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Bioluminescence in the sea pansy Renilla involves three distinct proteins: Ca2+-actived coelenterazine-binding protein(CBP),Renilla luciferase(RLuc)and Renilla green-fluorescent protein(RrGFP).[1,2](Scheme 1)The general bioluminescent process consists of three steps in Renilla.First,CBP releases coelenterazine on binding Ca2+ for the bioluminescent reaction in RLuc [3].Then,coelenterazine was oxidized to dioxetanone that decomposes to coelenterazide with blue-light emission(480 nm)in RLuc catalysis.[4].Third,the excitation energy was transferred to RrGFP via bioluminescence resonance energy transfer(BRET)from RLuc,which brings out a secondary green-light emission(505 nm).[1] So Renilla bioluminescence is an enzyme-luciferin reaction rather than a Ca2+-regulated photoprotein reaction.[5] To thoroughly understand this bioluminescence,the following issues were researched by the combined quantum/molecular mechanics(QM/MM)calculations: 1)the bioluminescence mechanism of the coelenterazine dioxetanone in Renilla; 2)the light emitter for the first bioluminescence in RLuc; 3)the light emitter for the secondary bioluminescence in RrGFP.