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Impact of Plasmon-Induced Atoms Migration in Harmonic Generation
ACS Photonics ( IF 6.5 ) Pub Date : 2018-02-08 00:00:00 , DOI: 10.1021/acsphotonics.7b01560 Liping Shi 1, 2 , Rana Nicolas 3 , Jose R. C. Andrade 1 , Willem Boutu 3 , Dominik Franz 3 , Torsten Heidenblut 4 , Carsten Reinhardt 5 , Uwe Morgner 1, 2 , Hamed Merdji 3 , Milutin Kovacev 1, 2
ACS Photonics ( IF 6.5 ) Pub Date : 2018-02-08 00:00:00 , DOI: 10.1021/acsphotonics.7b01560 Liping Shi 1, 2 , Rana Nicolas 3 , Jose R. C. Andrade 1 , Willem Boutu 3 , Dominik Franz 3 , Torsten Heidenblut 4 , Carsten Reinhardt 5 , Uwe Morgner 1, 2 , Hamed Merdji 3 , Milutin Kovacev 1, 2
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Under illumination of a Ti:sapphire femtosecond oscillator, amplification of third harmonic generation by subwavelength plasmonic apertures is observed. However, the harmonic yield efficiency decays rapidly over time. In this work we investigate the physical phenomena behind the temporal attenuation of the harmonic signal. From high-resolution scanning electron micrographs and two-dimensional energy dispersive X-ray maps, we conclude that the attenuation of the third harmonic is attributed to trapping of a low-density carbon layer inside the plasmonic apertures. Furthermore, we show that the profile of the carbon deposit follows the enhanced electric near-field distribution, which indicates that the carbon atoms are transported to the field hotspot by the plasmonically enhanced optical tweezer effect. From the measurement of linear transmission spectra, we find that the dielectric constant inside the nanoholes is increased by the carbon deposit. However, numerical simulations demonstrate that the increase of dielectric constant does not reduce the electric near-field enhancement factor. Therefore, the decay of third harmonic radiation is primarily due to the strong reabsorption by the carbon deposit inside the gold-free aperture.
中文翻译：
等离子体诱导的原子迁移对谐波产生的影响
在Ti：蓝宝石飞秒振荡器的照射下，观察到亚波长等离激元孔径放大了三次谐波。但是，谐波屈服效率会随时间迅速衰减。在这项工作中，我们研究了谐波信号的时间衰减背后的物理现象。从高分辨率扫描电子显微照片和二维能量色散X射线图，我们得出结论，三次谐波的衰减归因于在等离子体孔内捕获的低密度碳层。此外，我们表明碳沉积物的轮廓遵循增强的电近场分布，这表明碳原子通过等离子体增强的光镊效应被运输到了现场热点。通过线性透射光谱的测量，我们发现纳米孔内部的介电常数因碳沉积而增加。但是，数值模拟表明介电常数的增加不会降低电近场增强因子。因此，三次谐波辐射的衰减主要归因于无金孔内碳沉积物的强烈再吸收。
更新日期：2018-02-08
中文翻译：
等离子体诱导的原子迁移对谐波产生的影响
在Ti：蓝宝石飞秒振荡器的照射下，观察到亚波长等离激元孔径放大了三次谐波。但是，谐波屈服效率会随时间迅速衰减。在这项工作中，我们研究了谐波信号的时间衰减背后的物理现象。从高分辨率扫描电子显微照片和二维能量色散X射线图，我们得出结论，三次谐波的衰减归因于在等离子体孔内捕获的低密度碳层。此外，我们表明碳沉积物的轮廓遵循增强的电近场分布，这表明碳原子通过等离子体增强的光镊效应被运输到了现场热点。通过线性透射光谱的测量，我们发现纳米孔内部的介电常数因碳沉积而增加。但是，数值模拟表明介电常数的增加不会降低电近场增强因子。因此，三次谐波辐射的衰减主要归因于无金孔内碳沉积物的强烈再吸收。
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