Advanced nanoscale synthetic techniques provide a versatile platform for programmable control over the size, morphology, and composition of nanocrystals doped with lanthanide ions. Characteristic upconversion luminescence features originating from the 4f–4f optical transitions of lanthanides can be achieved through predesigned energy transfer pathways, enabling wide applications ranging from ultrasensitive biological detection to advanced spectroscopic instrumentation with high spatiotemporal resolution. Here, we review recent scientific and technological discoveries that have prompted the realization of these peculiar functions of lanthanide-doped upconversion nanocrystals and discuss the mechanistic studies of energy transfer involved in upconversion processes. These advanced schemes include cross relaxation-mediated depletion, multipulse sequential pumping, and nanostructural configuration design. Our emphasis is placed on disruptive technologies such as super-resolution microscopy, optogenetics, nanolasing, and optical anticounterfeiting, which take full advantage of the upconversion nanophenomena in relation to lanthanide-doped nanocrystals.
Achieving efficient photon upconversion under low irradiance is not only a fundamental challenge but also central to numerous advanced applications spanning from photovoltaics to biophotonics. However, to date, almost all approaches for upconversion luminescence intensification require stringent controls over numerous factors such as composition and size of nanophosphors. Here, we report the utilization of dielectric microbeads to significantly enhance the photon upconversion processes in lanthanide-doped nanocrystals. By modulating the wavefront of both excitation and emission fields through dielectric superlensing effects, luminescence amplification up to 5 orders of magnitude can be achieved. This design delineates a general strategy to converge a low-power incident light beam into a photonic hotspot of high field intensity, while simultaneously enabling collimation of highly divergent emission for far-field accumulation. The dielectric superlensing-mediated strategy may provide a major step forward in facilitating photon upconversion processes toward practical applications in the fields of photobiology, energy conversion, and optogenetics.
Graphene–Si Schottky junction solar cells are promising candidates for high-efficiency, low-cost photovoltaic applications. However, their performance enhancement is restricted by strong carrier recombination and relative low barrier height. Here, we demonstrated the successful construction of high-efficiency graphene–planar Si solar cells via modification of the Si surface with a molecule monolayer as well as tuning the interface band alignment with an organic electron blocking layer. Methylated Si showed the capability to effectively suppress the surface carrier recombination, leading to a remarkable improvement of device efficiency. The recombination was further reduced by inserting a thin P3HT organic layer; the unique band alignment could prevent electron transfer from n-Si to the graphene anode so as to minimize the current leakage. These methods, along with careful control of the graphene doping level and layer number, gave rise to a power conversion efficiency (PCE) as high as 10.56%. The scalability of the devices was further investigated by studying the device area dependent photovoltaic performance.