Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 17, Issue 24, Pages 16125-16135Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c5cp02145f
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Funding
- ERC [306536]
- Engineering and Physical Sciences Research Council [1214484] Funding Source: researchfish
- European Research Council (ERC) [306536] Funding Source: European Research Council (ERC)
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Temporary radical anions (resonances) of isolated co enzyme Q(0) (CQ(0)) and their associated above-threshold dynamics have been studied using frequency-, angle-, and time-resolved photoelectron imaging (FAT-PI). Experimental energetics and dynamics are supported with ab initio calculations. All results support that CQ(0) exhibits similar resonances and energetics compared with the smaller para-benzoquinone subunit, which is commonly considered as a prototype electrophore for larger biological para-quinone species. However, the above-threshold dynamics in CQ(0) relative to para-benzoquinone show significantly enhanced prompt detachment compared with internal conversion, particularly around the photoexcitation energy of 3.10 eV. The change in dynamics can be attributed to a combination of an increase in the shape character of the optically-accessible resonance at this energy, a decrease in the autodetachment lifetime due to the higher density of states in the neutral, and a decrease in the probability that the wavepacket formed in the Franck-Condon window can access the local conical intersection in CQ(0) over the timescale of autodetachment. Overall, this study serves as a clear example in understanding the trends in spectroscopy and dynamics in relating a simple prototypical para-quinone electrophore to a more complex biochemical species.
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