Excited-state dynamics and sequential two-photon upconversion excitation of Mo3+-doped chloro- and bromo-elpasolites

The photophysical properties of Mo3+-doped chloro- and bromo-elpasolites at 10 K and as a function of temperature are presented. Visible upconverted l uminescence is observed with near-infrared laser excitation, and the proper ties of this two-photon excitation process are experimentally characterized by a variety of luminescence and time-dependent measurements. Three upconv ersion mechanisms an active in these Mo3+-doped materials. Two involve the sequential absorption of two near-infrared photons of the same color, and a third involves the sequential absorption of two near-infrared photons of d ifferent colors. The two one-color upconversion mechanisms are distinguisha ble on the basis of time dependence measurements and simulations. Of the th ree mechanisms, the two-color sequential two-photon absorption process is f ound to be more efficient than the corresponding one-color mechanism by a f actor of >10(2), and this is related to the relatively small effective spin -orbit coupling magnitude in this ion. These excited-state processes are as sisted by an extremely long 10 K E-2 lifetime of 67.5 ms in 2.5% Mo3+:Cs2Na YCl6, and 48.5 ms in 2.5% Mo3+:Cs2NaYBr6. The upconversion properties of Mo 3+ presented here reflect the rich photophysics of this ion, and represent a significant new addition to the emerging area of transition-metal upconve rsion.