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Time-resolved investigation of laser-induced shape transformation of silver nanoparticles

机译：激光诱导的银纳米粒子形状转变的时间分辨研究

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摘要

Laser-induced permanent shape transformation dynamics of glass-embedded silver nanoparticles is investigated by a pulse-pair irradiation technique, where the nanoparticles are irradiated by pairs of time-delayed femtosecond laser pulses. The temporal evolution of surface plasmon extinction bands is obtained up to a time delay of 1 ns. We find that the aspect ratio of the modified nanoparticles, i.e., the observed dichroism, reduces rapidly to a minimum level within 20 ps after the laser irradiation. From that interpulse delay onward, the resulting aspect ratio stays at that minimum level until 100 ps. Subsequently, for longer time delays, the aspect ratio increases again until 1 ns. Temperature modeling of the nanoparticle-glass system gives evidence that the intermediately reduced dichroism is due to the high diffusion mobility that emitted silver ions can possess within a shell of heated glass around the nanoparticle, in a time window of 100 ps. For longer time delays the size of the heated glass shell gets reduced, thereby limiting the range of ionic diffusion. The theoretical estimations confirm the experimental results and suggest that the nanoparticle shape changes depend strongly on the thermal situation induced to the surrounding glass.
机译：通过脉冲对辐照技术研究了嵌入玻璃的纳米银的激光诱导的永久形状转变动力学，在该技术中，纳米粒子通过成对的延时飞秒激光脉冲辐照。表面等离激元消光带的时间演化可达到1 ns的时间延迟。我们发现，改性纳米颗粒的纵横比，即观察到的二色性，在激光辐照后的20 ps内迅速降低到最小水平。从该脉冲延迟开始，最终的宽高比将保持在最小水平，直到100 ps。随后，对于更长的时间延迟，长宽比再次增加直到1 ns。纳米粒子玻璃系统的温度模型表明，中间减少的二色性是由于高扩散迁移率所致，即发射的银离子可以在100 ps的时间窗口内在纳米粒子周围的加热玻璃壳中拥有。对于更长的时间延迟，加热的玻璃壳的尺寸减小，从而限制了离子扩散的范围。理论估计证实了实验结果，并表明纳米颗粒形状的变化很大程度上取决于周围玻璃的热态。

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