Change in the states of optically excited Rb atoms near sapphire surface

The changes in the states of excited Rb atoms approaching a single-crystal sapphire surface have been investigated by methods of laser-excitation spectroscopy and luminescence of Rb vapor in a cell with sapphire windows, the gap between which was varied from 250 to 500 nm. Upon resonant excitation of Rb atoms by two semiconductor lasers with powers of 20 and 40 mW, luminescence from optically excited 5D _3/2 and 5D _5/2 states and optically unexcited 6P _1/2 and 6P _3/2 states is observed. It is established that the luminescence intensity from unexcited states is only a few times lower than that from excited states, with allowance for the fact that excited atoms are rapidly and almost completely quenched on the sapphire surface. The found anomalously strong luminescence from optically unexcited 6P _J states is explained by their nonradiative occupation near the sapphire surface from optically excited 5P _J states, in which atoms fail to reach the sapphire surface because of the repulsion from it. This repulsion is due to the polarization interaction between sapphire and the atoms in the 5P _J states near the surface. Nonradiative transition from the 5P _J state to the 6P _J ^?1 state is accompanied by excitation of two optical phonons in sapphire.     

激发态铯原子间的碰撞能量转移

用激光抽运基态Cs₂分子,通过预离解或碰撞转移,由一部分的激发态Cs₂产生Cs原子6P,5D激发态。测量了Cs(5D)+Cs(6P)→Cs(7D_J)+Cs(6S)碰撞激发能量转移截面σ_(7DJ),以及Cs(7D_J)+Cs(6S)→除Cs(7D)外的态的截面σ_tr。结果是,对于J=5/2,3/2,σ_(7DJ)(以 关键词：     

Atomic and molecular ions in intense ultra-fast laser fields

The interaction of a 60 fs 790 nm laser pulse with beams of Ar⁺, C⁺, H₂ ⁺, HD⁺ and D₂ ⁺ are discussed. Intensities up to 10¹⁶ Wcm^-2 are employed. An experimental z-scanning technique is used to resolve the intensity dependent processes in the confocal volume.Received: 6 January 2003, Published online: 15 July 2003PACS: 32.80.Fb Photoionization of atoms and ions - 33.80.Rv Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states) - 42.50.Hz Strong-field excitation of optical transitions in quantum systems; multiphoton processes; dynamic Stark shift     

Even-parity states of the Sm atom with stepwise excitation

Two-colour stepwise excitation and photoionization schemes are adopted to study the spectra of high-lying states of the Sm atom. These bound even-parity states are excited with three different excitation paths from the 4f66s6p7DJ (J = 1, 2, 3) intermediate states, respectively. They are probed by photoionization process with an extra photon driving them to the continuum states. In this experiment, 270 states are detected in an energy range from 36160 cm-1 to 42250 cm-1, 109 of which are newly discovered, while the rest of them are confirmed to be the energy levels reported previously. Furthermore, based on the J-momentum selection rules of three excitation paths, a unique assignment of J-momentum for all observed states is determined, eliminating all remaining ambiguities in the literature. Finally, 53 single-colour transitions originating from the scanning laser are also identified. For all the relevant transitions, the information about their relative intensities is also given in the paper.     

Ba原子6pnd(J=1, 3)自电离光谱的实验研究

采用三台可调谐激光实施孤立实激发,分三步将处于基态的Ba原子激发到6p_1/2nd(J=1,3)和6p_3/2nd(J=1,3)自电离态上,获得了分别从6snd¹D₂(n=7—15)和6snd³D₂(n=7—12) 激发而得到的6p_1/2nd(J=1,3)和6p_3/2nd (J=1,3)自电离光谱,重点对主量子数n较低的自电离态进行了实验研究. 通过光谱的线形拟合得到了上述能级的位置和宽度等数据,进而获得了量子亏损和约化宽度等信息. 通过对不同系列的自电离光谱的分析和比较,详细讨论了这些自电离态的光谱特征及其复杂光谱结构的成因. 关键词： 孤立实激发 组态相互作用 自电离态     

Steady state signal in the limit of weak optical pumping with D1 or D2 line

The simplified rate equations for electronic polarization of alkali atoms in the hyperfine ground states are shown for circularly polarizedD ₁ andD ₂ lines in the limit of weak pumping. The rate equations include effects due to collisional and spin exchange relaxation of atoms in the ground state. Analytical forms of the repopulation pumping terms are shown assuming the standardJ-randomization model for relaxation of alkali atoms in resonant² P _J states and neglecting energy transfer. Analyses of the analytical steady state solutions have been performed to determine the conditions at which the longitudinal electronic orientation of alkali atoms 〈S _z〉 and the orientation of atoms in hyperfine sublevels 〈S _z〉 _f pass through zero.     

Spectroscopic investigations on NO+(x1∑+,a3∑+,A1Ⅱ) ion using multi-reference configuration interaction method and correlation-consistent sextuple b

Three low-lying electronic states (x¹∑⁺,a³∑⁺,and A¹Ⅱ) of NO⁺ ion are studied using the complete active space self-consistent-field (CASSCF) method followed by highly accurate valence internally contracted multi-reference configuration interaction (MRCI) approach in combination of the correlation-consistent sextuple basis set augmented with diffuse functions, aug-cc-pV6Z. The potential energy curves (PECs) of the NO⁺(x¹∑⁺,a³∑⁺,A¹Ⅱ) are calculated. Based on the PECs, the spectroscopic parameters R_e, D_e, ω_e, ω_eχ_e, α _e, B_e, and D₀ are reproduced, which are in excellent agreement with the available measurements. By numerically solving the radial Schrödinger equation of nuclear motion using the Numerov method, the first 20 vibrational levels, inertial rotation and centrifugal distortion constants of NO⁺(x¹∑⁺,a³∑⁺,A¹Ⅱ) ion are derived when the rotational quantum number J is equal to zero (J = 0) for the first time, which accord well with the available measurements. Finally, the analytical potential energy functions of these states are fitted, which are used to accurately derive the first 20 classical turning points when J = 0. These results are compared in detail with those of previous investigations reported in the literature.     

The quenching of Pb(6p 2 1 D 2) atoms in collisions with molecules

The collisions of metastable Pb(6p ^{2 1} D ₂) atoms with various molecules were studied by the diagnostics of radiation from a hollow cathode lamp and a laser on lead vapor. Experiments were performed for a gas flow of lead atoms with argon. The Pb(6p ^{2 1} D ₂) states were excited in a gas discharge in the presence of reagent gas molecules. The absolute rate constants for the quenching and chemical reactions of lead atoms in the ground and excited states were determined. The quantum efficiency of chemical reactions was close to one for the N₂O, CH₂Cl₂, SF₆, and CuBr molecules. Long-lived chemical compounds were formed in these reactions.     

Polarisierte Anregung der metastabilen 6s 5d-Terme im Ba I-Spektrum und Messung derg J-Faktoren

In an atomic beam experiment Ba-atoms were excited in the metastable levels of the 6s 5d-configuration by optical pumping and electron impact. The three states 6s 5d ¹ D ₂ and³ D _1,2 were populated by optical excitation of the 6s 6p ¹ P ₁- and³ P ₁-level resp., which decay partly into the metastable states. The¹ D ₂- and³ D ₃-level could be excited and aligned by impact of 50 eV-electrons. Radiofrequency transitions between Zeemansublevels were detected by resonance scattering of light and theg _J-values of the four 6s 5d-levels were measured:g _J(^1D ₂)=1.0032 (2),g _J(^3D ₁)=0.4986 (2),g _J(^3D ₂)=1.1638 (2) andg _J(^3D ₃)=1.3341 (2).     

An ab initio investigation of the low-lying electronic states of BeH

Potential energy curves(PECs) for the ground state(X 2 Σ +) and the four excited electronic states(A 2 Π,B 2 Π,C 2 Σ +,4 Π) of a BeH molecule are calculated using the multi-configuration reference single and double excited configuration interaction(MRCI) approach in combination with the aug-cc-pVTZ basis sets.The calculation covers the internuclear distance ranging from 0.07 nm to 0.70 nm,and the equilibrium bond length R e and the vertical excited energy T e are determined directly.It is evident that the X2Σ+,A2Π,B2Π,C2Σ+ states are bound and 4Π is a repulsive excited state.With the potentials,all of the vibrational levels and inertial rotation constants are predicted when the rotational quantum number J is set to be equal to zero(J = 0) by numerically solving the radial Schr¨odinger equation of nuclear motion.Then the spectroscopic data are obtained including the rotation coupling constant ω e,the anharmonic constant ωexe,the equilibrium rotation constant Be,and the vibration-rotation coupling constant αe.These values are compared with the theoretical and experimental results currently available,showing that they are in agreement with each other.     

Determination of natural radiative lifetimes and Landé factors for highly excitedF states in cesium

Natural radiative lifetimes and Landég _J factors for several highly excitedF states in cesium were measured using time-resolved fluorescence spectroscopy. TheF states were excited from the 5² D _5/2 state with a pulse-modulated CW dye laser, and the delayed-coincidence method was employed to record decay curves, which in some experiments exhibited Zeeman quantum beats. A further CW dye laser was used to produce the necessary population in the 5² D _5/2 state. The lifetimes in the sequence 11–16² F _7/2 follow an ^x scaling law withx=2.76 and the Landé factors agree with the predicted value, 1.143.     

激光束在漫射表面上的散射(Ⅱ)

首先在前文的基础上,对于用激光根据“光核、光带比”(D₂/D₁)来测定磨削工件表面光洁度的原理加以系统总结,然后按照经验关系R_x=5R_a(对于▽7以上光洁度),确定了表面随机高度的概率密度函数中的衰减系数。对于有限负指数型函数P₁(h)={e^{(-b(|h|/h_m))} 当|h|≤h_m; 0 当|h|>h_m, 定出b=1.23,对于正则型函数P₂(h)=e^{(-a2(h/h_m)2)} 定出a²=2.分别讨论了以上两种函数中h_m的物理意义(皆对应于1/2R_z)将前文中公式加以精确改进后,对P₁(h)和P₂(h)分别计算了D₂/D₁与R_x的关系曲线,即绝对定标曲线。最后还计算了衍射图样半强度宽与R_x的关系曲线。 关键词：     

基态S和D原子的低能弹性碰撞及SD(X2Π)自由基的准确相互作用势与分子常数

使用Gaussian03程序包提供的CCSD（T）理论及Duning等的相关一致基cc-pVnZ和aug-cc-pVnZ （n=2, 3, 4, 5）, 对SD（X²Π）自由基的平衡核间距、谐振频率及相互作用势进行了计算, 并拟合出了相应的光谱常数. 在CCSD（T）/aug-cc-pV5Z理论水平下, 光谱常数D₀, D_e, R 关键词： 弹性碰撞 总截面 光谱常数 分子常数     

Autler-Townes doublet in the absorption spectra for the transition between excited states of cold cesium atoms

Autler-Townes splitting in absorption spectra of the excited states 6 2 P 3/2-8 2 S 1/2 of cold cesium atoms confined in a magneto-optical trap has been observed.Experimental data of the Autler-Townes splitting fit well to the dressed-atom theory,by which the fact of the cold atoms dressed by cooling/trapping laser beams is revealed.The results of the theoretical fitting with experiment not only told us the effective Rabi frequency cold atoms experienced,but also could be used for measuring the probability amplitudes of the dressed states.     

Laser induced lasing in CS2 vapor

When CS₂, contained in a tube at pressures ranging from 350 to 450 mTorr, was optically excited by a pulsed laser at a wavelength of 343.6 nm to the J=29, v=(0, 10, 0), R ³ B ₂ state (i.e., the =0 component of the a ³ A ₂ state), six coherent emissions were observed along the same axis from both ends of the tube. These emissions possess the characteristics of the pump laser, such as linewidth, pulse duration and polarization, but do not need a cavity to gain amplification. The emissions terminate on the high vibrational states of the ground electronic state. A time delay between the pump laser and the emissions was observed. The emission intensity depends non-linearly on the CS₂ pressure and exhibits a third order power dependence. A cooperative stimulated emission model is proposed to explain this phenomenon.     

Theoretical investigations of spectroscopic parameters and molecular constants for electronic ground state of Cl2 and its isotopes

The potential energy curve of the Cl 2(X1Σg+) is investigated by the highly accurate valence internally contracted multireference configuration interaction (MRCI) approach in combination with the largest correlation-consistent basis set, aug-cc-pV6Z, in the valence range. The theoretical spectroscopic parameters and the molecular constants of three isotopes, 35Cl2, 35Cl37Cl and 37Cl2, are studied. For the 35Cl2 (X1Σg+), the values of D0 , De , Re , ωe , ωeχe , αe and Be are obtained to be 2.3921 eV, 2.4264 eV, 0.19939 nm, 555.13 cm-1 , 2.6772 cm-1 , 0.001481 cm-1 and 0.24225 cm-1 , respectively. For the 35Cl37Cl(X1Σg+), the values of D0 , De , Re , ωe , ωeχe , αe and Be are calculated to be 2.3918 eV, 2.4257 eV, 0.19939 nm, 547.68 cm-1 , 2.6234 cm-1 , 0.00140 cm-1 and 0.23572 cm-1 , respectively. And for the 37C2 (X1Σg+), the values of D0 , De , Re , ωe , ωeχe , αe and Be are obtained to be 2.3923 eV, 2.4257 eV, 0.19939 nm, 540.06 cm-1 , 2.5556 cm-1 , 0.00139 cm-1 and 0.22919 cm-1 , respectively. These spectroscopic results are in good agreement with the available experimental data. With the potential of Cl2 molecule determined at the MRCI/aug-cc-pV6Z level of theory, the total of 59 vibrational states is predicted for each isotope when the rotational quantum number J equals zero (J = 0). The theoretical vibrational levels, classical turning points, inertial rotation and centrifugal distortion constants are determined when J = 0, which are in excellent accordance with the available experimental findings.     

Infrared laser-emission study in a resonantly excited sodium vapor

We report on a study of time dependence of ir laser emission at 3.41 μm in a dense Na vapor that is resonantly excited to the 3² P levels by a flashlamp, pumped dye laser. Energy-pooling collisions (excitation transfer) between excited atoms create a large population inversion among the 5² S _1/2 and 4² P _3/2 states which is destroyed by electron collisions as a result of subsequent plasma formation. The ir laser emission may serve as a new diagnostic tool to follow the time evolution of such media.     

用双光子电离探测技术研究奇宇称的Sm原子光谱

采用两台激光器对Sm原子奇宇称激发态的光谱及其特性进行了系统研究.利用一台波长在585 nm到663 nm之间调谐的染料激光器,将Sm原子从某个4f⁶6s²⁷F_J(J=0—6)态激发到具有奇宇称的4f⁶6s6p或4f⁵5d6s²激发态.然后,采用波长固定在532 nm的强激光束,对处于上述奇宇称激发态的Sm原子进行双光子电离,以实现探测其光谱信息 关键词： 双光子电离 奇宇称态 Sm原子     

基态O和D原子的低能弹性碰撞及OD（X2Π）自由基的准确解析势与分子常数

利用CCSD（T）理论及相关一致五重基aug-cc-pV5Z构建了OD（X²Π）自由基的相互作用势, 计算了这个自由基的光谱常数D₀, D_e, R_e, ω_e, ω_eχe及B_e, 其值分别为44574,46225?eV,009702 nm, 2724923,453534和100096 cm^-1, 均与实验结果相符很好. 利用这一相互作用势, 在绝热近似下通过数值求解双原子分子核运动的径向薛定谔方程, 找到了J=0时OD（X²Π）自由基存在的全部23个振动态, 完整地求出了每一振动态的振动能级、振动经典转折点、惯性转动常数和离心畸变常数, 其值与实验结果相当一致. 在10×10^-11—10×10^-3a.u.的能量范围内研究了基态O和D原子沿OD（X²Π）势能曲线的弹性碰撞, 计算了这一碰撞的总截面和各分波截面, 分析了各分波截面对总截面的不同贡献. 结果表明: 总截面的形状主要由s分波截面决定, 尽管直到l = 12的其他分波截面均有形状共振存在, 但由于其强度较弱, 大都湮没在较强的s分波截面中. 关键词： 弹性碰撞 总截面 形状共振 光谱常数     

Resonance-enhanced multiple-photon ionisation spectroscopy of excited sulphur atoms

Sulfur atoms are produced in the excited 3s ²3p ^{4 1} D ₂ and 3s ²3p ^{4 1} S ₀ levels by two-photon photodissociation of CS₂ in the gas phase in the region 285–305 nm. These excited atoms are detected by three-photon (two to resonance) ionisation at selected laser wavelengths. Many new transitions have been observed which have not been reported previously. The new dark states that have been accessed by two-photon absorption have been characterised and the energy levels with respect to the ground ³ P ₂ state have been determined. Configuration interaction between 6p ³ P ₁, 6p ⁵ P ₁, and 4p¹ P ₁ states, and also between 6p ³ P ₂, 6p ⁵ P ₂, and 4p¹ D ₂ states has been observed. It is found that intermediate states reached from the ¹ S ₀ level through two-photon absorption lie above the first ionisation potential of S⁺(⁴ S ⁰). It is proposed that autoionisation into the ⁴ S ⁰+e^– continuum is a dominant mechanism in the decay of these levels, although ionisation by a further photon absorption is not ruled out.