Second-Order Nonlinear Optical Properties of an Amphiphilic Dye Embedded in a Lipid Bilayer. A Combined Molecular Dynamics-Quantum Chemistry Study
Second-Order Nonlinear Optical Properties of an Amphiphilic Dye Embedded in a Lipid Bilayer. A Combined Molecular Dynamics-Quantum Chemistry Study
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DOI：
10.1021/acs.jpcb.9b10988
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发表时间：
2020-03-19
影响因子：
3.3
通讯作者：
Champagne, Benoit
中科院分区：
文献类型：
--
作者：
Bouquiaux, Charlotte;Tonnele, Claire;Champagne, Benoit
通过结合分子动力学模拟和基于密度泛函理论的量子化学计算，计算了嵌入脂质双层的两亲性染料的二次谐波信号。这种计算方法可以深入了解完全水合的生物系统的形态和动力学，以及染料的几何形状和环境与其二阶非线性光学响应幅度之间的关系。结果指出，染料与膜的相互作用引起的动态第一超极化性显着增强，并强调了动力学、空间和静电效应的相对重要性。因此，这种计算方案对于合理化嵌入生物介质中的外源染料的二次谐波成像显微镜所揭示的非线性光学对比度特别相关。
The second harmonic signal of an amphiphilic dye embedded in a lipid bilayer has been calculated by combining molecular dynamics simulations and quantum chemistry calculations based on density functional theory. This computational approach provides insight into the morphology and dynamics of the fully hydrated biological system and the relationships linking the geometry and the environment of the dye to the amplitude of its second-order nonlinear optical response. The results point out a significant enhancement of the dynamic first hyperpolarizability of the dye induced by its interaction with the membrane and highlight the relative importance of dynamical, steric, and electrostatic effects. This computational scheme is thus particularly relevant for rationalizing the nonlinear optical contrasts revealed by second harmonic imaging microscopy of exogenous dyes embedded in biological media.