Non‐degenerate second‐order scattering and difference combination bands in infrared‐pump/anti‐Stokes resonance Raman‐probe experiments

Non‐degenerate second‐order scattering due to interaction of infrared and ultraviolet pulses is observed in picosecond infrared‐pump/anti‐Stokes Raman‐probe experiments under electronic resonance conditions. We detected resonance hyper‐Rayleigh scattering at the sum frequency of the pulses as well as the corresponding frequency‐down‐shifted resonance hyper‐Raman lines. Nearly coinciding resonance hyper‐Raman and one‐photon resonance Raman spectra indicate conditions of A‐term resonance Raman scattering. Second‐order scattering is distinguished from transient anti‐Stokes Raman scattering of v = 1 to v = 0 transitions and v = 1 to v′ = 1 combination transitions by taking into account their different spectral and temporal behaviour. Separating these processes is essential for a proper analysis of transient vibrational populations. Copyright © 2007 John Wiley & Sons, Ltd.     

双折射光纤受激拉曼散射偏光特性的实验研究

对椭圆芯光纤受激拉曼散射偏光特性进行了系统的实验研究。实验巾观察到8级斯托克斯线和2级反斯托克斯线,对不同偏振态的抽运光激励下各级斯托克斯线的偏振特性、拉曼频移等参量进行了分析,并给出了经验公式。其结果与实验数据符合良好。实验表明,双折射光纤受激拉曼谱的各级斯托克斯线的偏振状态不但与拉曼介质有关还与抽运光的偏振态有关,入射抽运光偏振态对低阶次的斯托克斯线拉曼频移的影响较小,而对高级斯托克斯线拉曼频移影响较大。     

Glass formation and Raman spectra of CaO–SiO2 glasses towards the orthosilicate limit

A series of silicate glasses formed in the binary system (1-X)CaO-XSiO₂with silica mole fractions X ranging from 0.61to 0.38have been prepared using container-less aerodynamic levitation techniques and CO₂-laser heating. Glasses with X<0.45were prepared for the first time but, no glass formation was possible at compositions X<0.38. Ambient temperature polarized and depolarized Raman spectra were measured for all these glasses. Qⁱ-speciation analysis of the isotropic Raman spectra shows that near X∼0.38the predominant structures present are the SiO₄⁴⁻ tetrahedra and the single bridged Q¹species. Oxygen bridging was present at all compositions studied while at X<0.45 small amounts of free oxygen anions was present. The data are compared with the resent NMR measurements obtained with the same glass samples used in the present study. Stokes and anti-Stokes Raman spectra were measured in low frequencies revealing the Boson peak (BP) at ∼50 and ∼70 cm⁻¹ for the corresponding polarized and depolarized configurations. On the Stokes side the BP frequencies exhibit a fictional shift due to contributions from the low frequency vibrational modes of the glass.     

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。     

From anti‐Stokes photoluminescence to resonant Raman scattering in GaN single crystals and GaN‐based heterostructures

The progress on anti‐Stokes photoluminescence and Stokes and anti‐Stokes Raman scattering in GaN single crystals and GaN/AlN heterostructures is reviewed. Anti‐Stokes photoluminescence investigated in the past was primarily attributed to two‐photon absorption, three‐photon absorption, and phonon‐assisted absorption. On the other hand, anti‐Stokes Raman scattering was used to determine electron‐phonon scattering time and decay time constant for longitudinal‐optical phonons. In a typical high electron mobility transistor based on GaN/AlN heterostructures, strong resonances were reached for first‐order and second‐order Raman scattering processes. Therefore, both Stokes and anti‐Stokes Raman intensities were dramatically enhanced. The feasibility of laser cooling of a nitride structure has been demonstrated. Anti‐Stokes photoluminescence and Raman scattering have potential applications in upconversion lasers and laser cooling of nitride ultrafast electronic and optoelectronic devices.     

Anti‐Stokes Raman spectroscopy as a method to identify the metallic and semiconducting configurations of double‐walled carbon nanotubes

Although Raman spectra reveal, as a signature of double‐walled carbon nanotubes (DWCNTs), two radial breathing mode (RBM) lines associated with the inner and outer tubes, the specification of their nature as metallic or semiconducting remains a topic for debate. Investigating the spectral range of the RBM lines, we present a new procedure of the indexing of the semiconducting or metallic nature of the inner and outer shell that forms the DWCNT. The procedure exploits the difference between the intensities of recorded anti‐Stokes Raman spectrum and the anti‐Stokes spectrum calculated by applying the Boltzmann formulae to the recorded Stokes spectrum. The results indicate that the two spectra do not coincide with what should happen in a normal Raman process, namely, that there are RBM lines of the same intensity in both spectra, as well as RBM lines of higher intensity that are observed in the calculated spectrum. This discrepancy results from the surface‐enhanced Raman scattering mechanism that operates differently on metallic or semiconducting nanotubes. In this context, the analysis of the RBM spectrum can reveal pairs of lines associated with the inner/outer shell structure of DWCNT, and when the intensities between the recorded and calculated spectra coincide, the nanotube is metallic; otherwise, the nanotube is semiconducting. Copyright © 2014 John Wiley & Sons, Ltd.     

Thermal conductivity of GexSb(As)ySe100‐x‐y glasses measured by Raman scattering spectra

We systematically measured thermal conductivity of Ge_xSb(As)₁₀Se_90−x, Ge_xSb₁₅Se_85−x, and Ge_xSb(As)₂₀Se_80−x chalcogenide glasses by measuring their Stokes and anti‐Stokes Raman scattering spectra and estimating the temperature raised by laser irradiation via the ratio of Stoke and anti‐Stokes scattering cross‐section. We aimed at demonstrating the viability of Raman scattering method for thermal conductivity measurements, and understanding the role of chemical composition in determining thermal conductivity of the chalcogenide glasses. We found that, while the values of the thermal conductivity measured in the paper are in a range from ~0.078 to 1.120 Wm^‐1K^‐1 that are in agreement with those reported data in the literatures, thermal conductivity increases before it reaches a maximum at the glass with chemically stoichiometric composition, and then decreases with increasing Ge content. We ascribed the threshold behavior of the thermal conductivity to the demixing of the structural units like GeSe₂, As₂Se₃ and Sb₂Se₃ from the main glass network. The present study demonstrated that Raman scattering method is simple and easy to measure thermal conductivity of the material. Copyright © 2014 John Wiley & Sons, Ltd.     

单模双折射光纤中的增益

在双折射光纤中,根据受激拉曼散射和参量放大共同作用下的斯托克斯波和反斯托克斯波所满足的耦合模方程,考虑输入泵浦波是线偏振光,推导出了与泵浦波偏振方向垂直的的斯托克斯波和反斯托克斯波的增益系数;研究了双折射色散缓变光纤中,斯托克斯波和反斯托克斯波增益随相关参量的变化关系。结果表明,与泵浦波偏振方向垂直的斯托克斯波和反斯托克斯波增益的变化趋势是完全相同和对称的;同时表明,通过改变失配系数 ,在适当的传输位置,可以实现对斯托克斯波和反斯托克斯波有选择性的输出,以达到输出频率转换的目的。     

Spectrally dispersed femtosecond CARS investigation of vibrational characteristics in ethanol

Spectrally dispersed femtosecond time‐resolved coherent anti‐Stokes Raman spectroscopy is applied to study the ultrafast vibrational dynamics in ethanol at room temperature. The anti‐Stokes intensities were monitored as a function of delay time and wavenumber. By simply changing the timing of the laser pulses, the vibrational dynamics between the excited Raman transitions in ethanol molecules can be tracked and detected. Copyright © 2014 John Wiley & Sons, Ltd.     

Joint Raman spectroscopic and quantum chemical analysis of the vibrational features of Cs2RuO4

The Raman spectroscopic characterization of the orthorhombic phase of Cs₂RuO₄ was carried out by means of group theory and quantum chemical analysis. Multiple models based on ruthenate (VI+) tetrahedra were tested, and characterization of all the active Raman modes was achieved. A comparison of Raman spectra of Cs₂RuO₄, Cs₂MoO₄, and Cs₂WO₄ was also performed. Raman laser heating induced a phase transition from an ordered to a disordered structure. The temperature‐phase transition was calculated from the anti‐Stokes/Stokes ratio and compared with the ones measured at macroscopic scale. The phase transition is connected with tilting and/or rotations of RuO₄ tetrahedra, which lead to a disorder at the RuO₄ sites. © 2015 The Authors. Journal of Raman Spectroscopy published by John Wiley & Sons Ltd.     

LDS751染料的受激喇曼散射

报道了用532nm激光抽运LDS751染料产生720—780nm可调谐染料激光输出的同时,观察到喇曼频移为102和45cm-1的反斯托克斯线,前者谱线较强,后者较弱.与这两条强线对应的斯托克斯线未能观察到.另外,还观察到喇曼频移为34cm-1的一级和二级斯托克斯线与反斯托克斯线 关键词： LDS751染料 受激喇曼散射 喇曼位移 斯托克斯线 反斯托克斯线     

Background removal from polarized Raman spectra of tooth enamel using the wavelet transform

A wavelet transformation method is introduced to remove the large fluorescence background from polarized Raman spectra of stained tooth enamel. This method exploits the wavelet multiresolution decomposition where the experimental Raman spectrum is decomposed into signals with different frequency components, and where the lowest frequency background and highest frequency noise are removed. This method is optimized using a simulated collection of parallel‐polarized and cross‐polarized Raman spectra of the enamel and then applied to a set of experimental data. The results show that the wavelet transform technique can extract the pure spectra from background and noise, with the depolarization ratio used to discriminate between early dental caries and sound enamel preserved. Copyright © 2010 Crown in the right of Canada. Published by John Wiley & Sons, Ltd.     

超短超强激光与气体靶相互作用中的背向受激Raman散射

 实验诊断测量了超短超强激光与气体靶相互作用产生的背向受激Raman散射,在实验条件下呈现强耦合模式,背向受激Raman散射出现非线性Stokes多峰伴线结构,峰值的频率间隔小于等离子体波的频率,可以大致地推断出激光打靶过程中产生的等离子体密度偏低,其结果与等离子体强耦合理论计算结果一致。     

若丹明B荧光增强二硫化碳高阶受激喇曼散射

 利用若丹明B乙醇溶液的荧光改变了二硫化碳的一至三阶Stokes喇曼谱线的强度分布,选择性地增强了三阶Stokes喇曼谱线。在泵浦功率密度为~560MW^.cm^-2时,对染料摩尔浓度分别为~10^-5、cm^-5散射池和~10^-4、1cm散射池进行实验,观察到二硫化碳的三阶Stokes喇曼谱线与染料激光形成的共振增强现象及、二阶Stokes喇曼谱线的部分或完全耗尽。     

Interference spectroscopy with coherent anti‐Stokes Raman scattering of noisy broadband pulses

We propose a new technique for comparing two Raman active samples. The method employs optical interference of the signals generated via coherent anti‐Stokes Raman scattering (CARS) of broadband laser pulses with noisy spectra. It does not require spectrally resolved detection, and no prior knowledge about either the Raman spectrum of the samples or the spectrum of the incident light is needed. We study the proposed method theoretically and demonstrate it in a proof‐of‐principle experiment on toluene and o‐xylene samples. Copyright © 2011 John Wiley & Sons, Ltd.     

碳纳米管的拉曼光谱及其温度效应

在室温下首次观察到碳纳米管的四级拉曼光谱，并且发现碳纳米管的Ｄ峰和Ｄ＊峰的斯托克斯线和反斯托克斯线频率不一致。此外，还发现碳纳米管的拉曼特征峰频率严重依赖样品的温度，随着温度增加，碳纳米管拉曼特征峰频率下移，频移与温度变化成线性关系。     

Quantitative analysis of sugar composition in honey using 532‐nm excitation Raman and Raman optical activity spectra

Raman spectroscopy based on the 1064‐nm laser excitation was suggested as a handy non‐invasive technique allowing to quickly determine sugar content in honey and similar food products. In the present study, the green 532‐nm laser radiation is explored instead as it provides higher‐quality spectra in a shorter time. The sample fluorescence was quenched by purification with activated carbon. For control mixture decomposition of Raman spectra to standard subspectra led to a typical error of the sugar content of 3%. Raman optical activity (ROA) spectra that could be measured at the shorter excitation wavelength as well provided a lower accuracy (~8%) than the Raman spectra because of instrumental sensitivity and noise limitations. The results show that Raman spectroscopy provides elegant and reliable means for fast analyses of sugar‐based food products. Copyright © 2016 John Wiley & Sons, Ltd.     

CARS temperature measurement in a LOX/CH4 spray flame

Coherent anti‐Stokes Raman scattering (CARS) spectroscopy has been used to investigate cryogenic liquid oxygen/gaseous methane (LOX/CH₄) flames on a medium‐size test facility at a pressure of 0.24 MPa and mass flow of 0.025 kg/s. Single‐shot, broadband CARS spectra with simultaneous detection of the Q‐branches of hydrogen and water molecules were recorded with good signal‐to‐noise ratio. Temperature was deduced from the H₂ and H₂O CARS profiles. The spatial temperature distribution in a comparatively harsh environment has been measured successfully. The measurements took place in the windowed combustion chamber of the DLR M3 test facility, aiming to provide data for validation of rocket combustor modeling. Copyright © 2010 John Wiley & Sons, Ltd.     

Range‐independent background subtraction algorithm for recovery of Raman spectra of biological tissue

An important requirement for the use of Raman spectroscopy for tissue diagnostic applications is an appropriate algorithm that can faithfully retrieve weak tissue Raman signals from the measured raw Raman spectra. Although iterative modified polynomial‐fitting‐based automated algorithms are widely used, these are sensitive to the choice of the fitting range, thereby leading to significantly different Raman spectra for different start and stop wavenumber selection. We report here an algorithm for automated recovery of the weak Raman signal, which is range independent. Given a raw Raman spectrum and the choice of the start and the stop wavenumbers, the algorithm first truncates the spectrum to include the raw data within this wavenumber range, linearly extrapolates the truncated raw spectrum beyond the points of truncation on the two sides by using coefficients of linear least‐square fit, adds two Gaussian peaks of appropriate height and width on the extrapolated linear wings on either side and then iteratively smoothens the data with all these add‐ons such that the smaller of the ordinate values of the smoothed and the starting raw data serve as the input to each successive round of iterative smoothing until the added Gaussian peaks are fully recovered. The algorithm was compared with the modified polynomial‐based algorithms using mathematically simulated Raman spectrum as well as experimentally measured Raman spectra from various biological samples and was found to yield consistently range‐independent and artifact‐free Raman signal with zero baseline. Copyright © 2012 John Wiley & Sons, Ltd.     

Continuous-wave rotational Raman laser in H(2)

A diode-pumped, far-off-resonance cw Raman laser in H(2) with rotational Stokes emission is reported for the first time to our knowledge. The Raman laser can produce single-wavelength emission at either 830 nm (rotational Stokes) or 1180 nm (vibrational Stokes) depending on the frequency tuning of the pump laser. The mirrors for the rotational cw Raman laser are easier to produce; the laser also exhibits a wider continuous tuning range and is less sensitive to thermal effects than the previously studied vibrational Raman laser [Opt. Lett. 26, 426 (2001) and references therein].