Targeted design leads to tunable photoluminescence from perylene dicarboxdiimide–poly(oxyalkylene)/siloxane hybrids for luminescent solar concentrators

Meazzini, Ilaria; Willis‐Fox, Niamh; Blayo, Camille; Arlt, Jochen; Clément, Sébastien; Evans, Rachel C.

doi:10.1039/c5tc03952e

Cited by 29 publications

(88 citation statements)

References 62 publications

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“…While LR305 shows a tendency to aggregate in ureasils, 6 we have recently shown that by covalently grafting the PDI-Sil analogue to the siloxane backbone of the ureasil, aggregation can be effectively reduced, leading to high PLQYs (~80%). 33 Herein, we show that due to excellent spectral overlap, p-O-TPE and PDI-Sil act as an efficient FRET pair in a ureasil waveguide. We observe that FRET also leads to reduced non-radiative relaxation of the p-O-TPE donor and extends the solar-harvesting window of the final LSC, giving rise to improved optical quantum efficiencies.…”

Section: Introductionmentioning

confidence: 80%

“…Water was obtained from Millipore Simpak 2 water purification system. Poly-diphenoxytetraphenylethylene (p-O-TPE) 30 and N,N-bis(3-triethoxysilylpropyl)-1,6,7,12-tetra-tertbutylphenoxyperylene-3,4:9,10-tetra-carboxdiimide 33 were synthesized as previously reported.…”

Section: Methodsmentioning

confidence: 99%

“…The choice of waveguide is also important, since both the donor and acceptor lumophores must be well-dispersed through the host. A family of organic-inorganic hybrid polymers known as ureasils have been demonstrated as excellent waveguides for LSCs 32,33,34,35 and other optical applications. 36 As hybrid materials, ureasils combine the easy processability and chemical functionality of organic polymers with the high optical transparency and stability of the typical inorganic waveguides.…”

Section: Introductionmentioning

confidence: 99%

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Luminescent Solar Concentrators Based on Energy Transfer from an Aggregation-Induced Emitter Conjugated Polymer

Lyu,

Kendall,

Meazzini

et al. 2019

Preprint

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Luminescent solar concentrators (LSCs) are solar-harvesting devices fabricated from transparent waveguide that is doped or coated with lumophores. Despite their potential for architectural integration, the optical efficiency of LSCs is often limited by incomplete harvesting of solar radiation and aggregation-caused quenching (ACQ) of lumophores in the solid state. Here, we demonstrate a multi-lumophore LSC design which circumvents these challenges through a combination of non-radiative Förster energy transfer (FRET) and aggregation-induced emission (AIE). The LSC incorporates a green-emitting poly(tetraphenylethylene), p-O-TPE, as an energy donor and a red-emitting perylene bisimide molecular dye (PDI-Sil) as the energy acceptor, within an organic-inorganic hybrid di-ureasil waveguide. Steady-state photoluminescence studies demonstrate that the di-ureasil host induced AIE from the p-O-PTE donor polymer, leading to a high photoluminescence quantum yield (PLQY) of ~45% and a large Stokes shift of ~150 nm.Covalent grafting of the PDI-Sil acceptor to the siliceous domains of the di-ureasil waveguide also inhibits non-radiative losses by preventing molecular aggregation. Due to the excellent spectral overlap, FRET was shown to occur from p-O-TPE to PDI-Sil, which increased with acceptor concentration. As a result, the final LSC (4.5 cm ´ 4.5 cm ´ 0.3 cm) with an optimised donoracceptor ratio (1:1 by wt%) exhibited an internal photon efficiency of 20%, demonstrating a viable design for LSCs utilising an AIE-based FRET approach to improve the solar-harvesting performance.reduced loss of absorbed photons as a result of the FRET process. Enhancement in the external photon efficiency of the donor-acceptor LSC was also observed due to the extended solarharvesting window provided by the complementary absorption spectra of the dual lumophore system. The results also demonstrate the importance of lumophore-waveguide interactions in determining the final LSC efficiency. Here, the di-ureasil waveguide is used to promote aggregation and thus switch-on emission from the AIE-donor, while simultaneously covalent grafting of the acceptor reduces ACQ. This study therefore demonstrates that the bottom-up design of integrated lumophore-waveguide materials is a viable strategy to overcome the intrinsic optical losses of LSCs and to boost their solar-harvesting performance. ASSOCIATED CONTENTSupporting Information.

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Section: Introductionmentioning

confidence: 80%

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Luminescent Solar Concentrators Based on Energy Transfer from an Aggregation-Induced Emitter Conjugated Polymer

Lyu,

Kendall,

Meazzini

et al. 2019

Preprint

Self Cite

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“…[12,13] The aggregate morphology andc rystal structure can also be controlled. [14][15][16][17][18][19][20][21][22] PDIs can interactt oc reate chiral or helical structures, [23] wires, [20,24] "fish-tail" structures, [25] liquid crystal phases, [26] self-assembled mixed aggregates, [27][28][29] and crystallites of varying degrees of disorder. [30,31] These molecular morphologyand electronic modificationshave facilitated many potential materials applications.…”

Section: Introductionmentioning

confidence: 99%

“…[30,31] These molecular morphologyand electronic modificationshave facilitated many potential materials applications. [2,17,[32][33][34] Although morphology control has been studied for av ariety of PDI systems, many of the approaches used to control aggregation have been performed in halogenated or organic solvents.T here has been an increasing interest in creating PDIs that are soluble in aqueous or more polar solvents. [18,19,[35][36][37][38][39][40] Many of these molecules use hydroxy-terminated, large dendritic [41] or oligosilsesquioxane [42][43][44] groups to deter aggregation and dimerization of the PDIs in these solutions.…”

Section: Introductionmentioning

confidence: 99%

Improving the Quantum Yields of Perylene Diimide Aggregates by Increasing Molecular Hydrophobicity in Polar Media

Austin

Mylon

et al. 2017

ChemPhysChem

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Here we report the quantum yield of four aggregated perylene diimide (PDI) species that vary by the length of the branched side chains attached at the N,N' imide positions. The PDI molecules were dissolved in binary water:methanol solvents as a means to vary the solvent polarity and control the degree of aggregation in solution. By performing spectroscopy, kinetics, and light scattering experiments, the nature of the molecular interactions in the solutions was determined. The maximum quantum yield of the aggregated molecules increased from 0.04 for the shortest chain molecule (B2) to 0.20 for the largest chain molecule (B13). The higher quantum yield of B13 compared with B2 correlates well with an increase in the fluorescence lifetime. The monomer emission lifetime was 4.8 ns whereas a lifetime as high as 21.2 ns was measured for the B13 aggregate fluorescence. A shorter sub-nanosecond lifetime was also measured for suspended colloids in B5, B9, and B13. The enhanced quantum yield is attributed to an increase of disorder in the B13 aggregates. As the polarity of the solution increases, the hydrophobic effect further enhances the disorder, and, therefore, the quantum yields in these particles.

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Towards Efficient Spectral Converters through Materials Design for Luminescent Solar Devices

2017

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Single-junction photovoltaic devices exhibit a bottleneck in their efficiency due to incomplete or inefficient harvesting of photons in the low- or high-energy regions of the solar spectrum. Spectral converters can be used to convert solar photons into energies that are more effectively captured by the photovoltaic device through a photoluminescence process. Here, recent advances in the fields of luminescent solar concentration, luminescent downshifting, and upconversion are discussed. The focus is specifically on the role that materials science has to play in overcoming barriers in the optical performance in all spectral converters and on their successful integration with both established (e.g., c-Si, GaAs) and emerging (perovskite, organic, dye-sensitized) cell types. Current challenges and emerging research directions, which need to be addressed for the development of next-generation luminescent solar devices, are also discussed.

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Targeted design leads to tunable photoluminescence from perylene dicarboxdiimide–poly(oxyalkylene)/siloxane hybrids for luminescent solar concentrators

Abstract: The chain length and branching of the organic backbone of poly(oxyalkylene)/siloxane ureasils can be used to control the placement and orientation of a covalently-grafted perylene, leading to tunable photoluminescence.

Cited by 29 publications

References 62 publications

Luminescent Solar Concentrators Based on Energy Transfer from an Aggregation-Induced Emitter Conjugated Polymer

Luminescent Solar Concentrators Based on Energy Transfer from an Aggregation-Induced Emitter Conjugated Polymer

Improving the Quantum Yields of Perylene Diimide Aggregates by Increasing Molecular Hydrophobicity in Polar Media

Towards Efficient Spectral Converters through Materials Design for Luminescent Solar Devices

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