Bio-inspired and Smart Materials, MESA+ Institute for Nanotechnology, University of Twente, 7500 AE Enschede, The Netherlands.
Sorbonne Universités, CNRS, Institut des NanoSciences de Paris (INSP), F-75005 Paris, France.
Proc Natl Acad Sci U S A. 2018 Apr 24;115(17):4334-4339. doi: 10.1073/pnas.1720742115. Epub 2018 Apr 6.
Cholesteric liquid crystal (CLC) droplets exhibit nontrivial topological features, which are controlled by the ratio between the cholesteric pitch and the droplet radius. The radial spherical structure (RSS) is of particular interest, as it reveals an onion-like concentric organization of the cholesteric helices, leading to the expression of spherical Bragg microcavities. Using an overcrowded alkene-based unidirectional molecular motor as a dopant, we show that the topological defect structure in the droplet can be activated by illumination. By using appropriate molecular motor concentrations, light can either break the symmetry of topological defects (as observed for the bent-twisted bipolar structure), or it can induce inversion of handedness in an onion-like organization (in the case of RSS). This latter feature may pave the way toward alternative activation modes of lasers based on cholesteric droplets. By also studying CLC droplets once they have reached full photoconversion at photostationary state (PSS), we highlight that the strong influence of confinement on the droplets structure occurs to the same extent after the helix inversion event. Our results are interpreted in terms of numerical simulations of the droplets' structure, which shed light on the major role played by curvature close to the droplets' center, this latter one becoming dominant when the droplet radius is small.
胆甾相液晶 (CLC) 液滴表现出非平凡的拓扑特征,这些特征由胆甾相螺距与液滴半径的比值控制。径向球型结构 (RSS) 特别有趣,因为它揭示了胆甾螺旋的洋葱状同心组织,导致形成球形布拉格微腔。我们使用一个拥挤的基于烯烃的单向分子马达作为掺杂剂,表明液滴中的拓扑缺陷结构可以通过光照来激活。通过使用适当的分子马达浓度,光可以打破拓扑缺陷的对称性(如弯曲扭曲双极结构所观察到的那样),或者它可以诱导洋葱状组织中手性的反转(在 RSS 的情况下)。后者可能为基于胆甾相液滴的激光开辟替代激活模式。通过研究一旦达到光稳定状态(PSS)的完全光转换的 CLC 液滴,我们强调,在螺旋反转事件之后, confinement 对液滴结构的强烈影响以相同的程度发生。我们的结果根据液滴结构的数值模拟进行解释,这些模拟揭示了靠近液滴中心的曲率所起的主要作用,当液滴半径较小时,后者变得占主导地位。