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Direct Flipping Dynamics and Quantized Enrichment of Chirality at Single-molecule Resolution

Overview
Journal Sci Adv
Specialties Biology
Science
Date 2024 Jul 12
PMID 38996014
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Abstract

Chirality is an important aspect of nature, and numerous macroscopic methods have been developed to understand and control chirality. For the chiral tertiary amines, their flexible flipping process makes it possible to achieve high chiral controllability without bond formation and breaking. Here, we present a type of stable chiral single-molecule devices formed by tertiary amines, using graphene-molecule-graphene single-molecule junctions. These single-molecule devices allow real-time, in situ, and long-time measurements of the flipping process of an individual chiral nitrogen center with high temporal resolution. Temperature- and bias voltage-dependent experiments, along with theoretical investigations, revealed diverse chiral intermediates, indicating the regulation of the flipping dynamics by energy-related factors. Angle-dependent measurements further demonstrated efficient enrichment of chiral states using linearly polarized light by a symmetry-related factor. This approach offers a reliable means for understanding the chirality's origin, elucidating microscopic chirality regulation mechanisms, and aiding in the design of effective drugs.

References
1.
Huang Y, Walji A, Larsen C, MacMillan D . Enantioselective organo-cascade catalysis. J Am Chem Soc. 2005; 127(43):15051-3. DOI: 10.1021/ja055545d. View

2.
MASON S . Origins of biomolecular handedness. Nature. 1984; 311(5981):19-23. DOI: 10.1038/311019a0. View

3.
Jia C, Ma B, Xin N, Guo X . Carbon Electrode-Molecule Junctions: A Reliable Platform for Molecular Electronics. Acc Chem Res. 2015; 48(9):2565-75. DOI: 10.1021/acs.accounts.5b00133. View

4.
Neugebauer M, Banzer P, Nechayev S . Emission of circularly polarized light by a linear dipole. Sci Adv. 2019; 5(6):eaav7588. PMC: 6598770. DOI: 10.1126/sciadv.aav7588. View

5.
Jia C, Migliore A, Xin N, Huang S, Wang J, Yang Q . Covalently bonded single-molecule junctions with stable and reversible photoswitched conductivity. Science. 2016; 352(6292):1443-5. DOI: 10.1126/science.aaf6298. View