Regulative control and enhancement of multi-color upconversion luminescence with DBR cavities

Abstract

Upconversion luminescence (UCL) of lanthanide-doped materials (e.g. NaYF4:Yb3+/Er3+) involves multi-step, multi-channel transitions (corresponding to multi-color emissions) in a multi-level system, and is a low-efficiency nonlinear process. Usually, the UCL is enhanced by local enhancement of the excited field or one of its multi-color emissions is promoted by matching with a resonance cavity mode based on Purcell effect. Here, we propose to regulatively control and enhance the UCL by fostering one color of the UCL emissions with a resonance mode and inhibiting the other with an anti-resonance or nonresonance mode in forbidden band in an optical cavity, so that excited-state ions (e.g. Er3+) transit to the ground state more via the fostered UCL emission channel, rather than the inhibited one. As such, high-contrast single-color UCL emission can be achieved with an enhancement beyond that of Purcell effect. For the purpose, superior mode properties of distributed Bragg reflector (DBR) cavities can be applied, whose forbidden band of the DBR layers and resonance cavity mode in the forbidden band can be independently tuned in positions to match with the UCL emissions for them to be inhibited and fostered respectively. In experimental implementation, multi-color UCL (e.g. red and green) of NaYF4:Yb3+/Er3+ nanoparticles embedded in such DBR cavities are studied. And high-contrast single-color UCL emissions are demonstrated with enhancements factors beyond Purcell factors calculated in numerical simulations. A hypothesis on modifications of intermediate transitions in the UCL processes, as feedbacks to influences of mode characteristics in the DBR cavities for regulative control, is also proposed to explain the phenomena. The work suggests a way to regulatively control multi-channel photon emissions in multi-level systems for enhanced single-channel photon emission.