Journal
PHOTOSYNTHESIS RESEARCH
Volume 143, Issue 2, Pages 115-128Publisher
SPRINGER
DOI: 10.1007/s11120-019-00677-y
Keywords
Biohybrid antenna; Light-harvesting complex 2 (LH2); Sequential energy transfer; Monoexponential dynamics; Lipid bilayer; Femtosecond transient absorption spectroscopy
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Funding
- JSPS KAKENHI [JP26107002, JP16J00627, 17H05255]
- [JP18H05160]
- [JP18H05180]
- Grants-in-Aid for Scientific Research [17H05255] Funding Source: KAKEN
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Enhancing the light-harvesting potential of antenna components in a system of solar energy conversion is an important topic in the field of artificial photosynthesis. We constructed a biohybrid light-harvesting complex 2 (LH2) engineered from Rhodobacter sphaeroides IL106 strain. An artificial fluorophore Alexa Fluor 647 maleimide (A647) was attached to the LH2 bearing cysteine residue at the N-terminal region (LH2-NC) near B800 bacteriochlorophyll a (BChl) assembly. The A647-attached LH2-NC conjugate (LH2-NC-A647) preserved the integrity of the intrinsic chromophores, B800- and B850-BChls, and carotenoids. Femtosecond transient absorption spectroscopy revealed that the sequential energy transfer A647 -> B800 -> B850 occurs at time scale of 9-10 ps with monoexponential dynamics in micellar and lipid bilayer systems. A B800-removed conjugate (LH2-NC[B800(-)]-A647) exhibited a significant decrease in energy transfer efficiency in the micellar system; however, surprisingly, direct energy transfer from A647 to B850 was observed at a rate comparable to that for LH2-NC-A647. This result implies that the energy transfer pathway is modified after B800 removal. The results obtained suggested that a LH2 complex is a potential platform for construction of biohybrid light-harvesting materials with simple energy transfer dynamics through the site-selective attachment of the external antennae and the modifiable energy-funnelling pathway.
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