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强飞秒激光脉冲激发的游离氯化钠纳米颗粒的尺寸依赖性离子发射不对称性。

Size-dependent ion emission asymmetry of free NaCl nanoparticles excited by intense femtosecond laser pulses.

作者信息

Antonsson E, Gerke F, Merkel L, Halfpap I, Langer B, Rühl E

机构信息

Physical Chemistry, Freie Universität Berlin, Arnimallee 22, D-14195 Berlin, Germany.

出版信息

Phys Chem Chem Phys. 2019 Jun 12;21(23):12130-12138. doi: 10.1039/c9cp00696f.

Abstract

We report on asymmetric ion emission of size-selected NaCl nanoparticles (d = 100-600 nm) ionized by intense femtosecond laser pulses (λ = 800 nm, peak intensity ∼1013 W cm-2). Velocity map imaging indicates that a higher ion yield is observed in the propagation direction of the laser pulses than in the opposite direction. This asymmetric ion emission is found to be size-dependent and increases with particle size. This pronounced size dependence is interpreted in terms of discrete dipole simulations of the internal electric field in the nanoparticles, which reveal that the internal field is enhanced in the forward propagation direction of the laser pulses, occurring for nanoparticles >100 nm. The ion emission asymmetry is further found to depend on the peak intensity of the laser radiation. Nanoparticles of 100 nm show a symmetric distribution of ion emission, while the ion emission for 600 nm particles is found to become increasingly symmetric as the peak intensity is increased. In addition to single pulse ionization experiments, we explore the angular distribution of ion emission of resonantly heated NaCl nanoparticles using a pump-probe setup. Here, ion emission is found to be more symmetric for resonantly heated nanoparticles than for single pulse excitation. These differences are explained by the absorption mechanism, where the probe pulse in a dual pulse experiment can be efficiently absorbed by plasmonic excitation for suitable delays between both laser pulses.

摘要

我们报道了通过强飞秒激光脉冲(λ = 800 nm,峰值强度 ∼10¹³ W cm⁻²)电离的尺寸选择的氯化钠纳米颗粒(d = 100 - 600 nm)的不对称离子发射。速度映射成像表明,在激光脉冲的传播方向上观察到的离子产率高于相反方向。发现这种不对称离子发射与尺寸有关,并随颗粒尺寸增加。这种明显的尺寸依赖性是根据纳米颗粒内部电场的离散偶极子模拟来解释的,该模拟表明,对于大于100 nm的纳米颗粒,内部场在激光脉冲的向前传播方向上增强。进一步发现离子发射不对称性取决于激光辐射的峰值强度。100 nm的纳米颗粒显示出离子发射的对称分布,而随着峰值强度增加,600 nm颗粒的离子发射变得越来越对称。除了单脉冲电离实验外,我们还使用泵浦 - 探测装置探索了共振加热的氯化钠纳米颗粒的离子发射角分布。在此,发现共振加热的纳米颗粒的离子发射比单脉冲激发更对称。这些差异通过吸收机制来解释,在双脉冲实验中,对于两个激光脉冲之间的合适延迟,探测脉冲可以通过等离子体激发被有效吸收。

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