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Title: Resolving structures of transition metal complex reaction intermediates with femtosecond EXAFS

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI: https://doi.org/10.1039/C9CP03483H · OSTI ID:1558679
ORCiD logo [1];  [2];  [3];  [4];  [5]; ORCiD logo [6];  [4];  [4];  [4];  [3];  [6];  [4]
  1. Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, USA, Linac Coherent Light Source
  2. Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, USA, Stanford Synchrotron Radiation Lightsource
  3. Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, USA
  4. Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, USA
  5. SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, USA
  6. Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, USA
+ Show Author Affiliations

Femtosecond-resolved Extended X-ray Absorption Fine Structure (EXAFS) measurements of solvated transition metal complexes are successfully implemented at the X-ray Free Electron Laser LCLS. Benchmark experiments on [Fe(terpy)2]2+ in solution show a signal-to-noise ratio on the order of 500, comparable to typical 100 ps-resolution synchrotron measurements. In the few femtoseconds after photoexcitation, we observe the EXAFS fingerprints of a short-lived (B100 fs) intermediate as well as those of a vibrationally hot long-lived (Bns) excited state.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-76SF00515; SC0014607
OSTI ID:
1558679
Alternate ID(s):
OSTI ID: 1546779
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Vol. 22 Journal Issue: 5; ISSN 1463-9076
Publisher:
Royal Society of Chemistry (RSC)Copyright Statement
Country of Publication:
United Kingdom
Language:
English
Citation Metrics:
Cited by: 16 works
Citation information provided by
Web of Science

References (46)

Anisotropy enhanced X-ray scattering from solvated transition metal complexes journal February 2018
Femtosecond X-ray Absorption Spectroscopy at a Hard X-ray Free Electron Laser: Application to Spin Crossover Dynamics journal January 2013
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT journal June 2005
Probing Cytochrome c Folding Transitions upon Phototriggered Environmental Perturbations Using Time-Resolved X-ray Scattering journal April 2018
Using Ultrafast X-ray Spectroscopy To Address Questions in Ligand-Field Theory: The Excited State Spin and Structure of [Fe(dcpp) 2 ] 2+ journal June 2019
Ultrafast X-ray Absorption Near Edge Structure Reveals Ballistic Excited State Structural Dynamics journal May 2018
Discovery and High-Throughput Screening of Heteroleptic Iridium Complexes for Photoinduced Hydrogen Production journal May 2005
XANES and EXAFS of dilute solutions of transition metals at XFELs journal August 2019
Achieving few-femtosecond time-sorting at hard X-ray free-electron lasers journal February 2013
First lasing and operation of an ångstrom-wavelength free-electron laser journal August 2010
Coherent structural trapping through wave packet dispersion during photoinduced spin state switching journal May 2017
Femtosecond XANES Study of the Light-Induced Spin Crossover Dynamics in an Iron(II) Complex journal January 2009
Observing Solvation Dynamics with Simultaneous Femtosecond X-ray Emission Spectroscopy and X-ray Scattering journal February 2016
High-brightness table-top hard X-ray source driven by sub-100-femtosecond mid-infrared pulses journal November 2014
Structure of Myoglobin: A Three-Dimensional Fourier Synthesis at 2 Å. Resolution journal February 1960
Tracking excited-state charge and spin dynamics in iron coordination complexes journal May 2014
Highly Accurate Excited-State Structure of [Os(bpy) 2 dcbpy] 2+ Determined by X-ray Transient Absorption Spectroscopy journal June 2014
Photon Beam Transport and Scientific Instruments at the European XFEL journal June 2017
K -edge absorption spectra of selected vanadium compounds journal November 1984
A multi-crystal wavelength dispersive x-ray spectrometer journal July 2012
Metalloprotein entatic control of ligand-metal bonds quantified by ultrafast x-ray spectroscopy journal June 2017
The MXAN procedure: a new method for analysing the XANES spectra of metalloproteins to obtain structural quantitative information journal December 2002
Soft x-ray absorption spectroscopy of metalloproteins and high-valent metal-complexes at room temperature using free-electron lasers journal September 2017
Tuning the Electronic Structure of Fe(II) Polypyridines via Donor Atom and Ligand Scaffold Modifications: A Computational Study journal August 2015
Ultrafast Excited State Relaxation of a Metalloporphyrin Revealed by Femtosecond X-ray Absorption Spectroscopy journal July 2016
A Multiplet Analysis of Fe K-Edge 1s → 3d Pre-Edge Features of Iron Complexes journal July 1997
X-ray detectors at the Linac Coherent Light Source journal April 2015
Detailed Characterization of a Nanosecond-Lived Excited State: X-ray and Theoretical Investigation of the Quintet State in Photoexcited [Fe(terpy) 2 ] 2+ journal March 2015
Probing the Anisotropic Distortion of Photoexcited Spin Crossover Complexes with Picosecond X-ray Absorption Spectroscopy journal February 2014
Sequential Activation of Molecular Breathing and Bending during Spin-Crossover Photoswitching Revealed by Femtosecond Optical and X-Ray Absorption Spectroscopy journal November 2014
The X-ray Pump–Probe instrument at the Linac Coherent Light Source journal April 2015
Design and performance of an ultra-high-vacuum-compatible artificial channel-cut monochromator journal December 2007
A multi-MHz single-shot data acquisition scheme with high dynamic range: pump–probe X-ray experiments at synchrotrons journal October 2016
Observing heme doming in myoglobin with femtosecond X-ray absorption spectroscopya) journal May 2015
Polarized XANES Monitors Femtosecond Structural Evolution of Photoexcited Vitamin B 12 journal January 2017
XAFS spectroscopy; fundamental principles and data analysis journal May 2000
Potential for biomolecular imaging with femtosecond X-ray pulses journal August 2000
Resolving the Ultrafast Changes of Chemically Inequivalent Metal–Ligand Bonds in Photoexcited Molecular Complexes with Transient X-ray Absorption Spectroscopy journal April 2019
Dynamic Jahn–Teller Effect in the Metastable High-Spin State of Solvated [Fe(terpy) 2 ] 2+ journal January 2015
Solar Energy Conversion by Dye-Sensitized Photovoltaic Cells journal October 2005
Theoretical approaches to x-ray absorption fine structure journal July 2000
Revealing hole trapping in zinc oxide nanoparticles by time-resolved X-ray spectroscopy journal February 2018
Femtosecond time-resolved X-ray absorption spectroscopy of anatase TiO2 nanoparticles using XFEL journal June 2017
Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated [ Co ( terpy ) 2 ] 2 + journal June 2016
Smoothing and Differentiation of Data by Simplified Least Squares Procedures. journal July 1964
Architecture of the Photosynthetic Oxygen-Evolving Center journal March 2004

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