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dc.contributor.advisorZysman-Colman, Eli
dc.contributor.advisorOlivier, Yoann
dc.contributor.authorHall, David Luke Starkey
dc.coverage.spatial339 p.en_US
dc.description.abstractThis thesis concerns the study of organic TADF materials, focussing on donor-acceptor (D-A TADF) and multi-resonance (MR-TADF) emitters. Materials were developed in silico, they were then synthesized, characterized and finally tested in OLED devices. Chapter 1 introduces the various radiative decay pathways available in electronically excited molecules from photoluminescence and electroluminescence. D-A TADF and MR-TADF emitters are discussed in detail. Chapter 2 introduces the background behind the computational methods undertaken. These include Hartree Fock, coupled cluster and DFT. Chapter 3 investigates the impact of donor dendrons in the TADF emitter 2CzPN. Donor extension improves kRISC but at the expense of increasing non-radiative pathways. Chapter 4 discloses a new acceptor unit, BImPy, which is coupled to phenoxazine as a donor, with TADF observed. The torsion angle within the acceptor was modulated as a function of N-substitution, with 4 emitters studied. In Chapter 5 a computational investigation of a series of 14 literature D-A TADF emitters is undertaken, with calculated T₁, T₂, S₁, ΔE[sub](ST), ΔE[sub](ST2) and ΔE[sub](T2T1) along with S₁, T₁ and T₂ excited state natures from DFT compared with SCS-CC2, with M06-2X and CAM-B3LYP performing well. Chapter 6 presents an accurate method for computational modelling of MR-TADF, SCS-CC2. This method is then used to design two new MR-TADF emitters which were synthesized and their optoelectronic properties evaluated with OLEDs fabricated. In Chapter 7 the calculated S₁, T₁ and ΔE[sub](ST) of 35 literature MR-TADF emitters from SCS-CC2 and TD(A)-DFT are compared with experimental values, with SCS-CC2 performing well. Using SCS-CC2 the properties of MR-TADF emitters are discussed and further studies of related INVEST materials and D-A emitters that contain a MR-TADF acceptors are undertaken. Chapter 8 presents a new class of MR-TADF emitter without acceptor units designed using SCS-CC2. Modest TADF in doped films and high performing hyperfluorescent OLEDs are presented.en_US
dc.publisherUniversity of St Andrews
dc.relationComputational design, synthesis and optoelectronic characterisation of thermally activated delayed fluorescent materials - Donor acceptor and Multiresonance designs (thesis data) Hall, D., University of St Andrews, 23 Feb 2023 DOI:
dc.rightsCreative Commons Attribution-NonCommercial-NoDerivatives 4.0 International*
dc.subjectCoupled clusteren_US
dc.subjectD-A TADFen_US
dc.titleComputational design, synthesis and optoelectronic characterisation of thermally activated delayed fluorescent materials : donor-acceptor and multi-resonance designsen_US
dc.contributor.sponsorLeverhulme Trusten_US
dc.type.qualificationnamePhD Doctor of Philosophyen_US
dc.publisher.institutionThe University of St Andrewsen_US
dc.publisher.departmentUniversité de Monsen_US
dc.rights.embargoreasonThesis restricted in accordance with University regulations. Restricted until 11th April 2023en

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