Perdeuteration of poly[2-methoxy-5-(2′-ethylhexyloxy)-1,4-phenylenevinylene] (d-MEH-PPV): control of microscopic charge-carrier spin–spin coupling and of magnetic-field effects in optoelectronic devices

Control of the effective local hyperfine fields in a conjugated polymer, poly[2-methoxy-5-(2′-ethylhexyloxy)-1,4-phenylenevinylene] (MEH-PPV), by isotopic engineering is reported. These fields, evident as a frequency-independent line broadening mechanism in electrically detected magnetic resonance (EDMR) spectroscopy, originate from the unresolved hyperfine coupling between the electronic spin of charge carrier pairs and the nuclear spins of surrounding hydrogen isotopes. The room temperature study of effects caused by complete deuteration of this polymer through magnetoresistance, magnetoelectroluminescence, coherent pulsed and multi-frequency EDMR, as well as inverse spin-Hall effect measurements, confirm the weak hyperfine broadening of charge-carrier magnetic resonance lines. As a consequence, we can resolve coherent charge-carrier spin-beating, allowing for direct measurements of the magnitude of electronic spin-spin interactions. In addition, the weak hyperfine coupling allows us to resolve substantial spin-orbit coupling effects in the EDMR spectra, even at low magnetic field strengths. These results illustrate the dramatic influence of hyperfine fields on the spin physics of organic light-emitting diode (OLED) materials at room temperature, and point to routes to reaching exotic ultra-strong resonant-drive regimes in the study of light-matter interactions