The reactivity of dissolved O2, a ubiquitous impurity in aqueous solutions, with H-terminated Si(111) surfaces
was quantified using a new technique that exploits kinetic competition between an impurity and an etchant
to produce impurity-concentration-dependent changes in the steady-state etch morphology. This method is
applicable to any impurity that alters the etch morphology. The impurity-induced changes are quantified
using scanning tunneling microscopy measurements and atomistic, concentration-dependent kinetic Monte
Carlo simulations. The site-specific reactivity of O2(aq) is surprisingly anisotropic. Oxidation of the highly
strained dihydride step site is 4 times faster than oxidation of the relatively unstrained monohydride step site.
Both steps are 104 times more reactive than terrace sites. The observed site-specific reaction rates are highly
correlated to local strain. FTIR measurements of the Si−H stretch vibration showed that dissolved O2 inserts
O atoms into surface Si−Si back-bonds without removing the H-termination. Dissolved O2 does not attack
Si−H bonds, because neither Si−H consumption nor silanol production is observed.
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