Liu Zheyun, Li Xiankun, Zhong Frank W, Li Jiang, Wang Lijuan, Shi Yigong, Zhong Dongping
Department of Physics, Department of Chemistry and Biochemistry, and Programs of Biophysics, Chemical Physics, and Biochemistry, The Ohio State University, Columbus, Ohio 43210, United States.
Columbia University, New York, New York 10027, United States.
J Phys Chem Lett. 2014 Jan 2;5(1):69-72. doi: 10.1021/jz402396k.
UVR8 is a recently discovered UV-B photoreceptor with a homodimer as the active state. UV-B perception of an interfacial tryptophan (W285) causes dissociation of the dimer into two functional monomers. Here, we investigate the molecular mechanism behind UV perception by W285 in UVR8. We observed a significant quenching dynamics in about 150 ps within the interfacial four-tryptophan cluster and an unusual resonance energy transfer from the other ten tryptophans to the tryptophan cluster in 1-2 nanoseconds to enhance functional efficiency. With mutation of W285 to F, the quenching dynamics is highly suppressed in this intact mutant dimer and the overall fluorescence intensity dramatically increases by a factor of 6, indicating W285 as a dominant quencher. These results reveal a unique energy transfer mechanism for efficient UV perception and the critical functional role of W285 for primary quenching dynamics for initiating dimer dissociation to trigger the function.
UVR8是一种最近发现的UV-B光感受器,其活性状态为同型二聚体。界面色氨酸(W285)对UV-B的感知会导致二聚体解离成两个功能性单体。在此,我们研究了UVR8中W285对紫外线感知背后的分子机制。我们观察到界面四色氨酸簇内约150皮秒内有显著的猝灭动力学,以及在1 - 2纳秒内从其他十个色氨酸到色氨酸簇的异常共振能量转移,以提高功能效率。将W285突变为F后,在这个完整的突变二聚体中猝灭动力学受到高度抑制,整体荧光强度显著增加了6倍,表明W285是主要的猝灭剂。这些结果揭示了一种独特的能量转移机制,用于高效的紫外线感知,以及W285在启动二聚体解离以触发功能的初级猝灭动力学中的关键功能作用。