De novo design of energy transfer proteins housing excitonically coupled chlorophyll special pairs

Autor: Nathan Ennist, Shunzhi Wang, Madison Kennedy, Mariano Curti, George Sutherland, Cvetelin Vasilev, Rachel Redler, Valentin Maffeis, Saeed Shareef, Anthony Sica, Ash Hua, Arundhati Deshmukh, Adam Moyer, Derrick Hicks, Avi Swartz, Ralph Cacho, Nathan Novy, Asim Bera, Alex Kang, Banumathi Sankaran, Matthew Johnson, Mike Reppert, Damian Ekiert, Gira Bhabha, Lance Stewart, Justin Caram, Barry Stoddard, Elisabet Romero, C. Neil Hunter, David Baker
Rok vydání: 2023
Popis: 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 independent of complexities of native photosynthetic proteins, and as a first step towards synthetic photosystems for new energy conversion technologies, we designed C2-symmetric proteins that precisely position chlorophyll dimers. X-ray crystallography shows that one designed protein binds two chlorophylls in a binding orientation matching native special pairs, while a second positions them in a previously unseen geometry. Spectroscopy reveals excitonic coupling, and fluorescence lifetime imaging demonstrates energy transfer. We designed special pair proteins to assemble into 24-chlorophyll octahedral nanocages; the design model and cryo-EM structure are nearly identical. The design accuracy and energy transfer function of these special pair proteins suggest that de novo design of artificial photosynthetic systems is within reach of current computational methods.
Databáze: OpenAIRE