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.