Upconverted excitation energy lock-in for deep-ultraviolet enhancement

Abstract Photon upconversion of near-infrared (NIR) irradiation into deep-ultraviolet (UV) emission offers many exciting opportunities for drug release in deep tissues, photodynamic therapy, solid-state lasing, energy storage, and photocatalysis. However, NIR-to-deep-UV upconversion remains a daunting challenge due to low quantum efficiency. Here, we report an unusual six-photon upconversion process in Gd3+/Tm3+-codoped nanoparticles comprising a heterogeneous, core-multishell nanostructure. This multishell design efficiently suppresses energy consumption induced by interior energy traps, maximizes cascade sensitizations of the NIR excitation, and promotes upconverted deep-UV emission from high-lying excited states. We released the intense six-photon-upconverted UV emissions at 253 nm under 808-nm excitation. This work provides new insight into mechanistic understanding of the upconversion process within the heterogeneous architecture, while offering exciting opportunities for developing nanoscale deep-UV emitters that can be remotely controlled in deep tissues upon NIR illumination.