In situ speciation and spatial mapping of Zn products during pulsed laser ablation in liquids (PLAL) by combined synchrotron methods.
In situ speciation and spatial mapping of Zn products during pulsed laser ablation in liquids (PLAL) by combined synchrotron methods.
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DOI：
10.1039/d0nr01500h
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发表时间：
2020-06
期刊：
影响因子：
6.7
通讯作者：
S. Reich;J. Göttlicher;A. Ziefuss;R. Streubel;Alexander Letzel;A. Menzel;O. Mathon;S. Pascarelli;T. Baumbach;M. Zuber;Bilal Gökce;S. Barcikowski;A. Plech
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文献类型：
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作者：
S. Reich;J. Göttlicher;A. Ziefuss;R. Streubel;Alexander Letzel;A. Menzel;O. Mathon;S. Pascarelli;T. Baumbach;M. Zuber;Bilal Gökce;S. Barcikowski;A. Plech
液体中的脉冲激光烧蚀是一个分级的多步骤过程，以产生纯无机纳米粒子胶体。控制这一过程是阻碍个别步骤和结构形成的部分理解。原位X射线方法被用来解决宏观动力学的纳秒PLAS以及分析烧蚀物种的分布和形态与微秒的时间分辨率。高时间分辨率可以通过基于同步加速器的方法来实现，该方法能够“单次”采集。通过Shack-Hartmann装置（XHI）和小角X射线散射（SAXS）进行的X射线多重对比成像解决了瞬态空化气泡内不断变化的纳米颗粒，而分散模式的X射线吸收光谱则可以获得总的材料产量和喷出物的化学状态。据证实，在烧蚀过程中直接产生纳米颗粒，以及检测到的反应性材料，这是在早期阶段确定为锌原子。空泡内的纳米颗粒显示出金属特征，在逐渐氧化之前，这种特征持续了几毫秒。烧蚀被描述为目标的相爆炸与完全蒸发共存。氧化仅作为已经形成的纳米颗粒的后续步骤发生。
Pulsed laser ablation in liquids is a hierarchical multi-step process to produce pure inorganic nanoparticle colloids. Controlling this process is hampered by the partial understanding of individual steps and structure formation. In situ X-ray methods are employed to resolve macroscopic dynamics of nanosecond PLAL as well to analyse the distribution and speciation of ablated species with a microsecond time resolution. High time resolution can be achieved by synchrotron-based methods that are capable of 'single-shot' acquisition. X-ray multicontrast imaging by a Shack-Hartmann setup (XHI) and small angle X-ray scattering (SAXS) resolve evolving nanoparticles inside the transient cavitation bubble, while X-ray absorption spectroscopy in dispersive mode opens access to the total material yield and the chemical state of the ejecta. It is confirmed that during ablation nanoparticles are produced directly as well as reactive material is detected, which is identified in the early stage as Zn atoms. Nanoparticles within the cavitation bubble show a metal signature, which prevails for milliseconds, before gradual oxidation sets in. Ablation is described by a phase explosion of the target coexisting with full evaporation. Oxidation occurs only as a later step to already formed nanoparticles.