Abstract

Homochirality is very important in the formation of advanced biological structures, but the origin and evolution mechanisms of homochiral biological structures in complex hierarchical process is not clear at the single-molecule level. Here we demonstrate the single-molecule investigation of biological homochirality in the hierarchical peptide assembly, regarding symmetry break, chirality amplification, and chirality transmission. We find that homochirality can be triggered by the chirality unbalance of two adsorption configuration monomers. Co-assembly between these two adsorption configuration monomers is very critical for the formation of homochiral assemblies. The site-specific recognition is responsible for the subsequent homochirality amplification and transmission in their hierarchical assembly. These single-molecule insights open up inspired thoughts for understanding biological homochirality and have general implications for designing and fabricating artificial biomimetic hierarchical chiral materials.

Highlights

  • Homochirality is very important in the formation of advanced biological structures, but the origin and evolution mechanisms of homochiral biological structures in complex hierarchical process is not clear at the single-molecule level

  • Scanning tunneling microscopy (STM) combined with density functional theory (DFT) calculations reveal that two kinds of chiral adsorption configuration monomers with unequal amount coexist on the surface

  • STM observation (Fig. 1b) confirmed that two kinds of adsorption configurations coexist on the Cu(111) surface when valinomycin molecules were deposited on the Cu(111) surface at 78 K

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Summary

Introduction

Homochirality is very important in the formation of advanced biological structures, but the origin and evolution mechanisms of homochiral biological structures in complex hierarchical process is not clear at the single-molecule level. We investigate the surface-mediated homochirality evolution process in the hierarchical assembly of valinomycin from single-molecule to supramolecular level. STM combined with density functional theory (DFT) calculations reveal that two kinds of chiral adsorption configuration monomers with unequal amount coexist on the surface.

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