Berraud-Pache Romain, Navizet Isabelle
Université Paris-Est, Laboratoire Modélisation et Simulation Multi Echelle, MSME, UMR 8208 CNRS, UPEM, 5 bd Descartes, 77454 Marne-la-Vallée, France.
Phys Chem Chem Phys. 2016 Oct 5;18(39):27460-27467. doi: 10.1039/c6cp02585d.
In this publication we conduct calculations on a newly synthesised red-shifted emitter of luciferin in order to understand what are the main contributions to the colour-shifting emission. Indeed the bioluminescent system, especially from fireflies, is one of the main resources for medical imaging but its efficiency greatly depends on the wavelength of the emission. We performed classical molecular dynamics followed by quantum mechanics/molecular mechanics (QM/MM) calculations, with either density functional theory or multiconfigurational reference second-order perturbation theory on different emitters to obtain bioluminescence emission. We analysed the calculations and investigated the effects which play a non-negligible role in the emission, like the effect of the surroundings or the effect of the conformation of the emitter. Finally, in the absence of crystallographic structures, we proposed the most likely conformation for the emitter in the bioluminescence process.
在本出版物中，我们对一种新合成的红移荧光素发射体进行了计算，以了解对颜色变化发射的主要贡献是什么。实际上，生物发光系统，尤其是萤火虫的生物发光系统，是医学成像的主要资源之一，但其效率在很大程度上取决于发射波长。我们进行了经典分子动力学计算，随后采用量子力学/分子力学（QM/MM）计算，运用密度泛函理论或多组态参考二阶微扰理论对不同的发射体进行计算，以获得生物发光发射。我们分析了计算结果，并研究了在发射过程中起不可忽视作用的影响因素，如周围环境的影响或发射体构象的影响。最后，在没有晶体结构的情况下，我们提出了生物发光过程中发射体最可能的构象。
