Quantum theory of electron stimulated desorption

The process of electron stimulated desorption of adsorbates from metal surfaces is investigated within the framework of quantum mechanical scattering theory. The Born-Oppenheimer adiabatic approximation is assumed to be valid for the adsorbate motion. The transition amplitude for desorption via the resonant excitation of excited states of the adsorbate then can be factorized into an electronic excitation amplitude and a Franck-Condon factor. The Franck-Condon factor is more complicated than in molecules. The continuum of substrate excitations coupling to the adsorbate gives rise to an absorptive part of the Born-Oppenheimer potential governing the motion of the adsorbate in the excited state. This absorptive part leads to a considerable reduction of the desorption cross section. Explicit quantum mechanical expressions for the corresponding reduction factor are given.The desorption of neutrals is considered in some detail. It turns out that within the adiabatic approximation this process requires the existence of neutral excited states of the adsorbate. The reneutralization of ionic excited states by electron capture from the substrate back into the ground state of the adsorbate, while possible on purely energetical grounds, occurs with zero probability in the adiabatic approximation and thus cannot be responsible for the large abundance of neutral desorbing particles. Neutral excited states of the adsorbate in principle should show up in inelastic electron scattering. The relation between electron stimulated desorption cross sections and inelastic electron scattering cross sections is discussed briefly.On leave of absence from (present address) Physikdepartment der TUM, München-Garching and Max-Planck-Institut für Festkörperforschung, Stuttgart     

The excitation of collective nuclear states by high energy particles

The excitation of collective nuclear states by high energy particles is considered within the framework of the Glauber theory. The approach is based on the adiabatic approximation and expansion of the scattering amplitude in powers of the nonsphericity parameter. The formulae for the excitation cross sections of the rotational and one- and two-phonon vibrational states, as well as the elastic scattering cross section with the collective motion included, are obtained. The effect of nucleon correlations in both elastic and inelastic cross sections is also studied. The theoretical predictions are compared to new data on 1 GeV proton scattering by ⁵⁸Ni, ²⁰⁸Pb, ¹²C, ⁴⁰Ca and ³⁹K. A comparison with electron scattering data is simultaneously carried out. The agreement with the experimental data is generally good.     

Excitation of nuclear collective states by heavy ions within the model of semimicroscopic optical potential

The (semi)microscopic double-folding nucleus-nucleus optical potentials are suggested for consideration of inelastic scattering with excitation of collective nuclear states by using the adiabatic approach and the elastic scattering amplitude in the high-energy approximation. The analytical expression for inelastic scattering amplitude is obtained keeping the first-order terms in the deformation parameter of a potential. Calculations of inelastic cross sections for the ¹⁷O heavy ions scattered on different nuclei at about hundred MeV/nucleon are made, and the acceptable qualitative agreement with the experimental data is obtained without introducing free parameters. The prospect of the method for further applications is discussed. The text was submitted by the authors in English.     

Inelastic scattering of heavy ions at intermediate energies with excitations of nuclear collective states

Excitation of low-lying nuclear collective states upon scattering of heavy ions with energies of several tens of MeV/nucleon has been studied. The interaction potential leading to excitation is chosen in the form of a derivative of the microscopic (or semimicroscopic) nucleus-nucleus double-folding optical potential. Elastic and inelastic scattering cross sections have been calculated within the high-energy approximation; the inelastic scattering amplitude was obtained in the first order in the deformation parameter. The cross sections are compared with the experimental data on scattering of ¹⁷O from a series of nuclei with excitation of the 2⁺ level.     

Elastic and inelastic scattering of nucleons from 16O

Measurements of differential elastic and inelastic cross sections for neutron scattering from ¹⁶O at incident energies 18 to 26 MeV are presented. In addition to cross sections for neutron scattering differential cross sections for proton scattering up to 66 MeV are described in terms of phenomenological optical model potentials. At 24.5 MeV incident energy inelastic scattering up to 11.5 MeV excitation was measured. The elastic and inelastic compound nucleus contributions were examined. Direct inelastic scattering from the normal parity states was calculated using the DWBA and coupled-channel formalisms. The inelastic scattering cross section from non-normal parity state 2⁻ was calculated using the coupled-channel formalism via multi-step processes. Cross sections due to inelastic scattering from some of the states, which are thought to be members of an excited state rotational band were calculated using both vibrational and rotational approaches and were compared.     

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.     

On the lifetime of certain excited states of chemisorbed atoms

For the determination of the ESD (electron stimulated desorption) cross section, the deexcitation process of the adsorbate plays an important role. In this paper we calculate the decay rate of the neutral adsorbate which is excited to the antibonding state, taking into account the electron-hole excitations in the metal. A similar technique which was used by Nozieres and Dominicis for the X-ray emission problem is applied for the summation of the diagram expansion. The lifetime of the antibonding state is estimated by the use of a simple model for the electron-hole excitation spectrum.     

Scattering of excitons by excitons in semiconducting quantum well structures

We have theoretically investigated the scattering of excitons by excitons in a two-dimensional semiconducting quantum well system. The scattering cross sections have been calculated using the Born approximation for both the elastic and inelastic scattering of the excitons by excitons. The threshold for inelastic scattering is increased over the value in a bulk semiconductor because of the enhancement of the exciton binding energy by its confinement. The behavior of the scattering cross section as a function of the energy of relative motion of the excitons is different than in the bulk and the cross section is a more sensitive function of the ratio of the electron and hole masses than in the bulk.     

Excitation of states of medium-mass nuclei in the region of giant resonances in inelastic deuteron scattering

Results are presented that were obtained by measuring a continuum in the inelastic scattering of 37-MeV deuterons on ¹²C, ⁴⁸Ti, and ^58,64Ni nuclei in the angular range 16° ≤ θ ≤ 61°. Broad excitation maxima are found for deuteron scattering angles in the range θ ≤ 21°. The region of a broad maximum includes giant resonances of target nuclei, whose levels are excited quite readily at E _d = 37 MeV. Summation of the inelastic-scattering cross sections over all final states of the excited| nucleus and the use of completeness of the wave functions for these states make it possible to express the total cross section for inelastic (incoherent) deuteron scattering only in terms of the wave functions for the ground state of the target nucleus. The corresponding quasielastic-scattering amplitude is taken in the diffraction approximation. Nucleon correlations in the target nucleus are disregarded. Upon disregarding a small contribution of multiple quasielastic scattering at small scattering angles, the cross section for incoherent deuteron scattering is represented approximately as the product of known factors—the square of the absolute value of the amplitude for diffractive quasielastic scattering and the effective number of target nucleons scattering deuterons. The results of these calculations agree qualitatively with experimental data.     

Collisional and radiative processes with participation of highly excited states of atoms and molecules

A number of processes in which highly excited states of atoms and molecules participate are investigated. These processes are of interest for the kinetics of a low-temperature plasma, for atomic and molecular spectroscopy, and for astrophysics. A quasiclassical theory is developed for transitions between Rydberg states with change of the principal quantum number, and also for the processes of direct and associative ionization of highly excited atoms, which result from collisions between a neutral particle and its atomic core. The state of the inner electrons of a quasimolecular (molecular) ion is not altered by transitions of the outer electrons. Specific calculations are carried out for the case of the collision of hydrogen H(n) with helium He (1s²) atoms. It is shown that the cross sections and the rate constants of these processes are determined in this case by the mechanism investigated in the paper, and not by scattering of the Rydberg electron by the neutral particle. The cross sections for dipole excitation and dissociation of molecular ions from high vibrational energy levels by electron impact is calculated in the Born-Coulomb approximation. The cross sections and the rates of dissociative and three-particle attachment of electrons to ions are determined. The processes of autoionization and autodissociation decay of Rydberg states of vibrationally excited molecules are determined. Also investigated are radiative transitions near the dissociation limit of diatomic molecular ions and neutral molecules, viz., photodissociation and radiative decay of high vibrational levels, and photodissociation and translational (inverse-bremsstrahlung) absorption in collision of atomic particles.Translated from Trudy Ordena Lenina Fizicheskogo Instituta im. P. Lebedeva AN SSSR, Vol. 145, pp. 80–130, 1984.     

On the Born-Oppenheimer approximation of wave operators in molecular scattering theory

In this paper we study the diatomic molecular scattering by reducing the number of particles through Born-Oppenheimer approximation. Under a non-trapping assumption on the effective potential of the molecular Hamiltonian we use semiclassical resolvent estimates to show that non-adiabatic corrections to the adiabatic (or Born-Oppenheimer) wave operators are small. Furthermore we study the classical limit of the adiabatic wave operators by computing its action on quantum observables microlocalized by use of coherent states.     

Large-angle scattering of heavy ions: (II). General structure of inelastic cross section

Closed-form expressions are derived for the differential cross section of inelastic heavy-ion scattering at large angles. The inelastic transition amplitude given by the distorted-waves theory for excitation of low-lying collective states is evaluated by an extension of analytic methods developed in the preceding paper for elastic large-angle scattering. The very close relation between the inelastic and elastic cross sections is displayed. In particular it is shown that the angular distributions have a universal form, and that the backward-angle inelastic excitation function has, aside from a slowly varying overall energy dependence, an oscillatory gross structure of diffractive origin which is nearly identical to that of the elastic excitation function, irrespective of the physical mechanism involved.     

α-Nucleus Scattering at High Energies

In this paper ,the differential cross sections of the elastic and inelastic scattering of alpha-particle of energy 1.37GeV on the 2⁺ and 3^－ excited states of ¹²C and Ca isotopes are calculated by the method of the inelastic two-composite-particle system scattering theory at high energy.The results are in agreement with experimental data.The importance of the virtual excitation in calculating the differential cross section of the elastic is descussed.     

165Ho fast neutron cross sections

Total neutron cross sections of¹⁶⁵ Ho were measured from 0.1 to 1.5 MeV with resolutions of ? 2.5 keV. The observed total cross sections varied slowly with energy and displayed no significant structure. Differential neutron elastic and inelastic scattering cross sections were determined at intervals of ?50keV from 0.3 to 1.5 MeV. The inelastic excitation of states in¹⁶⁵Ho at; 98, 214, 371, 460, 517, 586, 712, 824, 995, 1104 and 1143 keV was positively observed with probably identification of several additional states. The observed excited structure and the respective cross sections were correlated with known single-particle and collective states and with excited structure postulated from systematics. The measured cross sections were compared with calculated values based upon spherical and deformed optical-potentials, and compound-nuclear processes. Total cross sections were best described by a spherical potential while the differential elastic angular distributions were better represented by deformed-potential calculations. Resonance interference effects were found small and, at the energies of the present experiments, the contribution of direct processes was not large.     

Isotope effects in electron impact desorption of CO and O2 adsorbed on the (110) plane of tungsten

Results on the isotope effect for total and ionic desorption cross sections in the electron impact desorption of various binding states of CO on the (110) plane of tungsten, and of oxygen on this plane are presented and discussed. It is shown that the observations allow a dissection of cross sections into excitation cross sections and escape probabilities, and that the latter can be used to estimate lifetimes of excited or ionic states. It is found that excitation cross sections for total desorption are of the order of 10^?16–10^?17 cm², but seem to be significantly smaller in some cases for excitation to ionic states, suggesting that different excitations are involved. In all cases examined here the isotope effect for total desorption is much smaller than for ion production. This can be explained by the fact that ion lifetimes are somewhat shorter than those of excited neutrals. Lifetimes are estimated, in the cases examined, to be of the order of 10^?14s.     

Closed-form quantal description of inelastic heavy ion scattering

The amplitude for inelastic heavy ion scattering, given by the distorted-wave theory for excitation of low-lying collective states, is evaluated in closed form. Use is made of the Austern-Blair relation and of other approximations appropriate for strongly absorptive interaction to express the inelastic partial-wave amplitude entirely in terms of the elastic S-matrix elements in the initial and final channels. The resulting formulae display explicitly the various contributions to the transition amplitude, whose superposition gives rise to the variety of interference patterns observable in the angular distributions and excitation functions of inelastic heavy ion scattering. It is shown that, as for elastic scattering, the dominant mechanism in inelastic heavy ion collisions near and above the Coulomb barrier is diffractive scattering of Fresnel type.     

Isotope effects in electron impact desorption of CO and O2 adsorbed on the (110) plane of tungsten

Results on the isotope effect for total and ionic desorption cross sections in the electron impact desorption of various binding states of CO on the (110) plane of tungsten, and of oxygen on this plane are presented and discussed. It is shown that the observations allow a dissection of cross sections into excitation cross sections and escape probabilities, and that the latter can be used to estimate lifetimes of excited or ionic states. It is found that excitation cross sections for total desorption are of the order of 10⁻¹⁶–10⁻¹⁷ cm², but seem to be significantly smaller in some cases for excitation to ionic states, suggesting that different excitations are involved. In all cases examined here the isotope effect for total desorption is much smaller than for ion production. This can be explained by the fact that ion lifetimes are somewhat shorter than those of excited neutrals. Lifetimes are estimated, in the cases examined, to be of the order of 10⁻¹⁴s.