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arXiv 2303.04513cond-mat.mes-hallphysics.optics
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时间分辨单粒子X射线散射揭示电子密度是相干等离激元纳米颗粒振荡的来源

Time-resolved single-particle x-ray scattering reveals electron-density as coherent plasmonic-nanoparticle-oscillation source

D. Hoeing, R. Salzwedel, L. Worbs, Y. Zhuang, A. K. Samanta, J. Lübke, A. Estillore, K. Dlugolecki, C. Passow, B. Erk, N. Ekanayaje, D. Ramm, J. Correa, C. C. P… 展开作者

D. Hoeing, R. Salzwedel, L. Worbs, Y. Zhuang, A. K. Samanta, J. Lübke, A. Estillore, K. Dlugolecki, C. Passow, B. Erk, N. Ekanayaje, D. Ramm, J. Correa, C. C. Papadooulou, A. T. Noor, F. Schulz, M. Selig, A. Knorr, K. Ayyer, J. Küpper, H. Lange

AI总结:

本研究结合瞬态吸收光谱与时间分辨单粒子X射线衍射成像,测量纳米颗粒呼吸振荡起始,并提出无拟合参数模型,证明光致电子密度梯度是主要相干驱动源。

摘要:

光激发等离激元纳米颗粒的动力学目前被理解为一系列连续的散射事件,涉及脉冲光激发后的热化过程。其中一个重要步骤是纳米颗粒呼吸振荡的启动。根据已确立的实验和模型,这些振荡由热化电子向晶格的统计性热传递引起。由于缺乏关于呼吸振荡起始的实验数据而出现相位不匹配,因此必须纳入热电子压力带来的额外贡献。我们使用光学瞬态吸收光谱和时间分辨单粒子X射线衍射成像来探测受激电子系统和晶格。时间分辨单粒子成像数据直接提供了呼吸振荡起始时的结构信息,并证实除热膨胀外还需要额外的激发机制;同时,结构与光学联合数据中观测到的相位依赖性与以往研究相矛盾。因此,我们建立了一个新模型,无需使用拟合参数即可复现全部实验观测结果。我们将光致电子密度梯度确定为主要驱动来源。

英文摘要:

Dynamics of optically-excited plasmonic nanoparticles are presently understood as a series of sequential scattering events, involving thermalization processes after pulsed optical excitation. One important step is the initiation of nanoparticle breathing oscillations. According to established experiments and models, these are caused by the statistical heat transfer from thermalized electrons to the lattice. An additional contribution by hot electron pressure has to be included to account for phase mismatches that arise from the lack of experimental data on the breathing onset. We used optical transient-absorption spectroscopy and time-resolved single-particle x-ray-diffractive imaging to access the excited electron system and lattice. The time-resolved single-particle imaging data provided structural information directly on the onset of the breathing oscillation and confirmed the need for an additional excitation mechanism to thermal expansion, while the observed phase-dependence of the combined structural and optical data contrasted previous studies. Therefore, we developed a new model that reproduces all our experimental observations without using fit parameters. We identified optically-induced electron density gradients as the main driving source.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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