The hyperfine interaction role in the spin response of π-conjugated polymer films and spin valve devices

Although the hyperfine interaction (HFI) has been foreseen to play an important role in organic spin response, clear experimental evidence for it has been scarce. We studied and compared spin dynamics in films and organic spin-valve (OSV) devices based on π-conjugated polymers made of protonated, H-, deuterated, D-hydrogen (having a weaker HFI strength, aHFI), and 13C-rich chains (having stronger aHFI). We demonstrate that HFI indeed plays a crucial role in the spin dynamics of all three polymer isotopes. Films based on the D-polymer show substantial narrower optically detected magnetic resonance of spin ½ polarons; whereas due to the longer spin diffusion, OSV devices based on D-polymers show substantially larger magnetoresistance. We also found that the giant magnetoresistance (GMR) steep temperature dependence in OSV devices is isotope independent, showing that is due to the magnetic response of the ferromagnetic electrodes. In addition, we found that the GMR steep voltage dependence is isotope dependent indicating that is due to a spin injection process at the electrodes, rather than spin transport through the organic interlayer. Finally we report GMR response in OSV devices made of C60 interlayer having very weak HFI. These devices show sharp GMR response, and may therefore be excellent candidates for room temperature operation.