Tabletop Femtosecond M-edge X-ray Absorption Near-Edge Structure of FeTPPCl: Metalloporphyrin Photophysics from the Perspective of the Metal.
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| Title: | Tabletop Femtosecond M-edge X-ray Absorption Near-Edge Structure of FeTPPCl: Metalloporphyrin Photophysics from the Perspective of the Metal. |
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| Authors: | Ryland, Elizabeth S.1, Ming-Fu Lin1,2, Verkamp, Max A.1, Kaili Zhang1, Benke, Kristin1, Carlson, Michaela1, Vura-Weis, Josh1 vuraweis@illinois.edu |
| Source: | Journal of the American Chemical Society. 4/4/2018, Vol. 140 Issue 13, p4691-4696. 6p. |
| Subjects: | Femtosecond pulses, X-ray absorption, Porphyrins, Chromophores, Photoreceptors |
| Abstract: | Iron porphyrins are the active sites of many natural and artificial catalysts, and their photoinduced dynamics have been described as either relaxation into a vibrationally hot ground state or as a cascade through metal-centered states. In this work, we directly probe the metal center of iron(III) tetraphenyl porphyrin chloride (FeTPPCl) using femtosecond M2,3-edge X-ray absorption near-edge structure (XANES) spectroscopy. Photoexcitation at 400 nm produces a (π, π*) state that evolves in 70 fs to an iron(II) ligand-to-metal charge transfer (LMCT) state. The LMCT state relaxes to a vibrationally hot ground state in 1.13 ps, without involvement of (d,d) intermediates. The tabletop extremeultraviolet probe, combined with semiempirical ligand field multiplet calculations, clearly distinguishes between metal-centered and ligand-centered excited states and resolves competing accounts of Fe(III) porphyrin relaxation. This work introduces tabletop M-edge XANES as a valuable tool for measuring femtosecond dynamics of molecular transition metal complexes in the condensed phase. [ABSTRACT FROM AUTHOR] |
| Copyright of Journal of the American Chemical Society is the property of American Chemical Society and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.) | |
| Database: | Engineering Source |
| FullText | Text: Availability: 0 |
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| Header | DbId: egs DbLabel: Engineering Source An: 128955162 AccessLevel: 6 PubType: Academic Journal PubTypeId: academicJournal PreciseRelevancyScore: 0 |
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| Items | – Name: Title Label: Title Group: Ti Data: Tabletop Femtosecond M-edge X-ray Absorption Near-Edge Structure of FeTPPCl: Metalloporphyrin Photophysics from the Perspective of the Metal. – Name: Author Label: Authors Group: Au Data: <searchLink fieldCode="AR" term="%22Ryland%2C+Elizabeth+S%2E%22">Ryland, Elizabeth S.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Ming-Fu+Lin%22">Ming-Fu Lin</searchLink><relatesTo>1,2</relatesTo><br /><searchLink fieldCode="AR" term="%22Verkamp%2C+Max+A%2E%22">Verkamp, Max A.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Kaili+Zhang%22">Kaili Zhang</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Benke%2C+Kristin%22">Benke, Kristin</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Carlson%2C+Michaela%22">Carlson, Michaela</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Vura-Weis%2C+Josh%22">Vura-Weis, Josh</searchLink><relatesTo>1</relatesTo><i> vuraweis@illinois.edu</i> – Name: TitleSource Label: Source Group: Src Data: <searchLink fieldCode="JN" term="%22Journal+of+the+American+Chemical+Society%22">Journal of the American Chemical Society</searchLink>. 4/4/2018, Vol. 140 Issue 13, p4691-4696. 6p. – Name: Subject Label: Subjects Group: Su Data: <searchLink fieldCode="DE" term="%22Femtosecond+pulses%22">Femtosecond pulses</searchLink><br /><searchLink fieldCode="DE" term="%22X-ray+absorption%22">X-ray absorption</searchLink><br /><searchLink fieldCode="DE" term="%22Porphyrins%22">Porphyrins</searchLink><br /><searchLink fieldCode="DE" term="%22Chromophores%22">Chromophores</searchLink><br /><searchLink fieldCode="DE" term="%22Photoreceptors%22">Photoreceptors</searchLink> – Name: Abstract Label: Abstract Group: Ab Data: Iron porphyrins are the active sites of many natural and artificial catalysts, and their photoinduced dynamics have been described as either relaxation into a vibrationally hot ground state or as a cascade through metal-centered states. In this work, we directly probe the metal center of iron(III) tetraphenyl porphyrin chloride (FeTPPCl) using femtosecond M2,3-edge X-ray absorption near-edge structure (XANES) spectroscopy. Photoexcitation at 400 nm produces a (π, π*) state that evolves in 70 fs to an iron(II) ligand-to-metal charge transfer (LMCT) state. The LMCT state relaxes to a vibrationally hot ground state in 1.13 ps, without involvement of (d,d) intermediates. The tabletop extremeultraviolet probe, combined with semiempirical ligand field multiplet calculations, clearly distinguishes between metal-centered and ligand-centered excited states and resolves competing accounts of Fe(III) porphyrin relaxation. This work introduces tabletop M-edge XANES as a valuable tool for measuring femtosecond dynamics of molecular transition metal complexes in the condensed phase. [ABSTRACT FROM AUTHOR] – Name: AbstractSuppliedCopyright Label: Group: Ab Data: <i>Copyright of Journal of the American Chemical Society is the property of American Chemical Society and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.) |
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| RecordInfo | BibRecord: BibEntity: Identifiers: – Type: doi Value: 10.1021/jacs.8b01101 Languages: – Code: eng Text: English PhysicalDescription: Pagination: PageCount: 6 StartPage: 4691 Subjects: – SubjectFull: Femtosecond pulses Type: general – SubjectFull: X-ray absorption Type: general – SubjectFull: Porphyrins Type: general – SubjectFull: Chromophores Type: general – SubjectFull: Photoreceptors Type: general Titles: – TitleFull: Tabletop Femtosecond M-edge X-ray Absorption Near-Edge Structure of FeTPPCl: Metalloporphyrin Photophysics from the Perspective of the Metal. Type: main BibRelationships: HasContributorRelationships: – PersonEntity: Name: NameFull: Ryland, Elizabeth S. – PersonEntity: Name: NameFull: Ming-Fu Lin – PersonEntity: Name: NameFull: Verkamp, Max A. – PersonEntity: Name: NameFull: Kaili Zhang – PersonEntity: Name: NameFull: Benke, Kristin – PersonEntity: Name: NameFull: Carlson, Michaela – PersonEntity: Name: NameFull: Vura-Weis, Josh IsPartOfRelationships: – BibEntity: Dates: – D: 04 M: 04 Text: 4/4/2018 Type: published Y: 2018 Identifiers: – Type: issn-print Value: 00027863 Numbering: – Type: volume Value: 140 – Type: issue Value: 13 Titles: – TitleFull: Journal of the American Chemical Society Type: main |
| ResultId | 1 |
