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Surface mapping based on the correlated emission of ions and electrons from hypervelocity C60 impactsEller, Michael 14 March 2013 (has links)
High resolution mapping of molecular species, specifically sub-micrometer spatial resolution mapping, is at the forefront of recent interest in Secondary Ion Mass Spectrometry (SIMS). Large projectiles, e.g. C60, Au400, display high quasi-molecular ion yields with reduced fragment ion yields compared to atomic or polyatomic projectiles. However, the application of large projectiles in a sub-micrometer beam is hampered by limitations in source brightness and angular emission characteristics which are incompatible with tight focusing. An alternate approach to a focused beam is to reduce the beam intensity to less than 1000 impacts per second (referred to as the event-by-event mode) and localize each projectile impact via an electron emission microscope. The characterization and performance of such an instrument for localizing individual projectile impacts of 15-75keV C60 with sub-micrometer spatial resolution are described here.
The quest for localizing single cluster impacts requires an understanding of the relationship between SI and electron emissions. It was found that electron emission is observed independently of the number or type of secondary ion emitted for flat homogeneous samples. The independence of ion and electron emission confirms the rationale for using the emitted electrons to localize individual projectile impacts. Further investigation of electron emission revealed that the electron yield is characteristic of the class of sample investigated (e.g. metal, organic, semiconductor). The electron yield was found to depend on the size and topology of the sample. Additionally, the electron yield increases with increasing projectile velocity.
The use of the novel instrumentation presented here, necessitated the development of custom acquisition and analysis software. The analysis of co-emitted species from nano-metric dimensions is enhanced with the ability to perform multiple coincidence/anti-coincidence calculations. New concepts were implemented for integrating localization and mass spectrometry via software solutions for image analysis and localization and subsequently correlation between emitted ions and electrons. The result is software and instrumentation capable of generating ion maps with sub-micrometer spatial resolution.
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Nano-Domain Analysis Via Massive Cluster Secondary Ion Mass Spectrometry in the Event-by-Event ModePinnick, Veronica Tiffany 2009 December 1900 (has links)
Secondary ion mass spectrometry (SIMS) is a surface analysis technique which characterizes species sputtered by an energetic particle beam. Bombardment with cluster projectiles offers the following notable advantages over bombardment with atomic ions or small clusters: enhanced emission of molecular ions, low damage cross-section, and reduced molecular fragmentation. Additionally, in the case of Au4004 and C60 impacts, desorption originates from nanometric volumes. These features make clusters useful probes to obtain molecular information from both nano-objects and nano-domains. The "event-by-event bombardment/detection mode" probes nano-objects one-at-a-time, while collecting and storing the corresponding secondary ion (SI) information.
Presented here are the first experiments where free-standing nano-objects were bombarded with keV projectiles of atomic to nanoparticle size. The objects are aluminum nano-whiskers, 2 nm in diameter and ~250 nm in length. Au4004 has a diameter of ~2 nm, comparable to the nominal diameter of the nanowhiskers. There are notable differences in the SI response from sample volumes too small for full projectile energy deposition. The whisker spectra are dominated by small clusters?the most abundant species being AlO- and AlO2-. Bulk samples have larger yields for AlO2- than for AlO-, while this trend is reversed in whisker samples. Bulk samples give similar abundances of large SI clusters, while whisker samples give an order of magnitude lower yield of these SIs. Effective yields were calculated in order to determine quantitative differences between the nano-objects and bulk samples.
The characterization of individual nano-objects from a mixture is demonstrated with negatively charged polymer spheres that are attracted to and retained by the nano-whiskers. The spheres are monodisperse polystyrene nanoparticles (30nm diameter). Our results show that the event-by-event mode can provide information on the nature, size, relative location, and abundance of nano-objects in the field of view. This study presents the first evidence of quantitative molecular information originating from nano-object mixtures.
Biologically relevant systems (solid-supported lipid bilayers) were also characterized using Au5 , Au4004 and C60 . Organization-dependent SI emission was observed for phosphocholine bilayers. Lipid domain formation was also investigated in bilayers formed from cholesterol and a mixed lipid system. Trends in the correlation coefficient suggest that cholesterol segregates from the surrounding lipid environment during raft formation.
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Non-Canonical Amino Acids as Minimal Tags for Investigating Protein Organization and TurnoverGebura-Vreja, Ingrid-Cristiana 14 October 2015 (has links)
No description available.
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Studies of Singly and Multiply Charged Secondary Ion Emission And The Effects Of Oxygen On Ionization And Sputter ErosionJanuary 2012 (has links)
abstract: Mass spectrometric analysis requires that atoms from the sample be ionized in the gas phase. Secondary ion mass spectrometry achieves this by sputtering samples with an energetic primary ion beam. Several investigations of the sputtering and ionization process have been conducted. Oxygen is commonly used in secondary ion mass spectrometry (SIMS) to increase ion yields, but also can complicate the interpretation of SIMS analyses. An 18O implant in silicon has been used to quantify the oxygen concentration at the surface of sputtered silicon in order to study the dependence on oxygen of several sputtering and depth profile phenomena. The ion yield dependence of trace elements in silicon on the surface oxygen concentration is a function of the ionization potential of the element. The ion yield is high and unaffected by oxygen for elements with low ionization potential and ranges over several orders of magnitude for elements with high ionization potential. Depth resolution in sputter profiles has been shown to be degraded by the presence of oxygen, the mechanism of this effect has been investigated using an 18O implant to quantify oxygen levels and it is shown that the process does not appear to be a consequence of surface oxide formation. Molecular ions are a source of mass interference in SIMS analysis, and multiply charged atomic ion signals might be interference-free due to the possible instability of multiply-charged molecular ions. Sputtered SiH2+, AlH2+, BeH2+, Mo22+ and Mg22+ ions have been observed and appear surprisingly stable. The formation mechanism of some of these species has been explored. / Dissertation/Thesis / Ph.D. Chemistry 2012
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Boron Isotopic Composition of the Subcontinental Lithospheric MantleJanuary 2014 (has links)
abstract: Boron concentrations and isotopic composition of phlogopite mica, amphibole, and selected coexisting anhydrous phases in mantle-derived xenoliths from the Kaapvaal Craton were measured by secondary ion mass spectrometry in an effort to better understand the B isotope geochemistry of the subcontinental lithospheric mantle (SCLM) and its implications for the global geochemical cycle of B in the mantle. These samples display a wide, and previously unrecognized, range in their boron contents and isotopic compositions reflecting a complex history involving melt depletion and metasomatism by subduction- and plume-derived components, as well as late stage isotopic exchange related to kimberlite emplacements. Micas from ancient lithospheric harzburgite metasomatized by slab-derived fluids suggest extensive B-depletion during subduction, resulting in low-B, isotopically light compositions whereas kimberlite-related metasomatic products and a sample from the 2 Ga Palabora carbonatite have boron isotopic compositions similar to proposed primitive mantle. The results suggest that subduction of oceanic lithosphere plays a limited role in the B geochemistry of the convecting mantle. / Dissertation/Thesis / Masters Thesis Geological Sciences 2014
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Bacterial attachment to polymeric materials correlates with molecular flexibility and hydrophilicitySanni, O., Chang, Chien-Yi, Anderson, D.G., Langer, R., Davies, M.C., Williams, P.M., Williams, P., Alexander, M.R., Hook, A.L. 09 December 2014 (has links)
Yes / A new class of material resistant to bacterial attachment has been discovered that is formed from polyacrylates with hydrocarbon pendant groups. In this study, the relationship between the nature of the hydrocarbon moiety and resistance to bacteria is explored, comparing cyclic, aromatic, and linear chemical groups. A correlation is shown between bacterial attachment and a parameter derived from the partition coefficient and the number of rotatable bonds of the materials' pendant groups. This correlation is applicable to 86% of the hydrocarbon pendant moieties surveyed, quantitatively supporting the previous qualitative observation that bacteria are repelled from poly(meth)acrylates containing a hydrophilic ester group when the pendant group is both rigid and hydrophobic. This insight will help inform and predict the further development of polymers resistant to bacterial attachment. / Wellcome Trust (grant number 085245) and EMRP (IND56)
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Chemical, Isotopic, and Textural Characteristics of Diamond Crystals and Their Mineral Inclusions from A154 South (Northwest Territories), Lynx (Quebec), and Kelsey Lake (Colorado): Implications for Growth Histories and Different Mantle EnvironmentsVan Rythoven, Adrian David 31 August 2012 (has links)
Parcels of diamond crystals from the A154 South kimberlite diatreme, Northwest Territories (n=281), and the Lynx kimberlite dyke, Quebec (n=6598) were examined in terms of colour, size, morphology, and UV fluorescence (A154 South samples only). A subset of stones from each parcel (A154 South: n=60, Lynx: n=20) were cut and polished to expose internal zonation and mineral inclusions. Exposed primary mineral inclusions were quantitatively analyzed for major elements by EMPA.
Diamond crystals from the Kelsey Lake kimberlite diatreme, Colorado (n=20), were cut into plates and analyzed for nitrogen aggregation states by FTIR. Twelve of these stones were then analyzed with further subsets from A154 South (n=18) and Lynx (n=16) for carbon isotope ratios and nitrogen abundances by SIMS. Every diamond crystal cut and polished had its internal zonation imaged with CL.
Mineral inclusion data from A154 South and Lynx show that the mantle keel of the Slave craton is slightly less depleted than that of the Superior craton, and both are less depleted than those of the Kaapvaal and Siberian cratons. Equilibration conditions plot on hotter geothermal gradients (surface heat flows ~42 mW/m2) than for those of typical Archean cratons (≤40 mW/m2). Equilibration temperatures (~1150-1250°C) are ~100-200°C hotter than previously reported from Kelsey Lake (~1020°C).
Kelsey Lake and A154 South samples have carbon isotope ratios and nitrogen contents typical of most diamond populations worldwide. Diamond crystals from Lynx are entirely different, consisting of mostly Type II diamond with δ13C (vs. PDB) values from approximately -3.6 ‰ to +1.7 ‰. These 13C-enriched samples are suggested to be the result of extreme Rayleigh fractionation of diamond from a carbonate fluid and possibly input of carbon sourced from subducted abiotic oceanic crust. Also notable is that growth trends (δ13C-[NT]) for most of the samples studied show little or no consistency with published fractionation models.
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Chemical, Isotopic, and Textural Characteristics of Diamond Crystals and Their Mineral Inclusions from A154 South (Northwest Territories), Lynx (Quebec), and Kelsey Lake (Colorado): Implications for Growth Histories and Different Mantle EnvironmentsVan Rythoven, Adrian David 31 August 2012 (has links)
Parcels of diamond crystals from the A154 South kimberlite diatreme, Northwest Territories (n=281), and the Lynx kimberlite dyke, Quebec (n=6598) were examined in terms of colour, size, morphology, and UV fluorescence (A154 South samples only). A subset of stones from each parcel (A154 South: n=60, Lynx: n=20) were cut and polished to expose internal zonation and mineral inclusions. Exposed primary mineral inclusions were quantitatively analyzed for major elements by EMPA.
Diamond crystals from the Kelsey Lake kimberlite diatreme, Colorado (n=20), were cut into plates and analyzed for nitrogen aggregation states by FTIR. Twelve of these stones were then analyzed with further subsets from A154 South (n=18) and Lynx (n=16) for carbon isotope ratios and nitrogen abundances by SIMS. Every diamond crystal cut and polished had its internal zonation imaged with CL.
Mineral inclusion data from A154 South and Lynx show that the mantle keel of the Slave craton is slightly less depleted than that of the Superior craton, and both are less depleted than those of the Kaapvaal and Siberian cratons. Equilibration conditions plot on hotter geothermal gradients (surface heat flows ~42 mW/m2) than for those of typical Archean cratons (≤40 mW/m2). Equilibration temperatures (~1150-1250°C) are ~100-200°C hotter than previously reported from Kelsey Lake (~1020°C).
Kelsey Lake and A154 South samples have carbon isotope ratios and nitrogen contents typical of most diamond populations worldwide. Diamond crystals from Lynx are entirely different, consisting of mostly Type II diamond with δ13C (vs. PDB) values from approximately -3.6 ‰ to +1.7 ‰. These 13C-enriched samples are suggested to be the result of extreme Rayleigh fractionation of diamond from a carbonate fluid and possibly input of carbon sourced from subducted abiotic oceanic crust. Also notable is that growth trends (δ13C-[NT]) for most of the samples studied show little or no consistency with published fractionation models.
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Studies of transport in some oxides by gas phase analysisDong, Qian January 2004 (has links)
No description available.
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Fluorine Partitioning Between Nominally Anhydrous Minerals (Olivine, Clinopyroxene, and Plagioclase) and Silicate Melt using Secondary Ion Mass Spectrometry and Newly Synthesized Basaltic Fluorine Microanalytical Glass StandardsJanuary 2012 (has links)
abstract: Fluorine (F) is a volatile constituent of magmas and hydrous mantle minerals. Compared to other volatile species, F is highly soluble in silicate melts, allowing F to remain in the melt during magma differentiation and rendering F less subject to disturbance during degassing upon magma ascent. Hence, the association between fluorine in basalts and fluorine in the mantle source region is more robust than for other volatile species. The ionic radius of F- is similar to that of OH- and O2-, and F may substitute for hydroxyl and oxygen in silicate minerals and melt. Fluorine is also incorporated at trace levels within nominally anhydrous minerals (NAMs) such as olivine, clinopyroxene, and plagioclase. Investigating the geochemical behavior of F in NAMs provides a means to estimate the pre-eruptive F contents of degassed magmas and to better understand the degassing behavior of H. The partition coefficients of F were determined for clinopyroxene, olivine, plagioclase, and hornblende within melts of olivine-minette, augite-minette, basaltic andesite, and latite compositions. The samples analyzed were run products from previously-published phase-equilibria experiments. Fluorine was measured by secondary ion mass spectrometry (SIMS) using an 16O- primary beam and detection of negative secondary ions (19F-, 18O-, 28Si-). SIMS ion intensities are converted to concentrations by analyzing matrix-matched microanalytical reference materials and constructing calibration curves. For robust F calibration standards, five basaltic glasses (termed Fba glasses) were synthesized in-house using a natural tholeiite mixed with variable amounts of CaF2. The Fba glasses were characterized for F content and homogeneity, using both SIMS and electron-probe microanalysis (EPMA), and used as F standards. The partition coefficients for clinopyroxene (0.04-028) and olivine (0.01-0.16) varied with melt composition such that DF (olivine-minette) < DF (augite-minette) < DF (basaltic andesite) < DF (latite). Crystal chemical controls were found to influence the incorporation of F into clinopyroxene, but none were found that affected olivine. Fluorine partitioning was compared with that of OH within clinopyroxenes, and the alumina content of clinopyroxene was shown to be a strong influence on the incorporation of both anions. Fluorine substitution into both olivine and clinopyroxene was found to be strongly controlled by melt viscosity and degree of melt polymerization. / Dissertation/Thesis / Ph.D. Geological Sciences 2012
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