Ratio estimation in SIMS analysis Ogliore, R.C.; Huss, G.R.; Nagashima, K.
Nuclear instruments & methods in physics research. Section B, Beam interactions with materials and atoms,
09/2011, Letnik:
269, Številka:
17
Journal Article
Recenzirano
The determination of an isotope ratio by secondary ion mass spectrometry (SIMS) traditionally involves averaging a number of ratios collected over the course of a measurement. We show that this ...method leads to an additive positive bias in the expectation value of the estimated ratio that is approximately equal to the true ratio divided by the counts of the denominator isotope of an individual ratio. This bias does not decrease as the number of ratios used in the average increases. By summing all counts in the numerator isotope, then dividing by the sum of counts in the denominator isotope, the estimated ratio is less biased: the bias is approximately equal to the ratio divided by the summed counts of the denominator isotope over the entire measurement. We propose a third ratio estimator (Beale’s estimator) that can be used when the bias from the summed counts is unacceptably large for the hypothesis being tested. We derive expressions for the variance of these ratio estimators as well as the conditions under which they are normally distributed. Finally, we investigate a SIMS dataset showing the effects of ratio bias, and discuss proper ratio estimation for SIMS analysis.
The Low-Energy Telescope (LET) is one of four sensors that make up the Solar Energetic Particle (SEP) instrument of the IMPACT investigation for NASA’s STEREO mission. The LET is designed to measure ...the elemental composition, energy spectra, angular distributions, and arrival times of H to Ni ions over the energy range from ∼3 to ∼30 MeV/nucleon. It will also identify the rare isotope
3
He and trans-iron nuclei with 30≤
Z
≤83. The SEP measurements from the two STEREO spacecraft will be combined with data from ACE and other 1-AU spacecraft to provide multipoint investigations of the energetic particles that result from interplanetary shocks driven by coronal mass ejections (CMEs) and from solar flare events. The multipoint in situ observations of SEPs and solar-wind plasma will complement STEREO images of CMEs in order to investigate their role in space weather. Each LET instrument includes a sensor system made up of an array of 14 solid-state detectors composed of 54 segments that are individually analyzed by custom Pulse Height Analysis System Integrated Circuits (PHASICs). The signals from four PHASIC chips in each LET are used by a Minimal Instruction Set Computer (MISC) to provide onboard particle identification of a dozen species in ∼12 energy intervals at event rates of ∼1,000 events/sec. An additional control unit, called SEP Central, gathers data from the four SEP sensors, controls the SEP bias supply, and manages the interfaces to the sensors and the SEP interface to the Instrument Data Processing Unit (IDPU). This article outlines the scientific objectives that LET will address, describes the design and operation of LET and the SEP Central electronics, and discusses the data products that will result.
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We review recent results on O‐ and Mg‐isotope compositions of refractory grains (corundum, hibonite) and calcium, aluminum‐rich inclusions (CAIs) from unequilibrated ordinary and carbonaceous ...chondrites. We show that these refractory objects originated in the presence of nebular gas enriched in 16O to varying degrees relative to the standard mean ocean water value: the Δ17OSMOW value ranges from approximately −16‰ to −35‰, and recorded heterogeneous distribution of 26Al in their formation region: the inferred (26Al/27Al)0 ranges from approximately 6.5 × 10−5 to <2 × 10−6. There is no correlation between O‐ and Mg‐isotope compositions of the refractory objects: 26Al‐rich and 26Al‐poor refractory objects have similar O‐isotope compositions. We suggest that 26Al was injected into the 26Al‐poor collapsing protosolar molecular cloud core, possibly by a wind from a neighboring massive star, and was later homogenized in the protoplanetary disk by radial mixing, possibly at the canonical value of 26Al/27Al ratio (approximately 5 × 10−5). The 26Al‐rich and 26Al‐poor refractory grains and inclusions represent different generations of refractory objects, which formed prior to and during the injection and homogenization of 26Al. Thus, the duration of formation of refractory grains and CAIs cannot be inferred from their 26Al‐26Mg systematics, and the canonical (26Al/27Al)0 does not represent the initial abundance of 26Al in the solar system; instead, it may or may not represent the average abundance of 26Al in the fully formed disk. The latter depends on the formation time of CAIs with the canonical 26Al/27Al ratio relative to the timing of complete delivery of stellar 26Al to the solar system, and the degree of its subsequent homogenization in the disk. The injection of material containing 26Al resulted in no observable changes in O‐isotope composition of the solar system. Instead, the variations in O‐isotope compositions between individual CAIs indicate that O‐isotope composition of the CAI‐forming region varied, because of coexisting of 16O‐rich and 16O‐poor nebular reservoirs (gaseous and/or solid) at the birth of the solar system, or because of rapid changes in the O‐isotope compositions of these reservoirs with time, e.g., due to CO self‐shielding in the disk.
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Ratios determined from counting a subset of atoms in a sample are positively biased relative to the true ratio in the sample (Ogliore et al. 2011). The relative magnitude of the bias is ...approximately equal to the inverse of the counts in the denominator of the ratio. SIMS studies of short‐lived radionuclides are particularly subject to the problem of ratio bias because the abundance of the daughter element is low, resulting in low count rates. In this paper, we discuss how ratio bias propagates through mass‐fractionation corrections into an isochron diagram, thereby affecting the inferred initial ratio of short‐lived radionuclides. The slope of the biased isochron can be either too high or too low, depending on how it is calculated. We then reanalyze a variety of previously published data sets and discuss the extent to which they were affected by ratio bias. New, more accurate, results are presented for each study. In some cases, such as for 53Mn‐53Cr in pallasite olivines and 60Fe‐60Ni in chondrite sulfides, the apparent excesses of radiogenic isotopes originally reported disappear completely. Many of the reported initial 60Fe/56Fe ratios for chondrules from ordinary chondrites are no longer resolved from zero, though not all of them. Data for 10Be‐10B in CAIs were only slightly affected by bias because of how they were reduced. Most of the data sets were recalculated using the ratio of the total counts, which increases the number of counts in the denominator isotope and reduces the bias. However, if the sum of counts is too low, the ratio may still be biased and a less‐biased estimator, such as Beale’s estimator, must be used. Ratio bias must be considered in designing the measurement protocol and reducing the data. One can still collect data in cycles to permit editing of the data and to monitor and correct for changes in ion‐beam intensity, even if total counts are used to calculate the final ratio. The cycle data also provide a more robust estimate of the uncertainties from temporal variations in the secondary ion signal.
The presence of crystalline silicates in the comae of comets, inferred through infrared observations, has been a long-standing puzzle. Crystalline silicates are unexpected if comets are composed of ...pristine interstellar material, since interstellar silicates are almost entirely amorphous. Heating to >1100 K can anneal silicates to crystallinity, but no protoplanetary heating sources have been identified that were sufficiently strong to heat materials in the outer nebula to such high temperatures. This conundrum led to the suggestion that large-scale mixing was important in the protoplanetary disk. Reports of refractory calcium-aluminum-rich inclusion-like objects and large concentrations of noble gases in Stardust samples underscore the need for such mixing. However, the evidence from the Stardust samples until now has been largely anecdotal, and it has not been possible to place quantitative constraints on the mixing fraction. Here we report synchrotron-based X-ray microprobe measurements of the relative concentrations of the chemical state of iron in material from a known comet, the Jupiter-family comet 81P/Wild2. We find that the comet is rich in iron sulfides. The elemental S/Fe ratio based on the sulfide concentration, S/Fe >0.31(2s), is higher than in most chondritic meteorites. We also found that Fe-bearing silicates are at least 50% crystalline. Based on these measurements, we estimate the fraction v of inner nebular material in 81P/Wild2. With the lower bound on the crystalline Fe-bearing silicate fraction, we find that v>0.5. If the observed S depletion in the inner solar system predated or was contemporaneous with large-scale mixing, our lower bound on the S/Fe ratio gives an upper bound on v of ~0.65. This measurement may be used to test mixing models of the early solar system.
We investigated the surface texture and chemical compositions of two ~40-μm particles returned from the surface regolith of asteroid Itokawa (RB-DQ04-0062 and RB-DQ04-0091) by the Japan Aerospace ...Exploration Agency’s Hayabusa mission. We identified splash melts, surface blistering, and many small adhering particles. Seven focused ion beam sections were extracted from both Itokawa particles, targeting one splash melt and ten adhering particles to investigate their composition and provenance and the role of micrometeoroid impacts on Itokawa’s surface. Based on the particle’s structure, mineralogy, and interface between the adhering particle and host grain, we identified lithic fragments and particles deposited by impact. These have morphologies and compositions consistent with impact-generated deposits: two have morphologies and compositions that are consistent with impact-generated silica glass, and one was a Ni-free, metallic Fe, and S-rich assemblage that was likely generated by vapor recondensation during a micrometeoroid impact. This study shows that, even though its regolith is young, micrometeoroid impacts have altered the regolith of asteroid Itokawa.
This study aims to understand the formation of hydrated micrometeorites through detailed descriptions of their mineralogy and measurements of their isotopic compositions. The secondary mineralogy of ...hydrated cometary micrometeorites may differ from hydrated asteroidal particles because the conditions of cometary alteration were likely different from asteroidal aqueous alteration. In addition, the O isotopic composition of secondary minerals in cometary particles may also be distinct and reflect the presence of spatially distinct water reservoirs in the solar nebula 1-4. Here we present the mineralogy and oxygen isotope compositions of magnetite grains and a magnetite- dolomite assemblage that were identified in five hydrated AMMs. The purpose of these measurements is to investigate the diversity of the water reservoir from which hydrated AMMs formed and the temperature at which these minerals co-precipitated.
We report the petrology, O isotopic composition, and Al-Mg isotope systematics of a chondrule fragment from the Jupiter-family comet Wild 2, returned to Earth by NASA's Stardust mission. This object ...shows characteristics of a type II chondrule that formed from an evolved oxygen isotopic reservoir. No evidence for extinct super(26)Al was found, with ( super(26)Al/ super(27)Al) sub(0) < 3.0 x 10 super(-6). Assuming homogenous distribution of super(26)Al in the solar nebula, this particle crystallized at least 3 Myr after the earliest solar system objects-relatively late compared to most chondrules in meteorites. We interpret the presence of this object in a Kuiper Belt body as evidence of late, large-scale transport of small objects between the inner and outer solar nebula. Our observations constrain the formation of Jupiter (a barrier to outward transport if it formed further from the Sun than this cometary chondrule) to be more than 3 Myr after calcium-aluminum-rich inclusions.
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