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From plasma to nanoparticles: optical and particle emission of a spark discharge generator

机译：从等离子体到纳米颗粒：火花放电发电机的光学和颗粒发射

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The increased demand for high purity nanoparticles (NPs) of defined geometry necessitates the continuous development of generation routes. One of the most promising physical techniques for producing metal, semiconductor or alloy NPs in the gas phase is spark discharge NP generation. The technique has a great potential for up-scaling without altering the particles. Despite the simplicity of the setup, the formation of NPs in a spark discharge takes place via complex multi-scale processes, which greatly hinders the investigation via conventional NP measurement techniques. In the present work, time-resolved optical emission spectroscopy (OES) was used to provide information on the species present in the spark from as early as approximately 100 ns after the initiation of the discharge. We demonstrate that operando emission spectroscopy can deliver valuable insights into NP formation. The emission spectra of the spark are used to identify, among others, the main stages of material erosion and to calculate the quenching rate of the generated metal vapour. We demonstrate that the alteration of key control parameters, that are typically used to optimize NP generation, clearly affect the emission spectra. We report for Cu and Au NPs that the intensity of spectral lines emitted by metal atoms levels off when spark energy is increased above an energy threshold, suggesting that the maximum concentration of metal vapour produced in the generator is limited. This explains the size variation of the generated NPs. We report a strong correlation between the optical and particle emission of the spark discharge generator, which demonstrate the suitability of OES as a valuable characterization tool that will allow for the more deliberate optimization of spark-based NP generation.
机译：对于限定的几何形状的高纯度纳米颗粒（NP）的需求增加必要生成路线的不断发展。一个用于在气相中生产金属，半导体或合金纳米颗粒的最有希望的物理技术是火花放电NP生成。该技术具有向上扩展的巨大潜力，而不改变颗粒。尽管设置的简单性，NP的一个火花放电形成需要通过复杂的多尺度方法，其极大地阻碍通过常规NP测量技术调查地方。在目前的工作，时间分辨发射光谱（OES）来从提供关于存在于该火花物种信息作为放电开始后早在约100毫微秒。我们证明operando发射光谱可以提供宝贵的见解NP形成。火花的发射光谱被用于识别，除其他外，材料侵蚀的主要阶段，并计算所产生的金属蒸汽的淬火速率。我们表明，关键控制参数，即通常用来优化NP生成的改变，明确地影响发射光谱。我们报告的Cu和Au中的NP其由金属原子水平时火花能量高于能量阈值增加，这表明在发电机产生的金属蒸汽的最大浓度被限制掉发射光谱线的强度。这解释了产生的纳米粒子的大小变化。我们报告的火花放电发生器，其证明OES的适用性作为一种有价值的表征工具，将允许基于火花NP一代更加审慎优化的光学和粒子发射之间存在很强的相关性。

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