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This study reveals how pressure enhances near-infrared (NIR) luminescence in gold nanoclusters by controlling structural distortion. One nanocluster ([Au11]-1) achieved a record 75.6% NIR photoluminescence quantum yield (PLQY) under pressure.

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Area of Science:

  • Materials Science
  • Nanotechnology
  • Solid-State Physics

Background:

  • Achieving efficient near-infrared (NIR) luminescence in atomically precise gold nanoclusters is hindered by the gold core's vibrational freedom.
  • Existing methods struggle to overcome intrinsic limitations in photoluminescence quantum yield (PLQY) for solid-state gold nanoclusters.

Purpose of the Study:

  • To investigate the piezoluminescence behavior of two synthesized gold nanoclusters, [Au11](PPh3)8Cl2]Cl (Au11-1) and Au11(PPh3)7Cl3 (Au11-2), under hydrostatic pressure.
  • To elucidate the structure-property relationships governing NIR luminescence enhancement in gold nanoclusters under pressure.

Main Methods:

  • Synthesis of two distinct gold nanoclusters, Au11-1 and Au11-2.
  • Systematic investigation of NIR piezoluminescence under hydrostatic pressure.
  • In situ high-pressure angle-dispersive X-ray diffraction, theoretical calculations, femtosecond transient absorption, and Raman spectroscopy.

Main Results:

  • Au11-1 demonstrated a remarkable increase in NIR-PLQY from 0.3% to 75.6% at 3.6 GPa, the highest reported for solid-state gold nanoclusters.
  • Au11-2 exhibited monotonic luminescence quenching under compression.
  • Distinct anisotropic compressions and differential structural distortions of the gold core were observed in Au11-1 and Au11-2, correlating with luminescence changes.

Conclusions:

  • Pressure-induced directional structural distortion in Au11-1 suppresses nonradiative losses from low-frequency vibrations, leading to significant NIR piezoluminescence enhancement.
  • The study establishes a clear correlation between NIR-PLQY and metal core vibration relaxation at the atomic scale.
  • Provides a novel strategy for designing high-performance NIR luminescent materials through controlled structural distortion.