Using femtosecond tabletop XUV spectroscopy to study nickel catalysis

Benke, Kristopher

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https://hdl.handle.net/2142/104367 Copy

Description

Title

Using femtosecond tabletop XUV spectroscopy to study nickel catalysis

Author(s)

Benke, Kristopher

Contributor(s)

Vura-Weis, Josh

Issue Date

2019-06-19

Keyword(s)

High-harmonic generation and XUV spectroscopy

Date of Ingest

• 2019-07-15T22:16:47Z
• 2020-01-25T19:30:16Z

Abstract

To improve the efficiency of first row transition metal catalysts to match their precious metal counterparts, a method must be used that can look at snapshots of the catalytic reaction and identify the salient qualities of key intermediates. Ultrafast tabletop extreme ultraviolet (XUV) spectroscopy is well suited to this purpose because it is sensitive to a metal’s oxidation state, spin state, and ligand field. In addition, it can be performed in the lab rather than at a largescale facility like a synchrotron or X-FEL. To demonstrate sensitivity of XUV spectroscopy to the electronic structure of nickel-centered complexes, I measure the photophysics of a nickel dithiocarbamate complex, nickel bis(diethyldithiocarbamate), chosen due to its similarities to catalytically-active nickel dithiolenes. I show how the electron density moves across the highly covalent nickel-sulfur bonds after excitation of an LMCT transition. Examining the excited state dynamics with XUV spectroscopy allows for clearer determination of the metal spin state and electron density, filling in gaps in the picture drawn by transient optical spectroscopy. Transient XUV spectroscopy is shown to measure both the electronic structure of the metal and the electron density on the ligand, providing a powerful tool to study charge flow between metal and ligand.

Publisher

International Symposium on Molecular Spectroscopy

Type of Resource

text

Genre of Resource

Conference Paper / Presentation

Language

eng

Permalink

http://hdl.handle.net/2142/104367

DOI

https://doi.org/10.15278/isms.2019.WK07

Copyright and License Information

Copyright 2019 Kristopher Benke

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