Observation of sharp resonances in the spontaneous Raman spectrum of a single optically levitated microdroplet

Sharp resonances have been observed in the spontaneous Raman spectra of single, optically levitated microdroplets. The droplets, 10 to 35 μm in diameter, were suspended by a CW argon laser beam which also served as the Raman excitation source. Experiments with dioctyl phthalate (DOP) and silicone oil confirmed that all Raman bands present in the bulk liquid spectra were also observable in the levitated droplet spectra, in agreement with previous micro-Raman studies of droplets on substrates. However, superimposed on the spectra of the levitated droplets was a series of sharp features not present in the bulk liquid spectra. Time-resolved experiments with growing DOP droplets showed that the sharp Raman features have the same origin as the elastic light scattering and flourescence resonances observed in previous studies of microspheres and fibers.     

Optical phase change in bismuth through structural distortions induced by laser irradiation

ABSTRACT

Semimetal bismuth (Bi) is known to possess a wide range of peculiar properties, owing to its unique electronic band structure. Its electronic band can easily be distorted by structural changes, and thereby undergo transitions between semimetal to either semiconductor or metal states. Utilising a focused laser beam, one can easily introduce structural defects, along with phase changes, oxidation, and morphological modifications. Confocal Raman microscopy indicated that the as-fabricated Bi droplets inhibit the Raman signal from the underlying silicon (Si) substrate. After a laser flash heating step, the intensity of Si optical phonons was strongly enhanced at the positions of Bi droplets, and exceeding the intensity from the bare Si substrate. Thus, such laser irradiating step on the Bi droplets induces an optical phase change. The optical phase change was detected as going from inhibition to strong enhancement of the underlying Si substrate Raman signal. From the observed Bi optical phonon modes (E_g and A_1g), alterations in the Raman peaks due to laser exposure indicated that the ordered crystallinity in pristine Bi droplets became deteriorated. The effects of atomic displacements and loss of structural order in Bi droplets impacts its dielectric response. The observed Si Raman signal enhancement is similar to the surface-enhanced Raman scattering effect typically known for noble metals.     

光纤维中的喇曼混频

我们在656厘米^-1到1343厘米^-1的频率范围研究了光纤维的调谐喇曼混频(RM)效应。在实验中观察到下列现象:相干反斯托克斯喇曼散射(CARS)的大小与逆喇曼吸收(VRA)的大小成反比;RM对受激喇曼散射(SRS)的强度分布有强烈影响。除了观测到相干斯托克斯(CSRS)和CARS辐射,还观测到二级相干斯托克斯(SOCSRS)和相干反斯托克斯(SOCARS)辐射。对实验结果进行了讨论。 关键词：     

苏氨酸的太赫兹及拉曼光谱研究

采用太赫兹时域光谱和拉曼光谱法对L-苏氨酸多晶粉末进行测试研究,获得了样品在0.2—2.8 THz（6.7—93.2 cm^-1）波段的特征吸收和10—4000 cm^－1波段的拉曼散射谱;分别在6.7—93.2 cm^－1和400—4000 cm^－1两个波段进行了吸收光谱与拉曼散射光谱的对比,根据晶胞分子所属的空间群,对隶属于分子的极性和非极性振动模式（A, B₁, 关键词： 太赫兹光谱 拉曼散射 氨基酸     

Raman characterization of high-pressure phase transition in AlN nanowires

High-pressure phase transition of AlN nanowires was investigated in the range of 0-33.1 GPa by in situ Raman spectrum method in diamond anvil cell (DAC). The A1 (LO) vibration mode exhibits considerably asymmetry and broadening, indicating the occurrence of wurtzite-to-rocksalt phase transition. The Raman signal of high-pressure phase can be assigned to the disorder activated Raman scattering of rocksalt AlN. After fully releasing pressure, the Raman characterization of high-pressure phase was quenched. According to the pressure dependence of phonon frequency of AlN nanowires, the difference of transiton path between AlN nanowires and bulk materials was discussed and the mode Grüneisen parameters were determined.     

L-天冬氨酸在银胶体中吸附状态的表面增强拉曼光谱研究

利用表面增强拉曼光谱 (Surface EnhancedRamanScattering,SERS)研究了L 天冬氨酸在银溶胶体中的吸附状态及其浓度变化对表面增强拉曼散射效应的影响 ,并探讨了L 天冬氨酸在银溶胶表面的吸附作用特点和规律。实验结果表明 ,L 天冬氨酸在银溶胶中有明显的SERS信号 ,经过分析表明 ,该化合物能够吸附在银表面 ,这种吸附是通过羧基和氨基中的氮原子与银结合来实现的 ,L 天冬氨酸分子中带有负电荷的羧基和氨基中带有孤对电子的氮原子都能与银原子配位 ,其中羧基在银表面的增强为电荷转移机制增强 ,具有化学吸附的特征 ;氨基在银表面的增强为电磁场增强机制 ,为物理吸附。而且SERS强度随着L 天冬氨酸浓度的变化而改变 ,当其浓度为 10 - 3mol·L- 1 时增强效果较好 ,当浓度降低 ,增强作用也逐步变弱     

Determination of the LO phonon energy by using electronic and optical methods in AlGaN/GaN

The longitudinal optical (LO) phonon energy in AlGaN/GaN heterostructures is determined from temperature-dependent Hall effect measurements and also from Infrared (IR) spectroscopy and Raman spectroscopy. The Hall effect measurements on AlGaN/GaN heterostructures grown by MOCVD have been carried out as a function of temperature in the range 1.8-275 K at a fixed magnetic field. The IR and Raman spectroscopy measurements have been carried out at room temperature. The experimental data for the temperature dependence of the Hall mobility were compared with the calculated electron mobility. In the calculations of electron mobility, polar optical phonon scattering, ionized impurity scattering, background impurity scattering, interface roughness, piezoelectric scattering, acoustic phonon scattering and dislocation scattering were taken into account at all temperatures. The result is that at low temperatures interface roughness scattering is the dominant scattering mechanism and at high temperatures polar optical phonon scattering is dominant.     

A practical method for diameter,number density and material characterization of 40–90 µm size droplets by stimulated Raman scattering

We demonstrate that the technique of Stimulated Raman Scattering (SRS) is a practical method for the simultaneous characterization of diameter, number density and constituent material of microsize droplets. The method is applicable to all Raman active materials and to droplets with a diameter of at least 8 µm. Our experimental study was focused on water and ethanol monodisperse droplets in the diameter range of 40–90 µm. Results of a single laser pulse and multiple pulses are analyzed, indicating that the SRS method can diagnose droplets of mixed liquids and ensembles of polydisperse droplets.     

水体的温度变化对测定溶解有机物浓度的影响

用激光诱导荧光(LIF)方法研究了水体的温度变化对溶解有机物(DOM)发射荧光强度的影响。随着温度的增加,DOM的荧光强度和水的拉曼散射强度不断降低。在20～75 ℃范围之内,对归一化荧光强度与温度关系曲线进行线性拟合,计算出归一化荧光强度随温度升高的变化梯度平均值为-5.24×10-4 ℃-1,根据归一化荧光强度与浓度的关系,给出了所测DOM的浓度随着温度升高的平均下降速率为-3.45×10-3 (mg·L-1)·℃-1。因此,在这一温度范围内测量时,假设归一化荧光强度不变,则温度变化将引起DOM浓度最大为8.45%的相对变化。     

Spatially resolved Raman scattering for multi-species and temperature analysis in technically applied combustion systems: Spray flame and four-cylinder in-line engine

Spatially resolved Raman scattering is used to measure the single shot stoichiometry before ignition inside a realistic internal combustion engine with high single shot precision of l%–4% (depending on the extent of spatial averaging). The high precision results from the simultaneous detection of fuel and N₂ (O₂), which yields stoichiometry via a relative measurement. The cycle-to-cycle fluctuations of stoichiometry are clearly resolved. The feasibility of averaged spatially resolved simultaneous multi-species detection is demonstrated in a commercial oil-burning furnace as well. The limited precision that is usually obtained in Raman scattering by interfering emissions is highly improved using the fact that the interfering emission is unpolarized whereas Raman scattering is highly polarized. Therefore, Raman measurements provided good signal-to-noise ratios in the spray flame even in the area where fuel droplets occur and during combustion in the engine. The optical multichannel analyzer yields one-dimensional spatial resolution, and offers the capability to easily combine Raman scattering with Rayleigh scattering and laser-induced fluorescence detection of minority species.     

Microcrystalline Diamond Powders As Promising Objects for Generation of Multifrequency Stimulated Raman Scattering

Optics and Spectroscopy - Regular trends of Raman scattering in microcrystalline diamond powders as a function of size of the diamond microcavities are investigated in the range of the latter...     

以Y/Ni为催化剂制备的单壁碳纳米管的拉曼光谱研究

采用电弧放电法以Y/Ni为催化制备了单壁碳纳米管（SWNTs），对样品进行了扫描电镜、透射电镜和拉曼光谱的研究。所制备的样品中单壁碳纳米管的含量较高。对单壁碳纳米管的共振拉曼散射增强效应进行了观察，随激光波长的不同，单壁碳纳米管的拉曼光谱也随之变化，尤其是低频区径向呼吸模的变化比较明显。利用布里渊区折叠法计算了单壁碳纳米管的电子态密度曲线，根据SWNTs电子态密度尖峰之间的能量差、管子的直径和呼吸模频率建立了一个图表，并对SWNTs的呼吸模进行了归属。分析结果表明：样品中单壁碳纳米管的直径分布在0.79-1.76nm范围，金属管和半导体管均存在，并且直径在1.45nm附近的碳管居多。     

Surface acoustic phonon modes of Ge nanocrystals embedded in SiO2

Ge nanocrystals (NCs) embedded in SiO₂ are synthesized by ion implantation, and the surface vibrational modes of the Ge NCs are investigated using the low-frequency Raman scattering (LFRS) technique. LFRS studies show distinct low-frequency Raman modes in the range 6.5-21.2 cm⁻¹ for the Ge NCs depending on the implant dose and annealing temperature. These low-frequency Raman modes are attributed to the confined surface acoustic phonon modes of Ge NCs with (0,0) spheroidal mode and (0,3) torsional modes. Our results are in excellent agreement with the recent theoretical predictions of surface vibrational modes in Ge NCs.     

反斯托克斯拉曼光谱在BaTiO_3铁电相变研究中的应用

从理论上讨论了一阶和二阶斯托克斯与反斯托克斯拉曼散射截面的温度依赖关系;在２９３Ｋ至４０１Ｋ的温度范围内,测量了ＢａＴｉＯ３单晶斯托克斯和反斯托克斯过程的偏振拉曼光谱;通过对ＢａＴｉＯ３单晶斯托克斯和反斯托克斯拉曼光谱的综合分析,证实在Ｘ（ＺＺ）Ｙ几何配置下测量到的位于２７５和５１４ｃｍ－１处的强峰为一阶拉曼光谱。此结果支持了ＢａＴｉＯ３铁电相变机制的有序—无序模型。     

非晶La_(1-x)Nd_xP_5O_(14)的拉曼散射研究

本文利用拉曼散射对非晶 La_(1-X)Nd_XP_5O_(14)及其晶化过程进行了研究。拉曼散射表明在非晶La_(1-X)Nd_XP_5O_(14)中仍保留着晶态 La_(1-X)Nd_XP_5O_(14)中具有的 PO_4~(3-)四面体结构单元。非晶La_(1-X)Nd_XP_5O_4在不同温度下晶化,其拉曼谱线的频率不同,这一现象可用应力模型给予解释。     

0.67 PbMg1/3Nb2/3O3-0.33 PbTiO3单晶中软模模式指认

应用显微拉曼技术对弛豫型铁电体0.67PbMg1/3Nb2/3O3-0.33PbTiO3(0.67PMN-0.33PT)的偏振拉曼光谱随温度变化的研究表明,在-196到600°C温度范围内0.67PMN-0.33PT存在两次相变:三方到四方(R-T)相变和四方到立方(T-C)相变。R-T相变的特征是106cm-1软模(-196°C时)随温度的升高而湮没到80cm-1"静态"模式中。依照群论分析,0.67PMN-0.33PT的80cm-1和106cm-1(-196℃时)两个模式分别为E(1TO)和A1(1TO)模。文章对三方相的对称结构(C3v点群)在背向散射配置下不同偏振方向的拉曼散射效率进行了计算。计算结果表明晶体中的A1(1TO)和E(1TO)模式能够通过使用不同的散射配置进行识别。理论计算和实验结果相比较得到了很好的吻合。     

以非晶碳作硅基红外增透膜的实验研究

在室温下，用激光烧蚀石墨靶方法在单晶硅衬底表面沉积了不同厚度的非晶碳膜。对膜进行了表面形貌观察，测试并分析了膜的拉曼散射光谱和傅里叶变换红外光谱。发现膜同晶石墨杂质较少，观察到1200cm^-1附近的非晶金刚石拉曼峰，膜层在红外的光透过率高，在硅衬底上适宜于制作波长短于8μm的红外增透膜。     

钴的表面增强拉曼散射中的电磁增强因子计算

本文初步探讨了钴电极的表面增强拉曼散射机理。采用二维阵列理论模型在 0 .5～ 4.0eV的光子能量范围对钴纳米椭球阵列的表面增强拉曼散射 (SERS)现象进行了理论分析。有关计算表明 ,经过合适的表面粗糙化的钴金属电极能产生较弱的表面增强效应 (SERS增强因子约 1 0 2 ～ 1 0 4 ) ,制备出具有高纵横比的纳米粒子阵列是得到钴体系较大的SERS增强因子的关键     

Energy characteristics of photothermal vibrational instability at stimulated Raman and Mandelstam-Brillouin scattering in aerosol droplets

The threshold intensity and the combination frequencies for photothermal vibrational instability in high-Q aqueous aerosol droplets in the two-mode regime have been calculated. The selection rules for coupling electromagnetic and temperature modes in a droplet are obtained. A comparative analysis of the threshold excitation intensities of photothermal vibrational instability, stimulated Mandelstam-Brillouin scattering, and stimulated Raman scattering in droplets is performed. It is shown that photothermal vibrational instability in the two-mode regime can be developed at a pump intensity of about 10⁴ W/cm² for droplets with radii of 2–20 μm for a pump wavelength of 0.532 μm. A method of remote measurement of the microphysical droplet parameters from the additional periodic temperature shift of droplet eigenfrequencies in the spectrum of stimulated Raman scattering and lasing is proposed.     

基于人造金刚石晶体的拉曼激光器研究进展

受激拉曼散射是一种重要的非线性光学频率变换技术,在拓展激光波段方面有十分广泛的应用前景。因此,寻找具有优良光学性质的拉曼介质,提高拉曼激光器性能,具有重要的研究价值。相比于传统的固体拉曼晶体,人造金刚石晶体具有拉曼增益系数大、拉曼频移大、导热率高和透过性好等显著优点,基于人造金刚石晶体的拉曼激光器能够获得更高的输出功率和转换效率。本文简要介绍了化学气相沉积法(CVD)制备的金刚石晶体的光学性质和热学特性,总结了基于人造金刚石晶体的拉曼激光器在紫外波段、可见光波段及红外波段的研究现状,并对其发展进行了展望。