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This thesis concerns itself with the scientific study of the recently discovered organic magnetoresistance (OMAR) whose underlying mechanism is currently not known with certainty. As an introduction, we briefly review the major findings from prior work done by my colleagues. They found that OMAR can be as large as ~10% magnetoresistance at 10 mT magnetic fields at room temperature. Both OMAR and other kinds of magnetic field effect data in organics can be fitted using the empirical laws B^2/(B^2+B_0^2) or B^2/(|B|+B_0)^2, dependent on material. The fitting parameter B_0 is a measure of the characteristic magnetic field strength of OMAR.
We explore the dependence of B_0 on material parameters to clarify the origin of OMAR. Various pi-conjugated semiconductor OMAR devices were studied to explore the possibility that hyperfine interaction causes OMAR. For a quantitative analysis of the experiments, we developed a theoretical fitting formula to relate B_0 to the hyperfine coupling strength.
In addition, organic materials with different spin-orbit coupling strengths were also measured. Fluorescence and phosphorescence spectroscopies were used to estimate the spin-orbit coupling strength from the measured spectra. For analyzing our measurements, we developed a fitting formula from the time-dependent Schrodinger equation that takes into account the combined effect of hyperfine and spin-orbit coupling on spin-dynamics. We found that in the case of strong spin-orbit coupling, it dominates the behavior, resulting in magnetic field effect traces that are much wider than those in ordinary organics. However, a small cone remains at zero field with a width equal to the hyperfine coupling strength. We find qualitative agreement between the experimental results and the model.
We also investigated the question whether OMAR is related to an excitonic effect, or is primarily a transport effect. We measured the magnetic field effects on current, photocurrent and electroluminescence to address this question. By varying the injection efficiency of the minority carriers, we show that OMAR most likely is not an excitonic effect.
Our results provide strong evidence in support of the claim that OMAR is caused by spin-dynamics. However, further study is required to study the mechanism connecting spin-dynamics and conductivity.