Tuning Hyperfine Fields in Conjugated Polymers for Coherent Organic Spintronics

An appealing avenue for organic spintronics lies in direct coherent control of the spin population by means of pulsed electron spin resonance techniques. Whereas previous work has focused on the electrical detection of coherent spin dynamics, we demonstrate here the equivalence of an all-optical approach, allowing us to explore the influence of materials chemistry on the spin dynamics. We show that deuteration of the conjugated polymer side groups weakens the local hyperfine fields experienced by electron hole pairs, thereby lowering the threshold for the resonant radiation intensity at which coherent coupling and spin beating occur. The technique is exquisitively sensitive to previously obscured material properties and offers a route to quantifying and tuning hyperfine fields in organic semiconductors.