Abstract

Fluoride-based compounds doped with rare-earth cations are the preferred choice of materials to achieve efficient upconversion, of interest for a plethora of applications ranging from bioimaging to energy harvesting. Herein, we demonstrate a simple route to fabricate bright upconverting films that are transparent, self-standing, flexible, and emit different colors. Starting from the solvothermal synthesis of uniform and colloidally stable yttrium fluoride nanoparticles doped with Yb3+ and Er3+, Ho3+, or Tm3+, we find the experimental conditions to process the nanophosphors as optical quality films of controlled thickness between few hundreds of nanometers and several micrometers. A thorough analysis of both structural and photophysical properties of films annealed at different temperatures reveals a tradeoff between the oxidation of the matrix, which transitions through an oxyfluoride crystal phase, and the efficiency of the upconversion photoluminescence process. It represents a significant step forward in the understanding of the fundamental properties of upconverting materials and can be leveraged for the optimization of upconversion systems in general. We prove bright multicolor upconversion photoluminescence in oxyfluoride-based phosphor transparent films upon excitation with a 980 nm laser for both rigid and flexible versions of the layers, being possible to use the latter to coat surfaces of arbitrary shape. Our results pave the way toward the development of upconverting coatings that can be conveniently integrated in applications that demand a large degree of versatility.

Highlights

  • Upconversion (UC) photoluminescence is a nonlinear optical phenomenon by which a material emits light at higher frequency than the one used for excitation, typically in the near-infrared (NIR)

  • We report a simple method to develop nanophosphor pastes to fabricate optical quality films of controlled thickness from YF3:Yb3+,X3+ (X = Er, Ho, or Tm) nanoparticles synthesized at low temperature, following a solvothermal route

  • UC photoluminescence (UCPL) spectra of (Yb3+, Er3+)-doped nanophosphor films with a thickness of ∼15 μm annealed at temperatures ranging from 400 °C to 550 °C for 6 h are shown in Figure 2a. 980 nm laser light is absorbed by the Yb3+ ions and energy is transferred between 2F5/2 and 4I11/2 levels of Yb3+ and Er3+, respectively

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Summary

Introduction

Upconversion (UC) photoluminescence is a nonlinear optical phenomenon by which a material emits light at higher frequency than the one used for excitation, typically in the near-infrared (NIR). This way, nonvisible light is converted into the visible region of the electromagnetic spectrum.[1−4]. This phenomenon is of great interest for a wide variety of research fields, including bioimaging,[5−7] optogenetics,[8] superresolution microscopy,[4,9] light guiding,[10] light harvesting,[11−15] color displays,[16] or sensing.[17,18] UC luminescent materials are generally phosphors, i.e., inorganic hosts doped with rare-earth (RE) cations, e.g., Er3+, Ho3+, and Tm3+, with unique ladderlike energy levels. Oxide hosts typically feature better thermal stability, these matrices come with higher phonon energies, being inclined to suffer from lower UC efficiencies.[27,28] it remains intriguing to develop

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