论文标题

拉普拉斯级量子流体力学理论

Laplacian-Level Quantum Hydrodynamic Theory for Plasmonics

论文作者

Baghramyan, Henrikh M., Della Sala, Fabio, Ciracì, Cristian

论文摘要

对亚波长金属颗粒和纳米含量结构的光学响应的​​准确描述是血浆的关键问题。量子流体力学理论(QHT)已成为计算金属纳米颗粒(NP)的光学响应的​​强大方法,因为它考虑了非局部性和溢出效应。然而,通过常规QHT获得的金属NP的吸收光谱,即融合了Thomas-Fermi(TF)和VonWeizsäcker(vw)动能(KE)贡献,可以受到比本地级别表面等位基本(LSP)更高的能量的多种能量共振的影响。这些峰不存在于参考时间依赖性密度功能理论(TD-DFT)光谱中,相反,仅存在宽阔的肩膀。此外,我们在这里表明,这些峰错误地降低了LSP峰强度,并且对仿真域的大小具有很大的依赖性,以便对QHT吸收光谱进行正确计算可能是有问题的。在本文中,我们介绍了一种更通用的QHT方法,该方法根据电子密度的拉普拉斯(Laplacian)($ q $)介绍了KE的贡献,因此,超出了TFVW功能的仅梯度依赖性。我们表明,采用具有与$ q^2 $成比例的术语的KE功能可导致吸收光谱无伪峰,并具有正确强度和数值稳定的Bennett State的LSP共振。最后,我们提出了一种新颖的拉普拉斯级ke能量功能,该功能非常准确,可描述具有不同尺寸和二聚体的NP的光学性质。

An accurate description of the optical response of subwavelength metallic particles and nanogap structures is a key problem of plasmonics. Quantum hydrodynamic theory (QHT) has emerged as a powerful method to calculate the optical response of metallic nanoparticles (NPs) since it takes into account nonlocality and spill-out effects. Nevertheless, the absorption spectra of metallic NPs obtained with conventional QHT, i.e., incorporating Thomas-Fermi (TF) and von Weizsäcker (vW) kinetic energy (KE) contributions, can be affected by several spurious resonances at energies higher than the main localized surface plasmon (LSP). These peaks are not present in reference time-dependent density-functional-theory (TD-DFT) spectra, where, instead, only a broad shoulder exists. Moreover, we show here that these peaks incorrectly reduce the LSP peak intensity and have a strong dependence on the simulation domain size so that a proper calculation of QHT absorption spectra can be problematic. In this article, we introduce a more general QHT method accounting for KE contributions depending on the Laplacian of the electronic density ($q$), thus, beyond the gradient-only dependence of the TFvW functional. We show that employing a KE functional with a term proportional to $q^2$ results in an absorption spectrum free of spurious peaks, with LSP resonance of correct intensity and numerically stable Bennett state. Finally, we present a novel Laplacian-level KE energy functional that is very accurate for the description of the optical properties of NPs with different sizes as well as for dimers.

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