期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 144, 期 6, 页码 2657-2666出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c11306
关键词
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资金
- National Research Foundation of Korea (NRF) - Korean government (MSIT) [2018R1A5A1025208]
- Institute for Basic Science in Korea [IBS-R010-D1]
- [NRF-2016R1A5A1009405]
The study shows that circularly polarized light can induce chirality at the supramolecular level, and the chirality information can be nonlinearly amplified in the system. Opposite chirality can override molecular information when the enantiomeric excess is low.
Circularly polarized light (CPL) is an inherently chiral entity and is considered one of the possible deterministic signals that led to the evolution of homochirality. While accumulating examples indicate that chirality beyond the molecular level can be induced by CPL, not much is yet known about circumstances where the spin angular momentum of light competes with existing molecular chiral information during the chirality induction and amplification processes. Here we present a light-triggered supramolecular polymerization system where chiral information can both be transmitted and nonlinearly amplified in a sergeants-and-soldiers manner. While matching handedness with CPL resulted in further amplification, we determined that opposite handedness could override molecular information at the supramolecular level when the enantiomeric excess was low. The presence of a critical chiral bias suggests a bifurcation point in the homochirality evolution under random external chiral perturbation. Our results also highlight opportunities for the orthogonal control of supramolecular chirality decoupled from molecular chirality preexisting in the system.
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