Repulsion-induced surface-migration, by ballistics and bounce

The motion of adsorbate molecules across surfaces is fundamental to self-assembly, material growth, and heterogeneous catalysis. Recent Scanning Tunneling Microscopy studies have demonstrated the electron-induced long-range surface-migration of ethylene, benzene, and related molecules, moving tens of Angstroms across Si(100). We present a model of the previously unexplained long-range recoil of chemisorbed ethylene across the surface of silicon. The molecular dynamics reveal two key elements for directed long-range migration: first ‘ballistic’ motion that causes the molecule to leave the ab initio slab of the surface traveling 3–8 Å above it out of range of its roughness, and thereafter skipping-stone ‘bounces’ that transport it further to the observed long distances. Using a previously tested Impulsive Two-State model, we predict comparable long-range recoil of atomic chlorine following electron-induced dissociation of chlorophenyl chemisorbed at Cu(110)

Contrasting fast precipitation responses to tropospheric and stratospheric ozone forcing

The precipitation response to radiative forcing (RF) can be decomposed into a fast precipitation response (FPR), which depends on the atmospheric component of RF, and a slow response, which depends on surface temperature change. We present the first detailed climate model study of the FPR due to tropospheric and stratospheric ozone changes. The FPR depends strongly on the altitude of ozone change. Increases below about 3 km cause a positive FPR; increases above cause a negative FPR. The FPR due to stratospheric ozone change is, per unit RF, about 3 times larger than that due to tropospheric ozone. As historical ozone trends in the troposphere and stratosphere are opposite in sign, so too are the FPRs. Simple climate model calculations of the time-dependent total (fast and slow) precipitation change, indicate that ozone's contribution to precipitation change in 2011, compared to 1765, could exceed 50% of that due to CO2 change.