A novel high-sensitive upconversion thermometry strategy: Utilizing synergistic effect of dual-wavelength lasers excitation to manipulate electron thermal distribution

摘要

Conventional upconversion thermometry strategy, based on the thermally coupled levels (TCL) of lanthanide ions, confronts a dilemma in simultaneously achieving high absolute/relative temperature (T) sensitivities (S-a and S-r) and good signal discriminability. Herein, a novel thermometry strategy by utilizing the synergistic effect of dual-wavelength lasers to manipulate electron thermal distribution is proposed to go beyond the limitation of the TCL-based strategy. In the case of NaGdF4: 20%Yb3+, 2%Er3+ nanoparticles upon 980 & 1530 nm dual-excitation, it is found that more efficient utilization of excited photons results in a higher electron concentration in ladder-like energy levels of Er3+, owing to the diverse pumping routes, which increases transition rate of the T-dependent phonon-assisted cross-relaxation process, and in turn establishes a thermally-sensitive electronic connection between Er3+: H-2(11/2),S-4(3/2) and Er3+: F-4(9/2). Remarkably, not only a highest record value of S-a (0.0365 K-1) for the Er3+ doped host materials in the physiological temperature range (303-343 K) is achieved, but also a high S-r (1.29% K-1) and an excellent signal discriminability (Delta lambda = 112 nm) are obtained. Combining a much intensified upconversion (UC) signal and a good size/shape homogeneity in nanometer scale, the investigated NaGdF4: 20%Yb3+, 2%Er3+ upon dual-wavelength excitation is potentially applicable in the intracellular thermal sensing and imaging. This work exploits an effective way to develop high-performance T-sensors, and the proposed thermometry strategy can be extended to surges of the other lanthanide ions doped systems pumped by multiple-wavelength lasers.