飞秒时间分辨实验中相关函数和时间零点的确定

结合飞秒激光在研究分子激发态弛豫动力学中的应用,介绍了几种飞秒时间分辨实验中确定泵浦激光脉冲与探测激光脉冲的相关函数和时间零点的方法.对于波长在可见波段的泵浦和探测激光脉冲,我们可以利用非线性光学的技术手段,探测泵浦光与探测光的和频光的强度随二者间的时间延迟的变化来确定相关函数和时间零点;对于波长在紫外甚至更短的波段的泵浦和探测激光脉冲,由于单脉冲能量比较低,目前还很难利用技术手段来测定泵浦激光与探测激光的相关函数及时间零点,可以利用某些原子气体(如Xe)或某些具有短寿命态的分子作平行实验进行间接测量.     

飞秒时间分辨实验中泵浦-探测交叉相关函数的测量和时间零点的确定

飞秒激光技术的出现使得实时探测与跟踪激发态超快弛豫动力学过程成为可能,并能够给出激发态动力学过程清晰的物理图像。而在飞秒时间分辨实验中,泵浦-探测相关函数和时间零点直接影响实验结果的可靠性和准确性。本文结合飞秒激光在分子激发态超快动力学过程中的应用进展,介绍了根据实验条件和要求,在具体实验过程中泵浦-探测相关函数测量和时间零点确定的几种方法。实验中选择可见光作为泵浦光和探测光时,可以通过测定随泵浦-探测时间延迟变化的泵浦激光与探测激光的和频/差频光强来确定泵浦探测交叉相关函数和时间零点;而选择中心波长在紫外甚至真空紫外的激光脉冲作为泵浦光或探测光时,泵浦-探测交叉相关函数通常采用校正的方法测量。     

利用圆锥辐射优化飞秒荧光光谱的光学参量放大

基于非共线光学参量放大的飞秒时间分辨荧光光谱技术是一种新的超快光谱研究方法.文章研究了荧光放大的参量过程.超连续的种子光其瞬时光强可以被线性放大.由于系统高达107的放大能力,泵浦脉冲能量的微小不稳定性在最终放大输出信号中将产生很大起伏.提出了一种利用圆锥辐射作为参考消除此干扰的方法.研究表明,探测的荧光动力学曲线有显著改善.     

基于瞬态光栅频率分辨光学开关法测量飞秒脉冲的研究

超宽光谱的飞秒脉冲测量一直是超快激光领域的重要研究方向之一.常规的飞秒脉冲自相关方法是通过测量自相关倍频信号来获得,而倍频信号具有波长选择性,不同中心波长的飞秒脉冲测量需要更换不同的倍频晶体,十分不方便.因此,提出了一种改进型的瞬态光栅频率分辨光学开关(TG-FROG)方法用于测量飞秒脉冲.该方法结合四波混频和频率分辨光学开关方法,其基本过程是将待测脉冲分为三束,其中两束脉冲经过精密的延时控制并聚焦在光学介质上达到时空重合,利用三阶非线性效应产生稳定的瞬态光栅作为开关光;另一束脉冲作为探测光与产生的瞬态光栅进行相互作用产生一个信号光,使用光谱仪对该信号光的光谱与延迟时间进行测量,并通过反演迭代算法处理而获取待测飞秒脉冲的光谱与电场信息.该方法只需要待测光的功率密度达到三阶非线性效应就可以实现测量,因此可以应用于任意中心波长的飞秒脉冲测量.利用该方法对中心波长分别为800 nm, 400 nm的飞秒脉冲,以及超连续亚10 fs的周期量级超宽光谱飞秒脉冲进行了测量,并与常规的干涉自相关仪器测量结果进行了比较,所得测量结果基本一致.实验结果表明,建立的基于TG-FROG方法对不同中心波长,不同脉冲宽度的飞秒脉冲测量是十分有效的.     

纳米光学和生物单分子探测

纳米光学技术展示了纳米级探测本领，同时生物单分子探测所需要分辨尺度也是纳米数量级的，因此在生物单分子探测过程中，纳米光学发挥了巨大的作用．文章介绍了与生物单分子探测技术相关的纳米光学技术，包括量子近场光学探针技术、近场光学成像技术(包括扫描近场光学显微术及全内反射荧光显微术)和激光光钳测控技术及它们在生物单分子探测上的进展，从而在染色、成像、测控三个方面展示了纳米光学技术在生物方面的应用，并对其未来的发展方向进行了展望．     

飞秒激光作用下金掺杂硅酸盐玻璃的光致晶化研究

研究了金掺杂硅酸盐玻璃在飞秒激光辐照和热处理作用下的光致晶化行为，分析探讨了其机理和激光辐照条件的影响.吸收光谱测试表明玻璃内部析出金纳米颗粒. 金纳米颗粒掺杂玻璃在近共振纳秒脉冲作用下显示了强的光限幅效应, 且改变飞秒激光诱导参数可改变该复合玻璃的光学非线性. 关键词： 光致晶化 飞秒激光 金纳米颗粒 硅酸盐玻璃 光限幅     

InP纳米颗粒的超快动力学和光学非线性

通过飞秒泵浦-探测方法测量了波长为800 nm时InP半导体纳米颗粒激发态的瞬态动力学过程。观察到一个快速的光致漂白建立和一个漂白的恢复过程,分析饱和吸收的来源可能是带填充效应引起跃迁的饱和吸收。对于漂白恢复中的快过程是由于自由载流子的弛豫,而慢成分是由于光激发载流子在很短的时间内受陷于表面态形成的限域载流子的弛豫。通过飞秒光克尔效应(OKE)方法测量材料的超快非线性响应曲线,计算了材料的光学三阶非线性极化率,分析了非线性的来源。     

纳米尺度的光学成像与纳米光谱———近场光学与近场光学显微镜的进展

近场光学是指当光探测器及探测器－样品间距均小于辐射波长条件下的光学现象．利用近场光学扫描显微镜和近场光谱仪，不但能够以突破衍射极限的超高分辨率在纳米尺度实现光学成像，而且还可获得纳米微区的光谱信息．文章介绍近场光学的原理及其在凝聚态物理领域中的应用与进展，并给出了我们的初步结果     

纳变尺度的光学成像与纳米光谱：近场光学与近场光学显微镜的进展

近场光学是指当光探测器及探测器一样品间距均小于辐射波长条件下的光学现象，利用近场光学扫描显微镜和近场光谱仪，不但能够以突破衍射极限的超高分辨率在纳米尺度实现光学成像，而且还可获得纳米微区的光谱信息，文章介绍近场光学的原理及其在凝聚态物理领域中的应用与进展，并给出了我们的初步结果。     

细菌视紫红质近场光存储特性的研究

结合近场光学显微镜，利用菌紫质M态和基态之间的跃迁，对BR—D96N样品作了静态近场光存储特性的研究。结果表明，近场区域内细菌视紫外质在光激发前后对红光的吸收有较大差别，而且激发后无光照时会缓慢弛豫到激发前的状态，具有光致变色特性和热弛豫特性，可望作为近场光存储材料和微光学信息处理器件材料。     

Scanning Near-Field Optical Microscopy and Microspectroscopy of Green Fluorescent Protein in Intact Escherichia coli Bacteria

Scanning near-field optical microscopy (SNOM) yields high-resolution topographic and optical information and constitutes an important new technique for visualizing biological systems. By coupling a spectrograph to a near-field microscope, we have been able to perform microspectroscopic measurements with a spatial resolution greatly exceeding that of the conventional optical microscope. Here we present SNOM images of Escherichia coli bacteria expressing a mutant green fluorescent protein (GFP), an important reporter molecule in cell, developmental, and molecular biology. Near-field emission spectra confirm that the fluorescence detected by SNOM arises from bacterially expressed GFP molecules.     

Photopatterning of a monomolecular dye film by means of scanning near-field optical microscopy

Patterned bleaching of a photolabile monomolecular dye film by means of scanning near-field optical microscopy (SNOM) is demonstrated. After exposure, the written patterns were verified by SNOM with fluorescence detection. The adsorption of appropriate material to such near-field optically created patterns seems now feasible. The ultimate resolution limit of a monomolecular dye film for patterned bleaching by SNOM is discussed on the basis of a simple model.     

照明模式SNOM中样品对近场光场分布的影响

在同时考虑样品的形貌及材料光学参量和入射光偏振模式的情况下,利用基于边界元方法编写的二维矢量电磁场计算程序,对工作在照明模式下的扫描近场光学显微镜（Scanning Near-field Optical Microscope,SNOM）的近场矢量电磁场分布进行了数值计算模拟研究.结果表明,在没有表面形貌特征时,探针的光能量透射率随样品材料的折射率和损耗角的增加而增大,而样品表面光斑尺寸受折射率和损耗角的影响很小;对有形貌特征的探针扫描像研究结果表明,SNOM的分辨率随着样品的折射率和损耗角的增加而提高;对SNOM不同的工作模式的扫描成像信号进行的计算结果表明,恒定间距扫描方式比恒定高度扫描方式对样品表面的细节有较强的分辨能力.     

Development of Scanning Near-Field Optical Microscope Working under Cryogenic Temperature and Strong Magnetic Field

We report on the development of a cantilever-based scanning near-field optical microscope (SNOM) working in an extreme environment, at cryogenic temperature around 10 K and under strong magnetic field up to 7 T. We designed a new optical system based on an infinite conjugate microscope, which extracts the near-field signal from a small aperture through a narrow chamber into free space as collimated light. Using this system, we successfully measured near-field and topographical images of a metal-hole sample simultaneously. Combining the local optical accessing technique with the external control of the electronic state, this SNOM system will be a powerful tool to study optical properties of semiconductor nanostructures.     

Scanning near-field optical/atomic force microscopy for fluorescence imaging and spectroscopy of biomaterials in air and liquid: Observation of recombinantEscherichia coli with gene coding to green fluorescent protein

We have developed a system of scanning near-field optical/atomic force microscopy (SNOM/AFM) for fluorescence imaging and spectroscopy of biomaterials in air and liquid. SNOM/AFM uses a bent optical fiber simultaneously as a dynamic force AFM cantilever and a SNOM probe. Optical resolution of SNOM images shows about 50 nm in an illumination mode for a standard sample of a patterned chromium layer of 20 nm thickness on a quartz glass plate. The SNOM/AFM system contains a photon counting system and polychrometer/ICCD (intensified charge coupled device) system for observation of the fluorescence image and spectrograph of micro areas, respectively. The gene coding to green fluorescence protein (GFP) was cloned in recombinantEscherichia coli (E. coli). Topography, fluorescence image and spectrograph of recombinantE. coli by SNOM/AFM showed a difference in fluorescence in individualE. coli. Fluorescence activity of GFP can thus be used as a convenient indicator of transformation. SNOM/AFM is also applicable to observe immobilizedE. coli on a glass plate in water with a liquid chamber and may allow the viewing of observation of floating organisms.     

25 nm resolution single molecular fluorescence imaging by scanning near-field optical/atomic force microscopy

High-resolution single molecular near-field fluorescence images were observed by scanning near-field optical/atomic force microscopy (SNOM/AFM). We modified the SNOM/AFM for both high-resolution fluorescence imaging and high-resolution topographic imaging. The imaged fluorophore, Alexa 532, is prepared with a poly-methyl-methacrylate (PMMA) film coating. A fluorescence resolution of 25 nm was obtained with a simultaneous topographic image of a flat surface. A sample prepared with a lower PMMA concentration exhibited a rough surface in the micro area. The results for the flat surface indicated that the fluorescence resolution is worst in the rough surface sample, that the maximum fluorescence intensities for the individual fluorophore are similar, and that the decay rate is faster. Thus, we concluded that the morphological effect is an important factor in fluorescence image resolution and the apparent lifetimes of the fluorescence molecules.     

Theoretical Analyses on the Resolution of Collection Mode Scanning Near-Field Optical Microscopy

Numerical simulations have been carried out in the framework of waveguide theory to model collection mode scanning near-field optical microscopy (SNOM). The theoretical model includes the optical fiber end and describes the metal coated aperture on the probe tip. The developed formalism goes beyond the existing Bethe-Bouwkamp theories for electromagnetic transmission of subwavelength apertures. The finite coating and optical fiber end are now taken into account. The new features enable us to simulate the near-field probes that are widely used in the collection mode SNOM. The emphases of the numerical analyses have been mainly on the resolution mechanism of the microscopy. Influence on the resolution from important parameters of the probe tips, such as the size of the apertures and the probe-sample distance, is extensively studied. The resolution dependence has been analyzed in the light of the near-field coupling efficiency of the probe tip. An optimum tip size has been found which is balanced between the significant signal transmission and the resolution of the device.     

Optical near-field mapping of bright and dark quantum dot states

We theoretically investigate scanning near-field optical microscopy (SNOM) of semiconductor quantum dots. A general theoretical framework is developed that accounts for photo excitation and relaxation in complex dielectric environments. We find that in the near-field regime bright and dark excitonic states become mixed, opening new channels for the coupling to the electromagnetic field.     

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.     

SETUP AND APPLICATION OF SCANNING NEAR-FIELD OPTICAL MICROSCOPY

The research on the setup and application of scanning near-field optical microscopy (SNOM) performed in our laboratory is reviewed in this report. We have constructed a versatile low temperature scanning near-field optical microscope with the capability of near-field imaging and spectroscopy, operating at liquid nitrogen temperature. A special designed coaxial double lens was used to introduce the illumination beam through a 200μm fiber; the detected optical signal was transmitted via a fiber tip to an avalanche photon detector. The performance test shows the stability of the new design. The shear force image and optical image of a standard sample are shown. A system of SNOM working at room temperature and atmosphere was used to characterize semiconductors and bio-molecular samples. It revealed the unique features of semiconductor microdisks in the near-field that is significantly different from that of far-field. The effects of different geographic microstructures on the near-field light distribution of InGaP, GaN, and InGaN multi-quantum-well microdisk were observed.