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Fluids can cycle and migrate through planetary bodies, transporting soluble ions and influencing physical properties of the surrounding rock or magma, such as fracture toughness, seismic wave velocity, melting point, viscosity, and more. Precipitated minerals, fluids trapped in inclusions, and free pore fluids can be used to constrain fluid provenance, mixing relationships, and paleoenvironmental information such as temperature, pressure, redox conditions, salinity, and pH. In my thesis, I discuss my research on topics pertaining to the geochemistry associated with fluid-rock interactions that occur from the depths of the lithospheric mantle to Earth\u2019s surface. Broadly, these chapters address open questions pertaining to 1) the retention timescales and metasomatic overprinting of fluids sourced from the mantle in obducted peridotites, 2) the capacity for pedogenic Mg-carbonates to preserve palaeohydrological information with implications for Martian carbonates, and 3) the influences hydrous fluids have on lithospheric magmas and minerals.
\r\n\r\nHelium isotopes are arguably the best tracer for fluid sources in Earth materials at the planetary scale. \u00b3He/\u2074He ratios of the Earth\u2019s 1) continental crust, 2) atmosphere, 3) upper mantle, and 4) core or deep isolated mantle (mantle plume source) vary by over two orders of magnitude, offering considerable dynamic range compared to measurement precision. While helium isotope signatures in Earth\u2019s mantle have been determined almost exclusively by the analysis of helium retained in mantle xenoliths, phenocrysts, erupted glasses, and vent gases, this selection introduces a sampling bias towards fluids that have been transported to Earth\u2019s surface by eruptive processes. In contrast, residual mantle peridotites take much longer to arrive at Earth\u2019s surface and are therefore more susceptible to metasomatic processes that can overprint primary helium isotopic signatures. In Chapter 1, I use concentrations and isotopes of helium and argon along with concentrations of U and Th to place constraints on the sources and siting of helium retained in exhumed mantle peridotites collected from Twin Sisters Mountain of the Northern Cascades in Washington State, USA. Helium isotope ratios of peridotites from the Twin Sisters Mountain span from 0.8 to 6 times the atmospheric ratio (1RA=1.4*10\u207b\u2076 \u00b3He/\u2074He). Fluid inclusions in these peridotites capture a two-component mixture that included a mantle-like endmember (~6 RA) and a serpentinizing endmember (1.0 \u00b1 0.5 RA) that is consistent with a mixture of surface-derived groundwater, leached crustal radiogenic helium and reworked mantle helium. While these components are not effectively isolated by extraction using vacuum crushing and powder fusion, step-heating analysis reveals that the serpentinizing endmember is released at lower temperatures (<1000\u00b0C) and the mantle-like endmember is released at higher temperatures. Results demonstrate that helium signatures can be retained in lithospheric peridotites against both diffusive loss and radiogenic ingrowth over at least 10\u2078-year timescales but can be greatly modified by cryptic metasomatic processes during emplacement.
\r\n\r\nMg-carbonates have become increasingly relevant in the scientific community due to their orbital and in situ detection on the Martian surface. Like Ca-carbonate on Earth, Martian Mg-carbonates may preserve paleoenvironmental information associated with their formation on Mars billions of years ago, shedding light on habitability. Yet, unlike Ca-carbonates, the capacity for Mg-carbonates to preserve paleoenvironmental information through trace element signatures associated with their source fluids has not been well established for surficial magnesite samples on Earth. In Chapter 2, I 1) develop a digestion protocol to selectively digest Mg-carbonates (magnesite \u00b1 dolomite) while obviating influences of contaminant phases and ions adsorbed to mineral surfaces, 2) validate a method to analyze trace elements with Mg-matrix by solution ICP-MS, and 3) apply these procedures to determine trace element concentrations of pedogenic Mg-carbonates sampled along a depth profile in the Kunwarara open pit magnesite mine in Queensland, Australia. Results from this study confirm that the method we implemented selectively digests magnesite \u00b1 dolomite. A relationship between negative Ce anomaly in the carbonates and Fe/Mn-oxides/hydroxides in corresponding host sediment collected along the depth profile demonstrates that pedogenic magnesites can capture redox gradients in the soil column. This finding implies that Ce anomaly in carbonates can potentially be used to place constraints on the paleo-redox conditions associated with Mg-carbonate formation on ancient Mars.
\r\n\r\nNumerous questions in Earth science depend on quantitative understanding of how elements fractionate during melting and crystallization. To name a few: assessment of how lithospheric fluids influence geodynamical processes, constraining mechanisms that led to the formation of the Earth\u2019s continental crust, evaluation of elemental fluxes from the mantle to Earth's surface, calibration of a reliable crustal barometer, and gauging how magmatism and plate tectonics differed with the higher geothermal gradients of a younger Earth. MELTS thermodynamic software is a widely available free tool utilized by geoscientists to both test hypotheses and model the geochemistry of magmatic processes. However, minerals of the amphibole supergroup, although common in magmatic systems, rarely crystallize in MELTS simulations, even when well controlled experiments demonstrate that they should. The decrease in the Gibbs energy needed to stabilize amphibole in MELTS is often on the order of the configurational entropy contribution to the Gibbs energy associated with minor elements that are not present in any of the current amphibole solution models used in MELTS but are frequently incorporated in the amphibole crystal lattice. In Chapter 3, I outline a framework for a volume model for monoclinic amphiboles that can be used in an expanded amphibole solution model to be incorporated in MELTS software. A volume model is prerequisite to calibrating the other model terms because it accounts for differences in pressure among experimental constraints. The framework I develop extends the model to include minor components that are not present in existing versions of the MELTS amphibole models. I calibrate a preliminary model using a dataset composed of x-ray refinements that supply amphibole volume and site occupancy data. Results reveal regions in parameter space where data is limited and the sensitivity that model coefficients have to uncertainties in the data, suggesting that filtering the dataset to remove outliers may be necessary.
", "date": "2024", "date_type": "degree", "id_number": "CaltechTHESIS:09282023-195100516", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:09282023-195100516", "related_url": { "items": [ { "description": "Article adapted for Ch. 1", "type": "doi", "url": "https://doi.org/10.1016/j.gca.2023.05.015" } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "NSF Graduate Research Fellowship", "grant_number": "DGE\u20101745301" } ] }, "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "suggestions": "Released 2023-10-10.", "deposited_by": "Carl Swindle", "deposited_on": "2023-10-03 18:22:36", "doi": "10.7907/5mbh-jw64", "divisions": { "items": [ "div_gps" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "farley@caltech.edu", "id": "Farley-K-A", "name": { "family": "Farley", "given": "Kenneth A." }, "orcid": "0000-0002-7846-7546", "role": "advisor" }, { "email": "asimow@caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "orcid": "0000-0001-6025-8925", "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "asimow@caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "orcid": "0000-0001-6025-8925", "role": "chair" }, { "email": "farley@caltech.edu", "id": "Farley-K-A", "name": { "family": "Farley", "given": "Kenneth A." }, "orcid": "0000-0002-7846-7546", "role": "member" }, { "email": "eiler@caltech.edu", "id": "Eiler-J-M", "name": { "family": "Eiler", "given": "John M." }, "orcid": "0000-0001-5768-7593", "role": "member" }, { "email": "ems@caltech.edu", "id": "Stolper-E-M", "name": { "family": "Stolper", "given": "Edward M." }, "orcid": "0000-0001-8008-8804", "role": "member" }, { "email": "tissot@caltech.edu", "id": "Tissot-F-L-H", "name": { "family": "Tissot", "given": "Fran\u00e7ois L. H." }, "orcid": "0000-0001-6622-2907", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2023-09-26", "gradofc_approval_date": "2023-10-03", "review_status": "approved", "option_major": { "items": [ "geol" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2024", "author_list": "Swindle, Carl Raymond", "advisor_list": "Farley, Kenneth A. and Asimow, Paul David", "comittee_list": "Asimow, Paul David; Farley, Kenneth A.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/14229", "eprint_id": 14229, "rev_number": 58, "documents": [ { "id": "/id/document/119282", "doc_id": 119282, "rev_number": 7, "files": [ { "id": "/id/file/362817", "fileid": 362817, "datasetid": "document", "objectid": 119282, "filename": "MLewis Supplementary Data File Chapters 2-6.xlsx", "mime_type": "application/vnd.openxmlformats-officedocument.spreadsheetml.sheet", "hash": "e0b2e2fa1783d188801ed7bf24d80396", "hash_type": "MD5", "filesize": 1355296, "mtime": "2021-06-02 16:55:07", "url": "/14229/3/MLewis Supplementary Data File Chapters 2-6.xlsx" } ], "eprint_id": 14229, "pos": 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"filename": "indexcodes.txt", "mime_type": "text/x-c", "hash": "6cb6340f4d895c8cef12247ef2f433a2", "hash_type": "MD5", "filesize": 42681, "mtime": "2021-06-24 18:10:24", "url": "/14229/8/indexcodes.txt" } ], "eprint_id": 14229, "pos": 8, "placement": 8, "mime_type": "text/x-c", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/119316" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/119316" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/119316" } ] } } ], "eprint_status": "archive", "userid": 12508, "dir": "disk0/00/01/42/29", "datestamp": "2021-06-03 18:46:25", "lastmod": "2021-06-10 15:48:55", "status_changed": "2021-06-03 18:46:25", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "madjlewis@gmail.com", "id": "Lewis-Madeline-Janine", "name": { "family": "Lewis", "given": "Madeline Janine" }, "orcid": "0000-0001-7968-2822", "show_email": "NO" } ] }, "title": "Magmatic Differentiation in Arc and Mid Ocean Ridge Settings", "ispublished": "unpub", "full_text_status": "public", "keywords": "Magma; geochemistry; petrology; geochronology; magmatic arc; mid-ocean ridge; differentiation; volcano; iron formation", "abstract": "The compositional variation of igneous rocks and construction of Earth's crust is the result of magmatic differentiation -- crystallization, melting, and assimilation mechanisms that\r\ncause the composition of magmas to change over time. This thesis investigates magma generation and evolution at both convergent and divergent plate boundaries. The resulting magmatic arcs and mid-ocean ridges create the vast majority of Earth's crust, though the details of crustal construction and the specific processes that generate the observed magmatic and volcanic products are complex. Accordingly, this work uses the geochemical signatures encoded in rocks and minerals to explain magmatic differentiation histories in multiple tectonic settings.
\r\n\r\nHere, I present five main studies that utilize field and textural observations, geochemical analyses, and computational modeling to investigate the compositional structure of the crust beneath magmatic arcs and mid-ocean ridges. In addition, this work explores the pyroclastic and sedimentary products dispersed by magmatically heated hydrothermal fluids in submarine environments. Chapters 2 and 3 investigate the crystallization histories of mafic intrusions in the eastern-central Sierra Nevada batholith paleo-continental arc, California. This work has implications for the compositional and temporal generation of both mafic and evolved magmas throughout the batholith and in other continental arcs. Chapters 4 and 5 explore records of submarine volcanic ash deposits associated with explosive mid-ocean ridge eruptions from the East Pacific Rise and Pacific-Antarctic Ridge, as well as the effects that sea level change has on melting of the mantle, eruption styles, and the compositional evolution of mid-ocean ridge magmas. Chapter 6 examines the mineral hosting of rare earth elements (REEs) in the Wadi Karim banded iron formation, and the implications of element mobility on interpretations based on REE abundances.
", "date": "2021", "date_type": "degree", "id_number": "CaltechTHESIS:06022021-034345855", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:06022021-034345855", "related_url": { "items": [ { "description": "Article adapted for Chapter 4", "type": "doi", "url": "https://doi. org/10.1029/2017GC007341" } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "AGeS2, via NSF", "grant_number": "EAR-1759200" }, { "agency": "NSF", "grant_number": "EAR- 1551433" }, { "agency": "NSF", "grant_number": "OCE-1558372" }, { "agency": "NSF", "grant_number": "EAR-1558372" } ] }, "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "deposited_by": "Madeline Lewis", "deposited_on": "2021-06-03 18:46:25", "doi": "10.7907/a1ky-ab66", "divisions": { "items": [ "div_gps" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "cbucholz@caltech.edu", "id": "Bucholz-C-E", "name": { "family": "Bucholz", "given": "Claire E." }, "orcid": "0000-0003-3252-7109", "role": "co-advisor" }, { "email": "asimow@caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "orcid": "0000-0001-6025-8925", "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "grr@caltech.edu", "id": "Rossman-G-R", "name": { "family": "Rossman", "given": "George Robert" }, "orcid": "0000-0002-4571-6884", "role": "chair" }, { "email": "wfischer@caltech.edu", "id": "Fischer-W-W", "name": { "family": "Fischer", "given": "Woodward W." }, "orcid": "0000-0002-8836-3054", "role": "member" }, { "email": "ems@caltech.edu", "id": "Stolper-E-M", "name": { "family": "Stolper", "given": "Edward M." }, "orcid": "0000-0001-8008-8804", "role": "member" }, { "email": "cbucholz@caltech.edu", "id": "Bucholz-C-E", "name": { "family": "Bucholz", "given": "Claire E." }, "orcid": "0000-0003-3252-7109", "role": "member" }, { "email": "asimow@caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "orcid": "0000-0001-6025-8925", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2021-05-18", "gradofc_approval_date": "2021-06-03", "review_status": "approved", "option_major": { "items": [ "geochem" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. 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"Joseph Anthony" }, "orcid": "0000-0003-1196-7877", "show_email": "NO" } ] }, "title": "Paleomagnetism and Geochemistry of Basalts in the North American Cordillera, Davis Strait, and Antarctica", "ispublished": "unpub", "full_text_status": "public", "keywords": "Basalt, paleomagnetism, igneous, petrology, ophiolite, flood basalt, mass extinction, dike, north atlantic, large igneous province, volcano, volcanology, magnetic field", "abstract": "Chapter 1 is an introduction to the thesis and contains a brief summary on how the chapters relate to each other. In Chapter 2, we present new whole-rock geochemical data from the Brooks Range Ophiolite (BRO) together with new mineral chemistry data from the BRO, South Sandwich forearc, Izu-Bonin forearc, and Hess Deep. In Chapter 3, we use a combination of paleomagnetic data and thermal modeling to create a magnetic geothermometer (MGT) that can constrain the active transport lifetime of magmatic conduits and igneous intrusions. In Chapter 4, we present new stratigraphic and paleomagnetic data from Paleocene flood basalts on Baffin Island. In Chapter 5, we present new paleomagnetic and paleointensity data from the James Ross Island volcanic group, located on the Antarctic Peninsula.
", "date": "2021", "date_type": "degree", "id_number": "CaltechTHESIS:06022021-013516525", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:06022021-013516525", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "NSF", "grant_number": "EAR-1550934" }, { "agency": "NSF", "grant_number": "CAREER 1848554" }, { "agency": "Geological Society of America/NSF", "grant_number": "AGeS2" }, { "agency": "NSF", "grant_number": "1911699" }, { "agency": "NSF", "grant_number": "ANT-1341729" }, { "agency": "National Geographic Society", "grant_number": "CP4-144R-18" } ] }, "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "deposited_by": "Joseph Biasi", "deposited_on": "2021-06-02 23:12:44", "doi": "10.7907/hbs7-aw47", "divisions": { "items": [ "div_gps" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "asimow@caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "orcid": "0000-0001-6025-8925", "role": "advisor" }, { "email": "kirschvink@caltech.edu", "id": "Kirschvink-J-L", "name": { "family": "Kirschvink", "given": "Joseph L." }, "orcid": "0000-0001-9486-6689", "role": "advisor" }, { "email": "cbucholz@caltech.edu", "id": "Bucholz-C-E", "name": { "family": "Bucholz", "given": "Claire E." }, "orcid": "0000-0003-3252-7109", "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "grr@caltech.edu", "id": "Rossman-G-R", "name": { "family": "Rossman", "given": "George Robert" }, "orcid": "0000-0002-4571-6884", "role": "chair" }, { "email": "asimow@caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "orcid": "0000-0001-6025-8925", "role": "member" }, { "email": "kirschvink@caltech.edu", "id": "Bucholz-C-E", "name": { "family": "Bucholz", "given": "Claire E." }, "orcid": "0000-0003-3252-7109", "role": "member" }, { "email": "cbucholz@caltech.edu", "id": "Kirschvink-J-L", "name": { "family": "Kirschvink", "given": "Joseph L." }, "orcid": "0000-0003-3252-7109", "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2021-05-20", "gradofc_approval_date": "2021-06-02", "review_status": "approved", "option_major": { "items": [ "geochem" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2021", "author_list": "Biasi, Joseph Anthony", "advisor_list": "Asimow, Paul David; Kirschvink, Joseph L.; et el.", "comittee_list": "Rossman, George Robert; Asimow, Paul David; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/10237", "eprint_id": 10237, "rev_number": 41, "documents": [ { "id": "/id/document/80140", "doc_id": 80140, "rev_number": 4, "files": [ { "id": "/id/file/226422", "fileid": 226422, "datasetid": "document", "objectid": 80140, "filename": "Thesis_Solomatova_2017.pdf", "mime_type": "application/pdf", "hash": "d03896da0d5ed43aaac5e348d40ede12", "hash_type": "MD5", "filesize": 18112158, "mtime": "2017-06-05 17:07:51", "url": "/10237/1/Thesis_Solomatova_2017.pdf" } ], "eprint_id": 10237, "pos": 1, "placement": 1, "mime_type": "application/pdf", "format": "application/pdf", 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"main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/80140" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/80140" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/80140" } ] } } ], "eprint_status": "archive", "userid": 9962, "dir": "disk0/00/01/02/37", "datestamp": "2017-06-05 22:56:13", "lastmod": "2019-10-04 00:16:30", "status_changed": "2017-06-05 22:56:13", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "nsolomat@gmail.com", "id": "Solomatova-Natalia-Viatcheslavovna", "name": { "family": "Solomatova", "given": "Natalia Viatcheslavovna" }, "orcid": "0000-0002-2331-3427", "show_email": "NO" } ] }, "title": "Iron-bearing Oxides, Silicate Glasses and Carbonates at Lower Mantle Pressures", "ispublished": "unpub", "full_text_status": "public", "keywords": "mineral physics; high pressure; spin transition; lower mantle; ferropericlase, silicate glasses, carbonates", "abstract": "Iron is the fourth most abundant element in Earth\u2019s mantle and it affects geophysically observable properties, such as the density, sound velocities, viscosity and transport properties of mantle phases. Additionally, the concentration of iron in minerals and melts of the lower mantle dictates their structure and stability. Thus, understanding the effect of iron is important to interpret seismically observable complexities and understand their effect on processes in the deep Earth. In this thesis, I use experimental and theoretical methods to improve our understanding of the high-pressure behavior of iron-bearing periclase (\u201cferropericlase\u201d), silicate glasses and carbonates.
\r\n\r\nFerropericlase is thought to represent a significant fraction of Earth\u2019s lower mantle, and may explain the slow compressional and shear sound velocities of ultra-low velocity zones at the core-mantle boundary. To understand the effect of iron concentration on the (Mg,Fe)O solid solution, the equation of state and hyperfine parameters of (Mg,Fe)O with 48 mol% FeO were measured using X-ray powder diffraction and time-domain M\u00f6ssbauer spectroscopy, respectively, and the spin crossover behavior was compared to that of (Mg,Fe)O with 10 to 60 mol% FeO. I find that iron-rich ferropericlase at core-mantle boundary pressures likely contains a significant fraction of high-spin iron, contributing a positive buoyancy to promote topographic relief of ultra-low velocity zones in the lowermost mantle.
\r\n\r\nSome ultra-low velocity zones, particularly those at the base of the central parts of large low shear velocity provinces, may be best explained by the presence of iron-bearing silicate melts. The behavior of iron in silicate melts is poorly understood, but may be approximated by iron-bearing silicate glasses. I measured the hyperfine parameters of iron-bearing rhyolitic glass up to ~120 GPa and basaltic glasses up to ~90 GPa using time-domain M\u00f6ssbauer spectroscopy. Iron within these glasses experiences changes in coordination environment with increasing pressure without undergoing a high-spin to low-spin transition. Thus, ferrous iron in chemically\u2013complex silicate melts likely exists in a high-spin state throughout most of Earth\u2019s mantle.
\r\n\r\nDecomposition of carbonates may be responsible for creating silicate melts within the lower mantle by lowering the melting temperature of surrounding rock. Identifying and characterizing the stability of carbonate phases is therefore a necessary step towards understanding the transport and storage of carbon in Earth\u2019s interior. Dolomite is one of the major mineral forms in which carbon is subducted into the Earth\u2019s mantle. Although iron-free dolomite is expected to break down upon compression into single-cation carbonates, high-pressure polymorphs of iron-bearing dolomite may resist decomposition. Using a genetic algorithm that predicts crystal structures (USPEX), I have found a monoclinic phase with space group C2/c that has a lower energy than all previously reported dolomite structures at pressures above 15 GPa, and the substitution of iron for magnesium stabilizes monoclinic dolomite with respect to decomposition at certain pressures of the lower mantle.
\r\n\r\nIn this thesis, I demonstrate that iron undergoes a spin transition in (Mg,Fe)O, (Mg,Fe)CO3 and Ca(Mg,Fe)(CO3)2, while iron in basaltic and silicate glasses likely does not experience a spin transition up to lowermost mantle pressures. Additionally, I find that the amount of iron in (Mg,Fe)O and Ca(Mg,Fe)(CO3)2 dictates the dynamic and thermodynamic stabilities of those phases within Earth\u2019s lower mantle.
", "date": "2017", "date_type": "degree", "id_number": "CaltechTHESIS:05312017-162026972", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:05312017-162026972", "related_url": { "items": [ { "description": "Adapted for Ch. 3.", "type": "doi", "url": "http://dx.doi.org/10.2138/am-2016-5510" }, { "description": "Adapted for Ch. 6.", "type": "doi", "url": "http://dx.doi.org/10.2138/am-2017-5830" } ] }, "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "National Science Foundation", "grant_number": "EAR-CAREER-0956166 " }, { "agency": "National Science Foundation", "grant_number": "CSEDI-EAR-1161046" }, { "agency": "National Science Foundation", "grant_number": "CSEDI-EAR-1600956" }, { "agency": "National Science Foundation", "grant_number": "EAR-1322082" }, { "agency": "National Science Foundation", "grant_number": "EAR-1551433" } ] }, "collection": "CaltechTHESIS", "reviewer": "Melissa Ray", "suggestions": "Files temporarily withheld until Jun 12, 2017 - released to public view 6/12/2017", "deposited_by": "Natalia Solomatova", "deposited_on": "2017-06-05 22:56:13", "doi": "10.7907/Z99021TX", "divisions": { "items": [ "div_gps" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "jackson@gps.caltech.edu", "id": "Jackson-J-M", "name": { "family": "Jackson", "given": "Jennifer M." }, "role": "advisor" }, { "email": "asimow@gps.caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "clay@gps.caltech.edu", "id": "Clayton-R-W", "name": { "family": "Clayton", "given": "Robert W." }, "role": "chair" }, { "email": "jackson@gps.caltech.edu", "id": "Jackson-J-M", "name": { "family": "Jackson", "given": "Jennifer M." }, "role": "member" }, { "email": "asimow@gps.caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "member" }, { "email": "grr@gps.caltech.edu", "id": "Rossman-G-R", "name": { "family": "Rossman", "given": "George Robert" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2017-05-23", "gradofc_approval_date": "2017-06-05", "review_status": "approved", "option_major": { "items": [ "geophys" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2017", "author_list": "Solomatova, Natalia Viatcheslavovna", "advisor_list": "Jackson, Jennifer M. and Asimow, Paul David", "comittee_list": "Clayton, Robert W.; Jackson, Jennifer M.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/7887", "eprint_id": 7887, "rev_number": 39, "documents": [ { "id": "/id/document/41879", "doc_id": 41879, "rev_number": 3, "files": [ { "id": "/id/file/126069", "fileid": 126069, "datasetid": "document", "objectid": 41879, "filename": "wolf_thesis.pdf", "mime_type": "application/pdf", "hash": "0c6e210368a5019a1c428f99bfb5510e", "hash_type": "MD5", "filesize": 10970602, "mtime": "2013-06-11 00:37:46", "url": "/7887/1/wolf_thesis.pdf" } ], "eprint_id": 7887, "pos": 1, "placement": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "full 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In this thesis, I present work that helps constrain the equation of state properties of iron-bearing Mg-silicate perovskite as well as oxide-silicate melts. I use a mixture of experimental, statistical, and theoretical techniques to obtain knowledge about these phases. These include laser-heated diamond anvil cell experiments, Bayesian statistical analysis of powder diffraction data, and the development of a new simplified model for understanding oxide and silicate melts at mantle conditions. By shedding light on the thermodynamic properties of such ubiquitous Earth-forming materials, I hope to aid our community\u2019s progress toward understanding the large-scale processes operating in the Earth\u2019s mantle, both in the modern day and early in Earth\u2019s history.", "date": "2013", "date_type": "degree", "id_number": "CaltechTHESIS:06102013-170950875", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:06102013-170950875", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "CSEDI", "grant_number": "EAR-0855815" }, { "agency": "NSF", "grant_number": "EAR 0711542 " }, { "agency": "NSF", "grant_number": "GRFP" }, { "agency": "NSF", "grant_number": "EAGER" } ] }, "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Aaron Wolf", "deposited_on": "2013-06-12 18:43:25", "doi": "10.7907/TJ86-C566", "divisions": { "items": [ "div_gps" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "asimow@caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "advisor" }, { "email": "jackson@gps.caltech.edu", "id": "Jackson-J-M", "name": { "family": "Jackson", "given": "Jennifer M." }, "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "gab@gps.caltech.edu", "id": "Blake-G-A", "name": { "family": "Blake", "given": "Geoffrey A." }, "role": "chair" }, { "email": "asimow@gps.caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "member" }, { "email": "jackson@gps.caltech.edu", "id": "Jackson-J-M", "name": { "family": "Jackson", "given": "Jennifer M." }, "role": "member" }, { "email": "djs@gps.caltech.edu", "id": "Stevenson-D-J", "name": { "family": "Stevenson", "given": "David John" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2013-05-29", "gradofc_approval_date": "2013-06-11", "review_status": "approved", "option_major": { "items": [ "plansci" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. 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"type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/37081" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/37081" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/37081" } ] } } ], "eprint_status": "archive", "userid": 1102, "dir": "disk0/00/00/76/16", "datestamp": "2013-04-22 17:14:36", "lastmod": "2019-10-04 00:00:15", "status_changed": "2013-04-22 17:14:36", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "clairewaller@gmail.com", "id": "Thomas-Claire-Waller", "name": { "family": "Thomas", "given": "Claire Waller" }, "show_email": "NO" } ] }, "title": "Liquid Silicate Equation of State: Using Shock Waves to Understand the Properties of the Deep Earth", "ispublished": "unpub", "full_text_status": "public", "keywords": "equation of state; liquid silicate; shock wave", "abstract": "The equations of state (EOS) of several geologically important silicate liquids have been constrained via preheated shock wave techniques. Results on molten Fe2SiO4 (fayalite), Mg2SiO4 (forsterite), CaFeSi2O6 (hedenbergite), an equimolar mixture of CaAl2Si2O8-CaFeSi2O6 (anorthite-hedenbergite), and an equimolar mixture of CaAl2Si2O8-CaFeSi2O6-CaMgSi2O6(anorthite-hedenbergite-diopside) are presented. This work represents the first ever direct EOS measurements of an iron-bearing liquid or of a forsterite liquid at pressures relevant to the deep Earth (> 135 GPa). Additionally, revised EOS for molten CaMgSi2O6 (diopside), CaAl2Si2O8 (anorthite), and MgSiO3 (enstatite), which were previously determined by shock wave methods, are also presented.
\r\n\r\nThe liquid EOS are incorporated into a model, which employs linear mixing of volumes to determine the density of compositionally intermediate liquids in the CaO-MgO-Al2O3-SiO2-FeO major element space. Liquid volumes are calculated for temperature and pressure conditions that are currently present at the core-mantle boundary or that may have occurred during differentiation of a fully molten mantle magma ocean.
\r\n\r\nThe most significant implications of our results include: (1) a magma ocean of either chondrite or peridotite composition is less dense than its first crystallizing solid, which is not conducive to the formation of a basal mantle magma ocean, (2) the ambient mantle cannot produce a partial melt and an equilibrium residue sufficiently dense to form an ultralow velocity zone mush, and (3) due to the compositional dependence of Fe
(1) The presence of small amounts of water dissolved within nominally-anhydrous minerals in the earth has significant effects on the chemistry of melting in the Earth\u2019s mantle. Upwelling rock containing water will melt at greater depths than the same rock would if it were volatile-free, and the chemistry of these hydrous melts is expected to be quite different from that of anhydrous melts. We have developed new experimental techniques and applied them to melting under pressures where hydrous melting is of the greatest natural importance. We have also controlled the content of carbon, another volatile element, to produce melts from a range of compositions not previously sampled experimentally.
\r\n\r\nThe liquid composition shows a number of interesting properties. Compared to anhydrous melts from the same pressure, it shows decreased modal olivine and increased silica content. Compared to carbon-containing experiments, it suggests that carbon interacts with water when both volatiles are present, and may act to oppose the effects of water. The presence of a hydrous liquid also has an important effect on the coexisting solid chemistry. High-aluminum clinopyroxenes are commonly observed at this pressure in anhydrous systems. However, in all of our volatile-containing experiments, the clinopyroxenes show a substantial decrease in aluminum content and an increase in calcium content. Many elements, including water, enter into the clinopyroxene structure by coupled substitution with aluminum, and thus reduced clinopyroxene aluminum content during natural melting will decrease the partitioning of these elements during melting.
\r\n\r\n(2) Variations in the modal abundance of olivine are the main mineralogical differences amongst typical Hawaiian lavas. A large quantity of olivine must crystallize from the Hawaiian parental liquids prior to eruption to produce the erupted lavas. The chemistry and abundance of these olivines reflects the behavior of the magmatic system in a number of ways. We have used the chemistry of these olivines and lavas to estimate the parental liquid compositions in Hawaiian volcanoes, to infer the relationship between the olivines and the lavas that host them, and to probe the evolution of Hawaiian volcanoes over time.
\r\n", "date": "2010", "date_type": "degree", "id_number": "CaltechTHESIS:11062009-091851899", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechTHESIS:11062009-091851899", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "funders": { "items": [ { "agency": "NSF Ocean Sciences Marine Geology and Geophysics program", "grant_number": "OCE-0241716" }, { "agency": "NSF Ocean Sciences Marine Geology and Geophysics program", "grant_number": "OCE-0550216" } ] }, "collection": "CaltechTHESIS", "reviewer": "Gayle Hammer", "deposited_by": "Joseph Balta", "deposited_on": "2010-01-07 17:56:17", "succeeds": 5358, "doi": "10.7907/7NM9-AB40", "alt_title": { "items": [ "Experimental Investigation of Hydrous Melting of the Earth\u2019s Upper Mantle", "Olivine Abundances and Compositions in Hawaiian Lavas" ] }, "divisions": { "items": [ "div_gps" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "asimow@gps.caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "ems@gps.caltech.edu", "id": "Stolper-E-M", "name": { "family": "Stolper", "given": "Edward M." }, "role": "chair" }, { "email": "asimow@gps.caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "member" }, { "email": "eiler@gps.caltech.edu", "id": "Eiler-J-M", "name": { "family": "Eiler", "given": "John M." }, "role": "member" }, { "email": "grr@gps.caltech.edu", "id": "Rossman-G-R", "name": { "family": "Rossman", "given": "George Robert" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_defense_date": "2009-11-20", "gradofc_approval_date": "2010-01-06", "review_status": "approved", "option_major": { "items": [ "geol" ] }, "copyright_statement": "Author's Rights Authorization: I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted here is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive license to archive and make accessible, under the conditions specified under \"Thesis Availability\" in this submission, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation, or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2010", "author_list": "Balta, Joseph Brian", "advisor_list": "Asimow, Paul David", "comittee_list": "Stolper, Edward M.; Asimow, Paul David; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/790", "eprint_id": 790, "rev_number": 34, "documents": [ { "id": "/id/document/1184", "doc_id": 1184, "rev_number": 3, "files": [ { "id": "/id/file/7439", "fileid": 7439, "datasetid": "document", "objectid": 1184, "filename": "Hebert_Chapter0.pdf", "mime_type": "application/pdf", "filesize": 307683, "mtime": "2012-12-26 02:32:26", "url": "/790/1/Hebert_Chapter0.pdf" } ], "eprint_id": 790, "pos": 1, "placement": 2, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Hebert_Chapter0.pdf", "language": "en", "security": "public", "license": "other", "main": "Hebert_Chapter0.pdf", 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"2008-03-06", "lastmod": "2019-12-03 23:55:34", "status_changed": "2009-09-25 01:46:36", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "labaker@gps.caltech.edu", "id": "Hebert-Laura-Baker", "name": { "family": "Hebert", "given": "Laura Baker" }, "show_email": "NO" } ] }, "title": "(I) A Coupled Geochemical and Geodynamical Approach to Subduction Zone Modeling and (II) Development of Color in Greenish Quartz", "ispublished": "unpub", "full_text_status": "public", "keywords": "green quartz; low viscosity channel; modeling; subduction", "abstract": "(I) We couple a petrological model with a 2D thermal and variable viscosity flow model to describe and compare fundamental processes occurring within subduction zones. We study the thermal state and phase equilibria of the subducting oceanic slab and mantle wedge and constrain fluid flux, presenting model results spanning normal ranges in subduction parameters. Coupling between the chemistry and the dynamics results in the development of a stable slab-adjacent low-viscosity region defined by hydrous phases and higher concentrations of water in nominally anhydrous minerals, bounded by the water-saturated solidus.
\r\n\r\nSubduction parameters are significant to the position of dehydration reactions within the slab and the geochemistry of fluids initiating flux melting. Modeling of fluid transport mechanisms and potential melt migration processes based on coupled modeling with the addition of fluid-mobile trace elements was performed. There is a progression of geochemical characteristics described in previous studies of arc lava datasets that can be duplicated with these models.
\r\n\r\nA localized low-viscosity, low-density geometry within the wedge, predicted by coupled modeling of the Izu-Bonin system, is required to match observations of topography, gravity, and geoid anomalies. Based on this, predictions can be made as to specific low-viscosity geometries associated with geophysical signals for other subduction zones based on regional subduction parameters.
\r\n\r\n(II) Naturally occurring greenish quartz found within the context of amethyst-bearing deposits is not simply the result of the exposure of amethyst to thermal bleaching. Rather, it can represent a set of distinct color varieties resulting from the changing chemical and thermal nature of the precipitating solution. Greenish quartz occurs at the Thunder Bay Amethyst Mine Panorama, Thunder Bay, Ontario, Canada, in several distinct varieties. Spectroscopic, irradiation, and controlled heating studies show that changes in salinity and temperature of the hydrothermal system that produced the deposit and changes in quartz growth rate are reflected in coloration. As the system evolved, a minor ferric component appears to change position from interstitial to substitutional within specific growth sectors. Greenish colors within the quartz are consistently correlated with the speciation of hydrous components.
\r\n", "date": "2008", "date_type": "degree", "id_number": "CaltechETD:etd-02272008-172649", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-02272008-172649", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2008-03-06", "doi": "10.7907/71YF-WH65", "alt_title": { "items": [ "(I) A Coupled Geochemical and Geodynamical Approach to Subduction Zone Modeling & (II) Development of Color in Greenish Quartz", "Development of Color in Greenish Quartz" ] }, "divisions": { "items": [ "div_gps" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "email": "asimow@gps.caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "advisor" }, { "email": "gurnis@gps.caltech.edu", "id": "Gurnis-M-C", "name": { "family": "Gurnis", "given": "Michael C." }, "role": "co-advisor" } ] }, "thesis_committee": { "items": [ { "email": "eiler@gps.caltech.edu", "id": "Eiler-J-M", "name": { "family": "Eiler", "given": "John M." }, "role": "chair" }, { "email": "grr@gps.caltech.edu", "id": "Rossman-G-R", "name": { "family": "Rossman", "given": "George Robert" }, "role": "member" }, { "email": "gurnis@gps.caltech.edu", "id": "Gurnis-M-C", "name": { "family": "Gurnis", "given": "Michael C." }, "role": "member" }, { "email": "asimow@gps.caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2008-02-27", "thesis_defense_date": "2008-02-15", "thesis_approved_date": "2008-03-06", "gradofc_approval_date": "2008-03-06", "review_status": "approved", "option_major": { "items": [ "geochem" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2008", "author_list": "Hebert, Laura Baker", "advisor_list": "Asimow, Paul David and Gurnis, Michael C.", "comittee_list": "Eiler, John M.; Rossman, George Robert; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/5042", "eprint_id": 5042, "rev_number": 15, "documents": [ { "id": "/id/document/7987", "doc_id": 7987, "rev_number": 3, "files": [ { "id": "/id/file/49165", "fileid": 49165, "datasetid": "document", "objectid": 7987, "filename": "oleary_thesis.pdf", "mime_type": "application/pdf", "filesize": 1591882, "mtime": "2012-12-26 03:14:06", "url": "/5042/1/oleary_thesis.pdf" } ], "eprint_id": 5042, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "oleary_thesis.pdf", "language": "en", "security": "public", "license": "other", "main": "oleary_thesis.pdf", 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], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/50/42", "datestamp": "2007-01-11", "lastmod": "2020-02-19 18:23:24", "status_changed": "2009-09-25 03:31:29", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "oleary.julie@gmail.com", "id": "O'Leary-Julie-Ann", "name": { "family": "O'Leary", "given": "Julie Ann" }, "show_email": "YES" } ] }, "title": "Hydrogen Isotope Geochemistry of the Mantle: Constraints from Back Arc Basin Basalts and Mantle Xenoliths", "ispublished": "unpub", "full_text_status": "public", "keywords": "back arc basin; hydrogen isotopes; Mariana trough; nominally anhydrous minerals; water in minerals", "abstract": "A new technique for measuring the hydrogen isotopic compositions of small quantities of hydrous and nominally anhydrous silicate materials was developed. The hydrogen isotopic composition of mantle derived basalts and nominally anhydrous minerals were measured to examine the systematics of the hydrogen isotope geochemistry of the mantle and to better constrain the mantle water cycle.
\r\n\r\nBack arc basin basalts (BABB) from the Mariana Trough are variably enriched in deuterium relative to mid ocean ridge basalts (MORBs). The \u03b4D values of 15 Mariana Trough BABB samples range from -74 \u2030 to -34 \u2030. High \u03b4D values in BABB lavas are associated with the trace element signature of H2O rich fluids derived from the altered oceanic crust that is subducting into the mantle. We calculate a mixing model to constrain the isotopic composition and trace element chemistry of the fluid infiltrating the back arc lava source region. The \u03b4D value of the infiltrating fluid is close to -30 \u2030. When the composition of the infiltrating fluid is compared to a forward calculation of the hydrogen isotopic evolution of altered oceanic crust it indicates that hydrous fluids in the back arc source region originate from the hydrated lithospheric mantle section of altered oceanic crust. Forward model calculations predict that hydrogen deeply subducted into the mantle may have an isotopic composition that is highly fractionated from the initial composition of altered oceanic crust.
\r\n\r\nPyroxenes from mantle xenoliths are deuterium depleted relative to all mantle materials, with \u03b4D values ~50 \u2030 lower than average MORB. Using continuous flow mass spectrometry we analyzed the hydrogen isotopic composition of clinopyroxene and orthopyroxene from mantle xenoliths. Our results confirm the previous observations of very low \u03b4D values for xenoliths from continental interiors but found \u03b4D values similar to MORB in Central American arc xenoliths. The relationship between \u03b4D and water content observed in pyroxenes suggests that most mantle xenoliths have undergone extensive degassing (40% \u2013 60%) and therefore the hydrogen content of upper mantle minerals may be higher than previously thought.
", "date": "2007", "date_type": "degree", "id_number": "CaltechETD:etd-12182006-072449", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-12182006-072449", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2007-01-11", "doi": "10.7907/6QQX-ED22", "divisions": { "items": [ "div_gps" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Eiler-J-M", "name": { "family": "Eiler", "given": "John M." }, "role": "advisor" }, { "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "asimow@gps.caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "chair" }, { "email": "ems@expet.gps.caltech.edu", "id": "Stolper-E-M", "name": { "family": "Stolper", "given": "Edward M." }, "role": "member" }, { "email": "grr@gps.caltech.edu", "id": "Rossman-G-R", "name": { "family": "Rossman", "given": "George Robert" }, "role": "member" }, { "email": "eiler@gps.caltech.edu", "id": "Eiler-J-M", "name": { "family": "Eiler", "given": "John M." }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2006-12-18", "thesis_defense_date": "2006-09-05", "thesis_approved_date": "2007-01-11", "review_status": "approved", "option_major": { "items": [ "geochem" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2007", "author_list": "O'Leary, Julie Ann", "advisor_list": "Eiler, John M. and Asimow, Paul David", "comittee_list": "Asimow, Paul David; Stolper, Edward M.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1779", "eprint_id": 1779, "rev_number": 70, "documents": [ { "id": "/id/document/2886", "doc_id": 2886, "rev_number": 11, "files": [ { "id": "/id/file/17582", "fileid": 17582, "datasetid": "document", "objectid": 2886, "filename": "Appendix1.pdf", "mime_type": "application/pdf", "filesize": 354022, "mtime": "2012-12-26 02:41:53", "url": "/1779/1/Appendix1.pdf" } ], "eprint_id": 1779, "pos": 1, "placement": 9, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "Appendix1.pdf", "language": "en", "security": "public", "license": "other", "main": "Appendix1.pdf", 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121244, "rev_number": 1, "files": [ { "id": "/id/file/366636", "fileid": 366636, "datasetid": "document", "objectid": 121244, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "8cc7e1222c75daebbeb2a997bc09da07", "hash_type": "MD5", "filesize": 4579, "mtime": "2021-06-23 21:21:03", "url": "/1779/46/indexcodes.txt" } ], "eprint_id": 1779, "pos": 46, "placement": 46, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/2900" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/2900" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/2900" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/17/79", "datestamp": "2007-05-31", "lastmod": "2019-12-20 19:51:41", "status_changed": "2009-09-25 02:15:06", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "smiller@gps.caltech.edu", "id": "Miller-Sarah-Ann", "name": { "family": "Miller", "given": "Sarah Ann" }, "show_email": "NO" } ] }, "title": "Alkaline Earth Element Partitioning in Simplified Magmatic Systems", "ispublished": "unpub", "full_text_status": "public", "keywords": "alkaline earth elements; anorthite; melt thermodynamics; radium; trace element partitioning", "abstract": "Trace element distributions between mineral and melt phases have proven to be important recorders of igneous differentiation histories, but this utility depends on thorough understanding of their partitioning behavior. We propose a theory for crystal-melt trace element partitioning that considers the energetic consequences of crystal-lattice strain, of multi component major-element silicate liquid mixing, and of trace element activity coefficients in melts. We demonstrate application of the theory using newly determined partition coefficients for Ca, Mg, Sr, and Ba between pure anorthite and seven CMAS liquid compositions at 1330 \u00b0C and 1 atm. By selecting a range of melt compositions in equilibrium with a common crystal composition at equal liquidus temperature and pressure, we have isolated the contribution of melt composition to divalent trace element partitioning in this simple system. The partitioning data are fit to Onuma curves with parameterizations that can be thermodynamically rationalized in terms of the melt major element activity product (aAl2O3)(aSiO22) and lattice strain theory modeling. Residuals between observed partition coefficients and the lattice strain plus major oxide melt activity model are then attributed to non-ideality of trace constituents in the liquids. The activity coefficients of the trace species in the melt are found to vary systematically with composition. Accounting for the major and trace element thermodynamics in the melt allows a good fit in which the parameters of the crystal lattice strain model are independent of melt composition.\r\n\r\nWe also present the first experimental measurements of mineral-melt radium partitioning. Ion probe analyses of coexisting anorthite and CMAS glass phases produce a molar DRa = 0.040 \u00b1 0.006 and DRa/DBa = 0.23 at 1400 \u00b0C and 1 atm. Our results indicate that lattice strain partitioning models fit the divalent (Ca, Sr, Ba, Ra) partition coefficient data of this study well, supporting previous work on crustal melting and magma chamber dynamics that has relied on such models to approximate radium partitioning behavior in the absence of experimentally determined values. ", "date": "2007", "date_type": "degree", "id_number": "CaltechETD:etd-05132007-103357", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05132007-103357", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "deposited_by": "Imported from ETD-db", "deposited_on": "2007-05-31", "doi": "10.7907/90DK-3398", "divisions": { "items": [ "div_gps" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "advisor" }, { "id": "Burnett-D-S", "name": { "family": "Burnett", "given": "Donald S." }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "grr@gps.caltech.edu", "id": "Rossman-G-R", "name": { "family": "Rossman", "given": "George Robert" }, "role": "chair" }, { "email": "burnett@gps.caltech.edu", "id": "Burnett-D-S", "name": { "family": "Burnett", "given": "Donald S." }, "role": "member" }, { "email": "ems@gps.caltech.edu", "id": "Stolper-E-M", "name": { "family": "Stolper", "given": "Edward M." }, "role": "member" }, { "email": "eiler@gps.caltech.edu", "id": "Eiler-J-M", "name": { "family": "Eiler", "given": "John M." }, "role": "member" }, { "email": "asimow@gps.caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2007-05-13", "thesis_defense_date": "2006-12-06", "thesis_approved_date": "2007-05-31", "review_status": "approved", "option_major": { "items": [ "geochem" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2007", "author_list": "Miller, Sarah Ann", "advisor_list": "Asimow, Paul David and Burnett, Donald S.", "comittee_list": "Rossman, George Robert; Burnett, Donald S.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/1874", "eprint_id": 1874, "rev_number": 13, "documents": [ { "id": "/id/document/3167", "doc_id": 3167, "rev_number": 3, "files": [ { "id": "/id/file/18975", "fileid": 18975, "datasetid": "document", "objectid": 3167, "filename": "wzhr_thesis.pdf", "mime_type": "application/pdf", "filesize": 23110022, "mtime": "2012-12-26 02:43:25", "url": "/1874/1/wzhr_thesis.pdf" } ], "eprint_id": 1874, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": "wzhr_thesis.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/19863" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/19863" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/19863" } ] } }, { "id": "/id/document/19863", "doc_id": 19863, "rev_number": 3, "files": [ { "id": "/id/file/18973", "fileid": 18973, "datasetid": "document", "objectid": 19863, "filename": "preview.png", "mime_type": "image/png", "hash": "16e69d955f2f34f2aacbd31f64e1ddd6", "hash_type": "MD5", "filesize": 28416, "mtime": "2012-12-26 02:43:25", "url": "/1874/2/preview.png" } ], "eprint_id": 1874, "pos": 2, "placement": 2, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "public", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/3167" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/3167" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/3167" } ] } }, { "id": "/id/document/121466", "doc_id": 121466, "rev_number": 1, "files": [ { "id": "/id/file/366858", "fileid": 366858, "datasetid": "document", "objectid": 121466, "filename": "indexcodes.txt", "mime_type": "text/plain", "hash": "ee4089ec718eb28829adf62cacdc949e", "hash_type": "MD5", "filesize": 41673, "mtime": "2021-06-23 21:27:08", "url": "/1874/3/indexcodes.txt" } ], "eprint_id": 1874, "pos": 3, "placement": 3, "mime_type": "text/plain", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/3167" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/3167" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/3167" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/18/74", "datestamp": "2005-05-20", "lastmod": "2021-04-16 23:02:51", "status_changed": "2009-09-25 02:18:26", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "zwang1@ccny.cuny.edu", "id": "Wang-Zhengrong", "name": { "family": "Wang", "given": "Zhengrong" }, "show_email": "YES" } ] }, "title": "Oxygen Isotope Studies of the Petrogenesis of Hawaiian Lavas and a Theoretical Study on Equilibrium Thermodynamics of Multiply-Substituted Isotopologues", "ispublished": "unpub", "full_text_status": "public", "keywords": "HSDP; isotopologue; KSDP; oxygen isotope", "abstract": "Temporal oxygen isotope variations have been discovered in both Mauna Kea and Koolau volcanoes after detailed studies of the Hawaiian Scientific Drilling Project (HSDP-phase II) and Koolau Scientific Drilling Project (KSDP). In both volcanoes, oxygen isotope compositions of olivine phenocrysts all converge to 'Mauna Loa-like' values from depleted or enriched composition, respectively and yet, the interpretations are totally different. In the studies of HSDP core, many lines of geochemical evidences strongly indicate that low-[delta18]O values characteristic of Kea trend Hawaiian lavas are the product of contamination by hydrothermally altered rocks in the volcanic edifice. In the studies of KSDP core and submarine Koolau landslides, a full diversity of [delta18]O values correlate with trace element and radiogenic isotope compositions of host lavas. These correlations are interpreted as reflecting mixing between partial melts of high-[delta18]O and normal-[delta18]O components. A magma mixing model has been constructed to simultaneously explain the oxygen isotope, major element, trace element and radiogenic isotope variations defined by these correlations. This model indicates that the Koolau shield-building lavas are mixtures of 75~100% melt of mantle peridotite with 0~25% eclogite melt, the protolith of which is Mid-Ocean Ridge Basalt (MORB) with Depleted Mantle Model (DMM) age of at least 1.8\u00b10.3 billions years. [delta18]O value of this eclogite component is predicted to be 11.3\u00b11.5\u2030, implying it is an upper crustal (layer 1 or 2) basalt or gabbro with a low-temperature alteration history; contains a small amount of sediment; and has experienced partial melting before forming eclogite.
\r\n\r\nI also derived a method for systematically evaluating clumped-isotope effects in the abundances of all isotopologues in thermodynamically equilibrated populations of O2, CO, N2, NO, CO2 and N2O between 1000 and 193 to 77 K. This method uses Urey-type algorithms to evaluate partition functions and equilibrium constants of isotope exchange reactions, and simultaneously solves for abundance of each isotopologue of a given molecule constrained by all independent equilibria. Calculation results show that, in most cases, multiply-substituted isotopologues of these mono-molecular gases are predicted to be enriched relative to stochastic (random) distributions by ca. 1 to 2 per mil at earth-surface temperatures.
", "date": "2005", "date_type": "degree", "id_number": "CaltechETD:etd-05192005-000025", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05192005-000025", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2005-05-20", "doi": "10.7907/zrza-wc92", "alt_title": { "items": [ "Theoretical Study on Equilibrium Thermodynamics of Multiply-Substituted Isotopologues" ] }, "divisions": { "items": [ "div_gps" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Eiler-J-M", "name": { "family": "Eiler", "given": "John M." }, "role": "advisor" }, { "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "burnett@gps.caltech.edu", "id": "Burnett-D-S", "name": { "family": "Burnett", "given": "Donald S." }, "role": "chair" }, { "email": "ems@gps.caltech.edu", "id": "Stolper-E-M", "name": { "family": "Stolper", "given": "Edward M." }, "role": "member" }, { "email": "hptaylor@gps.caltech.edu", "id": "Taylor-H-P", "name": { "family": "Taylor", "given": "Hugh P." }, "role": "member" }, { "email": "eiler@gps.caltech.edu", "id": "Eiler-J-M", "name": { "family": "Eiler", "given": "John M." }, "role": "member" }, { "email": "farley@gps.caltech.edu", "id": "Farley-K-A", "name": { "family": "Farley", "given": "Kenneth A." }, "role": "member" }, { "email": "asimow@gps.caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2005-05-19", "thesis_defense_date": "2005-04-05", "thesis_approved_date": "2005-05-20", "review_status": "approved", "option_major": { "items": [ "geochem" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2005", "author_list": "Wang, Zhengrong", "advisor_list": "Eiler, John M. and Asimow, Paul David", "comittee_list": "Burnett, Donald S.; Stolper, Edward M.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/2086", "eprint_id": 2086, "rev_number": 11, "documents": [ { "id": "/id/document/3777", "doc_id": 3777, "rev_number": 3, "files": [ { "id": "/id/file/22160", "fileid": 22160, "datasetid": "document", "objectid": 3777, "filename": "Staneff_g_2005.pdf", "mime_type": "application/pdf", "filesize": 32208062, "mtime": "2012-12-26 02:46:51", "url": "/2086/1/Staneff_g_2005.pdf" } ], "eprint_id": 2086, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "language": "en", "security": "public", "license": "other", "main": "Staneff_g_2005.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/20441" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/20441" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/20441" } ] } }, { "id": "/id/document/20441", "doc_id": 20441, "rev_number": 2, "files": [ { "id": "/id/file/22158", "fileid": 22158, "datasetid": "document", "objectid": 20441, "filename": "preview.png", "mime_type": "image/png", "hash": "6f27e8a55c7fdc81aadc99d4f875dd54", "hash_type": "MD5", "filesize": 15386, "mtime": "2012-12-26 02:46:50", "url": "/2086/2/preview.png" } ], "eprint_id": 2086, "pos": 2, "placement": 2, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "public", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/3777" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/3777" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/3777" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/20/86", "datestamp": "2005-05-26", "lastmod": "2021-11-05 17:58:36", "status_changed": "2009-09-25 02:26:17", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "email": "gstaneff@alumni.caltech.edu", "id": "Staneff-Geoffrey-D", "name": { "family": "Staneff", "given": "Geoffrey D." }, "show_email": "YES" } ] }, "title": "High-Pressure Synthesis of Thermoelectric Materials", "ispublished": "unpub", "full_text_status": "public", "keywords": "nano-composite; Pressure; Skutterudite; Thermoelectrics", "abstract": "New thermoelectric materials were synthesized using high-pressure techniques. The synthetic limits of cerium filling in cobalt triantimonide were explored and a model for successful synthesis conditions was generated. The high-pressure technique expanded the practical filling limit from x=0.07 to x=0.5 in the CexCo4Sb12 system. Explorations of cerium filled ruthenium-rhodium triantimonide were also undertaken, using our previous work to guide the synthesis attempt. This material was predicted to have outstanding thermoelectric properties, but our investigations did not confirm this result. The filled skutterudite, Ce(Ru0.67Rh0.33)4Sb12, exhibited the low thermal conductivity anticipated, approximately half the total thermal conductivity of a binary CoSb3 skutterudite over a wide range in temperatures. The electrical properties were insufficient to produce a high efficiency thermoelectric, but these results did suggest incorporated rare earth filling atoms do not fully ionize when incorporated into the skutterudite structure. Modification of the carrier type should therefore be investigated by solid solution on the transition metal or pnictide sites and not the filling ion.
\r\n\r\nThe high-pressure synthesis techniques developed for skutterudite synthesis were then employed to sinter nano-scale silicon-germanium compounds. A sintering figure of merit was created to justify the use of high-pressure synthesis, which later proved to be a useful tool for planning subsequent experiments. Sintered silicon, germanium, and silicon-germanium composites were obtained, with the nano-scale grain structure and chemical heterogeneity of the starting powder aggregate intact.
\r\n\r\nFuture work in high-pressure synthesis should be undertaken to quantify the sintering figure of merit presented in this work. The ability to produce a dense multiphase material with a controlled nano-structure should provide a great boon to thermoelectrics research. The high-pressure synthesis technique provides an method to mix two thermoelectric materials without homogenizing them. Both the two-phased solid and the network of nano-scale grains provide powerful tools for minimizing the thermal conductivity of a thermoelectric device component.
", "date": "2005", "date_type": "degree", "id_number": "CaltechETD:etd-05262005-004951", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05262005-004951", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2005-05-26", "doi": "10.7907/HWWN-NS80", "divisions": { "items": [ "div_eng" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "orcid": "0000-0001-6025-8925", "role": "advisor" } ] }, "thesis_committee": { "items": [ { "email": "asimow@gps.caltech.edu", "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "orcid": "0000-0001-6025-8925", "role": "chair" }, { "email": "btf@caltech.edu", "id": "Fultz-B-T", "name": { "family": "Fultz", "given": "Brent T." }, "orcid": "0000-0002-6364-8782", "role": "member" }, { "email": "grr@gps.caltech.edu", "id": "Rossman-G-R", "name": { "family": "Rossman", "given": "George Robert" }, "orcid": "0000-0002-4571-6884", "role": "member" }, { "email": "wag@wag.caltech.edu", "id": "Goddard-W-A-III", "name": { "family": "Goddard", "given": "William A., III" }, "orcid": "0000-0003-0097-5716", "role": "member" }, { "email": "wlj@caltech.edu", "id": "Johnson-W-L", "name": { "family": "Johnson", "given": "William Lewis" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2005-05-26", "thesis_defense_date": "2004-11-24", "thesis_approved_date": "2005-05-26", "review_status": "approved", "option_major": { "items": [ "matsci" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2005", "author_list": "Staneff, Geoffrey D.", "advisor_list": "Asimow, Paul David", "comittee_list": "Asimow, Paul David; Fultz, Brent T.; et el." }, { "id": "https://thesis.library.caltech.edu/id/eprint/2291", "eprint_id": 2291, "rev_number": 14, "documents": [ { "id": "/id/document/4321", "doc_id": 4321, "rev_number": 2, "files": [ { "id": "/id/file/24976", "fileid": 24976, "datasetid": "document", "objectid": 4321, "filename": "AkinsThesis_final_1sided.pdf", "mime_type": "application/pdf", "filesize": 1273040, "mtime": "2012-12-26 02:49:41", "url": "/2291/1/AkinsThesis_final_1sided.pdf" } ], "eprint_id": 2291, "pos": 1, "mime_type": "application/pdf", "format": "application/pdf", "format_desc": "AkinsThesis_final_1sided.pdf", "language": "en", "security": "public", "license": "other", "main": "AkinsThesis_final_1sided.pdf", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "content": "final", "relation": { "items": [ { "type": "http://eprints.org/relation/hasVolatileVersion", "uri": "/id/document/20908" }, { "type": "http://eprints.org/relation/haspreviewThumbnailVersion", "uri": "/id/document/20908" }, { "type": "http://eprints.org/relation/hasVersion", "uri": "/id/document/20908" } ] } }, { "id": "/id/document/20908", "doc_id": 20908, "rev_number": 2, "files": [ { "id": "/id/file/24974", "fileid": 24974, "datasetid": "document", "objectid": 20908, "filename": "preview.png", "mime_type": "image/png", "hash": "c0b0dbe2bdca32e446476ca42658efd6", "hash_type": "MD5", "filesize": 8679, "mtime": "2012-12-26 02:49:41", "url": "/2291/2/preview.png" } ], "eprint_id": 2291, "pos": 2, "placement": 2, "mime_type": "image/png", "format": "image/png", "language": "en", "security": "public", "license": "other", "main": "preview.png", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/4321" }, { "type": "http://eprints.org/relation/ispreviewThumbnailVersionOf", "uri": "/id/document/4321" }, { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/4321" } ] } }, { "id": "/id/document/122591", "doc_id": 122591, "rev_number": 1, "files": [ { "id": "/id/file/367989", "fileid": 367989, "datasetid": "document", "objectid": 122591, "filename": "indexcodes.txt", "mime_type": "text/x-c", "hash": "e6f3a52a649894c90445466642b3a2d2", "hash_type": "MD5", "filesize": 15902, "mtime": "2021-06-23 22:01:34", "url": "/2291/3/indexcodes.txt" } ], "eprint_id": 2291, "pos": 3, "placement": 3, "mime_type": "text/x-c", "format": "other", "format_desc": "Generate index codes conversion from application/pdf to indexcodes", "language": "en", "security": "public", "license": "other", "main": "indexcodes.txt", "media_duration": "0", "media_aspect_ratio": "0", "media_sample_start": "0", "media_sample_stop": "0", "relation": { "items": [ { "type": "http://eprints.org/relation/isVersionOf", "uri": "/id/document/4321" }, { "type": "http://eprints.org/relation/isVolatileVersionOf", "uri": "/id/document/4321" }, { "type": "http://eprints.org/relation/isIndexCodesVersionOf", "uri": "/id/document/4321" } ] } } ], "eprint_status": "archive", "userid": 2, "dir": "disk0/00/00/22/91", "datestamp": "2003-06-09", "lastmod": "2021-02-11 00:47:55", "status_changed": "2009-09-25 02:33:41", "type": "thesis", "metadata_visibility": "show", "creators": { "items": [ { "id": "Akins-Joseph-Albert", "name": { "family": "Akins", "given": "Joseph Albert" }, "show_email": "NO" } ] }, "title": "Dynamic Compression of Minerals in the MgO-FeO-SiO\u2082 System", "ispublished": "unpub", "full_text_status": "public", "keywords": "Hugoniot; mantle; melt; shock wave; silicates", "abstract": "The first shock wave experiments performed on silicate materials were reported for quartz in 1962. The intervening forty years have allowed for extensive investigation of SiO\u2082 by dynamic, static and theoretical means. Previous studies have concluded that quartz transforms completely to stishovite at ~40 GPa and melts at ~115 GPa along its Hugoniot. Recent discoveries that SiO\u2082 transforms to phases slightly more dense than stishovite have led to a reexamination of the dynamic compression of SiO\u2082 in this thesis. Based on comparing calculated Hugoniots to data for multiple initial SiO\u2082 phases, it is proposed that, in addition to the stishovite and melt transitions, quartz is completely transformed to the CaCl2 structure at ~70 GPa. Coesite shows evidence of complete transformation to stishovite at ~ 50 GPa, and to the CaCl2 structure at ~65 GPa. Due to the higher temperature achieved in the quartz samples the slope of the stishovite-CaCl2 phase boundary is constrained to be ~180 K/GPa.
\r\n\r\nFrom a similar analysis of Hugoniot data collected for high quality MgSiO3 natural crystal and synthetic glass in this study, and existing data, it is concluded that along the crystal Hugoniot akimotoite is attained at ~70 GPa, perovskite structure at ~110 GPa and melt at ~ 170 GPa. It is found that the melt is 2-3 % denser than the solid at pressures greater than 100 GPa, after correcting for thermal differences in the two regimes. An important implication is a negative Clapeyron slope, leading to a decreasing melting temperature with increasing pressure, above ~ 100 GPa. These observations increase the possibility of the existence of a significant amount of partial melt in the lowermost mantle, e.g., the ultra low velocity zone.
", "date": "2003", "date_type": "degree", "id_number": "CaltechETD:etd-05302003-142219", "refereed": "FALSE", "official_url": "https://resolver.caltech.edu/CaltechETD:etd-05302003-142219", "rights": "No commercial reproduction, distribution, display or performance rights in this work are provided.", "collection": "CaltechTHESIS", "reviewer": "Kathy Johnson", "deposited_by": "Imported from ETD-db", "deposited_on": "2003-06-09", "doi": "10.7907/NA1N-0B58", "alt_title": { "items": [ "Dynamic Compression of Minerals in the MgO-FeO-SiO2 System" ] }, "divisions": { "items": [ "div_gps" ] }, "institution": "California Institute of Technology", "thesis_type": "phd", "thesis_advisor": { "items": [ { "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "advisor" } ] }, "thesis_committee": { "items": [ { "id": "Asimow-P-D", "name": { "family": "Asimow", "given": "Paul David" }, "role": "chair" }, { "id": "Stevenson-D-J", "name": { "family": "Stevenson", "given": "David John" }, "role": "member" }, { "id": "Rossman-G-R", "name": { "family": "Rossman", "given": "George Robert" }, "role": "member" } ] }, "thesis_degree": "PHD", "thesis_degree_grantor": "California Institute of Technology", "thesis_submitted_date": "2003-05-30", "thesis_defense_date": "2003-05-30", "thesis_approved_date": "2003-06-09", "review_status": "approved", "option_major": { "items": [ "geol" ] }, "copyright_statement": "I hereby certify that, if appropriate, I have obtained a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee.\n\nI hereby grant to California Institute of Technology or its agents the non-exclusive\nlicense to archive and make accessible, under the conditions specified below,\nmy thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report.", "resource_type": "thesis", "pub_year": "2003", "author_list": "Akins, Joseph Albert", "advisor_list": "Asimow, Paul David", "comittee_list": "Asimow, Paul David; Stevenson, David John; et el." } ]