Rob Roundy Thesis Defense 02/11/14

Thesis Defense

Rob Roundy

Tuesday, February 11, 2014
4:00 pm (334 JFB)


Spin-dependent recombination of polaron pairs and spin relaxation of a single polaron are the most fundamental processes are responsible for the performance of organic-spintronics-based devices such as light-emitting diodes and organic spin valves[1]. In organic materials, with no spin-orbit coupling, both processes are due to random hyperfine fields created by protons neighboring the polaron sites.

The essence of spin-dependent recombination is that in order to recombine the pair must be in the singlet state. Hyperfine fields acting on the electron and hole govern the spin-dynamics of localized pairs during the waiting time for recombination. We demonstrate that for certain domain of trapping configurations of hyperfine fields, crossover to the singlet state is quenched. This leads to the blocking of current. The phenomenon of organic magnetoresistance (OMAR) is described by counting the weights of trapping configurations as a function of magnetic field. This explains the universality of the lineshapes of the OMAR curves. In finite samples incomplete averaging over the hyperfine fields gives rise to mesoscopic fluctuations of the current response. We also demonstrate that under the condition of magnetic resonance, new trapping configurations emerge. This leads to nontrivial evolution of current through the sample with microwave power.

When discussing spin-relaxation two questions can be asked: (a) How does the local spin polarization decay as a function of distance from the spin-polarized injector? (b) How does the injected spin decay as a function of time after spatial averaging? With regard to (a), we demonstrate that, while decaying exponentially on average, local spin-polarization exhibits giant fluctuations from point to point. Concerning (b), we find that for a spin-carrier which moves diffusively in low dimensions the decay is faster than a simple exponent. The underlying physics for both findings is that in describing spin evolution it is necessary to add up amplitudes for partial spin-rotations in hyperfine fields on different sites.

[1] This work was supported through MRSEC DMR-112125.

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