Ultrahigh frequency additional background radiation of the lower ionosphere during strong geomagnetic disturbances

In periods of high solar activity and the formation of geomagnetic storms, additional background incoherent ultrahigh frequency (UHF) radiation with decimeter to millimeter wavelengths in the high E and D layers of the Earth’s ionosphere is generated. This emission is produced by transitions between Rydberg states of atoms and molecules of atmospheric gases, which are excited by electrons and are surrounded by a neutral species of the medium. At present, there is no reliable information on the integrated intensity of UHF radiation in this wavelength range. This problem can be solved on knowledge of the dynamics of collisional and radiative quenching of Rydberg states and of the kinetics of their population in the lower ionosphere. An analysis of the available experimental data shows that the radiation is generated in an atmospheric layer located at altitudes between 50 and 110 km. The current theory is discussed and the ways of its further improvement connected with the development of more rigorous theoretical methods for describing the effect of neutral particles of medium on the collisional and radiative quenching dynamics, including the elementary processes with participation of the nitrogen and oxygen molecules, are suggested. For quantitatively estimates the influence of excited particles on the incoherent UHF radiation of the atmosphere, it is necessary carrying out of the preliminary calculations the potential energy surfaces and dynamics of nonadiabatic transitions between Rydberg states, construction the electronic wave functions, and determination the dipole moments of the allowed transitions and the emission line shapes. Obtained results can be included into the general kinetic scheme which defines of the UHF radiation intensity versus the density and temperature of the atmosphere. Accompanying its infrared (IR) radiation can be used to define of Rydberg states.     

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.     

Semiclassical theory of the radiative-collisional cascade in a Rydberg atom

We have developed a two-dimensional semiclassical model of the radiative-collisional cascade for hydrogen-like systems. We describe the collisions with electrons and ions by classical diffusion in the space of principal and orbital quantum numbers and use an iterative procedure that consistently takes into account the quantum nature of the radiative cascade for radiative transitions. The model establishes the correspondence between the quantum and classical approaches and indicates that the latter cannot be directly used to calculate the population kinetics of highly excited atomic states. Our calculations of the two-dimensional populations of highly excited atomic hydrogen states for selective, three-body, and photorecombination sources of population allow the data of one-dimensional kinetic models to be refined. The calculated intensities of recombination lines demonstrate the degree of nonequilibrium of the Rydberg state populations under typical astrophysical plasma conditions.     

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.     

Electron spectroscopy of autoionizing states of nitrogen atoms

During excitation of N₂, NO and N₂O molecules by fast neutral 1¹S helium atoms, highly excited molecular states are formed which yield, through predissociation, autoionizing nitrogen atoms. The energy of electrons released in autoionization was measured and the energy and plausible spectroscopic assignment of autoionizing levels was determined. The excited levels belong to Rydberg series converging to the N⁺(¹D) series limit. Besides molecular states derived by correlation of the final atoms, highly excited molecular parent states are also discussed.     

Differential cross sections for muonic hydrogen scattering on hydrogen molecules

The results of first calculations of the differential cross sections for muonic hydrogen scattering on hydrogen molecules are presented. They are functions of the initial and final kinetic energy of the system and the scattering angle. These calculations are based on the respective set of cross sections for muonic hydrogen scattering on hydrogen nuclei, obtained within the framework of the adiabatic method. The Fermi pseudopotential method is used to estimate the molecular binding effects. The influence of electrons on the cross sections under consideration is described in terms of the effective screening potential. Rotational and vibrational transitions are taken into account. The calculated molecular differential cross sections show a strong angular dependence. This effect is very significant for the electronic contributions to the cross sections, e.g. for collision energies above approximately 0.1 eV only the cross sections of small scattering angles are influenced considerably by the screening. Since these differential cross sections give detailed information about the final energies and complicated angular distributions of the scattered muonic atoms they are the proper basis for calculations concerning the deceleration of muonic hydrogen atoms in molecular hydrogen targets and for Monte Carlo simulations of different experiments in muonic physics.     

Laser-stimulated formation and stabilization of antihydrogen atoms

Laser-stimulated radiative transitions from states close to the ionization threshold to low-lying atomic levels are considered for protons (antiprotons) in a cold electron (positron) plasma and estimates for the resulting formation rate of hydrogen (antihydrogen) atoms in the ground state are given. The estimates apply to both laser-stimulated recombination and induced radiative stabilization of high Rydberg levels. First experiments concerning laser-stimulated recombination in merged beams of electrons and protons are discussed, which have confirmed the rate predictions for this process. In view of antihydrogen formation in a cold trapped positron plasma, the use of two successive stimulated transitions is considered for obtaining a high formation rate of ground-state atoms at relatively low radiation intensity.     

Vibrational excitation and negative ion production in radio frequency parallel plate H2 plasmas

A theoretical study of the vibrational kinetics and attachment in low pressure hydrogen plasmas produced by Radio Frequency (RF) discharges is performed. In particular we study the influence of gas/surface kinetic processes such as the vibrational deactivation and the atomic recombination of molecules. The production of vibrationally excited molecules by the surface recombination of atoms is also considered. The study is realized by means of a self-consistent one dimensional kinetic model, and a parallel plate RF discharge test case is implemented. Results show that surface processes are able to affect the vibrational distribution function (vdf) and the negative ion (H-) density. The effect of vibrational exothermicity of H atom recombination is also discussed as a way to reduce the gap between theory and experimental results. Moreover, it is shown that the H- ion heating by the electric field strongly affects the detachment rate: this effect is specially important for negative ions produced through Rydberg states in this kind of discharges.     

Reactions of excited atoms and molecules with atoms and molecules

Ionizing collisions of long lived excited particles with atoms and molecules are studied by a cross beam technique. For the first time reactions of atoms in high Rydberg states are included in the investigation. In this paper we report relative cross sections for the production of the ions RH⁺, RH ₂ ⁺ , and H ₂ ⁺ by collisions of excited rare gas atoms R^* with H₂. With HD as the target molecule the isotope effect for the production of RD⁺ and RH⁺ has been determined. In the case of argon and krypton, ions are produced only by the high Rydberg states, whereas in the case of helium and neon only the metastable states contribute to a measurable extent. The data indicate, that the reaction mechanism is different in principle for metastable and highly excited atoms. Simple models are proposed to explain the experimental results.     

Transfer of a weakly bound electron in collisions of Rydberg atoms with neutral particles. II. Ion-pair formation and resonant quenching of the Rb(nl) and Ne(nl) States by Ca, Sr, and Ba atoms

Electron-transfer processes are studied in thermal collisions of Rydberg atoms with alkaline-earth Ca(4s ²), Sr(5s ²), and Ba(6s ²) atoms capable of forming negative ions with a weakly bound outermost p-electron. We consider the ion-pair formation and resonant quenching of highly excited atomic states caused by transitions between Rydberg covalent and ionic terms of a quasi-molecule produced in collisions of particles. The contributions of these reaction channels to the total depopulation cross section of Rydberg states of Rb(nl) and Ne(nl) atoms as functions of the principal quantum number n are compared for selectively excited nl-levels with l ? n and for states with large orbital quantum numbers l = n ? 1, n ? 2. It is shown that the contribution from resonant quenching dominates at small values of n, and the ion-pair formation process begins to dominate with increasing n. The values and positions of the maxima of cross sections for both processes strongly depend on the electron affinity of an alkaline-earth atom and on the orbital angular momentum l of a highly excited atom. It is shown that in the case of Rydberg atoms in states with large l ～ n ? 1, the rate constants of ion-pair formation and collisional quenching are considerably lower than those for nl-levels with l ? n.     

Atoms and ions in superfluid helium

Optical spectra, level population and nonradiative deexcitation processes of atomic impurities in liquid helium have been investigated. The recombination of electrons and positive metal ions are described by the tunneling model. This model explains the population gap of 1.8 eV below the ionisation limit which was observed for several neutral defect atoms in liquid helium. In the framework of a pseudopotential theory excited singlet levels of Ba, Ca and Na atoms are recalculated and compared to experimental data. Non-spherical atomic defects for excited p-states are treated also. Quadrupole vibrations of these distorted defect structures are assumed to be responsible for inducing multiphonon transitions between excited atomic states.     

Spin-flip cross sections in muonic hydrogen scattering on hydrogen molecules

The results of calculations of the total cross sections of spin-flip processes in low energy muonic hydrogen scattering on hydrogen molecules are presented. These calculations are based on the respective set of cross sections for muonic hydrogen scattering on hydrogen nuclei, obtained within the framework of the multichannel adiabatic method. All combinations of the three hydrogen isotopes are considered. Molecular binding effects are described in terms of the Fermi pseudopotential method. Electron screening effects are calculated in the distorted wave Born approximation. Rotational and vibrational transitions of the molecules, due to collisions with muonic hydrogen atoms, are taken into account. The molecular and electron screening corrections do not exceed a few tens per cent for lowest collision energies.     

Dissociation of 14N2+ ions induced by slow electrons

The cross sections and thermal rate coefficients for the dissociative recombination (DR) of the molecular nitrogen ions initially in the first four vibrational levels of the ground electronic state have been computed in the framework of the multichannel quantum defect theory. An energy range of 0.001–1 eV has been considered. The contribution of the indirect DR mechanism involving Rydberg states associated with the first excited ion core has also been investigated.     

Efficient production of ground-state potassium molecules at sub-mK temperatures by two-step photoassociation

We have developed a two-step " R-transfer" method that efficiently produces translationally ultracold potassium molecules in the X (1)Sigma(+)(g) electronic ground state. Laser-cooled atoms are initially photoassociated at large internuclear separation R to form molecules in high vibrational levels of the 1 (1)Pi(g) state, which are in turn excited by an additional laser to shorter-range Rydberg states such as 5 (1)Pi(u) and 6 (1)Pi(u). Subsequent radiative decay produces ground-state molecules at rates up to 10(5) molecules/second per vibrational level.     

飞秒时间分辨质谱和光电子影像对分子激发态动力学的研究

分子量子态的研究,特别是分子激发态演化过程的研究不仅可以了解分子量子态的基本特性和量子态之间的相互作用,而且可以了解化学反应过程和反应通道间的相互作用.飞秒时间分辨质谱和光电子影像是将飞秒抽运-探测分别与飞行时间质谱和光电子影像相结合的超快谱学方法,为实现分子内部量子态探测,研究分子量子态相互作用及超快动力学过程提供了强有力的工具,可以在飞秒时间尺度下研究单分子反应过程中的光物理或光化学机理.本文详细介绍了飞秒时间分辨质谱和光电子影像的技术原理,并结合本课题组的工作,展示了这两种方法在量子态探测及相互作用研究领域,特别是激发态电子退相、波包演化、能量转移、分子光解动力学以及分子激发态结构动力学研究中的广泛应用.最后,对该技术的发展前景以及进一步的研究工作和方向进行了展望.     

Vibrational population densities of the A3Σu+, B3Πg, W3Δu, B'3Σu-, and C3Πu states in nitrogen plasmas

Population densities of vibrational levels of triplet excited states have been calculated using a collisional-radiative model applicable to nitrogen gas discharges with a Maxwellian electron energy distribution. Relative contributions of various electron impact and radiative processes, including intrasystem cascade, to the total cross sections of the triplet excited states are investigated.     

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.     

Perturbation of the excited states of the hydrogen atom and hydrogen-like ions by a neutral atom

Owing to the degeneracy of the energy levels, the wavefunction of the electron in the excited states of the hydrogen atom and hydrogen-like ions perturbed by a neutral atom B is significantly different from the wavefunction of the unperturbed state. The perturbed function has a wide high maximum in the region of atom B, which is explained by multiple collisions of the electron with atom B, because the classical trajectories in the Coulomb field are closed and the size of atom B is much smaller than the size of the excited-state orbit. The radiative lifetimes of the excited states are much larger than those of unperturbed states. The orbital angular momentum L of the excited electron is strongly changed in collisions with atom B owing to the quantum interference or mixing of the temporal phases of adiabatic wavefunctions. The cross sections for such a change in the orbital angular momentum are several orders of magnitude larger than the cross sections found in early investigations in the approximation of the single collision of the electron with atom B.     

The pairing of electronic states in alternant hydrocarbons

The pairing of Hückel molecular orbitals in an alternant hydrocarbon holds in a more general sense for wave functions which make complete allowance for the correlation of π electrons within the atomic orbital scheme. The new pairing property holds exactly in the scope of Pariser, Parr, and Pople's approximations, and leads to an exact correspondence between every detail of the excited states, the electronic spectra and electron resonance spectra of positive and negative hydrocarbon ions. Neutral molecules have a half-filled electron shell in which electrons and holes are on an equal footing. This causes the electron distribution to be uniform in every electronic state, and leads to two kinds of excited state—‘even’ and ‘odd’—as Pariser first suggested. Transitions between states of the same parity are forbidden. In neutral radicals the spin density vanishes in all the bonds, and in both radicals and molecules the bond orders vanish between atoms of the same set (starred or unstarred).     

Use of photoprocesses with charge transfer to excite active laser media

Conclusions A survey of various methods of optical excitation of ionic states, including excimer states, of molecules demonstrates the extensive potential optical pumping and makes it possible to determine the trends that are promising for further searches. Noticeable among them, firstly, is direct optical excitation and its accompanying secondary chemical processes with phototransport of electrons, which offer the researchers the largest choice of specific molecules and excitation mechanisms. We have shown, with molecular chlorine as the example, that the search for working media for optical pumping need not be limited to heavy molecules. The use of a complicated isotopic composition of molecules, Zeeman splitting of levels in a magnetic field, and impact broadening of spectral lines makes it possible to extend, within reasonable limits, the method of wide-band pumping to include also light molecules. As to secondary exchange reactions with charge transfer, in which optically excited molecules participate, it can be seen from the results of estimates of the cross sections that they constitute the largest class of excimerformation reactions and are characterized by additional possibilities of spectrally controlling the course of the reactions for the purpose of obtaining various products.Other promising methods considered here are production of ionic photodissociation states, including polar photodissociation, and also chemical radiative collisions.Note particularly the need for continuing the search for polyatomic excimers. It is obvious that production of such excimers is possible in media having a more complicated molecular composition, where such an advantage of optical pumping as the absence of induced absorption at the lasing wavelength is most strongly manifested.Quantum Radiophysics Laboratory, Lebedev Physics Institute. Translated from Preprint No. 23 of the Lebedev Physics Institute, Academy of Sciences of the USSR, Moscow, 1990.