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      Synergistic photoluminescence enhancement in conjugated polymer-di-ureasil organic–inorganic composites†

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          Abstract

          Energy transfer between a hybrid di-ureasil host and conjugated polymer dopants results in a dramatic enhancement in the photoluminescence quantum yield due to exciton isolation at long-lived trap sites.

          Abstract

          Poly(fluorene) conjugated polyelectrolyte (CPE)-di-ureasil organic–inorganic composites have been prepared using a versatile sol–gel processing method, which enables selective localisation of the CPE within the di-ureasil matrix. Introduction of the CPE during the sol–gel reaction leads to a homogeneous distribution of the CPE throughout the di-ureasil, whereas a post-synthesis solvent permeation route leads to the formation of a confined layer of the CPE at the di-ureasil surface. The CPE and the di-ureasil both function as photoactive components, contributing directly to, and enhancing the optical properties of their composite material. The bright blue photoluminescence exhibited by CPE-di-ureasils is reminiscent of the parent CPE; however the distinct contribution of the di-ureasil to the steady-state emission profile is also apparent. This is accompanied by a dramatic increase in the photoluminescence quantum yield to >50%, which is a direct consequence of the synergy between the two components. Picosecond time-correlated single photon counting measurements reveal that the di-ureasil effectively isolates the CPE chains, leading to emissive trap sites which have a high radiative probability. Moreover, intimate mixing of the CPE and the di-ureasil, coupled with their strong spectral overlap, results in efficient excitation energy transfer from the di-ureasil to these emissive traps. Given the simple, solution-based fabrication method and the structural tunability of the two components, this approach presents an efficient route to highly desirable CPE-hybrid materials whose optoelectronic properties may be enhanced and tailored for a targeted application.

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          Most cited references61

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          Relationship between Absorption Intensity and Fluorescence Lifetime of Molecules

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            Excitons in nanoscale systems.

            Nanoscale systems are forecast to be a means of integrating desirable attributes of molecular and bulk regimes into easily processed materials. Notable examples include plastic light-emitting devices and organic solar cells, the operation of which hinge on the formation of electronic excited states, excitons, in complex nanostructured materials. The spectroscopy of nanoscale materials reveals details of their collective excited states, characterized by atoms or molecules working together to capture and redistribute excitation. What is special about excitons in nanometre-sized materials? Here we present a cross-disciplinary review of the essential characteristics of excitons in nanoscience. Topics covered include confinement effects, localization versus delocalization, exciton binding energy, exchange interactions and exciton fine structure, exciton-vibration coupling and dynamics of excitons. Important examples are presented in a commentary that overviews the present understanding of excitons in quantum dots, conjugated polymers, carbon nanotubes and photosynthetic light-harvesting antenna complexes.
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              Semiconducting Polyfluorenes—Towards Reliable Structure-Property Relationships

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                Author and article information

                Journal
                Chem Sci
                Chem Sci
                Chemical Science
                Royal Society of Chemistry
                2041-6520
                2041-6539
                1 December 2015
                17 September 2015
                : 6
                : 12
                : 7227-7237
                Affiliations
                [a ] School of Chemistry and CRANN , Trinity College , The University of Dublin , Dublin 2 , Ireland . Email: raevans@ 123456tcd.ie
                [b ] Makromolekulare Chemie , Bergische Universität Wuppertal , 42097 Wuppertal , Germany
                [c ] Chemistry Department , University of Coimbra , 3004-535 Coimbra , Portugal
                [d ] Collaborative Optical Spectroscopy , Micromanipulation and Imaging Centre (COSMIC) and SUPA , School of Physics and Astronomy , King's Buildings , University of Edinburgh , EH9 3JZ , UK
                [e ] Departamento de Física and CICECO , Universidade de Aveiro , 3810-193 Aveiro , Portugal
                Author information
                http://orcid.org/0000-0002-4152-5896
                http://orcid.org/0000-0003-4747-6535
                http://orcid.org/0000-0003-3127-2298
                Article
                c5sc02409a
                10.1039/c5sc02409a
                5947540
                b0236319-2cd7-459b-b6bc-2fba955051dd
                This journal is © The Royal Society of Chemistry 2015

                This article is freely available. This article is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported Licence (CC BY-NC 3.0)

                History
                : 4 July 2015
                : 17 September 2015
                Categories
                Chemistry

                Notes

                †Electronic supplementary information (ESI) available: Synthesis and experimental methods, solvent permeation data, structural characterisation data (powder X-ray diffractograms, 29Si and 13C solid-state MAS NMR spectra), supporting PL and excitation spectra, ps-TCSPC decay curves and fitting data, and FTIR fitting data. See DOI: 10.1039/c5sc02409a


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