4.4 μm中红外激光外差光谱探测技术研究

在国内首次报道以窄线宽的4.4 μm外腔量子级联激光(QCL)作为本地振荡光源,黑体作为辐射光源的激光外差光谱实验装置的建立和测量工作。激光外差光谱是一种高灵敏度的光谱探测技术,并可以用于发展一种小型的光谱探测系统,进行地基或星载的地球大气或天文观测。介绍了激光外差的基本理论、装置的建立和实验测量工作。此激光外差光谱实验装置采用4.4 μm外腔量子级联激光,出光功率高达180 mW,在4.38～4.52 μm间连续可调,具有很宽的光谱调谐范围,能实现CO₂,CO和N₂O等大气重要分子的同时测量。通过开展不同压力下CO₂气体的激光外差光谱测量,对激光外差光谱实验装置的性能进行了评估。目前该激光外差系统的信噪比达到86,低于散粒噪声极限条件的理论计算值287,系统的光谱分辨率约为0.007 8 cm-1,能满足较窄线宽条件下的高分辨率激光外差光谱的测量。分析结果表明,中红外激光外差光谱系统具有很高的瞬态信噪比及光谱分辨率,在高精度测量大气温室气体的柱浓度和温室气体垂直廓线分布方面具有广阔的应用前景。     

Optimally chirped CARS using fiber stretchers

High spectral resolution coherent anti-Stokes Raman scattering (CARS) spectroscopy and microscopy are demonstrated with femtosecond laser systems. We perform optimal chirping in glass fibers and demonstrate a spectral resolution enhancement to better than 26 cm⁻¹, which is limited by the bandwidth of the measured resonances. Considering the convolution with the resonance bandwidth this corresponds to a spectral resolution of approximately 2.5 cm⁻¹, which is an enhancement by a factor of 165 with respect to the use of bandwidth-limited pulses. In microscopic imaging, a water background suppression of 81.5% is achieved.     

空间外差光谱仪定标方法研究

空间外差光谱仪(SHS)是近年来迅速发展起来的新型超光谱分析技术,但针对该项技术的定标研究方法还不成熟。本文在分析空间外差仪原理的基础上,探讨了SHS实验室定标方法,内容包括光谱定标和辐射定标。利用可调谐激光器与元素光谱灯,根据光谱带宽内的发射谱线所对应的波长,以及探测器尺寸与系统带宽之间的关系,设计了光谱定标方案。定标结果显示仪器光谱分辨率和光谱范围与理论设计值一致,通过多次光谱稳定性测试,光谱漂移较小。在辐射定标中,利用积分球系统进行了稳定性定标,利用标准灯和漫反射板完成了响应度定标,并利用定标系数进行了实例验证。定标结果显示该方法能够满足空间外差光谱仪定标要求,为获取的光谱数据进行定量反演奠定了基础。     

基于激光外差技术的高分辨率整层大气透过率测量

激光外差技术是一种高灵敏度的光谱探测技术,利用该技术研制的装置易于集成化小型化,可以进行地基或星载的地球大气或天文观测。基于激光外差光谱测量技术,结合自研的太阳跟踪仪建立了一套高分辨率整层大气透过率测量系统,系统分辨率约为0.006 cm-1。该系统利用太阳光和红外激光在非线性探测器中进行光学混频,通过对获取的混频信号进行电子学滤波和平方率探测,获得了高光谱分辨率的外差信号。采用Langley-plot定标法对测量系统进行定标,获取了仪器标定常数和对应的大气总光学厚度,实现了中红外波段整层大气透过率的实时测量。同时,将实测整层大气透过率与MODTRAN5.0软件仿真计算的结果进行对比分析,两者的一致性较好。分析表明该测量系统具有很高的分辨率并且性能稳定可靠,在大气科学、天文观测和激光大气传输等研究领域具有广阔的应用前景。     

Rare-earth-doped materials for applications in quantum information storage and signal processing

Realization of practical quantum memory and optical signal processing systems critically depends on suitable materials that offer specific combinations of properties. Solid-state materials such as rare-earth ions doped into dielectric crystals are one of the most promising candidates for several quantum information storage protocols, including quantum storage of single photons. This article provides an overview of rare-earth-doped material properties and summarizes some of the most promising materials studied in our laboratory and by other groups for applications in quantum information storage and for ultra-wide bandwidth signal processing. Understanding and controlling spectral diffusion in these materials, which ultimately limits the achievable performance of any quantum memory system, is also briefly reviewed. Applications in quantum information impose stringent requirements on laser phase and frequency stability, and employing a narrow spectral hole in the inhomogeneous absorption profile in these materials as a frequency reference can dramatically improve laser stability. We review our work on laser frequency and phase stabilization and report our recent results on using a narrow spectral hole as a passive dynamic spectral filter for laser phase noise suppression, which can dramatically narrow the laser linewidth with or without the requirement of active feedback.     

激光带宽抑制光束小尺度自聚焦效应的条件

激光带宽有利于抑制光束的小尺度自聚焦效应,从而突破非线性效应的限制提高高能固体激光器的输出功率。研究表明,带宽抑制小尺度自聚焦效应的程度与带宽和脉宽之比密切相关,相同脉宽条件下带宽越大对空间小尺度自聚焦的抑制作用越明显,而带宽一定时随着脉冲宽度的增大,带宽的抑制作用则逐渐变弱。在实际的钕玻璃激光放大系统中,由有限的增益带宽以及增益窄化等因素所限制的带宽量,决定了在这类固体激光系统中需要脉冲宽度短至皮秒量级才能有效利用激光带宽抑制小尺度自聚焦效应,而对于长至数十皮秒,甚至纳秒量级的长脉冲而言,如此有限的带宽量对小尺度自聚焦的抑制几乎不起作用。     

Preparation of relativistic 7Li+ ion beams for precision experiments at storage rings

Heavy ion storage rings allow for tests of the structure of local space time via the Doppler effect. At the TSR/Heidelberg an experiment with high resolution laser spectroscopy at ⁷Li⁺ is performed. To gain the maximum resolution for saturation spectroscopy new methods of relativistic ion beam preparation and diagnostics have been developed. The laser cooling of the beam allows for precision determination of the mean velocity of the ions. A novel phase synchronous detection scheme, ultimately sensitive to single ions, gives insights into the cooling mechanism and dynamics. With an additional synchronous excitation scheme systematic uncertainties of the test experiment can be drastically reduced. After separation of the ground state ions from the triplet states of ⁷Li⁺ by the combination of laser and electron cooling, a bunched and cooled ensemble of fast moving high precision clocks with minimized perturbations by space charge effects and intra beam scattering is available. This revised version was published online in August 2006 with corrections to the Cover Date.     

Coherent Phase Control of Multiphoton Ionization in Three-Level Ladder-Type System

We present the theoretical investigation of photoelectron spectroscopy resulting from the strong field induced multiphoton ionization in a typical three-level ladder-style system. Our theoretical results show that the photo-electron spectral structure can be alternatively steered by spectral phase modulation. This physical mechanism for strong field quantum control is explicitly exploited by the time-dependent dressed state population. It is concluded that the phase-shaped laser pulses can be used to selectively manipulate the multiphoton ionization process in complicated quantum systems.     

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.     

Compact spectroscopy system based on tunable organic semiconductor lasers

We applied a continuously tunable organic semiconductor thin film laser for high resolution transmission spectroscopy. Using a suitable encapsulation application of that low-cost laser device allowed us to realize a very compact and durable measurement system incorporating only very few optical components. To demonstrate the capability of our setup for high-resolution photospectroscopy, we measured the transmission curve of a narrow laser line filter. The resulting data was in good agreement with a measurement of the filter characteristic done using a commercial spectrometer. Our system is capable of measuring optical density (OD) values up to OD 5. A key for future systems is a novel low-cost mechanical tuning method for position-dependent distributed feedback lasers which enables high-speed tuning with wavelength access times under 10 ms independent of the tuning bandwidth.     

高功率超短脉冲激光系统中光谱增益窄化补偿的调制函数

 设计了一种与高功率超短脉冲激光放大过程中获得的总增益、增益介质的带宽、激光带宽、脉冲中心波长等参数相关的调制函数,对激光放大过程中的光谱增益窄化进行补偿。此调制函数的优越性在于,对不同性能的激光系统,无需改变调制函数的形式就能适用。通过数值模拟的方法,讨论了在不同增益介质带宽、激光带宽、脉冲中心波长下的补偿效果。此调制函数在高功率超短脉冲激光系统中有良好的应用前景。     

DESIRS: a state‐of‐the‐art VUV beamline featuring high resolution and variable polarization for spectroscopy and dichroism at SOLEIL

DESIRS is a new undulator‐based VUV beamline on the 2.75 GeV storage ring SOLEIL (France) optimized for gas‐phase studies of molecular and electronic structures, reactivity and polarization‐dependent photodynamics on model or actual systems encountered in the universe, atmosphere and biosphere. It is equipped with two dedicated endstations: a VUV Fourier‐transform spectrometer (FTS) for ultra‐high‐resolution absorption spectroscopy (resolving power up to 10⁶) and an electron/ion imaging coincidence spectrometer. The photon characteristics necessary to fulfill its scientific mission are: high flux in the 5–40 eV range, high spectral purity, high resolution, and variable and well calibrated polarizations. The photon source is a 10 m‐long pure electromagnetic variable‐polarization undulator producing light from the very near UV up to 40 eV on the fundamental emission with tailored elliptical polarization allowing fully calibrated quasi‐perfect horizontal, vertical and circular polarizations, as measured with an in situ VUV polarimeter with absolute polarization rates close to unity, to be obtained at the sample location. The optical design includes a beam waist allowing the implementation of a gas filter to suppress the undulator high harmonics. This harmonic‐free radiation can be steered toward the FTS for absorption experiments, or go through a highly efficient pre‐focusing optical system, based on a toroidal mirror and a reflective corrector plate similar to a Schmidt plate. The synchrotron radiation then enters a 6.65 m Eagle off‐plane normal‐incidence monochromator equipped with four gratings with different groove densities, from 200 to 4300 lines mm^?1, allowing the flux‐to‐resolution trade‐off to be smoothly adjusted. The measured ultimate instrumental resolving powers are 124000 (174 µeV) around 21 eV and 250000 (54 µeV) around 13 eV, while the typical measured flux is in the 10¹⁰–10¹¹ photons s^?1 range in a 1/50000 bandwidth, and 10¹²–10¹³ photons s^?1 in a 1/1000 bandwidth, which is very satisfactory although slightly below optical simulations. All of these features make DESIRS a state‐of‐the‐art VUV beamline for spectroscopy and dichroism open to a broad scientific community.     

Spectral modulation of ultra-broadband femtosecond laser pulses based on surface plasmon resonance

The surface plasmon resonance (SPR) for spectral modulation of the femtosecond laser pulses with 110 nm ultra-broad bandwidth is demonstrated on the basis of the development of ultrashort pulse laser sources which supports good spatial resolution and high peak intensity. Employing the femtosecond surface plasmon polariton pulses launched by a Kretschmann configuration, whose reflectivity curve has the characteristic of the ultra-broad bandwidth, we observe a frequency-dependent loss with greater attenuation at the peak of the spectrum profile than in the wings, which is very useful for adequate spectral modulation. The SPR for the spectral modulation is investigated in theoretical and experimental aspects. The arbitrary spectral modulation of the femtosecond laser pulses can be fulfilled by controlling and optimizing the SPR of the gold film. The experimental result agrees well with the calculation.     

High-resolution cavity-tuned ringdown spectrometer using a narrow-bandwidth pulsed laser source

A novel method of cavity ringdown spectroscopy is proposed to achieve high spectral resolution with tunable narrow bandwidth pulsed lasers. We demonstrate a cavity-tuned ringdown configuration in which only a single cavity mode is kept excited near the carrier frequency of a narrow bandwidth pulse laser. This is done simply by making a cavity resonance actively track the frequency reference served by the cw injection seed of the pulsed laser source. We present the servo mechanism used in the cavity resonance tracking, reliable procedures for transverse mode matching, and the evidence of single longitudinal mode excitation. The spectrometer performance is tested to record weak molecular overtone features of acetylene around the wavelength of 570 nm, showing cavity tracking stability within 5-MHz uncertainty which overcomes the bandwidth limit of pulsed laser sources itself. PACS 42.62.Fi; 42.60.Da; 33.20.Kf     

Sub-Doppler laser spectroscopy

Ideal primary data in atomic and molecular physics would include the energy levels of single isolated atoms and molecules, and an approximation to these is obtained from spectra of gases at low pressures. In classical spectroscopy a severe barrier to spectral resolution and measurement precision is often encountered because of the Doppler effect. The absorption frequency of an atom or molecule is modified by its velocity, and so a spectral line will be broadened because of the thermal distribution of velocities in a gas. The barrier can, however, be overcome by using lasers in a variety of different ways. This article introduces the two primary techniques now employed, namely Lamb dip and two-photon spectroscopy, and a variety of examples are discussed. Alternative strategies employing molecular beams, laser cooling and time resolution are also outlined. Limitations on extreme resolution are considered, and the article concludes with a section on laser frequency stabilization and frequency standards which often rely on sub-Doppler spectra.     

Cavity-enhanced direct frequency comb spectroscopy

Cavity-enhanced direct frequency comb spectroscopy combines broad spectral bandwidth, high spectral resolution, precise frequency calibration, and ultrahigh detection sensitivity, all in one experimental platform based on an optical frequency comb interacting with a high-finesse optical cavity. Precise control of the optical frequency comb allows highly efficient, coherent coupling of individual comb components with corresponding resonant modes of the high-finesse cavity. The long cavity lifetime dramatically enhances the effective interaction between the light field and intracavity matter, increasing the sensitivity for measurement of optical losses by a factor that is on the order of the cavity finesse. The use of low-dispersion mirrors permits almost the entire spectral bandwidth of the frequency comb to be employed for detection, covering a range of ～?10% of the actual optical frequency. The light transmitted from the cavity is spectrally resolved to provide a multitude of detection channels with spectral resolutions ranging from several gigahertz to hundreds of kilohertz. In this review we will discuss the principle of cavity-enhanced direct frequency comb spectroscopy and the various implementations of such systems. In particular, we discuss several types of UV, optical, and IR frequency comb sources and optical cavity designs that can be used for specific spectroscopic applications. We present several cavity-comb coupling methods to take advantage of the broad spectral bandwidth and narrow spectral components of a frequency comb. Finally, we present a series of experimental measurements on trace gas detections, human breath analysis, and characterization of cold molecular beams. These results demonstrate clearly that the wide bandwidth and ultrasensitive nature of the femtosecond enhancement cavity enables powerful real-time detection and identification of many molecular species in a massively parallel fashion.     

Multi-channel magnetic resonance spectroscopy through time domain multiplexing

Time domain multiplexing (TDM) is presented as a viable approach to increasing the sensitivity and efficiency of magnetic resonance spectroscopic (MRS) experiments through multi-channel signal acquisition. By switching very rapidly between coils of a receive phased array, TDM receiver extensions allow the acquisition of multiple, independent spectra through a single channel magnetic resonance console. A TDM receiver extension designed for imaging and spectroscopy is described, and the impact of this hardware extension on the processing and quantitation of MRS data is addressed. The primary complication involves the use of fixed bandwidth RF band-pass filters that can not be adjusted to match the spectral width of the desired MRS experiment.MRS sequences whose bandwidths are narrower than the bandwidth provided by TDM band-pass filters can be acquired through TDM with minimal loss of SNR as long as two constraints are met. The first constraint requires that the entire bandwidth of the band-pass filters be sampled at or more rapidly than the Nyquist rate associated with their bandwidth, to prevent extra noise from aliasing into the final spectrum. The second requirement is that spectral resolution be held constant to that of the desired experiment.Results from a two-channel multiplexed MRS experiment, conducted according to these guidelines, illustrate that TDM can be used to allow acquisition of multi-channel MRS experiments through single channel console systems with a minimal loss in SNR.     

Stimulated Raman spectroscopy using chirped pulses

We present a detailed theoretical and experimental characterization of a new methodology for stimulated Raman spectroscopy using two duplicates of a chirped, broadband laser pulse. Because of the linear variation of laser frequency with time (‘chirp’), when the pulses are delayed relative to one another, there exists a narrow bandwidth, instantaneous frequency difference between them, which, when resonant with a Raman‐active vibration in the sample, generates stimulated Raman gain in one pulse and inverse Raman loss in the other. This method has previously been used for coherent Raman imaging and termed ‘spectral focusing’. Here, gain and loss signals are spectrally resolved, and the spectrally integrated signals are used to determine the spectral resolution of the measured Raman spectrum. Material dispersion is used to generate a range of pulse durations, and it is shown that there is only a small change in the magnitude of the signal and the spectral resolution as the pulse is stretched from 800 to 1800 fs in duration. A quantitative theory of the technique is developed, which reproduces both the magnitude and linewidth of the experimental signals when third‐order dispersion and phase‐matching efficiency are included. The theoretical calculations show that both spectral resolution and signal magnitude are severely hampered by the third‐order dispersion in the laser pulse, and hence, a minimal amount of chirp produces the most signal with only a slight loss of spectral resolution. Copyright © 2014 John Wiley & Sons, Ltd.     

光源尺寸和光谱带宽对波带板成像的影响

X射线菲涅耳波带板成像能实现亚微米空间分辨能力,有可能应用于激光等离子体或聚变靶的高分辨X射线成像诊断.之前的数值模拟研究表明,成像分辨能力受光源尺寸、入射光或成像光谱带宽的影响.本文报道在632.8 nm为中心波长的可见光波段,对波带板成像的数值模拟和原理性验证实验.数值模拟表明:随着扩展光源尺寸增加,视场中央分辨能力基本不变,而像对比度下降;随着成像的光谱带宽的增加,视场中央分辨能力与像对比度同时下降.实验证实了数值模拟的结论,且实验与数值模拟结果的定量比较也符合得较好.     

HITRAP: A Facility for Experiments with Trapped Highly Charged Ions

HITRAP is a planned ion trap facility for capturing and cooling of highly charged ions produced at GSI in the heavy-ion complex of the UNILAC-SIS accelerators and the ESR storage ring. In this facility heavy highly charged ions up to uranium will be available as bare nuclei, hydrogen-like ions or few-electron systems at low temperatures. The trap for receiving and studying these ions is designed for operation at extremely high vacuum by cooling to cryogenic temperatures. The stored highly charged ions can be investigated in the trap itself or can be extracted from the trap at energies up to about 10 keV/q. The proposed physics experiments are collision studies with highly charged ions at well-defined low energies (eV/u), high-accuracy measurements to determine the g-factor of the electron bound in a hydrogen-like heavy ion and the atomic binding energies of few-electron systems, laser spectroscopy of HFS transitions and X-ray spectroscopy. This revised version was published online in July 2006 with corrections to the Cover Date.