Nonlinear surface plasmon polaritonic crystals

We present an overview of the optical properties of nonlinear surface plasmon polaritonic crystals and their applications to control light with light. Surface plasmon polaritonic crystals are periodically nanostructured metal surfaces or thin metal films that act as two‐dimensional photonic crystals for surface polaritons. Hybritization of such nanostructures with dielectrics exhibiting an optical nonlinear response allows utilization of the electromagnetic field enhancement effects to observe nonlinear effects and bistable behaviour at low light intensities. By changing the geometry of the nanostructured film, the dispersion of the crystal is modified and, thus, electromagnetic mode structure and associated density of states can be controllably tuned in the desired spectral range. This provides enhanced flexibility in engineering the nonlinear optical response of plasmonic crystals in a chosen spectral range for both control and signal wavelengths.     

Design and synthesis of plasmonic magnetic nanoparticles

Core–shell nanoparticles containing both iron oxide and gold are proposed for bioseparation applications. The surface plasmon resonance of gold makes it possible to track the positions of individual particles, even when they are smaller than the optical diffraction limit. The synthesis of water-dispersible iron oxide-gold nanoparticles is described. Absorption spectra show the plasmon peaks for Au shells on silica particles, suggesting that thin shells may be sufficient to impart a strong surface plasmon resonance to iron oxide-gold nanoparticles. Dark field optical microscopy illustrates the feasibility of single-particle detection. Calculations of magnetophoretic and drag forces for particles of different sizes reveal design requirements for effective separation of these small particles.     

About the nature of increase of the nonlinear optical response of a rough surface

It is shown that during the propagation of surface plasmon polariton (SPP) in the system of two touching spheres (or cones) when one is a metal and the other is a semiconductor, the conditions of strong localization of the surface wave are realized. At the point of contact, an essential decrease of the wavelength of the SPP is observed and the diffraction processes do not hinder its localization on the nanometric scale. As a result, wave fields increase anomalously. The considered phenomena open a new possibility to propose the experimental way for exploring the gigantic enhancement of the nonlinear optical response from a rough surface.     

表面等离子激元非线性表面增强拉曼散射效应

本文采用热蒸发法制备得到纳米Ag颗粒作为增强拉曼衬底, 利用入射光子与纳米颗粒表面价电子的相互作用机理, 激发出高能表面等离子激元, 其表面等离子形成的高能"热点"起到表面增强拉曼散射效果. 通过比较不同入射光强下的拉曼峰强, 指出纳米Ag颗粒的增强拉曼散射效果可以实现低探测光强下的高散射强度, 即纳米Ag颗粒的表面等离子激元具有非线性的表面增强拉曼散射效果, 可降低对样品的光、热损伤, 以利于拓展拉曼散射光谱的应用范围. 同时比较不同纳米Ag颗粒衬底的表面增强拉曼散射效果表明, 采用的热蒸发工艺具有较大的工艺域度, 具有较强的工艺兼容性.     

Ultrafast nonlinear optical response of a single gold nanorod near its surface plasmon resonance

The ultrafast optical nonlinearity of an optically characterized single gold nanorod is investigated around its surface plasmon resonance, by combining a far-field spatial modulation technique with a high sensitivity pump-probe setup. The spectrally and temporally dependent response is quantitatively interpreted in terms of the bulklike optical nonlinearity enhanced by the plasmonic effect. The plasmon resonance dynamics is shown to be mostly governed by nonequilibrium electron and phonon processes. Their contributions to the nonlinear optical response of a single metal nano-object are elucidated, and the latter is connected to the nonlinearities of ensembles.     

Nonlinear excitation of surface plasmon polaritons by four-wave mixing

We demonstrate nonlinear excitation of surface plasmons on a gold film by optical four-wave mixing. Two excitation beams of frequencies omega(1) and omega(2) are used in a modified Kretschmann configuration to induce a nonlinear polarization at a frequency of omega(4wm)=2omega(1)-omega(2), which gives rise to surface plasmon excitation at a frequency of omega(4wm). We observe a characteristic plasmon dip at the Kretschmann angle and explain its origin in terms of destructive interference. Despite a nonvanishing bulk response, surface plasmon excitation by four-wave mixing is dominated by a nonlinear surface polarization. To interpret and validate our results, we provide a comparison with second-harmonic generation.     

Time-resolved nonlinear surface plasmon optics

A new surface-sensitive method of time-resolved optical studies is proposed. The method consists in the independent excitation of several surface electromagnetic waves (SEW) by two laser femtosecond pulse beams with varied time delay Δτ and distance Δr between corresponding excitation regions on the surface. To fulfill the phase-matching condition for plasmon-photon coupling, metal grating is used. Due to nonlinear plasmon interaction, the optical radiation with ω₁ + ω₂ and 2ω₁ ? ω₂ (where ω₁, ω₂ are corresponding laser beam frequencies) is generated. The intensity of this nonlinear response versus Δτ and Δr are studied. The direct measurements of the SEW temporal properties are presented. Experiments of this type are important for the development of femtosecond surface plasmon optics.     

基于双矩形腔边耦合波导的等离子体诱导透明效应

为了降低功耗、实现超快速响应,设计了一种基于双矩形腔边耦合等离子体波导系统,并研究了其等离子体诱导透明效应.采用光学Kerr效应超快调控石墨烯-Ag复合材料波导结构,实现1 ps量级的超快响应时间.动态调控等离子体波导的传输相移,当泵浦光强为5.83 MW/cm^2时,等离子体诱导透明系统能够实现透射光谱π相移,这是因为基于石墨烯-Ag复合材料结构等离子体波导具有大的等效光学Kerr非线性系数,表面等离子体激元局域光场和等离子体诱导透明效应慢光对光学Kerr效应产生了协同增强作用,大大降低了系统获得透射光谱π相移的泵浦光强.等离子体诱导透明效应透明窗口的可调谐带宽为40 nm,系统的群延时控制在0.15 ps到0.85 ps之间,并且光波通过间接耦合或者相位耦合机制实现了等离子体诱导透明效应相移倍增效应.耦合模式理论计算结果很好地吻合了时域有限差分法仿真模拟结果,研究结果对于低功耗、超快速非线性响应和紧凑型光子器件的设计和制作具有一定的参考意义.     

Graphene supports the propagation of subwavelength optical solitons

Nonlinear propagation of light in a graphene monolayer is studied theoretically. It is shown how the large intrinsic nonlinearity of graphene at optical frequencies enables the formation of quasi one‐dimensional self‐guided beams (spatial solitons) featuring subwavelength widths at moderate electric‐field peak intensities. A novel class of nonlinear self‐confined modes resulting from the hybridization of surface plasmon polaritons with graphene optical solitons is also demonstrated.     

金属/电介质颗粒复合介质的非线性交流响应

推广T矩阵法来研究二组分颗粒复合介质的非线性交流响应，解析推导出基频、三次及五次谐波频率下的有效线性介电常数及三阶和五阶非线性极化率的解析表达式.当组分颗粒的介电常数为实数时，表达式同以前微扰理论完全一致.进一步数值计算了金属-电介质复合介质的有效非线性交流响应，数值结果表明，体系的三阶、五阶非线性极化率在表面等离子共振频率附近有明显增强，而且，随着体积分数提高，共振峰增强且伴随着共振频率红移现象.还进一步讨论了维度效应对体系非线性交流响应的影响. 关键词： T矩阵方法 复合介质 非线性交流响应     

Nonlinear optical response from composites based on nanostructures consisting of an absorbing core and metallic shell near the plasmon resonance

The object of experimental study and numerical simulation is the nonlinear optical response from composites with nanoparticles consisting of a nonlinearly absorbing dielectric core and a metallic shell. It is shown that a small spread in nanoparticle sizes near the plasmon resonance may significantly change the dependence of the nonlinear optical response on the concentration of nanoparticles of each size.     

The optical transmission characteristics through gold nanoslit arrays embedded in nonlinear medium

We present the numerical investigation of the optical transmission through a periodic gold nanoslit array embedded in the Kerr type nonlinear medium by using a developed two-dimensional Finite Different Time Domain (FDTD) method. The enhanced transmission in the nonlinear structure is attributed to the collaboration of the surface plasmon resonance and the localized waveguide resonance. We show that, in a certain intensity range, with the increase of the incident intensity, the transmission resonance peaks redshift obviously, and peak values decrease firstly and then increase; with the gold film thickness and the embedded depth becoming larger, transmission resonance peaks of both types redshift significantly, and the peak number, peak value and the half peak width change obviously. The electric fields distributions for different embedded depths of the gold slits at various resonance wavelengths are simulated to illuminate the underlying physical mechanisms. It is expected that these results obtained here will help to design nonlinear subwavelength metallic grating devices.     

Ultrafast optical nonlinear properties of metal nanoparticles

The physical origin and the dynamics of the ultrafast optical nonlinear response of noble metal nanoparticles are analyzed around the surface plasmon resonance frequency using extension of the bulk metal electron kinetics and band structure models. The computed spectral and temporal responses are found to be in very good agreement with the measured ones in silver when taking into account the impact of electron excitation on both the interband absorption and electron optical scattering rate. A good reproduction of the strong excitation regime experimental results is also obtained in the case of gold, with a dominant contribution of the interband effect. Received: 4 July 2001 / Published online: 10 October 2001     

Controlling electric fields spatially by graded metamaterials: Implication on enhanced nonlinear optical responses

The local electric field of a graded metal-dielectric cylinder, with complex permittivity given by a spatially dependent Drude model, has been derived analytically in terms of hypergeometric functions. Our results show that the electric field inside the cylinder can be confined in desired positions. Thus one can achieve the control of electric fields by fabricating graded metamaterials with specific material parameters. The enhanced nonlinear optical responses are also examined. The results suggest that the gradation-controlled field distribution may be a consequence of a combination of surface plasmon resonance and microgeometry in graded metamaterials.     

Characteristic energy loss spectra of copper crystals with surfaces described by LEED

Energy distributions of electrons back-scattered from copper (100) and (110) surfaces have been obtained for incident electron energies in the range 30 to 350 eV. The relations between optical measurements and the characteristic energy losses, as well as the effect of interband transitions on the bulk and surface plasmon frequencies in metals which do not have ideally free electron plasmas are discussed. By chemisorbing increasing amounts of oxygen on the clean surface, the surface plasmon loss peak was identified in the copper energy loss spectrum from its intensity dependence on the dielectric constant at the surface. This peak has been identified by previous authors as the bulk plasmon loss of a single s-electron plasma oscillation. Our identification of the surface plasmon loss peak implies that the d-electrons in copper do participate in the plasma oscillation and that the bulk plasmon frequency is shifted from its free electron value because of interband transitions.     

Messung der Energieverlustspektren von Aluminium- und Silberfolien mit hoher Auflösung

The energy loss spectra of polycrystalline aluminium and silver foils have been measured with high resolution. For the plasmon energy of aluminium 14.97 eV is obtained. The half width of the plasmon peak is 0.60 eV corresponding to a relaxation time τ=1.1×10^?15 sec in fair agreement with optical data. In silver films of certain thicknesses the surface plasmon peak and the plasmon peak can be separated in the energy loss spectrum. The values of the energy losses are 3.64 and 3.78 eV respectively.     

Transmission of light through coaxial and non-coaxial double-layer gold slit arrays

We investigate numerically the transmittance of light through gold double-layer structures with periodic coaxial and non-coaxial slits. We attribute the enhanced optical transmission to the surface plasmon resonance collaborating with the localized waveguide resonance. The transmission spectra and the surface electric fields are used to characterize the resonances of both types. For the coaxial system, with the increase of the slit width of the second layer, the resonance peak values of both types increase sharply at first until the two layers have the same slit width and then decrease dramatically; additionally, the center of the localized waveguide resonance peak shifts to shorter wavelength noticeably, but the surface plasmon peak center moves negligibly. As regards the non-coaxial structure, it shows a similar behavior of the localized waveguide resonance peak to that of the coaxial one; however, the surface plasmon resonance peak behaves in a different way. These results may be associated with the surface plasmon coupling modes and the Fabry–Perot cavity modes in the double-layer structure.     

Linear and nonlinear optical properties of Au/SiO2 nanocomposite prepared by P123

Mesoporous silica thin films loaded with gold nanoparticles are synthesized in the presence of EO20PO70EO20（P123）.Transmission electron microscope images show that the matrix of the nanocomposite is an ordered porous structure with a two-dimensional hexagonal phase.The wide-angle X-ray diffraction pattern implies that the nanocomposite contains gold crystals.These metallic nanoparticleembedded solid thin films show some linear and nonlinear optical properties due to their special structure and composition.Gold nanoparticles bring about surface plasmon resonance,and an absorption peak stemming from this effect has been observed.The linear absorption property is analyzed by a quantum mechanism,and the results show that it is influenced by the size and volume fraction of gold nanoparticles. Furthermore,it shows an obviously clear nonlinear optical property measured by the z-scan technique.The magnitude of the nonlinear refractive index of the nanocomposite is estimated to be about 10？ 10 cm 2 /W.     

Size-dependent nonlinear optical properties and thermal lens in silver nanoparticles

We have investigated the nonlinear response of the silver nanoparticle samples in a low-power regime of electromagnetic field based on nonlocal thermo-optic models. In this work, the experimental investigation of the thermo-optic nonlinear response of Ag colloids containing different size of silver nanoparticles is reported. The colloidal nanoparticle samples were synthesized by nanosecond pulsed laser ablation of Ag bulk in acetone. The sample containing Ag was characterized by linear absorption spectroscopy and transmission electron microscopy. Using the z-scan technique, the behavior of thermal nonlinear refractive index of colloid was studied at different concentrations of silver nanoparticles. Observation of asymmetrical configurations of the z-scan data indicates that nonlinear refraction occurring in the Ag samples is related to the thermo-optical process. The optical limiting here is due to nonlinear refraction of the samples arising from thermal lens formation under low-power CW excitation. When the laser power is low, the self-defocusing effect is mainly dominated by surface plasmon resonance effect. Results show that with increasing concentration of nanoparticles in acetone, the nonlinear refractive index increases while the threshold power of optical limiting decreases.     

Front Cover Picture: Laser & Photon. Rev. 7(2)/2013

Nonlinear propagation of light in a graphene monolayer is studied theoretically. In this article, it is shown how the large intrinsic nonlinearity of graphene at optical frequencies enables the formation of quasi one‐dimensional self‐guided beams (spatial solitons) featuring subwavelength widths at moderate electric‐field peak intensities. A novel class of nonlinear self‐confined modes resulting from the hybridization of surface plasmon polaritons with graphene optical solitons is also demonstrated. (Picture:M. L. Nesterov et al. dx.doi.org/10.1002/lpor.201200079 , pp. L7–L11, in this issue)