Artificial all-surface-atomic 2D sheets can trigger breakthroughs in tailoring the physical and chemical properties of advanced functional materials. Here, the conceptually new all-surface-atomic semiconductors of SnS and SnSe freestanding sheets are realized using a scalable strategy. As an example, all-surface-atomic SnS sheets undergo surface atomic elongation and structural disordering, which is revealed by X-ray absorption fine structure spectroscopy and first-principles calculations, endowing them with high structural stability and an increased density of states at the valence band edge. These exotic atomic and electronic structures make the all-surface-atomic SnS sheet-based photoelectrode exhibit an incident photon-to-current conversion efficiency of 67.1% at 490 nm, much higher than the efficiencies of other visible-light-driven water splitting. A photocurrent density of 5.27 mA cm-2, which is two orders of magnitude higher than that of the bulk counterpart, is also achieved for the all-surface-atomic SnS sheets-based photoelectrode. This will allow the manipulation of the basic properties of advanced materials on the atomic scale, thus paving the way for innovative applications.
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