4.8 Article

Chirality transfer from a 3D macro shape to the molecular level by controlling asymmetric secondary flows

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NATURE COMMUNICATIONS
卷 13, 期 1, 页码 -

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NATURE PORTFOLIO
DOI: 10.1038/s41467-022-29425-y

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资金

  1. European Research Council Starting Grant microCrysFact (ERC-2015-STG) [677020]
  2. Swiss National Science Foundation [200021_181988]
  3. MCIN/AEI [PID2020-116612RB-C33]
  4. EU, from the Horizon 2020 FETOPEN project SPRINT [801464]
  5. Swiss National Science Foundation (SNF) [200021_181988] Funding Source: Swiss National Science Foundation (SNF)

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This article presents an example of chirality transfer from the chiral shape of a 3D helical channel to chiral supramolecular aggregates, where the handedness of the helical channel determines the direction of enantioselection. By combining numerical simulations and experimental data, the authors demonstrate the possibility of controlling enantioselectively molecular processes at the nanometer scale by modulating the geometry and operating conditions of fluidic reactors.
Homochirality is a fundamental feature of living systems, and its origin is still an unsolved mystery. Previous investigations showed that external physical forces can bias a spontaneous symmetry breaking process towards deterministic enantioselection. But can the macroscopic shape of a reactor play a role in chiral symmetry breaking processes? Here we show an example of chirality transfer from the chiral shape of a 3D helical channel to the chirality of supramolecular aggregates, with the handedness of the helical channel dictating the direction of enantioselection in the assembly of an achiral molecule. By combining numerical simulations of fluid flow and mass transport with experimental data, we demonstrated that the chiral information is transferred top-down thanks to the interplay between the hydrodynamics of asymmetric secondary flows and the precise spatiotemporal control of reagent concentration fronts. This result shows the possibility of controlling enantioselectively molecular processes at the nanometer scale by modulating the geometry and the operating conditions of fluidic reactors. External physical forces can bias a spontaneous symmetry breaking process but whether the shape of a reactor plays a role in chiral symmetry breaking processes is an open question. Here, the authors demonstrate chirality transfer from the chiral shape of a 3D helical channel to chiral supramolecular aggregates whereby the handedness of the helical channel dictates the direction of enantioselection.

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