纳米尺度下的局域场增强研究进展

金属纳米颗粒的等离激元共振引起的局域场增强效应,对显微成像、光谱学、半导体器件、非线性光学等诸多领域都具有极大的应用潜力。尤其是在光学纳米材料领域,通过亚波长金属纳米颗粒与电介质的组合引起局域场增强效应,提高了纳米材料的光学性能,并促进纳米材料在光学领域的应用。本文主要综述几种常见纳米结构所产生的局域场增强效应及其应用,详细介绍并总结了金属纳米材料的不同结构参数与局域场增强的关系及局域场增强在非线性光学、光谱学、半导体器件等领域的应用。未来,随着对金属纳米材料的研究愈发深入,局域场增强的应用将更加广泛,这将对诸多领域的发展产生重要影响。     

椭圆截面金纳米管近场增强特性的研究

本文基于时域有限差分方法(finite difference time domain, FDTD)研究了入射光波长、入射光偏振方向、纳米管几何形状、 管壁厚度及内核和包埋介质的变化对椭圆截面金纳米管近场分布特征的影响. 研究发现, 入射光波长为纳米管等离激元共振波长时, 纳米管近场增强最大; 入射光偏振方向与椭圆长轴夹角的增加会导致管内的场强迅速增大; 椭圆管半短轴变大可以调节纳米管场强分布从两端高、中间低变化为均匀分布; 内核和包埋介质介电常数的增大均会使得纳米管内部及周围场强逐渐减弱.     

Effect of metallic nanoparticle sizes on the local field near their surface

We have used numerical calculations based on Mie theory to analyze the near field distribution patterns for 4–150 nm spherical silver nanoparticles (nanospheres). We have shown that as the nanoparticle sizes increase, the region where “hot spots” are concentrated is shifted to the forward hemisphere. We have observed a nonmonotonic dependence of the maximum attainable local field enhancement factor on the size of the silver nanospheres. We have determined a correlation between the optimal nanosphere size for the maximum attainable local field enhancement factor and the optical absorption efficiency factor. We have established a nonmonotonic dependence of the optimal size of the nanoparticles and the maximum attainable local field enhancement factor on the refractive index of the surrounding medium. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 75, No. 6, pp. 831–837, November–December, 2008.     

二维亚波长金属小孔阵列的透射光增强效应

对金属薄膜上的二维亚波长小孔阵列的光透射增强现象进行了数值模拟，结果显示不仅实际金属薄膜上的小孔阵列结构具有透射增强效应，理想导体薄膜的相同结构也具有透射增强效应，但没有实际金属薄膜的增强明显-通过分析指出，这种小孔阵列的光透射增强效应是一种复杂的波导耦合效应-与金属薄膜上的表面电流一样，表面等离激元波具有将入射光能量从金属表面向小孔转移的作用，但不是透射增强的本质原因- 关键词： 表面电流 共振耦合 透射增强 表面等离激元     

Numerical analysis of surface plasmon nanocavities formed inthickness-modulated metal－insulator－metal waveguides

The enhancement characteristics of the local field in the surface plasmon nanocavities are investigated numerically. The cavity is constructed by placing a defect structure in the thickness-modulated metal--insulator--metal waveguide Bragg gratings. The characteristic impedance based transfer matrix method is used to calculate the transmission spectra and the resonant wavelength of the cavities with various geometric parameters. The finite-difference time-domain method is used to obtain the field pattern of the resonant mode and validate the results of the transfer matrix method. The calculation and simulation results reveal the existence of resonant wavelength shift and intensity variation with structural parameters, such as the modulation period of the gratings, the length and the width of the defect structure. Both numerical analysis and theoretical interpretation on these phenomena are given in details.     

Enhanced photon emission by field emission resonances and local surface plasmon in tunneling junction

We investigated the photon emission spectra on Ag (111) surface excited by tunneling electrons using a low temperature scanning tunneling microscope in ultrahigh vacuum. Characteristic plasmon modes were illustrated as a function of the bias voltage. The one electron excitation process was revealed by the linear relationship between the luminescence intensity and the tunneling current. Luminescence enhancement is observed in the tunneling regime for the relatively high bias voltages, as well as at the field emission resonance with bias voltage increased up to 9 V. Presence of a silver (Ag) nanoparticle in the tunneling junction results in an abnormally strong photon emission at the high field emission resonances, which is explained by the further enhancement due to coupling between the localized surface plasmon and the vacuum. The results are of potential value for applications where ultimate enhancement of photon emission is desired.     

Plasmonic nanostructures for local field enhancement in the UV region

In this work we describe an ultraviolet subwavelength focusing in plasmonic nanostructures. A system which provides a 20–25 times local field enhancement at a wavelength of 350 nm is proposed. This system represents a metalized V-shaped groove in a surface of a dielectric medium. Subwavelength focusing is achieved by a plasmon wave propagation along the surface of metal film and by the transfer of electromagnetic field through the dielectric medium. The influence of system parameters on a local field enhancement is investigated. A simplified model that allows for determining the geometric parameters of an optimized resonator is proposed.     

Influence of polarization direction, incidence angle, and geometry on near-field enhancement in two-layered gold nanowires

The influences of polarization direction, incidence angle, and geometry on near-field enhancements in two-layered gold nanowires (TGNWs) have been investigated by using the vector wave function method. When the polarization direction is perpendicular to the incidence plane, the local field factor (LFF) in TGNW decreases first and then increases with the increase in the incidence angle. The minimum LFF is observed at an incidence angle of 41°. It is found that the increase in the dielectric constant of the inner core leads to a decrease in the LFF. With the increase in the inner core radius, the LFF in TGNW increases first and then decreases, and the maximum LFF is observed at an inner core radius of 27 nm. On the other hand, when the polarization direction is parallel to the incidence plane, the collective motions of the induced electrons are enhanced gradually with the decrease in the incidence angle, and hence the near-field enhancement is increased.     

Interplay between out-of-plane magnetic plasmon and lattice resonance for modified resonance lineshape and near-field enhancement in double nanoparticles array

Two-dimensional double nanoparticle （DNP） arrays are demonstrated theoretically, supporting the interaction between out-of-plane magnetic plasmons and in-plane lattice resonances, which can be achieved by tuning the nanoparticle height or the array period due to the height-dependent magnetic resonance and the periodicity-dependent lattice resonance. The interplay between the two plasmon modes can lead to a remarkable change in resonance lineshape and an improvement on magnetic field enhancement. Simultaneous electric field and magnetic field enhancement can be obtained in the gap region between neighboring particles at two resonance frequencies as the interplay occurs, which presents “open” cavities as electromagnetic field hot spots for potential applications on detection and sensing. The results not only offer an attractive way to tune the optical responses of plasmonic nanostructure, but also provide further insight into the plasmon interactions in periodic nanostructure or metamaterials comprising multiple elements.     

金纳米环双体尺寸和耦合效应对表面等离子体共振特性的影响

采用离散偶极子近似方法系统地研究了金纳米环双体的消光光谱及其电场分布. 计算结果表明, 金纳米环双体在耦合作用下的共振消光峰对应着不同振动模式, 改变金纳米环双体的排列方式、 间距和尺寸大小, 其表面等离子体共振消光峰发生红移或蓝移. 因此可以通过对金纳米环双体结构参数和排列方式的设定, 调节其表面等离子体共振消光峰的位置. 电场分布表明, 水平排列的金纳米环双体较单个金纳米环产生更强的局部表面增强电场. 适当的小间距, 较大的内外半径的金纳米环水平阵列更适合做表面增强拉曼散射的衬底, 在生物分子检测等领域具有潜在的应用.     

Fano-like resonance characteristics of asymmetric Fe_2O_3@Au core/shell nanorice dimer

A geometrical configuration of Fe2O3/Au core-shell nanorice dimer is proposed and its multipolar plasmon Fano- like resonance characteristics are theoretically investigated by generalizing the plasmon hybridization model of individual nanorice to the bright and dark modes of the nanorice dimer. Under the irradiation of polarization light, the extinction spectra of the nanorice dimer are numerically simulated by using the finite element method （FEM）. Our studies show that the Fano-like resonance of the nanorice dimer results in an asymmetric line shape of the Fano dip in the extinction spectrum which can be controlled by varying the structure parameters of the nanorice dimer. Meanwhile, there is a giant field enhancement at the gap between the two nanorices on account of the plasmonic coupling in the nanorice dimer. The aforementioned two characteristics of the nanorice dimer are useful for plasmon-induced transparency and localized surface plasmon resonance sensors.     

内嵌圆饼空心方形银纳米结构的光学性质

采用离散偶极子近似方法计算了内嵌圆饼空心方形银纳米结构的消光光谱以及其近场的电场强度分布,并进一步与空心方形纳米结构的消光光谱和表面电场做比较.结果表明,在耦合作用下内嵌圆饼空心方形银纳米结构不仅产生了新的共振模式,而且新的共振模式在传统表面增强拉曼散射的激发波长范围内,进而可以弥补由于实验上运用纳米切片法所制备的空心方形纳米结构尺寸较大导致其共振吸收峰在远红外波长范围的不足.此外,可以通过改变内嵌圆饼空心方形银纳米结构的形貌参数调节其表面等离子体共振峰的共振波长,以满足在表面增强拉曼散射、生物分子或化学分子探测上的应用.     

Design of a sector bowtie nano-rectenna for optical power and infrared detection

We designed a sector bowtie nanoantenna integrated with a rectifier (Au−TiO_x−Ti diode) for collecting infrared energy. The optical performance of the metallic bowtie nanoantenna was numerically investigated at infrared frequencies (5−30 μm) using three-dimensional frequency-domain electromagnetic field calculation software based on the finite element method. The simulation results indicate that the resonance wavelength and local field enhancement are greatly affected by the shape and size of the bowtie nanoantenna, as well as the relative permittivity and conductivity of the dielectric layer. The output current of the rectified nano-rectenna is substantially at nanoampere magnitude with an electric field intensity of 1 V/m. Moreover, the power conversion efficiency for devices with three different substrates illustrates that a substrate with a larger refractive index yields a higher efficiency and longer infrared response wavelength. Consequently, the optimized structure can provide theoretical support for the design of novel optical rectennas and fabrication of optoelectronic devices.     

Surface plasmon polaritons frequency-blue shift in low confinement factor excitation region

Surface plasmon polaritons' (SPPs') frequency blue shift is observed in finite-difference time-domain (FDTD) simulation of parallel electron excitation Au bulk structure. Comparing with cold dispersion of SPPs, an obvious frequency blue shift is obtained in low confinement region excitation simulation results. Then, according to SPPs' transverse attenuation characteristics, the excited frequency mode instead of cold dispersion corresponding frequency mode matches it. Thence, this excited mode is confirmed to be SPPs' mode. As is well known the lower the frequency, the smaller the confinement factor is and the lower the excitation efficiency, the wider the bandwidth of excited SPPs is. And considering the attenuation in whole structure, the excited surface field contains attenuation signal. In a low confinement factor region, the higher the SPPs' frequency, the higher the excitation efficiency is, while broadband frequency information obtained in attenuation signal provides high frequency information in stimulation signal. Thence, in the beam-wave interaction, as the signal oscillation time increases, the frequency of the oscillation field gradually increases. Thus, compared with cold dispersion, the frequency of excited SPP is blueshifted This hypothesis is verified by monitoring the time domain signal of excited field in low and high confinement factor regions and comparing them. Then, this frequency-blue shift is confirmed to have commonality of SPPs, which is independent of SPPs' material and structure. Finally, this frequency-blue shift is confirmed in an attenuated total reflection (ATR) experiment. Owing to frequency dependence of most of SPPs' devices, such as coherent enhancement radiation and enhancement transmission devices, the frequency-blue shift presented here is of great influence in the SPPs applications.     

Optical absorption tunability and local electric field distribution of gold-dielectric-silver three-layered cylindrical nanotube

The effects of inner nanowire radius, shell thickness, the dielectric functions of middle layer and surrounding medium on localized surface plasmon resonance (LSPR) of gold-dielectric-silver nanotube are studied based on the quasi-static approximation. Theoretical calculation results show that LSPR of gold-dielectric-silver nanotube and LSPR numbers can be well optimized by adjusting its geometrical parameters. The longer wavelength of $\left|\omega_{-}^{-}\right\rangle$ mode takes place a distinct red-shift with increasing the inner nanowire radius and the thickness of middle dielectric layer, while a blue-shift with increasing outer nanotube thickness. The physical mechanisms are explained based on the plasmon hybridization theory, induced charges and phase retardation. In addition, the effects of middle dielectric function and surrounding medium on LSPR, and the local electric field factor are also reported. Our study provides the potential applications of gold-dielectric-silver nanotube in biological tissues, sensor and related regions.     

亚波长金属光栅的光耦合增强效应及透射局域化的模拟研究

介质层上的亚波长金属光栅产生的表面等离子体（surface plasmons,SPs）可以极大地增强光栅下介质层内的透射光强.增强作用从500 nm延续到近红外区域.在波长610 nm附近有接近110%的增强,在波长700 nm及740 nm处也有180%左右的增强.而这个波长范围与薄膜太阳能电池的吸收谱很相近,因此这种结构有望大幅度提高薄膜太阳能电池及不同波长光探测器等光电转换器件的光耦合效率. 关键词： 表面等离子体 亚波长光栅 薄膜太阳能电池 透射增强     

基于光子晶体光纤交叉敏感分离的磁场温度传感研究

提出了一种基于定向耦合效应和表面等离子共振效应的交叉敏感分离的磁场温度传感结构.在光子晶体光纤的一个特定空气孔中填充磁流体,利用磁流体的磁光效应和定向耦合效应形成磁场传感通道;在垂直方向的另一空气孔的内壁镀金纳米薄膜并填充甲苯液体,利用甲苯的温敏效应和表面等离子共振效应形成温度传感通道.对应输出谱出现两个损耗峰,测量损耗峰位置可以间接测出磁场强度和温度变化.通过理论计算()和结构优化,在90—270 Oe1 Oe=10~3/(4π) A/m范围内,磁场强度的灵敏度最高可达1.16 nm/Oe;在25—60?C范围内,温度的灵敏度可达-9.07 nm/?C.虽然填充的两种液体的折射率都受环境温度的影响,但通过建立灵敏度系数矩阵,可以消除磁场强度与温度的交叉敏感,实现磁场温度双参量的高灵敏度检测.     

On the extinction multipole plasmons in gold nanorods

On the basis of the T-matrix formalism and numerical simulations, we derive an explicit rule for partial multipole contributions to the plasmon resonances of gold nanorods at a fixed or random orientation. The parity of a given spectral resonance number n coincides with the parity of their multipole contributions l, where l is equal to or greater than n, and the total resonance magnitude is determined by the lowest multipole contribution. We also investigate the dependence of multipole plasmons on the size, shape, and orientation of nanorods with respect to the polarized incident light. It is shown that the multipole resonance wavelengths as a function of the aspect ratio divided by the resonance number collapse onto one linear scaling curve. This scaling is explained by using the plasmon standing wave concept introduced by Schider et al. [Plasmon dispersion relation of Au and Ag nanowires. Phys Rev B 2003;68:155427].     

Tens of thousands‐fold upconversion luminescence enhancement induced by a single gold nanorod

Upconversion nanoparticles (UCNPs) have gained increasing attention for their wide applications in bioimaging, displays and photovoltaics. However, low efficiency has been an ongoing challenge for further developments. In this work, it is proposed that the ultrasmall size of UCNPs is essential for achieving large enhancement factors and experimentally demonstrated with 4‐nm UCNPs. A strategy of plasmonic dual resonance is proposed in which two distinct localized surface plasmon resonance (LSPR) peaks of gold nanorods (GNRs) were designed to perfectly match both the excitation and emission light wavelength of UCNPs. Combining the excitation enhancement and Purcell effect, a huge enhancement factor of tens of thousands‐fold is stochastically demonstrated for single UCNPs in solution. The largest overall enhancement region is close to the end of a GNR but not in its central part. The excitation enhancement (up to three orders of magnitude) and the emission enhancement (larger than one order of magnitude) induced by the Purcell effect are experimentally demonstrated separately. This study provides insight into how to achieve a very large upconversion enhancement factor with surface plasmons and will catalyze development of UCNPs’ extensive applications.

     

Enhanced photoluminescence of CdSe quantum dots by the coupling of Ag nanocube and Ag film

The coupling of local surface plasmon(LSP) of nanoparticle and surface plasmon(SP) mode produced by metal film can lead to the enhanced electromagnetic field, which has an important application in enhancing the fluorescence of quantum dots(QDs). Herein, the Ag nanocube and Ag film are used to enhance the fluorescence of CdSe QDs. The enhancement is found to relate to the sizes of the Ag nanocube and the thickness of the Ag film. Moreover, we also present the fluorescence enhancement caused by only SP. The result shows that the coupling between metal nanoparticles and metal film can realize larger field enhancement. Numerical simulation verifies that a nanocube can localize a strong electric field around its corner. All the results indicate that the fluorescence of QDs can be efficiently improved by optimizing the parameters of Ag film and Ag cubes.