QM/MM Investigations on the Bioluminescent Decomposition of Coelenterazine Dioxetanone in Obelin |
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Authors: | YUE Ling |
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Institution: | Key Laboratory for Non-equilibrium Synthesis and Modulation of Condensed Matter, Ministry of Education, School of Sciences, Xi'an Jiaotong University, Xi'an 710049, P. R. China |
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Abstract: | The bioluminescent mechanism of colenterazine dioxetanone(CZD) in the photoprotein of Obelia(obelin) was investigated by the combined quantum and molecular mechanics(QM/MM) method at TD-DFT level, which involved the real protein environment in decomposition of 1,2-dioxetanones. The anionic decomposition of CZD in (CZD+H2O)- model can go through a charge transfer(CT) catalyzed asynchronous-concerted process, which can be elucidated by the gradual reversible CT initiated luminescence(GRCTIL) mechanism. The neutral CZD in (CZDH+H2O) decomposes through an uncatalyzed non-CT biradical process. The anionic decomposition catalyzed by CT, in which the S0/S1 surface "double crossing" hence has ability to provide high quantum yield of singlet chemiexcitation is thus more possible in bioluminescence of photoprotein. |
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Keywords: | 1 2-Dioxetanone Bioluminescence Coelenterazine Photoprotein Quantum and molecular mechanics |
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