nitrate (4+/-3%), meat cooking (3+/-2%), gasoline-powered motor vehicle exhaust (2+/-2%), and road dust (2+/-2%). Distinct seasonality is observed in source contributions, including higher contributions from wood combustion during the colder months of October and January. In addition, higher percentages of unexplained fine organic carbon concentrations are observed in July, which are likely due to an increase in secondary organic aerosol formation during the summer season.

Neurovascular coupling reflects the close temporal and regional linkage between neural activity and cerebral blood flow. Although providing mechanistic insight, our understanding of neurovascular coupling is largely limited to nonphysiological ex vivo preparations and non-human models using sedatives/anesthetics with confounding cerebrovascular implications. Herein, with particular focus on humans, we review the present mechanistic understanding of neurovascular coupling and highlight current approaches to assess these responses and the application in health and disease. Moreover, we present new guidelines for standardizing the assessment of neurovascular coupling in humans. To improve the reliability of measurement and related interpretation, the utility of new automated software for neurovascular coupling is demonstrated, which provides the capacity for coalescing repetitive trials and time intervals into single contours and extracting numerous metrics (e.g., conductance and pulsatility, critical closing pressure, etc.) according to patterns of interest (e.g., peak/minimum response, time of response, etc.). This versatile software also permits the normalization of neurovascular coupling metrics to dynamic changes in arterial blood gases, potentially influencing the hyperemic response. It is hoped that these guidelines, combined with the newly developed and openly available software, will help to propel the understanding of neurovascular coupling in humans and also lead to improved clinical management of this critical physiological function.