American Chemical Society
nl1c00232_si_001.pdf (1.45 MB)

Multiphoton Upconversion Enhanced by Deep Subwavelength Near-Field Confinement

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journal contribution
posted on 2021-03-09, 15:37 authored by Jiahui Xu, Zhaogang Dong, Mohamed Asbahi, Yiming Wu, Hao Wang, Liangliang Liang, Ray Jia Hong Ng, Hailong Liu, Renaud A. L. Vallée, Joel K. W. Yang, Xiaogang Liu
Efficient generation of anti-Stokes emission within nanometric volumes enables the design of ultracompact, miniaturized photonic devices for a host of applications. Many subwavelength crystals, such as metal nanoparticles and two-dimensional layered semiconductors, have been coupled with plasmonic nanostructures for augmented anti-Stokes luminescence through multiple-harmonic generation. However, their upconversion process remains inefficient due to their intrinsic low absorption coefficients. Here, we demonstrate on-chip, site-specific integration of lanthanide-activated nanocrystals within gold nanotrenches of sub-25 nm gaps via bottom-up self-assembly. Coupling of upconversion nanoparticles to subwavelength gap-plasmon modes boosts 3.7-fold spontaneous emission rates and enhances upconversion by a factor of 100 000. Numerical investigations reveal that the gap-mode nanocavity confines incident excitation radiation into nanometric photonic hotspots with extremely high field intensity, accelerating multiphoton upconversion processes. The ability to design lateral gap-plasmon modes for enhanced frequency conversion may hold the potential to develop on-chip, background-free molecular sensors and low-threshold upconversion lasers.