Photon upconversion (UC) is a technology that can increase solar utilization efficiencies in broad photoenergy conversion systems by converting lower-energy photons into usable higher-energy photons. Recently, UC using triplet-triplet annihilation (TTA) of organic molecules has drawn attention because it is presently the only method applicable to weak and noncoherent light. To date, many attempts have been made to realize this UC technology in forms suitable for applications, but they typically suffer from either high cost or insufficient stability and/or safety of materials. Recently, a new class of liquid called deep eutectic solvents (DESs) has emerged as low-cost green fluids that possess low toxicity and vapor pressure, biodegradability, and high thermal stability. DESs have been proposed as an alternative to ionic liquids. This article develops triplet-sensitized UC samples using DESs that are found to be suitable solvents for this purpose, attaining a new materials platform for UC with the aforementioned advantages. The high thermal stability of the samples is qualitatively confirmed and their UC quantum yields are determined to be 0.11-0.21 (based on the definition that the maximum quantum yield is 0.5) depending on the DES composition. The triplet lifetime of the emitter 9,10-diphenylanthracene increases with DES viscosity, resulting in unique kinetics. Analysis of photophysical experimental results allows the relevant physics governing the performance of this sample system to be determined and discussed. Overall, a novel UC platform that simultaneously achieves high thermal stability, low cost, and environmental friendliness is developed using DESs as the solvent.
Photon upconversion based on triplet-triplet annihilation (TTA-UC) is a technology to convert presently wasted sub-bandgap photons to usable higher-energy photons. In this paper, ionogel TTA-UC samples are first developed by gelatinizing ionic liquids containing triplet-sensitizing and light-emitting molecules using an ionic gelator, resulting in transparent and nonflammable ionogel photon upconverters. The photophysical properties of the ionogel samples are then investigated, and the results suggest that the effect of gelation on the diffusion of the solutes is negligibly small. To further examine this suggestion and acquire fundamental insight into the solute transport properties of the samples, the diffusion of charge-neutral solute species over much longer distances than microscopic interpolymer distances is measured by electrochemical potential-step chronoamperometry. The results reveal that the diffusion of solute species is not affected by gelation within the tested gelator concentration range, supporting our interpretation of the initial results of the photophysical investigations. Overall, our results show that the advantage of nonfluidity can be imparted to ionic-liquid-based photon upconverters without sacrificing molecular diffusion, optical transparency, and nonflammability.
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