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Fluorescence umpolung enables light-up sensing of N-acetyltransferases and nerve agents.

Chenxu YanZhi-Qian GuoWeijie ChiWei FuSyed Ali Abbas AbediXiaogang LiuHe TianWei-Hong Zhu
Published in: Nature communications (2021)
Intramolecular charge transfer (ICT) is a fundamental mechanism that enables the development of numerous fluorophores and probes for bioimaging and sensing. However, the electron-withdrawing targets (EWTs)-induced fluorescence quenching is a long-standing and unsolved issue in ICT fluorophores, and significantly limits the widespread applicability. Here we report a simple and generalizable structural-modification for completely overturning the intramolecular rotation driving energy, and thus fully reversing the ICT fluorophores' quenching mode into light-up mode. Specifically, the insertion of an indazole unit into ICT scaffold can fully amplify the intramolecular rotation in donor-indazole-π-acceptor fluorophores (fluorescence OFF), whereas efficiently suppressing the rotation in their EWT-substituted system (fluorescence ON). This molecular strategy is generalizable, yielding a palette of chromophores with fluorescence umpolung that spans visible and near-infrared range. This strategy expands the bio-analytical toolboxes and allows exploiting ICT fluorophores for light-up sensing of EWTs including N-acetyltransferases and nerve agents.
Keyphrases
  • energy transfer
  • quantum dots
  • single molecule
  • living cells
  • small molecule
  • signaling pathway
  • high glucose
  • drug induced
  • molecular dynamics simulations
  • stress induced
  • electron transfer