Fast, low-noise, mode-by-mode, cavity-enhanced absorption spectroscopy by diode-laser self-locking

A new technique of cavity enhanced absorption spectroscopy is described. Molecular absorption spectra are obtained by recording the transmission maxima of the successive TEM_oo resonances of a high-finesse optical cavity when a Distributed Feedback Diode Laser is tuned across them. A noisy cavity output is usually observed in such a measurement since the resonances are spectrally narrower than the laser. We show that a folded (V-shaped) cavity can be used to obtain selective optical feedback from the intracavity field which builds up at resonance. This induces laser linewidth reduction and frequency locking. The linewidth narrowing eliminates the noisy cavity output, and allows measuring the maximum mode transmissions accurately. The frequency locking permits the laser to scan stepwise through the successive cavity modes. Frequency tuning is thus tightly optimized for cavity mode injection. Our setup for this technique of Optical-Feedback Cavity-Enhanced Absorption Spectroscopy (OF-CEAS) includes a 50 cm folded cavity with finesse ∼20 000 (ringdown time ∼20 μs) and allows recording spectra of up to 200 cavity modes (2 cm⁻¹) using 100 ms laser scans. We obtain a noise equivalent absorption coefficient of ∼5×10⁻¹⁰ cm⁻¹ for 1 s averaging over scans, with a dynamic range of four orders of magnitude.     

CO2的腔增强吸收与高灵敏吸收光谱研究

腔增强吸收光谱(CEAS)是在衰荡吸收光谱的基础上发展起来的一种新型的直接吸收光谱技术.文章报道了用中心输出波长为1.573μm的窄线宽连续可调谐半导体激光器(DFB封装)作光源,用两块高反射率平凹透镜(在1.573μm附近,凹面反射率R～99.4%,曲率半径r～1 m)组成对称共焦腔作吸收池的腔增强吸收光谱系统.采用扫描腔长的方法改变谐振腔的模式,当激光器的输出频率与谐振腔的某一腔模之间满足共振匹配关系时,激光被耦合到谐振腔内,用探测器接收透过谐振腔的光信号,同时用波长计精确测量激光器的输出波长.在33.5 cm长的吸收池内测量了吸收强度为1.816×10-23cm-1·(molecule·cm-2)-1的二氧化碳分子的弱吸收谱线,探测灵敏度达到了6.78×10-7 cm-1.实验结果表明,腔增强吸收光谱具有灵敏度高,装置简单,易于操作等优点.     

Optical-feedback cavity-enhanced absorption spectroscopy with a quantum cascade laser

Optical-feedback cavity-enhanced absorption spectroscopy is demonstrated in the mid-IR by using a quantum cascade laser (emitting at 4.46 μm). The laser linewidth reduction and frequency locking by selective optical feedback from the resonant cavity field turns out to be particularly advantageous in this spectral range: It allows strong cavity transmission, which compensates for low light sensitivity, especially when using room-temperature detectors. We obtain a noise equivalent absorption coefficient of 3 × 10(-9)/cm for 1 s averaging of spectra composed by 100 independent points. At 4.46 μm, this yields a detection limit of 35 parts in 10(12) by volume for N(2)O at 50 mbar, corresponding to 4 × 10(7) molecules/cm(3), or still to 1 fmol in the sample volume.     

磁旋转腔增强光谱技术

为了提高吸收光谱的探测灵敏度,在弱吸收或短光程吸收的情况下实现高灵敏探测,将腔增强光谱技术与磁旋转光谱技术有效地结合起来,发展了高灵敏的磁旋转腔增强吸收光谱技术,并通过测量O2 的三重禁戒跃迁谱线验证了该技术的探测灵敏度。实验采用环型增强腔,以避免光束的返回对激光器的干扰。给出了腔的耦合匹配条件,以及镜面反射率、腔损耗对增强因子的影响;同时也给出了在实验中对光谱信号的处理方法。测量结果表明,在谐振腔精细度为F=48,腔内总损耗为13%,以及腔镜的耦合效率为 95%的情况下,对 O2 分子最小相对吸收度约为4.5×10-8(1 s积分时间)。     

Saturated absorption spectroscopy of acetylene molecules with an optical nanofiber

We performed saturated absorption spectroscopy of acetylene (C?H?) ν? + ν? band transitions with an optical nanofiber (ONF). Owing to high-intensity light around the ONF, we observed a Lamb dip at relatively low-power laser (~10 mW) without a cavity. Our results showed that the simple ONF spectrometer is advantageous for performing saturation absorption spectroscopy and serves as a practical low-cost wavelength reference in the optical fiber communication band.     

Real-time detection of 13CH4 in ambient air by use of mid-infrared cavity leak-out spectroscopy

We report on spectroscopic real-time detection of (13)CH(4) in ambient air. Our measurements were carried out by means of cavity leak-out absorption spectroscopy employing a tunable cw laser in the mid-infrared spectral region near lambda = 3 mum. A CO laser in combination with tunable microwave sideband generation was used as the light source. Using a 50-cm-long ringdown cell with R = 99.98% mirrors, we achieved a detection limit of 290 parts in 10(12) (ppt) (13)CH(4) in ambient air (integration time, 100 s). The corresponding noise-equivalent absorption coefficient was 5 x 10(-9)/cm.     

Frequency-agile,rapid scanning spectroscopy: absorption sensitivity of 2 × 10−12 cm−1 Hz−1/2 with a tunable diode laser

We present ultrasensitive measurements of molecular absorption using frequency-agile rapid scanning, cavity ring-down spectroscopy with an external-cavity diode laser. A microwave source that drives an electro-optic phase modulator with a bandwidth of 20 GHz generates pairs of sidebands on the probe laser. The optical cavity provides for high sensitivity and filters the carrier and all but a single, selected sideband. Absorption spectra were acquired by stepping the tunable sideband from mode-to-mode of the ring-down cavity at a rate that was limited only by the cavity decay time. This approach allows for scanning rates of 8 kHz per cavity resonance, a minimum detectable absorption coefficient of 1.7 × 10^?11 cm^?1 after only 20 ms of averaging, and a noise-equivalent absorption coefficient of 1.7 × 10^?12 cm^?1 Hz^?1/2. By comparison with cavity-enhanced laser absorption spectrometers reported in the literature, the present system is, to the best of our knowledge, among the most sensitive and has by far the highest spectrum scanning rate.     

低温辐射计黑体腔吸收率分析

低温辐射计是目前国际上光辐射功率计量中准确度最高的测量系统,其光辐射测量不确定度可达10-5量级,目前国内仅有少数研究机构从国外引进低温辐射计开展计量研究,亟待发展国产低温辐射计替代进口产品。由于低温辐射计采用低温超导状态下的电替代测量原理进行光辐射功率测量,发展低温辐射计的难点之一在于研制黑体吸收腔这一核心光辐射接收器件,并要求黑体腔在各波长下的吸收率都要达到0.999 9以上。为研制超高光谱吸收率的黑体吸收腔,系统性分析了各影响黑体腔光谱吸收率因素,在此基础上利用蒙特卡罗光线追迹方法重点研究了光谱波长、腔体长度、黑材料漫反射系数、黑材料吸收率和入射光空间位置等对斜底黑体腔光谱吸收率的影响。研究结果表明：在300～1 100 nm波长范围内黑体腔吸收率与其内壁涂黑材料的吸收率呈正相关,且在300～1 000 nm范围内的吸收率都达到了0.999 9以上,其中在700 nm处的吸收率取得最大值0.999 941 5,表明采用该类型黑材料的黑体腔只在300～1 000 nm范围内满足低温辐射计设计要求,后续需要根据仿真和测试结果对低温辐射计在不同波长下的光电不等效性进行修正;在黑体腔结构和口径确定的情况下,黑体腔吸收率将随腔长增加而逐渐升高,在40 mm后变化趋缓,并在65 mm后逐渐趋于平衡,考虑到低温辐射计低温舱对腔体尺寸的限制,认为腔体长度与口径之比为6.5时较为合适;黑体腔吸收率还受黑材料的漫反射系数影响,随着黑材料漫反射系数的提高,腔体吸收率呈现近似线性下降,所以在选择黑体腔涂黑材料时,在吸收率等指标相同的情况下应尽量选择镜面吸收黑;黑材料吸收率从0.8到1的变化过程中,腔体吸收率提升了0.05个百分点,且黑材料吸收率为0.92时腔体吸收率可达到0.999 9以上,表明黑材料在其有效工作波长范围内任一点的光谱吸收率都要大于0.92;腔体吸收率还受入射光投射的空间位置影响,光线位置越靠近斜底腔顶点处,腔体吸收率越高,但整体吸收率变化不明显,光线位置对腔体吸收率影响只有不到0.004个百分点,几乎可以忽略,认为斜底腔不同位置处的吸收率是均匀的。研究结果对低温辐射计黑体腔研制有一定参考价值。     

Theoretical investigation on the intracavity Doppler effect in continuous wave swept-cavity ringdown spectroscopy

We theoretically investigate the spectral measurement errors that are apt to occur in continuous wave (CW) cavity ringdown (CRD) techniques suffering intracavity Doppler shifts. In the typical CW CRD scheme based on a cavity sweep operation for the resonant coupling of a probe laser into a ringdown cavity, the intracavity probe light detunes gradually over time, carrying time-dependent loss information of an absorption feature. Frequency-drifting ringdown signals are theoretically modelled and found to result in erroneous absorption spectra that exhibit the frequency shift of absorption profiles as well as linewidth broadening. PACS 42.62.Fi; 42.60.Da; 42.25.BS     

A theoretical study on the effect of a permeable membrane in the air cavity of a double-leaf microperforated panel space sound absorber

A double-leaf microperforated panel absorber (DLMPP) is composed of a two microperforated panel (MPP) with a air cavity in-between, and without any backing structure. It shows a Helmholtz-type resonance peak absorption and additional low frequency absorption, therefore it can be used as a wideband space sound absorber. In this study, a theoretical study is made to examine the effect of a permeable membrane inside the air-cavity. Permeable membranes are studied in our previous studies and proved to be effective to improve the sound absorption performance of various type MPP sound absorbers. We investigate the absorption characteristics of a DLMPP with a permeable membrane in the cavity through numerical examples, and also studied the effect of honeycomb in the cavity of the same sound absorption structure.     

Mode-by-mode optical feedback: cavity ringdown spectroscopy

We describe a new continuous wave cavity ringdown spectroscopy (cw-CRDS) approach using an extended cavity diode laser (ECDL) optically self-locked to a high finesse cavity including an intracavity glass plate under the Brewster angle. Low noise, mode-by-mode absorption spectra are recorded at a high acquisition rate (laser frequency scan greater than 400 GHz/s) and covering four orders of magnitude in absorption coefficient. Sampling spectra with the fixed high finesse cavity frequency comb provides high precision frequency markers. An original scheme for the laser beam shut-down, based on signal shape analysis and the diode laser injection current control, is presented. This scheme avoids any supplementary switching device. To retrieve ringdown processing at a kilohertz rate several exponential decay fit algorithms are compared. Performances of this new scheme are demonstrated with the observation of very weak lines of the oxygen B-band around 680 nm. Atmospheric spectra of isolated lines averaged for less than 10 s show a baseline noise of 5×10^-10 cm^-1 and a single point minimum detectable absorption loss over a one-second measurement interval of 2×10^-10 cm/ is obtained. PACS 07.88.+y; 42.55.Px; 42.62.Fi     

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。     

一种中红外腔增强甲醛检测系统的研制

介绍了研制的一种基于共轴锁模腔增强吸收光谱技术的中红外甲醛气体检测系统。系统采用了发射中心波长为3.6 μm的带间级联激光器为光源,以高精度F-P谐振腔作为气体反应池,通过激光在谐振腔内的多次反射极大地提高了有效吸收路径。为了实现甲醛检测,利用Pound-Drever-Hall（PDH）技术将激光频率和腔谐振频率锁定至波长为3 599.08 nm的甲醛吸收峰上。实验发现,谐振腔腔长容易受到外界环境的影响产生变化,导致系统失去锁定,产生测量误差;为了抑制这一现象,提高系统的准确性和抗干扰性,采用了动态PDH锁定技术,通过低频锯齿波信号对腔长进行小范围内的周期性调制,使得腔谐振频率在目标气体吸收峰附近缓慢来回变化;通过选择合适的扫描范围使得在扫描过程中激光与谐振腔保持频率锁定。系统通过光电探测器采集谐振腔透射光强信号,通过对腔透射信号进行拟合计算来确定甲醛浓度。为了验证检测系统的有效性、评估系统的性能,采用质量流量计配备了6种不同浓度的甲醛气体样品并开展了甲醛吸收光谱测量实验、系统标定实验和稳定性实验。实验结果显示,在0～10 mL·L-1范围内,腔透射信号拟合值与甲醛浓度之间呈现出良好的线性关系;通过Allan方差分析得到当积分时间为1 s时系统检测下限为52.8 nL·L-1,积分时间为14 s时检测下限可以降至3.3 nL·L-1。此外,通过增加谐振腔的腔镜反射率和腔长可以提高有效吸收路径,进一步降低检测下限。该系统灵敏度高、响应速度快,具有较好的抗干扰性和长期稳定性,在痕量甲醛检测方面具有广阔的应用前景。     

Surface plasmon-enhanced dual-band infrared absorber for VO_x-based microbolometer application

We propose a periodic structure as an extra absorption layer(i.e., absorber) based on surface plasmon resonance effects, enhancing dual-band absorption in both middle wavelength infrared(MWIR) and long wavelength infrared(LWIR)regions. Periodic gold disks are selectively patterned onto the top layer of suspended SiN/VO_2/SiN sandwich-structure.We employ the finite element method to model this structure in COMSOL Multiphysics including a proposed method of modulating the absorption peak. Simulation results show that the absorber has two absorption peaks at wavelengths λ =4.8 μm and λ = 9 μm with the absorption magnitudes more than 0.98 and 0.94 in MWIR and LWIR regions, respectively. In addition, the absorber achieves broad spectrum absorption in LWIR region, in the meanwhile, tunable dual-band absorption peaks can be achieved by variable heights of cavity as well as diameters and periodicity of disk. Thus, this designed absorber can be a good candidate for enhancing the performance of dual band uncooled infrared detector, furthermore, the manufacturing process of cavity can be easily simplified so that the reliability of such devices can be improved.     

Cavity enhanced absorption spectroscopy for N_2O detection at 2.86 μm using a continuous tunable color center laser

The cavity enhanced absorption technique is applied to N2O detection around 2.86 μm using a continuous-wave color center laser. A high-finesse triangular ring cavity is used in this technology. Transmission through the cavity is obtained by jittering the cavity-length with a piezo on one of the cavity mirrors. A minimum detectable absorption coefficient of 2 × 10-6 cm-1 is achieved with a mirror reflectivity of 99.24%, corresponding to a N2O detection limit of 600 parts per billion.     

Ba原子6s6p1P1←6s6s1S0跃迁的光腔衰荡光谱

建立了一套光腔衰荡原子束吸收光谱测量装置,并对Ba原子的6s6p¹P₁←6s6s¹S₀吸收谱线用光腔衰荡光谱方法进行了测量,得到了Ba原子在553.548nm不同温度下的吸收谱线线型.实验结果表明,该装置测量吸收灵敏度达到6×10^-7. 关键词： 光腔衰荡 吸收光谱 Ba原子     

腔衰荡光谱技术测量O2禁戒跃迁绝对吸收截面

腔衰荡光谱技术(CRDS)不仅具有较高的测量灵敏度,还可对样品的绝对吸收进行测量。采用连续激光腔衰荡光谱技术,通过测量O2分子三重禁戒跃迁b1∑g X3∑g-(3,0)带RQ(5)谱线(波数17266.090 cm-1)处,极限真空及不同气压下的衰荡时间,利用逼近法得到空腔寿命为2.9174 ms,由此拟合获得其绝对吸收截面为1.4998(±0.0967)×10-26cm2,与先前的文献估计值一致。由空腔寿命获得的谐振腔高反镜的反射比为99.989(±0.001)%,较通常的测量方法更为精确,该实验条件下的等效吸收程长比几何程长增大了约9090倍。     

Mid-infrared cavity leak-out spectroscopy for ultrasensitive detection of carbonyl sulfide

We present a ringdown absorption spectrometer based on a continuous-wave CO laser in the mid-infrared spectral region near lambda = 5 microm. Using a linear ringdown cavity (length, 0.5 m) with R > = 99.99% mirrors, we observed a noise-equivalent absorption coefficient of 7 x 10(-11) cm(-1) Hz(-1/2). This is 2 orders of magnitude improved compared with previous values. With this setup we studied the spectroscopic detection of carbonyl sulfide (here abbreviated OCS) traces in ambient air and in exhaled breath. We achieved a detection limit of 7 parts in 10(12) (parts per trillion) OCS in ambient air, which is unprecedented and shows great promise for environmental and biomedical applications.     

散弹噪声极限稳定度优于1×10-13τ-1/2的铷频标物理系统

近年来,铷原子频标研究取得长足进展,频率稳定度达到10^-13τ^-1/2量级.为进一步改善铷频标稳定度性能,本文设计了一种高信噪比物理系统.物理系统中的腔泡组件采用微波场磁力线与量子化轴方向高度平行的开槽管式微波腔,滤光泡和吸收泡独立控温.抽运光源采用了光学滤光和同位素滤光双重滤光方案.本文实测了背景光电流I₀和鉴频斜率K_d,结果分别为95 μA和7.7 nA/Hz,在此基础上计算物理系统的散弹噪声极限稳定度为7.5×10^-14τ^-1/2.研究结果表明,只要锁频环路的电子学噪声得到有效控制,铷频标的频率稳定度突破1×10^-13τ^-1/2,进入10^-14τ^-1/2量级是完全可能的.     

Controllable optical response in hybrid opto-electromechanical systems

We theoretically investigate the analog of electromagnetically induced absorption and parametric amplification in a hybrid opto-electromechanical system consisting of an optical cavity and a microwave cavity coupled to a common mechanical resonator. When the two cavity modes are driven by two pump fields, a weak probe beam is applied to the optical cavity to monitor the optical response of the hybrid system, which can be effectively controlled by adjusting the frequency and power of the two pump fields. We find that the analog of electromagnetically induced absorption and parametric amplification can appear in the probe transmission spectrum when one cavity is pumped on its red sideband and another is pumped on its blue sideband. These phenomena can find potential applications in optical switching and signal amplification in the quantum information process.