Origin of the high upconversion green luminescence efficiency in ���-NaYF4:2% Er3+,20% Yb3+

Site-selective spectroscopy in hexagonal beta-NaYF4:Er3+,Yb3+ has revealed different environments for Er3+ ions (multisite formation). The low-temperature S-4(3/2) -> (I15/2Er3+)-I-4 green emission depends on the excitation wavelength associated with the F-4(7/2) Er3+ level. We have studied the effect of hydrostatic pressure on the green, red, and blue Er3+ emission upon NIR excitation at similar to 980 nm, in order to establish the role played by energy resonance conditions and the multiple Er3+ sites due to the disordered structure for the upconversion (UC) process (energy tuning). The variation of photoluminescence spectra and lifetimes as a function of pressure and temperature reveals that the origin of the high green UC efficiency of the beta-NaYF4:Er3+,Yb3+ compound is mainly due to the multisite distribution, and the low phonon energy of the host lattice.

Relation between Excitation Power Density and Er3+ Doping Yielding the Highest Absolute Upconversion Quantum Yield

The upconversion quantum yield (UCQY) is one of the most significant parameters for upconverter materials. A high UCQY is essential for a succesful integration of upconversion in many applications, such as harvesting of the solar radiation. However, little is known about which doping level of the rare-earth ions yields the highest UCQY in the different host lattices and what are the underlying causes. Here, we investigate which Er3+ doping yields the highest UCQY in the host lattices ��-NaYF4 and Gd2O2S under 4I15/2 ��� 4I13/2 excitation. We show for both host lattices that the optimum Er3+ doping is not fixed and it actually decreases as the irradiance of the excitation increases. To find the optimum Er3+ doping for a given irradiance, we determined the peak position of the internal UCQY as a function of the average Er���Er distance. For this purpose, we used a fit on experimental data, where the average Er���Er distance was calculated from the Er3+ doping of the upconverter samples and the lattice parameters of the host materials. We observe optimum average Er���Er distances for the host lattices ��-NaYF4 and Gd2O2S with differences <14% at the same irradiance levels, whereas the optimum Er3+ doping are around 2�� higher for ��-NaYF4 than for Gd2O2S. Estimations by extrapolation to higher irradiances indicate that the optimum average Er���Er distance converges to values around 0.88 and 0.83 nm for ��-NaYF4 and Gd2O2S, respectively. Our findings point to a fundamental relationship and focusing on the average distance between the active rare-earth ions might be a very efficient way to optimize the doping of rare-earth ions with regard to the highest achievable UCQY.