Accurate determination of sulfur isotopes (δ33S and δ34S) in sulfides and elemental sulfur by femtosecond laser ablation MC-ICP-MS with non-matrix matched calibration†,Journal of Analytical Atomic Spectrometry

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Accurate determination of sulfur isotopes (δ33S and δ34S) in sulfides and elemental sulfur by femtosecond laser ablation MC-ICP-MS with non-matrix matched calibration†
Journal of Analytical Atomic Spectrometry ( IF 3.1 ) Pub Date : 2017-09-26 00:00:00 , DOI: 10.1039/c7ja00282c
Jiali Fu _{1,

2,

3,

4,

5} , Zhaochu Hu _{1,

2,

3,

4,

5} , Jianwei Li _{1,

2,

3,

4,

5} , Lu Yang _{6,

7,

8} , Wen Zhang _{1,

2,

3,

4,

5} , Yongsheng Liu _{1,

2,

3,

4,

5} , Qiuli Li _{5,

9,

10,

11,

12} , Keqing Zong _{1,

2,

3,

4,

5} , Shenghong Hu _{1,

2,

3,

4,

5}

Affiliation

The isotopic composition of sulfur is a vital tracer used in the Earth and planetary sciences. In this study, the laser- and ICP-induced isotopic fractionation in S-rich minerals (sulfides and elemental S) with different matrices was investigated by using 257 nm femtosecond (fs) and 193 nm ArF excimer nanosecond (ns) laser ablation systems coupled to a Neptune Plus MC-ICP-MS. Compared to ns-LA-MC-ICP-MS, higher sensitivity (1.4–2.4 times) under similar instrumental conditions and better precision (∼1.6-fold) under the same signal intensity condition were achieved by fs-LA-MC-ICP-MS. In addition, a fs-laser provides less fluence and matrix dependent S isotopic fractionation, and more stable transient isotopic ratios compared to a ns-laser. Better results acquired by fs-LA-MC-ICP-MS were attributed to the smaller size of particles and less thermal effect produced by using the fs-laser, which were evidenced by the morphologies of the ablation craters and ejected aerosol particles of P-S-1 (the pressed powder pellet of IAEA-S-1) and PPP-1 (a pyrite single crystal from the Sukhoi Log deposit). The ICP-induced isotopic fractionation (matrix effect) was still found in fs-LA-MC-ICP-MS under the maximum sensitivity conditions. However, a significant reduction of the matrix effect was obtained under robust plasma conditions at a lower makeup gas flow rate (0.52–0.54 l min⁻¹) relative to the maximum sensitivity condition (0.6 l min⁻¹) for S isotope analysis. This could be ascribed to the particles that not only pass into the higher temperature ICP for a longer residence time at a lower makeup gas flow rate that resulted in more efficient vaporization of the particles, but also experience a more robust plasma induced by adding 4–6 ml min⁻¹ N₂ into the plasma. Furthermore, under the robust conditions, the results of six reference materials with different matrices obtained by fs-LA-MC-ICP-MS with non-matrix matched calibration with a spot size of 20–44 μm showed excellent agreement with the reference values (the accuracy of 0.01–0.15‰ for δ³⁴S and 0.11–0.45‰ for δ³³S and the precision of 0.16–0.40‰ (2 s) for δ³⁴S and 0.35–0.78‰ (2 s) for δ³³S) and the mass-dependent fractionation line, validating the applicability of the proposed approach for providing high-quality in situ isotope data (δ³³S and δ³⁴S) of sulfides and elemental sulfur at high spatial resolution using non-matrix matched analysis.

中文翻译：

精确地确定硫同位素（的δ ³³ S和δ ³⁴ S）在硫化物和元素硫通过飞秒激光烧蚀MC-ICP-MS与非基质匹配校准†

硫的同位素组成是地球和行星科学中使用的重要示踪剂。在这项研究中，通过使用257 nm飞秒（fs）和193 nm ArF受激准分子纳秒（ns）激光烧蚀系统，研究了不同基质的富S矿物（硫化物和元素S）中激光和ICP诱导的同位素分馏升级到Neptune Plus MC-ICP-MS。与ns-LA-MC-ICP-MS相比，fs-LA-MC-ICP-MS在相同的仪器条件下具有更高的灵敏度（1.4-2.4倍），在相同的信号强度条件下具有更高的精度（约1.6倍）。多发性硬化症。另外，与ns激光器相比，fs激光器提供的通量和基质依赖性S同位素分馏较少，并且瞬态同位素比更稳定。通过fs-LA-MC-ICP-MS获得的更好结果归因于使用fs激光的颗粒尺寸较小和产生的热效应较小，这由消融坑和射出的PS-气溶胶颗粒的形态所证明。 1（IAEA-S-1的压制粉末颗粒）和PPP-1（来自Sukhoi Log矿床的黄铁矿单晶）。在最大灵敏度条件下，仍在fs-LA-MC-ICP-MS中发现ICP诱导的同位素分级分离（基质效应）。但是，在强劲的等离子体条件下，在较低的尾吹气流速（0.52-0.54 l min）下，基质效应得到了显着降低。它们的形状由烧蚀坑的形态和PS-1（IAEA-S-1的压制粉末颗粒）和PPP-1（来自Sukhoi Log矿的黄铁矿单晶）喷出的气溶胶颗粒证明。在最大灵敏度条件下，仍在fs-LA-MC-ICP-MS中发现ICP诱导的同位素分级分离（基质效应）。但是，在强劲的等离子体条件下，在较低的尾吹气流速（0.52-0.54 l min）下，基质效应得到了显着降低。它们的形状由烧蚀坑的形态和PS-1（IAEA-S-1的压制粉末颗粒）和PPP-1（来自Sukhoi Log矿的黄铁矿单晶）喷出的气溶胶颗粒证明。在最大灵敏度条件下，仍在fs-LA-MC-ICP-MS中发现ICP诱导的同位素分级分离（基质效应）。但是，在强劲的等离子体条件下，在较低的尾吹气流速（0.52-0.54 l min）下，基质效应得到了显着降低。^-1）相对于S同位素分析的最大灵敏度条件（0.6 l min^-1）。这可能归因于这样的颗粒：不仅在较低的尾吹气流速下进入较高温度ICP的时间更长，从而导致颗粒更有效地汽化，而且通过加入4 –至少6 ml^-1 N₂进入血浆。此外，在稳定的条件下，通过fs-LA-MC-ICP-MS进行的非基质匹配校准的六种不同基质的标准样品的斑点尺寸为20-44μm，结果与基准值具有极佳的一致性（ 0.01-0.15‰的准确性δ ³⁴ S和0.11〜0.45‰， δ³³ S和的0.16-0.40的精度‰（2秒） δ ³⁴ S和0.35-0.78‰（2个）， δ ³³ S）和所述质量依赖性分馏线，验证了该方法的适用性，用于提供高-quality原位同位素数据（ δ ³³ S和δ ³⁴ S）使用非匹配矩阵分析硫化物和元素硫在高空间分辨率的。

更新日期：2017-09-26

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