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J Phys Condens Matter ; 33(40)2021 Jul 30.
Artigo em Inglês | MEDLINE | ID: mdl-34265758

RESUMO

A fundamental question for the adsorption of any gas molecule on surfaces is its saturation coverage, whose value can provide a comprehensive examination for the adsorption mechanisms, dynamic and kinetic processes involved in the adsorption processes. This investigation utilizes scanning tunneling microscopy to visualize the H2O adsorption processes on the Si(100) surface with a sub-monolayers (<0.05 ML) of chemically-reactive dangling bonds remaining after exposure to (1) a hydrogen atomic beam, (2) H2O, and (3) Cl2gases at room temperature. In all three cases, each of the remaining isolated single dangling bonds (sDB) adsorb and is passivated by either of the two dissociation fragments, the H or OH radical, to form a surface Si-H and Si-OH species. A new adsorption mechanism, termed 'dissociative and asynchronous chemisorption', is proposed for the observation presented herein. Upon approaching a sDB site, the H2O molecule breaks apart into two fragments. One is chemisorbed to the sDB. The other attaches to the same or the neighboring passivated dimer to form a transition state of surface diffusion, which then diffuses on the mostly passivated surface and is eventually chemisorbed to another reactive site. In other words, the chemisorption reactions of the two fragments after dissociation occur at different and uncorrelated time and places. This adsorption mechanism suggests that a diffusion transition state can be an adsorption product in the first step of the dissociative adsorption processes.

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