Tailoring spin mixtures by ion-enhanced Maxwell magnetic coupling in color-tunable organic electroluminescent devices

In this work, we show that the spin dynamics of excitons can be dramatically altered by Maxwell magnetic field coupling, together with an ion-enhanced, low-internal-splitting-energy organic semiconducting emitter. By employing a unique, alternating current (AC)-driven organic electroluminescent (OEL) device architecture that optimizes this magnetic field coupling, almost complete control over the singlet-to-triplet ratio (from fluorescent to phosphorescent emission in a single device) is realized. We attribute this spin population control to magnetically sensitive polaron–spin pair intersystem crossings (ISCs) that can be directly manipulated through external driving conditions. As an illustration of the utility of this approach to spin-tailoring, we demonstrate a simple hybrid (double-layer) fluorescence–phosphorescence (F–P) device using a polyfluorene-based emitter with a strong external Zeeman effect and ion-induced long carrier diffusion. Remarkable control over de-excitation pathways is achieved by controlling the device-driving frequency, resulting in complete emission blue–red color tunability. Picosecond photoluminescence (PL) spectroscopy directly confirms that this color control derives from the magnetic manipulation of the singlet-to-triplet ratios. These results may pave the way to far more exotic organic devices with magnetic-field-coupled organic systems that are poised to usher in an era of dynamic spintronics at room temperature.