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Monitoring excited state dynamics in cis-[Ru(bpy)2(py)2]2+ by ultrafast synchrotron techniques

Paper ID Volume ID Publish Year Pages File Format Full-Text
54109 46997 2014 12 PDF Available
Title
Monitoring excited state dynamics in cis-[Ru(bpy)2(py)2]2+ by ultrafast synchrotron techniques
Abstract

•Synchrotron-based techniques are powerful tools in detecting ultrafast structural changes in photoactive metal complexes.•We combined TR-XSS and TR-XAS to study the excited state dynamics and photochemistry of cis-[Ru(bpy)2(py)2]Cl2 in water.•TR-XSS captured the release of one pyridine and the subsequent coordination of a water molecule after 800 ns excitation.•Differential fitting of 100 ps-TR-XAS data elucidated the 3MLCT geometry, in excellent agreement with DFT analysis.•In this work we summarize these recent insights, with an emphasis on the employed multitechique DFT-assisted methodology.

Photoactive metal complexes are applied in a variety of fields, including solar energy conversion, catalysis and medicinal chemistry. Their effectiveness depends on the excited-state features that control the nature of photoreaction intermediates and photoproducts. For this reason, the structural determination of light-induced transient species is fundamental for a rational design of novel photoactive metal complexes. Among the available time-resolved methods, synchrotron-based techniques are emerging as successful tools in detecting ultrafast structural changes in molecules. The aim of this contribution is to review the results obtained by our group combining TR-XSS (Time-Resolved X-ray Solution Scattering) and TR-XAS (Time-Resolved X-ray Absorption Spectroscopy) to study the excited state dynamics in cis-[Ru(bpy)2(py)2]Cl2, a model compound for ligand releasing applications. Besides a comprehensive summary of our previous work, we report here new findings we obtained by analysis of 100 ps-resolution TR-XSS dataset. The potential of these techniques towards applications in catalysis are discussed in comparison to other time resolved spectroscopies.

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Keywords
APS, Advanced photon source; DFT, Density functional theory; DW, Debye–Waller; ES, Excited state; ESRF, European synchrotron radiation facility; EXAFS, Extended X-ray absorption fine structure; GS, Ground state; MC, Metal centred (excited state); MLCT, Me
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Monitoring excited state dynamics in cis-[Ru(bpy)2(py)2]2+ by ultrafast synchrotron techniques
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Publisher
Database: Elsevier - ScienceDirect
Journal: Catalysis Today - Volume 229, 15 June 2014, Pages 34–45
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
Get Full-Text Now
Don't Miss Today's Special Offer
Price was $35.95
You save - $31
Price after discount Only $4.95
100% Money Back Guarantee
Full-text PDF Download
Online Support
Any Questions? feel free to contact us