Tao X, Dong Z C, Yang J L, Luo Y, Hou J G, Aizpurua J
Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China.
J Chem Phys. 2009 Feb 28;130(8):084706. doi: 10.1063/1.3080766.
We investigate theoretically the influence of a dielectric layer on light emission induced by a scanning tunneling microscope through a combined approach of classical electrodynamics and first-principles calculations. The modification of the junction geometry upon the insertion of a dielectric layer is treated first by using the density functional theory to calculate the effective potential along the surface normal and then by solving a one-dimensional Schrodinger equation to obtain the exact distance between the tip and the substrate for a given current and bias voltage. The modified external field with the inclusion of a dielectric layer is evaluated by using the Fresnel formula. The local-field enhancement factor and radiated power are calculated by the boundary element method for two typical systems, W-tip/C(60)/Au(111) and W-tip/Al(2)O(3)/NiAl(110). The calculated results indicate that the insertion of a dielectric layer tends to reduce the light emission intensity considerably but hardly changes the spectral profile with no substantial peak shifts with respect to the layer-free situation, in agreement with experimental observations. The suppression of the radiated power is mainly due to the increase in the tip-metal separation and the resultant reduction in the electromagnetic coupling between the tip and metal substrate.
我们通过经典电动力学和第一性原理计算相结合的方法,从理论上研究了介电层对扫描隧道显微镜诱导发光的影响。首先,利用密度泛函理论计算沿表面法线方向的有效势,处理插入介电层后结几何结构的变化,然后通过求解一维薛定谔方程,得到给定电流和偏置电压下针尖与衬底之间的精确距离。利用菲涅耳公式评估包含介电层的修正外场。采用边界元法计算了两个典型体系W针尖/C(60)/Au(111)和W针尖/Al(2)O(3)/NiAl(110)的局域场增强因子和辐射功率。计算结果表明,插入介电层往往会显著降低发光强度,但几乎不改变光谱轮廓,相对于无介电层的情况没有明显的峰位移动,这与实验观测结果一致。辐射功率的抑制主要是由于针尖与金属间距的增加以及针尖与金属衬底之间电磁耦合的相应减小。