Time-resolved energy-dispersive XAS studies of photoinduced electron transfer intermediates in electron donor-acceptor complexes

Lin X. Chen; Peter L. Lee; David Gosztola; Walter A. Svec; Michael R. Wasielewski

doi:10.1107/S0909049598014861

Time-resolved energy-dispersive XAS studies of photoinduced electron transfer intermediates in electron donor-acceptor complexes

Lin X. Chen^*, Peter L. Lee, David Gosztola, Walter A. Svec, Michael R. Wasielewski

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

11 Scopus citations

Abstract

The structure around the Fe atom of a photoinduced electron transfer intermediate in a di-porphyrin electron donor/acceptor complex is studied with time-resolved energy dispersive X-ray absorption spectroscopy. Photoinduced electron transfer from the lowest excited triplet state of a Zn porphyrin attached at a fixed 25 D distance by means of a long spacer molecule to an Fe(III) porphyrin occurs with a 6 ms time constant at 77 K. Time domain X-ray absorption measurements show that Fe(III) is transiently photoreduced to Fe(II) and that the bond between the Fe atom and a pyridine molecule ligated to it weakens substantially upon reduction of the Fe. Coupling of ligand loss to reduction of Fe(III) to Fe(II) provides a mean of stabilizing the reduced intermediate.

Original language	English (US)
Pages (from-to)	403-405
Number of pages	3
Journal	Journal of Synchrotron Radiation
Volume	6
Issue number	3
DOIs	https://doi.org/10.1107/S0909049598014861
State	Published - May 1 1999

Keywords

Energy dispersive XAS
Photoinduced electron transfer
Porphyrin complexes
Time-resolved XAFS
XANES

ASJC Scopus subject areas

Radiation
Nuclear and High Energy Physics
Instrumentation

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title = "Time-resolved energy-dispersive XAS studies of photoinduced electron transfer intermediates in electron donor-acceptor complexes",

abstract = "The structure around the Fe atom of a photoinduced electron transfer intermediate in a di-porphyrin electron donor/acceptor complex is studied with time-resolved energy dispersive X-ray absorption spectroscopy. Photoinduced electron transfer from the lowest excited triplet state of a Zn porphyrin attached at a fixed 25 D distance by means of a long spacer molecule to an Fe(III) porphyrin occurs with a 6 ms time constant at 77 K. Time domain X-ray absorption measurements show that Fe(III) is transiently photoreduced to Fe(II) and that the bond between the Fe atom and a pyridine molecule ligated to it weakens substantially upon reduction of the Fe. Coupling of ligand loss to reduction of Fe(III) to Fe(II) provides a mean of stabilizing the reduced intermediate.",

keywords = "Energy dispersive XAS, Photoinduced electron transfer, Porphyrin complexes, Time-resolved XAFS, XANES",

author = "Chen, {Lin X.} and Lee, {Peter L.} and David Gosztola and Svec, {Walter A.} and Wasielewski, {Michael R.}",

year = "1999",

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T1 - Time-resolved energy-dispersive XAS studies of photoinduced electron transfer intermediates in electron donor-acceptor complexes

AU - Chen, Lin X.

AU - Lee, Peter L.

AU - Gosztola, David

AU - Svec, Walter A.

AU - Wasielewski, Michael R.

PY - 1999/5/1

Y1 - 1999/5/1

N2 - The structure around the Fe atom of a photoinduced electron transfer intermediate in a di-porphyrin electron donor/acceptor complex is studied with time-resolved energy dispersive X-ray absorption spectroscopy. Photoinduced electron transfer from the lowest excited triplet state of a Zn porphyrin attached at a fixed 25 D distance by means of a long spacer molecule to an Fe(III) porphyrin occurs with a 6 ms time constant at 77 K. Time domain X-ray absorption measurements show that Fe(III) is transiently photoreduced to Fe(II) and that the bond between the Fe atom and a pyridine molecule ligated to it weakens substantially upon reduction of the Fe. Coupling of ligand loss to reduction of Fe(III) to Fe(II) provides a mean of stabilizing the reduced intermediate.

AB - The structure around the Fe atom of a photoinduced electron transfer intermediate in a di-porphyrin electron donor/acceptor complex is studied with time-resolved energy dispersive X-ray absorption spectroscopy. Photoinduced electron transfer from the lowest excited triplet state of a Zn porphyrin attached at a fixed 25 D distance by means of a long spacer molecule to an Fe(III) porphyrin occurs with a 6 ms time constant at 77 K. Time domain X-ray absorption measurements show that Fe(III) is transiently photoreduced to Fe(II) and that the bond between the Fe atom and a pyridine molecule ligated to it weakens substantially upon reduction of the Fe. Coupling of ligand loss to reduction of Fe(III) to Fe(II) provides a mean of stabilizing the reduced intermediate.

KW - Energy dispersive XAS

KW - Photoinduced electron transfer

KW - Porphyrin complexes

KW - Time-resolved XAFS

KW - XANES

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