基于等离激元纳米结构非线性响应的超快光开关及脉冲激光器

非线性光学作为现代光学的一门重要分支,在各个领域都有着重要的研究意义和应用价值.然而,受限于材料固有的非线性极化率和与外来光场的有限作用长度,其非线性光学响应很弱.等离激元纳米结构可以将外来光场束缚在纳米结构周围,在光谱共振局域空间内形成一个巨大的电磁场增强,从而极大地促进光与物质的相互作用,提高了非线性光学响应.超快脉冲激光由于其优异的性能已经广泛应用于光通信、精密测量、生物医学、军用激光武器等重要领域,虽然商用的激光器已经发展得非常成熟,可以达到超高的峰值功率、超短的脉宽以及超高的重频,但是在中远红外波段的超快脉冲研究仍然是一个缺口,所以寻找一种性能优异的可饱和吸收体材料对于脉冲激光的发展具有重要的意义.本文综述了基于贵金属和非贵金属的等离激元纳米结构在超快光开关和脉冲激光方面的应用进展.很多宽禁带半导体,通过掺杂可以表现出类似金属的性质,由于掺杂可以形成自由载流子,当其尺寸在纳米尺度时,就会表现出局域表面等离激元共振的特性,从而实现超快的非线性光学响应,并且掺杂的载流子浓度不能达到金属载流子的浓度,可以有效减小过高载流子引起的带间损耗.通过泵浦探测和Z扫描测试发现,这些等离激元纳米结构在红外波段表现出超快的非线性光学响应以及宽带可调的性质,可以产生几百飞秒量级的脉冲激光,表明它们在超快光子学领域有很大的应用前景.最后总结了不同体系等离激元材料的优势和不足,展望了未来的发展和需要改进的工作.     

Ge-Ga-Cd硫化物玻璃的超快三阶非线性光学性质与结构关系研究

本文采用飞秒时间分辨光学克尔门技术测量了GeS2-Ga2S3-CdS硫化物玻璃体系的超快三阶非线性光学响应，所用激光波长分别为820nm和640nm。?实验结果证明了GeS2-Ga2S3-CdS组分玻璃具有很大的飞秒超快三阶非线性光学响应，另外，其Kerr信号随摩尔组分的不同呈显著变化。通过拉曼光谱结构分析，探讨了此系列硫化物玻璃的三阶非线性光学性质与结构的关系，结果表明构成玻璃网络的四面体结构单元[GeS4]([GaS4])对其超快三阶光学非线性起重要作用。实验还表明了此硫化物玻璃体系的超快三阶非线性不符合半经验的Miller定律。     

石墨烯光学性质及其应用研究进展

石墨烯因其优异的光学和电学性能,及其与硅基半导体工艺的兼容性,而备受学术界和工业界的广泛关注。作为一种独特的二维原子晶体材料,石墨烯有着优异的机械性能、超高的热导率和载流子迁移率、超宽带的光学响应谱及极强的非线性光学特性,使其在新型光学和光电器件领域具有得天独厚的优势。一系列基于石墨烯的新型光电器件先后被研制出,已显示出优异的性能和良好的应用前景。本文将介绍石墨烯光学性质、与光的相互作用以及提高方法,并给出其在光子和光电子器件领域的应用,分析了这些器件所使用的结构及特点,重点阐述了在全内反射结构下,石墨烯与光相互作用的增强及其偏振依赖性质,及其利用该偏振依赖性质在光学传感、光存储等方面的应用,以及在细胞传感方面的重要发现。最后对石墨烯光学性质及其应用的现状进行了总结和展望。     

有机自组装低维圆偏振发光材料的研究进展

具有圆偏振发光(CPL)性质的材料由于在3D显示、光学存储以及光学防伪等领域的重要应用,近年来越来越受到研究人员的关注。超分子策略能够将不同类型的分子组装成具有独特功能的低维(零维、一维和二维等)结构,因而成为构筑CPL活性有机低维材料的最有效方法之一。本文从超分子自组装驱动力的角度综述了近几年自组装CPL活性有机低维材料的研究进展。首先,本文系统地总结了现阶段设计自组装CPL活性有机低维材料的策略,其次重点讨论了这类材料的性能及应用,最后探讨了这一领域未来的发展机遇和挑战。     

基于相变材料超表面的光学调控

超表面光学完美结合了传统的几何、物理光学理论和前沿的纳米技术,近年来引起科研工作者的广泛关注.在线性光学领域,它已广泛用于对光波的振幅、相位进行调控,如平面透镜、全息成像和热辐射器件等.在非线性光学领域,针对它在高次谐波生成、超快激光器等方面的研究工作也方兴未艾.本文分别从理论和应用角度,分析总结了国内外超表面光学调控方向的研究进展,重点介绍了利用相变材料实现动态光学调控的前沿研究工作,并讨论了未来发展前景以及需要解决的难题.     

低维材料非线性光学与器件专题编者按

正2004年,石墨烯的首次发现为具有独特光子和光电特性的二维材料的发展打开了大门.二维材料通常被称为原子薄层材料,其厚度可减至单层或几层.强的层内共价和弱的层间范德瓦耳斯力是二维材料的典型特征.不同厚度和电子结构的二维材料使其可以在紫外到太赫兹的波长范围内进行光学响应,极大地扩展了二维材料在光子学领域的应用范围.二维材料还具有优异的光子特性,如泡利阻塞诱导的饱和吸收、超快的弛豫时间和高度的光学非线性,为其在光子学领域广泛的应用奠定了基础.由于原子层的二维材料具有机械稳定性和表面自然钝化的特点,可无选择性地牢固地集成到其他结构中,如平面波导、玻璃纤维、光学微腔和其他二维层状结构,而不会出现"晶格失配"问题.此外,二维材料的光学性质可以通过电选通、光激励、或化学掺杂来精确控制.     

稀土材料的超快共振非线性光学特性研究

用抽运-探测技术测量光学响应材料非线性极化率的方法，研究了稀土材料非线性折射率的共振增强和超快响应的非线性动力学过程。测得钕玻璃的三阶非线性折射 率强度系数为10^-14cm^2/W，比其基质的非线性折射率强度系数提高了2个量级。用该方法研究了Nd:YVO4、Er:YAG等晶体的超快非线性响应过程。实验结果与理论分析表明，抽支-探测技术是测量非线性极化率的简单而又灵敏的方法。这一测量技术对研究与开发超高速光响应器件具有重要的实用价值。     

微微秒时域上对二维卟啉类分子材料的三阶非线性光学性质的研究

报道了针对二维卟啉类有机分子材料的光学非线性性质研究，讨论了几种非对称配置电负性分子团对构成分子的光学非线性的影响，表明配置的分子基团电负性越大，合成分子非线性超级化率越大，实验研究了这些分子的光学非线性响应特性，分析了各种非线性机制在分子非线性响应中的作用。     

有机自由基发光体

有机自由基由于存在未配对或弱成键电子,因而具有独特的基态开壳电子结构。这类开壳电子结构的分子体系可展示出特殊的物理性质,如近红外吸收、非线性光学响应、可逆电子氧化还原、磁学性质等,有望成为下一代光电磁信息功能材料。然而,绝大多数自由基在光激发态下以非辐射方式释放能量,从而表现为弱发光或不发光。近年来,以三芳基甲基自由基衍生物为代表的双线态自由基发光体逐渐引起研究者的关注,其红光发射的荧光量子产率可达到90%以上,且成功地应用于有机电致发光器件(OLED)。自由基发光体是在基态和激发态均具备自由基特征的新型分子体系,其分子结构设计与发光性质调控是该领域的关键难题。在已报道的仅有的少数发光自由基的基础上,人们更多地期待获得性能优异、可选择性调色的多种类发光自由基及其作为功能材料的潜在应用。本文总结了发光自由基的分子结构、物理性质和构效关系,以及激发态发光机制与自由基非辐射跃迁抑制机理等,讨论了目前的研究现状和未来的研究挑战。     

分子动力学模拟方法在非线性光学中的应用

有机分子非线性光学材料在频率转换、电光调制和双光子吸收等方面具有重要的应用.介绍了近年来分子动力学模拟方法在有机分子非线性光学性质理论研究中的主要应用,包括电场极化效应、局域场因子、非线性极化率和双光子吸收等.此外,结合最新的科研工作,介绍了分子动力学模拟方法在溶剂效应和聚集效应研究中发挥的重要作用. 关键词： 分子动力学模拟 溶剂效应 聚集效应 双光子吸收     

Nonlinear spectrum effect on the coherent control of molecular systems

This work demonstrates that the detuning of the fs-laser spectrum from the two-photon absorption band of organic materials can be used to reach further control of the two-photon absorption by pulse spectral phase manipulation. We investigate the coherent control of the two-photon absorption in imidazole-thiophene core compounds presenting distinct two-photon absorption spectra. The coherent control, performed using pulse phase shaping and genetic algorithm, exhibited different growth rates for each sample. Such distinct trends were explained by calculating the two-photon absorption probability considering the intrapulse interference mechanism, taking into account the two-photon absorption spectrum of the samples. Our results indicate that tuning the relative position between the nonlinear absorption and the pulse spectrum can be used as a novel strategy to optimize the two-photon absorption in broadband molecular systems.     

Role of doubled-frequency absorption in two-photon response of the Si MSM structure

The physical mechanism of two-photon response was studied in this paper by measuring characteristics of the two-photon response of the Si metal–semiconductor–metal (MSM) structure sample. The two-photon response includes two-photon absorption (TPA) and doubled-frequency absorption (DFA). An experiment was designed to measure the photocurrent dependence on incident light power, the dependence of the photoelectric signal on the applied voltage and the relationship between the photoelectric current and the light-spot position. The experimental fact that two-photon response of the silicon sample is relative to the applied electric field shows that DFA is the main physical mechanism of two-photon response and establishes the foundation for fabricating high-sensitivity two-photon response Si photodetector.     

单光子和双光子激发的超歧化聚合物的光谱学特性研究

研究了二种新型超歧化聚合物在氯仿和二甲基甲酰胺溶剂中的飞秒激光单光子和双光子激发的光谱学特性．这二种聚合物是以苯为核、以对二甲氧基苯为连接单元，分别以二甲基苯胺为端基或以特丁基苯为端基的超歧化共轭聚合物．结果表明这种超歧化聚合物具有较大的溶剂极性相关的飞秒双光子吸收截面，不同的端基不仅影响分子内的电荷转移，而且导致超歧化分子共轭程度的变化．作为一种潜在的光学非线性材料，利用这种大的双光子吸收截面的超歧化聚合物可实现了飞秒双光子直写的三维高密度数据存储．     

Mathematical modeling of two-photon thermal fields in laser–solid interaction

In this paper, we have developed an analytical model to study the temperature distributions in IR optical materials heated by laser pulses. Our model takes into account the two-photon absorption (TPA). The calculations are based on a three-dimensional model of heat diffusion in solids using the integral transform method. We find out the rigorous analytical expression of the thermal field when one considers both one- and two-photon absorption. The model is valid for any laser–solid system whose interaction can be described by the generalized Beer–Lambert law. Specific results are presented for an application of the model to ZnSe sample. We find out that TPA can produce detectable temperature variation.     

Acetylene-Substituted Two-Photon Absorbing Molecules With Rigid Elongated Pi-Conjugation: Synthesis,Spectroscopic Properties and Two-Photon Fluorescence Cell Imaging Applications

Two asymmetrical molecules with substituted acetylene as central rigid elongated conjugation are reported as potential chromophores for two-photon microscopic imaging. These molecules consist of a typical D–π–A structure, have different donors (D), the same π-conjugated center (π) and the same acceptor (A). Structural characterization and spectroscopic properties, including single-photon (linear) absorption, quantum yields, single-photon fluorescence, and two-photon absorption spectra, were studied in solvents with different polarity. These acetylene-substituted molecules were found to have high two-photon absorption cross-sections (for example, 690 GM for molecule 1 in toluene), which were determined by a two-photon induced fluorescence method using a femtosecond Ti: sapphire laser as excitation source. Single- and two-photon cellular imaging experiments demonstrate that the substituted acetylene derivatives could be one kind of promising two-photon fluorescence probes for cellular imaging.     

溶剂对N-{4-[(反式)-2-(4-硝基苯基)乙烯基]苯基}-N,N-二苯氨基分子双光子吸收特性的影响

在从头计算的基础上,利用两态模型对溶剂对N-{4-[(反式)-2-(4-硝基苯基)乙烯基]苯基}-N,N-二苯氨基分子双光子吸收特性的影响进行了理论研究.计算结果表明,溶剂对该分子的双光子吸收截面影响较大,双光子吸收截面随着溶剂极性的增加而增加.     

双光子吸收材料二苯乙烯衍生物的合成及光谱性质

设计、合成并用红外光谱、1H NMR、元素分析表征了三种用于双光子吸收材料的二苯乙烯衍生物,4,4′-双(二苯氨基-反式-苯乙烯基)联苯(BPSBP),4,4′-双(二乙氨基-反式-苯乙烯基)联苯(BESBP)和4,4′-双(9-咔唑基-反式-苯乙烯基)联苯(BCSBP)。实验结果表明三者最强的单光子吸收出现在350～400 nm之间,且单光子吸收和荧光光谱中表现出明显的溶剂化显色效应,揭示了分子内对称电荷转移的本质,双光子荧光光谱则揭示了单光子和双光子吸收具有相同的发射机理。利用双光子上转换荧光法测试发现,三种双光子吸收材料在800 nm飞秒激光的激发下具有较大的吸收截面,分别为892,617和483 GM,这表明在双光子领域有潜在的应用价值。     

Transparency due to dipole–dipole interaction in photonic crystals doped with nanoparticles

In this paper, we have studied the two-photon absorption process in photonic crystals doped with four-level nanoparticles. It is considered that all the levels of the particles are interacting with the photonic crystal. The decay linewidths of all the four levels are included in the calculations of two-photon absorption process. The effect of the dipole–dipole interaction has also been included in the formulation. Numerical simulations have been performed for the two-photon absorption spectrum on an isotropic photonic crystal. It is found that the system switches between the transparent and the nontransparent states due to the dipole–dipole interaction. The phenomenon of switching depends on the linewidths of these states.     

Two-photon induced optical-power limiting and upconverted superradiance properties of a new organic dye HEASPI

A new organic dye trans-4-[p-(N-ethyl-N-hydroxyethylamino)styryl]-N-methylpyridinium iodide (abbreviated as HEASPI hereafter) with large two-photon absorption (TPA) cross section and excellent upconverted superradiance properties was synthesized in our group recently. The TPA cross section was measured to be σ₂′=7.0×10⁻⁴⁸ cm⁴ s/photon by using an open aperture Z-scan system. Linear absorption, single-photon induced fluorescence, two-photon induced fluorescence and two-photon pumped (TPP) upconverted superradiance properties were systematically studied. The highest net upconversion efficiency from the absorbed pump energy to the output upconverted superradiance energy is as high as 19.6% at the pump energy of 2.07 mJ from a mode-locked Nd : YAG picosecond laser. The dye solution also shows a clear optical power limiting effect.