Creating novel thermally activated delayed fluorescence (TADF) emitters for light-emitting electrochemical cells (LEECs) and organic light-emitting diodes (OLEDs) applications and their structure-property relationship

Developing organic light-emitting diodes (OLEDs) as the next generation display devices is not only of industrial interest, but also a scientific challenge in and of itself that requires multi-disciplinary efforts to make the technology successful. Thermally activated delayed fluorescence (TADF) is a recent breakthrough in OLED technology whose prime value is to enable purely organic emitters to recruit the dark triplet excitons in the device, thus avoiding expensive and toxic rare metal based emitters. This thesis is centred on TADF and contains work in three major areas. Firstly, novel ionic TADF emitters were designed for use in light-emitting electrochemical cells (LEECs), which is an alternative electroluminescent device technology to OLEDs, with a much simplified fabrication procedure and architecture. The vast majority of these ionic emitters are based on reported TADF scaffolds where the donors were tethered with an imidazolium hexafluorophosphate group to obtain the ionic character required for LEEC devices (TL and BTL series, Chapter 2). On the other hand, TADF emitters with a carboxylate group were also designed which act as both acceptor and intrinsic charged functionality for LEEC applications (CTL series, Chapter 2). Secondly, attempts were made to create novel TADF molecular scaffolds in order to enrich the current library of TADF emitters. Research efforts were focused on polyaromatic moieties such as anthracene (An series, Chapter 4) and fluoranthene (FA series, Chapter 4) that are seldom reported in TADF literature. In addition, TADF emitters with phosphine oxide as the acceptor group have also been studied (PO series, Chapter 5). Lastly, structure-property relationship studies of TADF emitters were undertaken as a function of tuning of donor and acceptor functionalities using both theoretical and experimental approaches in order to gain more insight for designing desirable TADF emitters (Chapter 3)