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Jaque, Daniel

Publications and source records attributed to Jaque, Daniel.

A Generalized Approach to Photon Avalanche Upconversion in Luminescent Nanocrystals

Photon avalanching nanoparticles (ANPs) exhibit extremely nonlinear upconverted emission valuable for subdiffraction imaging, nanoscale sensing, and optical computing. Avalanching has been demonstrated with Tm 3+ -, Pr 3+ -, or Nd 3+ -doped nanocrystals, but their emission is limited to a few wavelengths and materials. Here, we utilize Gd 3+ -assisted energy migration to tune the emission wavelengths of Tm 3+ -sensitized ANPs and generate highly nonlinear emission from Eu 3+ , Tb 3+ , Ho 3+ , and Er 3+ ions. The upconversion intensities of these spectrally discrete ANPs scale with nonlinearity factor s = 10-17 under 1064 nm excitation at power densities as low as 7 kW cm -2 . This strategy for imprinting avalanche behavior on remote emitters can be extended to fluorophores adjacent to ANPs, as here we demonstrate with CdS/CdSe/CdS core/shell/shell quantum dots. ANPs with rationally designed energy transfer networks provide the means to transform conventional linear emitters into a highly nonlinear ones, expanding the use of photon avalanching in biological, chemical, and photonic applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Tuning Phonon Energies in Lanthanide‐doped Potassium Lead Halide Nanocrystals for Enhanced Nonlinearity and Upconversion

Abstract Optical applications of lanthanide‐doped nanoparticles require materials with low phonon energies to minimize nonradiative relaxation and promote nonlinear processes like upconversion. Heavy halide hosts offer low phonon energies but are challenging to synthesize as nanocrystals. Here, we demonstrate the size‐controlled synthesis of low‐phonon‐energy KPb 2 X 5 (X=Cl, Br) nanoparticles and the ability to tune nanocrystal phonon energies as low as 128 cm −1 . KPb 2 Cl 5 nanoparticles are moisture resistant and can be efficiently doped with lighter lanthanides. The low phonon energies of KPb 2 X 5 nanoparticles promote upconversion luminescence from higher lanthanide excited states and enable highly nonlinear, avalanche‐like emission from KPb 2 Cl 5 : Nd 3+ nanoparticles. The realization of nanoparticles with tunable, ultra‐low phonon energies facilitates the discovery of nanomaterials with phonon‐dependent properties, precisely engineered for applications in nanoscale imaging, sensing, luminescence thermometry and energy conversion.

Zhang, Zhuolei↗

Tuning Phonon Energies in Lanthanide-doped Potassium Lead Halide Nanocrystals for Enhanced Nonlinearity and Upconversion

Optical applications of lanthanide-doped nanoparticles require materials with low phonon energies to minimize nonradiative relaxation and promote nonlinear processes like upconversion. Heavy halide hosts offer low phonon energies but are challenging to synthesize as nanocrystals. Here, we demonstrate the size-controlled synthesis of low-phonon-energy KPb 2 X 5 (X=Cl, Br) nanoparticles and the ability to tune nanocrystal phonon energies as low as 128 cm -1 . KPb 2 Cl 5 nanoparticles are moisture resistant and can be efficiently doped with lighter lanthanides. Further, the low phonon energies of KPb 2 X 5 nanoparticles promote upconversion luminescence from higher lanthanide excited states and enable highly nonlinear, avalanche-like emission from KPb 2 Cl 5 : Nd 3+ nanoparticles. The realization of nanoparticles with tunable, ultra-low phonon energies facilitates the discovery of nanomaterials with phonon-dependent properties, precisely engineered for applications in nanoscale imaging, sensing, luminescence thermometry and energy conversion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗