Nemati Ahlam, Querciagrossa Lara, Callison Corinne, Shadpour Sasan, Nunes Gonçalves Diana P, Mori Taizo, Cui Ximin, Ai Ruoqi, Wang Jianfang, Zannoni Claudio, Hegmann Torsten
Materials Science Graduate Program, Kent State University, Kent, OH, USA.
Advanced Materials and Liquid Crystal Institute, Kent State University, Kent, OH, USA.
Sci Adv. 2022 Jan 28;8(4):eabl4385. doi: 10.1126/sciadv.abl4385. Epub 2022 Jan 26.
Chirality, as a concept, is well understood at most length scales. However, quantitative models predicting the efficacy of the transmission of chirality across length scales are lacking. We propose here a modus operandi for a chiral nanoshape solute in an achiral nematic liquid crystal host showing that that chirality transfer may be understood by unusually simple geometric considerations. This mechanism is based on the product of a pseudoscalar chirality indicator and of a geometric shape compatibility factor based on the two-dimensional isoperimetric quotients for each nanoshape solute. The model is tested on an experimental set of precisely engineered gold nanoshapes. These libraries of calculated and in-parallel acquired experimental data among related nanoshapes pave the way for predictive calculations of chirality transfer in nanoscale, macromolecular, and biological systems, from designing chiral discriminators and enantioselective catalysts to developing chiral metamaterials and understanding nature's innate ability to transfer homochirality across length scales.
作为一个概念,手性在大多数长度尺度上都得到了很好的理解。然而,缺乏预测手性跨长度尺度传递效率的定量模型。我们在此提出一种在手性向列型液晶主体中的手性纳米形状溶质的运作方式,表明手性传递可以通过异常简单的几何考虑来理解。这种机制基于一个赝标手性指标与一个基于每个纳米形状溶质的二维等周商的几何形状兼容性因子的乘积。该模型在一组精确设计的金纳米形状的实验装置上进行了测试。这些相关纳米形状之间的计算数据和并行获取的实验数据文库为纳米尺度、大分子和生物系统中的手性传递预测计算铺平了道路,从设计手性鉴别器和对映选择性催化剂到开发手性超材料以及理解自然界在跨长度尺度传递同手性的内在能力。