ArticleJournal of the American Chemical Society2016
Ultrafast Excited State Relaxation of a Metalloporphyrin Revealed by Femtosecond X-ray Absorption Spectroscopy.
Article in Journal of the American Chemical Society, 2016. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 28 papers.
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28 citing papers in PubMed, 98 citations in OpenAlex.
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- A Metallosupramolecular Receptor for Squaraine Dyes Enabling Ultrafast Dark Resonance Energy Transfer.Angewandte Chemie (International ed. in English) · 2026Article
- Influence of hydrogen bonding on twisted intramolecular charge transfer in coumarin dyes: an integrated experimental and theoretical investigation.RSC advances · 2025Article
- X-ray Absorption Spectroscopy of Dilute Metalloenzymes at X-ray Free-Electron Lasers in a Shot-by-Shot Mode.The journal of physical chemistry letters · 2025Article
- Excited-State Identification of a Nickel-Bipyridine Photocatalyst by Time-Resolved X-ray Absorption Spectroscopy.The journal of physical chemistry letters · 2024Article
- Nonadiabatic Charge Transfer within Photoexcited Nickel Porphyrins.The journal of physical chemistry letters · 2024Article
- Room temperature X-ray absorption spectroscopy of metalloenzymes with drop-on-demand sample delivery at XFELs.Pure and applied chemistry. Chimie pure et appliquee · 2023Article
- Molecular Design Principles to Elongate the Metal-to-Ligand Charge Transfer Excited-State Lifetimes of Square-Planar Nickel(II) Complexes.Journal of the American Chemical Society · 2022Article
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- Hole Dynamics in Photoexcited Hematite Studied with Femtosecond Oxygen K-edge X-ray Absorption Spectroscopy.The journal of physical chemistry letters · 2022Article
- Towards Understanding Excited-State Properties of Organic Molecules Using Time-Resolved Soft X-ray Absorption Spectroscopy.International journal of molecular sciences · 2021Article
- Capturing photochemical and photophysical transformations in iron complexes with ultrafast X-ray spectroscopy and scattering.Chemical science · 2021Review
- Ultrafast time-resolved x-ray absorption spectroscopy of ionized urea and its dimer throughStructural dynamics (Melville, N.Y.) · 2021Article
- The central role of the metal ion for photoactivity: Zn-Chemical science · 2021Article
- Using X-ray free-electron lasers for spectroscopy of molecular catalysts and metalloenzymes.Nature reviews. Physics · 2021Article
- Short-lived metal-centered excited state initiates iron-methionine photodissociation in ferrous cytochrome c.Nature communications · 2021Article
- Ultrafast structural dynamics of in-cage isomerization of diiodomethane in solution.Chemical science · 2020Article
- Simulation of time-resolved x-ray absorption spectroscopy of ultrafast dynamics in particle-hole-excited 4-(2-thienyl)-2,1,3-benzothiadiazole.Structural dynamics (Melville, N.Y.) · 2020Article
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Authors and funding
12 authors at 4 institutions in 2 countries.
Funding
Abstract
Photoexcited Nickel(II) tetramesitylporphyrin (NiTMP), like many open-shell metalloporphyrins, relaxes rapidly through multiple electronic states following an initial porphyrin-based excitation, some involving metal centered electronic configuration changes that could be harnessed catalytically before excited state relaxation. While a NiTMP excited state present at 100 ps was previously identified by X-ray transient absorption (XTA) spectroscopy at a synchrotron source as a relaxed (d,d) state, the lowest energy excited state (J. Am. Chem. Soc., 2007, 129, 9616 and Chem. Sci., 2010, 1, 642), structural dynamics before thermalization were not resolved due to the ∼100 ps duration of the available X-ray probe pulse. Using the femtosecond (fs) X-ray pulses of the Linac Coherent Light Source (LCLS), the Ni center electronic configuration from the initial excited state to the relaxed (d,d) state has been obtained via ultrafast Ni K-edge XANES (X-ray absorption near edge structure) on a time scale from hundreds of femtoseconds to 100 ps. This enabled the identification of a short-lived Ni(I) species aided by time-dependent density functional theory (TDDFT) methods. Computed electronic and nuclear structure for critical excited electronic states in the relaxation pathway characterize the dependence of the complex's geometry on the electron occupation of the 3d orbitals. Calculated XANES transitions for these excited states assign a short-lived transient signal to the spectroscopic signature of the Ni(I) species, resulting from intramolecular charge transfer on a time scale that has eluded previous synchrotron studies. These combined results enable us to examine the excited state structural dynamics of NiTMP prior to thermal relaxation and to capture intermediates of potential photocatalytic significance.
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