杂质对溶胶-凝胶SiO2薄膜激光损伤的影响

 采用溶胶-凝胶法制备了含有吸收性杂质和非吸收性杂质的SiO₂增透膜,采用波长为1 064 nm的激光对其进行了小光斑激光预处理,对比研究了预处理前后的激光损伤差异,研究表明：激光预处理对于洁净的SiO₂薄膜影响不大;含10 μm SiO₂颗粒杂质的样品微透镜效应很明显,容易成为损伤起始的种子,激光预处理后情况有所改善;含有CeO₂颗粒杂质的样品表现出了很强的吸收性质,损伤阈值降低到不足洁净样品的一半。所有样品激光预处理后损伤形貌未发生变化,透光率峰值均有约50 nm的蓝移。     

红细胞显微激光共焦拉曼散射光谱扫描技术研究

采用显微激光共焦拉曼散射光谱扫描系统对活态红细胞进行拉曼光谱(点测定、线扫描、二维扫描)测定及成像的技术与方法进行了研究,并对514 nm激光对红细胞在拉曼扫描中的影响进行了评价。通过扫描前后细胞的拉曼光谱变化和亮场图像变化确定了在不同扫描模式下既可获得较好的拉曼散射信号,又不会影响细胞生命活动与功能的合适扫描参数的设置。对于点扫描模式,样品激光功率是重点调节的参数,一般应小于1.5 mW。对于线扫描模式,照射激光功率和扫描间隔(步进)是要重点关注的参数。小扫描间隔意味着激光能量相对聚集,易对细胞造成损伤;大扫描间隔可以较好地降低激光对细胞的损伤,但是空间分辨率会因此而下降。对于线扫描,建议扫描间隔大于0.5 μm、照射激光功率小于0.7 mW。对于二维扫描,除照射激光功率、扫描间隔需要调节外,其他扫描参数也要作相应调节以降低激光对红细胞的影响,可适当降低样品温度和增加共焦孔径尺寸降低二维扫描过程中激光对红细胞的影响。1.0 μm扫描间隔、0.7 mW的照射激光功率和500 μm共焦孔径,以及样品温度适当调低可得到较好的二维红细胞拉曼图像。对于所有扫描模式,如果得到的红细胞的拉曼信号足够强,也可适当降低曝光积分时间以降低激光对红细胞的影响。实验前进行实验过程的优化对活态细胞的拉曼测试也非常重要。     

Rapid shifted excitation Raman difference spectroscopy with a distributed feedback diode laser emitting at 785 nm

A distributed feedback (DFB) laser diode emitting at 785 nm was tested and applied as a light source for shifted excitation Raman difference spectroscopy (SERDS). Due to the physical properties of the laser diode, it was possible to shift the emission wavelength by 8 cm^-1 (0.5 nm) required for our SERDS measurements by simply changing the injection current. The internal grating ensured single mode operation at both wavelength with the frequency stability of ±0.06 cm^-1 (0.004 nm) required for high resolution Raman spectroscopic applications. The shifted spectra were used for calculating enhanced Raman spectra being obscured by a strong scattering background. A 16 dB (≈38 fold) improvement of the signal-to-background noise S̄/σ_B was demonstrated using blackboard chalk as a sample. The tunable DFB laser is a versatile excitation source for SERDS, which could be used in any dispersive Raman system to subtract fluorescence contributions and scattering background. PACS 82.80.Gk; 42.55.-f; 42.64.Fi     

A new quantitative Raman measurement scheme using Teflon as a novel intensity correction standard as well as the sample container

A novel and reliable quantitative Raman measurement scheme has been proposed for the analyses of ethanol and isopropanol solutions. Teflon tubing was employed as an effective intensity correction standard as well as the sample cell. This allowed for the synchronous collection of the mixed Raman spectrum from the Teflon standard and the sample without any extra optical configuration. A non‐overlapping Teflon band was used as the standard peak to correct the Raman intensity changes resulting from laser power variations. In addition to the use of Teflon tubing,a wide area illumination (WAI) scheme was employed, which made the laser illumination into a circle of 6 mm diameter (area: 28.7 mm²), to cover a wide sample area. The WAI scheme improved the reliability of the Raman measurement by significantly increasing the reproducibility of the sampling owing to a decreased sensitivity to sample placement with respect to the focal plane as well as a wider sample coverage area. The resulting Raman spectra were more reproducible and more representative of the correct sample composition. Overall, a superior prediction performance was achieved using the WAI scheme compared to the conventional Raman collection method. The proposed system has great potential for use in the quantitative analysis of diverse liquid samples with good reproducibility. Copyright © 2006 John Wiley & Sons, Ltd.     

An original approach for Raman spectroscopy analysis of radioactive materials and its application to americium‐containing samples

An approach for Raman measurements of highly radioactive samples is presented here. The innovative part of this approach lies in the fact that no single part of the Raman equipment is in direct contact with the radioactive sample, as the sample is sealed in an alpha‐tight capsule. Raman analysis is effectively performed through the optical‐grade quartz window closing the capsule. This allows performing micro‐Raman measurements on radioactive samples with no limitations on the laser source wavelength, polarisation mode, spectrometer mode and microscope mode (provided the focal length of the microscope objective is greater than the thickness of the quartz window and with sub mg samples). Some example results are shown and discussed. In particular, some spectral features of americium‐containing oxide nuclear fuel specimens are presented. Raman spectra clearly reveal in these specimens the presence of abundant oxygen defects induced in the fcc fluorite lattice by trivalent americium. In order to complete the analysis the Raman spectrum of pure americium dioxide was also measured with a lower energy excitation source compared with previous research. The current results seem to be consistent with the possible occurrence of a photolysis process induced by the Raman laser, resulting in the formation of hyperstoichiometric americium sesquioxide Am₂O_{3 + z}. Such a photolytic process is deemed to be unavoidable when visible lasers are used as excitation sources for the Raman analysis of americium dioxide. © 2015 The Authors Journal of Raman Spectroscopy Published by John Wiley & Sons, Ltd.     

Highly efficient Raman conversion in O2 pumped by a seeded narrow band second-harmonic Nd:YAG laser

The first-Stokes conversion efficiency for a stimulated Raman scattering (SRS) is usually very low in gaseous oxygen media. In 3.0 Mpa O₂, a single longitudinal mode second harmonic Nd:YAG laser pump source gives a typical vibrational first-Stokes conversion efficiency of only 2.5%, In comparison, the accompanying stimulated Brillouin scattering (SBS) attains a reflectivity of 67%. However, by seeding an OPO beam into the Raman cavity, the first-Stokes photon conversion efficiency now attains a peak value of 54%, while the SBS reflectivity reduces to 5% in a 6.1 Mpa 41:59 O₂/ He mixture. This 54% efficiency was obtained for a seeder laser pulse-width less than one half that of pump laser (6.8 ns). A first-Stokes peak power conversion efficiency as high as 88% has been obtained when the pump and seeder pulse peaks coincide. So, we may expect a higher first-Stokes photon conversion efficiency if the seeder pulse-width can be made equal to or larger than that of the pump pulse. On the other hand, the beam quality of the first-Stokes in an O₂/ He mixture excels that of the pump laser for a seeder energy of 5 mJ and pump energy of 50 mJ. However, at pump energies higher than 105 mJ and a pump laser repetition rate of 10 Hz, the thermal defocusing effect worsens the first-Stokes beam quality. This thermal defocusing effect is a result of the Raman heat release and could be eliminated by fast circulating and cooling the Raman gas medium.     

HERAS: A helium jet to prevent damage on works of art in Raman experiments

Raman spectroscopy is often used for non‐destructive analysis of works of art, polymers and biological materials, but in some cases, the laser beam can cause damages on the surface being studied due to the deposited beam energy. When possible, such damage can be prevented by minimizing laser intensity or acquisition time, but this is usually available only on high sensitivity bench‐top spectrometers. Portable Raman spectrometers are commonly not so flexible and an alternative is needed to ensure the safe study of sensitive works of art and other fragile materials. A helium jet aimed directly at the laser spot may prevent this damage from occurring and, in some cases, helps improving the Raman spectra. We designed a simple system (HERAS, Helium Raman System) consisting of a pinhole collimator, coupled to a helium line and a gas mass flux control and tested it on pyroxylin, vermilion and ochre paint references and pigment samples, using a 785 nm portable Raman spectrometer at various laser powers. Experimental conditions slightly differ for each sample, but small burns on the surface were avoided in all cases and only some ablation was observed on the most sensitive materials. The use of this coupled system allows the non‐destructive application of Raman to a wider variety of materials, while the technique remains portable. This setup may be used in bench‐top apparatus as well. Copyright © 2013 John Wiley & Sons, Ltd.     

A comparative performance evaluation of micro-Raman spectrograph using holographic notch filter and dielectric filter

An indigenously designed and developed micro-Raman spectrograph, consisting of a diode-pumped solid-state green laser for the excitation of Raman scattering, a Raman imaging microscope, CCD as a detector and a notch filter, has been extensively studied to evaluate its performance. A dielectric edge filter (having 27 alternate layers of SiO₂ and TiO₂) and a holographic notch filter (Oriel make) have been used to block the Rayleigh scattered light from the sample to the entrance slit of the spectrograph. Holographic notch filter is found to be able to record the Raman shifts below 700 cm⁻¹ conveniently whereas dielectric edge filter (27 layers) has enabled the spectrograph to record the Raman spectra very efficiently after a wave-number shift of 700 cm⁻¹. It has also been observed that the instrument using the edge filter provides a peculiar spectrum consisting of three spectral lines having Raman shifts as 569, 1328 and 1393 cm⁻¹ in the Raman spectrum of a weakly scattering sample with large reflectivity. Similarly, a spectrum consisting of multiple lines has been observed when the instrument is being operated using a holographic notch filter. These spectral lines are not observed in the case of liquid samples such as benzene, carbon tetrachloride, ethanol, diethyl ether etc. The origin of these peculiar spectral lines has been briefly discussed in the paper. Additionally, a major motivation for this work is to utilize the results for the selection of an appropriate filter depending on the type of the sample, i.e. weakly scattered and highly reflecting sample or highly scattered and low reflecting sample.     

Efficient cw sodium dimer Raman laser operation in a high-temperature sapphire cell

cw Raman lasing of Na₂ molecules generated in a heated, sealed-off, all-sapphire cell is demonstrated. Being not damaged by highly corrosive alkaline vapours, this type of cell enables operation without buffer gas in contrast to the normal heatpipe operation of these lasers. This allows us to study Raman lasers in alkaline vapours in new regimes and under ideal conditions. With an argon ion pump laser at 488 nm, Raman laser operation at 525 nm with more than 10% efficiency and thresholds below 0.2 mW for a cell without buffer gas (length 9 cm) have been obtained so far. The low thresholds, being a factor of 10 less than for comparable heatpipe operation, gives us the chance to use low-power diode lasers as pump sources and to realize compact reliable Raman laser systems. Received: 17 May 1999 / Published online: 25 August 1999     

Irradiation effects in CaF2 probed by Raman scattering

The formation conditions and dynamics of Ca colloids and point defects that appear in irradiated single crystals of CaF₂ were investigated by Raman spectroscopy. The intensity changes in the Raman spectra because of the presence of different concentrations of point defects and Ca colloids that emerged in CaF₂ after irradiation with 2.2 GeV Au ions were used to study their distribution and stability under illumination with three laser wavelengths (473, 532 and 633 nm) at different output powers (2 to 200 mW). A damage saturation at a fluence of 6 × 10¹¹ ion cm⁻² was observed. The dependence of the spectral changes on the ion fluence can be described by a core/halo damage cross‐section model. A radius of 13–18 nm was obtained for the outer (halo) cylinder, in agreement with previous swelling studies. Illuminations of irradiated samples with blue (473 nm) and green (532 nm) lasers were found to be extremely efficient in bleaching the samples, while illumination with a red (633 nm) laser did not lead to a sample recovery. This indicates that the bleaching process is governed by recombination of point defects that have to overcome an energy barrier. Typical time constants for the processes involved are presented. Copyright © 2016 John Wiley & Sons, Ltd.     

Synthesis of hafnium tungstate by a CO2 laser and its microstructure and Raman spectroscopic study

Densely packed hafnium tungstate blocks were synthesized by rapid solidification with a CO₂ laser. It is shown that the optimum synthesis conditions for HfW₂O₈ are around 700 W laser power and 1 mm/s scan speed. Scanning electron microscopy (SEM) observation shows that the blocks consist of oriented nano‐threads/rods that grew horizontally on the surface region and vertically in the interior. The orientations of the nanostructures are governed by the heat transfer directions on the surface and in the interior. Raman spectroscopic and X‐ray diffraction studies show that the samples solidified in the cubic structure with minor contents of the orthorhombic phase. This is explained by a compressive stress induced during the rapid solidification process due to a sudden drop of temperature of the molten pool to the ambient. The stress is estimated to be about 0.6 GPa by comparison with high‐pressure Raman study. Some specific Raman bands appear in the samples synthesized with the laser synthetic route but not in the sample by solid‐state reaction. Copyright © 2008 John Wiley & Sons, Ltd.     

无固体窗口拉曼池的受激拉曼散射实验研究

在高功率激光作用下,拉曼池窗口及其膜层很容易被激光损坏。设计了一种新型的无固体窗口的拉曼池,利用安装在拉曼池两端的两个快门来取代通常的固体窗口,拉曼池内充有与环境气体密度接近的混合气体,在快门打开后的一定时间内,气体扩散不占主导地位,从而实现拉曼转换。研究了窗口气体流动对受激拉曼散射的影响。     

Laser-heating diamond anvil cell studies of simple molecular systems at high pressures and temperatures

We report the application of new laser-heating techniques and sample preparation procedures for simple molecular materials (diatomic molecules and water) under high pressure in the diamond anvil cell (DAC). Both continuous and pulsed laser heating was employed. We probed the materials using Raman spectroscopy and also by analyzing the time evolution of the temperature of the metallic coupler that is used to absorb laser radiation and heat the sample. Raman measurements of H₂, D₂, N₂, H₂O and O₂ show a broadening of intramolecular vibrations at high P−T conditions, indicating a decreasing molecular lifetime, and hence suggest an increasing molecular dissociation. In diatomic molecules the intramolecular bonding can be further probed by observations of sidebands corresponding to vibrational transitions from excited states; the energies of these sidebands imply intramolecular potentials that become increasingly less anharmonic as pressure is increased. We also show that the pulsed heating technique combined with instantaneous radiative temperature measurements provides a useful tool for studies of thermochemical properties and phase transformation boundaries.     

Parameter identification and synchronization between uncertain stimulated Raman scattering and NH3 laser

The parameter identifiers and synchronization controllers are designed based on stability theory in order to realize the synchronization of two chaotic systems with diverse structures and the parameter identification of the uncertain system. The stimulated Raman scattering and NH₃ laser are taken as examples. The simulation results show that the global synchronization between the uncertain stimulated Raman scattering and the NH₃ laser can be achieved, and all the parameters in the stimulated Raman scattering system can be identified simultaneously. The method is proved effective and feasible.     

Laser-induced decomposition of sodium azide

The decomposition of sodium azide, NaN₃, has been studied using a pulsed carbon dioxide laser. Chemiluminescence associated with the decomposition has been measured with and, without, the azide surface in the detector field of view. Near the decomposition threshold, emission has been observed in the wings of the Na 3p → 3s transition at 589 nm that has not been observed in previous azide decomposition experiments. This emission may be a result of surface reactions. Raman and visible absorption spectra have been obtained for the irradiated material; a new, as yet unidentified, band was observed in the Raman spectrum.     

Ellipsometry of GeO<Subscript>2</Subscript> films with Ge nanoclusters: Influence of the quantum-size effect on refractive index

Using the methods of scanning and spectral laser ellipsometry and Raman scattering spectroscopy, GeO₂ films containing Ge nanoclusters with a Ge/GeO₂ mole ratio of 1: 1 are studied. A substantial difference is found between the experimental spectral dependence of the complex permittivity of the films and the one calculated for the effective medium in the Bruggeman model. The distinction can be qualitatively explained by the influence of the quantum-size effect. With the use of theoretical models for quantitative analysis, this approach will make it possible to determine the phase composition and dimensions of the nanoclusters of germanium in a contactless way without destructing the film.     

L-Band Multi-Wavelength Brillouin–Raman Fiber Laser with 20-GHz Channel Spacing

Abstract

A tunable multi-wavelength L-band Brillouin–Raman fiber laser with a 20-GHz channel spacing utilizing bidirectional ring cavity is proposed and experimentally investigated. The laser employs a co-pumped dispersion compensating fiber as a gain medium for both Brillouin and Raman gains. With a Raman pump of 425 mW, the laser system can generate up to 12 double-spaced Brillouin Stokes signals. This simple laser configuration provides stable Brillouin Stokes signals in the absence of self-lasing cavity modes with a tuning range exceeding 35 nm without using any filtering mechanism. The Stokes signals have more than 20 dB of optical signal-to-noise ratio.     

Linear wave-vector dependence of an optical phonon frequency in Bi12GeO20 in the vicinity of the Brillouin zone center

A Raman spectroscopic study of a zone center optical phonon of Bi₁₂GeO₂₀ which exhibits simultaneously a LO-TO and a linear wave-vector dependent splitting is presented. These are separated experimentally by studying the Raman line with a piezoelectrically scanned Fabry-Perot interferometer and the sample with and without an applied uniaxial stress.     

Resonant Raman studies of surface composition and structural ordering in laser-irradiated Hg1-xCdxTe

1-x Cd_xTe for x=0.165 and x=0.18. The annealing was performed in air with a Nd:YAG laser tuned to the first harmonic. A pulse duration of 72 ns and irradiation energy densities of 270 and 400 mJ/cm² were used. Information on both the structural ordering and the alloy composition in irradiated Hg_1-xCd_xTe was obtained by resonance Raman spectroscopy with laser photon energies of between 2.41 and 2.54 eV. The presented Raman spectra from annealed samples indicate structural disorder and a decrease in the degree of alloying as a result of Hg outdiffusion and segregation caused by laser-induced nonequilibrium melting and solidification. Moreover, a shift of the maximum resonant enhancement for the TO₂, LO₂, A, and LO₁&TO₁ modes in the case of a Hg_0.82Cd_0.18Te sample, annealed by 400 mJ/cm² laser pulse, to higher photon energy points to an increase in the composition from x=0.18 to x?0.3. Received: 14 July 1997/Accepted: 10 October 1997     

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.