Ultrafast Elemental and Oxidation-State Mapping of Hematite by 4D Electron Microscopy
We describe a new methodology that sheds light on the fundamental electronic processes that occur at the subsurface regions of inorganic solid photocatalysts. Three distinct kinds of microscopic imaging are used that yield spatial, temporal, and energy-resolved information. We also carefully conside...
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| Vydáno v: | Journal of the American Chemical Society Ročník 139; číslo 13; s. 4916 - 4922 |
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| Hlavní autoři: | , , , , |
| Médium: | Journal Article |
| Jazyk: | angličtina |
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United States
05.04.2017
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| ISSN: | 1520-5126 |
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| Abstract | We describe a new methodology that sheds light on the fundamental electronic processes that occur at the subsurface regions of inorganic solid photocatalysts. Three distinct kinds of microscopic imaging are used that yield spatial, temporal, and energy-resolved information. We also carefully consider the effect of photon-induced near-field electron microscopy (PINEM), first reported by Zewail et al. in 2009. The value of this methodology is illustrated by studying afresh a popular and viable photocatalyst, hematite, α-Fe
O
that exhibits most of the properties required in a practical application. By employing high-energy electron-loss signals (of several hundred eV), coupled to femtosecond temporal resolution as well as ultrafast energy-filtered transmission electron microscopy in 4D, we have, inter alia, identified Fe
ions that have a lifetime of a few picoseconds, as well as associated photoinduced electronic transitions and charge transfer processes. |
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| AbstractList | We describe a new methodology that sheds light on the fundamental electronic processes that occur at the subsurface regions of inorganic solid photocatalysts. Three distinct kinds of microscopic imaging are used that yield spatial, temporal, and energy-resolved information. We also carefully consider the effect of photon-induced near-field electron microscopy (PINEM), first reported by Zewail et al. in 2009. The value of this methodology is illustrated by studying afresh a popular and viable photocatalyst, hematite, α-Fe2O3 that exhibits most of the properties required in a practical application. By employing high-energy electron-loss signals (of several hundred eV), coupled to femtosecond temporal resolution as well as ultrafast energy-filtered transmission electron microscopy in 4D, we have, inter alia, identified Fe4+ ions that have a lifetime of a few picoseconds, as well as associated photoinduced electronic transitions and charge transfer processes. We describe a new methodology that sheds light on the fundamental electronic processes that occur at the subsurface regions of inorganic solid photocatalysts. Three distinct kinds of microscopic imaging are used that yield spatial, temporal, and energy-resolved information. We also carefully consider the effect of photon-induced near-field electron microscopy (PINEM), first reported by Zewail et al. in 2009. The value of this methodology is illustrated by studying afresh a popular and viable photocatalyst, hematite, α-Fe O that exhibits most of the properties required in a practical application. By employing high-energy electron-loss signals (of several hundred eV), coupled to femtosecond temporal resolution as well as ultrafast energy-filtered transmission electron microscopy in 4D, we have, inter alia, identified Fe ions that have a lifetime of a few picoseconds, as well as associated photoinduced electronic transitions and charge transfer processes. |
| Author | Thomas, John M Zewail, Ahmed H Zhou, Wuzong Baskin, J Spencer Su, Zixue |
| Author_xml | – sequence: 1 givenname: Zixue surname: Su fullname: Su, Zixue organization: Physical Biology Center for Ultrafast Science and Technology, Arthur Amos Noyes Laboratory of Chemical Physics, California Institute of Technology , Pasadena, California 91125, United States – sequence: 2 givenname: J Spencer surname: Baskin fullname: Baskin, J Spencer organization: Physical Biology Center for Ultrafast Science and Technology, Arthur Amos Noyes Laboratory of Chemical Physics, California Institute of Technology , Pasadena, California 91125, United States – sequence: 3 givenname: Wuzong orcidid: 0000-0001-9752-7076 surname: Zhou fullname: Zhou, Wuzong organization: School of Chemistry, University of St Andrews , St Andrews, Fife KY16 9ST, U.K – sequence: 4 givenname: John M surname: Thomas fullname: Thomas, John M organization: Department of Materials Science and Metallurgy, University of Cambridge , Cambridge CB3 0FS, U.K – sequence: 5 givenname: Ahmed H surname: Zewail fullname: Zewail, Ahmed H organization: Physical Biology Center for Ultrafast Science and Technology, Arthur Amos Noyes Laboratory of Chemical Physics, California Institute of Technology , Pasadena, California 91125, United States |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/28273420$$D View this record in MEDLINE/PubMed |
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| Title | Ultrafast Elemental and Oxidation-State Mapping of Hematite by 4D Electron Microscopy |
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