Leveraging excited-state coherence for synthetic control of ultrafast dynamics.

Nature
Bryan C PaulusJ K McCusker

Abstract

Design-specific control over excited-state dynamics is necessary for any application seeking to convert light into chemical potential. Such control is especially desirable in iron(II)-based chromophores, which are an Earth-abundant option for a wide range of photo-induced electron-transfer applications including solar energy conversion1 and catalysis2. However, the sub-200-femtosecond lifetimes of the redox-active metal-to-ligand charge transfer (MLCT) excited states typically encountered in these compounds have largely precluded their widespread use3. Here we show that the MLCT lifetime of an iron(II) complex can be manipulated using information from excited-state quantum coherences as a guide to implementing synthetic modifications that can disrupt the reaction coordinate associated with MLCT decay. We developed a structurally tunable molecular platform in which vibronic coherences-that is, coherences reflecting a coupling of vibrational and electronic degrees of freedom-were observed in ultrafast time-resolved absorption measurements after MLCT excitation of the molecule. Following visualization of the vibrational modes associated with these coherences, we synthetically modified an iron(II) chromophore to interfere with thes...Continue Reading

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Citations

Aug 19, 2020·Nature Chemistry·Julia A Weinstein
Dec 23, 2020·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Mohamed DarariPhilippe C Gros
Apr 21, 2021·Physical Chemistry Chemical Physics : PCCP·Kyle Barlow, J Olof Johansson
May 7, 2021·Accounts of Chemical Research·Christopher L WarkentinRenee R Frontiera
May 21, 2021·Journal of the American Chemical Society·Bryan C PaulusJames K McCusker
Jul 10, 2021·Chemical Communications : Chem Comm·Thomas ReuterKatja Heinze
Jul 17, 2021·The Journal of Physical Chemistry Letters·Pyosang KimLin X Chen
Nov 20, 2020·Journal of the American Chemical Society·Majed S FataftahDanna E Freedman
Jan 13, 2021·Journal of the American Chemical Society·Jakob B BilgerOliver S Wenger
Sep 2, 2021·The Journal of Physical Chemistry Letters·F HainerT Buckup
Sep 4, 2021·Journal of the American Chemical Society·Yusuke YonedaHiroshi Miyasaka
Sep 17, 2021·Journal of the American Chemical Society·Akin AydoganLudovic Troian-Gautier
Jan 14, 2022·Journal of the American Chemical Society·Wolfgang LeisAndreas Berkefeld

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Methods Mentioned

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