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Innovative bilayer nanofilms composed of semiconducting ZnS and ZnO hollow microspheres are successfully fabricated by an oil–water interfacial self‐assembly strategy. The photocurrent of the bilayer film‐based photodetectors is dependent on the stacking orders of the building blocks. The optimal optoelectronic properties of the ZnS(up)/ZnO(down) device are much better than those of the monolayer‐film...
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