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Title: Conjugated polymer-metal complexes for organic electronics
Author: Andernach, Rolf
ISNI:       0000 0004 5994 3353
Awarding Body: Imperial College London
Current Institution: Imperial College London
Date of Award: 2016
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Organometallic complexes play a crucial role in Organic Electronics and due to their interesting optoelectronic properties they have been widely applied in organic light-emitting diodes and organophotovoltaic devices. Organometallic complexes are often used in the form of small molecules and their exact orientation in the bulk material can have a major effect on device performance. In this work, different approaches of covalently incorporating metal-porphyrin complexes into polymers were explored with the aim of producing homogeneous donor-acceptor type polymers which allow for the elimination of phase separation effects within the active material of the respective devices. A set of design rules was developed for the creation of porphyrin-polymer complexes and their application as host-guest systems in the triplet-sensitisation of semi-conducting polymers was studied, determining the optimal functional groups as well as matching absorption and emission properties. To this end, a synthesis pathway was developed that enabled the creation of metal porphyrins as well as their specific functionalisation for use in different co-polymerisation reactions. Platinum (II), palladium (II) and zinc (II) porphyrins were synthesised and successfully incorporated into a series of semi-conducting polymers: regiorandom and regioregular poly(3-hexylthiophene) (P3HT), poly(bis(decylthiophene)phenylene) (TTP) and poly(para-phenylenevinylene) (PPV). Successful co-polymerisation was reported for all polymers and the electronic interaction between the polymer hosts and porphyrin guests was analysed. The successful creation of triplet-sensitised polymers was shown and the full triplet formation pathway was mapped by spectroscopic means, creating a novel tool for the generation and analysis of polymer triplet excitons. Finally, computational methods were used for the accurate description of polymer triplet excited states and their usefulness in the prediction of excited state properties was shown. Polymer models were designed, computed and compared to experimental data and the use of computational methods as a widely applicable and precise tool for determining polymer excited states was discussed, further substantiating the design rules developed throughout this work.
Supervisor: Heeney, Martin Sponsor: Not available
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral