학술논문

De novo design of proteins housing excitonically coupled chlorophyll special pairs
Document Type
article
Source
Nature Chemical Biology. 20(7)
Subject
Biological Sciences
Chemical Sciences
Physical Chemistry
Biotechnology
Affordable and Clean Energy
Chlorophyll
Crystallography
X-Ray
Models
Molecular
Photosynthesis
Energy Transfer
Cryoelectron Microscopy
Protein Conformation
Light-Harvesting Protein Complexes
Medicinal and Biomolecular Chemistry
Biochemistry and Cell Biology
Biochemistry & Molecular Biology
Biochemistry and cell biology
Medicinal and biomolecular chemistry
Language
Abstract
Natural photosystems couple light harvesting to charge separation using a 'special pair' of chlorophyll molecules that accepts excitation energy from the antenna and initiates an electron-transfer cascade. To investigate the photophysics of special pairs independently of the complexities of native photosynthetic proteins, and as a first step toward creating synthetic photosystems for new energy conversion technologies, we designed C2-symmetric proteins that hold two chlorophyll molecules in closely juxtaposed arrangements. X-ray crystallography confirmed that one designed protein binds two chlorophylls in the same orientation as native special pairs, whereas a second designed protein positions them in a previously unseen geometry. Spectroscopy revealed that the chlorophylls are excitonically coupled, and fluorescence lifetime imaging demonstrated energy transfer. The cryo-electron microscopy structure of a designed 24-chlorophyll octahedral nanocage with a special pair on each edge closely matched the design model. The results suggest that the de novo design of artificial photosynthetic systems is within reach of current computational methods.