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dc.contributor.authorKanibolotsky, Alexander L.
dc.contributor.authorLaurand, Nicolas
dc.contributor.authorDawson, Martin D.
dc.contributor.authorTurnbull, Graham A.
dc.contributor.authorSamuel, Ifor D.W.
dc.contributor.authorSkabara, Peter J.
dc.date.accessioned2019-07-09T11:30:07Z
dc.date.available2019-07-09T11:30:07Z
dc.date.issued2019-06-18
dc.identifier259545138
dc.identifierc8f60e91-fd7e-4f22-9110-f3d50fbe2dd9
dc.identifier85067420291
dc.identifier000472683000017
dc.identifier.citationKanibolotsky , A L , Laurand , N , Dawson , M D , Turnbull , G A , Samuel , I D W & Skabara , P J 2019 , ' Design of linear and star-shaped macromolecular organic semiconductors for photonic applications ' , Accounts of Chemical Research , vol. 52 , no. 6 , pp. 1665-1674 . https://doi.org/10.1021/acs.accounts.9b00129en
dc.identifier.issn0001-4842
dc.identifier.urihttps://hdl.handle.net/10023/18059
dc.descriptionP.J.S. and A.L.K. thank the EPSRC for funding under Grants EP/R03480X/1, EP/P02744X/2, and EP/N009908/2.en
dc.description.abstractOne of the most desirable and advantageous attributes of organic materials chemistry is the ability to tune the molecular structure to achieve targeted physical properties. This can be performed to achieve specific values for the ionization potential or electron affinity of the material, the absorption and emission characteristics, charge transport properties, phase behavior, solubility, processability, and many other properties, which in turn can help push the limits of performance in organic semiconductor devices. A striking example is the ability to make subtle structural changes to a conjugated macromolecule to vary the absorption and emission properties of a generic chemical structure. In this Account, we demonstrate that target properties for specific photonic applications can be achieved from different types of semiconductor structures, namely, monodisperse star-shaped molecules, complex linear macromolecules, and conjugated polymers. The most appropriate material for any single application inevitably demands consideration of a trade-off of various properties; in this Account, we focus on applications such as organic lasers, electrogenerated chemiluminescence, hybrid light emitting diodes, and visible light communications. In terms of synthesis, atom and step economies are also important. The star-shaped structures consist of a core unit with 3 or 4 functional connection points, to which can be attached conjugated oligomers of varying length and composition. This strategy follows a convergent synthetic pathway and allows the isolation of target macromolecules in good yield, high purity, and absolute reproducibility. It is a versatile approach, providing a wide choice of constituent molecular units and therefore varying properties, while the products share many of the desirable attributes of polymers. Constructing linear conjugated macromolecules with multifunctionality can lead to complex synthetic routes and lower atom and step economies, inferior processability, and lower thermal or chemical stability, but these materials can be designed to provide a range of different targeted physical properties. Conventional conjugated polymers, as the third type of structure, often feature so-called “champion” properties. The synthetic challenge is mainly concerned with monomer synthesis, but the final polymerization sequence can be hard to control, leading to variable molecular weights and polydispersities and some degree of inconsistency in the properties of the same material between different synthetic batches. If a champion characteristic persists between samples, then the variation of other properties between batches can be tolerable, depending on the target application. In the case of polymers, we have chosen to study PPV-type polymers with bulky side groups that provide protection of their conjugated backbone from π–π stacking interactions. These polymers exhibit high photoluminescence quantum yields (PLQYs) in films and short radiative lifetimes and are an important benchmark to monodisperse star-shaped systems in terms of different absorption/emission regions. This Account therefore outlines the advantages and special features of monodisperse star-shaped macromolecules for photonic applications but also considers the two alternative classes of materials and highlights the pros and cons of each class of conjugated structure.
dc.format.extent10
dc.format.extent4690287
dc.language.isoeng
dc.relation.ispartofAccounts of Chemical Researchen
dc.subjectQD Chemistryen
dc.subjectChemistry(all)en
dc.subjectNDASen
dc.subject.lccQDen
dc.titleDesign of linear and star-shaped macromolecular organic semiconductors for photonic applicationsen
dc.typeJournal articleen
dc.contributor.institutionUniversity of St Andrews. Organic Semiconductor Centreen
dc.contributor.institutionUniversity of St Andrews. School of Physics and Astronomyen
dc.contributor.institutionUniversity of St Andrews. Sir James Mackenzie Institute for Early Diagnosisen
dc.contributor.institutionUniversity of St Andrews. Centre for Biophotonicsen
dc.contributor.institutionUniversity of St Andrews. Condensed Matter Physicsen
dc.identifier.doi10.1021/acs.accounts.9b00129
dc.description.statusPeer revieweden


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