Abstract
Manipulating particle size is a powerful means of creating unprecedented optical properties in metals and semiconductors. Here we report an insulator system composed of NaYbF4:Tm in which size effect can be harnessed to enhance multiphoton upconversion. Our mechanistic investigations suggest that the phenomenon stems from spatial confinement of energy migration in nanosized structures. We show that confining energy migration constitutes a general and versatile strategy to manipulating multiphoton upconversion, demonstrating an efficient five-photon upconversion emission of Tm3+ in a stoichiometric Yb lattice without suffering from concentration quenching. The high emission intensity is unambiguously substantiated by realizing room-temperature lasing emission at around 311 nm after 980-nm pumping, recording an optical gain two orders of magnitude larger than that of a conventional Yb/Tm-based system operating at 650 nm. Our findings thus highlight the viability of realizing diode-pumped lasing in deep ultraviolet regime for various practical applications.
Highlights
Manipulating particle size is a powerful means of creating unprecedented optical properties in metals and semiconductors
The size effect is largely unexplored in lanthanide-doped upconversion nanoparticles, which represents an important family of optical materials characterized by large anti-Stokes shift, narrow emission bandwidths and long excited-state lifetimes
We describe an investigation of energy migration in a nanosized NaYbF4 lattice
Summary
Manipulating particle size is a powerful means of creating unprecedented optical properties in metals and semiconductors. We show that confining energy migration constitutes a general and versatile strategy to manipulating multiphoton upconversion, demonstrating an efficient five-photon upconversion emission of Tm3 þ in a stoichiometric Yb lattice without suffering from concentration quenching. The size effect is largely unexplored in lanthanide-doped upconversion nanoparticles, which represents an important family of optical materials characterized by large anti-Stokes shift, narrow emission bandwidths and long excited-state lifetimes. A high lanthanide content enhances energy migration through the crystal lattice, which usually leads to a depletion of the excitation energy[24,28]. Our mechanistic investigation reveals a spatial confinement of energy migration that prevents energy loss to the crystal lattice and increases the local density of excitation energy. We show that the technological advancement may revolutionize the fabrication of cost effective and compact diode-pumped solid-state deep ultraviolet lasers that are useful for environmental, life science and industrial applications[29]
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