Ligand-field symmetry effects in Fe(II) polypyridyl compounds probed by transient X-ray absorption spectroscopy

Hana Cho; Matthew L. Strader; Kiryong Hong; Lindsey Jamula; Eric M. Gullikson; Tae Kyu Kim; Frank M. F. de Groot; James K. McCusker; Robert W. Schoenlein; Nils Huse

doi:10.1039/C2FD20040F

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Faraday Discussions

Issue 0, 2012

Discussion summary and research papers, in physical chemistry, chemical physics and biophysical chemistry.

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Ligand-field symmetry effects in Fe(II) polypyridyl compounds probed by transient X-ray absorption spectroscopy

Hana Cho,^a^b Matthew L. Strader,^a Kiryong Hong,^b Lindsey Jamula,^c Eric M. Gullikson,^d Tae Kyu Kim,*^b Frank M. F. de Groot,^e James K. McCusker,^c Robert W. Schoenlein^a and Nils Huse*^a^f

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Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, USA

Department of Chemistry and Chemistry Institute of Functional Materials, Pusan National University, Busan, Republic of Korea
E-mail: tkkim@pusan.ac.kr

Department of Chemistry, Michigan State University, East Lansing, USA

Center for X-Ray Optics, Lawrence Berkeley National Laboratory, Berkeley, USA

Department of Chemistry, Utrecht University, Utrecht, Netherlands

Max Planck Research Department for Structural Dynamics at the University of Hamburg & Center for Free Electron Laser Science, Hamburg, Germany
E-mail: nils.huse@mpsd.cfel.de

Faraday Discuss., 2012,157, 463-474

DOI: 10.1039/C2FD20040F
Received 28 Feb 2012, Accepted 11 May 2012
First published online 07 Sep 2012

This article is part of themed collection: Molecular Reaction Dynamics in Gases, Liquids and Interfaces

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Ultrafast excited-state evolution in polypyridyl Fe(II) complexes is of fundamental interest for understanding the origins of the sub-ps spin-state changes that occur upon photoexcitation of this class of compounds as well as for the potential impact such ultrafast dynamics have on incorporation of these compounds in solar energy conversion schemes or switchable optical storage technologies. We have demonstrated that ground-state and, more importantly, ultrafast time-resolved X-ray absorption methods can offer unique insights into the interplay between electronic and geometric structure that underpins the photo-induced dynamics of this class of compounds. The present contribution examines in greater detail how the symmetry of the ligand field surrounding the metal ion can be probed using these X-ray techniques. In particular, we show that steady-state K-edge spectroscopy of the nearest-neighbour nitrogen atoms reveals the characteristic chemical environment of the respective ligands and suggests an interesting target for future charge-transfer femtosecond and attosecond spectroscopy in the X-ray water window.

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