Low energy electron attachment to condensed formic acid

Dissociative electron attachment to formic acid in the condensed phase is studied using improved mass spectrometric detection of the negative ion fragments. The desorbed yields are measured as a function of incident electron energy in the range between 3 to 20 eV. Unlike previous work, the formation of the dehydrogenated anion HCOO? is observed and the signal to noise ratio is much higher for all other ions detected, i.e. OH?, O? and H?. Resonant structure seen in all anion yield functions, is attributed to dissociative electron attachment (DEA), whereas above 14 eV nonresonant dipolar dissociation (DD) dominates the desorption yields

Diffraction in low-energy electron scattering from DNA: bridging gas phase and solid state theory

Using high-quality gas phase electron scattering calculations and multiple scattering theory, we attempt to gain insights on the radiation damage to DNA induced by secondary low-energy electrons in the condensed phase, and to bridge the existing gap with the gas phase theory and experiments. The origin of different resonant features (arising from single molecules or diffraction) is discussed and the calculations are compared to existing experiments in thin films.Comment: 40 pages preprint, 12 figures, submitted to J. Chem. Phy

Communication: Site-selective bond excision of adenine upon electron transfer

This work demonstrates that selective excision of hydrogen atoms at a particular site of the DNA base adenine can be achieved in collisions with electronegative atoms by controlling the impact energy. The result is based on analysing the time-of-flight mass spectra yields of potassium collisions with a series of labeled adenine derivatives. The production of dehydrogenated parent anions is consistent with neutral H loss either from selective breaking of C–H or N–H bonds. These unprecedented results open up a new methodology in charge transfer collisions that can initiate selective reactivity as a key process in chemical reactions that are dominant in different areas of science and technology

Dissociative electron attachment to the H2O molecule. I. Complex-valued potential-energy surfaces for the 2B1, 2A1, and 2B2 metastable states of the water anion

We present the results of calculations defining global, three-dimensional representations of the complex-valued potential-energy surfaces of the doublet B1, doublet A1, and doublet B2 metastable states of the water anion that underlie the physical process of dissociative electron attachment to water. The real part of the resonance energies is obtained from configuration-interaction calculations performed in a restricted Hilbert space, while the imaginary part of the energies (the widths) is derived from complex Kohn scattering calculations. A diabatization is performed on the 2A1 and 2B2 surfaces, due to the presence of a conical intersection between them. We discuss the implications that the shapes of the constructed potential-energy surfaces will have upon the nuclear dynamics of dissociative electron attachment to H2O. This work originally appeared as Phys Rev A 75, 012710 (2007). Typesetting errors in the published version have been corrected here.Comment: Corrected version of PRA 75, 012710 (2007

Dissociative electron attachment to the H2O molecule. II. Nuclear dynamics on coupled electronic surfaces within the local complex potential model

We report the results of a first-principles study of dissociative electron attachment to H2O. The cross sections are obtained from nuclear dynamics calculations carried out in full dimensionality within the local complex potential model by using the multi-configuration time-dependent Hartree method. The calculations employ our previously obtained global, complex-valued, potential-energy surfaces for the three (doublet B1, doublet A1, and doublet B2) electronic Feshbach resonances involved in this process. These three metastable states of H2O- undergo several degeneracies, and we incorporate both the Renner-Teller coupling between the B1 and A1 states as well as the conical intersection between the A1 and B2 states into our treatment. The nuclear dynamics are inherently multidimensional and involve branching between different final product arrangements as well as extensive excitation of the diatomic fragment. Our results successfully mirror the qualitative features of the major fragment channels observed, but are less successful in reproducing the available results for some of the minor channels. We comment on the applicability of the local complex potential model to such a complicated resonant system.Comment: Corrected version of Phys Rev A 75, 012711 (2007

Coulomb Explosion and Thermal Spikes

A fast ion penetrating a solid creates a track of excitations. This can produce displacements seen as an etched track, a process initially used to detect energetic particles but now used to alter materials. From the seminal papers by Fleischer et al. [Phys. Rev. 156, 353 (1967)] to the present [C. Trautmann, S. Klaumunzer and H. Trinkaus, Phys. Rev. Lett. 85, 3648 (2000)], `Coulomb explosion' and thermal spike models are treated as conflicting models for describing ion track effects. Here molecular dynamics simulations of electronic-sputtering, a surface manifestation of ion track formation, show that `Coulomb explosion' produces a `heat' spike so that these are early and late aspects of the same process. Therefore, differences in scaling are due to the use of incomplete spike models.Comment: Submitted to PRL. 4 pages, 3 figures. For related movies see: http://dirac.ms.virginia.edu/~emb3t/coulomb/coulomb.html PACS added in new versio

Multiple scattering approach to low-energy electron collisions with the water dimer

Multiple scattering theory is applied to low-energy electron collisions with a complex target formed of two molecular scatterers. The total T-matrix is expressed in terms of the T-matrix for each isolated molecule. We apply the approach to elastic electron-(H2O)2 collisions. Following the method developed in our previous work on crystalline ice, we impose a cut-off on the dipole outside the R-matrix sphere and an energy dependent cut-off on the angular momentum components of the monomer T-matrix. An R-matrix calculation of electron-dimer collisions is performed in order to evaluate the accuracy of the multiple scattering approach. The agreement between the two calculations is very good.Comment: 15 pages, 4 figures New submission: Added references Included PACS numbers Figure 3 slightly changed Additions made to the Conclusions and Discussion sectio

Electron Transmission Spectroscopy in Atomic Hydrogen

An electron transmission experiment is used to study the resonances in the total scattering cross section of atomic hydrogen below the threshold of the first excited state. The three lowest resonances, designated 1S, 3P, and 1D, are observed and their energies and decay widths are found to be in good agreement with the values predicted theoretically using close coupling with correlation