Molecular hyperfine fields in organic magnetoresistance devices

We calculate molecular hyperfine fields in organic magnetoresistance (OMAR) devices using ab initio calculations. To do so, we establish a protocol for the accurate determination of the average hyperfine field B-hf and apply it to selected molecular ions: NPB, TPD, and Alq(3). Then, we make devices with precisely the same molecules and perform measurements of the OMAR effect, in order to address the role of hole-transport layer in the characteristic magnetic field B-0 of OMAR. Contrary to common belief, we find that molecular hyperfine fields are not only caused by hydrogen nuclei. We also find that dipolar contributions to the hyperfine fields can be comparable to the Fermi contact contributions. However, such contributions are restricted to nuclei located in the same molecular ion as the charge carrier (intramolecular), as extramolecular contributions are negligible. DOI: 10.1103/PhysRevB.87.125204