triplet-fusion-upconversion-nanocapsule-synthesis

Triplet Fusion Upconversion Nanocapsule Synthesis

Triplet fusion upconversion (UC) allows for the generation of one high energy photon from two low energy input photons. This well-studied process has ...

Harvard University

Light-emitting diodes utilizing perovskite nanocrystals have generated strong interest in the past several years, with green and red devices showing high efficiencies. Blue devices, however, have lagged significantly behind. Here, it is shown that the device architecture plays a key role in this lag and that NiO , a transport layer in one of the highest efficiency devices to date, causes a significant reduction in perovskite luminescence lifetime. An alternate transport layer structure which maintains robust nanocrystal emission is proposed. Devices with this architecture show external quantum efficiencies of 0.50% at 469 nm, seven times higher than state-of-the-art devices at that wavelength. Finally, it is demonstrated that this architecture enables efficient devices across the entire blue-green portion of the spectrum. The improvements demonstrated here open the door to efficient blue perovskite light-emitting diodes.

Reducing Architecture Limitations for Efficient Blue Perovskite Light-Emitting Diodes.

Nanocrystals based on halide perovskites offer a promising material platform for highly efficient lighting. Using transient optical spectroscopy, we study excitation recombination dynamics in manganese-doped CsPb(Cl,Br) perovskite nanocrystals. We find an increase in the intrinsic excitonic radiative recombination rate upon doping, which is typically a challenging material property to tailor. Supported by  calculations, we can attribute the enhanced emission rates to increased charge carrier localization through lattice periodicity breaking from Mn dopants, which increases the overlap of electron and hole wave functions locally and thus the oscillator strength of excitons in their vicinity. Our report of a fundamental strategy for improving luminescence efficiencies in perovskite nanocrystals will be valuable for maximizing efficiencies in light-emitting applications.

Charge Carrier Localization in Doped Perovskite Nanocrystals Enhances Radiative Recombination.

Halide mixing is one of the most powerful techniques to tune the optical bandgap of metal-halide perovskites. However, halide mixing has commonly been observed to result in phase segregation, which reduces excited-state transport and limits device performance. While the current emphasis lies on the development of strategies to prevent phase segregation, it remains unclear how halide mixing may affect excited-state transport even if phase purity is maintained. Here, we study exciton transport in phase pure mixed-halide 2D perovskites of (PEA)Pb(I Br  ). Using transient photoluminescence microscopy, we show that, despite phase purity, halide mixing inhibits exciton transport. We find a significant reduction even for relatively low alloying concentrations. By performing Brownian dynamics simulations, we are able to reproduce our experimental results and attribute the decrease in diffusivity to the energetically disordered potential landscape that arises due to the intrinsic random distribution of alloying sites.

Halide Mixing Inhibits Exciton Transport in Two-dimensional Perovskites Despite Phase Purity.

Three-dimensional (3D) printing has exploded in interest as new technologies have opened up a multitude of applications, with stereolithography a particularly successful approach. However, owing to the linear absorption of light, this technique requires photopolymerization to occur at the surface of the printing volume, imparting fundamental limitations on resin choice and shape gamut. One promising way to circumvent this interfacial paradigm is to move beyond linear processes, with many groups using two-photon absorption to print in a truly volumetric fashion. Using two-photon absorption, many groups and companies have been able to create remarkable nanoscale structures, but the laser power required to drive this process has limited print size and speed, preventing widespread application beyond the nanoscale. Here we use triplet fusion upconversion to print volumetrically with less than 4 milliwatt continuous-wave excitation. Upconversion is introduced to the resin by means of encapsulation with a silica shell and solubilizing ligands. We further introduce an excitonic strategy to systematically control the upconversion threshold to support either monovoxel or parallelized printing schemes, printing at power densities several orders of magnitude lower than the power densities required for two-photon-based 3D printing.

Article	Year
Reducing Architecture Limitations for Efficient Blue Perovskite Light-Emitting Diodes. Advanced materials (Deerfield Beach, Fla.)\| PubMed ID: 29575250	2018
Charge Carrier Localization in Doped Perovskite Nanocrystals Enhances Radiative Recombination. Journal of the American Chemical Society\| PubMed ID: 33993693	2021
Halide Mixing Inhibits Exciton Transport in Two-dimensional Perovskites Despite Phase Purity. ACS energy letters\| PubMed ID: 35059502	2022
Triplet fusion upconversion nanocapsules for volumetric 3D printing. Nature\| PubMed ID: 35444324	2022

Mahesh K. Gangishetty

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