Raman response function of atmospheric air

A model of the full Raman response function of a gas mixture including rotational and vibrational motions of molecules is presented and is applied to examine the properties of the retarded optical nonlinearity of atmospheric air. For few-cycle laser pulses, broadband field waveforms, and/or high gas temperatures, both rotational and vibrational motions can significantly contribute to the Raman response of atmospheric air, with the ratio of the rotational and vibrational parts of the Raman response function controlled by the gas temperature and the temporal shape of the laser field.     

皮秒激光抽运高压H_2的受激拉曼散射研究

利用Nd :YAG锁模序列脉冲激光 (10 6 4nm)抽运充有高压H2 的拉曼池 ,输出光束经棱镜分光后投射在屏上 ,在可见光及近紫外光区用彩色胶卷摄得 15个受激拉曼散射光斑 ;经 1m光栅摄谱仪摄谱 ,在 36 5— 6 0 5nm波长范围内得到 6 5条受激拉曼谱线 .通过实验结果与理论计算值的比较 ,证明除了H2 的振动拉曼频移量 4 15 4 6cm- 1 外 ,还有多个振动及转动拉曼频移量共同参与作用 ,从而产生了从紫外到红外众多波长的受激拉曼散射光 .     

Generation of high-order rotational lines by four-wave Raman mixing using a high-power picosecond Ti:Sapphire laser

More than thirty rotational lines equally spaced by 587 cm^–1 are generated simultaneously in the vicinity of the fundamental line by four-wave Raman mixing using a high-power picosecond Ti:Sapphire laser as a pump source and hydrogen as a Raman medium. Since the wavelength of this multifrequency laser emission extends from the near-infrared to the near-ultraviolet, it can be utilized as a tunable light source for picosecond spectroscopy. Because of the wide spectral bandwidth available, this procedure has great potential for the generation of ultrashort laser pulses by mode-locking these emission lines.     

Efficient excitation of Raman coherence by a gradient force

The vibrational molecular excitation by strong laser fields have been studied. Starting with the molecular Hamiltonian, we derive the vibrational excitation rate due to a gradient of laser field and show that the rate can be two to three orders of magnitude larger than the regular Raman rates. The developed theory contributes to understanding of interaction of powerful laser pulses with molecular systems, and it might be used in developing quantitative coherent Raman spectroscopy. Copyright © 2013 John Wiley & Sons, Ltd.     

High efficiency long pulse FIR Raman conversion in ammonia

Generally the quantum efficiency of FIR Raman generation in molecular gases is below the theoretical value. This disagreement is particularly evident in Raman scattering from pulsed sources with short pulse length, when the vibrational saturation limits the power conversion. Other nonlinear processes can overcome this saturation, but they require a very intense pump power for too short a time to use the FIR radiation in high sensitive experiments with heterodyne detection. This is the case, for instance, of RFWM. In this work we describe the experimental conditions to achieve a high efficiency 90 micron Raman conversion in ammonia, with both short and long pulses.     

Instantaneous shifted‐excitation Raman difference spectroscopy (iSERDS)

Shifted‐excitation Raman difference spectroscopy (SERDS) is an experimental method to recover spontaneous Raman spectra despite the presence of strong fluorescence interference. The common scheme requires a tunable laser source and recording two spectra after each other. In this paper, an approach for instantaneous SERDS (iSERDS) is presented utilizing a broadband light source. The broadband radiation is spatially dispersed in the focal plane inside the object of investigation. The generated scattering signal is imaged onto the slit of an imaging spectrograph. The individual pixel lines on the detector represent Raman spectra with slightly shifted excitation wavelength and hence allow SERDS spectra to be derived. The proposed iSERDS technique is a suitable approach for obtaining Raman spectra from fluorescing samples provided they are homogenous on the length scale of the measurement volume. Copyright © 2014 John Wiley & Sons, Ltd.     

Stimulated Raman scattering and four-wave Raman mixing seeded by a supercontinuum generated in dibromomethane using picosecond and femtosecond laser sources

Stimulated Raman emission from liquid dibromomethane (vibrational Raman shift frequency, 588 cm⁻¹) is introduced into hydrogen gas (rotational Raman shift frequency, 587 cm⁻¹) as a seed beam, in order to generate numerous rotational lines by four-wave Raman mixing. Unexpectedly, a supercontinuum, which is generated by self-phase modulation in dibromomethane, acted as a seed beam to exclusively generate vibrational lines; the rotational lines are generated only when the supercontinuum is minimal. The former is explained by a competition between the high-gain vibrational and low-gain rotational Raman effects when strongly seeded by a supercontinuum. The latter is explained by stimulated Raman gain under the seed effect exclusively to the first-Stokes rotational line.     

Synthesis of periodic femtosecond pulse trains in the ultraviolet by phase-locked Raman sideband generation

We demonstrate a new technique for femtosecond-pulse generation that employs ultrafast modulation of a laser field phase by impulsively excited molecular rotational or vibrational motion with subsequent temporal compression. An ultrashort pump pulse at 800 nm performs impulsive excitation of a molecular gas in a hollow waveguide, and a weak delayed probe pulse at 400 nm is scattered on the temporal oscillations of its dielectric index. The resultant sinusoidal phase modulation of the probe pulse permits probe pulse temporal compression by use of both positively and negatively dispersive elements. The potential of this new method is demonstrated by the generation of a periodic train of 5.8-fs pulses at 400 nm with positive group-delay dispersion compensation.     

High-order stimulated Raman scattering in a highly transient regime driven by a pair of ultrashort pulses

We demonstrate efficient generation of high-order anti-Stokes Raman sidebands in a highly transient regime, using a pair of approximately 100-fs laser pulses tuned to Raman resonance with vibrational transitions in methane or hydrogen. The use of this technique looks promising for efficient subfemtosecond pulse generation.     

Phase‐shaping strategies for coherent anti‐Stokes Raman scattering

The identification of large molecules in complex environments requires probing of multiple vibrational resonances rather than a single resonance. Phase‐shaping the excitation pulses allows the coherent mixing of several resonances so that the presence of molecules can be inferred directly from the integrated output pulse energy. This avoids the need for the collection of spectra or multiple measurements. This article describes a particular implementation for coherent anti‐Stokes Raman scattering microscopy that uses a broadband pump and probe field in combination with a narrowband Stokes field. We numerically study the possibilities of optimizing selectivity, specificity, and sensitivity by precalculating pulse shapes using an evolutionary algorithm. Copyright © 2011 John Wiley & Sons, Ltd.     

Remote sensing of the atmosphere using ultrashort laser pulses

Theoretical and experimental studies were performed on the propagation of ultrashort optical terawatt pulses through the atmosphere. Propagation simulations of intense sub-picosecond pulses show that non-linear processes, such as white light generation, can be initiated at a chosen distance by selecting an appropriate group velocity dispersion. With this technique, a white light continuum was generated in the atmosphere whose spectral distribution was characterised in the visible and near infra-red. Applications of this novel light source for atmospheric remote sensing were investigated, combining lidar and time-resolved broadband absorption spectroscopy techniques. Measurements were performed on the oxygen molecule and water vapour. A comparison between the experimental results and the tabulated spectroscopic data led to an excellent correlation with measurements made on water vapour whereas observations on the oxygen showed discrepancy. This study demonstrates that the remote generation of a white light source represents a new way to access the range-resolved multi-trace gas analysis in the atmosphere. Received: 8 December 1999 / Revised version: 18 May 2000 / Published online: 16 August 2000     

荧光材料Y_2O_3:Eu变温拉曼光谱分析

本文用显微拉曼谱仪在波长为785 nm的激光激发下,对Y2O3:Eu陶瓷在温度83-473 K间进行了系统的变温拉曼实验研究。实验发现Y2O3:Eu的一些振动模在低温下没有出现,只有当温度达到一定值之后才可以被观察到,分析表明这是由于温度变化引起的简并振动模式分裂。此外,Y2O3:Eu的拉曼峰位、半高全峰宽(FWHM)也是温度的非线性函数,且不同的拉曼峰遵循不同的函数关系,本文分析这是由于晶格的各向异性导致的。     

Raman spectroscopy with LED excitation source

We propose and experimentally demonstrate a novel instrument arrangement, which allows for the collection of Raman spectra with a broadband light source. This is achieved by spatially dispersing the optical spectrum in the focal plane and confocally reimaging the Raman signal, which originates from different locations, onto the entrance slit of an imaging spectrometer. Using this approach and broadband radiation derived from a commercially available LED, we acquired high signal‐to‐noise spectra with a spectral resolution limited by the spectral resolution of a spectrometer. Copyright © 2013 John Wiley & Sons, Ltd.     

Detecting nanoparticles by “listening”

In the macroscopic world, we can obtain some important information through the vibration of objects, that is, listening to the sound. Likewise, we can also get some information of the nanoparticles that we want to know by the means of “listening” in the microscopic world. In this review, we will introduce two sensing methods (cavity optomechanical sensing and surface-enhanced Raman scattering sensing) which can be used to detect the nanoparticles. The cavity optomechanical systems are mainly used to detect sub-gigahertz nano particle or cavity vibrations, while surface-enhanced Raman scattering is a well-known technique to detect molecular vibrations whose frequency generally exceeds terahertz. Therefore, the vibrational information of nanoparticles from low-frequency to high-frequency could be obtained by these two methods. The size of the viruses is at the nanoscale and we can regard it as a kind of nanoparticles. Rapid and ultrasensitive detection of the viruses is the key strategies to break the spread of the viruses in the community. Cavity optomechanical sensing enables rapid, ultrasensitive detection of nanoparticles through the interaction of light and mechanical oscillators and surface-enhanced Raman scattering is an attractive qualitatively analytical technique for chemical sensing and biomedical applications, which has been used to detect the SARS-CoV-2 infected. Hence, investigation in these two fields is of vital importance in preventing the spread of the virus from affecting human’s life and health.     

Ultrahigh efficiency laser wavelength conversion in a gas-filled hollow core photonic crystal fiber by pure stimulated rotational Raman scattering in molecular hydrogen

We report on the generation of pure rotational stimulated Raman scattering in a hydrogen gas hollow-core photonic crystal fiber. Using the special properties of this low-loss fiber, the normally dominant vibrational stimulated Raman scattering is suppressed, permitting pure conversion to the rotational Stokes frequency in a single-pass configuration pumped by a microchip laser. We report 92% quantum conversion efficiency (40 nJ pulses in 2.9 m fiber) and threshold energies (3 nJ in 35 m) more than 1 x 10(6) times lower than previously reported. The control of the output spectral components by varying only the pump polarization is also shown. The results point to a new generation of highly engineerable and compact laser sources.     

Phase-matched high harmonic generation for the study of rotational coherence molecular dynamics

We report the observation of periodic modulations in the high order harmonic radiation from diatomic molecules in a semi-infinitive gas cell when a preceding femtosecond laser beam, which is off-axis to the high-harmonic generation beam, modifies the phase-matching condition through the field-free alignment of the molecules. The observed modulations of the high harmonic radiation versus the time delay between the pulses result from periodic changes in the nonlinear refractive index associated with rotational Raman coherence. This opens up a new potential technique for studying rotational coherence dynamics in the ground states of molecules.     

差频可调谐太赫兹技术的新进展

太赫兹技术在最近30年来得到快速发展, 并在医学、生物、农业、材料、安检、通信、天文等领域得到广泛应用. 从太赫兹源的频谱特性可以分为窄带(单频)太赫兹源和宽带太赫兹源. 从频谱技术方面来说, 相干的宽带和窄带太赫兹谱是一种互补性关系, 具有各自的技术特点和应用范围. 宽带太赫兹谱可以用于快速获取较宽频谱范围的分子振转谱, 实现混合特征谱的快速检测或成像. 窄带太赫兹源具有很好的光谱灵敏度和分辨率, 适用于太赫兹抽运-探测、分子振转能级谱精细结构分辨 以及太赫兹远程探测和成像. 因此研制具有可调谐的高峰值功率的窄带太赫兹源是适用于探测和识别分子振转能级指纹谱的应用需求, 而差频技术是获得高功率和宽调谐窄带太赫兹源最重要的技术之一. 为了突出该技术的最新进展, 本综述引证论文仅仅限于近5 年来基于差频技术产生太赫兹波的研究进展, 分为光学激光差频源和量子级联激光器差频源两大部分. 对于光学激光差频源, 分别对目前文献报道的各种双波长差频源和太赫兹产生用的非线性晶体进行分类介绍, 并给出所采用的技术和实验结果; 对于量子级联激光器差频源, 分别介绍了量子级联激光器中的差频产生技术和波长调谐技术的最新进展. 量子级联激光器差频太赫兹源是目前实现量子级联激光器在太赫兹波段室温运转的惟一技术, 是实现小型化、窄带宽调谐和室温运转太赫兹源的新发展领域, 值得关注.     

绝对探测大气温度的纯转动拉曼激光雷达系统

纯转动拉曼激光雷达是探测大气温度廓线的重要手段之一,其正常工作需要配置其他并行校正设备,制约其在气象及环境监测领域中的实用化进程.基于大气氮气分子的纯转动拉曼谱型对温度的依赖性,提出并设计了绝对探测大气温度廓线的纯转动拉曼激光雷达系统.系统采用波长532 nm且脉冲能量300 m J的激光激励源和口径250 mm卡塞格林望远镜的接收器,设计了衍射光栅和光纤Bragg光栅结合的多通道并行纯转动拉曼光谱分光系统;仿真分析氮气和氧气分子的纯转动拉曼散射谱线间关系,优化选择了6条氮气分子的纯转动拉曼谱线以直接反演大气温度,设计了两级滤光器间转接光纤阵列的结构;基于最小二乘原理推导了绝对探测大气温度的反演算法,并结合标准大气模型,分析了纯转动拉曼激光雷达绝对探测大气温度的探测性能.结果表明,所设计纯转动拉曼激光雷达系统可直接反演大气温度廓线,在测量时间17 min内,温度偏差小于0.5 K的探测高度达2.0 km.     

拉曼光谱技术研究男性生殖生育

拉曼光谱通过记录光与物质作用时频率的改变,进而获得物质分子振动、转动信息,从而实现物质分子结构及其变化的检测。相比于常规生化检测分析方法,拉曼光谱技术具有无损、非标记检测及对检测样品要求低等优点。 拉曼光谱技术已广泛应用于生物医学领域的研究,如人体组织、器官、细胞以及人体体液的各种疾病诊断、检测研究。本文主要综述了拉曼光谱技术在人体精液的研究进展,首先介绍了拉曼光谱技术(包含表面增强拉曼光谱)在法医学领域针对精液整体开展的研究及相关的数据处理方法,然后重点介绍拉曼光谱在男性生殖生育方面的研究,即分别介绍了可客观反映精液质量及男性生殖生育能力的基于精液(精浆)拉曼光谱的定性和定量检测分析;另外,介绍了基于显微拉曼光谱技术开展的单精子水平的精子质量的刻画和评估,以及目前研究初步获得的有望用于优质精子判别的拉曼光谱标记指标,最后展望了拉曼光谱技术在生殖生育领域的应用发展前景。     

Selective excitation of molecular mode in a mixture by femtosecond resonance-enhanced coherent anti-Stokes Raman scattering spectroscopy

Femtosecond time-resolved coherent anti-Stokes Raman scattering (CARS) spectroscopy is used to investigate gaseous molecular dynamics. Due to the spectrally broad laser pulses, usually poorly resolved spectra result from this broad spectroscopy. However, it can be demonstrated that by the electronic resonance enhancement optimization control a selective excitation of specific vibrational mode is possible. Using an electronically resonance-enhanced effect, iodine molecule specific CARS spectroscopy can be obtained from a mixture of iodine-air at room temperature and a pressure of 1 atm (corresponding to a saturation iodine vapour as low as about 35 Pa). The dynamics on either the electronically excited state or the ground state of iodine molecules obtained is consistent with previous studies (vacuum, heated and pure iodine) in the femtosecond time resolved CARS spectroscopy, showing that an effective method of suppressing the non-resonant CARS background and other interferences is demonstrated.