Single-molecule insights into surface-mediated homochirality in hierarchical peptide assembly

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.

Chirality without Stereoisomers: Insight from the Helical Response of Bond Electrons

“…The existence of chirality has important implications [4][5][6] and the origin of chiral asymmetry [7] in molecular biology is one of the great mysteries in the understanding of the origin of life. [8][9][10][11][12][13][14][15] Recent investigations of structural chirality include those of DNA-stabilized silver clusters with circular dichroism spectra [16] and investigations of interlocked molecules, widely observed in biomacromolecules. [17] In 1848 Louis Pasteur proposed biomolecular homochirality as a possible simple 'chemical signature of life.…”

Towards homochiral supramolecular entities from achiral molecules by vortex mixing-accompanied self-assembly

“…S12†), suggesting an enantiomeric excess of 99.9% or above. These domains are much larger than those homochiral assemblies confirmed by scanning tunneling microscopy (STM) 59,60. It should be noted that the determination of enantiomeric excess and the homochirality by using microscope observation has already been applied for chiral nanofibers and semiconductor helices 59–62.…”

“…These domains are much larger than those homochiral assemblies confirmed by scanning tunneling microscopy (STM). 59 , 60 It should be noted that the determination of enantiomeric excess and the homochirality by using microscope observation has already been applied for chiral nanofibers and semiconductor helices. 59 – 62 Here, combining the high enantiomeric excess evaluated by SEM and the stable yet repeatable CD intensities of the assemblies, we could conclude that a near-unity homochiral assembly was obtained from achiral BTACA molecules through a vortex mixing self-assembly.…”

Control of chirality, bond flexing and anharmonicity in an electric field

“…The existence of chirality has important implications [1][2][3] and the origin of chiral asymmetry [4] in molecular biology is one of the great mysteries in the understanding of the origin of life [5][6][7][8][9][10][11][12]. In 1848 Louis Pasteur proposed biomolecular homochirality as a possible simple "chemical signature of life" [13].…”