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.     

Optically addressable selective nanovolume Raman spectroscopy of nanoparticles

We present recent experimental and theoretical advances in the selective nanovolume Raman spectroscopy of nanoparticles. Our setup is based on previously available microspectrometry imaging systems for working in the near-field domain combined with a stigmatic solid immersion lens. By spectrally selecting nanoparticles, we registered the spatial distribution of the emitted photons in x, y, z vectors to determine the position in the near-field domain. This near-field capability is applied to resolve local variations unambiguously in the Raman spectra for nanoparticles with unity throughput.     

Deterministic subwavelength control of light confinement in nanostructures

We propose a novel deterministic protocol, based on continuous light flows, that enables us to control the concentration of light in generic plasmonic nanostructures. Based on an exact inversion of the response tensor of the nanosystem, the so-called deterministic optical inversion protocol provides a physical solution for the incident field leading to a desired near-field pattern, expressed in the form of a coherent superposition of high-order beams. We demonstrate the high degree of control achieved on complex plasmonic architectures and quantify its efficiency and accuracy.     

A polarizing situation: Taking an in-plane perspective for next-generation near-field studies

By enabling the probing of light–matter interactions at the functionally relevant length scales of most materials, near-field optical imaging and spectroscopy accesses information that is unobtainable with other methods. The advent of apertureless techniques, which exploit the ultralocalized and enhanced near-fields created by sharp metallic tips or plasmonic nanoparticles, has resulted in rapid adoption of near-field approaches for studying novel materials and phenomena, with spatial resolution approaching sub-molecular levels. However, these approaches are generally limited by the dominant out-of-plane polarization response of apertureless tips, restricting the exploration and discovery of many material properties. This has led to recent design and fabrication breakthroughs in near-field tips engineered specifically for enhancing in-plane interactions with near-field light components. This mini-review provides a perspective on recent progress and emerging directions aimed at utilizing and controlling in-plane optical polarization, highlighting key application spaces where in-plane near-field tip responses have enabled recent advancements in the understanding and development of new nanostructured materials and devices.     

纳米颗粒近场空间光谱散射建模与显微成像分析

用非直观偏振参数显微成像,即采用在传统显微光路中插入模式化装置,通过拟合过滤后对所得数据反演成像,通过对金属纳米颗粒在近场空间散射光谱分析,来解决空间散射现象。用非直观偏振参数显微成像与传统直观成像做对比,并通过时域有限差分法建模仿真,来描述近场直观与非直观散射光谱的差异,对比结果发现,非直观偏振参数显微反演成像的分辨率比直观成像更高,不但能够清晰的探测到纳米颗粒的形状和电场分布,而且比直观成像获得更广泛的空间散射光谱。     

Signature of a Fano resonance in a plasmonic metamolecule's local density of optical states

We present measurements on plasmonic metamolecules under local excitation using cathodoluminescence which show a spatial redistribution of the local density of optical states at the same frequency where a sharp spectral Fano feature in extinction has been observed. Our analytical model shows that both near- and far-field effects arise due to interference of the same two eigenmodes of the system. We present quantitative insights both in a bare state, and in a dressed state picture that describe Fano interference either as near-field amplitude transfer between coupled bare states, or as interference of uncoupled eigenmodes in the far field. We identify the same eigenmode causing a dip in extinction to strongly enhance the radiative local density of optical states, making it a promising candidate for spontaneous emission control.     

Broadband near-field interference spectroscopy of metal nanoparticles using a femtosecond white-light continuum

We demonstrate a new nanoscale spectroscopic technique that combines subwavelength near-field imaging with broadband interference spectroscopy. We apply this technique to study phase spectra of surface plasmons in individual gold nanoparticles and nanoparticle dimers. Collective plasmon oscillations in selected nanostructures are excited by a femtosecond white-light continuum transmitted through a subwavelength aperture. The interference spectra detected in the far field result from the coherent superposition of the aperture field and the secondary field re-emitted by the nanostructure. The analysis of these spectra allows us to accurately measure the positions and damping constants of single-nanostructure plasmon resonances.     

Diamond nanoparticles as photoluminescent nanoprobes for biology and near-field optics

We present results showing the potential of diamond nanoparticles with size <50 nm as photoluminescent nanoprobes for serving as stable point-like emitters attached at the tip apex of a near-field optical microscope to achieve enhanced spatial resolution.     

A virtual optical probe based on evanescent wave interference

A virtual probe is a novel immaterial tip based on the near-field evanescent wave interference and small aperture diffraction, which can be used in near-field high-density optical data storage, nano-lithography, near-field optical imaging and spectral detection, near-field optical manipulation of nano-scale specimen, etc. In this paper, the formation mechanism of the virtual probe is analysed, the evanescent wave interference discussed theoretically, and the sidelobe suppression by small aperture is simulated by the three-dimensional finite-difference time-domain method. The simulation results of the optical distribution of the near-field virtual probe reveal that the transmission efficiency of the virtual probe is 10²－10⁴ times higher than that of the nano-aperture metal-coated fibre probe widely used in near-field optical systems. The full width at half maximum of the peak, in other words, the size of virtual probe, is constant whatever the distance in a certain range so that the critical nano-separation control in the near-field system can be relaxed. We give an example of the application of the virtual probe in ultrahigh-density optical data storage.     

Imaging Ultrafast Plasmon Dynamics within a Complex Dolmen Nanostructure Using Photoemission Electron Microscopy

We report direct nanoscale imaging of ultrafast plasmon in a gold dolmen nanostructure excited with the 7fs laser pulses by combining the interferometric time-resolved technology with the three-photon photoemission electron microscopy(PEEM).The interferometric time-resolved traces show that the plasmon mode beating pattern appears at the ends of the dimer slabs in the dolmen nanostructure as a result of coherent superposition of multiple localized surface plasmon modes induced by broad bandwidth of the ultrafast laser pulses.The PEEM measurement further discloses that in-phase of the oscillation field of two neighbor defects are surprisingly observed,which is attributed to the plasmon coupling between them.Furthermore,the control of the temporal delay between the pump and probe laser pluses could be utilized for manipulation of the near-field distribution.These findings deepen our understanding of ultrafast plasmon dynamics in a complex nanosystem.     

双色场驱动下高次谐波的径向量子轨道干涉

研究了双色场驱动下的高次谐波量子轨道的相位匹配特性. 通过调整激光束腰优化双色场空间分布, 可以有效地增加长轨道的径向相位匹配区域, 使得长轨道和短轨道在近轴处和离轴处都同时相位匹配.通过选取合适的近场空间过滤片, 可以获得清晰的径向干涉条纹. 这些结果在分辨不同的干涉现象以及更高精度的观察高阶轨道方面有很大的潜在应用价值. 关键词： 高次谐波 量子轨道 干涉     

纳米结构金属表面的近场电势分布

基于均匀外电场中金属纳米半球颗粒按一定对称性从平面衬底生长出的表面结构,建立纳米半球颗粒表面附近近场电势的理论模型.采用数值计算方法得到近场电势的空间分布,并以三维曲面的形式给出.结果表明:电势分布呈现明显的几何对称性.结果为解释与纳米结构薄膜表面有关的各种异常现象提供依据,为纳米结构薄膜材料的应用研究提供参考.     

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.     

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     

Evaluation of influence of anisotropic diffusion near a wall in near-field fluorescence correlation spectroscopy of nanoparticles

Fluorescence correlation spectroscopy (FCS) of colloidal nanoparticles using a near-field fiber probe was numerically simulated. The near-wall dynamics was simulated by accounting for the anisotropic mobility of nanoparticles owing to hydrodynamic interaction with a wall (Stokes viscous force). By comparing the simulation results with theoretical model calculations, we found that the influence of anisotropic diffusion is insignificant in near-field FCS autocorrelation analysis.     

Interference structure of the field of infrasonic directed sources in shallow water

The effect of the beam pattern of sources on the spatial interference structure of the infrasonic field in shallow water has been studied numerically. Calculations have been performed for a monopole and differently oriented dipoles and quadrupoles in the near-field zone, where the modes have not yet formed, as well as in the far-field zone, where the mode interference is observed. Dependence of the interference patterns at different frequencies on the emission and reception horizons, the multipole type, and the wave distance has been demonstrated. The importance of taking into account the horizontal beam pattern of sources in the far-field zone has been shown.     

Spectral features of electromagnetic field propagation along a nanoparticle chain

Numerical calculations are performed and spectral characteristics and spatial field distributions are studied upon excitation of a chain of two and three nanoparticles by a near-field optical microscope probe. It was found that there is a set of frequencies near the absorption line of nanoparticle material, at which the electromagnetic field can most efficiently propagate along the chain. It is shown that the efficiency of the electromagnetic energy transfer due to the quadrupole interaction between particles can exceed the efficiency of the transfer caused by the dipole interaction.     

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.     

Comments on the picosecond pulse width measurement by the single-shot second harmonic beam technique

We show that the measurement of the ultrashort light pulse duration by the single-shot second harmonic beam technique requires caution. It is found that the far-field distribution of the second harmonic radiation from non bandwidth-limited pulses shows a pronounced structure even if the near-field pattern is without structure. This interference effect is interpreted as being due to the special symmetry properties of the spatial coherence of the second harmonic beam. A simple method for a quick determination of the existence of the bandwidth-limited relation in an individual picosecond light pulse is proposed.     

Infrared imaging of single nanoparticles via strong field enhancement in a scanning nanogap

We demonstrate nanoscale resolved infrared imaging of single nanoparticles employing near-field coupling in the nanoscopic gap between the metal tip of a scattering-type near-field optical microscope and the substrate supporting the particles. Experimental and theoretical evidence is provided that highly reflecting or polariton-resonant substrates strongly enhance the near-field optical particle contrast. Using Si substrates we succeeded in detecting Au particles as small as 8 nm (相似文献