受激拉曼散射显微技术及其应用

随着光学显微技术的发展,人们得以在亚微米级的尺度观察微观世界,对破译生命活动密码起到了关键性推动作用.其中,相干拉曼散射(CRS)显微术作为一类基于分子特定振动提供成像衬度的技术,通过非线性光学过程大大增强了拉曼散射的信号,提高了成像速率和检测的灵敏度.根据非线性光学过程的不同,可将相干拉曼散射分为相干反斯托克斯拉曼散...     

表面等离子体受激辐射放大领结型纳米天线的SERS单分子探测(英文)

基于表面等离激子受激辐射放大原理,提出了一种应用于表面增强拉曼散射(SERS)单分子探测的领结型纳米天线结构。采用有限元方法(FEM)研究其局域表面等离子体共振(LSPR)和SERS特性。结果表明,该领结型纳米天线的局域表面等离子体共振强度和局域电场强度得到明显的增强,其散射截面为非表面等离激子受激辐射放大领结型纳米天线的1.1×104倍,局域电场强度为1×102倍。同时,该领结型纳米天线的表面增强拉曼散射增强因子最大达到1016,足以进行精确的单分子探测;整个纳米天线表面的增强因子也可达到1012,足以应用于单个生物分子的探测。     

反共振空芯光纤中氘气受激拉曼散射实验研究

报道了基于反共振空芯光纤的氘气单程和级联受激拉曼散射实验研究,详细分析了反共振空芯光纤中氘气受激拉曼散射的过程,研究了输出光谱和拉曼谱线功率随氘气压强和泵浦激光功率的变化规律,指出降低气压、采用峰值功率相对较低的泵浦脉冲可以有效抑制转动受激拉曼散射,提高振动受激拉曼散射效率。此外,通过进一步设计、拉制传输带位置合适、带宽较窄的反共振空芯光纤,利用1064 nm脉冲激光泵浦,可以实现高效的氘气一阶振动斯托克斯光(1561 nm)和二阶级联振动斯托克斯光(2925 nm)输出。     

光纤拉曼散射效应及其应用研究

测量了G652光纤和DCF光纤的背向散射光谱，在斯托克斯区观察到一级和二级拉曼背向散射光谱，在反斯托克区观察到一级拉曼背向散射光谱，首次在斯托克斯区和反斯托克区观察到ZX背向散光谱。光纤背向散射效率直接应用于光纤拉曼放大器和分布式光纤拉曼温度传感器系统。讨论了分布式光纤拉曼温度传感器系统工作原理、结构，给出了实验结果。     

CARS显微术的基本原理及其进展

相干反斯托克斯拉曼散射(CARS)以其散射强度高、方向性好、背景干扰小等优点成为分子研究的有力工具,CARS显微镜不仅可以对样品进行光谱研究,还可以对其进行功能性成像．提高了分子分析的信息量。介绍了CARS显微术的理论结果、不同结构及其在生物学领域的应用等。     

多元等离子体共振纳米结构的飞秒激光加工与拉曼检测应用

以多元金属纳米薄膜(金、银)为基底,利用飞秒激光加工技术制备得到多元等离子体纳米结构,并研究了其局域表面等离子体共振效应(Local Surface Plasmon Resonance,LSPR)和表面增强拉曼散射(Surface Enhanced Raman Scattering,SERS)性能。利用时域有限差分(Finite Difference Time Domain,FDTD)软件模拟了不同情况下(单层金膜、金银双层金属薄膜的平面以及阵列结构)的电场分布情况。根据仿真结果,相较于平面金属膜来说,飞秒激光制备的微纳结构阵列附近区域产生电磁场增强,集中在结构边缘处,且其强度变化与预期结果基本保持一致。此外,使用浓度为10-4 M和10-6 M的罗丹明(R6G)溶液进行SERS性能测试。测试的结果表明,单层平面金膜基本没有SERS峰值信号出现,而单层金膜上制备的等离子体纳米结构附近出现峰值信号,双层金属薄膜上制备的等离子体纳米结构展现出更高的SERS峰值信号。多元金属等离子体纳米结构展示出更强的局域表面等离子体共振效应,从而在表面增强拉曼散射、光催化、生物传感等领域具有广泛的应用。     

亚波长金属槽阵列表面电磁场增强

针对表面增强拉曼散射的应用,采用严格耦合波分析方法研究了亚波长金属槽阵列的表面电磁场增强效应。模拟阵列周期和槽深对阵列槽口处电磁场增强的影响,明确了结构内部共振效应对电磁场增强的贡献,分析了亚波长金属槽阵列拉曼散射的平均增强效果及阵列外空间中电磁场增强的有效作用范围。研究表明,在槽内共振效应的影响下,亚波长金属槽阵列在一个周期内的拉曼散射增强因子可达106数量级,并在垂直距离阵列表面1/5波长的范围内可得到明显的电磁场增强,超出该范围增强因子将迅速衰减到1的数量级。数值结果表明阵列表面电磁场增强几乎不受贵金属类型的影响。     

GdVO4晶体的受激拉曼散射

采用熔体提拉法生长出了高质量的a轴和c轴GdVO4单晶。测量了GdVO4晶体的室温透过光谱,结果表明GdVO4晶体的短波透过截止边为338 nm,长波透过截止边大于3000 nm,透过范围覆盖紫外、可见、近红外和部分中红外波段,因此可以在较宽波长范围内实现拉曼激光频移。研究了GdVO4晶体在532 nm和355 nm皮秒激光脉冲抽运下的受激拉曼散射(SRS)。采用腔外单次通过方式,获得了3级斯托克斯线(557.98 nm,586.86 nm,618.92 nm)和1级反斯托克斯线(508.01 nm),得到GdVO4晶体一级斯托克斯拉曼散射的稳态增益系数为26.6±0.2 cm/GW,二级斯托克斯拉曼散射的稳态增益系数为14.0±0.2 cm/GW,受激拉曼散射的整体转换效率达到43%。报道了GdVO4晶体355 nm激发的受激拉曼散射,观察到2级斯托克斯谱线(365.9 nm,378.1 nm),在此条件下测得一级斯托克斯谱线的拉曼增益高达114±9 cm/GW。     

基于COMSOL的柔性表面增强拉曼散射基底研究

为提高表面增强拉曼散射(Surface-enhanced Raman scattering, SERS)基底的性能，采用COMSOL Multiphysics仿真软件通过有限元法对两个相邻的纳米颗粒的模型进行仿真。仿真结果表明，当纳米颗粒半径一定时，增强因子随间距的增大而快速减小；当间距一定时，增强因子随半径的增大而增大，半径达到300 nm后，增强因子趋于稳定，且呈一定的下降趋势。同时，设计并构建了倒圆锥模型的SERS基底，仿真得到其增强因子为2.66×10⁵,相比于倒金字塔模型(增强因子为1.57×10⁵)具有更优异的性能。基于所得到的仿真结果对倒圆锥模型进行优化，银纳米颗粒间距从10 nm依次减小为5 nm,增强因子得到显著提高，极大地提高了表面增强拉曼散射基底的性能。     

太赫兹波段金属光子晶体光纤增强拉曼散射现象的研究

深入探究了金属光子晶体光纤的表面增强拉曼散射现象,建立了时域有限差分法的平板结构的模型,利用观察到的超强透射现象得到了发生拉曼散射的理论依据。金属光子晶体在太赫兹波照射下的表面电磁场增强效果的实验中得到:入射波能量越大,更易激发产生金属光子晶体的表面等离子体共振,可以使金属表面的增强效果得到较大增强;拉曼散射效果在太赫兹波段内十分明显,吸收光谱效果和荧光效应也相对较小,能够显著提高灵敏度和分辨率。     

High enhancement factor of Au nano triangular prism structure for surface enhanced coherent anti-Stokes Raman scattering

Coherent anti-Stokes Raman scattering spectroscopy(CARS) is a well-known detecting tool in biosensing and nonlinear spectroscopy. It can provide a non-invasive alternative without the need for exogenous labels, while the enhancement factor for surface plasmon resonances(SPR) are extensively used to increase the local field close to the oscillators and which can obtain high enhancement. In this work, we investigate the enhancement factor of our structure for surface-enhanced coherent anti-Stokes Raman scattering. The absorption spectrum of the structure has been studied, a wide range of absorption has been realized. The enhancement can be as high as 10¹⁶ over standard CARS. Our design is very useful for improving the enhancement factor of surface-enhanced coherent anti-Stokes Raman scattering.     

自组装法制备团簇Ag纳米结构衬底及其SERS

采用自组装方法,在3-Aminopropyltrimethoxy silane(APS)分子修饰后的玻璃衬底表面,获得了二维Ag纳 米结构衬底。在波长为532nm激光激发下,研究了沉积在衬底表面的 Rhodamine 6G(Rh6G)分子的拉曼光谱特性。结 果表明,制备的二维Ag纳米结构衬底具有强的拉曼增强特性,增强因子可以达到 10⁷ 倍。这说明,在外光场作用下,制备的Ag纳米结构衬底表面能够形成的强局部电磁场分布, 可以有效提升探针分子的光谱辐射效率,从而获得高增强拉曼散射。     

3D Aluminum Hybrid Plasmonic Nanostructures with Large Areas of Dense Hot Spots and Long‐Term Stability

Plasmonic materials possessing dense hot spots with high field enhancement over a large area are highly desirable for ultrasensitive biochemical sensing and efficient solar energy conversion; particularly those based on low‐cost noncoinage metals with high natural abundance are of considerable practical significance. Here, 3D aluminum hybrid nanostructures (3D‐Al‐HNSs) with high density of plasmonic hot spots across a large scale are fabricated via a highly efficient and scalable nonlithographic method, i.e., millisecond‐laser‐direct‐writing in liquid nitrogen. The nanosized alumina interlayer induces intense and dual plasmonic resonance couplings between adjacent Al nanoparticles with bimodal size distribution within each of the hybrid assemblies, leading to remarkably elevated localized electric fields (or hot spots) accessible to the analytes or reactants. The 3D‐stacked nanostructure substantially raises the hot spot density, giving rise to plasmon‐enhanced light harvesting from deep UV to the visible, strong enhancement of Raman signals, and a very low limit of detection outperforming reported Al nanostructures, and even comparable to the noble metals. Combined with the long‐term stability and good reproducibility, the 3D‐Al‐HNSs hold promise as a robust low‐cost plasmonic material for applications in plasmon‐enhanced spectroscopic sensing and light harvesting.     

叠层圆柱台表面等离激元器件的共振特性

基于金属纳米结构增强光与物质的相互作用,调控光学响应是光学前沿研究。金属纳米结构能显著增强电磁场和热点空间位置调控,是表面等离激元器件应用的关键。借鉴衍射光学元件设计思想,文中提出一种简单的多尺度叠层圆柱台（double stacked nanocone,DSC）金属纳米结构,实现近/远场深度调控。在给定激发条件下,DSC纳米结构中腔模与局域表面等离激元模式间产生杂化,实现多尺度级联场增强,远场响应也得到有效调制,且热点能有效地定位到纳米结构的上表面。进一步,提出并研究了掩模重构的纳米加工方法,低成本、可控地制备了DSC纳米结构,工艺控制是三台阶DSC器件特性的关键,实验结果与理论设计一致。     

苯的二级相干反斯托克斯喇曼散射(CARS)

设计了一套光路布置使用受激喇曼散射为相干光源,泵浦光子同受激光子之间混频,观测到苯的相干反斯托克斯喇曼散射共振现象,并获得很强的第二级相干反斯托克斯喇曼线.     

Stimulated Raman Scattering in Nanorod Silicon Carbide Films

When the film is excited by a very low excitation energy, the spontaneous Raman scattering emerges. The intensity of Raman scattering is proportional to the excitation power below the threshold excitation. When the excited power reaches the excitation threshold, the intensity of Stokes light strongly increases. Meanwhile an anti Stokes light at 495 nm and multiple order but small Stokes peaks occur. The intensity of Stokes light is much larger than that of anti Stokes. The full width of half maximum (FWHM) of Stokes peak is reduced from 0.4 nm to less than 0.2 nm, the scattering angle between both Stokes and incident lights becomes less than 1°, and the angle between the Stokes and anti Stokes lights is about 3°. When the exciting power is in excess of the threshold, anti Stokes and multiple Raman scattering peaks reappear. These experiments can be unlimitedly repeated. From this experiment, we can exclude the possibility of spontaneous Raman scattering. It is suggested that the nanorods are a quantum line dimension having a large surface. There will be Raman differential scattering section so long as the nanorod films become very strong scattering media; the surface enhanced Raman scattering will be produced, the nanorod films of SiC will form a strong multiple scattering resonance cavities so as to form the stimulated Raman scattering oscillation.     

Fabrication of a Macroporous Microwell Array for Surface‐Enhanced Raman Scattering

Here, a colloidal templating procedure for generating high‐density arrays of gold macroporous microwells, which act as discrete sites for surface‐enhanced Raman scattering (SERS), is reported. Development of such a novel array with discrete macroporous sites requires multiple fabrication steps. First, selective wet‐chemical etching of the distal face of a coherent optical fiber bundle produces a microwell array. The microwells are then selectively filled with a macroporous structure by electroless template synthesis using self‐assembled nanospheres. The fabricated arrays are structured at both the micrometer and nanometer scale on etched imaging bundles. Confocal Raman microscopy is used to detect a benzenethiol monolayer adsorbed on the macroporous gold and to map the spatial distribution of the SERS signal. The Raman enhancement factor of the modified wells is investigated and an average enhancement factor of 4 × 10⁴ is measured. This demonstrates that such nanostructured wells can enhance the local electromagnetic field and lead to a platform of ordered SERS‐active micrometer‐sized spots defined by the initial shape of the etched optical fibers. Since the fabrication steps keep the initial architecture of the optical fiber bundle, such ordered SERS‐active platforms fabricated onto an imaging waveguide open new applications in remote SERS imaging, plasmonic devices, and integrated electro‐optical sensor arrays.     

具有分形结构Ag纳米衬底的荧光增强效应

利用电化学沉积方法,制备出具有分形结构的Ag纳米荧光增强衬底。实验中,采用532nm连续光激发居于Ag纳米结构衬底表面附近的罗丹明6G(Rh6G)荧光分子,结果表明,具有分形结构的Ag纳米金属衬底对沉积在其表面的Rh6G分子表现出明显的荧光增强效应。根据局域场增强理论对所得实验结果进行分析,经过电化学方法制备出的分形Ag纳米结构,在外电磁场激发下能够形成较强的局域电磁场分布,从而有效地激发Rh6G荧光分子,增强其荧光辐射强度。