Resolving ultrafast photochemistry of coordination complexes using high harmonic generation xanes spectroscopy

Ryland, Elizabeth S.

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https://hdl.handle.net/2142/100781 Copy

Description

Title

Resolving ultrafast photochemistry of coordination complexes using high harmonic generation xanes spectroscopy

Author(s)

Ryland, Elizabeth S.

Contributor(s)

• Carlson, Michaela
• Benke, Kristin
• Lin, Ming-Fu
• Verkamp, Max A.
• Burhani, Muffaddal
• Zhang, Kaili
• Vura-Weis, Josh

Issue Date

2018-06-19

Keyword(s)

Dynamics and kinetics

Abstract

Extreme ultraviolet (XUV) spectroscopy is an inner shell technique that probes the M2,3 -edge excitation of atoms. Absorption of the XUV photon causes a 3p → 3d transition, the energy and multiplet of which is directly related to the element and ligand environment. This in-lab technique is thus element-, oxidation state-, spin state-, and ligand field specific and is a useful tool for the study of electron and energy transfer processes in materials and chemical biology. With the use of this technique and semi-empirical simulations, I have collected ultrafast transient M2,3 -edge absorption data of four different metalloporphyrinates (M = Fe, Co, Ni, Mn) in order to resolve the early time relaxation mechanism of these catalytically-relevant coordination complexes with femtosecond time resolution. This is the first instance of using tabletop transient XUV/VUV spectroscopy on coordination complexes and furthermore highlights the importance of directly probing of the metal center in these systems. I will additionally present ongoing work on applying this technique to the study of heterobimetallic systems with directly-interacting dual metal centers within a non-innocent ligand scaffold. The relation of function to metal-specific photodynamics will help lay essential groundwork for the development of multimetallic catalysts with efficiencies comparable to those found in nature.

Publisher

International Symposium on Molecular Spectroscopy

Type of Resource

text

Language

eng

Permalink

http://hdl.handle.net/2142/100781

DOI

10.15278/isms.2018.TD10

Copyright and License Information

Copyright 2018 Elizabeth S. Ryland

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