Journal
ADVANCED SCIENCE
Volume 8, Issue 6, Pages -Publisher
WILEY
DOI: 10.1002/advs.202003325
Keywords
lanthanide nanocrystals; luminescence; quenching; ytterbium ions
Categories
Funding
- ARC Discovery Early Career Researcher Award Scheme [DE180100669]
- Science and Technology Innovation Commission of Shenzhen [KQTD20170810110913065]
- Australia-China Joint Research Centre for Point-of-Care Testing [ACSRF65827, SQ2017YFGH001190]
- National Natural Science Foundation of China [21590791, 21771005, 21931001, 21425101]
- Ministry of Science and Technology (MOST) of China [2017YFA0205101, 2017YFA0205104]
- China Scholarship Council Scholarships [201706010060]
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This study reveals the formation of an energy-migration network by highly doping Yb3+ ions within the nanocrystal host, and the distinct behavior of Yb3+ in the networking state. The reversible effect of Yb-O coordination on luminescent properties of nanocrystals is demonstrated, providing important insights for the application and manipulation of nanomaterials.
At the organic-inorganic interface of nanocrystals, electron-phonon coupling plays an important but intricate role in determining the diverse properties of nanomaterials. Here, it is reported that highly doping of Yb3+ ions within the nanocrystal host can form an energy-migration network. The networking state Yb3+ shows both distinct Stark splitting peak ratios and lifetime dynamics, which allows quantitative investigations of quenching and thermal activation of luminescence, as the high-dimensional spectroscopy signatures can be correlated to the attaching and de-attaching status of surface molecules. By in-situ surface characterizations, it is proved that the Yb-O coordination associated with coordinated water molecules has significantly contributed to this reversible effect. Moreover, using this approach, the prime quencher -OH can be switched to -CH in the wet-chemistry annealing process, resulting in the electron-phonon coupling probability change. This study provides the molecular level insights and dynamics of the surface dark layer of luminescent nanocrystals.
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