Resonance ionization mass spectroscopy for trace analysis of neptunium

Resonance ionization mass spectroscopic (RIMS) measurements for trace analysis and spectroscopy of ²³⁷Np, the ecologically most important isotope of neptunium, are described. The chemical procedure for the separation of neptunium from aqueous samples as well as the preparation of filaments for RIMS are outlined. Several two- and three-step excitation schemes have been investigated in order to find suitable conditions for the sensitive detection of ²³⁷Np. Using a three-step, three-color excitation and ionization scheme an overall detection efficiency of 3×10^–8 was obtained, resulting in a detection limit of 4×10⁸ atoms (160 fg) of ²³⁷Np. The hyperfine structure splittings of the levels under investigation, which influence the detection limit, were measured. A new method to determine the first ionization potential (IP) was applied to neptunium yielding a value of IP=6.2655(2) eV.     

Theoretical Approach to Energy Resolution of Semiconductor Detectors

All processes occurring in semiconductor detectors during detection of primary monoenergetic particles lead to broadening of spectral lines. In this work, a general expression for the energy resolution of semiconductor detectors is obtained using the theory of branching cascade processes. It is shown that the general formula involves all contributions to the spectral line broadening described in the literature and additional contributions associated with fluctuations of electron and hole lifetimes caused by inhomogeneity of traps in the semiconductor material and fluctuations of the electronic channel gain.     

基于差频中红外激光的痕量气体高分辨光谱检测研究

研究了基于差频光源的高分辨中红外激光光谱检测系统,差频中红外光源使用两台近红外半导体激光器作为种子光源,采用PPLN晶体作为非线性混频器件,结合准相位匹配技术实现了3.2～3.7μm中红外相干光源输出,最大差频输出功率约为1μW.以CH4为例检验了系统的高分辨红外光谱检测特性,选择CH4分子3028.751cm-1 v3基频吸收线作为分析谱线,10cm光程的检测限为0.8ppm.光谱数据分析表明,系统检测限主要受到标准具光学噪音的限制.     

Transmission Properties of the Femtosecond Pulse Through a Near-field Optical Fiber probe

The experimental results are given on the broadening characteristics of the time and frequency profile of the femtosecond pulse passed through a SNOM fiber probe. The power threshold for the spectral and temporal broadening was 158 μw for pulses with 250 fs width and the repetition rate of 250 kHz at 830 nm wavelength. The time broadening reached lps for 250 fs incident pulse of 500 μw. A finite-difference time-domain (FDTD) simulation was carried out to illuminate the transmission properties of ultrafast pulse through the SNOM probe. The broadening influence on temporal resolution spectrum and near-field fluorescence excited by two-photon technique are discussed.     

Transmission Properties of the Femtosecond Pulse Through a Near-field Optical Fiber probe

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Air pressure broadening and shifting of high-J lines of (00011) ← (00001) band of CO2

The absorption spectra of carbon dioxide (isotope 626, natural abundance in air, ambient temperature) have been studied at total pressures 68-570 Torr with spectral resolution 0.003-0.005 cm⁻¹. The spectra were measured in the spectral domain of 2273-2393 cm⁻¹ by FTIR spectrometer Bruker IFS 125 HR equipped with White-type multipass cell (6.4-41.6 m) and with a cell having 10 cm optical path length. Pressure broadening and shift coefficients were obtained from a series of spectra by means of a nonlinear least-squares spectral fitting technique for the lines of the (00011)←(00001) band with rotational quantum number up to J=82. For fitting of the individual line shapes, we used the Voigt profile with pre-calculated Doppler broadening parameter. The experimental pressure broadening and shift coefficients are compared with the values available in spectroscopic databases HITRAN 2008 and Carbon Dioxide Spectroscopic Databank (CDSD-296) and with other experimental values reported in the literature.     

大气痕量气体遥感探测仪发展现状和趋势

阐述了大气痕量气体探测技术的发展历程;详细介绍了几种国外先进的大气痕量气体遥感探测仪器的设计理念、工作原理和功能、工作模式、谱段设置和主要技术指标。讨论了我国遥感用星载大气痕量气体探测仪器的发展现状,给出了两种典型探测仪器的工作模式、谱段设置和主要性能指标。指出了未来星载大气痕量气体探测仪器的发展方向是提高遥感仪器的光谱分辨率、空间分辨率、灵敏度和定标精度以及发展主动遥感技术等,意在为我国今后这一领域的发展提供借鉴。     

Detection of hydrogen isotope atoms by mass spectrometry combined with resonant ionization

We examined the application of mass spectrometric methods using resonant ionization by a tunable laser and proposed its use for analyzing hydrogen isotopes. We conducted resonance ionization mass spectrometry (RIMS) to detect gas-phase hydrogen isotope atoms. The ionization efficiency was increased by more than 1000 times that obtained with conventional methods using nonresonant ionization. Resonant laser ablation mass spectrometry (RLAMS) was applied for deuterium detection in solid samples. A graphite substrate implanted with deuterium was used for ordinary laser ablation mass spectrometry (LAMS) and RLAMS. The deuterium signal was observed very clearly by RLAMS, in contrast to LAMS. Mass spectrometry combined with resonance ionization was very useful for hydrogen isotope detection, because components with equal mass numbers were resolved and the method demonstrated higher ionization efficiency. Received: 4 November 1998 / Revised version: 12 January 1999 / Published online: 7 April 1999     

杨氏双缝干涉实验中光谱奇异现象的特性分析

研究了完全相干光和部分相干光分别照射双缝时,杨氏双缝干涉实验中干涉场区的光谱变化现象.根据干涉场中光谱标准矩定义了光谱的相对光谱移动和相对光谱增宽,并利用相对光谱位移和相对光谱增宽分析了光谱奇异现象的特性.研究结果表明,入射光的某些光谱参量（如源光谱宽度Γ0,中心拦截比ε,相对空间相干度Δ0）对相对光谱增宽的影响相当大.结果还表明了光谱标准矩方法是定量研究光在传输中的光谱变化以及光谱奇异现象的有效工具.     

Elemental analysis in environmental land samples by stand-off laser-induced breakdown spectroscopy

The stand-off detection and analysis of environmental land samples have been demonstrated using laser-induced breakdown spectrometry. The samples of interest have included soils and vegetation powder. Elements Hg, As, Pb, Zn, Cd and Cr have been spectrally analysed with a focus on Hg as a trace contaminant in the samples. It is found that element Fe, usually contained in land samples, is a main source of spectral interference for Hg detection due to its ever present iron emission line at 253.68 nm that is closely adjacent to the strongest Hg emission line at 253.65 nm, and hence, a high resolution of spectral detection is necessary. The strong spectral signals from Bremsstrahlung emission in laser-induced plasma and atomic emission of Fe of high concentration caused a significant reduction in detection resolution in the use of image intensifier of an ICCD. The limit of detection at ~8 ppm for Hg detection in soil samples with iron as a minor constituent has been achieved, using an optical chopper and a CCD detector for laser-induced breakdown spectroscopy (LIBS) signal detection. Such detection method in LIBS system has shown a great advantage in determining trace elements from interfering elemental constituents in land sample matrixes.     

Investigation of all-optical analog-to-digital quantization using a chalcogenide waveguide: A step towards on-chip analog-to-digital conversion

We have investigated all-optical analog-to-digital quantization by broadening the pulse spectrum in a chalcogenide (As₂S₃) waveguide and subsequently slicing the measured spectrum using an array of filters. Pulse spectral broadening was measured for 8 different power levels in a 6 cm long As₂S₃ waveguide and used to analyze an 8-level all-optical quantization scheme employing filters with full-width at half-maximum (FWHM) bandwidth of 2 nm. A supercontinuum spectrum with −15 dB spectral width up to 324 nm was observed experimentally at large powers. This large spectral broadening, combined with filtering using a 128 channel arrayed waveguide grating (AWG) with 2 nm filter spacing, has the potential for all-optical quantization with 7-bit resolution. In order to encode the quantized signal we propose an encoder scheme which can be implemented using optical Exclusive-OR gates. Demonstrating all-optical quantization using a planar waveguide is an important step towards realizing all-optical A/D conversion on a chip.     

Resonance ionization mass spectroscopy for nuclear research and trace analysis

Resonance ionization mass spectroscopy (RIMS) has been applied, firstly, to a study of the nuclear properties of short-lived Au isotopes at the on-line isotope separator ISOLDE at CERN and, secondly, to a trace-analysis experiment of Pu.     

基于差频中红外激光的痕量气体高分辨光谱检测研究

研究了基于差频光源的高分辨中红外激光光谱检测系统,差频中红外光源使用两台近红外半导体激光器作为种子光源,采用PPLN晶体作为非线性混频器件,结合准相位匹配技术实现了3.2~3.7 μm中红外相干光源输出,最大差频输出功率约为1 μW.以CH₄为例检验了系统的高分辨红外光谱检测特性,选择CH₄分子3 028.751 cm^-1 v₃基频吸收线作为分析谱线,10 cm光程的检测限为0.8 ppm.光谱数据分析表明,系统检测限主要受到标准具光学噪音的限制.     

FTIR被动遥测信噪比优化及在变电站SF6泄漏检测应用

被动FTIR红外遥测技术可应用于气体泄漏检测,气体检测下限与仪器信噪比密切相关。仪器信噪比与测量参数有关,如光谱分辨率、采样频率、积分时间、平均次数等,如何结合实际应用优化参数组合以实现最佳信噪比,目前还缺少系统分析。针对这一问题,从理论上分析了这些参数与信噪比关系,并归类为三个方面：（1）光谱分辨率,引用了Roland Harig给出的结论,当光谱分辨率低于特征峰半高全宽时,信噪比不变,但为了避免背景气体的交叉干扰,分辨率不宜设置过低,需要结合实际应用综合考虑;（2）降低采样频率能够减少计算量,缩小光谱范围,但采样频率和光谱范围与信噪比无关;（3）在积分时间和光谱平均次数方面,同样时间条件下,多次干涉图采集会引入零光程差的采样误差,使得噪声大于理论计算值,因而长积分时间获得信噪比优于多次平均。开展了六氟化硫（SF₆）泄漏检测实验,根据SF₆特征峰宽度选择4 cm-1分辨率,20 kHz采样频率兼顾了信噪比和检测时间,并利用FTIR巡检系统发现变电站泄漏点,证明了方法的有效性。     

金属稳定同位素标记生物分析进展

细胞和组织的很多特定功能都由其在不同的生理条件下的生物分子含量决定,极少数分子的改变就有可能影响细胞生物功能并触发疾病生理过程,因此高灵敏的生物分子检测技术在疾病机理研究和疾病早期诊断方面具有重要作用。金属稳定同位素和放射同位素化学性质相近,借鉴放射同位素标记的成功经验,通过金属稳定同位素标记多组分生物分子,可以用原子质谱高灵敏地检测多组分生物分子。作为灵敏准确的金属元素检测工具,电感耦合等离子体质谱检出限低、基体效应低、线性范围广、同位素谱线分辨率高,因此适用于金属元素标记生物分子检测。金属稳定同位素标记已经被广泛应用到蛋白质、核酸、酶活性、生物小分子、甚至单个细胞的检测中,取得了一些可喜的进展,并展现了广阔未来应用前景。金属稳定同位素标记生物分析方法有三个特性：高灵敏度-大多数金属的稳定同位素有较高的标记灵敏度,并且可以通过纳米材料标记等方法实现信号放大;多组分同时分析-质谱仪同位素谱线高分辨率提供了多组分分析能力;高准确度-同位素稀释法提供了可溯源到SI国际单位制的高准确度检测结果。为了更好的推动相关研究,简要介绍金属稳定同位素标记生物分析的进展,主要内容包括以下几个部分：金属稳定同位素检测工具-无机质谱、金属稳定同位素标记高灵敏度分析、金属稳定同位素标记多组分同时分析、金属稳定同位素标记高准确度分析、金属稳定同位素标记单细胞分析的进展。     

Band tunable X-ray flat crystal spectrometer for laser-produced plasma spectroscopy measurements

An updated design of a band-tunable flat crystal spectrometer is presented. The new configuration contributes to a broad spectral coverage with greater resolving power, a strong rejection of hard X-ray backgrounds, and decreased sensitivity to source broadening for an extended source. To verify the performance of the spectrometer, spectral lines were measured using a potassium acid phthalate crystal for highly ionized species of aluminum or silicon, and the results were compared by measuring H- and He-like Al and Si lines by rotating the crystal to selected Bragg angles, at the Shenguang II laser facility. The observed energy-coverage range is consistent with the theoretical predictions, as well as with the measured spectral resolution of ~300.     

Detrimental effect of self-phase modulation on the performance of Brillouin distributed fiber sensors

We show that the spectral broadening of the pump pulse through self-phase modulation in a time-domain distributed Brillouin sensor has a considerably detrimental effect in the measurement, especially in the case of long distances and high-resolution pulses. Using 30 ns pump pulses with peak power of 276 mW, self-phase modulation leads to a doubling of the effective gain linewidth after some 20 km, which is equivalent to a contrast loss of 2dB in the measurement. The impact is higher for shorter pulses (higher resolution). The theoretical modeling is fully confirmed by experimental results.     

A NEW GENERATION OF INSTRUMENTATION AND CAPABILITIES FOR ATOMIC MASS SPECTROMETRY

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Analytical characterization of spectral anomalies in polychromatic apertured beams

The power spectrum of polychromatic apertured spherical waves changes strongly in the vicinity of phase singularities. A spectral shift effect is observed and, in some cases, a spectral switch occurs together with a broadening of the power spectrum. Low-order moments of the power spectrum are evaluated in points of the focal volume with spectral anomalies. First-order analytical expressions are proposed for the evaluation of the relative spectral shift and the relative spectral broadening in the transverse focal plane and along the optical axis. The influence of the fractional bandwidth and the selected singularity order is considered.     

红外扫描和频振动光谱系统的激光线宽与光谱分辨率

本文报道了一个简化的利用可见光和红外光带宽来计算和频光谱分辨率的公式. 公式显示和频振动光谱的Voigt线宽可以通过振动模式的均匀线宽(洛伦兹线宽)、非均匀线宽(高斯线宽)、红外光与可见光的高斯线宽计算获得. 利用本实验室新搭建的频率分辨及偏振分辨的皮秒和频光谱系统验证了该公式的准确性. 实验结果显示,本激光系统获取的红外光的高斯线宽为1.5 cm^-1. 本激光系统的光谱分辨率约为4.6 cm^-1,结果与胆固醇单层膜光谱获取的光谱分辨率(3.5~5 cm^-1)基本一致.