基于噪声免疫腔增强光外差分子光谱技术实现光纤激光器到1530.58 nmNH_3亚多普勒饱和光谱的频率锁定

噪声免疫腔增强光外差分子光谱技术(NICE-OHMS)由于结合了频率调制光谱与腔增强光谱两种技术,不仅可以将激光耦合到高精细度谐振腔大幅提高腔内功率,还可以实现低气压样品气体的高灵敏测量,因此基于该技术可以实现分子吸收线的饱和,获得亚多普勒光谱,从而能作为激光频率锁定的参考.本文基于光纤激光器的NICE-OHMS技术,将光纤激光器频率锁定到NH3的亚多普勒吸收线上.首先分析了基于Pound-Drever-Hall和DeVoe-Brewer技术实现激光到腔模和调制频率到腔自由光谱区频率锁定的性能,之后在腔内气压为70 mTorr条件下,测量了半高全宽为2.05 MHz的NH3亚多普勒信号,最后将1.53μm的光纤激光器频率锁定到该亚多普勒吸收线上,相对频率偏差为16.3 kHz,阿伦方差结果显示,136 s积分时间下频率稳定度达到1.6×10~(-12).     

Cavity-enhanced absorption spectroscopy for shocktubes: Design and optimization

Cavity-enhanced absorption spectroscopy (CEAS) has generated much interest in shocktube kinetics studies because of its recent success in achieving improved sensitivity and high time resolution with robust optical alignment. While recent progress demonstrated experimental schemes including off-axis scanned-wavelength approach and on-axis ps-pulsed laser approach, that both successfully suppressed the laser-cavity coupling noise, this paper develops a theoretical model to predict the CEAS sensor performance that can be used as a design tool applicable to more generalized cases. The method models the optical field in the cavity based on the decentered Gaussian beam model, from which the cavity transmission spectrum and the laser-cavity coupling noise can be numerically calculated. The simulation results predict sensor performance for different cavity configurations and laser characteristics, including various degrees of laser-cavity mode-matching, laser linewidths, scanning rates, and cavity filling conditions. Simulation with example wavelengths in the ultraviolet, near-infrared, and mid-infrared showed increasing mode-matched beam waist size for increasing wavelengths. An off-axis alignment scheme was found to be capable of suppressing the coupling noise by two orders-of-magnitude at a moderate laser linewidth of 1?GHz. Coupling noise level on the order of 1e-5 for scanned-wavelength off-axis alignment case with a narrowband mid-infrared laser was obtained by model calculation and agreed with experimental results within acceptable uncertainty range. The developed method can serve to guide future design and optimization of CEAS system in shocktube studies.     

基于扫描激光的腔增强吸收光谱研究

介绍了一种建立在半导体激光扫描基础上的腔增强吸收光谱技术。简要介绍了从衰荡吸收光谱技术向腔增强吸收光谱的发展及腔增强吸收光谱的实验装置,实验证明能够将 DFB 型半导体激光与高精密光学谐振腔相结合,用简单的实验装置进行高灵敏、高分辨直接吸收光谱测量。实验中,激光器的输出波长用一台波长计精确测量,当激光器的输出频率与某一腔模的频率共振时,激光被耦合到一个用两块高反射率平凹透镜(在 1.572μm 附近,R~0.994)组成的 34cm 长的高精密光学谐振腔,通过测量激光透过谐振腔后的光强,得到了二氧化碳分子在6358.654cm-1附近的吸收光谱,探测灵敏度达到了 1.2×10-5cm-1。     

Multi-mode absorption spectroscopy, MUMAS, using wavelength modulation and cavity enhancement techniques

Multi-mode absorption spectroscopy, MUMAS, has been combined with the techniques of wavelength modulation spectroscopy, WMS, and cavity enhanced absorption spectroscopy, CEAS, to record multiple molecular transitions using a single laser and a single detector. MUMAS signals were recorded using a multi-mode diode laser of the A-band $b^{1}\varSigma _{g}^{+}\leftarrow X^{3}\varSigma _{g}^{-}Multi-mode absorption spectroscopy, MUMAS, has been combined with the techniques of wavelength modulation spectroscopy, WMS, and cavity enhanced absorption spectroscopy, CEAS, to record multiple molecular transitions using a single laser and a single detector. MUMAS signals were recorded using a multi-mode diode laser of the A-band b¹\varSigma _g⁺? X³\varSigma _g^-b^{1}\varSigma _{g}^{+}\leftarrow X^{3}\varSigma _{g}^{-} of molecular oxygen at 760 nm. Direct MUMAS and WMS-MUMAS signals were recorded using a White cell for air and pure oxygen for pressures in the range 0 to 1 bar. CEAS-MUMAS signals were recorded with and without WMS in an open enhancement cavity containing laboratory air. Enhancement of the signal-to-noise ratio has been obtained demonstrating the potential for increased detection sensitivity for gas-sensing applications of MUMAS.     

Application of magnetic field over-modulation for improved EPR linewidth measurements using probes with Lorentzian lineshape

Magnetic field modulation in CW electron paramagnetic resonance (EPR) is used for signal detection. However, it can also distort signal lineshape. In experiments where the linewidth information is of particular importance, small modulation amplitude is usually used to limit the lineshape distortion. The use of small modulation amplitude, however, results in low signal-to-noise ratio and therefore affects the precision of linewidth measurements. Recently, a new spectral simulation model has been developed enabling accurate fitting of modulation-broadened EPR spectra in liquids. Since the use of large modulation amplitude (over-modulation) can significantly enhance the EPR signal, the precision of linewidth measurements is therefore greatly improved. We investigated the over-modulation technique in EPR oximetry experiments using the oxygen-sensing probe lithium octa-n-butoxy-substitued naphthalocyanine (LiNc-BuO). Modulation amplitudes 2-18 times the intrinsic linewidth of the probe were applied to increase the spectral signal-to-noise ratio. The intrinsic linewidth of the probe at different oxygen concentrations was accurately extracted through curve fitting from the enhanced spectra. Thus, we demonstrated that the over-modulation model is also applicable to particulate oxygen-sensing probes such as LiNc-BuO and that the lineshape broadening induced by oxygen is separable from that induced by over-modulation. Therefore, the over-modulation technique can be used to enhance sensitivity and improve linewidth measurements for EPR oximetry with particulate oxygen-sensing probes with Lorentzian lineshape. It should be particularly useful for in vivo oxygen measurements, in which direct linewidth measurements may not be feasible due to inadequate signal-to-noise ratio.     

激光器特性在痕量气体检测中的影响

研究了激光器扫描步长和线宽两种特性对可调谐半导体激光吸收光谱检测系统的影响,理论上推导出激光与气体吸收谱线的作用原理,分析出扫描信号(锯齿波)的台阶间隔和高度影响激光器中心波长的扫描原理.设定了仿真参数,仿真出锯齿波台阶数与最大扫描误差关系曲线,得出扫描信号的一个周期内具有4000个台阶时,半高全宽(FWHM)大于0.01 cm-1,误差小于1‰;仿真出激光器线宽与最大幅值、线宽误差关系曲线,给出线宽误差最大为1%,0.5%时激光器线宽对应的最小FWHM.在温度系数n取0.9,大气展宽系数γair取0.005的条件下,给出温度T,压强P与FWHM关系图,推出了适用的压强与温度范围.为指导选取激光器与气体吸收谱线、提高系统检测限提供了相关理论依据.     

Measurement of the Rb D2 transition linewidth at ultralow temperature

The Rb D2 linewidth was studied using atoms cooled to a temperature of 50 μK that were contained in a magneto-optical trap. The transmission of a probe laser through the atom cloud was monitored using a CCD detector. The frequency of the probe laser was scanned across the resonance using an acousto-optic modulator. The observed lineshape was very well fitted by a Lorentzian function. The full width half maximum linewidth was examined as a function of the optical depth and the probe laser intensity. The extrapolated value at zero optical depth 6.062 ± 0.017 MHz corresponds to a 5P_3/2 lifetime of 26.25 ± 0.07 ns. This result agrees with lifetimes found in experiments that measured the temporal decay of fluorescence or photoassociation spectroscopy and is somewhat below the result of a relativistic many body perturbation calculation.     

Lineshape effects in atomic absorption spectroscopy

Deviations from Beer's Law caused by the relative lineshape functions of source and absorber in atomic absorption experiments are considered. The validity of using a modified form of the law incorporating a correction factor γ, which is particularly convenient in time-resolved atomic absorption experiments, to account for these deviations, has been critically examined for a wide range of source and absorber lineshapes using numerical evaluation of the transmission integrals involved. It is concluded that there is, in general, no theoretical justification for the use of such a γ factor, except in the case of large source linewidth/absorber linewidth ratios when the line broadening in the absorber involves a significant homogeneous (Lorentzian) contribution. The use of empirically determined γ factors, much different from unity to analyse experimental data, should be viewed with suspicion unless direct evidence is presented to show that under the experimental conditions γ happens to be constant or slowly varying.     

Linewidth Analysis of Spin Labels in Liquids: I. Theory and Data Analysis

We present a method of simulating the EPR spectra of spin labels in liquids using direct convolution of hyperfine splitting with Lorentzian linewidths. The aim is to simulate the experimental lineshape by considering all spectrometer characteristics as well as inhomogeneous and homogeneous linewidth effects. A major advance in this method is the correction for the broadening produced by Zeeman modulation commonly used to obtain EPR signals; this allows experimenters much more freedom to optimize their experimental conditions for the best signal-to-noise ratio. Microwave power broadening (saturation) effects on the EPR lines are significant even at very low observer levels. Successful simulation requires that all contributions from unresolved hyperfine splittings be explicitly included. Inhomogeneous broadening is dealt with by including all spins that interact with the electron (as a set of superhyperfine interactions); there is no "effective Gaussian" to substitute for the correct superhyperfine interactions. The effects of spin exchange on the linewidth and lineshape can be observed and must be taken into account in order to extract the fundamental linewidths.     

基于QCL的红外吸收光谱技术的研究进展

量子级联激光器作为一种新型的单极型半导体激光器,其峰值发射波长处于中红外波段（2.5~25 μm）,具有功率高、线宽窄、响应速率快等传统半导体激光器所没有的独特优势,且具有较高的探测灵敏度,非常适合中红外波段的气体分子的检测。可广泛应用于大气痕量气体、呼吸气体、燃烧气体、生化气体、机动车尾气、工业废气以及农药残留气体等低浓度气体的检测。因此,利用量子级联激光器对气体分子进行探测在非侵入式医学诊断、环境监测以及工农业生产等领域都具有十分重要的意义。自20世纪末量子级联激光器发明以来,室温激光器的性能得到了长足的进步,也出现了多种结构形式的量子级联激光器。这也使得量子级联激光器红外吸收光谱技术得到了很大的发展。事实上,很多光谱技术在量子级联激光器发明之前就已经得到了发展和应用,而利用量子级联激光器作为光源则在很大程度上扩展了可探测波段,也在一定程度上提高了探测极限。这其中就包括了直接吸收光谱技术、波长调制技术、腔衰荡光谱技术、腔增强吸收光谱技术以及光声光谱等。综述了国内外量子级联激光器进行红外吸收光谱技术的研究现状和发展趋势,分析了量子级联激光器红外吸收光谱技术在发展过程中所遇到的瓶颈以及后期得到的解决方案,比较详细地介绍了各种方法的原理、应用,并指出了在吸收光谱测量中的优缺点,同时对外场痕量气体探测作了简要总结。最后,对量子级联激光器红外吸收光谱技术在未来痕量气体探测上的应用和发展进行了展望,指出随着红外吸收光谱技术的快速发展,这些方法可以得到更有效的改进和发展,进而朝着高灵敏度、高集成度以及高时效方向发展。     

The role of laser linewidth and lineshape in pulsed two-photon absorption

The role of linewidth is examined for the three distinct intensity regimes which characterise the theory of multiphoton absorption. Re-examination of a two-photon experiment shows that a laser lineshape due to an Ornstein-Uhlenbeck process gives even closer agreement between theory and experiment than a gaussian.     

A quantum cascade laser-based optical feedback cavity-enhanced absorption spectrometer for the simultaneous measurement of CH4 and N2O in air

Optical feedback cavity-enhanced absorption spectroscopy (OF CEAS) has been demonstrated with a thermoelectrically cooled continuous wave distributed feedback quantum cascade laser (QCL) operating at wavelengths around 7.84 μm. The QCL is coupled to an optical cavity which creates an absorption pathlength greater than 1000 m. The experimental design allows optical feedback of infra-red light, resonant within the cavity, to the QCL, which initiates self-locking at each TEM₀₀ cavity mode frequency excited. The QCL linewidth is narrowed to below the mode linewidth, greatly increasing the efficiency of injection of light into the cavity. At the frequency of each longitudinal cavity mode, the absorption coefficient of an intracavity sample is obtained from the transmission at the mode maximum, measured with a thermoelectrically cooled detector: spectral line profiles of CH₄ and N₂O in ambient air were recorded simultaneously and with a resolution of 0.01386 cm^?1. A minimum detectable absorption coefficient of 5.5×10^?8 cm^?1 was demonstrated after an averaging time of 1 s for this completely thermoelectrically cooled system. The bandwidth-normalised limit for a single cavity mode is 5.6×10^?9 cm^?1?Hz^?1/2 (1σ).     

Absorption linewidth inversion with wavelength modulation spectroscopy

For absorption linewidth inversion with wavelength modulation spectroscopy(WMS), an optimized WMS spectral line fitting method was demonstrated to infer absorption linewidth effectively, and the analytical expressions for relationships between Lorentzian linewidth and the separations of first harmonic peak-to-valley and second harmonic zero-crossing were deduced. The transition of CO_2 centered at 4991.25 cm~(-1) was used to verify the optimized spectral fitting method and the analytical expressions. Results showed that the optimized spectra fitting method was able to infer absorption accurately and compute more than 10 times faster than the commonly used numerical fitting procedure. The second harmonic zero-crossing separation method calculated an even 6 orders faster than the spectra fitting without losing any accuracy for Lorentzian dominated cases. Additionally, linewidth calculated through second harmonic zero-crossing was preferred for much smaller error than the first harmonic peak-to-valley separation method. The presented analytical expressions can also be used in on-line optical sensing applications, electron paramagnetic resonance, and further theoretical characterization of absorption lineshape.     

Observation of photon recoil effects in single-beam absorption spectroscopy with an ultracold strontium gas

We report on observing photon recoil effects in the absorption of a single monochromatic light at 689 nm through an ultracold ⁸⁸Sr gas,where the recoil frequency is comparable to natural linewidth of the narrow-line transition 5s^{2 1}S₀-5s5p ³P₁ in strontium.In the regime of high-saturation,the absorption profile becomes asymmetric due to the photon-recoil shift,which is of the same order as the natural linewidth.The lineshape is described by an extension of the optical Bloch equations including the momentum transfers to atoms during emission and absorption of photons.Our work reveals the photon recoil effects in a simplest single-beam absorption setting,which is of significant relevance to other applications such as saturation spectroscopy,Ramsey interferometry,and absorption imaging.     

可调谐掺铥光纤激光器线宽压缩及其超光谱吸收应用

可调谐二极管激光吸收光谱技术是一种应用非常广泛的吸收光谱测量技术.利用宽带可调谐窄线宽光源进行吸收光谱测量的超光谱吸收技术可以在单次扫描中获取一段连续光谱的所有吸收数据,可大大提高可调谐二极管激光吸收光谱技术的数据信息容量和光谱诊断能力.分析了在2μm波段对水进行超光谱吸收测量时对激光器输出线宽的具体要求.利用掺铥光纤在2μm波段较宽的发射谱,采用可调谐法布里-珀罗滤波器和光纤可饱和吸收体相结合的技术方案搭建了一台宽带调谐窄线宽的2μm光纤激光器.获得了1840—1900 nm约60 nm范围的调谐光谱输出,激光器静态线宽仅为0.05 nm.利用该光源对空气中水在2μm波段的吸收光谱数据进行了超光谱吸收测量,在1856—1886 nm约30 nm的光谱范围内分辨了35条水的吸收谱线.通过对不同线宽条件下1870—1880 nm范围内的理论吸收光谱数据进行对比发现,测量数据无法有效分辨分别位于1873 nm和1877 nm处与强吸收线相邻的两条吸收谱线,且测量结果与激光线宽在0.08 nm条件下的HITRAN2012光谱数据库最为接近.这表明,在动态扫描过程中激光器的线宽得到了展宽.     

Analytical evaluation of the Fourier components of wavelength-modulated Gaussian functions

Modulation techniques are often used in experiments where noise levels are significant, enabling weak signals to be detected. Gaussian lineshapes can be present in situations such as with tunable diode laser absorption spectroscopy of low-pressure gases, requiring the evaluation of the Fourier components of Gaussian lineshapes. These Fourier components have been evaluated only numerically in the past. In the present research, we derive exact analytical expressions for the Fourier components of a modulated Gaussian signal. We also evaluate the dimensionless modulation amplitudes that maximize the even and odd harmonics.     

STUDY OF THE DOPPLER-FREE OPTICAL-OPTICAL TRIPLE-RESONANCE(DF-OOTR) SPECTROSCOPY AND ITS LINESHAPES

The Doppler-free optical-optical triple-resonance(DF-OOTR) spectroscopy and its line-shapes have been studied in detail theoretically and experimentally. The line center, linewidth and lineshape of an isolated DF-OOTR spectra component have been derived by using density matrix motion equation describing the interaction of a three-level system with three optical fields. The variations of the lineshape symmetry, the relative position and the strength of the Doppler-free Lorentzian dip to its background are comparable to the experimental traces varying with the relative intensities of the two mutual-saturating probe laser beams, as well as with the detuning of the first pumping laser from the intermediate level. The DF-OOTR technique shows a distinguished advantage especially in the labeling of the transitions and in the determination of absolute position of the upper level affected by perturbation shift, as these happened often in the dense molecular highly excited states.     

Development of high power ch3f laser systems for plasma diagnostics1

The operating characteristics of high power pulsed 496 μm CH₃F laser systems have been studied. A theoretical model which describes both the optical pumping and submillimeter wave emission has been developed. This model is used to account for measurements of saturated absorption of 9.55 μm CO₂ laser radiation in CH₃F gas. A 9 kW CH₃F oscillator has been built. This oscillator is characterized by a power conversion efficiency of ∼ 0.15% and dominant single longitudinal mode operation. The linewidth of this mode was ∼ 28 MHz. An oscillator amplifier system has been constructed and tested. Measurements of the frequency distribution of the radiation from this system indicate that the lineshape of the oscillator signal is preserved. Narrow linewidth CH₃F radiation in the 200 kW-1 MW range should be attainable by appropriate scaling of the present oscillator amplifier system.