The Blackett Laboratory, Department of Physics, Imperial College London , London SW7 2AZ, United Kingdom.
ACS Nano. 2017 Jan 24;11(1):953-960. doi: 10.1021/acsnano.6b07568. Epub 2016 Dec 19.
Benefiting from large intrinsic nonlinearities, low absorption, and high field enhancement abilities, all-dielectric nanoantennas are considered essential for efficient nonlinear processes at subwavelength volumes. In particular, when the dielectric nanoantenna supports the nonradiating anapole mode, characterized by a minimum in the extinction cross section and a maximum electric energy within the material, third harmonic generation (THG) processes can be greatly enhanced. In this work, we demonstrate that a higher-order anapole mode in a 200 nm thick germanium nanodisk delivers the highest THG efficiency on the nanoscale at optical frequencies. By doubling the diameter of a disk supporting the fundamental anapole mode, we discover the emergence of an anapole mode of higher order, with a valley in the extinction cross section significantly narrower than that of the fundamental anapole. Under this condition, we observe a highly improved electric field confinement effect within the dielectric disk, leading to THG conversion efficiencies as large as 0.001% at a third harmonic wavelength of 550 nm. In addition, by mapping the THG emission across the nanodisk, we are able to unveil the anapole near-field intensity distributions, which show excellent agreement with numerical simulations. Our findings remarkably expand contemporary knowledge on localized modes in dielectric nanosystems, revealing crucial elements for the elaboration of highly efficient frequency upconversion nanodevices.
得益于大的固有非线性、低吸收和高场增强能力,全介质纳米天线被认为是在亚波长体积中实现高效非线性过程的关键。特别是,当介电纳米天线支持非辐射各向同体模式时,其特征是消光截面最小,材料内的电能最大,三阶谐波产生 (THG) 过程可以大大增强。在这项工作中,我们证明了在 200nm 厚的锗纳米盘中,更高阶的各向同体模式在光学频率下提供了纳米尺度上最高的 THG 效率。通过将支持基态各向同体模式的圆盘直径加倍,我们发现了高阶各向同体模式的出现,其消光截面的谷比基态各向同体模式的更窄。在这种情况下,我们观察到介电盘内的电场限制效应显著增强,导致在 550nm 的三次谐波波长处的 THG 转换效率高达 0.001%。此外,通过在纳米盘上绘制 THG 发射,我们能够揭示各向同体近场强度分布,其与数值模拟结果非常吻合。我们的发现显著扩展了关于介电纳米系统中局域模式的当代知识,揭示了高效频率上转换纳米器件的关键要素。