Abstract
Deciphering the complicated excited-state process is critical for the development of luminescent materials with controllable emissions in different applications. Here we report the emergence of a photo-induced structural distortion accompanied by an electron redistribution in a series of gold nanoclusters. Such unexpected slow process of excited-state transformation results in near-infrared dual emission with extended photoluminescent lifetime. We demonstrate that this dual emission exhibits highly sensitive and ratiometric response to solvent polarity, viscosity, temperature and pressure. Thus, a versatile luminescent nano-sensor for multiple environmental parameters is developed based on this strategy. Furthermore, we fully unravel the atomic-scale structural origin of this unexpected excited-state transformation, and demonstrate control over the transition dynamics by tailoring the bi-tetrahedral core structures of gold nanoclusters. Overall, this work provides a substantial advance in the excited-state physical chemistry of luminescent nanoclusters and a general strategy for the rational design of next-generation nano-probes, sensors and switches.
Highlights
Deciphering the complicated excited-state process is critical for the development of luminescent materials with controllable emissions in different applications
We directly identify a significant structural distortion accompanied by an electron redistribution in three photoexcited atomically precise nanoclusters (Au24(S-TBBM)2030, Au14Cd1(SAdm)1231, and Au24(S-PET)2032, where S-TBBM = 4-tertbutylphenylmethancan, S-Adm = 1-adamantanethiol, and S-PET = 2-phenylethanethiol) using a combination of different spectroscopic techniques
As the atomic structures of Au nanoclusters have been totally solved by the single-crystal X-ray diffraction (XRD)[18,30,31], the atomic-scale structural origin of such excitedstate transformation can be fully unraveled
Summary
Deciphering the complicated excited-state process is critical for the development of luminescent materials with controllable emissions in different applications. We report the emergence of a photo-induced structural distortion accompanied by an electron redistribution in a series of gold nanoclusters Such unexpected slow process of excited-state transformation results in near-infrared dual emission with extended photoluminescent lifetime. This interesting phenomenon has endowed some organic molecules and metal complexes with two drastically different states, which are appealing for applications in sensing, probes, switches, and actuators[1,2,3,4,5,6,7,8,9,10,11,12,13,14,15,16,17] This combined excited-state process has not yet been identified in nanomaterials, which is probably because of the increased structural rigidity and enhanced electron delocalization as materials transition from the molecular scale to the nanoscale. This is the first time, to the best of our knowledge, that such a direct transfer event has been reported in metal nanoclusters
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