Local temperature pattern in plasmonic gold nanoshell: tuning the heat generation

Under quasi-steady-state conditions, we investigated the photo-heat conversion in a gold nanoshell by calculating the local equilibrium temperature distribution. In a thinner gold shell, the hot spots take place near the poles of both shell-surrounding and core-shell interface, perpendicularly to the incident field. In a thicker gold shell, the hot spots only take place near the core-shell interface. The maximum local temperature also depends greatly on the core media and shell thickness. Optimal heat generation can be obtained with small core dielectric constant and thin shell thickness. The mechanism of this local heating distribution is explained by the local field enhancement that is induced by the plasmon coupling.     

Internal reflection mode scanning near-field optical microscopy with the tetrahedral tip on metallic samples

An internal reflection mode is introduced for scanning near-field optical microscopy (SNOM) with the tetrahedral tip. A beam of light is coupled into the tip and the light specularly reflected out of the tip is detected as a photosignal for SNOM. An auxiliary STM mode is used to control the distance during the scanning process and to record the topography of the sample simultaneously with the SNOM image. Images were obtained of different metallic samples which show a contrast in the order of 10% of the total reflected photosignal. In images of metallic samples an inverted contrast is consistently obtained compared to images previously obtained of comparable samples in a transmission mode. The contrast shows a pronounced dependence on the polarization of the incident beam with respect to the orientation of the edges of the tip. In the case of gold surfaces, the photosignal as a function of distance between the tip and the surface shows a pronounced peak in the near-field range of 0–20 nm which is tentatively attributed to the excitation of surface plasmons on the gold surface. The pronounced near-field effects and the strong contrast in the near-field images and the resolution well below 50 nm are an indication of a highly efficient coupling of the incident beam to a local excitation of the tip apex which is essential for the function of the tip as a probe for SNOM. Received: 17 May 1999 / Accepted: 18 May 1999 / Published online: 21 October 1999     

Propagation and nanofocusing of infrared surface plasmons on tapered transmission lines: Influence of the substrate

We study the propagation of mid-infrared surface plasmons on non-tapered and tapered two-wire transmission lines on Si and CaF₂ substrates, the two materials representing substrates with large and small refractive index, respectively. A comparative numerical study predicts a larger effective wavelength and an increased propagation length (i.e. weaker damping) for the CaF₂ substrate. By near-field microscopy we image the near-field distribution along the transmission lines and experimentally verify surface plasmon propagation. Amplitude- and phase-resolved near-field images of a non-tapered transmission line on CaF₂ reveal a standing wave pattern caused by back-reflection of the surface plasmons at the open-ended transmission line. Calculated and experimental near-field images of tapered transmission lines on Si and CaF₂ demonstrate that for both substrates the mid-IR surface plasmons are compressed when propagating along the taper. Importantly, the nanofocus at the taper apex yields a stronger local field enhancement for the low-refractive index substrate CaF₂. We assign the more efficient nanofocusing on CaF₂ to the weaker damping of the surface plasmons.     

Plasmonic effects in near-field optical transmission enhancement through a single bowtie-shaped aperture

In this paper, the enhanced optical transmission through a special type of aperture of a bowtie shape is investigated through near-field imaging and finite-difference numerical analysis. Under linear polarizations in two orthogonal directions, the optical near fields of the bowtie aperture and comparable square and rectangular apertures made in gold and chromium thin films are measured and compared. The bowtie aperture is able to provide a nanometer-sized optical spot when the incident light is polarized across the bowtie gap and delivers a considerable amount of light. Localized surface plasmons are clearly observed in the near-field images for both bowtie and rectangular apertures in gold, but invisible in chromium. Finite-difference time-domain calculations reveal that, depending on the polarization of the incident light, the unique optical properties of the bowtie aperture are a result of either the optical waveguide and the coupled surface plasmon polariton modes existing in the bowtie gap or the coupling between the two open arms of the bowtie aperture. PACS 81.07.-b; 07.79.Fc; 71.36.+c; 78.66.Bz; 42.79.Gn; 42.79.Vb     

Optimization of near-field optical field of multi-layer dielectric gratings for pulse compressor

Multi-layer dielectric (MLD) gratings for pulse compressors in high-energy laser systems should provide high diffraction efficiency as well as high laser induced damage thresholds (LIDT). Nonuniform optical near-field distribution is one of the important factors to limit their damage resistant capabilities. Electric field distributions in the gratings and multi-layer film region are analyzed by using Fourier modal method. Optimization of peak electric field in the gratings ridge is performed with a merit function, including both diffraction efficiency and electric field enhancement when the top layer material is HfO₂ and SiO₂, respectively. A set of optimized gratings parameters is obtained for each structure, which reduce the peak electric field within the gratings ridge to being respective 1.39 and 1.84 times the value of incident light respectively. Finally, we also discuss the effects of gratings refractive index, gratings sidewall angle and incident angle on peak electric field in the gratings ridge.     

Simulated Output Images of Near-Field Optics by Volume Integral Equation: Object Placed on the Dielectric Substrate

We investigated near-field optical (NFO) imaging characteristics of a small object placed on a dielectric slab by a computer-code using a three-dimensional volume integral equation with an effective iteration technique called the generalized minimal residual method. A simplified three-dimensional NFO microscope that consists of a small dielectric object placed on the dielectric substrate and a small dielectric sphere as a scanning probe-tip was considered. Calculating two-dimensional output images obtained from scattered far fields, we studied the effect of the substrate on NFO output images, the comparison of NFO output images with electrostatic field around the small object, the dependence of output image characteristics on the wavelength and the difference of imaging characteristics between incident plane waves and incident evanescent waves.     

Single-metal-cluster local imaging: polarized scattered electric field calculation compared to the field’s modulus and phase observed in the optical near-field

Simultaneous topographical and near-field optical imaging have been performed on single gold particles of diameters close to 12 nm. The optical source is a linearly polarized laser diode operating at λ=780 nm away from the plasmon resonance of the particles. The experimental optical image is recorded with an apertureless scanning near-field optical microscope (ASNOM) operating in transmission mode. It is compared to the components of the polarized scattered electric field around a single cluster calculated using Mie formalism. We show that the tip used in the experiments is sensitive to the axial component of the scattered field, thus allowing us to obtain the amplitude and the phase of the local field. Our derivation brings out new information, usually shaded when applied to an ensemble of particles. In particular, the dipole model widely used to describe the scattered field by a spherical particle is not suitable to describe the three components of the scattered field in the near zone. Our results are of interest for fundamental studies of the optical properties of single metal clusters and the control of local phenomena such as enhancement, extinction, etc. PACS 07.79.Fc; 78.67.Bf; 78.35.+c     

Imaging contrast under aperture tip–nanoantenna array interaction

Periodic arrays of paired and single gold nanorods were imaged in the near field using reflection and transmission modes of a near-field scanning optical microscope at various wavelengths and polarizations of light in the visible range. The paired nanorods act like nanoantenna, and an array of them was initially designed as a negative-index material for the near infrared. Reverse contrast in reflection and transmission images is observed under illumination from the small aperture of a metal-coated fiber probe. By changing the relative orientation of the rods to the polarization, the reverse contrast switches to the normal contrast of near-field imaging. Coupling between the aperture and the nanorod array makes the contrast higher. Transmission through the aperture is enhanced if the aperture probe is positioned between the nanorods. The average near-field transmission exhibits an opposite sign of anisotropy relative to the far-field case. Aperture probes with larger diameters always show normal imaging contrast. The results demonstrate that the broad angular spectra of small-aperture sources play a crucial role in near-field interactions with nanorod arrays. The results also show that angular redistributions of these spectra after transmission or reflection from the nanorod array are likely due to excitation of localized and propagating plasmons.     

Near-field imaging of pyramid-like nanoparticles at a surface

An exact analytical solution of the self-consistent equation for the local field is used to calculate the near-field optical images of pyramid-like nano-objects placed at a surface of a solid. The diagram method developed previously for near-field image formation is generalized in order to describe layered objects, which are treated as many-body systems. The near-field optical images of triangular and square pyramids are calculated for the illumination configuration as well as those of triangular and square prisms. It is found that the near-field images of nanoparticles having the dielectric constant close to that of the substrate change rapidly and in a complicated manner with the probe–sample distance.     

Tuning the polarization states of optical spots at the nanoscale on the Poincaré sphere using a plasmonic nanoantenna

It is shown that the polarization states of optical spots at the nanoscale can be manipulated to various points on the Poincaré sphere using a plasmonic nanoantenna. Linearly, circularly, and elliptically polarized near-field optical spots at the nanoscale are achieved with various polarization states on the Poincaré sphere using a plasmonic nanoantenna. A novel plasmonic nanoantenna is illuminated with diffraction-limited linearly polarized light. It is demonstrated that the plasmonic resonances of perpendicular and longitudinal components of the nanoantenna and the angle of incident polarization can be tuned to obtain optical spots beyond the diffraction limit with a desired polarization and handedness.     

Adaptive ultrafast nano-optics in a tight focus

We theoretically demonstrate the control of electromagnetic field properties on a sub-diffraction length scale, by polarization shaping of tightly focused femtosecond laser pulses. The field distribution in a tight focus is represented as a superposition of plane waves. The near-field of a model nanostructure is then obtained as a sum of the near-field distributions induced by the planar waves components. A self-consistent solution of Maxwell’s equations in the frequency domain yields the near-field distributions for planar wave illumination. Adaptive optimization of the incident polarization pulse shape using an evolutionary algorithm allows controlling of a number of observables, such as local nonlinear flux, simultaneous spatial and temporal control of the intensity evolution, and control of the local spectrum. The tight focusing reduces the controllability of the flux distribution in comparison to plane wave illumination. However, it is still possible to control the spatial and temporal field evolution for particular locations in the vicinity of the nanostructure. PACS 42.65.Re; 78.47.+p; 78.67.-n; 82.53.-k     

Dipole and quadrupole surface plasmon resonance contributions in formation of near-field images of a gold nanosphere

Multipolar plasmon optical excitations at spherical gold nanoparticles and their manifestations in the particle images formatted in the particle surface proximity are studied. The multipolar plasmon size characteristic: plasmon resonance frequencies and plasmon damping rates were obtained within rigorous size dependent modelling. The realistic, frequency dependent dielectric function of a metal was used. The distribution of light intensity and of electric field radial component at the flat square scanning plane scattered by a gold sphere of radius 95 nm was acquired. The images resulted from the spatial distribution of the full mean Poynting vector including near-field radial components of the scattered electromagnetic field. Monochromatic images at frequencies close to and equal to the plasmon dipole and quadrupole resonance frequencies are discussed. The changes in images and radial components of the scattered electromagnetic field distribution at the scanning plane moved away from the particle surface from near-field to far-field region are discussed.     

Chirality, defects, and disorder in gold clusters

Theoretical and experimental information on the shape and morphology of bare and passivated gold clusters is fundamental to predict and understand their electronic, optical, and other physical and chemical properties. An effective theoretical approach to determine the lowest-energy configuration (global minimum) and the structures of low energy isomers (local minima) of clusters is to combine genetic algorithms and many-body potentials (to perform global structural optimizations), and first-principles density functional theory (to confirm the stability and energy ordering of the local minima). The main trend emerging from structural optimizations of bare Au clusters in the size range of 12-212 atoms indicates that many topologically interesting low-symmetry, disordered structures exist with energy near or below the lowest-energy ordered isomer. For example, chiral structures have been obtained as the lowest-energy isomers of bare Au₂₈ and Au₅₅ clusters, whereas in the size-range of 75-212 atoms, defective Marks decahedral structures are nearly degenerate in energy with the ordered symmetrical isomers. For methylthiol-passivated gold nanoclusters [Au₂₈(SCH₃)₁₆ and Au₃₈(SCH₃)₂₄], density functional structural relaxations have shown that the ligands are not only playing the role of passivating molecules, but their effect is strong enough to distort the metal cluster structure. In this work, a theoretical approach to characterize and quantify chirality in clusters, based on the Hausdorff chirality measure, is described. After calculating the index of chirality in bare and passivated gold clusters, it is found that the thiol monolayer induces or increases the degree of chirality of the metallic core. We also report simulated high-resolution transmission electron microscopy (HRTEM) images which show that defects in decahedral gold nanoclusters, with size between 1-2 nm, can be detected using currently available experimental HRTEM techniques.     

阿基米德螺旋微纳结构中的表面等离激元聚焦

研究光在微纳结构中的分布与传播, 实现在纳米范围内操纵光子, 对于微型光学芯片的设计有着重要意义. 本文利用聚焦离子束刻蚀方法, 在基底为石英玻璃的150 nm厚金膜上刻制了不同参数的阿基米德螺旋微纳狭缝结构, 通过改变入射光波长、手性、及螺旋结构手性和螺距等方式, 在理论和实验上系统地研究了阿基米德螺旋微纳结构中的表面等离激元聚焦性质. 我们发现, 除了入射激光偏振态、螺旋结构手性之外, 结构螺距与表面等离激元波长的比值也可以用来控制结构表面电场分布, 进而在结构中心形成0阶、1阶乃至更高阶符合隐失贝塞尔函数的涡旋电场. 通过相位分析, 我们对涡旋电场的成因进行了解释. 并利用有限时域差分的模拟方法计算了不同螺距时, 结构中形成的电场及相应空间相位分布. 最后利用扫描近场光学显微镜, 观测结构中不同的光场分布, 在结构中心得到了亚波长的聚焦光斑及符合不同阶贝塞尔函数的涡旋形表面等离激元聚焦环.     

Resonantly enhanced transmission of light through subwavelength apertures with dielectric filling

Using both analytical and numerical methods to study transmission of light through dielectric-filled subwavelength apertures in a real metal, we have found that a propagating mode can in principle exist inside a waveguide of arbitrary small size if a particular relationship between the dielectric constants of the cladding and filling materials at the incident frequency is satisfied. Practical transmission through a subwavelength aperture of finite depth can be enhanced when the depth is such that Fabry-Pérot-like resonances are excited. For 810 nm light incident on a silicon-filled 50-nm-diameter aperture in a 200-nm-thick gold film, we found that a normalized near-field intensity ratio of 1.6 at the exit can be achieved. This resonantly enhanced transmission phenomenon may be advantageously applicable to near-field scanning optical microscopy and single-molecule spectroscopy.     

Femtosecond-laser nanofabrication onto silicon surface with near-field localization generated by plasmon polaritons in gold nanoparticles with oblique irradiation

Nanohole fabrication process with gold nanoparticles irradiated by femtosecond laser at different incident angles is investigated. Nanoparticles with diameter of 200 nm and laser irradiation with center wavelength of 800 nm are used in the present study. The analysis of the electromagnetic field distribution in the near-field zone of the particle is made by simulations based on finite-differential time domain (FDTD) method. It is shown that when gold nanoparticle is irradiated by laser pulse surface plasmon excitation can be induced, and associated with it, high-intensity near field is produced in a limited area around the particle. It is found that the change of the irradiation conditions by means of irradiation from various incident directions gives a possibility of laser nanoprocessing with tunable characteristics. Our results show that enhanced optical intensity is able to be induced on the substrate surface regardless of incident direction of the laser due to the image charge interaction with the substrate. Furthermore, the use of p-polarized laser irradiation at a certain angle gives a minimum of the spatial dimensions of the enhanced zone on the substrate which is about two times smaller than that obtained at normal incidence.     

Near-field observation of plasmon excitation and propagation on ordered elliptical hole arrays

We report a near-field study of the excitation and propagation of surface plasmon on ordered Ag elliptical hole arrays with a scattering-type scanning near-field optical microscope. Strong dipole-like local plasmon is identified at each individual hole from near-field optical intensity and phase images. The excitation of the local plasmon at the elliptical hole is found to follow polarization excitation constraint. The coherent superposition of these local plasmon waves to form an extended surface plasmon wave propagating to an adjacent hole array is observed directly. The near-field results are consistent with the results obtained from far-field extraordinary transmission measurements. PACS 42.25.Bs; 42.25.Hz; 42.25.Ja; 42.25.Kb; 07.79.Fc     

AunY(n＝1—9)掺杂团簇的结构和电子性质研究

采用相对论有效原子实势(RECP)近似和密度泛函(B3LYP)方法，选择LANL2DZ基组，优化得到了Au_nY(n＝1—9)二元掺杂团簇稳定的基态结构和电子性质.研究结果表明，掺杂Y原子的Au_nY(n＝1—9)团簇随n的变化，其电离势、电子亲合能和费米能级与Au_n(n＝2—9)一样具有“奇-偶”振荡效应；团簇离子的稳定性具有“幻数”现象，Au₂Y⁺和Au₆Y⁺比其他团簇离子更稳定，与质谱实验结果一致；同一团簇中，团簇最稳定的异构体(基态)是趋于Y原子有最大的邻近的Au原子数. 关键词： Au-Y团簇 密度泛函 平衡几何结构 电子性质     

Uniform plasmonic near-field nanopatterning by backward irradiation of femtosecond laser

We present localized optical field distribution properties in the vicinity of gold particles on a silicon substrate by backward and forward irradiation. It is technically difficult to fabricate nanostructures on the surface by a conventional forward laser incident to the substrate because gold nanoparticles easily aggregate to form double-layered particle arrays. We calculated enhanced optical field properties in order to pattern the substrate surface only with a template of the bottom-layered particle arrays in the case that the backward irradiation of a femtosecond laser is used in the system of aggregated double-layered gold nanoparticle arrays. With the backward irradiation, the optical field intensity in the substrate for the double-layered hexagonal arrays is found to be only 30% lower than the mono-layered system. Moreover, a near field cannot be generated with the forward irradiation. As a result, only the backward irradiation scheme is found to be effective for uniform surface nanopatterning at enhanced plasmonic near-field zones.     

Surface plasmon enhanced ultra-low threshold second harmonic generation in periodically poled whispering gallery resonator

The surface plasmon enhanced ultra-low threshold second harmonic generation is observed, designed and simulated in whispering gallery resonator made of MgO doped periodically poled LiNbO₃. Here the electric field associated with incident optical radiation of picowatt level is amplified to milliwatt level through surface plasmon resonance in Kretschmann geometry which is formed by a BK₇ prism plane, 29 nm thin gold layer and 20 nm thin GaAs layer. This enhanced electric field then coupled to a whispering gallery resonator, which facilitated the generation of second harmonic for an incident laser radiation of picowatt level. In this proposed configuration with an incident optical power of 94.6 pW, generated second harmonic through whispering gallery resonator is found to be 14.6 mW.