Theory of enhanced second-harmonic generation in some artificial materials

We review the recent theoretical investigation on enhanced second-harmonic generation (SHG) in soft nonlinear optical materials based on ferrofluids, graded metallic films, and graded metal-dielectric films of anisotropic particles. The SHG of soft ferrofluid-based nonlinear optical materials possess magnetic-field controllabilities, i.e., magnetic-field-controllable anisotropy, red-shift and enhancement, which are caused to appear by the shift of a resonant plasmon frequency due to the formation of the chains of the coated nanoparticles. Both graded metallic films and graded metal-dielectric films of anisotropic particles can serve as a novel optical material for producing a broad structure in both the linear and SHG response and an enhancement in the SHG signal, due to the local field effects.      

Optical second-harmonic-generation probe of two-dimensional ferroelectricity

Optical second-harmonic generation (SHG) is used as a noninvasive probe of two-dimensional (2D) ferroelectricity in Langmuir-Blodgett (LB) films of the copolymer vinylidene fluoride with trifluoroethylene. The surface 2D ferroelectric-paraelectric phase transition in the topmost layer of the LB films and a thickness-independent (almost 2D) transition in the bulk of these films are observed in temperature studies of SHG.     

Enhanced nonlinear optical responses of materials: Composite effects

We review recent theoretical progress in understanding physical processes of composite effects on enhanced third-order nonlinear optical responses of various kinds of the recently-proposed nonlinear optical materials, namely, colloidal nanocrystals with inhomogeneous metallodielectric particles or a graded-index host, metallic films with inhomogeneous microstructures adjusted by ion doping or temperature gradient, composites with compositional gradation or graded particles, and magneto-controlled ferrofluid-based nonlinear optical materials.     

氧化铟锡薄膜的二阶非线性光学特性研究

利用二次谐波产生技术研究了氧化铟薄膜的非线性光学特性.氧化甸锡薄膜中多晶晶粒的优先取向,使其产生了非常强的二次谐波信号,并且在一定的薄膜存度以上,随薄膜厚度的增加二次谐波信号显著增强.由于多晶晶粒的优先取向使得薄膜基板平面内存在着非常明显的非线性光学各向异性.     

Magnetization-induced anisotropy of second harmonic generation in thin cobalt films

Magnetization-induced effects in the symmetry properties of optical second harmonic generation (SHG) are studied in thin cobalt films. We demonstrate that the application of an external magnetic field leads to the appearance of a strong SHG azimuthal anisotropy from the isotropic Au/Co structure. Symmetry analysis of the SHG dependencies, supported by the SHG interferometry measurements, indicates that the effective magnetic and crystallographic second-order susceptibilities are both of the same order of magnitude.     

Anisotropy of the optical and magneto-optical response of Au/Co/Au/Cu multilayers grown on vicinal Si (111) surfaces

The optical and magneto-optical second harmonic reflectivity response of Au/Co/Au/Cu multilayers grown on vicinal Si (111) substrates has been studied. These azimuthal optical non-linear experiments check the uniaxial character of the crystallinity of the Au buffer layer and the magnetic behavior of the ultrathin Co films in the metallic multilayer. They clearly show the strong dependence of the growth parameters and the misorientation of the vicinal surface on the SHG reflectivity signals. This uniaxial behavior is also correlated to linear MOKE experiments on the magnetic anisotropy with an easy magnetization axis parallel to the step edges. Received: 16 October 2001 / Published online: 29 May 2002     

Dielectric Chiral Metasurfaces for Second-Harmonic Generation with Strong Circular Dichroism

Dielectric chiral metasurfaces can generate harmonic waves with high efficiency and strong circular dichroism (CD), when they are supported by metallic substrates. Numerical results show that the second-harmonic generation (SHG) efficiency of about 10⁻³% for a peak pump intensity of about 5 GW cm⁻² can be achieved in the blue-UV, and the SHG CD reaches up to about 1.8, from a metasurface of Z-shaped lithium niobate nanoantenna array supported by gold substrate. Highly efficient and strong circular dichroic nonlinear responses are attributed to the plasmon-assisted local field enhancement in the dielectric chiral nanoantennae adjacent to the metallic substrate.     

超高真空中C60光聚合效应光学二次谐波的研究

利用１．０６４μｍ基频超短脉冲激光，使用光学二次谐波方法研究了超高真空中蒸镀在多晶银表面上的Ｃ６０薄膜紫外光照射下的光聚合现象，发现聚合以后的Ｃ６０二阶非线性响应增强，同时观察到光聚合的饱和效应，Ｃ６０光聚合二阶非线性的提高可以用电四极了磁偶极子对二次谐波贡献的增强来解释。     

Voigt位型下电介质/反铁磁/电介质结构二次谐波生成非倒易性研究

利用非线性传递矩阵方法研究了Voigt位型下电介质/反铁磁/电介质 结构二次谐波生成的非倒易性. 研究发现外加静磁场反向和电介质层排序翻转均对二次谐波输出产生影响, 出现了二次谐波生成的非倒易性. 二次谐波生成非倒易性频率区域在反铁磁共振区, 此区间正处于THz频段. 随着入射角度的增加, 非倒易性的效果越来越明显. 研究二次谐波生成的非倒易性, 可为反铁磁器件的设计加工提供理论支持.     

SiO2-GeO2薄膜二次谐波产生的稳定性研究

利用溶胶－凝胶（ｓｏｌ－ｇｅｌ）方法制备了ＳｉＯ２－ＧｅＯ２薄膜,并测量了薄样品电场极化后光学二次谐波信号的相对大小和时间弛以豫特性,通过对汪同衬底材料及不同温度下电场极化薄膜样品二次谐波信号的时间弛豫特性比较,表明薄膜与衬底之间界面电荷的稳定性受衬底材料体电导率的影响,从而影响了薄薄膜样品二次谐波信号的稳定性。     

Thin noble metal films on Si (111) investigated by optical second-harmonic generation and photoemission

Thin noble metal films (Ag, Au and Cu) on Si (111) have been investigated by optical second-harmonic generation (SHG) in combination with synchrotron radiation photoemission spectroscopy. The valence band spectra of Ag films show a quantization of the sp-band in the 4-eV energy range from the Fermi level down to the onset of the d-bands. For Cu and Au the corresponding energy range is much narrower and quantization effects are less visible. Quantization effects in SHG are observed as oscillations in the signal as a function of film thickness. The oscillations are strongest for Ag and less pronounced for Cu, in agreement with valence band photoemission spectra. In the case of Au, a reacted layer floating on top of the Au film masks the observation of quantum well levels by photoemission. However, SHG shows a well-developed quantization of levels in the Au film below the reacted layer. For Ag films, the relation between film thickness and photon energy of the SHG resonances indicates different types of resonances, some of which involve both quantum well and substrate states. Received: 16 October 2001 / Revised version: 14 March 2002 / Published online: 29 May 2002     

Second harmonic generation in composites of ellipsoidal particles with core–shell structure

We study the enhancement of the second-harmonic generation (SHG) coefficient in a random composite consisting of ellipsoidal particles with a core–shell structure in a linear dielectric host. The material making up the ellipsoidal core is assumed to be dielectric, but with a nonlinear susceptibility for SHG. The coating material is assumed to be metallic with a linear susceptibility. The effective SHG coefficient is derived and its expression is related to various local field factors. The numerical calculations of the effective SHG response per unit volume of nonlinear material can be greatly enhanced at certain frequencies. For coated ellipsoidal particles, the core–shell structure and the particle shape allow for tuning of the resonance through the choice of material parameters and/or the ratio of the core to shell volume fraction and the depolarization factor of the particles.     

金、铜、铂、银表面光学二次谐波参数的研究

以1.06μm激光为基频光,测量了金、铜、铂、银膜的反射二次谐波随基频光偏振角的变化,在b=-1的条件下拟合求得了这几种样品面谐波电流的唯象参数“a”值。     

Observation of Optical Second Harmonic Generation in Wet-Spun Films of Na-DNA

The observation of optical second harmonic generation (SHG) from wetspun films of Na-DNA is reported. The SHG signal is stronger at a relative humidity of 92% (corresponding to the B conformation of Na-DNA) than at low humidity of -33% (corresponding to a disordered conformation of Na-DNA). The strength of the SHG signal is also dependent on the orientation of the incident laser beam polarization with respect to the DNA helical axes.     

Nonlinear optical and electrostatic force microscopy for ferroelectric polarization imaging

Second-harmonic generation (SHG)-based nonlinear optical microscopy is used for spatially resolved imaging of the polarization switching in lead zirconium titanate ferroelectric thin films. The local SHG hysteresis loops reveal a strong dependence on film composition and structure. The SHG microscopy results are in good agreement with the efficiency of electrostatic force microscopy writing and allow us to predict the microscopic dielectric memory efficiency, both in contact and contact-less ways. Received: 15 January 2001 / Revised version: 27 March 2002 / Published online: 6 June 2002     

Second harmonic generation by cold-deposited silver films

The second harmonic generation (SHG) of light diffusely scattered by cold-deposited silver films is negligible with respect to the specular intensities. Therefore, a cold-deposited silver film is well approximated by a homogeneous effective medium. The intensities of SHG at 1.06 μm and the optical absorption at 0.53 μm depend on both the square of the internal effective field at 0.53 μm and a change in the same way when annealing the film. This can be understood by the assumption that SHG is also mainly following the electric field within the metal phase and surface contributions to SHG interfere destructively. This is corroborated by the observation that the SHG intensity does not show the ‘chemical first layer effects’ seen by surface-enhanced Raman scattering (SERS).     

手性薄膜表面二次谐波圆二向色性的研究

给出了螺旋型手性分子薄膜表面反射方向的圆二向色性的谐波强度表示式,分析了谐波的强度与手性分子的取向,分子的螺距和半径等结构参数的关系,给出了数值模拟结果,发现在入射光强一定的情况下,谐波强度在螺距和半径的取值范围内分别存在着最大值,以及螺距与半径之间满足的关系式随分子取向角的变化而不同。     

About the depth sensitivity of second-harmonic radiation in ultra-thin metal films

Second-harmonic generation (SHG) results for Ni and Co films on Cu (001) have been reinvestigated regarding the depth sensitivity of this technique for thin films. We find that tangential components of the nonlinear susceptibility are much more sensitive to real film properties than normal components, which are confined to surfaces and interfaces. In consequence, for SHG experiments on ultra-thin metal films, polarization combinations should be favored that possess only tangential susceptibility components, even though the yield is weaker. Additional phase measurements are necessary to obtain full information about the film. Received: 20 January 2002 / Published online: 6 June 2002     

4-硝基-4′-氨基偶氮苯的光学性质研究

采用紫外可见吸收和二次谐波产生技术研究了“推-拉”型偶氮苯分子Langmuir-Blodgett(LB)膜的光谱和二阶非线性光学特性.4-硝基-4′-氨基偶氮苯(NAA)分子能制成很好的LB多层膜,在稀溶液中以单体的反式异构体形式存在,在膜中主要以J-聚集体的形式存在,LB膜的紫外可见吸收谱的吸收峰较之溶液的发生了52 nm的红移.NAALB膜的二阶非线性极化率χ(2)为19.59×10－8 esu,一阶超极化率β值较大,约为1.974×10－29 esu.其光学二阶非线性起源于电偶极子机制.     

氰基团修饰的苯腙类有机分子掺杂极化聚合膜光学非线性的研究

采用实时测量光学二次谐波产生（ＳＨＧ）和吸收光谱的方法对苯腙类有机分子ＮＤＡ及一种新合成的经氰基团修饰的有机分子ＣＮＤＡ掺杂ＰＭＭＡ极化聚合膜的非线性光学性质进行了研究。实验中发现两种掺杂极化聚合膜的最佳电晕极化温度均低于它们的玻转温度,ＣＮＤＡ／ＰＭ－ＭＡ极化掺杂聚合膜的χ（２）较ＮＤＡ／ＰＭＭＡ极化聚合膜的大。结合极化前和极化后吸收峰强度的变化,得到ＣＮＤＡ分子的非线性极化率β约为１４６×１０－３０ｅｓｕ。在撤离极化场后,ＣＮＤＡ／ＰＭＭＡ的二次谐波强度的弛豫也比ＮＤＡ／ＰＭＭＡ的慢