Chemical Science Symposium 2022

Insights into the enzyme induced spatiotemporal dynamics of self assembled motifs Priyanka, Ekta Shandilya, Surinder Kaur Brar, Rishi Ram Mahat, Subhabrata Maiti IISER Mohali, India Biological functions typically involve a series of interlinked temporal events having specific spatial coordination among the interacting components so that the temporal events occur at specific locations or among specific compartments in the organism. Thus, continued efforts towards development of programmable matter on both temporal and spatial scales would be vital to creating biomimetic, dissipative materials with controllable functionality. Until now, reports of spatiotemporal surface pattern or self-organization have been restricted by oscillatory reaction-diffusion processes. Also, the self-organization of synthetic systems under dissipative conditions or under agonistic-antagonistic relationships among multiple components has been limited in mostly solution-phase materialistic studies. Herein, we have shown how the later approach can be used to generate template-driven self-organization at a specific location of a two-dimensional (2D) space in a temporal manner. In particular, we have used two enzymes, namely alkaline phosphatase (ALP) and hexokinase (HK) to show that it is possible to dissipate or sustain an ATP-driven assembly of a surfactant having dipicolylamine (DPA)•Zn2+ as the headgroup. Furthermore, we have borrowed this approach to create spatiotemporally distinct patterns of organized assemblies when surfactant and enzymes (ALP or HK) are operating in gradients from different locations, where the template has been distributed uniformly through the entire space. We have used both theory (DFT for studying the molecular interactions, thermodynamic binding parameters etc.; Python for numerical modeling and MATLAB for diffusion-dependent spatiotemporal assembly) and experiments to complement our findings. Overall, in this work, we have shown an elegant approach for the development of the spatiotemporally flexible surface pattern of organized assemblies by using both theory and experiment, and simultaneously it also showed a new route in gaining ‘spatial’ adaptability in a self-organized system with interacting components for the incorporation of programmed functionality. References 1. Priyanka; Shandilya, E.; Brar, S. K.; Mahato, R. R.; Maiti, S. Spatiotemporal Dynamics of Self-Assembled Structures in Enzymatically Induced Agonistic and Antagonistic Conditions. Chem. Sci. 2022, 13 (1), 274–282. https://doi.org/10.1039/ d1sc05353a.

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