利用自电离探测技术研究Sm原子Rydberg态光谱

采用孤立实激发与自电离探测技术相结合的方法对Sm原子偶宇称高激发态进行了系统研究.按照不同的自电离通道将所测数据进行了分类和比较,并进行了详细讨论.不仅报道了许多收敛于不同电离限的Rydberg态的能级位置和跃迁的相对强度等信息,而且还把处于同一能域内的Rydberg态和价态进行了辨识.另外,不但提供了一种有效识别不同类型的高激发态的鉴别技术,而且还对处于41800 cm^-1到43800 cm^-1能域内的Rydberg态和价态的光谱特性进行了详细分析和讨论. 关键词： 自电离探测 Rydberg态 Sm原子     

Sm原子的偶宇称高激发态的光谱研究

采用双色三步激发和光电离过程,对Sm原子的偶宇称高激发态的光谱进行了研究.先采用两条激发路线分别将Sm原子两步共振激发至待测的高激发态,然后利用光电离技术对其进行探测.分别将第一束激光的波长固定在627.50nm和624.41nm上,以便将Sm原子从亚稳态共振激发到由4f⁶6s6p电子组态所构成的两个原子状态上.第二束激光在440-700nm的波段范围内扫描,不仅使Sm原子在30040-38065cm^-1能域内的偶宇称高激发态上布居,将其进一步光电离,测量了其光谱.通过光谱定标和选择定则等分析手段,本工作不仅精确获得了136个态的能级位置,而且也唯一确定了其总角动量,并且给出了相关跃迁的相对谱线强度.     

Investigation of odd-parity Rydberg states of Eu I with autoionization detection

Isolated-core-excitation (ICE) scheme and autoionization detection are employed to study the bound Rydberg states of europium atom. The high-lying states with odd parity have been measured using the autoionization detection method with three different excitation paths via 4f⁷6s6p[ ⁸P_5/2], 4f⁷6s6p[ ⁸P_7/2] and 4f⁷6s6p[ ⁸P_9/2] intermediate states, respectively. In this paper the spectra of bound Rydberg states of Eu atom are reported, which cover the energy regions from 36000~cm^-1 to 38250~cm^-1 and from 38900~cm^-1 to 39500 cm^-1. The study provides the information about level energy, the possible J values and relative line intensity as well as the effective principal quantum number n^* for these states. This work not only confirms the previous results of many states, but also discovers 11 new Rydberg states of Eu atom.     

铕原子奇宇称高激发态共振电离光谱的研究

采用光电离探测和自电离探测这两种不同的探测方法对铕原子的高激发态光谱进行了详细研究.一方面,采用光电离探测技术,系统测量了在第一电离限之下处于43927—45010 cm^-1能域内的奇宇称能级的光谱.通过光谱定标和误差估算等分析手段,获得了32个共振跃迁峰的位置和强度等光谱信息.并根据所用的激发路线和相关的选择定则等原理,进而确定了这些能级的总角动量. 通过与相关文献资料的对比和分析,研究发现了12个新能级.另一方面,精心设计了一种能够有效识别不同类型高激发态的鉴别方法.对同一能域中 关键词： Eu原子光谱 奇宇称高激发态 孤立实激发（ICE） 自电离探测     

Eu原子偶宇称高激发态的场电离探测

利用共振激发技术和电场电离(EFI)方法研究了铕(Eu)原子偶宇称高激发态。实验共探测到89个态,其中报道了56个态的能级位置和光谱归属等信息。经过对有效主量子数和量子亏损进行理论分析,并结合文献结果的对比,不但认定它们属于4f76s(9S)np(8PJ或10PJ)里德伯系列,还填补了该系列中n=19～39各态的文献空白。另外,建议将Eu原子第一电离限修正为45734.2cm-1,同时解释了在其附近所观察到的宽峰的物理机制。     

Photoionization spectra of even-parity states of Sm atom with multistep excitation

Two-color stepwise excitation and photoionization schemes are adopted to study the spectra of bound even-parity high-lying states of the Sm atom with three different excitation paths via the 4f⁶6s6p ⁷D_J (J=1, 2 and 3) intermediate states. In order to obtain the information of these high-lying states, the Sm atom in these high-lying states is photoionized with an extra photon. Among 231 states detected in the energy region between 35,545 and 44,225 cm⁻¹, 108 states are newly discovered, while the rest can be identified as the same with the literature. In most cases, comparisons of the spectra corresponding to the three different excitation paths may partially determine the total angular momentum of the observed peaks with the selection rules. In addition, the relative intensities of all related transition lines are given.     

Eu原子4f~76snlRydberg态的研究

利用三步双色共振激发技术和三步三色孤立实激发技术,系统地研究了铕原子在42250—44510 cm~(-1)能域内的光谱特性,提供了该能域内56个束缚高激发态的光谱信息.为了能确定这些态的光谱归属,进行了两方面的探索:第一,观察能否利用孤立实激发技术,把处于这些态上的铕原子进一步共振激发到自电离态,从而推断这些态属于单电子激发的束缚Rydberg态还是属于双电子激发的价态,并对Rydberg态的电子组态进行了光谱确认;第二,通过计算这些态相对于各个电离阈的量子亏损并观察它们分别收敛于哪个电离阈,以便获取其主量子数的信息.最后,设计并采用了三种不同的激发路径,分别将原子布居到同一高激发能域并探测它们在该能域的光电离光谱.通过比较这些光谱的异同并结合上述激发路径所对应的跃迁选择定则,便可惟一地确定这些高激发态的总角动量.研究发现:所探测到的高激发束缚态只有三个属于单电子激发的束缚Rydberg态,其余都是价态.本文确定了这三个Rydberg态的电子组态和原子状态.     

Energy level analyses of even-parity J = 1 and 2 Rydberg states of Sn I by multichannel quantum defect theory

This paper analyzes the energy levels along the even-parity J=1 and 2 Rydberg series of Sn I by multichannel quantum defect theory. A good agreement between theoretical and experimental energy levels was achieved. Below 59198 cm-1, a total of 85 and 23 new energy levels, respectively, in the J=1 and J=2 series, which cannot be measured previously by experiments, are predicted in this work. Based on the calculated admixture coefficients of each channel, interchannel interactions were discussed in detail. The results are helpful to understand the characteristics of configuration interaction among even-parity levels in Sn I.     

用光电离技术探测钐原子的奇宇称束缚激发态的光谱

采用光电离探测方法,对钐原子奇宇称束缚激发态进行了系统研究.通过设计三条不同的激发路径, 采用共振激发方式,先将钐原子分三步从基态激发到不同的束缚激发态,然后采用光电离手段对其进行探测. 通过对第三步激发光的波长进行大范围的扫描,在同一能域内获得了三组不同的光谱. 通过比对三条路径所得到的三组光谱,不仅精确确定了大量奇宇称束缚激发态的能级位置, 而且还获得了相应跃迁的相对强度的信息.最后,通过运用三条不同的激发路径的选择定则, 还确定了上述能级的总角动量. 关键词： 钐原子 束缚激发态 奇宇称 光电离探测     

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.     

Electric field induced anomalies in frequency shift and collisional perturbations in the 5snd D2 Rydberg series of strontium in a heatpipe setup with ionization detection

We have examined the effect of weak DC electric field (2-20 V/cm) complimented by foreign gas collisions on the bound J = 2 even-parity 5snd ¹D₂ Rydberg states of neutral strontium. We use resonant two-photon transverse excitation, employing a narrow bandwidth tunable dye laser and an atomic jet in a heatpipe setup with ionization detection. In this paper we report certain anomalies in the observed spectra covering principal quantum number range n = 27-42 indicating a frequency shift reversal with nearly quadratic dependence on the field strength above an anti-resonance region. Furthermore, we have observed the emergence of highly localized doubly-excited 4d² states, including a remarkably broad perturber with large angular momentum, uncovering orbital contraction effect. This non-Rydberg excitation, which intrudes upon the two-photon spectrum with large energy overlap is due to single-photon excitations from the 5s5p ¹P₁ resonance level following molecular dissociation of the Sr₂ dimers suitably governed by binary atomic collisions. Our study which involves laser excitation complimented by electric field and collisions using inexpensive home-made setup opens up the possibilities for a new class of experiments, with considerable simplicity in the choice of excitation schemes for both Rydberg and non-Rydberg transitions, to reach states lying at high energies which cannot otherwise be accessed from the ground state due to parity and selection rules, while allowing one to probe localization properties of atomic wave functions.     

CASPT2 and CCSD(T) calculations of dipole moments and polarizabilities of acetone in excited states

The acetone molecule is investigated in its ground state and valence ^1,3n-π*, ^1,3π-π*, and ^1,3σ-π* excited states and Rydberg ^1,3n-3s, ^1,3π-3?, ^1,3n-3p_y and ^1,3π-3p_y states using the CASSCF, CASPT2, and CCSD(T) methods. Equilibrium geometries of excited states are obtained and their changes with respect to the ground state are discussed. For most excited states the C_2v symmetry of the ground state is lowered to the C_s symmetry. A series of valence vertical and adiabatic excitation energies is presented along with excitation energies for Rydberg states. The main body of the paper contains Finite-Field Perturbation Theory (FFPT) calculations of electric properties of the vertically as well as geometry relaxed excited states. Dipole moments of valence excited states decrease significantly upon excitation, being about one half of the ground state dipole moment. Polarizabilities usually change upon excitation much less (increase by about 30%) but hyperpolarizabilities are enhanced up to one or two orders of magnitude. The orientation of the dipole moment is reversed in some vertically excited Rydberg states. Properties of the ground and excited states are discussed considering alterations of the electronic structure and shifts in the geometry.     

利用光电离技术研究奇宇称的Sm原子光谱

采用一台频率可扫描的染料激光器将Sm原子从4f66s2 7FJ(J=1,2)态分别激发到具有不同电子组态的若干原子态上,然后利用光电离技术对处于上述状态的Sm原子进行高灵敏探测.通过波长固定在355nm的紫外激光器,我们对一系列具有4f66s6p或者4f55d6s2电子组态的原子状态进行了精密的光谱测量.本实验研究不但确定了这些态的能级位置,还给出了它们的相对光谱强度.通过理论方法对光谱数据详细的分析,我们不但确认了文献中Sm原子的部分奇字称能级的位置和光谱标识,还同时给出了许多新的跃迁及其光谱特性.     

Inelastic electron collisions with Rydberg atoms

The standard classical method of computer simulation is used for evaluation of the inelastic cross section in electron collisions with a highly excited (Rydberg) atom. In the course of collision, the incident and bound electrons move along classical trajectories in the Coulomb field of the nucleus, and the scattering parameters are averaged over many initial conditions. The reduced ionization cross section of a Rydberg atom by electron impact approximately corresponds to that of atoms in the ground states with valence s-electrons and coincides with the results of the previous Monte Carlo calculations. The cross section of an atom transition between Rydberg atom states as a result of electron impact is used for finding the stepwise ionization rate constant of atoms in collisions with electrons or the rate constant of three-body electron-ion recombination in a dense ionized gas because these processes are determined by kinetics of highly excited atom states. Surprisingly, the low-temperature limit of electron temperatures is realized when the electron thermal energy is lower than the atom ionization potential by about three orders of magnitude, as follows from the kinetics of excited atom states. The article is published in the original.     

An ab initio molecular orbital study of the electronically excited and cationic states of the ozone molecule and a comparison with spectral data

A number of valence and Rydberg, singlet and triplet excited states for ozone in the excitation energy range 1–12eV have been calculated by large scale CI methods preceded by MCSCF studies. A comparison of the theoretical intensity envelope with the VUV + EELS spectrum has been made. The present work supports the assignments for the Huggins + Hartley bands as having two electronic origins, 2 ¹A₁ and 1 ¹B₂. The experimental ～ 9.3eV and ～ 10.2eV bands of the VUV spectrum must have adventitious superposition of valence states on Rydberg transitions, because the high oscillator strengths of the valence states cannot be attributed to the 8.8eV broad band. A number of new valence and Rydberg states have been calculated, and these lead to the conclusion that the experimental 9–11 eV VUV spectral range in particular must yield more experimental states than the few so far identified. This suggests a major need for more sophisticated methods of experimental study for the excited state manifolds. The use of various MCSCF/CI studies of the vertical cationic states, supports the IP order as ²A₁ < ²B₂ < ²A₂. A re-analysis of the 12–13.4eV range of the UV-photoelectron band has been performed, with a view to determining the adiabatic IPs more accurately. The present work suggests that the adiabatic IP₂ lies at 12.86eV, slightly lower than has been assumed, with consequential effect on the analysis of the VUV spectrum near 9.4eV.     

The threshold electron impact spectrum of molecular oxygen

The threshold electron impact spectrum of molecular oxygen has been studied using a high energy resolution electron spectrometer in the energy region 2-15.2 eV and the penetrating field method for scattered electrons. The measured features such as core excited resonances as well as Rydberg and valence states are measured in threshold and metastable spectra. They are identified and assigned according to their energy positions, energy spacing between vibrational levels and compared with similar data from the literature. A good agreement was found in the energy positions between measured features and corresponding potential energy diagram for Rydberg states for molecular oxygen given by Morrill et al. [1].Received: 13 January 2004, Published online: 20 April 2004PACS: 34.80.Gs Molecular excitation and ionization by electron impact     

铈原子偶宇称自电离态激光共振电离光谱

给出了利用三色三光子激光共振电离光谱技术研究铈原子偶宇称自电离态的结果。27个有较大跃迁截面高奇宇称激发态被用作第二激发态。第三台染料激光波长在634～670nm范围内扫描,发现了141个偶宇称自电离态能级。为了寻求最佳电离方案,对有较大自电离态能级跃迁截面的各电离路径进行了初步的判定,推荐了8条较佳的电离路径。     

Cl2分子Rydberg态及混合Rydberg-价态多光子光谱

本工作结合多光子离化谱,激光诱导荧光及荧光激发谱技术,仔细研究Cl₂分子高激发Rydberg态和混合Rydbery-价态的结构及性质,定域了1¹∑_u⁺态内区的位置,证明2¹∑_u⁺态强的Rydberg-价混合特征,发现一新的u对称性Rydberg态并建议标识为¹∑_u态的激发,对三光子激发过程,2^{1关键词：}     

Resonance three-photon ionization of samarium atom by laser radiation in the range from 17200 to 17900 cm−1

For the first time, three-photon ionization of a samarium atom in the spectral range between 17200 and 17900 cm^?1 was studied. More than 300 peaks with different amplitudes and shape are revealed in the spectral efficiency of the Sm⁺ ion formation. The majority of peaks observed is attributed to two-photon excitation of the bound even-parity states in the energy range above 35780 cm^?1. The energies and the total momenta of the states are determined.     

Rydberg quantum computation with nuclear spins in two-electron neutral atoms

Alkaline-earth-like (AEL) atoms with two valence electrons and a nonzero nuclear spin can be excited to Rydberg state for quantum computing. Typical AEL ground states possess no hyperfine splitting, but unfortunately a GHz-scale splitting seems necessary for Rydberg excitation. Though strong magnetic fields can induce a GHz-scale splitting, weak fields are desirable to avoid noise in experiments. Here, we provide two solutions to this outstanding challenge with realistic data of well-studied AEL isotopes. In the first theory, the two nuclear spin qubit states |0〉 and |1〉 are excited to Rydberg states |r〉 with detuning Δ and 0, respectively, where a MHz-scale detuning Δ arises from a weak magnetic field on the order of 1 G. With a proper ratio between Δ and Ω, the qubit state |1〉 can be fully excited to the Rydberg state while |0〉 remains there. In the second theory, we show that by choosing appropriate intermediate states a two-photon Rydberg excitation can proceed with only one nuclear spin qubit state. The second theory is applicable whatever the magnitude of the magnetic field is. These theories bring a versatile means for quantum computation by combining the broad applicability of Rydberg blockade and the incomparable advantages of nuclear-spin quantum memory in two-electron neutral atoms.