On the orbital anisotropy in hematite nanorod-based photoanodes

The orbital anisotropy of hematite (-Fe 2 O 3 ) nanorod arrays, an engineered structure commonly investigated for applications in solar water oxidation photoanodes, is probed using polarization-dependent soft X-ray absorption spectroscopy at the O K-edge and at the Fe L 2,3 -edge. Thereby the unoccu...

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Published inPhysical chemistry chemical physics : PCCP Vol. 15; no. 32; pp. 13483 - 13488
Main Authors Kronawitter, Coleman X, Zegkinoglou, Ioannis, Shen, Shaohua, Guo, Jinghua, Himpsel, Franz J, Mao, Samuel S, Vayssieres, Lionel
Format Journal Article
LanguageEnglish
Published Cambridge Royal Society of Chemistry 28.08.2013
Subjects
Anisotropy
Arrays
Atomic structure
Chemistry
Exact sciences and technology
General and physical chemistry
Hematite
Iron
Nanostructure
Orbitals
Symmetry
Water
Conduction
Polarization
Binary compound
Iron oxide
Line shape
Metal ion
Hybridization
Density
Electrodes
Nanometer scale
Energy
Light
Corundum structure
Calculation
Oxidation
Solar radiation
Nanorod
Nanocrystal
Hematite
Transition element compounds
Crystals
Substrate
Anisotropy
Orbital
X ray absorption
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Abstract The orbital anisotropy of hematite (-Fe 2 O 3 ) nanorod arrays, an engineered structure commonly investigated for applications in solar water oxidation photoanodes, is probed using polarization-dependent soft X-ray absorption spectroscopy at the O K-edge and at the Fe L 2,3 -edge. Thereby the unoccupied states of -Fe 2 O 3 are examined. In the lowest energy region these are found to be strongly-hybridized Fe 3d (a 1g ) orbitals and O 2 ligand 2p orbitals, oriented along the c -axis. For [110]-oriented -Fe 2 O 3 nanocrystals the observed direction of strong hybridization is parallel to the substrate surface (perpendicular to the direction of electron conduction and light propagation in operating electrodes). The Fe L 3 -edge line shape and aspects of polarization dependence can be reproduced by crystal field atomic multiplet calculations of 2p-to-3d transitions for Fe 3+ in the D 3d point group symmetry of metal ions in the corundum structure. Both the O K-edge and Fe L 3 -edge spectra possess features that may be related to the high density of surface atoms in this nanoscale system. They are associated with partial coordination and therefore reduced symmetry compared to that for Fe 3+ in bulk crystals. This study establishes the orbital character and orientation of unoccupied states located at the conduction band minimum of hematite-nanorod arrays.
AbstractList The orbital anisotropy of hematite ( alpha -Fe sub(2)O sub(3)) nanorod arrays, an engineered structure commonly investigated for applications in solar water oxidation photoanodes, is probed using polarization-dependent soft X-ray absorption spectroscopy at the O K-edge and at the Fe L sub(2,3)-edge. Thereby the unoccupied states of alpha -Fe sub(2)O sub(3) are examined. In the lowest energy region these are found to be strongly-hybridized Fe 3d (a sub(1g)) orbitals and O super(2-) ligand 2p orbitals, oriented along the c-axis. For [110]-oriented alpha -Fe sub(2)O sub(3) nanocrystals the observed direction of strong hybridization is parallel to the substrate surface (perpendicular to the direction of electron conduction and light propagation in operating electrodes). The Fe L sub(3)-edge line shape and aspects of polarization dependence can be reproduced by crystal field atomic multiplet calculations of 2p-to-3d transitions for Fe super(3+) in the D sub(3d) point group symmetry of metal ions in the corundum structure. Both the O K-edge and Fe L sub(3)-edge spectra possess features that may be related to the high density of surface atoms in this nanoscale system. They are associated with partial coordination and therefore reduced symmetry compared to that for Fe super(3+) in bulk crystals.
The orbital anisotropy of hematite (α-Fe2O3) nanorod arrays, an engineered structure commonly investigated for applications in solar water oxidation photoanodes, is probed using polarization-dependent soft X-ray absorption spectroscopy at the O K-edge and at the Fe L2,3-edge. Thereby the unoccupied states of α-Fe2O3 are examined. In the lowest energy region these are found to be strongly-hybridized Fe 3d (a1g) orbitals and O(2-) ligand 2p orbitals, oriented along the c-axis. For [110]-oriented α-Fe2O3 nanocrystals the observed direction of strong hybridization is parallel to the substrate surface (perpendicular to the direction of electron conduction and light propagation in operating electrodes). The Fe L3-edge line shape and aspects of polarization dependence can be reproduced by crystal field atomic multiplet calculations of 2p-to-3d transitions for Fe(3+) in the D3d point group symmetry of metal ions in the corundum structure. Both the O K-edge and Fe L3-edge spectra possess features that may be related to the high density of surface atoms in this nanoscale system. They are associated with partial coordination and therefore reduced symmetry compared to that for Fe(3+) in bulk crystals.
The orbital anisotropy of hematite (-Fe 2 O 3 ) nanorod arrays, an engineered structure commonly investigated for applications in solar water oxidation photoanodes, is probed using polarization-dependent soft X-ray absorption spectroscopy at the O K-edge and at the Fe L 2,3 -edge. Thereby the unoccupied states of -Fe 2 O 3 are examined. In the lowest energy region these are found to be strongly-hybridized Fe 3d (a 1g ) orbitals and O 2 ligand 2p orbitals, oriented along the c -axis. For [110]-oriented -Fe 2 O 3 nanocrystals the observed direction of strong hybridization is parallel to the substrate surface (perpendicular to the direction of electron conduction and light propagation in operating electrodes). The Fe L 3 -edge line shape and aspects of polarization dependence can be reproduced by crystal field atomic multiplet calculations of 2p-to-3d transitions for Fe 3+ in the D 3d point group symmetry of metal ions in the corundum structure. Both the O K-edge and Fe L 3 -edge spectra possess features that may be related to the high density of surface atoms in this nanoscale system. They are associated with partial coordination and therefore reduced symmetry compared to that for Fe 3+ in bulk crystals. This study establishes the orbital character and orientation of unoccupied states located at the conduction band minimum of hematite-nanorod arrays.
Author Vayssieres, Lionel
Mao, Samuel S
Guo, Jinghua
Zegkinoglou, Ioannis
Kronawitter, Coleman X
Himpsel, Franz J
Shen, Shaohua
AuthorAffiliation Advanced Light Source
State Key Laboratory of Multiphase Flow in Power Engineering
University of Wisconsin
International Research Center for Renewable Energy
Department of Chemistry and Biochemistry
Lawrence Berkeley National Laboratory
University of California
Department of Mechanical Engineering
Xi'an Jiaotong University
Environmental Energy Technologies Division
Department of Physics
AuthorAffiliation_xml – name: University of California
– name: Department of Mechanical Engineering
– name: Lawrence Berkeley National Laboratory
– name: Xi'an Jiaotong University
– name: University of Wisconsin
– name: Environmental Energy Technologies Division
– name: Department of Physics
– name: Advanced Light Source
– name: State Key Laboratory of Multiphase Flow in Power Engineering
– name: International Research Center for Renewable Energy
– name: Department of Chemistry and Biochemistry
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  surname: Kronawitter
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– sequence: 2
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Issue 32
Keywords Water
Conduction
Polarization
Binary compound
Iron oxide
Line shape
Metal ion
Hybridization
Density
Electrodes
Nanometer scale
Energy
Light
Corundum structure
Calculation
Oxidation
Solar radiation
Nanorod
Nanocrystal
Hematite
Transition element compounds
Crystals
Substrate
Anisotropy
Orbital
X ray absorption
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Snippet The orbital anisotropy of hematite (-Fe 2 O 3 ) nanorod arrays, an engineered structure commonly investigated for applications in solar water oxidation...
The orbital anisotropy of hematite (α-Fe2O3) nanorod arrays, an engineered structure commonly investigated for applications in solar water oxidation...
The orbital anisotropy of hematite ( alpha -Fe sub(2)O sub(3)) nanorod arrays, an engineered structure commonly investigated for applications in solar water...
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SubjectTerms Anisotropy
Arrays
Atomic structure
Chemistry
Exact sciences and technology
General and physical chemistry
Hematite
Iron
Nanostructure
Orbitals
Symmetry
Title On the orbital anisotropy in hematite nanorod-based photoanodes
URI https://www.ncbi.nlm.nih.gov/pubmed/23839223
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