Long-term thermal quenching of upconversion (UC) limits
the usage
of UC materials in nanothermometers, lighting phosphors, etc. Although UC thermal enhancement has been achieved through thermal
alleviation of surface quenching, the regulation of the balance between
internal multiphonon nonradiative relaxation-induced thermal quenching
and external surface quencher release-induced thermal enhancement
is still a big challenge. Here, we demonstrate a new strategy to achieve
huge UC thermal enhancement by constructing surface-dominant quasi-2D
KLu2F7:20%Yb3+/2%Er3+@KLu2F7 core–shell nanoflakes with an ultrathin
thickness of 1.5 nm. The surface-dominant design enables enhancements
of ∼820-fold at the 523 nm band and ∼304-fold in total
as the temperature increases from 303 to 463 K. Similar huge UC thermal
enhancements are also observed in Ho3+ (∼383-fold)-
and Tm3+ (∼324-fold)-doped nanoflakes. Higher relative
and absolute sensitivities of the thermally coupled state pairs (Er3+:2H11/2/4S3/2) with respective plateau values of 0.940% K–1 (303
K) and 0.509% K–1 (463 K) are achieved, which obviously
outperform the thermal-quenching NaYF4:20%Yb3+/2%Er3+@NaYF4 nanoparticles. Moreover, the
highly thermally enhanced nanoflakes enable the development of temperature-dependent
anticounterfeiting inks and encryption, favoring the high-temperature
usage of luminescence materials.