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Reorganizing and shaping of embedded near-coalescence silver nanoparticles with off-resonance femtosecond laser pulses

机译：利用失谐飞秒激光脉冲对嵌入的近凝聚银纳米颗粒进行重组和整形

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摘要

We demonstrate that 2D distributions of non-spherical near-coalescence silver nanoparticles (NPs) embedded in an ultrathin dielectric film can be reorganized, shaped and aligned by exposure to ultrashort laser pulses. As-grown samples prepared by pulsed laser deposition show a broad absorption band with a surface plasmon resonance (SPR) at 650 nm, which can be blue-shifted down to 440 nm and transformed to show polarization anisotropy. In situ white light probing of the spectral sample transmission allows control during irradiation of the position and polarization anisotropy of the SPR, effectively controlling particle reorganization and shaping. Using the high spatial resolution of the optical probe technique (better than 10 μm), the dependence of the nanoparticle shape and distribution on the local fluence can be studied in a single irradiated region. The results inferred from the spectral measurements have been confirmed by TEM studies, showing the formation of nanoparticles with prolate shape, preferential alignment along the polarization axis of the laser and a narrow size distribution. This simple and efficient approach for NP shaping and the straightforward extension to multilayer systems offer excellent perspectives for optical encoding, multidimensional data storage and fabrication of complex, polarization-sensitive spectral masks starting from thin films with near-coalescence distributions of NPs.
机译：我们证明了嵌入超薄介电膜中的非球形近凝聚银纳米颗粒（NPs）的2D分布可以通过暴露于超短激光脉冲而进行重组，定型和对齐。通过脉冲激光沉积制备的成年样品在650 nm处显示出宽吸收带，并具有表面等离振子共振（SPR），可以将其蓝移至440 nm并转化为偏振各向异性。光谱样本透射的原位白光探测可在辐照SPR的位置和偏振各向异性期间进行控制，从而有效地控制粒子的重组和整形。使用光学探针技术的高空间分辨率（小于10μm），可以在单个照射区域中研究纳米颗粒形状和分布对局部注量的依赖性。由光谱测量推断出的结果已通过TEM研究得到证实，显示出具有长圆形，沿激光的偏振轴优先排列和窄尺寸分布的纳米颗粒的形成。这种简单而有效的NP成形方法以及对多层系统的直接扩展，为光学编码，多维数据存储以及制造复杂，对偏振敏感的光谱掩模（从具有NP的近凝聚分布的薄膜开始）提供了极好的视角。

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