Conspectus
In organic
electronic technologies,
Single-Layer Phosphorescent
Organic Light-Emitting Diodes (SL-PhOLEDs), made of only the electrodes
and the Emissive Layer (EML), are a new generation of simplified PhOLEDs.
In the field of the OLED, such a type of device has been studied for
a long time as they represent “ideal” devices. Indeed,
simplifying the classical multilayer structure of PhOLEDs (called
ML-PhOLEDs) is important to reduce the amount of commodities, the
manufacture complexity, and the production and recycling costs. However,
removing the functional organic blocking/transporting layers of an
ML-PhOLED stack leads to an intense decrease in the PhOLED performance.
This is the main problem; the researchers have faced in this field.
To keep a high performance without the different organic layers, the
effective injection, transport, and recombination of charges in the
device should be performed by the EML and more particularly by the
host materials. This host material should then display a set of electronic
and physical properties, essential to reach a high-efficiency SL-PhOLED.
However, reaching high-performance SL-PhOLED is far more difficult
than for ML-PhOLED and each molecular parameter of the host can dramatically
decrease the PhOLED performance. The molecular design of the host
is then crucial and a specific design has been particularly studied
in the last years, which consists of linking an electron-rich unit
to an electron-poor unit via a spiro linkage. This design called Donor-Spiro-Acceptor (D-Spiro-A) allows one to
gather all the required properties in a single host and has allowed,
in the past few years, important advances in the field. Nowadays,
the most efficient SL-PhOLEDs use this molecular design and our group
has particularly contributed to this research field. Thus, as the
D-Spiro-A molecular design nowadays provides SL-PhOLEDs
with the highest performance, a good understanding of its impact in
the device efficiencies appears particularly important. This is the
story we want to tell herein. In this Account, we discuss through
a structure/properties/device performance relationship study (triplet
state energy level, HOMO/LUMO energy levels, charge carriers mobilities,
thermal and morphological properties, and device performances), the
recent advances made by this design in the field of SL-PhOLEDs. This
Account will mainly focus on the association of phenylacridine-like
fragments (namely, phenylacridine, indoloacridine, quinolinophenothiazine,
and quinolinoacridine) as the electron-rich unit and fluorene/phosphine
oxide as the electron-poor unit, which is, in the light of the literature,
the combination that has allowed the most important advances in the
last years. Trying to unravel why this design has led to high performance
appears to be important for the future of SL-PhOLED technology and
may lead to new directions in terms of molecular design.