title: Experimental evidence for the influence of charge on the adsorption capacity of carbon dioxide on charged fullerenes.
abstract: We show, both experimentally and theoretically, that the adsorption of CO2 is sensitive to charge on a capturing model carbonaceous surface. In the experiment we doped superfluid helium droplets with C60 and CO2 and exposed them to ionising free electrons. Both positively and negatively charged C60(CO2)n(+/-) cluster ion distributions are observed using a high-resolution mass spectrometer and they show remarkable and reproducible anomalies in intensities that are strongly dependent on the charge. The highest adsorption capacity is seen with C60(+). Complementary density functional theory calculations and molecular dynamics simulations provided insight into the nature of the interaction of charged C60 with CO2 as well as trends in the packing of C60(+) and C60(-). The quadrupole moment of CO2 itself was found to be decisive in determining the charge dependence of the observed adsorption features. Our findings are expected to be applied for the adsorption of CO2 on charged surfaces in general.
authors.affiliation: Institut für Ionenphysik und Angewandte Physik, Leopold-Franzens-Universität Innsbruck, Technikerstr. 25, 6020 Innsbruck, Austria. Paul.Scheier@uibk.ac.at.
authors.forename: Stefan
authors.initials: S
authors.lastname: Ralser
authors.affiliation: Institut für Ionenphysik und Angewandte Physik, Leopold-Franzens-Universität Innsbruck, Technikerstr. 25, 6020 Innsbruck, Austria. Paul.Scheier@uibk.ac.at.
authors.forename: Alexander
authors.initials: A
authors.lastname: Kaiser
authors.affiliation: Institut für Ionenphysik und Angewandte Physik, Leopold-Franzens-Universität Innsbruck, Technikerstr. 25, 6020 Innsbruck, Austria. Paul.Scheier@uibk.ac.at.
authors.forename: Michael
authors.initials: M
authors.lastname: Probst
authors.affiliation: Institut für Ionenphysik und Angewandte Physik, Leopold-Franzens-Universität Innsbruck, Technikerstr. 25, 6020 Innsbruck, Austria. Paul.Scheier@uibk.ac.at.
authors.forename: Johannes
authors.initials: J
authors.lastname: Postler
authors.affiliation: Institut für Ionenphysik und Angewandte Physik, Leopold-Franzens-Universität Innsbruck, Technikerstr. 25, 6020 Innsbruck, Austria. Paul.Scheier@uibk.ac.at.
authors.forename: Michael
authors.initials: M
authors.lastname: Renzler
authors.affiliation: Department of Chemistry, York University, Toronto, ON, Canada M3J 1P3. dkbohme@yorku.ca.
authors.forename: Diethard K
authors.initials: DK
authors.lastname: Bohme
authors.affiliation: Institut für Ionenphysik und Angewandte Physik, Leopold-Franzens-Universität Innsbruck, Technikerstr. 25, 6020 Innsbruck, Austria. Paul.Scheier@uibk.ac.at.
authors.forename: Paul
authors.initials: P
authors.lastname: Scheier