Escárcega-Bobadilla Martha V, Maldonado-Domínguez Mauricio, Romero-Ávila Margarita, Zelada-Guillén Gustavo A
School of Chemistry, National Autonomous University of Mexico (UNAM), Circuito Escolar s/n, Ciudad Universitaria, 04510 Mexico City, Mexico.
Department of Computational Chemistry, J. Heyrovský Institute of Physical Chemistry, The Czech Academy of Sciences, Dolejškova 3, 18223 Prague 8, Czech Republic.
iScience. 2022 Jun 7;25(7):104545. doi: 10.1016/j.isci.2022.104545. eCollection 2022 Jul 15.
In the 1950s, Alan Turing showed that concerted reactions and diffusion of activating and inhibiting chemical species can autonomously generate patterns without previous positional information, thus providing a chemical basis for morphogenesis in Nature. However, access to these patterns from only one molecular component that contained all the necessary information to execute agonistic and antagonistic signaling is so far an elusive goal, since two or more participants with different diffusivities are a must. Here, we report on a single-molecule system that generates Turing patterns arrested in the solid state, where supramolecular interactions are used instead of chemical reactions, whereas diffusional differences arise from heterogeneously populated self-assembled products. We employ a family of hydroxylated organic salphen building blocks based on a bis-Schiff-base scaffold with portions responsible for either activation or inhibition of assemblies at different hierarchies through purely supramolecular reactions, only depending upon the solvent dielectric constant and evaporation as fuel.
20世纪50年代,艾伦·图灵表明,激活和抑制化学物质的协同反应与扩散能够在没有先前位置信息的情况下自主生成图案,从而为自然界中的形态发生提供了化学基础。然而,仅从一个包含执行激动和拮抗信号所需所有必要信息的分子成分中获取这些图案,迄今为止仍是一个难以实现的目标,因为必须有两个或更多具有不同扩散率的参与者。在此,我们报道了一个单分子系统,该系统能产生固态下停滞的图灵图案,其中超分子相互作用取代了化学反应,而扩散差异源于自组装产物的不均匀分布。我们使用了一族基于双席夫碱支架的羟基化有机双水杨醛配体构建块,其不同部分通过纯粹的超分子反应在不同层次上负责组装的激活或抑制,这仅取决于溶剂介电常数和作为驱动力的蒸发过程。