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Anomalous fluorescence in aqueous solutions is linked to charge-transfer-to-solvent excitations (CTTS). Solutes can prolong CTTS excited state lifetimes, enhancing fluorescence emission.

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Area of Science:

  • Physical Chemistry
  • Spectroscopy
  • Computational Chemistry

Background:

  • Anomalous fluorescence emissions from aqueous solutions of nonaromatic solutes have been reported.
  • The underlying mechanism and the influence of solute nature remain unclear.

Purpose of the Study:

  • To investigate the origin of anomalous fluorescence in aqueous solutions.
  • To determine if solute nature influences fluorescence characteristics.
  • To identify a common emission mechanism.

Main Methods:

  • Measured fluorescence spectra of 21 different aqueous solutions.
  • Employed time-dependent density functional theory (TD-DFT) on large water, NaCl/water, and glycerol/water clusters.

Main Results:

  • Observed similar emission characteristics across diverse solutes, indicating minimal solute influence.
  • Attributed anomalous emission to charge-transfer-to-solvent (CTTS) excitations.
  • Identified a diradical zwitterionic excited state at hydrogen-bond network defects.

Conclusions:

  • The S1 nonradiative decay pathway involves diradical recombination via librational motion.
  • Solute molecules appear to slow this recombination, increasing CTTS excited state lifetime and facilitating emission.
  • A common mechanism for anomalous fluorescence in aqueous solutions is proposed.