Christine Wiedinmyer

Quantifying the seasonal and interannual variability of North American isoprene emissions using satellite observations of the formaldehyde column

JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 111, D12315, doi:10.1029/2005JD006689, 2006 Quantifying the seasonal and interannual variability of North American isoprene emissions using satellite observations of the formaldehyde column Paul I. Palmer, 1,2 Dorian S. Abbot, 1 Tzung-May Fu, 1 Daniel J. Jacob, 1 Kelly Chance, 3 Thomas P. Kurosu, 3 Alex Guenther, 4 Christine Wiedinmyer, 4 Jenny C. Stanton, 5 Michael J. Pilling, 5 Shelley N. Pressley, 6 Brian Lamb, 6 and Anne Louise Sumner 7 Received 20 September 2005; revised 19 December 2005; accepted 14 February 2006; published 27 June 2006. [ 1 ] Quantifying isoprene emissions using satellite observations of the formaldehyde (HCHO) columns is subject to errors involving the column retrieval and the assumed relationship between HCHO columns and isoprene emissions, taken here from the GEOS- CHEM chemical transport model. Here we use a 6-year (1996–2001) HCHO column data set from the Global Ozone Monitoring Experiment (GOME) satellite instrument to (1) quantify these errors, (2) evaluate GOME-derived isoprene emissions with in situ flux measurements and a process-based emission inventory (Model of Emissions of Gases and Aerosols from Nature, MEGAN), and (3) investigate the factors driving the seasonal and interannual variability of North American isoprene emissions. The error in the GOME HCHO column retrieval is estimated to be 40%. We use the Master Chemical Mechanism (MCM) to quantify the time-dependent HCHO production from isoprene, a- and b-pinenes, and methylbutenol and show that only emissions of isoprene are detectable by GOME. The time-dependent HCHO yield from isoprene oxidation calculated by MCM is 20–30% larger than in GEOS-CHEM. GOME-derived isoprene fluxes track the observed seasonal variation of in situ measurements at a Michigan forest site with a 30% bias. The seasonal variation of North American isoprene emissions during 2001 inferred from GOME is similar to MEGAN, with GOME emissions typically 25% higher (lower) at the beginning (end) of the growing season. GOME and MEGAN both show a maximum over the southeastern United States, but they differ in the precise location. The observed interannual variability of this maximum is 20–30%, depending on month. The MEGAN isoprene emission dependence on surface air temperature explains 75% of the month-to-month variability in GOME-derived isoprene emissions over the southeastern United States during May–September 1996–2001. Citation: Palmer, P. I., et al. (2006), Quantifying the seasonal and interannual variability of North American isoprene emissions using satellite observations of the formaldehyde column, J. Geophys. Res., 111, D12315, doi:10.1029/2005JD006689. 1. Introduction [ 2 ] Emissions of volatile organic compounds (VOCs) from the terrestrial biosphere have important implications Division of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts, USA. Now at the School of Earth and Environment, University of Leeds, Leeds, UK. Harvard-Smithsonian Center for Astrophysics, Cambridge, Massachu- setts, USA. National Center for Atmospheric Research, Boulder, Colorado, USA. Department of Chemistry, University of Leeds, Leeds, UK. Department of Civil and Environmental Engineering, Washington State University, Pullman, Washington, USA. Battelle, Columbus, Ohio, USA. Copyright 2006 by the American Geophysical Union. 0148-0227/06/2005JD006689 for tropospheric ozone (O 3 ) [Wang and Shallcross, 2000], organic aerosols [Claeys et al., 2004], and climate change [Sanderson et al., 2003]. Local VOC emission data, representative of scales less than 1 km, are difficult to extrapolate, and consequently the magnitude and variabil- ity of these emissions is not well understood on conti- nental scales. Standard emission inventories based on ecosystem data and emission factors [Guenther et al., 2005] are poorly constrained. We have shown previously that observations of formaldehyde (HCHO) columns from the Global Ozone Monitoring Experiment (GOME) satel- lite instrument [Chance et al., 2000] provide information to estimate biogenic VOC emissions, specifically isoprene emissions, on a global scale and with resolution of the order of 100 km [Palmer et al., 2003]. We examine here the quantitative value of these data for better understand- D12315 1 of 14

Characterization of Airborne Microbial Communities at a High-Elevation Site and Their Potential To Act as Atmospheric Ice Nuclei

ABSTRACT Bacteria and fungi are ubiquitous in the atmosphere. The diversity and abundance of airborne microbes may be strongly influenced by atmospheric conditions or even influence atmospheric conditions themselves by acting as ice nucleators. However, few comprehensive studies have described the diversity and dynamics of airborne bacteria and fungi based on culture-independent techniques. We document atmospheric microbial abundance, community composition, and ice nucleation at a high-elevation site in northwestern Colorado. We used a standard small-subunit rRNA gene Sanger sequencing approach for total microbial community analysis and a bacteria-specific 16S rRNA bar-coded pyrosequencing approach (4,864 sequences total). During the 2-week collection period, total microbial abundances were relatively constant, ranging from 9.6 × 105 to 6.6 × 106 cells m−3 of air, and the diversity and composition of the airborne microbial communities were also relatively static. Bacteria and fungi were nearly equivalent, and members of the proteobacterial groups Burkholderiales and Moraxellaceae (particularly the genus Psychrobacter) were dominant. These taxa were not always the most abundant in freshly fallen snow samples collected at this site. Although there was minimal variability in microbial abundances and composition within the atmosphere, the number of biological ice nuclei increased significantly during periods of high relative humidity. However, these changes in ice nuclei numbers were not associated with changes in the relative abundances of the most commonly studied ice-nucleating bacteria.

Transport of Asian ozone pollution into surface air over the western United States in spring

and satellite measurements in May–June 2010 with a new global high-resolution (50 50 km 2 ) chemistry-climate model (GFDL AM3). We find that AM3 with full stratosphere-troposphere chemistry nudged to reanalysis winds successfully reproduces observed sharp ozone gradients above California, including the interleaving and mixing of Asian pollution and stratospheric air associated with complex interactions of midlatitude cyclone air streams. Asian pollution descends isentropically behind cold fronts; at 800 hPa a maximum enhancement to ozone occurs over the southwestern U.S., including the densely populated Los Angeles Basin. During strong episodes, Asian emissions can contribute 8–15 ppbv ozone in the model on days when observed daily maximum 8-h average ozone (MDA8 O3) exceeds 60 ppbv. We find that in the absence of Asian anthropogenic emissions, 20% of MDA8 O3 exceedances of 60 ppbv in the model would not have occurred in the southwestern USA. For a 75 ppbv threshold, that statistic increases to 53%. Our analysis indicates the potential for Asian emissions to contribute to high-O3 episodes over the high-elevation western USA, with implications for attaining more stringent ozone standards in this region. We further demonstrate a proof-of-concept approach using satellite CO column measurements as a qualitative early warning indicator to forecast Asian ozone pollution events in the western U.S. with lead times of 1–3 days.

A preliminary synthesis of modeled climate change impacts on U.S. regional ozone concentrations.

This paper provides a synthesis of results that have emerged from recent modeling studies of the potential sensitivity of U.S. regional ozone (O3) concentrations to global climate change (ca. 2050). This research has been carried out under the auspices of an ongoing U.S. Environmental Protection Agency (EPA) assessment effort to increase scientific understanding of the multiple complex interactions among climate, emissions, atmospheric chemistry, and air quality. The ultimate goal is to enhance the ability of air quality managers to consider global change in their decisions through improved characterization of the potential effects of global change on air quality, including O3 The results discussed here are interim, representing the first phase of the EPA assessment. The aim in this first phase was to consider the effects of climate change alone on air quality, without accompanying changes in anthropogenic emissions of precursor pollutants. Across all of the modeling experiments carried out by the differe...

Estimates of CO2 from fires in the United States: implications for carbon management

BackgroundFires emit significant amounts of CO2 to the atmosphere. These emissions, however, are highly variable in both space and time. Additionally, CO2 emissions estimates from fires are very uncertain. The combination of high spatial and temporal variability and substantial uncertainty associated with fire CO2 emissions can be problematic to efforts to develop remote sensing, monitoring, and inverse modeling techniques to quantify carbon fluxes at the continental scale. Policy and carbon management decisions based on atmospheric sampling/modeling techniques must account for the impact of fire CO2 emissions; a task that may prove very difficult for the foreseeable future. This paper addresses the variability of CO2 emissions from fires across the US, how these emissions compare to anthropogenic emissions of CO2 and Net Primary Productivity, and the potential implications for monitoring programs and policy development.ResultsAverage annual CO2 emissions from fires in the lower 48 (LOWER48) states from 2002–2006 are estimated to be 213 (± 50 std. dev.) Tg CO2 yr-1 and 80 (± 89 std. dev.) Tg CO2 yr-1 in Alaska. These estimates have significant interannual and spatial variability. Needleleaf forests in the Southeastern US and the Western US are the dominant source regions for US fire CO2 emissions. Very high emission years typically coincide with droughts, and climatic variability is a major driver of the high interannual and spatial variation in fire emissions. The amount of CO2 emitted from fires in the US is equivalent to 4–6% of anthropogenic emissions at the continental scale and, at the state-level, fire emissions of CO2 can, in some cases, exceed annual emissions of CO2 from fossil fuel usage.ConclusionThe CO2 released from fires, overall, is a small fraction of the estimated average annual Net Primary Productivity and, unlike fossil fuel CO2 emissions, the pulsed emissions of CO2 during fires are partially counterbalanced by uptake of CO2 by regrowing vegetation in the decades following fire. Changes in fire severity and frequency can, however, lead to net changes in atmospheric CO2 and the short-term impacts of fire emissions on monitoring, modeling, and carbon management policy are substantial.

Seasonal variability in bacterial and fungal diversity of the near-surface atmosphere.

Bacteria and fungi are ubiquitous throughout the Earths lower atmosphere where they often represent an important component of atmospheric aerosols with the potential to impact human health and atmospheric dynamics. However, the diversity, composition, and spatiotemporal dynamics of these airborne microbes remain poorly understood. We performed a comprehensive analysis of airborne microbes across two aerosol size fractions at urban and rural sites in the Colorado Front Range over a 14-month period. Coarse (PM10-2.5) and fine (PM2.5) particulate matter samples were collected at weekly intervals with both bacterial and fungal diversity assessed via high-throughput sequencing. The diversity and composition of the airborne communities varied across the sites, between the two size fractions, and over time. Bacteria were the dominant type of bioaerosol in the collected air samples, while fungi and plants (pollen) made up the remainder, with the relative abundances of fungi peaking during the spring and summer months. As bacteria made up the majority of bioaerosol particles, we analyzed the bacterial communities in greater detail using a bacterial-specific 16S rRNA gene sequencing approach. Overall, bacterial taxonomic richness and the relative abundances of specific bacterial taxa exhibited significant patterns of seasonality. Likewise, airborne bacterial communities varied significantly between sites and across aerosol size fractions. Source-tracking analyses indicate that soils and leaves represented important sources of bacteria to the near-surface atmosphere across all locations with cow fecal bacteria also representing an important source of bioaerosols at the more rural sites during early fall and early spring. Together, these data suggest that a complex set of environmental factors, including changes in atmospheric conditions and shifts in the relative importance of available microbial sources, act to control the composition of microbial bioaerosols in rural and urban environments.

Prescribed Fire As a Means of Reducing Forest Carbon Emissions in the Western United States

Carbon sequestration by forested ecosystems offers a potential climate change mitigation benefit. However, wildfire has the potential to reverse this benefit In the western United States, climate change and land management practices have led to increases in wildfire intensity and size. One potential means of reducing carbon emissions from wildfire is the use of prescribed burning,which consumes less biomass and therefore releases less carbon to the atmosphere. This study uses a regional fire emissions model to estimate the potential reduction in fire emissions when prescribed burning is applied in dry, temperate forested systems of the western U.S. Daily carbon dioxide (CO(2)) fire emissions for 2001-2008 were calculated for the western U.S. for two cases: a default wildfire case and one in which prescribed burning was applied. Wide-scale prescribed fire application can reduce CO(2) fire emissions for the western U.S. by 18-25%1 in the western U.S., and by as much as 60% in specific forest systems. Although this work does not address important considerations such as the feasibility of implementing wide-scale prescribed fire management or the cumulative emissions from repeated prescribed burning, it does provide constraints on potential carbon emission reductions when prescribed burning is used.

Future Changes in Biogenic Isoprene Emissions: How Might They Affect Regional and Global Atmospheric Chemistry?

Abstract Isoprene is emitted from vegetation to the atmosphere in significant quantities, and it plays an important role in the reactions that control tropospheric oxidant concentrations. As future climatic and land-cover changes occur, the spatial and temporal variations, as well as the magnitude of these biogenic isoprene emissions, are expected to change. This paper presents a study of the change in biogenic isoprene emissions that would result from both anthropogenic land-cover and climate-driven changes. Annual global isoprene emissions were estimated to be 522 Tg yr−1 under current climatological and land-cover conditions. When climate-driven land-cover changes are predicted, but climate does not change, total global emissions did not change significantly, although regional impacts were important. However, the use of future temperature and land-cover drivers to estimate isoprene emissions produced a global estimate of 889 Tg yr−1. Anthropogenic land-cover changes, such as urbanization and changes of...

What we breathe impacts our health: improving understanding of the link between air pollution and health

Air pollution contributes to the premature deaths of millions of people each year around the world, and air quality problems are growing in many developing nations. While past policy efforts have succeeded in reducing particulate matter and trace gases in North America and Europe, adverse health effects are found at even these lower levels of air pollution. Future policy actions will benefit from improved understanding of the interactions and health effects of different chemical species and source categories. Achieving this new understanding requires air pollution scientists and engineers to work increasingly closely with health scientists. In particular, research is needed to better understand the chemical and physical properties of complex air pollutant mixtures, and to use new observations provided by satellites, advanced in situ measurement techniques, and distributed micro monitoring networks, coupled with models, to better characterize air pollution exposure for epidemiological and toxicological research, and to better quantify the effects of specific source sectors and mitigation strategies.

Global Emissions of Trace Gases, Particulate Matter, and Hazardous Air Pollutants from Open Burning of Domestic Waste

The open burning of waste, whether at individual residences, businesses, or dump sites, is a large source of air pollutants. These emissions, however, are not included in many current emission inventories used for chemistry and climate modeling applications. This paper presents the first comprehensive and consistent estimates of the global emissions of greenhouse gases, particulate matter, reactive trace gases, and toxic compounds from open waste burning. Global emissions of CO2 from open waste burning are relatively small compared to total anthropogenic CO2; however, regional CO2 emissions, particularly in many developing countries in Asia and Africa, are substantial. Further, emissions of reactive trace gases and particulate matter from open waste burning are more significant on regional scales. For example, the emissions of PM10 from open domestic waste burning in China is equivalent to 22% of Chinas total reported anthropogenic PM10 emissions. The results of the emissions model presented here suggest that emissions of many air pollutants are significantly underestimated in current inventories because open waste burning is not included, consistent with studies that compare model results with available observations.