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Tuning the color of firefly bioluminescence: a theoretical study on luciferin and luciferase modifications

Tuning the color of firefly bioluminescence: a theoretical s...

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第十三届全国量子化学会议

作者： Yuan-Yuan Cheng Ya-Jun Liu Key Laboratory of Theoretical and Computational Photochemistry Ministry of Education College of ChemistryBeijing Normal University

Firefly bioluminescence has various applications, such as biological analysis. To enhance the detection sensitivity and extend the application scope, a wide range of bioluminescence color is required. Both luciferin and luciferase modifications can achieve this goal. Experimentally,several luciferin analogues have been synthesized[1,2], but a modified regulation has not been proposed. Theoretically, we investigate the spectral properties of series of oxyluciferin analogues in the gas phase by time-dependent density functional theory（TD DFT）. A systematic modified regulation is summarized and one oxyluciferin analogue emitting near-infrared light is suggested. Massive mutants of luciferase have been reported at experiment[3,4], but theoretical study on mutant is scarce. We study the spectral properties of oxyluciferin（keto-1 form） and suggested oxyluciferin analogue in four mutants（S284T, R218 A, R337 K and PpyLit[5]） by hybrid quantum mechanics/molecular mechanics（QM/MM） combined with molecular dynamics（MD） method. A high accuracy method, multistate complete active space second-order perturbation（MS-CASPT2）, is employed. The steric, electrostatic, and H-bond effects are discussing.

关键词： modification luciferin luciferase bioluminescence

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Neither luciferin nor oxyluciferin of Latia is fluorescent-evidence from theoretical study

Neither luciferin nor oxyluciferin of Latia is fluorescent-e...

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第十三届全国量子化学会议

作者： Mo-Han Yu Ya-Jun Liu Key Laboratory of Theoretical and Computational Photochemistry Ministry of Education College of ChemistryBeijing Normal University

Latia neritoides is a small limpet-like snail that produces a bright green bioluminescence（BL） via a unique light-emitting system. Its bioluminescent process, mechanism and even light emitter remains unknown, although this BL has been reported for decades. Unlike the other BLs, neither luciferin（Luc） nor oxyluciferin（OxyLuc） of Latia is fluorescent according to the previously experimental studies. In order to identify its bioluminophore, we studied the geometrical and electronic structures and absorption and fluorescence spectra of Latia Luc and its six analogues as well as its OxyLuc in the gas phase and water. The calculated results provide clear evidence to nonfluorescence of Luc and OxyLuc of Latia. For the analogues of Latia Luc, the electron-withdrawing or electron-donating ability of the substituted group influences the fluorescence. This study sheds new light on the road to understand the Latia BL.

关键词： Latia luciferin oxyluciferin absorption spectrum fluorescence spectrum

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Theoretical Study of Fridericia heliota Bioluminescence

Theoretical Study of Fridericia heliota Bioluminescence

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第十三届全国量子化学会议

作者： Yi-Qi Tang Ya-Jun Liu Key Laboratory of Theoretical and Computational Photochemistry Ministry of EducationCollege of ChemistryBeijing Normal University

Fridericia heliota is a novel bioluminescent oligochaete worm whose luminescent system is different from those of other luminous representatives in Oligochaeta. This uniqueness is of obvious interest to researchers and can also be potentially useful for analytical *** novel mechanism of light production seems to be highly similar to that of the well-studied firefly bioluminescence. Unfortunately, the lack of biological material significantly hampers the progress in unraveling its detailed mechanism and verifying the actual light emitter for the natural system. Herein, we have investigated the geometries and properties of the luciferin and oxyluciferin of Fridericia heliota via the density functional calculations. The calculations were performed in the gas phase and solution. The calculated results are expected to give some help for the above questions in theory.

关键词： Fridericia heliota luciferin oxyluciferin bioluminescence

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