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- All Subjects: Isotopes
- Creators: Herckes, Pierre
Description
This dissertation is presented in two sections. First, I explore two methods of using stable isotope analysis to trace environmental and biogeochemical processes. Second, I present two related studies investigating student understanding of the biogeochemical concepts that underlie part one. Fe and Hg are each biogeochemically important elements in their own way. Fe is a critical nutrient for phytoplankton, while Hg is detrimental to nearly all forms of life. Fe is often a limiting factor in marine phytoplankton growth. The largest source, by mass, of Fe to the open ocean is windblown mineral dust, but other more soluble sources are more bioavailable. To look for evidence of these non-soil dust sources of Fe to the open ocean, I measured the isotopic composition of aerosol samples collected on Bermuda. I found clear evidence in the fine size fraction of a non-soil dust Fe source, which I conclude is most likely from biomass burning. Widespread adoption of compact fluorescent lamps (CFL) has increased their importance as a source of environmental Hg. Isotope analysis would be a useful tool in quantifying this impact if the isotopic composition of Hg from CFL were known. My measurements show that CFL-Hg is isotopically fractionated, in a unique pattern, during normal operation. This fractionation is large and has a distinctive, mass-independent signature, such that CFL Hg can be uniquely identified from other sources. Misconceptions research in geology has been a very active area of research, but student thinking regarding the related field of biogeochemistry has not yet been studied in detail. From interviews with 40 undergraduates, I identified over 150 specific misconceptions. I also designed a multiple-choice survey (concept inventory) to measure understanding of these same biogeochemistry concepts. I present statistical evidence, based on the Rasch model, for the reliability and validity of this instrument. This instrument will allow teachers and researchers to easily quantify learning outcomes in biogeochemistry and will complement existing concept inventories in geology, chemistry, and biology.
ContributorsMead, Chris (Author) / Anbar, Ariel (Thesis advisor) / Semken, Steven (Committee member) / Shock, Everett (Committee member) / Herckes, Pierre (Committee member) / Hartnett, Hilairy (Committee member) / Arizona State University (Publisher)
Created2014
Description
Black carbon (BC) is the product of incomplete combustion of biomass and fossil fuels. It is found ubiquitously in nature and is relevant to studies in atmospheric science, soil science, oceanography, and anthropology. Black carbon is best described using a combustion continuum that sub-classifies BC into slightly charred biomass, char, charcoal and soot. These sub-classifications range in particle size, formation temperature, and relative reactivity. Interest in BC has increased because of its role in the long-term storage of organic matter and the biogeochemistry of urban areas. The global BC budget is unbalanced. Production of BC greatly outweighs decomposition of BC. This suggests that there are unknown or underestimated BC removal processes, and it is likely that some of these processes are occurring in soils. However, little is known about BC reactivity in soil and especially in desert soil. This work focuses on soot BC, which is formed at higher temperatures and has a lower relative reactivity than other forms of BC. Here, I assess the contribution of soot BC to central AZ soils and use the isotopic composition of soot BC to identify sources of soot BC. Soot BC is a significant (31%) fraction of the soil organic matter in central AZ and this work suggests that desert and urban soils may be a storage reservoir for soot BC. I further identify previously unknown removal processes of soot BC found naturally in soil and demonstrate that soil soot BC undergoes abiotic (photo-oxidation) and biotic reactions. Not only is soot BC degraded by these processes, but its chemical composition is altered, suggesting that soot BC contains some chemical moieties that are more reactive than others. Because soot BC demonstrates both refractory and reactive character, it is likely that the structure of soot BC; therefore, its interactions in the environment are complex and it is not simply a recalcitrant material.
ContributorsHamilton, George (Author) / Hartnett, Hilairy E (Thesis advisor) / Herckes, Pierre (Committee member) / Hall, Sharon (Committee member) / Arizona State University (Publisher)
Created2013
Description
Atmospheric deposition of iron (Fe) can limit primary productivity and carbon dioxide uptake in some marine ecosystems. Recent modeling studies suggest that biomass burning aerosols may contribute a significant amount of soluble Fe to the surface ocean. Existing studies of burn-induced trace element mobilization have often collected both entrained soil particles along with material from biomass burning, making it difficult to determine the actual source of aerosolized trace metals.
In order to better constrain the importance of biomass versus entrained soil as a source of trace metals in burn aerosols, small-scale burn experiments were conducted using soil-free foliage representative of a variety of fire-impacted ecosystems. The resulting burn aerosols were collected in two stages (PM > 2.5 μm and PM < 2.5 μm) on cellulose filters using a high-volume air sampler equipped with an all-Teflon impactor. Unburned foliage and burn aerosols were analyzed for Fe and other trace metals using inductively coupled plasma mass spectrometry (ICP-MS).
Results of this analysis show that less than 2% of Fe in plant biomass is likely mobilized as atmospheric aerosols during biomass burning events. The results of this study and estimates of annual global wildfire area were used to estimate the impact of biomass burning aerosols on total atmospheric Fe flux to the ocean. I estimate that foliage-derived Fe contributes 114 ± 57 Gg annually. Prior studies, which implicitly include both biomass and soil-derived Fe, concluded that biomass burning contributes approximately 690 Gg of Fe. Together, these studies suggest that fire-entrained soil particles contribute 83% (576 Gg) of Fe in biomass burning emissions, while plant derived iron only accounts for at most 17%.
In order to better constrain the importance of biomass versus entrained soil as a source of trace metals in burn aerosols, small-scale burn experiments were conducted using soil-free foliage representative of a variety of fire-impacted ecosystems. The resulting burn aerosols were collected in two stages (PM > 2.5 μm and PM < 2.5 μm) on cellulose filters using a high-volume air sampler equipped with an all-Teflon impactor. Unburned foliage and burn aerosols were analyzed for Fe and other trace metals using inductively coupled plasma mass spectrometry (ICP-MS).
Results of this analysis show that less than 2% of Fe in plant biomass is likely mobilized as atmospheric aerosols during biomass burning events. The results of this study and estimates of annual global wildfire area were used to estimate the impact of biomass burning aerosols on total atmospheric Fe flux to the ocean. I estimate that foliage-derived Fe contributes 114 ± 57 Gg annually. Prior studies, which implicitly include both biomass and soil-derived Fe, concluded that biomass burning contributes approximately 690 Gg of Fe. Together, these studies suggest that fire-entrained soil particles contribute 83% (576 Gg) of Fe in biomass burning emissions, while plant derived iron only accounts for at most 17%.
ContributorsSherry, Alyssa M (Author) / Anbar, Ariel D (Thesis advisor) / Herckes, Pierre (Thesis advisor) / Hartnett, Hilairy E (Committee member) / Fraser, Matthew (Committee member) / Arizona State University (Publisher)
Created2019
Description
Migrations, past and present, fundamentally influence human interaction, community building, and social evolution. Studies of contemporary migrations demonstrate that the form and intensity of interaction migrants maintain between homeland and host communities shape social dynamics, innovations, and identities. This dissertation applies a contemporary theoretical framework and biogeochemical analyses to elucidate the scale, processes, and impacts of migration in the hinterland of the pre-Hispanic Tiwanaku polity (ca. AD 500-1100). Social diversity is examined by reconstructing the migration histories and dietary choices of individuals interred at the Tiwanaku-affiliated site of Omo M10 in the Moquegua Valley of southern Peru.
Radiogenic strontium and stable oxygen isotope data from human dental and skeletal elements are used to characterize intra- and inter-individual paleomobility patterns at Omo M10. When contextualized with archaeological evidence, these data reveal multigenerational interaction through migration between communities in the highland Tiwanaku heartland and at Omo M10. The observed greater mobility of females and juveniles at Omo M10 indicates that women and families played an essential role in maintaining social relationships and persistent cultural continuity in Moquegua Tiwanaku life. Contact with the highlands waned over time as disruption in the urban highland centers likely weakened ties to peripheral lowland communities.
Stable carbon and nitrogen data from human dental and skeletal elements are employed to estimate intra- and inter-individual paleodietary patterns. Results indicate diet at Omo M10 varied depending on an individual’s community affiliation, sex, age, and level of mobility; diet broadly changed over time with shifting levels of interaction with highland Tiwanaku communities. Intra-individual biogeochemical analyses of migration and diet at Omo M10 contribute a nuanced perspective on the diverse experiences of multigenerational colonists on the periphery of the Tiwanaku polity.
Radiogenic strontium and stable oxygen isotope data from human dental and skeletal elements are used to characterize intra- and inter-individual paleomobility patterns at Omo M10. When contextualized with archaeological evidence, these data reveal multigenerational interaction through migration between communities in the highland Tiwanaku heartland and at Omo M10. The observed greater mobility of females and juveniles at Omo M10 indicates that women and families played an essential role in maintaining social relationships and persistent cultural continuity in Moquegua Tiwanaku life. Contact with the highlands waned over time as disruption in the urban highland centers likely weakened ties to peripheral lowland communities.
Stable carbon and nitrogen data from human dental and skeletal elements are employed to estimate intra- and inter-individual paleodietary patterns. Results indicate diet at Omo M10 varied depending on an individual’s community affiliation, sex, age, and level of mobility; diet broadly changed over time with shifting levels of interaction with highland Tiwanaku communities. Intra-individual biogeochemical analyses of migration and diet at Omo M10 contribute a nuanced perspective on the diverse experiences of multigenerational colonists on the periphery of the Tiwanaku polity.
ContributorsDahlstedt, Allisen Cecelia (Author) / Knudson, Kelly J. (Thesis advisor) / Buikstra, Jane E. (Committee member) / Goldstein, Paul S (Committee member) / Arizona State University (Publisher)
Created2019
Description
Iron (Fe) scarcity limits biological productivity in high-nutrient low-chlorophyll (HNLC) ocean regions. Thus, the input, output and abundance of Fe in seawater likely played a critical role in shaping the development of modern marine ecosystems and perhaps even contributed to past changes in Earth’s climate. Three sources of Fe—wind-blown dust, hydrothermal activity, and sediment dissolution—carry distinct Fe isotopic fingerprints, and can therefore be used to track Fe source variability through time. However, establishing the timing of this source variability through Earth’s history remains challenging because the major depocenters for dissolved Fe in the ocean lack well-established chronologies. This is due to the fact that they are difficult to date with traditional techniques such as biostratigraphy and radiometric dating. Here, I develop age models for sediments collected from the International Drilling Program Expedition 329 by measuring the Os (osmium) isotopic composition of the hydrogenous portion of the clays. These extractions enable dating of the clays by aligning the Os isotope patterns observed in the clays to those in a reference curve with absolute age constraints through the Cenozoic. Our preliminary data enable future development of chronologies for three sediment cores from the high-latitude South Pacific and Southern Oceans, and demonstrate a wider utility of this method to establish age constraints on pelagic sediments worldwide. Moreover, the preliminary Os isotopic data provides a critical first step needed to examine the changes in Fe (iron) sources and cycling on millions of years timescales. Fe isotopic analysis was conducted at the same sites in the South Pacific and demonstrates that there are significant changes in the sources of Fe to the Southern Ocean over the last 90 Ma. These results lay the groundwork for the exploration of basin-scale sources to Fe source changes, which will have implications for understanding how biological productivity relates to Fe source variability over geological timescales.
ContributorsTegler, Logan Ashley (Author) / Anbar, Ariel (Thesis director) / Herckes, Pierre (Committee member) / Romaniello, Stephen (Committee member) / Department of English (Contributor) / School of Molecular Sciences (Contributor) / Barrett, The Honors College (Contributor)
Created2018-05