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     

Plasmonic abilities of gold and silver spherical nanoantennas in terms of size dependent multipolar resonance frequencies and plasmon damping rates

Absorbing and emitting optical properties of a spherical plasmonic nanoantenna are described in terms of the size dependent resonance frequencies and damping rates of the multipolar surface plasmons (SP). We provide the plasmon size characteristics for gold and silver spherical particles up to the large size retardation regime where the plasmon radiative damping is significant. We underline the role of the radiation damping in comparison with the energy dissipation damping in formation of receiving and transmitting properties of a plasmonic particle. The size dependence of both: the multipolar SP resonance frequencies and corresponding damping rates can be a convenient tool in tailoring the characteristics of plasmonic nanoantennas for given application. Such characteristics enable to control an operation frequency of a plasmonic nanoantenna and to change the operation range from the spectrally broad to spectrally narrow and vice versa. It is also possible to switch between particle receiving (enhanced absorption) and emitting (enhanced scattering) abilities. Changing the polarization geometry of observation it is possible to effectively separate the dipole and the quadrupole plasmon radiation from all the non-plasmonic contributions to the scattered light.     

Local fields close to the surface of nanoparticles and aggregates of nanoparticles

A refined discussion of the near-field scattering of spherical nanoparticles and the electromagnetic fields close to the particle surface is given. New results for the dependence on the distance from the surface and the angular distribution of the scattered light in the near-field are given. It will be shown that the radial component of the electric field leads to striking differences in the phase functions in the near-field and the far-field. Exemplary computations are presented for Ag and Au particles with different size. In a second part the discussion is extended to assemblies of spherical Ag and Au nanoparticles. It will be shown that large near-fields at wavelengths commonly used in SERS experiments are obtained for aggregates. In the near-field scattering intensity “hot spots” mark regions between particles in the aggregate where the near-field is particularly high. Received: 4 May 2001 / Revised version: 20 July 2001 / Published online: 19 September 2001     

Anomalous light scattering by small particles

Light scattering by a small spherical particle with a low dissipation rate is discussed based upon the Mie theory. It is shown that if close to the plasmon (polariton) resonance frequencies the radiative damping prevails over dissipative losses, sharp giant resonances with very unusual properties may be observed. In particular, the resonance extinction cross section increases with an increase in the order of the resonance (dipole, quadrupole, etc.); the characteristic values of electric and magnetic near fields for the scattered light are singular in the particle size, while energy circulation in the near field is rather complicated, so that the Poynting vector field includes singular points whose number, types, and positions are very sensitive to fine changes in the incident light frequency. The results may provide new opportunities for a giant, controlled, highly frequency-sensitive enhancement and variation of electromagnetic field at nanoscales.     

Size characteristics of surface plasmons and their manifestation in scattering properties of metal particles

The change of the scattering properties of sodium, gold and silver spherical particles with size is discussed in the context of surface multipolar plasmon resonances. The presented surface plasmon size characteristics are abstracted from the quantity which is observed and deliver multipolar plasmon resonance frequencies and plasmon damping rates in the form of a continuous function of particle radius. The performed analysis of the plasmon dispersion relation is analogous to the problem of surface plasmon localized at a semi-infinite, flat metal/dielectric interface.Correlation between the multipolar plasmon resonance parameters, and the spectroscopic optical properties of conductive nanoparticles appearing as peaks in the measurable light intensities is analyzed. We discuss the fact, that such peaks arise from interference of all the electromagnetic fields contributing to the measured intensity, and not solely to the fields due to surface plasmon multipolar modes.We describe the results of light scattering experiment in orthogonal polarization geometries with use of spontaneously growing sodium droplets. The polarization geometry of the experiment allows for distinct separation of resonant contribution of dipole and quadrupole plasmon TM mode contributions to the measured intensities as a function of size.Predictions concerning size characteristics for dipole and quadrupole plasmons are compared with the results of light scattering experiments using spherical sodium droplets (our results) and gold and silver particles in suspension [other authors: Sönnichsen C, Franzl T, Wilk T, von Plessen G, Feldmann J. Plasmon resonances in large noble-metal clusters. New J Phys 2002; 4:93.1–8; Haiss W, Thanh NTK, Aveyard J, Fernig DG. Determination of size and concentration of gold nanoparticles from UV–vis spectra. Anal Chem 2007; 79:4215–21; Njoki PN, Lim I-IS, Mott D, Park H-Y, Khan B, Mishra S, et al. Size correlation of optical and spectroscopic properties for gold nanoparticles. J Phys Chem C 2007; 111:14664–9; Mock JJ, Barbic M, Smith DR, Schultz DA, Schultz S. Shape effects in plasmon resonance of individual colloidal silver nanoparticles. J Chem Phys 2002; 116:6755–9].     

Scattering from a slightly random, one-dimensional metal surface: 45° linearly polarized incidence, backscattering enhancement and degree of polarization

The scattering of an electromagnetic wave from a slightly random metal surface which supports the surface plasmon mode at optical frequencies is studied theoretically by means of a stochastic functional approach. In order to investigate the Stokes matrix or the state of polarizations, as well as the intensity of the scattered waves, the rough surface is assumed to be one dimensional, and is illuminated by a+45° linearly polarized plane electromagnetic (light) wave whose plane of incidence is perpendicular to the grooves of the surface. The stochastic wave fields are represented in terms of the Wiener-Hermite functionals, and the approximate solutions of the Wiener kernels are obtained for both TM- and TE-polarized components, from which the Stokes matrix elements can be determined. The dressed or perturbed plasmon mode in the presence of surface roughness is obtained by a mass operator involved in the solutions, and the enhanced backscattering closely related to the plasmon mode is studied in connection with the enhanced peak width and the mass operator for the dressed plasmon mode. The Stokes parameters and the degree of polarization are calculated numerically from various polarized components of the incoherent scattering distribution. To clarify the surface plasmon's association with the scattering characteristics, calculations are made for two kinds of random surfaces, a random surface with a centred Gaussian spectrum and a random grating with twin spectral peaks at the plasmon spatial frequency.     

Integral equation method in near-field optical microscopy of scattering

Based on the integral equation method, the boundary problem of classical optics of finding the strength of the electromagnetic field scattered by a probe positioned in the near zone of a plane surface is solved in the context of application in near-field optical microscopy of scattering. Only the dipole component of the scattered field was taken into account in the calculations. The obtained theoretical expressions were compared to the known experimental data on scanning the surface of SiC. Good agreement between the experimental and the theoretical results was obtained outside the region of the resonant interaction of the probe of a near-field microscope and the surface under study.     

柱状磁光颗粒的局域表面等离激元共振及尺寸效应

柱状磁光颗粒的局域表面等离激元共振为二维磁光光子晶体的手征性边缘模的生成提供了重要的机制. 但目前对此类颗粒的局域表面等离激元共振效应的研究局限于长波长近似下的结果, 且缺乏对发生共振时的远场与近场特征的深入了解. 本文从散射理论出发, 计算并分析了柱状磁光颗粒发生局域表面等离激元共振的条件与特殊的场特征, 并讨论了颗粒尺寸对共振峰的影响. 计算结果解释了实验中观察到的二维磁光光子晶体的共振带隙与在长波长近似下得到的局域表面等离激元共振频率的明显偏移, 并展示了颗粒在较大尺寸下形成的高阶共振峰, 这可能有助于利用共振效应在磁光光子晶体中实现多模的手征边缘态.     

Investigation of plasmonics resonance infrared bowtie metal antenna

An approximate resonance wavelength equation that varies with metal antenna structure size is developed to design a bowtie gold metal antenna working at near-infrared (IR) wavelength. Bowtie antenna structures with resonance wavelength of 1.06 μm, 1.55 μm and 10.6 μm are designed based on this equation. A finite-difference time domain (FDTD) algorithm with total field scattered field (TFSF) source simulation shows the resonance wavelength of the designed structures being precisely in agreement with the expected wavelengths from the equation. Planar integration of the metal bowtie antennas is discussed as well. Gold nanohole bowtie antenna arrays are fabricated and the near-field optical transmission properties of the nanohole array are investigated with a near-field scanning optical microscope (NSOM). Our experimental results verify the near-field optical transmission performance and further demonstrate that they are in agreement with the theoretical calculation results. The high enhancement efficiency and integration of the metal bowtie antennas open the possibility of a wide application in IR optoelectronics detection and imaging.     

Dual mode near-field scanning optical microscopy for near-field imaging of surface plasmon polariton

In this paper, we theoretically and experimentally demonstrate that metal coated apertured probes are efficient near-field probes on surfaces with high reflectivity for the scattering as well as for the collection mode near-field scanning optical microscopy (NSOM). We show that a blunt apertured metal coated tip is very effective in suppressing image dipoles which affect strongly the signals scattered from frequently used sharp metal tips or gold nanoparticle attached probes. By using a simultaneous collection and scattering mode (dual mode) NSOM we measure the near-field images of surface plasmon polariton (SPP) launched from a slit. The collection mode measures propagating SPP along lateral distance in a long scan range with high signal-to-noise ratio, and the scattering mode measures the polarization resolved near-field of SPP. Comparisons of the measured data obtained in the dual mode enable to easily characterize SPP and to separate the measured near-field into the propagating SPP and the directly transmitted light.     

Role of confined Bloch waves in the near field heat transfer between two photonic crystals

The near field heat transfer between two finite size one-dimensional photonic crystals separated by a small vacuum gap and maintained in nonequilibrium thermal situation is theoretically investigated. The main features of this electromagnetic transfer are discussed and compared with what is generally observed with media that support surface polaritons. It is shown that the presence of surface Bloch waves can significantly enhance heat transfers beyond the far field limit for both polarization states of electromagnetic field at subwavelength separation distances. A specific attention is addressed to the consequence of the slopes of surface Bloch waves dispersion curves on the heat transfer. In particular, it is shown that the localization of surface Bloch waves close to the light line allows to observe a transfer exaltaion at larger separation distances than the Wien wavelength. These results could open new possibilities for the development of innovative near-field technologies such as near-field thermophotovoltaic conversion, plasmon assisted nanophotolitography or near-field spectroscopy.     

Near-field spectroscopy of surface plasmons in flat gold nanoparticles

We use near-field interference spectroscopy with a broadband femtosecond, white-light probe to study local surface plasmon resonances in flat gold nanoparticles (FGNPs). Depending on nanoparticle dimensions, local near-field extinction spectra exhibit none, one, or two resonances in the range of visible wavelengths (1.6-2.6 eV). The measured spectra can be accurately described in terms of interference between the field emitted by the probe aperture and the field reradiated by driven FGNP surface plasmon oscillations. The measured resonances are in good agreement with those predicted by calculations using discrete dipole approximation. We observe that the amplitudes of these resonances are dependent upon the spatial position of the near-field probe, which indicates the possibility of spatially selective excitation of specific plasmon modes.     

Three-dimensional analysis of silver nano-particles doping effects on super resolution near-field structure

The super resolution near-field structure which incorporates a AgOx thin film was studied through the calculation using three-dimensional (3D) finite-difference time-domain method. The influences of the optical field distribution generate by some factors, e.g., the polarization direction, the wavelength of incident light and the size of silver nano-particles, which are sensitive to the surface plasmon resonance are discussed in detail. The goal of this study is to explain the physical mechanisms responsible for the super-resolution near-field structure phenomena in 3D model and give a better understanding of the optical properties between AgOx layer and incident light.     

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.     

Propagation oscillations in the near-field response of traveling surface waves launched by metallic nanoapertures

We discuss the implications of a frequency-dependent complex dielectric function ε(ω) of a metal for the interpretation of scanning near-field optical microscopy (SNOM) measurements in the vicinity of metallic nanoapertures. For subwavelength slits in gold films we observe distinct spatial intensity oscillations in the near-field signal for specific wavelengths in the visible spectrum. These oscillations of the SNOM signal far away from the nanoslit are ascribed to a constructive interference between the propagating surface plasmon (SP) with light scattered parallel to the gold–air interface. In these spatial SNOM-signal oscillations information about the surface plasmon dielectric function is encoded which can be extracted, for example, in surface plasmon interferometry for applications as sensors or waveguides.     

扫描近场光学显微镜的光耦合偶极子模型

为了研究扫描近场光学显微镜中探针和粗糙样品表面的耦合相互作用,提出了一种光耦合偶极子模型.在该模型中,探针和样品突起都由光极化偶极子表示,在准静态电磁场近似的情况下样品表面的诱导极化效应由影像偶极子表示,应用偶极子辐射理论可以得到系统的自洽场方程.此模型提供了一种直观分析扫描近场光学显微镜中探针和样品相互作用机理的方法.在此基础上,进一步讨论了金属样品的近场成像特点和其特有的局域光学共振现象.数值结果表明：不同于一般的介质样品,金属样品的近场图像与入射光频率直接相关,改变入射光的频率,获得的样品近场图像的形状和对比度都会发生变化.特别是当入射光频率处于样品极化共振范围内时,金属纳米粒子的极化率会出现光极化共振,这样就可以获得样品粒子的最大有效尺寸,为提高系统的分辨率提供了一条重要途径.     

Near-field and far-field modeling of scattered surface waves. Application to the apertureless scanning near-field optical microscopy

The detection of surface waves through scanning near-field optical microscopy (SNOM) is a promising technique for thermal measurements at very small scales. Recent studies have shown that electromagnetic waves, in the vicinity of a scattering structure such as an atomic force microscopy (AFM) tip, can be scattered from near to far-field and thus detected. In the present work, a model based on the finite difference time domain (FDTD) method and the near-field to far-field (NFTFF) transformation for electromagnetic waves propagation is presented. This model has been validated by studying the electromagnetic field of a dipole in vacuum and close to a dielectric substrate. Then simulations for a tetrahedral tip close to an interface are presented and discussed.     

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     

Phase singularity of surface plasmon polaritons generated by optical vortices

We demonstrate an experimental result that shows the phase singularity of surface plasmon waves generated by the direct transform of optical vortices at normal incidence focused on a structureless metal surface. The near-field two-dimensional intensity distribution near the focal plane is experimentally examined by using near-field scanning optical microscopy and shows a good agreement with the finite-difference time-domain simulation result. The experimental realization demonstrates a potential of the proposed excitation scheme to be reconfigured locally with advantages over structures milled into optically thick metallic films for plasmonics applications involving plasmonic vortices.     

Apertureless near-field laser nanotechnology

We consider apertureless near-field optics that provides subwavelength resolution. We study the enhancement of the electromagnetic field near nanospheres and under the tip of a scanning probe microscope using the finite difference time-domain (FDTD) method. We discuss the mechanisms of field enhancement connected with the system geometry (“lightning rod effect”) and resonance excitation of local plasmon eigenmodes for different materials of the tip and various geometrical parameters of the system. We describe the possible applications in nano-optics and nanotechnology. We present the experimental achievements in apertureless near-field nanolithography.