Effect of spatially nonlocal versus local optical response of a gold nanorod on modification of the spontaneous emission

The spontaneous emission rate of a two-level quantum emitter(QE)near a gold nanorod is numerically investigated.Three different optical response models for the free-electron gas are adopted,including the classical Drude local response approximation,the nonlocal hydrodynamic model,and the generalized nonlocal optical response model.Nonlocal optical response leads to a blueshift and a reduction in the enhancement of the spontaneous emission rate.Within all the three models,the resonance frequency is largely determined by the aspect ratio(the ratio of the nanorod length to the radius)and increases sharply with decreasing aspect ratio.For nanorod with a fixed length,it is found that the larger the radius is,the higher the resonance frequency is,and the smaller the enhancement is.However,if the length of the nanorod increases,the peak frequency falls sharply,while the spontaneous emission enhancement grows rapidly.For nanorod with a fixed aspect ratio,the peak frequency decreases slowly with increasing nanorod size.Larger nanorod shows smaller nonlocal effect.At a certain frequency,there is an optimal size to maximize the enhancement of the spontaneous emission rate.Higher order modes are more affected by the nonlocal smearing of the induced charges,leading to larger blueshift and greater reduction in the enhancement.These results should be significant for investigating the spontaneous emission rate of a QE around a gold nanorod.     

基于有限元法的光子并矢格林函数重整化及其在自发辐射率和能级移动研究中的应用

任意微纳结构中量子点的自发辐射率和能级移动均可用并矢格林函数表达.当源点和场点在同一位置时,格林函数的实部是发散的.为解决这一发散问题,可采用重整化格林函数方法.本文提出一种计算重整化格林函数和散射格林函数的方法.该方法利用有限元,计算点电偶极子的辐射场,将其在量子点体积内做平均得到重整化的并矢格林函数,减去均匀空间中解析的重整化格林函数,得到重整化的散射格林函数.在均匀空间情况下,本方法所得数值结果与解析解一致.将该方法应用到银纳米球系统,以解析的散射格林函数作为参考,结果表明该方法能准确处理散射格林函数的重整化问题.将该方法应用到表面等离激元纳米腔中,发现有极大的自发辐射增强和能级移动,且该结果不依赖于量子点的体积.这些研究在光与物质相互作用领域具有积极的意义.