4.8 Article

Caged structural water molecules emit tunable brighter colors by topological excitation

Journal

NANOSCALE
Volume 13, Issue 35, Pages 15058-15066

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1nr02389f

Keywords

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Funding

  1. NSFC [21872053, 21573074, 22172051]
  2. Science and Technology Commission of Shanghai Municipality [19520711400]
  3. Open Project Program of Academician and Expert Workstation
  4. JORISS program
  5. Postdoctoral Science Foundation of China [2018M640360]
  6. Shanghai Curui Low-Carbon Energy Technology Co., Ltd.

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The research found that structurally bound water molecules exhibit strong tunable photoluminescence, ultra-long lifetimes, and characteristics dependent on H-bond interactions in confined nanocavities. This emission behavior is due to topological excitations resulting from many-body quantum electron correlations in confined nanocavities, differing from local excitation of organic chromophores.
Intrinsically, free water molecules are a colourless liquid. If it is colourful, why and how does it emit the bright colours? We provided direct evidence that when water was trapped into the sub-nanospace of zeolites, the structural water molecules (SWs) exhibited strong tunable photoluminescence (PL) emissions from blue to red colours with unprecedented ultra-long lifetimes up to the second scale at liquid nitrogen temperature. Further controlled experiments and combined characterizations by time-resolved steady-state and ultra-fast femtosecond (fs) transient optical spectroscopy showed that the singly adsorbed hydrated hydroxide complex {OH-center dot H2O} as SWs in the confined nanocavity is the true emitter centre, whose PL efficiency strongly depends on the type and stability of the SWs, which is dominated by H-bond interactions, such as the solvent effect, pH value and operating temperature. The emission of SWs exhibits the characteristic of topological excitations (TAs) due to the many-body quantum electron correlations in confined nanocavities, which differs from the local excitation of organic chromophores. Our model not only elucidates the origin of the PL of metal nanoclusters (NCs), but also provides a completely new insight to understand the nature of heterogeneous catalysis and interface bonding (or state) at the molecule level, beyond the metal-centred d band theory.

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