scholarly journals Manipulating charge transfer excited state relaxation and spin crossover in iron coordination complexes with ligand substitution

2017 ◽  
Vol 8 (1) ◽  
pp. 515-523 ◽  
Author(s):  
Wenkai Zhang ◽  
Kasper S. Kjær ◽  
Roberto Alonso-Mori ◽  
Uwe Bergmann ◽  
Matthieu Chollet ◽  
...  
Keyword(s):  
Excited State ◽  
Charge Transfer ◽  
Free Electron ◽  
Free Electron Laser ◽  
Spin Crossover ◽  
Coordination Complexes ◽  
Ligand Substitution ◽  
X Ray ◽  
Laser Measurements ◽  
Iron Coordination

Optical and X-ray free-electron laser measurements reveal ligand substitution in an Fe(ii)-centered complex extends its MLCT lifetime.

scholarly journals Imaging ultrafast excited state pathways in transition metal complexes by X-ray transient absorption and scattering using X-ray free electron laser source

2016 ◽  
Vol 194 ◽  
pp. 639-658 ◽  
Author(s):  
Lin X. Chen ◽  
Megan L. Shelby ◽  
Patrick J. Lestrange ◽  
Nicholas E. Jackson ◽  
Kristoffer Haldrup ◽  
...  
Keyword(s):  
Excited State ◽  
Transition Metal ◽  
Free Electron ◽  
Free Electron Laser ◽  
Electronic Configuration ◽  
Laser Source ◽  
Relaxation Processes ◽  
Valence Orbital ◽  
X Ray ◽  
Orbital Energies

This report will describe our recent studies of transition metal complex structural dynamics on the fs and ps time scales using an X-ray free electron laser source, Linac Coherent Light Source (LCLS). Ultrafast XANES spectra at the Ni K-edge of nickel(ii) tetramesitylporphyrin (NiTMP) were measured for optically excited states at a timescale from 100 fs to 50 ps, providing insight into its sub-ps electronic and structural relaxation processes. Importantly, a transient reduced state Ni(i) (π, 3dx2−y2) electronic state is captured through the interpretation of a short-lived excited state absorption on the low-energy shoulder of the edge, which is aided by the computation of X-ray transitions for postulated excited electronic states. The observed and computed inner shell to valence orbital transition energies demonstrate and quantify the influence of the electronic configuration on specific metal orbital energies. A strong influence of the valence orbital occupation on the inner shell orbital energies indicates that one should not use the transition energy from 1s to other orbitals to draw conclusions about the d-orbital energies. For photocatalysis, a transient electronic configuration could influence d-orbital energies up to a few eV and any attempt to steer the reaction pathway should account for this to ensure that external energies can be used optimally in driving desirable processes. NiTMP structural evolution and the influence of the porphyrin macrocycle conformation on relaxation kinetics can be likewise inferred from this study.

scholarly journals Improved charge transfer multiplet method to simulateM- andL-edge X-ray absorption spectra of metal-centered excited states

2018 ◽  
Vol 25 (5) ◽  
pp. 1600-1608 ◽  
Author(s):  
Kaili Zhang ◽  
Gregory S. Girolami ◽  
Josh Vura-Weis
Keyword(s):  
Excited State ◽  
Charge Transfer ◽  
Excited States ◽  
Transition Metal Complexes ◽  
Software Package ◽  
Spin Crossover ◽  
Difference Spectra ◽  
X Ray ◽  
Spectroscopic Signatures ◽  
X Ray Absorption

Charge transfer multiplet (CTM) theory is a computationally undemanding and highly mature method for simulating the soft X-ray spectra of first-row transition metal complexes. However, CTM theory has seldom been applied to the simulation of excited-state spectra. In this article, theCTM4XASsoftware package is extended to simulateM2,3- andL2,3-edge spectra for the excited states of first-row transition metals and also interpret CTM eigenfunctions in terms of Russell–Saunders term symbols. These new programs are used to reinterpret the recently reported excited-stateM2,3-edge difference spectra of photogenerated ferrocenium cations and to propose alternative assignments for the electronic state of these cations responsible for the spectroscopic features. These new programs were also used to model theL2,3-edge spectra of FeIIcompounds during nuclear relaxation following photoinduced spin crossover and to propose spectroscopic signatures for their vibrationally hot states.

scholarly journals Ultrafast Dynamics of Plasmon-Mediated Charge Transfer in Ag@CeO2 Studied by Free Electron Laser Time-Resolved X-ray Absorption Spectroscopy

Nano Letters ◽  
2021 ◽  
Vol 21 (4) ◽  
pp. 1729-1734
Author(s):  
Jacopo Stefano Pelli Cresi ◽  
Emiliano Principi ◽  
Eleonora Spurio ◽  
Daniele Catone ◽  
Patrick O’Keeffe ◽  
...  
Keyword(s):  
Charge Transfer ◽  
Absorption Spectroscopy ◽  
Free Electron ◽  
Free Electron Laser ◽  
Ultrafast Dynamics ◽  
Time Resolved ◽  
X Ray ◽  
X Ray Absorption

scholarly journals Femtosecond X-ray Absorption Spectroscopy at a Hard X-ray Free Electron Laser: Application to Spin Crossover Dynamics

2013 ◽  
Vol 117 (4) ◽  
pp. 735-740 ◽  
Author(s):  
Henrik T. Lemke ◽  
Christian Bressler ◽  
Lin X. Chen ◽  
David M. Fritz ◽  
Kelly J. Gaffney ◽  
...  
Keyword(s):  
Absorption Spectroscopy ◽  
Free Electron ◽  
Free Electron Laser ◽  
Spin Crossover ◽  
Laser Application ◽  
X Ray ◽  
X Ray Absorption

scholarly journals Finding intersections between electronic excited state potential energy surfaces with simultaneous ultrafast X-ray scattering and spectroscopy

2019 ◽  
Vol 10 (22) ◽  
pp. 5749-5760 ◽  
Author(s):  
Kasper S. Kjær ◽  
Tim B. Van Driel ◽  
Tobias C. B. Harlang ◽  
Kristjan Kunnus ◽  
Elisa Biasin ◽  
...  
Keyword(s):  
Excited State ◽  
Potential Energy ◽  
Free Electron ◽  
Free Electron Laser ◽  
Potential Energy Surfaces ◽  
X Ray ◽  
X Ray Scattering ◽  
State Potential ◽  
Laser Techniques ◽  
Energy Surfaces

Combined X-ray free-electron laser techniques pinpoints loci of intersections between potential energy surfaces of a photo-excited 3d transition-metal centered molecule.

X-Ray Free Electron Laser Facility for Next Generation of Scientific Exploration and Discovery

2011 ◽  
Vol 131 (2) ◽  
pp. 68-71
Author(s):  
Etsuo FUJIWARA ◽  
Eiichi ANAYAMA ◽  
Yuichiro KATSUTA ◽  
Toshiki IZUTANI ◽  
Daichi OKUHARA ◽  
...  
Keyword(s):  
Free Electron ◽  
Free Electron Laser ◽  
Next Generation ◽  
X Ray ◽  
Scientific Exploration ◽  
Laser Facility

X-ray Free Electron Laser SACLA

2014 ◽  
Vol 134 (12) ◽  
pp. 836-839
Author(s):  
Junichi INOUE ◽  
Yuji TANAKA ◽  
Yuki MATSUMOTO ◽  
Kensuke KANDA
Keyword(s):  
Free Electron ◽  
Free Electron Laser ◽  
X Ray
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