On the mechanisms of formation of excited hydrogen atoms in a decaying helium-hydrogen plasma

We spectroscopically studied the population of the excited hydrogen atomic states with the principal quantum numbers n=3 and 4 in a decaying plasma produced by a pulsed discharge in a mixture of helium (p=40.4 Torr) with a small amount of hydrogen ([H₂]≈10¹² cm^?3). Experiments on recording the response of the spectral line intensities to a short-duration electron temperature perturbation revealed the contribution of electron-ion recombination to the population of the H*(n=3) states in the early afterglow. The ions produced by collisions of hydrogen molecules with metastable He(2³ S ₁) atoms, whose density decreases relatively rapidly with time in the decaying plasma, were assumed to be involved in this process. No population of the H*(n=4) atomic levels due to electron-ion recombination was found. Our experimental results are consistent with the conclusions of previous studies that excitation transfer during collisions of metastable helium molecules with hydrogen molecules plays a major role in the population of the excited hydrogen atomic states both with n=3 and with n=4 during most of the afterglow.     

On the nature of optically active centres in selfactivated luminophors of the CaWO4 type

The evidence in favour of the assumption that impurities of V group elements creates defects of the MeO′₄ type (centres of luminescence), Me?₃ and V_?, or WO₃ (capture centres) which are responsible for recombination afterglow different from the steady-state luminescence spectral distribution (Me = As, Sb, Nb, Ta; V₀ - oxygen vacancy) are presented. These same impurities, and phosphorous, lead to quenching of luminescence observed as afterglow with excitation quanta greater than 6.3 eV. This corresponds to the valued of the energy gap. Experimental data together with results of thermodynamic analysis lead to the conclusion that the luminescence of CaWO₄ and of other undoped oxygen containing compounds of transition elements luminophors is caused by direct self-activation connected with ability of these elements to convert spontaneously into a lower valency state and to form variable phases (non-stoichiometric compounds). It is proposed that in case of CaWO₄ centres of luminescence are formed by W⁵⁺.     

Stabilization of H centres in irradiated LiF:Mg crystals

Abstract

The paper is dedicated to investigation of possible ways of stabilization of the H centres created together with F and Mg⁺ centres in a process of decay of selftrapped exciton. As a main mode of the H centres stabilizationa capture of the H centre by magnesium-vacancy dipole and creation of V-type centre was suggested. This process was theoretically studied in the frames of model of molecular cluster which electron structure was calculated by the semi-empirical version of the Hartree-Fock method. For experimental corroboration of this process the relations between dependences of magnesium dipoles decrease on dose of gamma irradiation and corresponding dose dependences of the Mg⁺, Mg°, and F centres radiation creation were used.     

Recombination in Dense Ion Plasmas

A theory is developed to treat ion recombination in dense ion plasmas. Numerical results are obtained with the method of molecular dynamics. Exponential suppression of recombination is found for the discharge afterglow plasma in sulfur hexafluoride at strong Coulomb nonideality Γ. The reason for suppression is an increase of the recombination activation energy ΔE with increase of Γ. The range ΔE corresponds to the multiparticle fluctuations. Ion solvation is another suppression factor. Its importance is demonstrated for the discharge afterglow plasma in fluorine at weak Coulomb nonideality. The theory developed agrees with the experimental data available. (© 2013 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Untersuchung des „Auroral Afterglow“ und seiner Präparationsstadien

The decay of the continuum of the air afterglow was found to be equal in the whole spectral range used. In the beginning of the afterglow [NO] is not constant. N atoms from the discharge create 0 atoms by reacting with NO and retard the intensity decay. Later [NO] remains constant during the afterglow. The decay curves measured in the nitric oxide, and the Lewis-Rayleigh stage agree with the current theories of recombination of N₂ and NO by three-body collision. If the spectral intensity distribution in the Lewis-Rayleigh afterglow is due to the action of different third bodies, asReinecke suggested, his opinion is to be improved by accepting a two step reaction. The measurements can be interpretated, if the first one is responsible to the rate and the second one to the intensity distribution. No sign could be found for the Cario-Kaplan processes to be more frequent in the neighbourhood of the exciting discharge than that of recombination. On the other hand it could be shown, that the recombination of N atoms is severely hindered by transition into the auroral stage and additional collision processes become effective in the excitation of all transitions of the 1. pos. group.     

Formation of N2 C3Πu and B3Πg by dissociative recombination of Ar 2 + in Ar+N2 early afterglow

The hf pulse excited Ar + N₂ mixtures and early afterglow are investigated at total pressures from 266 to 1995 Pa using nitrogen of 0·05–0·5% concentration. The time-resolved intensity of Ar I atomic lines and N₂ (2nd pos., 1st pos. and 1st neg.) band systems exhibit an intense early afterglow (0·3 ms). Both the decay of electron densityn _e and that of molecular Ar ₂ ⁺ ions and enhancement of coefficient of dissociative recombination due to electron temperature decrease after the pulse lead to the formation of characteristic secondary maximum of Ar I spectral line and N₂ molecular band intensities in the momentt _m after cut-off the pulse. The values oft _m(B³_g)>t _m(C³_u)>t _m(Ar I) decrease with increasing total pressure and increase with growing concentration of N₂ in Ar. In the afterglow period the Ar ₂ ⁺ dissociatively recombine in 5p and 4p Ar states. As a result of radiative transitions the metastable Ar (³P_2,0) atoms are formed which consequently due to collisions with N₂ molecules create electronically excited N₂. With increasing nitrogen concentration this effect becomes less pronounced and at concentration of N₂ greater than 0·5% it is negligible.     

Role of neon in a decaying high-purity helium plasma

The evolution of the electron and atomic and molecular metastable densities and the radiation of the decaying plasma of helium with a 10^–5-fraction of neon additive is experimentally studied. A model of elementary processes in He–Ne plasma is constructed, which describes the formation and destruction of HeNe⁺ and Ne₂ ⁺ molecular ions and their contribution to the formation of the afterglow spectrum by the electronion recombination. The various criteria influence of neon on the parameters of the decaying plasma are studied. The possibility of determining the amount of neon in helium by measuring the relative intensities of helium molecular bands and neon spectral lines in the afterglow is considered.     

Pairs of F centres and CN− molecules in KCl: An ENDOR analysis

Abstract

Pair defects consisting of F centres and CN^? molecules as substitutional impurity anions (F_H(CN^?) centres) exhibit a strong coupling between the F centres and the CN^? molecules. This leads to an optical pumping of the CN^? vibrations via the F centre absorption band. We performed an Electron Nuclear Double Resonance (ENDOR) investigation in order to analyse the microscopic structure of these aggregate centres. The CN^? molecule occupies a [110] nearest anion position with respect to the F centre in two dynamic dipole orientations even at low temperature.     

Optical,magneto-optical and structural properties of F centres in BaFBr

Abstract

In BaFBr, a material which can be used as a storage phosphor for X-rays, two types of F centres can be created by additive coloration or by X-irradiation. The properties of both F centres which play an important role in the storage phosphor mechanism were investigated with optical and magneto-optical methods. The absorption bands, the emission bands, production, and stability of the F centres are discussed.     

Population of 2p 55s levels of neon in He-Ne plasma: I. The evolution of mechanisms in the discharge and the afterglow

The spectroscopic study of population processes of neon 2p ⁵5s states was carried out in helium afterglow with small admixture of neon at PHe = 38.1 torr, [He]/[Ne]=10^?5 with pulsed discharge afterglow in helium with small admixture of neon (pressure equal to 38.1 mm Hg; ). It is established that the main mechanism of population of 3s ₂ level (in Paschen’s notation) in the discharge and the initial after-glow is the excitation transfer from metastable atoms of He(2¹ S ₀). The other three levels—3s ₃, 3s ₄, and 3s ₅—corresponding to 2p ⁵5s configuration are populated in the afterglow as a result of the dissociative recombination HeNe⁺ of ions with electrons. The same process is also the main channel of population of 3s ₂ level in the late afterglow phase, when the concentration of He(2¹ S ₀) atoms is small. The hypothesis of recombination mechanism is confirmed by observation of the response of line intensities to pulsed electron heating. The partial coefficients of dissociative recombination into 2p ⁵5s states are estimated.     

Photostimulated luminescence in BaX 2 :Eu 2+ (X=Br,Cl) X-ray storage phosphors

The photostimulated luminescence (PSL) effect in BaX 2 :Eu 2+ (X=Br, Cl) is comparable to that observed in BaFBr:Eu 2+ which is used in commercial X-ray storage phosphor screens. After X-irradiation the PSL stimulation spectra of BaX 2 :Eu 2+ (X=Br, Cl) single crystals are identical to the F centre absorption spectra, i.e. the F centres are the PSL-active electron trap centres. The nature of the hole centres is still unknown. The PSL response time of about 0.70 v s is within experimental error of 0.02 v s identical to the Eu 2+ radiative lifetime, whereas in BaCl 2 :Eu 2+ the PSL response time is 0.60 v s, and thus longer than the Eu 2+ radiative lifetime of 0.47 v s.     

Investigation of excitation processes in a hollow-cathode discharge by time-resolved measurements in the vacuum u.v.

A spectrometer for the far u.v. range (λ = 30–300 nm) has been used, together with a sampling instrument (resolution 10^-9 s, time-intervals 10^?9to 10^?3s) for the measurement of afterglow. The measurements were confined to emission of the hollow cathode discharge. From the time constants of the afterglow, we conclude that the essential excitation processes for atoms in the hollow cathode are the following: direct electron excitation and three-body recombination.     

Deformation luminescence in KCl irradiated at room temperature

It has been found that there is a relationship between the thermoluminescence and the deformation luminescence of irradiated pure KCl samples. It is concluded that the luminescent process in the deformation luminescence is the recombination of interstitial halogen atoms with vacancy centres (F, M) as well as in the thermoluminescence.     

M-centre luminescence in NaF and LiF: towards a comprehensive interpretation of the m-centre emission properties in alkali halides

Abstract

Emission and excitation spectra were accurately detected as a function of the temperature (in the range 18-300 K) in NaF and LiF samples containing unperturbed M-centres: different coloration techniques and ageing effects were tested in order to obtain the pure M-emission band. On the basis of collected data new trends and correlations are proposed between the halfwidth of the emission bands (H), the effective modes (ω), and the Huang-Rhys factors (S) for M and F centres: the H(M) values are roughly half the H(F) ones, M-emission S values are very similar in different crystals, ω and H values for the M- and F-emissions are proportional to the transverse optical frequency ω_T values.     

First stage f centre formation in pure and doped KCl crystals by room temperaure X-irradiation

The electrical conductivity and optical absorption of potassium chloride crystals, pure and doped with divalent cation impurities, have been measured before and after X-irradiation at room temperature. The concentration of free positive ion vacancies at room temperature has been calculated from conductivity for each crystal before irradiation and is found to be much less than the first stage F centre concentration. This shows that both free and associated positive ion vacancies are the latent source of F centres in the first stage colouration. Pb^{+ +} ions trap electrons producing Pb^{+ +} and Pb⁰ centres and making free the associated cation vacancies. Such centres are not produced in Ca-doped crystals where impurity-vacancy complexes trap F centres producing Z centres. The higher ratio of F centres to positive ion vacancies in Pb-doped crystals indicates that free cation vacancies are more effective in producing F centres. However, the concentration of divalent cations is found to decrease in both the crystals after irradiation, the decrease being more in Ca-doped crystals.The author is indebted to Prof. H. N. Bose for helpful discussions. Thanks are also due to Dr. M. L. Mukherjee for providing the crystals.     

Localised transitions in luminescence of AlN ceramics

The photoluminescence (PL) and thermoluminescence (TL) properties of AlN ceramics revealed under UV irradiation are determined mainly by oxygen-related centres, giving rise to the UV (around 3.18 eV) and the Blue (2.58 eV) bands. It was found that the UV irradiation-generated donor–acceptor pairs (DAPs), responsible for the UV emission band, are randomly distributed with regard to separation distance. Luminescence properties of AlN are interpreted basing on the model of localised recombination involving electron tunnel transitions from the excited state of D to the ground state of A, proposed by Jain et al. (2012). The observed features of PL, afterglow and TL of AlN ceramics are explained by dependence of tunnelling recombination probability on separation distance between D and A implied by the used model.     

Recombination population of excited states of the hydrogen atom in an He-H<Subscript>2</Subscript> plasma

The population of excited states of the hydrogen atom in an afterglow plasma produced by a pulsed discharge in helium (40 Torr) with a small admixture of hydrogen ([H₂] ≈ 10¹² cm^?3) has been studied spectroscopically. The contribution from electron-ion recombination Γ ₃ ^rec to the production rate of atoms H(n = 3) has been separated. On the basis of an experiment in which the response of the spectral line intensities to the perturbation of the electron temperature in the afterglow phase was observed, the dependence Γ ₃ ^rec (T _e ～ T _e ^?(0.9–1.0) has been obtained in the region kT _e = 0.026–0.064 eV.     

Red-shift in the photostimulation of the X-ray storage phosphor RbBr:Ga+

Abstract

By means of magnetic circular dichroism of the optical absorption and photostimulated luminescence (PSL) the X-ray induced formation of F_A and F centres in RbBr:(Ga⁺, Li⁺) was investigated. It turnes out that RbBr:Ga⁺ co-doped with 1% Li⁺ in the melt reveals the largest red-shift of the PSL excitation bands to 790 nm, whereby the F_A to F ratio increases up to about 10% with decreasing X-ray dose. This is more than statistically expected (6%). High X-ray doses destroy F_A centres. However, up to 15% of the simultaneously generated F centres could be converted into the F_A species by appropriate bleaching with 633 nm light into the F centre absorption band.     

Electronic relaxations of radiative defects of the anion sublattice in caesium bromide crystals and exoemission of electrons

The thermostimulated exoelectron emission (TSEE) is applied for investigation of the processes of radiative defects recombination in the nearsurface layer. Results of TSEE studies of radiatively excited CsBr crystals are presented. Dose dependences of the decay kinetics, TSEE spectrum structure and exosums were studied. Concentration of exoemission-active centres (EAC) and TSEE kinetics parameters have been calculated on the base of the bulk thermoactivated anion sublattice defect recombination. The attained result correlate with the electron centres concentration for irradiated crystals. In the framework of the Auger-like anion defects recombinational bulk model of exoemission from irradiated wide-band-gap crystals, the energy spectra of the exoelectrons excited on the F-centres are attained.     

Deformation-induced excitation of the luminescence centres in coloured alkali halide crystals

The present paper reports the deformation-induced excitation of the luminescence centres in coloured alkali halide crystals. The peaks of the mechanoluminescence (ML) in γ-irradiated KCl, KBr, KI, NaCl and LiF crystals lie at 455, 463, 472, 450 and 485 nm, i.e. at 2.71, 2.67, 2.62, 2.75 and 2.56 eV, respectively. From the similarity between the ML spectra and the thermoluminescence (TL) and afterglow spectra, the ML of KCl, KBr, KI, NaCl and LiF crystals can be assigned to the deformation-induced excitation of the halide ions in V₂-centres or any other hole centres. For the deformation-induced excitation of the halide ions in V₂-centres, or in other centres, the following four models may be considered: (i) free electron generation model, (ii) electron–hole recombination model, (iii) dislocation exciton radiative decay model and (iv) dislocation exciton energy transfer model. The dislocation exciton energy transfer model is found to be suitable for the coloured alkali halide crystals. According to the dislocation exciton energy transfer model, during the deformation of solids the moving dislocations capture electrons from the F-centres and then they capture holes from the hole centres and consequently the formation of dislocation excitons takes place. Subsequently, the energy released during the decay of dislocation excitons excites the halide ions of the V₂-centres or any other hole centres and the light emission occurs during the de-excitation of the excited halide ions, which is the characteristic of halide ions. The mechanism of ML in irradiated alkali halide crystals is different from that of the TL in which the electrons released form F-centres due to the thermal vibrations of lattices reach the conduction band and the energy released during the electron–hole recombination excites the halide ions in V₂-centres or in any other hole centres. It is shown that the phenomenon of ML may give important information about the dislocation bands in coloured alkali halide crystals.