Organic spintronic devices utilizing spin-injection, spin-tunneling and spin-dependent transport

Ran Lin

doi:10.17077/etd.xdxqvuz5

Spintronics, also known as spin electronics, or magnetoelectronics, refers to the study of the role that electron and (less frequently) nuclear spins play in solid state physics, and a group of devices that specifically exploit both the intrinsic spin of the electron and its associated magnetic moment, in addition to its fundamental electronic charge. As a principal type of spintronic device, a spin-valve is a device that uses ferromagnetic electrodes to polarize and analyze the electronic spins. The electrical resistance of the device depends sensitively on the relative magnetization of its two ferromagnetic electrodes, a phenomenon referred to as Giant Magnetoresistance (GMR). Having been successfully applied in the field of data storage, GMR also shows potential for future logic devices. Organic semiconductors possess many advantages in electronic device applications. Therefore, using organic semiconductors in spintronics is very interesting and promising, in part, because of their exceptionally long spin-decoherence times. This thesis concerns itself with the scientific study of magnetic field and spin effects in organic spin valves (OSV) and organic light emitting diodes (OLED). Three projects were finished, achieving a better understanding of the transportation of charge and spin carriers inside organic films, and paving the way to enhancing the spin diffusion length and the organic magnetoresistance (OMAR) effect. Firstly, C60 films were used as the spin-transport layer of OSV devices, because of its low hyperfine coupling and high mobility, which prior work suggested to be beneficial. Subsequently we studied the spin injection and transport properties by measuring the devices' magnetoresistance (MR) response at various biasing voltages, V, temperatures, T and different C60 film thickness. But we do not observe a significantly increased spin-diffusion length compared to OSV devices based on other organic semiconductors. We propose conductivity mismatch as a likely cause of the loss of spin-valve signal with increasing C60 layer thickness. There exists some disagreement in the scientific literature regarding whether OSV operate in the so-called tunneling regime or the so-called injection regime. To shed light on this question, we fabricated spin-valve devices made of organic semiconductor thin films of rubrene sandwiched between ferromagnetic cobalt and iron electrodes. Current-voltage (I-V) characteristics in Co/AlOx/rubrene/Fe junctions with a rubrene layer thickness, d, ranging from 5-50 nm, were measured, and we found two different modes of conductivity. The first mode, tunneling, occurs in relatively thin junctions, d < 15 nm, and decays exponentially with increasing rubrene thickness. We determined the tunneling decay length to be 1 nm. The tunneling mode is also characterized by a weak temperature dependence and a nearly parabolic differential conductance. The second mode, injection followed by hopping, occurs in relatively thick devices, d ≥ 15 nm, and can be identified by strongly temperature dependent, highly non-linear I-V traces that are similar to those commonly measured in organic injection devices such as OLEDs. We observed MR in devices with a rubrene thickness of 5 nm and 10 nm. Those devices are clearly in the tunneling regime. For the 15 nm device, for which the tunneling current is just barely measurable we could not observe MR. In the third project, we show that the performance of both OMAR and OSV devices very sensitively depends on whether the metallic layers are deposited by thermal evaporation or electron-beam evaporation. A strongly reduced spin diffusion length and an enhanced OMAR response can be achieved in devices fabricated by electron-beam evaporation. Then we showed that the difference must be attributed to the generation of traps resulting from the exposure of the organic layer to X-ray bremsstrahlung that is generated during the e-beam evaporation process. We also used the thermally stimulated current technique (TSC) to characterize these traps.

Organic spintronic devices utilizing spin-injection, spin-tunneling and spin-dependent transport

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