Optical Emission of Molecular Hydrogen in a Recombining Hydrogen Plasma

We observed optical emission of molecular hydrogen in a recombining hydrogen plasma with an electron temperature of 0.1 eV and an electron density of 3 × 10¹²cm^–3. The optical emission intensities of molecular hydrogen in the recombining plasma were roughly 10%–45% of those in an ionizing plasma with an electron temperature of 4 eV. The ratio was greater for a transition line originated from an excited state with a larger vibrational quantum number. Because of the low electron temperature of 0.1 eV, the production processes of excited states are not considered electron impact excitation in the recombining plasma. Possible recombination processes are discussed which produce excited states of molecular hydrogen in the recombining plasma (© 2012 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Delayed Ionization and Delayed Detachment in Molecules and Clusters

被激发到电离阈值以上的分子体系的演化依赖于激发态的特征和与连续态的耦合等多种参数. 这些特性主要是与分子体系的复杂性,更准确地说与分子的大小,态密度,内自由度中的耦合强度有关.本文通过Na2的里德堡态的自电离,富勒烯C60的延迟电离,阴离子小团簇的延迟解离研究了在小分子中起主导作用的自电离和在大分子以及团簇中出现的延迟电离之间的转变过程. 由于这些体系中相对较慢的内能转移过程,这些研究是在纳秒激光的激发下进行.     

AunPt-阴离子小团簇的量子化学研究

在相对论有效势(RECP)近似下,用基于密度泛函理论(B3LYP)的从头计算方法和LANL2DZ基组,系统研究了阴离子团簇AunPt-(n=1-5)g能的几何构型和电子态,确定了低能量异构体.结果表明.AunPt-团簇的剩余电子改变了中性团簇AunPt的稳定结构,这种影响随团簇体积的增大而减小.     

高电荷态离子N6+、O5+、Ne4+与He原子碰撞激发过程的实验研究

利用电子迥旋共振(ECR)多电荷离子源产生的高电荷态离子束和LHT—30VUV真空紫外单色仪,研究了N~6+、O~5+、Ne~4+与He碰撞激发过程,观察到单电子俘获、双电子俘获和入射离子直接激发三种激发过程。 We have investigated the excitation processes in collisions between N~(6+), O~(5+), Ne~(4+) andHe by using the ECR ionic source and the LHT-30 VUV Monochromator. The emission spectra showthat there are three channels of excitation in the N~(6+)+He collision system: (1) Single electroncapture into excited states; (2) Double electron capture into excited states; (3) Direct excitation ofincident ions.     

Spectroscopic Mapping of the Nonequilibrium between Electron and Excitation Temperatures in a 1 ATM Helium ARC

The thermostatic states of a 100 amp, 1.016 bar, free-burning helium short arc with a 10 mm electrode gap are mapped from spectroscopic measurements at eight cross sections. The theoretical model used is a multifluids model extended to consider nonequilibrium between electron and excitation temperatures, as well as simple nonequilibrium among excited electronic levels. Seven helium lines are used to determine population densities and upper level excitation temperatures. The electron density is calculated from continuum intensity measurements at C4690. Electron temperatures are found from an astrophysical method suggested by Athay and Menzel. The effective total excitation temperature is obtained by iteration using the multifluids model. The results indicate total excitation temperature values close to the usually calculated "LTE" temperatures, but electron temperatures up to three times larger than the total excitation temperature on the arc centerline near the electrodes. The ratio is approximately 1.5 in the middle of the arc. The heavy particle kinetic temperatures appear to follow the electron temperature, except near the anode, where they drop to values smaller than the total excitation temperatures.     

Singlet excited states of anions with higher main group elements

Previous studies have shown that dipole-bound excited states exist for certain small anions. However, valence excited states have been reported for some closed-shell anions, but those with singlet valence excited states have, thus far, contained a single silicon atom. This work uses high-level coupled cluster theory previously shown to reproduce excited state energies to better than 0.1 eV compared with experiment in order to examine the electronic excited state properties of anions containing silicon and other higher main group atoms as well as their first row analogues. Of the 14 anions involved in this study, 9 possess bound excited states of some kind: CH₂SN^?, C₃H^?, CCSiH^?, CCSH^?, CCNH^?₂, CCPH^?₂, BH₃PH^?₂, AlH₃NH^?₂ and AlH₃PH^?₂. Two possess clear valence states: CCSiH^? and its first row analogue C₃H^?. Substantial mixing appears to be present in the valence and dipole-bound characters for the first excited state wavefunctions of many of the systems reporting excited states, but the mixing is most pronounced with the ammonia borane-like AlH₃NH^?₂, and AlH₃PH^?₂ anions. Inclusion of second row atoms in anions whose corresponding radical is strongly dipolar increases the likelihood for the existence of excited states of any kind, but among the systems considered to date with this methodology, only the nature of group 14 atoms in small, closed-shell anions has yet been shown to allow valence singlet excited states.     

ZnS:Ho3+的光谱特性

本工作系统地研究了Ho3+在ZnS中的光谱特性。利用不同激发波长的发射光谱、激发光谱和发光衰减鉴别出29000-14000cm-1范围内的激发谱线和发射谱线所对应的跃迁。共观察到5G5′,5G4,5G5,5G6,3K8,5F2,5F3和5S2八个4f能级的发射和5G6,5G5,3K7,3H6和5G3(3L9)五个4f能级的激发。由发射光强随温度的变化规律,研究了Ho3+的5G5′和5G4,5F3和5S2能级间的多声子弛豫过程以及5G6,3K3,5F2和5F3能级间的热平衡过程。通过近带边激发下的发光行为,提出Ho3+在ZnS中的近带边激发下发光是借助于能量传递过程,不同激发态借助不同的传递途径,而且不同的发光中心也具有不同的传递机制。     

Fluorescence quenching as a method of identification of the character of photoreactions in excited states of molecules

We consider the steady-state monochromatic excitation of a luminophore that has fluorescent products. We consider how the fluorescence of singlet states is affected by different means of quenching highlying excited states such as quenching with impurities, temperature quenching, and shortening the lifetime with induced transitions in the light field. We show that the use of different methods of fluorescence quenching opens new possibilities for studying photoreactions that proceed via excited singlet states. Our consideration concerns a wide range of primary photoprocesses, such as electron density redistribution (internal electron transfer) in the excited state, protolytic reactions, intramolecular proton transfer (phototautomerization), hydrogen bond formation, intermolecular relaxation of molecules in solutions, and formation of excimers and exciplexes. The obtained relations have been used to analyze experimental fluorescence spectra of solutions of some organic compounds, including derivatives of 3-hydroxyflavone and 3-aminophthalimide, subjected to quenching by different methods.     

Properties of resonant interatomic Coulombic decay in Ne dimers

Properties of the interatomic Coulombic decay (ICD) process in Ne dimers have been obtained by tracking the formation of energetic Ne+ ions. The double photoionization cross section, deduced from the Ne+/Ne+ coincidence signal, is dominated by the ICD process and presents a threshold 280 meV below the atomic Ne+2s(-1) threshold. Rydberg excitation of a 2s electron in the dimer creates molecular Rydberg states whose Sigma and Pi symmetries have been resolved. These excited states decay by a resonant ICD process releasing an energetic Ne+ ion and a neutral excited Ne* fragment. Subsequent autoionization of the Ne* fragment explains a double photoionization threshold below the dimer 2s ionization threshold.     

绿色长余辉材料MgAl_2O_4∶Mn~(2+)的合成及其发光特性

采用高温固相法在1350℃下合成了Mn2+掺杂的MgAl2O4发光材料,利用X射线衍射对所合成样品的结构进行了表征。用209nm的紫外灯照射样品后,观察到来自Mn2+的4T1-6A1跃迁的绿色长余辉发光。发光的激发光谱表明:Mn2+-3d组态内存在一系列强的激发峰,分别在279,361,386,427,451nm,同时还有209nm处的Mn-O电荷迁移带,激发该吸收带会产生很强的绿色余辉。测量了余辉的衰减曲线及热释光谱,分析了Mn2+掺杂浓度对样品余辉性质的影响,给出了余辉产生的可能模型。     

Optical absorption in boron clusters B6 and B 6 + : a first principles configuration interaction singles approach

The linear optical absorption spectra in neutral boron cluster B₆ and cationic B₆ ⁺ are calculated using a first principles correlated electron approach. The geometries of several low-lying isomers of these clusters were optimized at the coupled-cluster singles doubles (CCSD) level of theory. With these optimized ground-state geometries, excited states of different isomers were computed using the configuration-interaction singles (CIS) approach. The many-body wavefunctions of various excited states have been analyzed and the nature of optical excitation involved are found to be of collective, plasmonic type. We also benchmark our CIS results against more sophisticated equation-of-motion (EOM) CCSD approach for a few isomers.     

Temperature dependence of the electron self-energy in a polar-crystal slab

In this paper we investigate temperature dependence of the electron self-energy in the polar-crystal slab using Green-function method. We introduce Q2D free Green's function for the first time. Numerical calculations of the electron self-energy using GaAs as an example are performed. The results show that the electron self-energy is a decreasing function of temperature. In calculation, we consider the effect of the excited states on the electron self-energy and find the ground-state energy be about 11% lower than that of bulk polaron. The results also imply that the high excited states pay a larger contribution to the electron self-energy with increasing temperature.     

Decay,interference, and chaos

We establish a close quantitative analogy between the excitation and ionization process of highly excited one electron Rydberg states under microwave driving and charge transport across disordered 1D lattices. Our results open a new arena for Anderson localization -- a disorder induced effect -- in a large class of perfectly deterministic, decaying atomic systems.Received: 15 November 2002, Published online: 8 July 2003PACS: 32.80.Rm Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states) - 05.45.Mt Quantum chaos; semiclassical methods - 72.15.Rn Localization effects (Anderson or weak localization)     

Electron exchange in dissociative excitation of molecular hydrogen using polarized electrons

The effects of electron exchange and spin orbit interaction in dissociative excitation processes in H2 molecules have been explored using excitation by polarized electrons. Observations of the circular and linear Stokes polarizations of the Balmer-alpha photons determined the alignment and orientation of the excited atomic hydrogen atoms, the excited molecular states, and the dissociative excitation processes via predissociation with short and long range transitions.     

Theoretical study of the time-resolved photoelectron spectrum of Na 2F: effects of thermal initial conditions

The excited state dynamics of the Na₂F cluster initiated by a femtosecond laser pulse is studied considering a thermally excited initial sample. Within a pump-probe set-up, the time-dependent photoelectron spectrum is calculated, which is shown to be a sensitive tool to study intramolecular motion of the cluster. Temperature effects are taken into account through thermal averaging over the time-dependent spectra obtained from different initial vibrational states of the cluster. The nuclear motion upon laser excitation is described by full-dimensional quantum wavepacket propagation using explicit, realistic pump and probe pulses. The characteristic features of the time-resolved photoelectron spectra of the Na₂F cluster, identified as due to periodic bending motion of the cluster as well as to the excitation of the stretching mode, are found to be robust against increasing vibrational temperature of the cluster beam. This finding is important for possible future experiments.     

Quantum fluctuation in excited states of mesoscopic LC circuits at finite temperature

We discuss quantum fluctuation in excited states(named thermo number states) of mesoscopic LC circuits at a finite temperature.By introducing the coherent thermo state into the thermo field dynamics pioneered by Umezawa and using the natural representation of thermo squeezing operator we can concisely derive the fluctuation.The result shows that the noise becomes larger when either temperature or the excitation number increases.     

介质阻挡放电六边形斑图稳定过程的光谱研究

采用发射光谱法,首次研究了等离子体参数及激发状态对介质阻挡放电六边形斑图稳定性的影响。在氩气/空气混合气体的介质阻挡放电中,随着电压的升高,放电丝直径增大,六边形斑图逐渐稳定,同时放电颜色由紫色逐渐变为灰白色,说明其等离子体状态及参数可能发生了变化。测量了六边形斑图放电过程中氮分子谱线和氩原子谱线相对于氩原子763.51 nm的相对强度、分子振动温度和电子激发温度随外加电压的变化。结果发现：氮分子谱线相对强度随电压增加而降低,氩原子谱线相对强度却升高;分子振动温度与电子激发温度均随电压增加而增大。这些现象表明：随着电压增大,电子能量增加。由此,氩原子激发增多,放电丝直径增大,介质表面上沉积的壁电荷面积增大,放电丝之间的相互作用增强,六边形斑图趋于稳定。     

(19)F-(19)F and (19)F-(1)H spin-spin coupling constants in cyclic FH polymers (FH)(n), n=2-6

Spin-spin coupling constants (2h)J(F-F), (1)J(F-H), and (1h)J(H-F) have been obtained for cyclic complexes (FH)(n), with n=2-6, from ab initio equation-of-motion coupled cluster singles and doubles (EOM-CCSD) calculations. Although both the Fermi-contact (FC) term and (2h)J(F-F) increase and become positive as the cluster size increases, the FC term is not a good quantitative approximation to (2h)J(F-F). The paramagnetic spin-orbit (PSO) and spin-dipole (SD) terms which contribute to (2h)J(F-F) appear to be sensitive to the orientation of the hydrogen-bonded pair. However, the large increase in the FC term and (2h)J(F-F) as the size of the cluster increases is due primarily to the reorganization of sigma electron densities in both ground and excited states, and is another manifestation of cooperativity effects in hydrogen-bonded cyclic polymers. The FC term and (1)J(F-H) always increase upon complex formation, but (1)J(F-H) increases only slightly as the size of the cluster increases due to a concurrent decrease in the PSO term. The changes in (1)J(F-H) as a function of polymer size reflect the polarization of electron density away from H and toward F in the ground state, and the electron reorganization which occurs in the excited states which couple to the ground states through the FC and PSO operators. The FC term is a good approximation to (1h)J(H-F), and is always negative, indicating that the hydrogen bonds in the FH clusters are traditional hydrogen bonds.     

Spin-state transition in LaCoO3: direct neutron spectroscopic evidence of excited magnetic states

A gradual spin-state transition occurs in LaCoO3 around T approximately 80-120 K, whose detailed nature remains controversial. We studied this transition by means of inelastic neutron scattering and found that with increasing temperature an excitation at approximately 0.6 meV appears, whose intensity increases with temperature, following the bulk magnetization. Within a model including crystal-field interaction and spin-orbit coupling, we interpret this excitation as originating from a transition between thermally excited states located about 120 K above the ground state. We further discuss the nature of the magnetic excited state in terms of intermediate-spin (t(2g)(5)e(g)(1), S=1) versus high-spin (t(2g)(4)e(g)(2), S=2) states. Since the g factor obtained from the field dependence of the inelastic neutron scattering is g approximately 3, the second interpretation is definitely favored.     

Spectroscopic measurements in nitrogen arcs with respect to local thermodynamic equilibrium

A wall-stabilized nitrogen arc at atmospheric pressure was studied spectroscopically in the current range from 20 to 70 A with the aim of detecting departures from LTE. Measurements of the relative intensity of several N(I) lines showed that the populations of the upper excited states are in equilibrium for currents greater than approx. 25 A. Comparisons of the excitation temperatures obtained from relative intensities with the electron temperature and with the temperature curves calculated for different departures from LTE show that deviations from equilibrium are small at the arc center for electron densities above approx. 4 × 10¹⁶ cm^-3. Deviations between the radial profiles of the electron and excitation temperatures were observed for currents between 35 and 55 A.