Proceedings of the National Academy of Sciences · 2017 · 94 citations · 34 references
Natural SciencesChemistryMaterials ScienceNanomaterialsNanotechnologySemiconductor MaterialsNanocatalysisOptical Properties Of SemiconductorsPhotocatalysisPhotochemistryQuantum DotsSemiconductor NanomaterialsEnergyNanoparticlesPhotocatalytic MaterialsPhotochemical ProcessesPhotophysical MechanismsSemiconductor PhotocatalysisSemiconductor PhotocatalystsSemiconductor Quantum Dots
manner. Surprisingly, we find that the photocatalytic reaction switches on and off stochastically despite the fact that the illumination is kept constant. The on and off states follow truncated and full-scale power-law distributions in broad time scales spanning 3-4 orders of magnitude, respectively, which can be described with a statistical model involving stochastic reactions rates at multiple active sites. This phenomenon is analogous to fluorescence photoblinking, but the underlying mechanism is different. As individual nanocatalyst represents the elementary photocatalytic platform, the discovery of the intermittent nature of the photocatalysis provides insights into the fundamental photochemistry and photophysics of semiconductor nanomaterials, which is anticipated to substantially benefit broad application fields such as clean energy, pollution treatment, and chemical synthesis.
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