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https://doi.org/10.1021/jacs.4c10962
Copy DOIPublication Date: Oct 25, 2024 | |
Citations: 1 |
Photogenerated charge separation is pivotal for effecting efficient photocatalytic reactions. Understanding this process with spatiotemporal resolution is vital for devising highly efficient photocatalysts. Here, we employed pump-probe transient reflection microscopy to directly observe the temporal and spatial evolution of photogenerated electrons and holes on the surface of facet-engineered bismuth vanadate (BiVO4) crystals. The findings suggest that the anisotropic built-in field of BiVO4 crystals propels the separation of photogenerated electrons and holes toward different facets through a two-step process across varying time scales. Photogenerated electrons and holes undergo ultrafast separation within ∼6 ps, with electrons transforming into localized small polarons toward the {010} facets of truncated BiVO4 octahedral crystals. However, the photogenerated holes prolong their separation up to ∼2000 ps in a drift-diffusion manner before ultimately accumulating on the {120} facets. This work provides a comprehensive visualization of spatiotemporal charge separation at the nano/microscale on semiconductor photocatalysts, which is beneficial for understanding the photocatalysis mechanism.
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