TY - JOUR
T1 - Low-energy (5-250eV) electron-stimulated desorption of H+, H2+, and H+(H2O)n from low-temperature water ice surfaces
AU - Herring-Captain, Janine
AU - Grieves, Gregory A.
AU - Alexandrov, Alex
AU - Sieger, Matthew T.
AU - Chen, Haiyan
AU - Orlando, Thomas M.
PY - 2005/7/15
Y1 - 2005/7/15
N2 - Low-energy (5-250eV) electron-stimulated desorption (ESD) has been used to study the production and removal of H+, H2+, and H+(H2O)n=1-8 from porous amorphous solid water (PASW), amorphous solid water (ASW), and crystalline (CI) water ice films. The threshold energies for ESD of H+ and H2+ from CI and H+ and H+(H2O) from both PASW and ASW are ∼22±3eV. There is also a H2+ yield increase at ∼40±3eV and a ∼70±3eV threshold for ESD of H+(H2O)n=2-8 for all phases of ice. H2+ production and desorption involves direct molecular elimination and reactive scattering of an energetic proton. Both of these channels likely involve localized two-hole one-electron and or two-hole final states containing 4a1, 3a1, and or 2a1 character. The 70eV cluster ion threshold implicates either an initial (2a1-2) state localized on a monomer or the presence of at least two neighboring water molecules each containing a single hole. The resulting correlated two-hole or two-hole, one-electron configurations are localized within a complex and result in an intermolecular Coulomb repulsion and cluster ion ejection. The H+(H2O)n yields are highest from PASW relative to ASW and CI and decrease with temperature, whereas the H2+ yields are highest for CI and increase with temperature. The temperature effects and cluster ion distributions are accounted for by distance and temperature dependent hole screening. Changes in screening, hole lifetimes and hopping probabilities are greatest for a1 levels. This is supported by valence band photoemission studies of ice as a function of temperature.
AB - Low-energy (5-250eV) electron-stimulated desorption (ESD) has been used to study the production and removal of H+, H2+, and H+(H2O)n=1-8 from porous amorphous solid water (PASW), amorphous solid water (ASW), and crystalline (CI) water ice films. The threshold energies for ESD of H+ and H2+ from CI and H+ and H+(H2O) from both PASW and ASW are ∼22±3eV. There is also a H2+ yield increase at ∼40±3eV and a ∼70±3eV threshold for ESD of H+(H2O)n=2-8 for all phases of ice. H2+ production and desorption involves direct molecular elimination and reactive scattering of an energetic proton. Both of these channels likely involve localized two-hole one-electron and or two-hole final states containing 4a1, 3a1, and or 2a1 character. The 70eV cluster ion threshold implicates either an initial (2a1-2) state localized on a monomer or the presence of at least two neighboring water molecules each containing a single hole. The resulting correlated two-hole or two-hole, one-electron configurations are localized within a complex and result in an intermolecular Coulomb repulsion and cluster ion ejection. The H+(H2O)n yields are highest from PASW relative to ASW and CI and decrease with temperature, whereas the H2+ yields are highest for CI and increase with temperature. The temperature effects and cluster ion distributions are accounted for by distance and temperature dependent hole screening. Changes in screening, hole lifetimes and hopping probabilities are greatest for a1 levels. This is supported by valence band photoemission studies of ice as a function of temperature.
UR - http://www.scopus.com/inward/record.url?scp=33749233450&partnerID=8YFLogxK
U2 - 10.1103/PhysRevB.72.035431
DO - 10.1103/PhysRevB.72.035431
M3 - Article
AN - SCOPUS:33749233450
SN - 1098-0121
VL - 72
JO - Physical Review B - Condensed Matter and Materials Physics
JF - Physical Review B - Condensed Matter and Materials Physics
IS - 3
M1 - 035431
ER -