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Development of analytical technique for in-situ determinations of trace elements using LA-ICP-MS and its application to metals in Acfer 094 chondrite

槇納, 好岐東京大学 DOI:10.15083/0002004739

2022.06.22

概要

Chondrites are one of the most primitive materials in the Solar System, and the cosmochemical features of the chondrites can provide various important clues to understand the diversity of the constituting materials through the evolution sequence of the Solar System and planets. Both the mineralogical, chemical and isotopic signature of the chondrites can vary significantly due to different physicochemical reactions, reflecting the evolution of the Solar System. Despite the obvious success in obtaining the genetic link between the origin of the chondrites and spatial distribution of elements within the Solar System, the elemental distribution in chondrites, that reflect the physicochemical conditions of the reaction, are not well understood. Thus, elucidation of the mechanism of variations of the elemental composition of the chondrites is still a key issue to understand the chemical evolution of the Solar System.

Metals in the chondritic materials are mainly composed of Fe-Ni metallic alloys and were ubiquitously present in almost all the chondrites. The Fe-Ni metals contain series of siderophile elements (iron-loving elements) in various concentration levels, that reflects the physicochemical conditions, such as formation temperature and oxygen fugacity, and thus, the cosmochemical features of metal grains can be used to decipher the chemical evolution of our Solar System.

To do this, we have developed a new analytical technique using the laser ablation-ICP-mass spectrometry (LA-ICP-MS technique) to derive reliable elemental data from the Fe-Ni metals presented in chondrites, aiming at to understand evolution sequence of the Solar System. LAICP-MS has been used for the in-situ trace elemental analysis, however, the practical use of the LA-ICP-MS technique for chondrites was retarded by both the lower elemental sensitivity and lower spatial resolution, and thus, further improvement of the elemental sensitivity and ability to measure siderophile elements from small sized metal grains were highly desired. To study the chemical fractionation of the early Solar System recorded in metals in chondrite, we improved the analytical technique including instrumental and methodological developments and applied the technique to the Acfer 094 chondrite.

In Chapter 1, we reviewed the background of (i) chemical fractionation in the early Solar System, (ii) chondrite and their chemical composition, (iii) trace elements in metal phase, and (iv) LA-ICP-MS.

In Chapter 2, new analytical technique to determine trace elements in metal grains of the chondrites based on the LA-ICP-MS was described.

In Section 2.1, new protocols for laser sampling using the very low fluence was developed (i.e., soft ablation protocol). With the soft ablation protocol, selective ablation of only metal grains can be made, abbreviating the risk of laser ablation of silicate phases, thus an elemental analysis of metal grains smaller than the laser spot size can be made.

In Section 2.2, a multiple spot laser ablation (msLA) using the high-repetition rate laser system was developed to improve the analytical sensitivity and the calibration technique. With the multiple spot laser ablation, laser-induced sample aerosols released from the inclusion can be integrated within the sampling cell, and the resulting mixture of the sample aerosols was then introduced into the ICP-MS within in short time period. The unique features achieved by the multiple spot ablation were described in this thesis.

In Chapter 3, newly developed analytical technique using the combination of soft ablation protocol and multiple spot ablation technique were demonstrated and applied for the elemental analysis from Fe-Ni metals in Acfer 094 chondrite. Based on the data obtained here, the fractionation process of trace elements in metal grains associated with ameboid olivine aggregates (AOAs), chondrule and matrix in Acfer 094 was discussed. The compositions of highly refractory elements (Re, Os, W, and Ir) in the Fe-Ni metals found in the AOAs showed complementary results to those found in Ca-Al-rich inclusions (CAIs). The measured complementarity of the refractory elements between AOAs and CAIs suggests that the AOAs were formed through condensation from the gas reservoir, which CAIs were already removed.

In Chapter 4, the summary of this thesis and the future prospects are described.

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Development of analytical technique for in-situ determinations of trace elements using LA-ICP-MS and its application to metals in Acfer 094 chondrite

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