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Plasmon resonances in metallic nanoparticles result in enhanced light absorption and hot carrier generation. Although hot carriers are short-lived, their energy can be extracted in optical form resulting in photon upconversion. Two low energy photons absorbed by a plasmonic nanostructure, create a hot electron and a hot hole. These hot carriers get injected into an adjacent semiconductor quantum well where they radiatively recombine to emit a higher energy photon resulting in photon upconversion. This process involves injection of an electron and a hole across the same interface making it charge neutral. The upconversion emission has a linear dependence on the incident light intensity, making it promising for applications requiring low power operation. Theoretical studies show that a silver/semiconductor system can have an ideal efficiency of 25%.
Our experimental demonstration of this new scheme utilizes GaN/InGaN quantum wells decorated with both silver and gold. The use of two metals reduces band-bending in the semiconductor. Illuminating the sample with light spanning wavelengths of 500-540 nm produces upconversion photoluminescence centered at 435 nm. Control samples including undecorated quantum wells and metal nanostructures on a glass substrate do not show any upconversion ruling out possibilities of upconversion in individual materials. Further, the linear dependence of the upconverted light intensity with incident intensity rules out any non-linear or Auger mediated mechanisms. We will describe how this hot carrier upconversion process promises to be broadband, tunable, and more efficient than existing solid-state upconversion schemes, and discuss potential applications in solar energy, security, and photodetection applications.
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