3 years ago

Fusion of Ultraviolet–Visible and Infrared Transient Absorption Spectroscopy Data to Model Ultrafast Photoisomerization

Fusion of Ultraviolet–Visible and Infrared Transient Absorption Spectroscopy Data to Model Ultrafast Photoisomerization
Gotard Burdzinski, Michel Sliwa, Julien Rehault, Maylis Orio, Cyril Ruckebusch, Bruno Debus
Ultrafast photoisomerization reactions generally start at a higher excited state with excess of internal vibrational energy and occur via conical intersections. This leads to ultrafast dynamics which are difficult to investigate with a single transient absorption spectroscopy technique, be it in the ultraviolet–visible (UV–vis) or infrared (IR) domain. On one hand, the information available in the UV–vis domain is limited as only slight spectral changes are observed for different isomers. On the other hand, the interpretation of vibrational spectra is strongly hindered by intramolecular relaxation and vibrational cooling. These limitations can be circumvented by fusing UV–vis and IR transient absorption spectroscopy data in a multiset multivariate curve resolution analysis. We apply this approach to describe the spectrodynamics of the ultrafast cis–trans photoisomerization around the C–N double bond observed for aromatic Schiff bases. Twisted intermediate states could be elucidated, and isomerization was shown to occur through a continuous complete rotation. More broadly, data fusion can be used to rationalize a vast range of ultrafast photoisomerization processes of interest in photochemistry.

Publisher URL: http://dx.doi.org/10.1021/acs.jpclett.7b01255

DOI: 10.1021/acs.jpclett.7b01255

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