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Title: Excited state electron and energy relays in supramolecular dinuclear complexes revealed by ultrafast optical and X-ray transient absorption spectroscopy

Abstract

Here, the kinetics of photoinduced electron and energy transfer in a family of tetrapyridophenazine-bridged heteroleptic homo- and heterodinuclear copper(I) bis(phenanthroline)/ruthenium(II) polypyridyl complexes were studied using ultrafast optical and multi-edge X-ray transient absorption spectroscopies. This work combines the synthesis of heterodinuclear Cu(I)–Ru(II) analogs of the homodinuclear Cu(I)–Cu(I) targets with spectroscopic analysis and electronic structure calculations to first disentangle the dynamics at individual metal sites by taking advantage of the element and site specificity of X-ray absorption and theoretical methods. The excited state dynamical models developed for the heterodinuclear complexes are then applied to model the more challenging homodinuclear complexes. These results suggest that both intermetallic charge and energy transfer can be observed in an asymmetric dinuclear copper complex in which the ground state redox potentials of the copper sites are offset by only 310 meV. We also demonstrate the ability of several of these complexes to effectively and unidirectionally shuttle energy between different metal centers, a property that could be of great use in the design of broadly absorbing and multifunctional multimetallic photocatalysts. This work provides an important step toward developing both a fundamental conceptual picture and a practical experimental handle with which synthetic chemists, spectroscopists, and theoreticians may collaborate tomore » engineer cheap and efficient photocatalytic materials capable of performing coulombically demanding chemical transformations.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [3]
  1. Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, USA
  2. X-ray Science Division, Argonne National Laboratory, Argonne, USA
  3. Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, USA, Department of Chemistry
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1410479
Alternate Identifier(s):
OSTI ID: 1421973
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Chemical Science
Additional Journal Information:
Journal Name: Chemical Science Journal Volume: 9 Journal Issue: 4; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Hayes, Dugan, Kohler, Lars, Hadt, Ryan G., Zhang, Xiaoyi, Liu, Cunming, Mulfort, Karen L., and Chen, Lin X. Excited state electron and energy relays in supramolecular dinuclear complexes revealed by ultrafast optical and X-ray transient absorption spectroscopy. United Kingdom: N. p., 2018. Web. doi:10.1039/C7SC04055E.
Hayes, Dugan, Kohler, Lars, Hadt, Ryan G., Zhang, Xiaoyi, Liu, Cunming, Mulfort, Karen L., & Chen, Lin X. Excited state electron and energy relays in supramolecular dinuclear complexes revealed by ultrafast optical and X-ray transient absorption spectroscopy. United Kingdom. doi:10.1039/C7SC04055E.
Hayes, Dugan, Kohler, Lars, Hadt, Ryan G., Zhang, Xiaoyi, Liu, Cunming, Mulfort, Karen L., and Chen, Lin X. Mon . "Excited state electron and energy relays in supramolecular dinuclear complexes revealed by ultrafast optical and X-ray transient absorption spectroscopy". United Kingdom. doi:10.1039/C7SC04055E.
@article{osti_1410479,
title = {Excited state electron and energy relays in supramolecular dinuclear complexes revealed by ultrafast optical and X-ray transient absorption spectroscopy},
author = {Hayes, Dugan and Kohler, Lars and Hadt, Ryan G. and Zhang, Xiaoyi and Liu, Cunming and Mulfort, Karen L. and Chen, Lin X.},
abstractNote = {Here, the kinetics of photoinduced electron and energy transfer in a family of tetrapyridophenazine-bridged heteroleptic homo- and heterodinuclear copper(I) bis(phenanthroline)/ruthenium(II) polypyridyl complexes were studied using ultrafast optical and multi-edge X-ray transient absorption spectroscopies. This work combines the synthesis of heterodinuclear Cu(I)–Ru(II) analogs of the homodinuclear Cu(I)–Cu(I) targets with spectroscopic analysis and electronic structure calculations to first disentangle the dynamics at individual metal sites by taking advantage of the element and site specificity of X-ray absorption and theoretical methods. The excited state dynamical models developed for the heterodinuclear complexes are then applied to model the more challenging homodinuclear complexes. These results suggest that both intermetallic charge and energy transfer can be observed in an asymmetric dinuclear copper complex in which the ground state redox potentials of the copper sites are offset by only 310 meV. We also demonstrate the ability of several of these complexes to effectively and unidirectionally shuttle energy between different metal centers, a property that could be of great use in the design of broadly absorbing and multifunctional multimetallic photocatalysts. This work provides an important step toward developing both a fundamental conceptual picture and a practical experimental handle with which synthetic chemists, spectroscopists, and theoreticians may collaborate to engineer cheap and efficient photocatalytic materials capable of performing coulombically demanding chemical transformations.},
doi = {10.1039/C7SC04055E},
journal = {Chemical Science},
number = 4,
volume = 9,
place = {United Kingdom},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1039/C7SC04055E

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Cited by: 8 works
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Figures / Tables:

Fig. 1 Fig. 1: Chemical structures of ligands, dinuclear complexes, and mononuclear complexes studied in this work. The nomenclature and color scheme (boxes) introduced here is used throughout the text.

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    • Lazorski, Megan S.; Gest, Riley H.; Elliott, C. Michael
    • Journal of the American Chemical Society, Vol. 134, Issue 42
    • DOI: 10.1021/ja3085093

    Probing the Electronic Structure of a Photoexcited Solar Cell Dye with Transient X-ray Absorption Spectroscopy
    journal, June 2012

    • Van Kuiken, Benjamin E.; Huse, Nils; Cho, Hana
    • The Journal of Physical Chemistry Letters, Vol. 3, Issue 12
    • DOI: 10.1021/jz300671e

    Self-assembling hydrogel scaffolds for photocatalytic hydrogen production
    journal, October 2014

    • Weingarten, Adam S.; Kazantsev, Roman V.; Palmer, Liam C.
    • Nature Chemistry, Vol. 6, Issue 11
    • DOI: 10.1038/nchem.2075

    Towards artificial photosynthesis: ruthenium–manganese chemistry for energy production
    journal, January 2001

    • Sun, Licheng; Hammarström, Leif; Åkermark, Björn
    • Chemical Society Reviews, Vol. 30, Issue 1
    • DOI: 10.1039/a801490f

    Excited-state interconversion between emissive MLCT levels in a dinuclear Ru(ii) complex containing a bridging ligand with an extended π system
    journal, January 2000

    • Flamigni, Lucia; Encinas, Susana; Barigelletti, Francesco
    • Chemical Communications, Issue 13
    • DOI: 10.1039/b004109m

    Copper(i) dye-sensitized solar cells with [Co(bpy)3]2+/3+ electrolyte
    journal, January 2013

    • Bozic-Weber, Biljana; Constable, Edwin C.; Fürer, Sebastian O.
    • Chemical Communications, Vol. 49, Issue 65
    • DOI: 10.1039/c3cc44595j

    Detection of a charge-separated catalyst precursor state in a linked photosensitizer-catalyst assembly
    journal, January 2013

    • Mukherjee, Anusree; Kokhan, Oleksandr; Huang, Jier
    • Physical Chemistry Chemical Physics, Vol. 15, Issue 48
    • DOI: 10.1039/c3cp54420f

    X-ray transient absorption structural characterization of the 3MLCT triplet excited state of cis-[Ru(bpy)2(py)2]2+
    journal, January 2013

    • Borfecchia, Elisa; Garino, Claudio; Salassa, Luca
    • Dalton Transactions, Vol. 42, Issue 18
    • DOI: 10.1039/c3dt32865a

    Cu( i ) vs. Ru( ii ) photosensitizers: elucidation of electron transfer processes within a series of structurally related complexes containing an extended π-system
    journal, January 2018

    • Zhang, Ying; Traber, Philipp; Zedler, Linda
    • Physical Chemistry Chemical Physics, Vol. 20, Issue 38
    • DOI: 10.1039/c8cp04595j

    Application of a multi-element Ge detector in laser pump/x-ray probe time-domain x-ray absorption fine structure
    journal, February 2002

    • Jennings, Guy; Jäger, Wighard J. H.; Chen, Lin X.
    • Review of Scientific Instruments, Vol. 73, Issue 2
    • DOI: 10.1063/1.1433947

    Powering the planet: Chemical challenges in solar energy utilization
    journal, October 2006

    • Lewis, N. S.; Nocera, D. G.
    • Proceedings of the National Academy of Sciences, Vol. 103, Issue 43, p. 15729-15735
    • DOI: 10.1073/pnas.0603395103

    Biomimetic and Microbial Approaches to Solar Fuel Generation
    journal, December 2009

    • Magnuson, Ann; Anderlund, Magnus; Johansson, Olof
    • Accounts of Chemical Research, Vol. 42, Issue 12
    • DOI: 10.1021/ar900127h

    A Molecular Tetrad That Generates a High-Energy Charge-Separated State by Mimicking the Photosynthetic Z-Scheme
    journal, March 2016

    • Favereau, Ludovic; Makhal, Abhinandan; Pellegrin, Yann
    • Journal of the American Chemical Society, Vol. 138, Issue 11
    • DOI: 10.1021/jacs.5b12650

    Design of Efficient Photoinduced Charge Separation in Donor–Copper(I)–Acceptor Triad
    journal, November 2014

    • Sandroni, Martina; Maufroy, Antoine; Rebarz, Mateusz
    • The Journal of Physical Chemistry C, Vol. 118, Issue 49
    • DOI: 10.1021/jp507984s

    MODELS FOR BACTERIAL PHOTOSYNTHESIS: ELECTRON TRANSFER FROM PHOTOEXCITED SINGLET BACTERIOPHEOPHYTIN TO METHYL VIOLOGEN AND m-DINITROBENZENE
    journal, December 1978


    Cu( i ) vs. Ru( ii ) photosensitizers: elucidation of electron transfer processes within a series of structurally related complexes containing an extended π-system
    journal, January 2018

    • Zhang, Ying; Traber, Philipp; Zedler, Linda
    • Physical Chemistry Chemical Physics, Vol. 20, Issue 38
    • DOI: 10.1039/c8cp04595j

    Remarkably long-lived excited states of copper photosensitizers containing an extended π-system based on an anthracene moiety
    journal, January 2019

    • Giereth, Robin; Reim, Immanuel; Frey, Wolfgang
    • Sustainable Energy & Fuels, Vol. 3, Issue 3
    • DOI: 10.1039/c8se00521d