Electro-optic spectral tuning in a continuous-wave, asymmetric-duty-cycle, periodically poled LiNbO(3) optical parametric oscillator

We demonstrate electro-optic spectral tuning in a continuous-wave periodically poled LiNbO(3) (PPLN) optical parametric oscillator (OPO). We achieve 8.91 cm(-1) of rapid spectral tuning, with a linear tuning rate of 2.89 cm(-1) /(kV/mm), by applying electric fields up to +/-1.5 kV/mm across the crystal while it is operating within the OPO. Intentionally poling the PPLN crystal with an asymmetric domain structure enables tuning, and numerical predictions closely match the experimental observations. The tuning is considerably larger than the typical operational bandwidth of the OPO, indicating that we are in fact shifting the gain curve of the PPLN crystal.     

Wavelength modulated off-axis integrated cavity output spectroscopy in the near infrared

A novel instrument based on an improved off-axis alignment of integrated cavity output spectroscopy (OA-ICOS) in conjunction with a wavelength modulation (WM) technique, was developed using a DFB diode laser operating in the near infrared at 1.573 μm (6357.3 cm^-1). The laser-based sensor employed a 44 cm optical cavity that provided an effective absorption path length of ∼68 m. A minimum detectable absorption of approximately 3.6 ppmv Hz^-1/2 or 2.3×10^-7 Hz^-1/2 per optical pass was obtained using second harmonic detection. We demonstrated that by implementation of the WM technique to OA-ICOS in the near infrared, the detection sensitivity was improved by a factor of 14 compared to that obtained with OA-ICOS. Measurements of CO₂ mixing ratios in ambient air have been performed by using both OA-ICOS and WM-OA-ICOS techniques for performance comparison. PACS 42.62.Fi; 07.07.Df; 33.20.Ea     

Frequency-agile kilohertz repetition-rate optical parametric oscillator based on periodically poled lithium niobate

We report kilohertz repetition-rate pulse-to-pulse wavelength tuning from 3.22 to 3.7 mum in a periodically poled lithium niobate (PPLN) optical parametric oscillator (OPO). Rapid tuning over 400 cm(-1) with random wavelength accessibility is achieved by rotation of the pump beam angle by no more than 24 mrad in the PPLN crystal by use of an acousto-optic beam deflector. Over the entire tuning range, a near-transform-limited OPO bandwidth can be obtained by means of injection seeding with a single-frequency 1.5-mum laser diode. The frequency agility, high repetition rate, and narrow bandwidth of this mid-IR PPLN OPO make it well suited as a lidar transmitter source.     

Cs(6D_J)+(H_2,H_e)的反应与非反应碰撞能量转移

在样品池条件下,利用原子荧光光谱方法,测量了Cs(6DJ)与H2,He碰撞中的反应与非反应能量转移截面.利用脉冲激光886nm线双光子激发Cs(6S)到Cs(6D3/2)态,原子荧光中除含有6D3/2→6P的直接荧光外,还含有6D5/2→6P的转移荧光.利用三能级模型的速率方程分析,在不同的He和H2密度下,分别测垦直接荧光与转移荧光的时间积分荧光强度比,得到了6D3/2与H2和He碰撞的精细结构转移截面分别为σ=(55±13)×10-16和(16±4)×10-16 cm2,同时确定了6D5/2与H2和He的碰撞猝灭速率系数.6D5/2态与H2的碰撞猝灭速率系数比6D5/2与He的大,它是反应与非反应速率系数之和,利用实验数据确定非反应速率系数为6.3×10-10 cm3·s-1,得到6D5/2与H2的反应截面为(2.0±0.8)×10-16 cm2.利用不同H2(或He)密度下6D5/2→6P3/2时间积分荧光强度,得到6D3/2与H2反应截面为(4.0±1.6)×10-16 cm2,6D3/2与H2反应的活性大于6D5/2.     

ZnGeP2 optical parametric oscillator with 3.8-12.4-mum tunability

A ZnGeP>(2) (ZGP) optical parametric oscillator (OPO) with wide mid-IR tunability has been demonstrated. The singly resonant angle-tuned ZGP OPO was pumped by 100-ns erbium laser pulses at lambda =2.93mum and yielded output that was continuously tunable from 3.8 to 12.4 mum (type I phase matching) and from 4 to 10 mum (type II phase matching). An OPO pump threshold was less than 1 mJ in the whole 4-12 mum range of the output, and the quantum conversion efficiency reached 35%. An OPO linewidth was typically a few wave numbers; however, with a single intracavity etalon (uncoated Si plate) in a type II OPO it was narrowed to <0.5cm(-1). We demonstrate the sensitive detection of N(2)O gas with the narrow-linewidth OPO.     

Broadly tunable noncritically phase-matched ZnGeP2 optical parametric oscillator with a 2-microJ pump threshold

We report a high-repetition-rate (1-10-kHz) optical parametric oscillator (OPO) based on noncritically phase-matched ZnGeP2 (ZGP). The pump source was an OPO based on periodically pole lithium niobate that was pumped in turn by a Q-switched diode-pumped 1-microm Nd:YAG laser. The ZGP OPO yielded continuously tunable output from 3.7 to 10.2 microm by tuning of the pump wavelength from 2.3 to 3.7 microm. At the optimal pump focusing, the minimum ZGP OPO threshold achieved was 2 microJ, which is to our knowledge the lowest ever reported for a singly resonant OPO. The output energy in the 6-8-microm range was > 20 microJ, and the quantum efficiency of converting 1-microm radiation to the mid IR exceeded 10%.     

高位K2(1Λg) 与基态原子的碰撞转移

在K原子密度约为0.5～5×1016cm-3的样品池中,脉冲激光710 nm线双光子激发K2基态到高位1Λg态,研究了K2(1Λg)+ K(4S)碰撞转移过程.K原子密度由测量KD2线蓝翼对白光的吸收得到.测量不同K密度下1Λg态发射的时间分辨荧光强度,它是一条指数衰减曲线,由此得到1Λg态的有效寿命,从描绘出的有效寿命倒数与K原子密度关系直线的斜率得到1Λg态总的碰撞猝灭截面为(2.1±0.2)×10-14cm2,从截距得到的辐射寿命为(22±2)ns.测量了K的6S →4P3/2和4D→4P3/2在不同K密度下的时间积分荧光强度,得到了K2(1Λg)+K→K2(11∑ +g)+K(6S,4D)碰撞转移截面为(1.5±0.3)×10-15cm2(对转移到6S)和(8.5±3.0)×10-15cm2(对转移到4D).     

Continuous wave optical parametric oscillator for quartz-enhanced photoacoustic trace gas sensing

A continuous wave optical parametric oscillator, generating up to 300 mW idler output in the 3–4 μm wavelength region, and pumped by a fiber-amplified DBR diode laser is used for trace gas detection by means of quartz-enhanced photoacoustic spectroscopy (QEPAS). Mode-hop-free tuning of the OPO output over 5.2 cm^-1 and continuous spectral coverage exceeding 16.5 cm^-1 were achieved via electronic pump source tuning alone. Online monitoring of the idler wavelength, with feedback to the DBR diode laser, provided an automated closed-loop control allowing arbitrary idler wavelength selection within the pump tuning range and locking of the idler wavelength with a stability of 1.7×10^-3 cm^-1 over at least 30 min. Using this approach, we locked the idler wavelength at an ethane absorption peak and obtained QEPAS data to verify the linear response of the QEPAS signal at different ethane concentrations (100 ppbv-20 ppmv) and different power levels. The detection limit for ethane was determined to be 13 ppbv (20 s averaging), corresponding to a normalized noise equivalent absorption coefficient of 4.4×10^-7 cm^-1  W/Hz^1/2. PACS 42.55.Wd; 42.65.Yj; 42.62.Fi     

Cs(6DJ)+Cs(6S1/2)非弹性碰撞转移截面的测定

在9×1014～2.1×1015cm-3 Cs密度范围内,利用脉冲激光双光子激发Cs(6S1/2)到Cs(6D5/2)态,使用原子荧光光谱方法,通过三能级模型的速率方程分析,由对直接荧光和转移荧光的时间积分强度的测量,得到6D5/2→6D3/2精细结构转移截面为(2.1±0.4)×10-14cm2,而6D3/2态向6D以外态的转移截面为(1.6±0.4)×10-14cm2,它应是过程Cs(6 D3/2)+Cs(6S)→Cs(6P)+Cs(6P),6D3/2→7P3/2和6D3/2→7 P1/2碰撞转移截面之和.第二个实验可以得到6 D3/2→7P3/2和6D3/2→7 P1/2的碰撞转移截面.在1×1012～6×1012cm-3的低密度Cs蒸气中,激光双光子激发6S至6D3/2或6D5/2态,测量6DJ→6PJ'与7PJ"→6S1/2的时间积分荧光强度比,得到6D3/2→7P1/2与6D5/2→7R3/2的碰撞转移截面分别为(7.6±2.4)×10-15cm2与(1.6±0.5)×10-15cm2.由此得到碰撞能量合并的逆过程即[Cs(6D3/2)+Cs(6S1/2)→Cs(6P)+Cs(6P)]的转移截面为(1.3±0.4)×10-14cm2.     

Design considerations in high-sensitivity off-axis integrated cavity output spectroscopy

Off-axis integrated cavity output spectroscopy (OA-ICOS) has generated much interest because it potentially allows highly sensitive field measurements with robust optical alignment. We discuss here design choices involved in design of an OA-ICOS instrument and how these choices impact instrument sensitivity, using as our example the design of the Harvard ICOS isotope instrument, which demonstrates the highest reported sensitivity for mid-IR OA-ICOS (2.4×10^-11 cm^-1Hz^-1/2 at 6.7 μm, obtained during measurements of water vapor isotopologues H₂O, HDO, and H₂  ¹⁸O in the laboratory and onboard NASA’s WB-57 high-altitude research aircraft). We compare the sensitivity of several OA-ICOS instruments with differing design parameters, show how comparisons are hindered by differing definitions of instrument performance metrics, and suggest a common metric of MDA_meas, the fractional absorption equivalent to 1σ uncertainty in an actual measurement, normalized to 1 s integration. We also note that despite an emphasis on sensitivity in the literature, in the Harvard ICOS isotope instrument and likely also similar instruments, systematic errors associated with fitting of the baseline laser power are of equal importance to total measurement uncertainty.     

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.     

Mid-infrared optical parametric oscillator based on ZnGeP2 pumped by 2-μm laser

We present a 3 5 μ m optical parametric oscillator (OPO) based on ZGP pumped by KTP OPO 2.1-μ m laser. The tuning curves of ZGP OPO are calculated. The 8 ×6 ×18 (mm) ZGP crystal, whose end faces are antireflection coated at 2.1 and 3.7 4.6 μ m, is cut as θ =53.5°, φ =0°. When the pump power of 2.1-μ m polarized laser is 15 W at 8 kHz, 5.7-W output power and 46.6% slope efficiency are obtained with a ZGP type I phase match. Central wavelengths of the signal and idler lasers are 4.10 and 4.32 μ m, respectively. Pulse duration is about 27 ns. Beam quality factor M 2 is better than 1.8. The tunability of 3 5 μ m can be achieved by changing the angle of the ZGP crystal.     

基于离轴积分腔输出光谱的燃烧场CO浓度测量研究

CO是碳氢燃料不完全燃烧的重要产物,常常被作为反应燃烧效率的标志物,燃烧场CO组分浓度的精确测量对提高燃烧效率、减少污染物排放具有重要意义。离轴积分腔输出光谱(OA-ICOS)是一种利用物质对激光的特异性吸收,实现对该物质分析和测量的技术,具有非接触、稳定和高灵敏度等优点。针对燃烧场CO浓度低,背景信号干扰强等特点,采用分布反馈式(DFB)激光器搭建基于离轴积分腔输出光谱的CO浓度测量系统,通过直接吸收光谱的测量方法实现对高温燃烧场CO浓度测量。利用仿真模拟的方法,在所用激光器中心波长的附近选出了常温下谱线强度较为突出,高温下不受其他燃烧产物干扰的第一泛频带R(10)吸收谱线。通过固定光程池对比吸光度的方法标定了OA-ICOS系统的有效光程;通过比较不同扫描频率下吸收谱线的信噪比和线型拟合残差标准差,得到最佳波长扫描频率;通过测量不同浓度CO混合气体的吸收信号分析了系统误差。探究了不同燃烧情况下CH₄/Air预混平焰炉上CO的产生情况,根据燃烧场测量区域温度分布情况描述了温度分布不确定度对CO测量结果的影响。当量比为1.0时,在10 ms的测量时间分辨率下,噪声等...     

1.315 μm波长附近实际大气高分辨率吸收光谱

 用窄线宽、脉冲可调谐光参量振荡器（OPO）作光源，使用光程长达1 097m的怀特池，采用单探测器分时复用的探测方法，首次在吸收池中精确测量了实际大气中1.315 μm波长附近高分辨率吸收光谱，实验验证了实际大气中水汽是该波段的主要吸收气体；得到了实际大气中吸收分子在氧碘激光波长（7 603.14cm^-11）处的吸收截面为 (1.05±0.09)×10^-24 cm²(标准大气条件下）以及在该波段主要吸收谱线的参数，包括吸收线的位置、线强度、压力加宽半宽度等。利用实测的线参数计算了在氧碘激光波长附近大气分子的吸收截面，发现吸收最小的波长分别位于7 603.31和7 603.93cm^-1，其值约为(8.9±0.8)×10^-25 cm²，比氧碘激光波长处的吸收截面约小15%。     

Dynamics for Reactions of Ion Pairs in Aqueous Solution: Reactivity of Tosylate Anion Ion Paired with the Highly Destabilized 1-(4-Methylphenyl)-2,2,2-Trifluoroethyl Carbocation

The sum of the rate constants for solvolysis and scrambling of carbon bridging and nonbridging oxygen-18 at 4-MeC(6)H(4)CH(CF(3))OS((18)O(2))Tos in 50/50 (v/v) trifluoroethanol/water, (k(solv) + k(iso)) = 5.4 × 10(-6) s(-1), is 50% larger than k(solv) = 3.6 × 10(-6) for the simple solvolysis reaction of the sulfonate ester. This shows that the ion pair intermediate of solvolysis undergoes significant internal return to form reactant. These data give a value of k(-1) = 1.7 × 10(10) s(-1) for internal return of the carbocation-anion pair to the substrate. This rate constant is larger than the value of k(-1) = 7 × 10(9) s(-1) reported for internal return of an ion pair between the 1-(4-methylphenyl)ethyl carbocation and pentafluorobenzoate anion to the neutral ester (4-MeC(6)H(4)CH(CH(3))O(2)CC(6)F(5)) in the same solvent. The partitioning of ion pairs to the 1-(4-methylphenyl)ethyl carbocation and to the highly destabilized 1-(4-methylphenyl)2,2,2-trifluoroethyl carbocation is compared and contrasted.     

Cs_2(B~1Π_u)态与基态Cs原子间的碰撞激发转移

在Cs2密度约为2×1013 cm-3的纯Cs样品池中,脉冲激光激发Cs2(X1 Σg+)至B 1Πu态,利用原子和分子荧光光谱方法研究了Cs2(B 1Πu)+Cs(6S)的碰撞激发转移过程.用736 nm激发Cs2到B 1Πu(v＜10),这时预解离不发生.由B 1Πu→X1 Σg+时间分辨跃迁信号得到B 1Πu态的辐射寿命为(35±7)ns,B1Πu态与Cs原子碰撞转移总截面为(4.0±0.5)×10-14 cm2.用705 nm激发至B 1Πu(v＞30)态,这时发生预解离,在不同的Cs密度下,测量了I(D1),I(D2)和分子带的时间积分荧光的相对强度,得到了预解离率为(4.3±1.7)×105 s-1(对预解离到6P3/2)和(4.7±1.9)×106 s-1(对预解离至6P1/2);碰撞转移截面为(0.45±0.18)×10-14 cm2(对转移到6 P1/2)和(4.3±1.7)×10-14 cm2(对转移到6P3/2).结果表明,如果B 1Πu(v)是束缚的,6P原子由碰撞转移产生;如果B 1Πu(v)是预解离的,则6P原子由预解离和碰撞转移产生.     

Compact, 1.5 mJ, 450 MHz, CdSiP2 picosecond optical parametric oscillator near 6.3 μm

We report a compact, efficient, high-energy, and high-repetition-rate mid-IR picosecond optical parametric oscillator (OPO) based on the new nonlinear material CdSiP(2) (CSP). The OPO is synchronously pumped by a master oscillator power amplifier system at 1064.1 nm, providing 1 μs long macropulses constituting 8.6 ps micropulses at 450 MHz, and it can be tuned over 486 nm across 6091-6577 nm, covering the technologically important wavelength range for surgical applications. Using a compact (～30 cm) cavity and improved, high-quality nonlinear crystal, idler macropulse energy as high as 1.5 mJ has been obtained at 6275 nm at a photon conversion efficiency of 29.5%, with >1.2 mJ over more than 68% of the tuning range, for an input macropulse energy of 30 mJ. Both the signal and idler beams are recorded to have good beam quality with a Gaussian spatial profile, and the extracted signal pulses are measured to have durations of 10.6 ps. Further, from the experimentally measured transmission data at 1064 nm, we have estimated the two-photon absorption coefficient of CSP to be β=2.4 cm/GW, with a corresponding energy bandgap, E(g)=2.08 eV.     

Cs(6P)+(Ne,N2)碰撞能量转移

在气体样品池条件下,研究了Cs(6P3/2) (Ne,N2)碰撞能量转移过程.用调频半导体激光器激发Cs原子至Cs(6P3/2)态,在不同的Ne或N2气压下,测量了直接6P3/2→6S1/2荧光和转移6P1/2→6S1/2荧光,对于6P3/2与Ne的碰撞,电子态能量仅能转移为Ne原子的平动能.在与N2的碰撞中,向分子振转态的转移是重要的.利用速率方程分析,可以得到碰撞转移速率系数,对于Ne,6PJ精细结构碰撞转移速率系数为1.45×10-12cm3·s-1.对于N2,测量6P Ne和6P N2二种情况下荧光的相对强度比,确定精细结构速率系数为1.64×10-12cm3·s-1,6P态猝灭速率系数为4.88×10-12cm3·s-1.     

Quartz enhanced photoacoustic spectroscopy with a 3.38 μm antimonide distributed feedback laser

A system for gas sensing based on the quartz-enhanced photoacoustic spectroscopy technique has been developed. It makes use of a quantum well distributed feedback (DFB) laser diode emitting at 3.38 μm. This laser emits near room temperature in the continuous wave regime. A spectrophone, consisting of a quartz tuning fork and two steel microresonators were used. Second derivative wavelength modulation detection is used to perform low concentration measurements. The sensitivity and the linearity of the Quartz enhanced photoacoustic spectroscopy (QEPAS) sensor were studied. A normalized noise equivalent absorption coefficient of 4.06×10(-9) cm(-1)·W/Hz(1/2) was achieved.     

Widely and continuously tunable optical parametric oscillator based on a cylindrical periodically poled KTiOPO(4) crystal

We report on what is to our knowledge the first realization of a quasi-phase-matched optical parametric oscillator (OPO) based on a crystal with a cylindrical shape. The main reason for interest in this device is its broad, continuous tuning. In experiments with a 1064-nm pump, the signal tuning range was equal to 525 nm (1515-2040 nm), and the corresponding idler was continuously tuned over 1340 nm (2220-3560 nm). The angular tuning was 26 degrees , with only a minor variation of the OPO threshold over the entire tuning range.