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J Phys Chem B. 2018 Jan 18;122(2):927-932. doi: 10.1021/acs.jpcb.7b06989. Epub 2017 Nov 15.

Strong O 2p-Fe 3d Hybridization Observed in Solution-Grown Hematite Films by Soft X-ray Spectroscopies.

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Advanced Light Source, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
Department of Chemistry, Merkert Chemistry Center, Boston College , Chestnut Hill, Massachusetts 02467, United States.
Department of Chemistry and Biochemistry, University of California , Santa Cruz, California 95064, United States.


Photoelectrochemical (PEC) water splitting holds the potential as a direct route for solar energy conversation and storage. The performance of a PEC device is strongly influenced by the electronic properties of the photonanode surface. It has been shown that the synthesis methods can have a profound impact on the electronic properties and PEC performance of various photoelectrode materials such as hematite. Soft X-ray spectroscopic techniques, including O K-edge XAS and Fe L-edge XAS/XES, have been employed to investigate how the synthesis methods impact the electronic structure of resulting hematite materials. It is found that the hematite samples via solution regrowth methods show dramatically increased 3d-4sp band ratios in O K-edge XAS spectra and decreased relative elastic peak intensities in Fe L-edge RIXS spectra compared with samples synthesized via ALD or solution grown. The difference observed in O-K and Fe-L spectra indicated that solution regrowth strategy alters the O 2p-Fe 3d hybridization and hence the electronic structure of the hematite films, which proves to be beneficial for PEC performance of the hematite photoanode. Our findings provided new insights and potentially useful strategies for enhancing the PEC performance of photoanode materials.


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