Abstract:
:Coherent multidimensional electronic spectroscopy is commonly used to investigate photophysical phenomena such as light harvesting in photosynthesis in which the system returns back to its ground state after energy transfer. By contrast, we introduce multidimensional spectroscopy to study ultrafast photochemical processes in which the investigated molecule changes permanently. Exemplarily, the emergence in 2D and 3D spectra of a cross-peak between reactant and product reveals the cis-trans photoisomerization of merocyanine isomers. These compounds have applications in organic photovoltaics and optical data storage. Cross-peak oscillations originate from a vibrational wave packet in the electronically excited state of the photoproduct. This concept isolates the isomerization dynamics along different vibrational coordinates assigned by quantum-chemical calculations, and is applicable to determine chemical dynamics in complex photoreactive networks.
journal_name
Proc Natl Acad Sci U S Aauthors
Ruetzel S,Diekmann M,Nuernberger P,Walter C,Engels B,Brixner Tdoi
10.1073/pnas.1323792111subject
Has Abstractpub_date
2014-04-01 00:00:00pages
4764-9issue
13eissn
0027-8424issn
1091-6490pii
1323792111journal_volume
111pub_type
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