Water Network-Dependent Charge Translocation in the NO^+ \cdot (H_2O)_3 Clusters: AN Old Riddle of the Ionosphere Brings a Microscopic Grotthuss Mechanism Down to Earth

Details Water Network-Dependent Charge Translocation in the NO^+ \cdot (H_2O)_3 Clusters: AN Old Riddle of the Ionosphere Brings a Microscopic Grotthuss Mechanism Down to Earth Water Network-Dependent Charge Translocation in the NO^+ \cdot (H_2O)_3 Clusters: AN Old Riddle of the Ionosphere Brings a Microscopic Grotthuss Mechanism Down to Earth

Jun 2009

adsabs.harvard.edu/cgi-bin/nph-data_query?bibcode=2009mss..confemg01r&link_type=abstract

"International Symposium On Molecular Spectroscopy, 64th Meeting, Held 22-26 June, 2009 at Ohio State University. http://molspec

Computer Science

Infrared/Raman

Scientific paper

The dominant ions in the D-region of the ionosphere are proton hydrates, H^+ \cdot (H_2O)_n, which are formed through a complex mechanism involving clustering, and a water network-mediated reaction, NO^+ \cdot (H_2O)_3 + H_2O ⟶ H^+ \cdot (H_2O)_3 + HNO_2, that proceeds to products only upon addition of the fourth water molecule. The presence of reactive and non-reactive isomers of NO^+ \cdot (H_2O)_3 has been invoked to explain the relatively slow rate of HNO_2 formation from the trihydrate. To address this hypothesis, we have employed isomer-selective, pump-probe spectroscopy to determine the infrared signatures of species nominally present in the NO^+ \cdot (H_2O)_3 ion packet prepared in a supersonic jet ion source. Indeed two isomers are found to be present. Strong differences in the spectral patterns of the two isomers suggest that they have quite different geometries, which would be consistent with the isomer-specific reactivity model. One of the patterns yields strongly red-shifted activity in the OH stretching region around 2800 cm^{-1}, which is readily explained by the expected behavior of the bridging hydrogen atoms in a chain structure. The motion of these protons is reminiscent of the von Grotthuss mechanism where sequential dissociation and reformation of OH bonds translocates a proton over large distances by passing through a series of small, pairwise exchanges.

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