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In situ speciation and spatial mapping of Zn products during pulsed laser ablation in liquids (PLAL) by combined synchrotron methods.
Nanoscale ( IF 6.7 ) Pub Date : 2020-06-16 , DOI: 10.1039/d0nr01500h
Stefan Reich 1 , Jörg Göttlicher , Anna Ziefuss , René Streubel , Alexander Letzel , Andreas Menzel , Olivier Mathon , Sakura Pascarelli , Tilo Baumbach , Marcus Zuber , Bilal Gökce , Stephan Barcikowski , Anton Plech
Affiliation  

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.

中文翻译:

通过组合同步加速器方法在液体中脉冲激光烧蚀(PLAL)过程中对锌产品进行原位形成和空间定位。

液体中的脉冲激光烧蚀是生产纯无机纳米粒子胶体的分级多步骤过程。对单个步骤和结构形成的部分理解阻碍了对这一过程的控制。原位X射线方法用于解析纳秒级PLAL的宏观动力学,并以微秒级的时间分辨率分析烧蚀物种的分布和形态。可以通过基于同步加速器的方法实现高时间分辨率,该方法能够“单次”采集。通过Shack-Hartmann装置(XHI)和小角度X射线散射(SAXS)进行的X射线多对比度成像可解决瞬态空化气泡内部不断发展的纳米粒子,而在分散模式下的X射线吸收光谱可提供获得总材料收率的途径。喷射物的化学状态。证实了在消融期间直接产生纳米颗粒以及检测到反应性材料,其在早期被识别为Zn原子。空化气泡中的纳米颗粒显示出金属特征,在逐渐发生氧化之前,这种现象持续数毫秒。消融是通过目标蒸发与完全蒸发共存的阶段爆炸来描述的。氧化仅发生在已经形成的纳米颗粒的后续步骤中。
更新日期:2020-07-09
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