Drobnyh Elena, Sukharev Maxim
Department of Physics, Arizona State University, Tempe, Arizona 85287, USA.
J Chem Phys. 2020 Mar 7;152(9):094706. doi: 10.1063/1.5143238.
Optical properties of periodic arrays of nanoholes of a triangular shape with experimentally realizable parameters are examined in both linear and nonlinear regimes. By utilizing a fully vectorial three-dimensional approach based on the nonlinear hydrodynamic Drude model describing metal coupled to Maxwell's equations and Bloch equations for molecular emitters, we analyze linear transmission, reflection, and nonlinear power spectra. Rigorous numerical calculations demonstrating second and third harmonic generation by the triangular hole arrays are performed. It is shown that both the Coulomb interaction of conduction electrons and the convective term contribute on equal footing to the nonlinear response of metal. It is demonstrated that the energy conversion efficiency in the second harmonic process is the highest when the system is pumped at the localized surface plasmon resonance. When molecular emitters are placed on a surface of the hole array line shapes, the second harmonic signal exhibits three peaks corresponding to second harmonics of the localized surface plasmon mode and upper and lower polaritonic states.
研究了具有实验可实现参数的三角形纳米孔周期阵列在线性和非线性区域的光学性质。通过利用基于非线性流体动力学德鲁德模型的全矢量三维方法,该模型描述了与麦克斯韦方程组和分子发射体的布洛赫方程耦合的金属,我们分析了线性透射、反射和非线性功率谱。进行了严格的数值计算,证明了三角形孔阵列产生的二次和三次谐波。结果表明,传导电子的库仑相互作用和对流项对金属的非线性响应贡献相同。结果表明,当系统在局域表面等离子体共振处泵浦时,二次谐波过程中的能量转换效率最高。当分子发射体放置在孔阵列线形状的表面上时,二次谐波信号呈现出三个峰,分别对应于局域表面等离子体模式的二次谐波以及上、下极化子态。