School of Chemistry and Chemical Engineering, Queen's University, Belfast, Northern Ireland, BT9 5AG, UK.
Nat Commun. 2019 Jan 21;10(1):49. doi: 10.1038/s41467-018-07902-7.
Molecular-logic based computation (MLBC) has grown by accumulating many examples of combinational logic gates and a few sequential variants. In spite of many inspirations being available in biology, there are virtually no examples of MLBC in chemistry where sequential and combinational operations are integrated. Here we report a simple alcohol-ketone redox interconversion which switches a macrocycle between a large or small cavity, with erect aromatic walls which create a deep hydrophobic space or with collapsed walls respectively. Small aromatic guests can be captured or released in an all or none manner upon chemical command. During capture, the fluorescence of the alcohol macrocycle is quenched via fluorescent photoinduced electron transfer switching, meaning that its occupancy state is self-indicated. This represents a chemically-driven RS Flip-Flop, one of whose outputs is fed into an INHIBIT gate. Processing of outputs from memory stores is seen in the injection of packaged neurotransmitters into synaptic clefts for onward neural signalling. Overall, capture-release phenomena from discrete supermolecules now have a Boolean basis.
基于分子逻辑的计算 (MLBC) 通过积累许多组合逻辑门和少数顺序变体的例子而发展起来。尽管生物学中有许多灵感,但在化学中实际上没有 MLBC 的例子,其中顺序和组合操作是集成的。在这里,我们报告了一种简单的醇酮氧化还原相互转化,它可以在大环之间切换大或小的空腔,具有直立的芳香壁,分别形成深疏水性空间或塌陷的壁。小的芳香客体可以通过化学指令以全部或无的方式被捕获或释放。在捕获过程中,醇大环的荧光通过荧光光诱导电子转移开关而猝灭,这意味着其占据状态是自我指示的。这代表了一种化学驱动的 RS 触发器,其输出之一被馈入 INHIBIT 门。从离散超分子中进行捕获-释放现象的处理可以在将封装的神经递质注入突触间隙以进行神经信号传递中看到。总的来说,现在离散超分子的捕获-释放现象具有布尔基础。