Near-Field Induced Reaction Yields from Nanoparticle Clusters
Near-Field Induced Reaction Yields from Nanoparticle Clusters
复制标题
DOI：
10.1021/acsphotonics.0c00823
复制
发表时间：
2020-07-15
期刊：
影响因子：
7
通讯作者：
Kling, Matthias F.
中科院分区：
文献类型：
--
作者：
Rosenberger, Philipp;Rupp, Philipp;Kling, Matthias F.
雾化纳米颗粒上的超快光诱导分子反应可能阐明纳米颗粒光活性的早期步骤，并在从化学、医学到气候科学等领域产生潜在影响。在测量光诱导反应产率时，纳米颗粒流的原位形态区分是至关重要的，但缺乏。在这里，我们通过实验证明，利用反应纳米显微镜技术，强飞秒脉冲诱导的去质子化反应的质子动量对单个二氧化硅纳米球及其团簇表现出清晰、可区分的特征。我们的发现得到了经典轨迹蒙特卡罗模拟的支持。结果证明了光诱导过程中单粒子及其团簇反应产率的原位单次判别方法。我们发现簇的电离在足够低的强度下占主导地位，这为解决先前观察到的实验数据和理论处理之间的差异提供了一个解释，这些处理只考虑了单个纳米颗粒。
Ultrafast light-induced molecular reactions on aerosolized nanoparticles may elucidate early steps in the photoactivity of nanoparticles with potential impact in fields ranging from chemistry and medicine to climate science. In situ morphology discrimination for nanoparticle streams when measuring light-induced reaction yields is crucial, but lacking. Here, we experimentally demonstrate, using the reaction nano-scopy technique, that proton momenta from deprotonation reactions induced by intense femtosecond pulses exhibit clear, distinguishable signatures for single silica nanospheres and their clusters. Our findings are supported by classical trajectory Monte Carlo simulations. The results demonstrate an in situ single-shot discrimination method between reaction yields from photoinduced processes on single particles and their clusters. We find that the ionization of clusters dominates at sufficiently low intensities, providing an explanation to resolve previously observed discrepancies between experimental data and theoretical treatments, which considered only single nanoparticles.