Atmospheric Sciences Commons^™

Inverse Modeling Of Atmospheric Ch4 And Δ13C-Ch4 Measurements From Surface Observation Sites To Understand Trends In Global Methane Emissions Over More Than Three Decades, Sayantani Karmakar

Dissertations and Theses

Methane (CH₄) is the second most important greenhouse gas with a radiative forcing of 0.97 W/m² including both direct and indirect effects and a global warming potential of 28 over a 100-year time horizon. Unlike CO₂ whose rate of growth in the atmosphere has remained positive and increased in recent decades, the behavior of atmospheric methane is considerably more complex and is much less understood on account of the spatiotemporal variability of its emissions which include biogenic (e.g., wetlands, ruminants, rice agriculture), thermogenic (fossil fuels), and pyrogenic (i.e., biomass burning) sources. After sustained growth during most …

An Integrative Model For Soil Biogeochemistry And Methane Processes: I. Model Structure And Sensitivity Analysis, Daniel M. Ricciuto, Xiaofeng Xu, Xiaoying Shi, Yihui Wang, Xia Song, Christopher W. Schadt, Natalie A. Griffiths, Jiafu Mao, Jeffrey M. Warren, Peter E. Thornton, Jeff Chanton, Jason K. Keller, Scott D. Bridgham, Jessica Gutknecht, Stephen D. Sebestyen, Adrien Finzi, Randall Kolka, Paul J. Hanson

Biology, Chemistry, and Environmental Sciences Faculty Articles and Research

Environmental changes are anticipated to generate substantial impacts on carbon cycling in peatlands, affecting terrestrial-climate feedbacks. Understanding how peatland methane (CH₄) fluxes respond to these changing environments is critical for predicting the magnitude of feedbacks from peatlands to global climate change. To improve predictions of CH₄ fluxes in response to changes such as elevated atmospheric CO₂ concentrations and warming, it is essential for Earth system models to include increased realism to simulate CH₄ processes in a more mechanistic way. To address this need, we incorporated a new microbial-functional group-based CH₄ module into the Energy …

Predicting Spatial Patterns In Precipitation Isotope (Δ2h And Δ18o) Seasonality Using Sinusoidal Isoscapes, Scott T. Allen, James W. Kirchner, Gregory R. Goldsmith

Biology, Chemistry, and Environmental Sciences Faculty Articles and Research

Understanding how precipitation isotopes vary spatially and temporally is important for tracer applications. We tested how well month‐to‐month variations in precipitation δ18O and δ2H were captured by sinusoidal cycles, and how well spatial variations in these seasonal cycles could be predicted, across Switzerland. Sine functions representing seasonal cycles in precipitation isotopes explained between 47% and 94% of the variance in monthly δ18O and δ2H values at each monitoring site. A significant sinusoidal cycle was also observed in line‐conditioned excess. We interpolated the amplitudes, phases, and offsets of these sine functions across the landscape, using multiple linear …

Wildfire Emissions In The Context Of Global Change And The Implications For Mercury Pollution, Aditya Kumar

Dissertations, Master's Theses and Master's Reports

Wildfires are episodic disturbances that exert a significant influence on the Earth system. They emit substantial amounts of atmospheric pollutants, which can impact atmospheric chemistry/composition and the Earth’s climate at the global and regional scales. This work presents a collection of studies aimed at better estimating wildfire emissions of atmospheric pollutants, quantifying their impacts on remote ecosystems and determining the implications of 2000s-2050s global environmental change (land use/land cover, climate) for wildfire emissions following the Intergovernmental Panel on Climate Change (IPCC) A1B socioeconomic scenario.

A global fire emissions model is developed to compile global wildfire emission inventories for major atmospheric …

Multiple Metabolisms Constrain The Anaerobic Nitrite Budget In The Eastern Tropical South Pacific, Andrew R. Babbin, Brian D. Peters, Calvin W. Mordy, Brittany Widner, Karen L. Casciotti, Bess B. Ward

OES Faculty Publications

The Eastern Tropical South Pacific is one of the three major oxygen deficient zones (ODZs) in the global ocean and is responsible for approximately one third of marine water column nitrogen loss. It is the best studied of the ODZs and, like the others, features a broad nitrite maximum across the low oxygen layer. How the microbial processes that produce and consume nitrite in anoxic waters interact to sustain this feature is unknown. Here we used ¹⁵N-tracer experiments to disentangle five of the biologically mediated processes that control the nitrite pool, including a high-resolution profile of nitrogen loss rates. …

Unraveling The Fingerprints Of Nox Using Stable Isotopes: Implications For Nox Source Partitioning And Oxidation Chemistry, Wendell William Walters

Open Access Dissertations

The nitrogen (N) and oxygen (O) stable isotope composition (δ15N & δ18O) of nitrogen oxides (NOx )may be a useful tool for constraining NOx emission sources as well as for understanding the atmospheric oxidation pathways responsible for its removal if various NOx sources and sink processes exhibit characteristic isotopic compositions (“fingerprints”). However, this requires (1) an accurate and complete inventory of δ15N(NOx) values from major emission sources, (2) an assessment of the kinetic and equilibrium isotope effects that can impact δ15N and δ18O values of NOx, (3) and test these assumptions by conducting accurate in situ δ15N and δ18O measurements …

Source-Specific Molecular Signatures For Light-Absorbing Organic Aerosols, Amanda Susan Willoughby

Chemistry & Biochemistry Theses & Dissertations

Organic aerosols (OA) are universally regarded as an important component of the atmosphere based on quantitative significance as well as the far-reaching impact they have on global climate forcing and human health. Despite the acknowledged importance, OA amounts and impacts remain the largest uncertainties regarding radiative forcing estimates. Incomplete chemical characterization of aerosol organic matter (OM) and a lack of concrete source apportionment is a major source of this uncertainty. The primary focus of this study is to provide much needed molecular details regarding ambient OA from key emission sources, and establish links between molecular and optical properties.

Complete chemical …

Tb196: Temperature, Soil Moisture, And Streamflow At The Bear Brook Watershed In Maine (Bbwm), Ivan J. Fernandez, Joseph E. Karem, Stephen A. Norton, Lindsey E. Rustad

Ivan J. Fernandez

The Bear Brook Watershed in Maine is a whole-ecosystem chemical manipulation initiated in 1987 to study the effects of acid deposition on forests and surface waters. The focus of this research was to understand the biogeochemical response of watersheds with emphasis on chemistry and hydrology. In 2001 a program was initiated to provide more detailed measurements of temperature and moisture to examine critical linkages amongst chemical, biological, and physical processes that ultimately work together to define ecosystem function. The purpose of this publication is to provide data from the initial phase of soil temperature, air temperature, and soil moisture measurements …

The Great 2012 Arctic Ocean Summer Cyclone Enhanced Biological Productivity On The Shelves, Jinlun Zhang, Carin Ashjian, Robert Campbell, Victoria Hill, Yvette H. Spitz, Michael Steele

OES Faculty Publications

A coupled biophysical model is used to examine the impact of the great Arctic cyclone of early August 2012 on the marine planktonic ecosystem in the Pacific sector of the Arctic Ocean (PSA). Model results indicate that the cyclone influences the marine planktonic ecosystem by enhancing productivity on the shelves of the Chukchi, East Siberian, and Laptev seas during the storm. Although the cyclone's passage in the PSA lasted only a few days, the simulated biological effects on the shelves last 1 month or longer. At some locations on the shelves, primary productivity (PP) increases by up to 90% and …

Wetlands And Greenhouse Gas Fluxes: Causes And Effects Of Climate Change – A Meta-Analysis, Robert E. Ventura

Pomona Senior Theses

Climate change is one of the largest problems facing this generation. Anthropogenically caused increases of greenhouse gas emissions is a significant culprit to this problem. Although the obvious problems such as cars, industry, and urbanism garnish a significant amount of the criticism, natural sources such as wetlands are also beginning to contribute to this issue. This is becoming increasingly significant as wetlands shift from being sinks of greenhouse gases to becoming sources as various anthropogenic impacts, including global warming itself, begin to affect the health of the wetlands. The aim of this project is to look at four common types …

Atmospheric Methane Over The Arctic Ocean: Thermal Ir Satellite And Ship- Based Observations, Leonid Yurganov

Leonid Yurganov

Recent warming of the Arctic stimulated speculations about dissociation of methane hydrates in the Arctic seabed and a new climatic positive feedback. Here, for the first time, methane low tropospheric satellite retrievals over the Arctic from two instruments: AIRS (Atmospheric IR Sounder) and IASI (Infrared Atmospheric Sounding Interferometer) were analyzed. Analyzed are data for areas over open water with high values of the vertical thermal contrast (ThC, defined here as the temperature difference between the surface and altitude of 4 km); they have been found to be reliable. The seasonal cycles of the data well correlate with the cycles measured …

Water And Energy Balance Response Of A Riparian Wetland To The Removal Of Phragmites Australis, Phillip Mykleby

Department of Earth and Atmospheric Sciences: Dissertations, Theses, and Student Research

Vegetation and climate both play integral roles in water availability, particularly for arid to semi-arid regions. Changes in these variables can lead to extreme shortages in water for regions that rely on water for crop irrigation (i.e., the Great Plains). The objective of this study is to evaluate the impacts of vegetation on water availability in the Republican River basin in central Nebraska. Decreases in streamflow have been observed in the river basin for many years and, as a result, an invasive riparian plant species (Phragmites australis) is being removed in an effort to reduce evapotranspiration and reclaim …

A Paleoclimate Modeling Experiment To Calculate The Soil Carbon Respiration Flux For The Paleocene-Eocene Thermal Maximum, David M. Tracy

Masters Theses 1911 - February 2014

The Paleocene-Eocene Thermal Maximum (PETM) (55 million years ago) stands as the largest in a series of extreme warming (hyperthermal) climatic events, which are analogous to the modern day increase in greenhouse gas concentrations. Orbitally triggered (Lourens et al., 2005, Galeotti et al., 2010), the PETM is marked by a large (-3‰) carbon isotope excursion (CIE). Hypothesized to be methane driven, Zeebe et al., (2009) noted that a methane based release would only account for 3.5°C of warming. An isotopically heavier carbon, such as that of soil and C3 plants, has the potential to account for the …

Spatial Patterns Of Drought Triggers And Indicators, Joseph P. Robine

Department of Environmental Studies: Undergraduate Student Theses

Drought is a reoccurring phenomenon with widespread economic, social, and environmental impacts. Unlike other disasters, a drought cannot be easily detected. In addition, droughts are widespread and develop slowly over time making it difficult to detect its onset and monitor its severity and impacts. To assist in monitoring the severity and spatial extent of droughts, drought managers frequently use indicators and triggers. Drought indicators are meteorological or hydrological variables or indices that quantify or describe the level of drought severity. A drought trigger is a value of an indicator that initiates management and response actions. Despite the clear importance of …

Fossil And Contemporary Aerosol Particulate Organic Carbon In The Eastern United States: Implications For Deposition And Inputs To Watersheds, Andrew S. Wozniak, James E. Bauer, Rebecca M. Dickhut

Chemistry & Biochemistry Faculty Publications

Atmospheric particulate matter samples were collected from mid-Atlantic and northeastern U. S. (Virginia and New York, respectively) sites to assess the fossil versus contemporary sources contributing to aerosol organic carbon (OC) and the implications for its deposition to watersheds. Mean particulate matter total OC (TOC) deposition rates (wet + dry deposition) were calculated to be 1.6 and 2.4 mg C m^-2 d^-1 for the Virginia and New York sites, respectively. Wet deposition of particulate TOC was determined to be the dominant depositional mode, accounting for >65% (Virginia) and >80% (New York) of total aerosol TOC deposition. Isotopic mass …

On The Fractional Solubillity Of Copper In Marine Aerosols: Toxicity Of Aeolian Copper Revisited, Edward R. Sholkovitz, Peter N. Sedwick, Thomas M. Church

OES Faculty Publications

Paytan et al. (2009) argue that the atmospheric deposition of aerosols lead to copper concentrations that are potentially toxic to marine phytoplankton in a large area of tropical and subtropical North Atlantic Ocean. A key assumption in their model is that all marine aerosols (mineral dust and anthropogenic particles) have a high (40%) fractional solubility of copper. Our data show that the fractional solubility of copper for Saharan dust over the Sargasso Sea and Bermuda is significantly lower (1-7%). In contrast, anthropogenic aerosols with non-Saharan sources have significantly higher values (10-100%). Hence, the potential Cu toxicity in the tropical and …

Tb202: Composition And Biomass Of Forest Floor Vegetation In Experimentally Acidified Paired Watersheds At The Bear Brook Watershed In Maine, Peter Kenlan, G. B. Wiersma, A. S. White, I. J. Fernandez

Technical Bulletins

The percentage cover (abundance), frequency of occurrence, biomass, species richness, and species diversity of understory herbs was measured on a paired watershed ecosystem in eastern Maine, USA. This paired watershed site (Bear Brook Watershed in Maine, BBWM) has had the West Bear Brook Watershed treated bi-monthly with granular ammonium sulfate at a rate of 28.8 kg S ha-1 yr-1 and 25.2 kg N ha-1 yr-1 since 1989. East Bear Brook Watershed serves as the reference site. More than 100 plots were randomly located across the two watersheds. The data suggest that there is generally a lower frequency of occurrence of …

Anthropogenic Osmium In Rain And Snow Reveals Global-Scale Atmospheric Contamination, Cynthia Chen, Peter N. Sedwick, Mukul Sharma

OES Faculty Publications

Osmium is one of the rarer elements in seawater, with typical concentration of ≈10 x 10^-15 g g^-1 ( 5.3 x 10^-14 mol kg^-1. The osmium isotope composition (¹⁸⁷Os/¹⁸⁸Os ratio) of deep oceans is 1.05, reflecting a balance between inputs from continental crust (≈ 1.3) and mantle/cosmic dust (≈ 0.13). Here, we show that the ¹⁸⁷Os/¹⁸⁸Os ratios measured in rain and snow collected around the world range from 0.16 to 0.48, much lower than expected (>1), but similar to the isotope composition of ores (approximate to 0.2) …

From Debate To Design: Issues In Clean Energy And Climate Change Law And Policy, Leslie Parker, Jennifer Ronk, Rachel Maxwell, Bradford Gentry, Marijn Wilder, James Cameron

Yale School of the Environment Publications Series

A report on the work of the REIL Network 2007-2008

Technical Note: Molecular Characterization Of Aerosol-Derived Water Soluble Organic Carbon Using Ultrahigh Resolution Electrospray Ionization Fourier Transform Ion Cyclotron Resonance Mass Spectrometry, As Wosniak, Je Bauer, Rl Sleighter, Rm Dickhut, Pg Hatcher

VIMS Articles

Despite the acknowledged relevance of aerosol-derived water-soluble organic carbon (WSOC) to climate and biogeochemical cycling, characterization of aerosol WSOC has been limited. Electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI FT-ICR MS) was utilized in this study to provide detailed molecular level characterization of the hi(,h molecular weight (HMW; m/z>223) component of aerosol-derived WSOC collected from rural sites in Virginia and New York, USA. More than 3000 peaks were detected by ESI FT-ICR MS within a m/z range of 223-600 for each sample. Approximately 86% (Virginia) and 78% (New York) of these peaks were assigned molecular formulas …

Tb196: Temperature, Soil Moisture, And Streamflow At The Bear Brook Watershed In Maine (Bbwm), Ivan J. Fernandez, Joseph E. Karem, Stephen A. Norton, Lindsey E. Rustad

Technical Bulletins

The Bear Brook Watershed in Maine is a whole-ecosystem chemical manipulation initiated in 1987 to study the effects of acid deposition on forests and surface waters. The focus of this research was to understand the biogeochemical response of watersheds with emphasis on chemistry and hydrology. In 2001 a program was initiated to provide more detailed measurements of temperature and moisture to examine critical linkages amongst chemical, biological, and physical processes that ultimately work together to define ecosystem function. The purpose of this publication is to provide data from the initial phase of soil temperature, air temperature, and soil moisture measurements …

Iron In Ice Cores From Law Dome: A Record Of Atmospheric Iron Deposition For Maritime East Antarctica During The Holocene And Last Glacial Maximum, Ross Edwards, Peter N. Sedwick, Vin Morgan, Claude Boutron

OES Faculty Publications

Total dissolvable iron (TDFe) was measured in sections of ice cores recovered from Law Dome on the coast of Wilkes Land, East Antarctica. These samples include ice dating from the Last Glacial Maximum (LGM), the Last Deglaciation, and the early and mid Holocene as well as samples from the Anthropocene that have been dated with seasonal to annual resolution. Combining our TDFe concentration data with estimates of the ice accumulation rate, we estimate the atmospheric iron deposition for Law Dome and the adjacent Southern Ocean during these periods. Our results indicate that the atmospheric iron deposition flux to this region …

Monsoon-Driven Biogeochemical Processes In The Arabian Sea, Jerry D. Wiggert, Raleigh Hood, Karl Banse, John Kindle

Faculty Publications

Although it is nominally a tropical locale, the semiannual wind reversals associated with the Monsoon system of the Arabian Sea result annually in two distinct periods of elevated biological activity. While in both cases monsoonal forcing drives surface layer nutrient enrichment that supports increased rates of primary productivity, fundamentally different entrainment mechanisms are operating in summer (Southwest) and winter (Northeast) Monsoons. Moreover, the intervening intermonsoon periods, during which the region relaxes toward oligotrophic conditions more typical of tropical environments, provide a stark contrast to the dynamic biogeochemical activity of the monsoons. The resulting spatial and temporal variability is great and …

Sources And Cycling Of Carbonyl Sulfide In The Sargasso Sea, Gregory A. Cutter, Lynda S. Cutter, Katherine C. Filippino

OES Faculty Publications

The cycling of the radiatively important gas carbonyl sulfide (OCS) was studied in surface waters of the Sargasso Sea. In August 1999, surface OCS concentrations averaged 8.6 pmol L^-1, showed minor diel variations, and varied little with depth. An OCS precursor, total dissolved organic sulfur (DOS), was lowest at the surface (40 nmol L^-1) and increased with depth. The photoproduction rate of OCS from in situ incubations averaged 9.6 pmol L^-1 h^-1, whereas dark production was 7.0 pmol L^-1 h^-1. Apparent quantum yields were 10^-5-10^-7 from 313-436 …

New Evidence For Enhanced Ocean Primary Production Triggered By Tropical Cyclone, I. Lin, W. Timothy Liu, Chun-Chieh Wu, George T. F. Wong, Chuanmin Hu, Zhiqiang Chen, Wen-Der Liang, Yih Yang, Kon-Kee Liu

OES Faculty Publications

[1] New evidence based on recent satellite data is presented to provide a rare opportunity in quantifying the long-speculated contribution of tropical cyclones to enhance ocean primary production. In July 2000, moderate cyclone Kai-Tak passed over the South China Sea (SCS). During its short 3-day stay, Kai-Tak triggered an average 30-fold increase in surface chlorophyll-a concentration. The estimated carbon fixation resulting from this event alone is 0.8 Mt, or 2-4% of SCS's annual new production. Given an average of 14 cyclones passing over the SCS annually, we suggest the long-neglected contribution of tropical cyclones to SCS's annual new production may …

Dark Production: A Significant Source Of Oceanic Cos, M. Von Hobe, Gregory A. Cutter, A. J. Kettle, M. O. Andreae

OES Faculty Publications

Carbonyl sulfide (COS) in air and dissolved in seawater was determined during a cruise in August 1999 in the Sargasso Sea in the northwest Atlantic Ocean. Dissolved concentrations at the sea surface displayed only a weak diel cycle with a mean of 8.6 ± 2.8 pmol dm⁻³ owing to low abundance of photochemical precursors and high temperatures causing rapid hydrolysis. Depth profiles measured over the oceanic mixed layer revealed significant vertical gradients of COS concentration with higher values at the surface, suggesting that the rate of photochemical production at the surface exceeds the rate of vertical mixing. The mean …

A Numerical Model Of The Global Carbon Cycle To Predict Atmospheric Carbon Dioxide Concentrations, Alexis Demitrios Kambis

Dissertations, Theses, and Masters Projects

A numerical model of the global carbon cycle is presented which includes the effects of anthropogenic &CO\sb2& emissions &(CO\sb2& produced from fossil fuel combustion, biomass burning, and deforestation) on the global carbon cycle. The model is validated against measured atmospheric &CO\sb2& concentrations. Future levels of atmospheric &CO\sb2& are then predicted for the following scenarios: (1) Business as Usual (BaU) for the period 1990-2000; (2) Same as (1), but with no biomass burning; (3) Same as (1), but with no fossil fuel combustion; (4) Same as (1), but with a doubled atmospheric &CO\sb2& concentration and a 2 K warmer surface temperature …