远红外激光磁共振光谱技术及对含碳自由基分子的观测

本文报道国内建成的远红外激光磁共振 (FIRLMR)光谱仪的技术特点和工作原理。该谱仪采用CO2 激光横向泵浦远红外激光 ,样品吸收池置于远红外激光谐振腔内 ,由聚丙烯薄膜与远红外激光增益池隔开以获得很高的灵敏度 ,从而对寿命很短的自由基分子进行研究。利用该光谱仪在远红外波段测量得到了多个瞬态自由基分子CCH ,CF和CH2 的光谱 ,这些自由基分子由微波放电产生的氟原子与甲烷CH4 反应生成。     

CO2激光可调谐边带的获得及特性测量

采用由CdTe晶体构成的微波行波调制器,实现了用可调微谐波对CO_2激光的高频电光幅度调制,在CO_2激光各输出支线的两侧可产生4.4GHz范围内连续调谐且频率可直读的边带.对边带特性进行了测量,结果与理论预期符合得较好.     

用于铯原子内态操控的双光子拉曼激光的产生及应用

双光子拉曼过程是一种有效制备和控制原子内态的方法, 在原子内态操控和基于原子的量子信息处理中具有重要意义. 研制用于特定原子的拉曼激光是实现该过程的重要一步. 报道了利用光纤波导相位调制器及滤波器等实现用于铯原子内态操控的拉曼激光的方法, 并成功用于单个铯原子的内态精密操控. 通过4.6 GHz的微波信号源直接驱动波导相位调制器高效地获得光场的调制边带, 并利用自由光谱区为9.19 GHz的法布里-珀罗腔将载波及二阶边带滤掉, 获得了频率精确、相差9.19 GHz的拉曼激光. 经过基于光纤振幅调制器的功率稳定系统, 最终可以获得总功率为73 μupW、长时间内波动为2.2%的拉曼激光束, 并将此光束用于激发单个铯原子, 实现了|6S_1/2, F=4, mF=0和|6S_1/2, F=3, mF=0 之间的可控拉比操作.     

WnSi02,±(n=1～5)团簇结构与光谱的理论研究

利用密度泛函理论(DFT)在B3LYP/Lanl2dz水平上对WnSi0,2±(n=1～5)团簇的各种可能构型进行了几何结构优化,预测了各团簇的基态结构.并对基态构型的平均结合能、能隙、红外光谱及拉曼光谱进行了系统的理论分析.结果表明:WnSi0,2±(n=2～5)团簇的基态结构及亚稳态结构中的Si-Si原子不成键,W5Si0,2±团簇的基态构型与W7团簇的基态构型相似,W3Si2+团簇的基态构型与W0,5±团簇的基态构型相似;W5Si2-团簇是比较理想的复合材料;WnSi0,2±(n=1～5)团簇的所有IR吸收峰都属于红外光谱中的指纹区的特征吸收区域;除W4Si2-团簇外,其它团簇都具有非刚性特性.     

CO_2激光边带光谱仪用于SF_6分子v_3带Q支吸收谱的研究

用绝对频率精度优于1.2MHz的CO_2激光边带光谱仪记录了SF_6分子v_3带Q支的多普勒受限吸收谱,光谱范围在CO_2激光10P(16)支线中心两侧,距支线中心8.0～12.4 GHz。用内插法以<6MHz的均方误差测量了百余条跃迁谱线的频率,并标识出Q_Z、Q_R、Q_X、Q_W、Q_A等亚支的谱线,量子数J从26到83。用最小二乘法拟合实验数据得到了v_3带的部分光谱常数。     

光泵远红外激光器中的光束匹配

本文对CO_2激光束与开式腔远红外激光器的匹配问题进行了分析,给出了远红外工作物质对CO_2激光的吸收率与耦合孔逸出损失之间的定量关系,指出对确定的远红外共振腔有一最佳的匹配发散角。在该角度下,工作物质有最大的激活体积,并可获得较高的远红外激光输出。     

三价稀土离子在晶体中的发光及其电子顺磁共振和电子-核双共振光谱的光学探测

我们研究了Nd~(3 )离子的荧光,实验条件如下:在有磁场Ho的情况下,同时用微波(v_M=24.10 GHz)和氩激光(19429.69cm~(-1))激发～2.0°K的LaCl_3单晶,其中少量的La~(3 )离子用Nd~( 3)离子取代。当|(?)o|和v_M的值使Nd~(3 )在它的基态~4I_(9/2)、u=5/2或光激发态~4I_(15/2),W_1,μ=1/2或~4I_(13/2),X_1,μ=1/2时有磁共振,可观察到~4G_(7/2),E_1,μ=3/2→~4I_(11/2)荧光的加强。当磁场频率与~(143)Nd核     

强耦合光机械腔中的简正模式分裂和冷却

研究由辐射压力与驱动Fabry-Perot光学腔相耦合而产生的腔光机械动力学行为. 通过量子朗之万方程具体研究了机械振子的涨落光谱、机械阻尼与共振频移和基态冷却. 随着输入激光功率的增加,振子的涨落光谱呈现简正模式分裂的现象,并且数值模拟结果和实验结果相符合. 同时推导了有效机械阻尼和共振频移. 红移边带导致了机械模的冷却,蓝移边带引起了机械模的放大. 此外,引入一种近似机制来研究振子的基态冷却,并且考虑在解析边带机制下简正模式分裂对机械振子冷却的影响. 最后,数值讨论了初始浴温度、输入激光功率和机械品质因数这三个因素对机械振子冷却的影响. 关键词： 腔光机械 辐射压力 简正模式分裂 冷却     

BeF2分子基态势能函数研究

利用密度泛函理论（DFT）B3LYP/aug-cc-PVTZ方法对BeF和BeF2分子进行计算, BeF分子的基态电子态为X2Σ+,平衡核间距Re=0.1367 nm,BeF2分子最稳定构型为D∞h构型,基态电子态为X1Σg+,离解能De=13.4 eV。利用最小二乘法拟合了BeF分子基态的Murrell-Sorbie势能函数,并得到其光谱数据与力常数。结合全局多体项展式方法,导出了基态BeF2分子基态势能函数的解析表达式,该函数准确反映了BeF2分子的结构以及静态反应特征,这些结果为进一步探索BeF2的微观分子反应动力学提供了基础。     

基于金刚石NV色心系综磁强计相干布局振荡研究

本文介绍了我们通过利用两路微波共同作用下来进行NV色心的量子调控,实验结果出现"烧孔"现象并降低线宽,与此同时得到直流磁噪声灵敏度。在连续波实验条件下,两路微波都调谐到NV色心系综基态3A2之间的共振频率,一路泵浦微波(Pump)设定为给定的频率(m_s=0?ms=±1),一路探测微波(Probe)设定为扫频。在本次实验中我们关注的是两个微波场在NV基态之间跃迁相同的情况(ms=0?ms=+1)。在这种方法下,观察到的光谱表现出一个复杂的窄线宽结构,当探测微波功率一定时,泵浦微波功率越低,线宽越窄。当泵浦微波功率不变,改变微波频率时,烧孔一直出现在改变的微波频率处,最后我们对信号进行了调制解调,由于NV色心系综磁检测的灵敏度与解调曲线的最大斜率成反比,发现相干布局现象的调制斜率提高了20%,进一步提高了直流散粒噪声灵敏度。     

The infrared spectrum of the Ar-CO complex Comprehensive analysis including van der Waals stretching and bending states

The infrared spectrum of the weakly-bound Ar-CO van der Waals complex in the 2150 cm^-1 region of the CO stretch has been studied using a continuous supersonic slit jet expansion coupled with a tunable laser spectrometer, and also with a cooled (57 K) long-path cell coupled with a Fourier transform spectrometer. Seven new subbands were observed, and previously observed bands were observed in greater detail. Four substates were thus identified for the first time, including the excited van der Waals stretching state, v ₃ = 1, and the excited bend, v ₂ = 1, within the ground CO stretching state, v _CO = 0. A comprehensive simultaneous analysis was made of all the existing infrared and microwave data on the complex for levels with K < 5, in order to obtain an accurate and self-consistent set of substate origins, rotational parameters, and centrifugal distortion parameters. A strong Coriolis interaction between K = 1 of the excited bend and K = 0 of the excited stretch was analysed in detail.     

Ultrahigh-resolution spectrometer for the 5-microm wavelength region

We present an ultrahigh-resolution saturation spectrometer based on a line-tunable carbon monoxide laser near 60 THz (lambda = 5 microm). A spectral resolution of 14 kHz (Dnu/nu = 2.3 x 10(-10)) for CO fundamental-band transitions was achieved, which improves on earlier results by one order of magnitude. A frequency-locking scheme using tunable microwave sidebands provides tunability and absolute frequency control of the CO laser on the kilohertz. Transit-time broadening and pressure broadening of the observed transitions are significantly reduced by use of expanded laser beams in a 24-m absorption cell at pressures down to 0.0 1Pa. The new spectrometer is suitable for the study of saturation line shapes and the development of a new generation of frequency standards in the 60-THz region.     

Rotational Spectroscopy and Ring-Puckering Conformation of 3-Hydroxytetrahydrofuran

The microwave spectrum of 3-hydroxytetrahydrofuran was recorded using a Fourier transform microwave spectrometer; the rotational constants (MHz) are: A = 5581.8230(7), B = 3638.8316(7), and C = 2924.7410(7). Microwave spectra for four (13)C isotopic species were recorded in natural abundance. Stark effect measurements were used to determine the projections of the dipole moment on the principal inertial axes: μ(a) = 0.956(1) D, μ(b) = 0.875(2) D, μ(c) = 1.050(2) D, and μ(tot) = 1.667(2) D. The internal coordinates of the carbon and oxygen atoms were least-squares fit to the 15 moments of inertia, and the best-fit structure is a C(4')-endo envelope ring conformation, in good agreement with ab initio calculations (MP2/6-31Gdaggerdagger). Copyright 2000 Academic Press.     

Tunable far-infrared spectroscopy extended to 9.1THz

We synthesized tunable far-infrared radiation at frequencies higher than 9 THz (300 cm (-1)) by mixing CO(2) laser, (15)NH(3) laser, and microwave radiation in a W-Co metal-insulator-metal diode. We used this farinfrared radiation to accurately measure torsion-rotation transitions of CH(3)OH in the 8-9-THz region. We also measured the frequency of the aP(7, 3) (15)NH(3) laser transition.     

Rotational Spectra of XeH and Its Isotopic Species

Frequencies of rotational transitions of XeH⁺ and its isotopic species were measured in the 1–5 THz region with a highprecision far-infrared spectrometer using a tunable radiation source. Measured frequencies were analyzed together with previous microwave and infrared measurements to refine mass-independent Dunham parameters.     

The rotational spectrum and hyperfine structure of arsenic monophosphide, AsP

Arsenic monophosphide has been prepared by laser ablation of arsenic in the presence of PH₃. The J = 2-1 and 1-0 transitions in both the ground and first excited vibrational states have been measured with a cavity pulsed jet Fourier-transform microwave spectrometer. An improved equilibrium internuclear distance (r_e) has been obtained. Hyperfine structure in the rotational spectrum of AsP has been resolved and has led to the first determinations of the As nuclear quadrupole coupling constant and both nuclear spin-rotation constants. The data enable the electronic structure of AsP to be compared with those of other mixed Group 15 diatomic molecules.     

Diode laser measurements of line strengths and collisional half-widths in thev2band of14NH3 and15NH3

A tunable diode laser spectrometer was used to perform measurements of half-widths and intensities of several rotational lines in v₂-band of ammonia. The intensity measurements of 16 lines of¹⁵NH₃ allowed us to estimate v₂-band strength of this molecule at 298 K to be S_v ⁰=(550±10) cm^–2-atm^–1.     

Pressure broadening parameters of the hydroxyl radical A 2 Σ+ (υ’=0) ← X 2 Π3/2 (υ=0) transitions at ca. 308 nm

Pressure broadening widths and pressure-induced frequency shifts for the hydroxyl radical Q11([see full textsee full text]), Q21([see full textsee full text]), Q11(2), Q21(2) absorption lines in the A band at ca. 308 nm have been determined in the presence of a variety of gases (N2, Ar, Ne and He). Hydroxyl radicals were formed using either a microwave discharge or a vacuum ultra-violet photolysis of water vapour and were detected using direct absorption spectroscopy with a bandwidth normalised noise equivalent absorption sensitivity of 5 ×10-5 Hz-1/2. A tunable external cavity diode laser at 835 nm and a single-frequency continuous-wave intracavity frequency-doubled diode laser at 488 nm were used to produce tunable continuous-wave light at 308 nm by sum-frequency generation in a -BaB2O4 crystal.     

High Resolution Linear Laser Absorption Spectroscopy-Review

Throughout the optical spectral region from the visible to the far infrared, lasers have in recent years become increasingly important for high resolution spectroscopy in both laboratory measurements and practical applications. In general, laser sources can be classified into broadly tunable and discretely tunable types with the gas laser belonging to the latter. While gas lasers oscillate in narrow lines scattered throughout the optical spectral region, broadly tunable laser emissions cover a range of wide spectral region depending on the lasing media and operating characteristics. For example, the Pb-salt diode laser covers the spectral region from about 2.6 to 30 μm, the dye laser from 400 to 700 nm, the color center laser from 0.8 to 3.3 μm, the difference frequency spectrometer from 2.2 to 4.2 μm and the spin-flip Raman laser from 5.2 to 6.0 μm. The very limited tunability of the gas laser can sometimes be extended to many times the Doppler width by Zeeman tuning the gain medium or pressure broadening the gain profile or electrooptically modulating the laser output frequency with a tunable microwave source.     

Microwave Spectrum of 1-Cyano-3-fluoro-but-1-ene

The rotational spectrum of the 1-cyano-3-fluoro-but-1-ene has been recorded with a pulsed-nozzle microwave Fourier transform spectrometer over the range 6-20 GHz. The frequencies were fitted to the Hamiltonian of Watson (A-reduction, I(r) representation). The resulting rotational constants are A = 7493.404(1) MHz, B = 1211.9831(2) MHz, and C = 1096.0908(1) MHz. By comparing the experimental rotational constants with those obtained by ab initio calculations, we found without ambiguity that the stable conformation for the molecule is the one with the fluorine atom lying in the C&bond;CCN plane (CF-eclipsed conformer). Copyright 2000 Academic Press.