Temperature measurements in condensed phases using non‐resonant femtosecond stimulated Raman scattering

We have previously demonstrated the capability of femtosecond stimulated Raman scattering (FSRS) data to measure the temperature (T) of condensed matter at the molecular vibrational level. [Phys. Rev. Lett. 2011, 107, 43001] In this paper, we expand the theory for the FSRS temperature dependence by considering the effects of an isolated change of T as well as a coupled change of T and chemical concentration. We point out that the origin of the temperature sensitivity of the Stokes to anti‐Stokes ratio of FSRS lies in the exponential nonlinearity of the gain and loss. We establish that FSRS of two Raman modes can be used to simultaneously determine the vibrational temperature and the change in concentration of the species contributing to those two modes. Single‐shot experimental results using FSRS are presented to demonstrate over four orders of magnitude higher efficiency than spontaneous Raman in small volume samples with picosecond resolution. Copyright © 2012 John Wiley & Sons, Ltd.     

拉曼增益系数可分离光纤中的受激拉曼散射

给出了拉曼增益系数分离光纤的定义,在考虑了N个单色光之间的两两受激拉曼散射,得到了这种光纤中单向传输的N个不同的单色光之间的受激拉曼散射（SRS）稳态耦合波方程的解析解。它适用于各单色光功率任意大小、光频率分布不均匀时的一般情况。这一结果可应用于光纤通信系统、拉曼光纤放大器和拉曼光纤激光器的设计与分析。最后把解析解与数值解进行了比较,两者取得了很好的一致。     

飞秒受激拉曼光谱线形:基于泵浦及探测脉冲光的共振条件研究

Resonance enhancement has been increasingly employed in the emergent femtosecond stimulated Raman spectroscopy (FSRS) to selectively monitor molecular structure and dynamics with improved spectral and temporal resolutions and signal-to-noise ratios. Such joint efforts by the technique-and application-oriented scientists and engineers have laid the foundation for exploiting the tunable FSRS methodology to investigate a great variety of photosensitive systems and elucidate the underlying functional mechanisms on molecular time scales. During spectral analysis, peak line shapes remain a major concern with an intricate dependence on resonance conditions. Here, we present a comprehensive study of line shapes by tuning the Raman pump wavelength from red to blue side of the ground-state absorption band of the fluorescent dye rhodamine 6G in solution. Distinct line shape patterns in Stokes and anti-Stokes FSRS as well as from the low to high-frequency modes highlight the competition between multiple third-order and higher-order nonlinear pathways, governed by different resonance conditions achieved by Raman pump and probe pulses. In particular, the resonance condition of probe wavelength is revealed to play an important role in generating circular line shape changes through oppositely phased dispersion via hot luminescence (HL) pathways. Meanwhile, on-resonance conditions of the Raman pump could promote excited-state vibrational modes which are broadened and red-shifted from the coincident ground-state vibrational modes, posing challenges for spectral analysis. Certain strategies in tuning the Raman pump and probe to characteristic regions across an electronic transition band are discussed to improve the FSRS usability and versatility as a powerful structural dynamics toolset to advance chemical, physical, materials, and biological sciences.     

液芯波导中受激动力学散射与受激拉曼散射的竞争

研究了液芯波导中受激拉曼散射和受激动力学散射的阈值随泵浦激光脉宽的变化，发现受激动力学散射的阈值随泵浦脉冲前沿增长率增大而下降。研究了受激动力学散射和受激拉曼散射的竞争，结果表明受激动力学散射可分解为两种成分，其中与瞬态泵浦功率密度增长率相关的成分在大于阈值的泵浦脉冲前沿处于竞争优势，与瞬态泵浦功率密度相关的成分在高泵浦功率密度处于竞争优势，并讨论了其相应的机制。     

KDP晶体受激拉曼散射特性

详细比较了磷酸二氢钾(KDP)晶体的自发拉曼散射和受激拉曼散射光谱,在受激拉曼散射(SRS)中观察到了自发拉曼散射中最强的振动模的三阶Stokes光(559.43,589.74,623.50nm),由于其他振动模的受激拉曼散射增益系数较小,其SRS光谱未观察到。另外,比较了传统生长的未退火和退火后的KDP晶体及快速生长的锥区和柱区KDP晶体的受激拉曼散射增益系数,结果表明生长方法和热退火对KDP晶体的受激拉曼散射增益系数无明显影响。     

KDP晶体受激拉曼散射特性

详细比较了磷酸二氢钾(KDP)晶体的自发拉曼散射和受激拉曼散射光谱,在受激拉曼散射(SRS)中观察到了自发拉曼散射中最强的振动模的三阶Stokes 光(559.43, 589.74, 623.50 nm),由于其他振动模的受激拉曼散射增益系数较小,其SRS光谱未观察到。另外,比较了传统生长的未退火和退火后的KDP晶体及快速生长的锥区和柱区KDP晶体的受激拉曼散射增益系数,结果表明生长方法和热退火对KDP晶体的受激拉曼散射增益系数无明显影响。     

Stimulated Raman backscattering from an ultrashort laser interacting with underdense plasmas

We present experimental results of the stimulated Raman backscattering instability (BSRS) in an ultrashort intense (45fs, 5.7×10¹⁷Wcm^-2) laser pulse interacting with an optically ionized helium gas. We have studied the stimulated Raman backscattering reflectivity and the phenomenon of the transition from strongly coupled BSRS to weakly coupled BSRS. We have obtained a good agreement between our experimental results and the theory of BSRS.     

Coherent anti‐Stokes Raman scattering in Raman lasers and Raman wavelength converters

In this paper recent research progress on the use of Coherent Anti‐Stokes Raman Scattering (CARS) in Raman lasers and Raman wavelength converters is reviewed. The latest insights in the physical nature and behavior of CARS are addressed, and the recent performance breakthroughs in CARS‐based Raman wavelength conversion are discussed. Based on the new findings regarding the behavior of CARS, a physical explanation for apparent inconsistencies in various experimental observations of Raman wavelength conversion is provided. To conclude it is shown that these recent insights also pave the way to the development of a novel CARS‐based mechanism for reducing the heat dissipation in Raman lasers.     

光解产生的铅原子中受激喇曼散射和共振激光辐射

用2660(?)的紫外激光解离PbCl_2分子时,发现在3740(?)和3734(?)波长上有较强的受激辐射输出.根据它们的光谱特性和铅原子的能级结构判断,这些辐射是基于双光子解离PbCl_2分子得到的铅原子在6p~(23)P_2亚稳能级上的布居而产生的光泵共振激光辐射和受激喇曼散射.提出了描述整个过程的理论模型,通过拟合实验结果,确定了2660(?)激光双光子解离PbCl_2产生6p~(23)P_2亚稳态铅原子的光解系数.当PbCl_2分子密度为N_(00)=6.21×10~(16)cm~(-3)时,光解产生的铅原子在6p~(23)P_2和6p~(21)D_2这两个亚稳态的最大布居数近似相等,称为2.0×10~(16)cm~(-3).     

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     

Stimulated Raman scattering in three-dimensional photonic crystals

The results of experimental studies of stimulated Raman scattering of light (SRS) excited in three-dimensional photonic crystals — synthetic opal matrices infiltrated with Raman active media are presented. It is shown that the SRS threshold in such structures decreases with respect to the SRS threshold in Raman active bulk materials. The influence of the photonic-band structure of the active materials used on the SRS properties is estimated.     

用染料荧光增益增强弱增益拉曼模式的受激拉曼散射的经典理论

建立了用染料荧光增益增强弱拉曼模式的受激拉曼散射(SRS)的经典理论,详细给出了拉曼增益gR,染料荧光增益gD和总损耗α的表达式,并在其推导过程中对经典理论作了修正,最后得到了荧光增益和受激拉曼增益可以共同使SRS强度的指数部分快速增长的结果,可以很好地解释观察到的实验现象,并为其提供理论依据。     

受激拉曼散射中的二阶量子关联

利用全量子理论和多模受激拉曼散射模型，研究了拉曼放大中，考虑泵浦光耗散时，斯托克斯光和泵浦光二阶量子关联函数随相互作用距离变化的特性，在不计及色散的影响时，斯托克斯光和泵浦光的二阶量子关联函数的变化主要取决于输入斯托克斯光和泵浦光的光强比，在极限情况下，本文的计算结果与拉曼产生的计算结果和经典耦合波理论的计算结果相符合。     

光纤-氮系统的受激拉曼散射

在实验上,对三种不同长度的石英光纤进行了高温高压扩氮制成了光纤氮拉曼增益介质,给出了测试SRS光谱的实验装置、光谱及传输模式照片.在理论上和实验上讨论了阈值条件和谱线宽度与抽运光功率之间的关系,实验结果和理论计算基本符合.同时,在实验上还观测到微弱的氮分子和石英分子间的耦合模式. 关键词： 光纤-氮系统 受激拉曼散射 传输模式 阈值条件     

部分离化激光等离子体的受激喇曼散射不稳定性

由于部分离化激光等离子体中存在束缚电子，它可显著改变其参量不稳定性。本文分析了部分离化激光等离子体的受激喇曼散射的非线性色散关系，计算了钕玻璃倍频和三倍频激光受激喇曼散射的增长率，结果表明，前向受激喇曼散射显著增强，后向受激喇曼散射影响不大。     

Ultrafast Raman loss spectroscopy

This paper deals with a new form of nonlinear Raman spectroscopy called ‘ultrafast Raman loss spectroscopy (URLS)’. URLS is analogous to stimulated Raman spectroscopy (SRS) but is much more sensitive than SRS. The signals are background (noise) free unlike in coherent anti‐Stokes Raman spectroscopy (CARS) and it provides natural fluorescence rejection, which is a major problem in Raman spectroscopy. In addition, being a self‐phase matching process, the URLS experiment is much easier than CARS, which requires specific phase matching of the laser pulses. URLS is expected to be alternative if not competitive to CARS microscopy, which has become a popular technique in applications to materials, biology and medicine. Copyright © 2009 John Wiley & Sons, Ltd.     

水的低频受激拉曼散射

利用532 nm的脉冲激光进行了水的受激拉曼散射研究. 水的低激发光能量下主要表现为受激Stocks和反Stocks 3426 cm^-1谱线; 在能量大于140 mJ时出现低频率313 cm^-1受激Stocks谱线, 同时出现后向3389和3268 cm^-1 的受激Stocks谱线. 实验结果表明, 在较强的激光作用下, 水的结构表现为冰的Ⅷ相.     

高压氢激发态之间的受激喇曼散射

本文采用非稳腔输出的XeCl准分子激光,首次观察到高压氢高激发态之间的受激喇曼散射,并讨论了它们产生的条件.     

Au纳米粒子增强丙酮受激拉曼散射研究

受激拉曼散射(stimulated Raman scattering,SRS)具有激光的特性,并且容易获取不同波长的激光,从而成为调谐激光频率的重要途径之一。然而,由于其转化效率低,限制了它的实际应用。金属纳米粒子具有很强的表面增强效应,曾被广泛地用于增强拉曼散射而获得良好的效果。本文提出将金属纳米粒子的这种性质用于增强SRS。把Au纳米粒子混合于拉曼介质丙酮中,以532nm的纳秒脉冲激光作为激发光,研究了Au纳米粒子在丙酮中的浓度对丙酮SRS一阶Stokes光强的影响,并通过仿真计算对实验结果进行了解释和分析。     

铯原子介质中受激拉曼四波混频的光放大特性

实验研究了在铯原子介质中受激拉曼四波混频过程中,注入的探针光与所产生的共轭光的增益特性,具体比较了在探针场分别作为Stokes场和Anti-Stokes场情况下,增益随粒子数密度、泵浦光频率失谐的依赖关系,并分析了其增益谱线线型和谱宽.为进一步开展基于受激拉曼四波混频进行量子关联光束的制备提供了主要实验参数的选择参考.