We exploited the thermal annealing of poly(3-hexylthiophene) (P3HT) molecularly p-doped with the strong electron acceptor 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ) as a tool for tuning the doping concentration as a quasi singular parameter. Via directed dopant desorption, we could unravel the complex microstructure of this semicrystalline system, leading to a detailed growth model solely based on complementary experimental evidence from scattering and spectroscopic techniques. We find the crystalline portion of p-doped P3HT to comprise regions, where dopant anions pack with the polymer chains in a metastable, cocrystalline structure with additional ionized dopants dispersed in the alkyl chain region of P3HT. Simultaneously, regions exist where the pristine polymer backbones closely pack. The dedoping via dopant desorption through thermal annealing reveals the dopants within the mixed crystalline phase to be thermally least stable. Notably, their initial desorption does not alter the thin film conductivity, which indicates this phase to be not crucial for charge transport. Upon further dopant desorption, the pristine P3HT backbone phase prevails with dopant anions remaining still dispersed in the alkyl chain region of the film. During the entire dedoping, we did not observe indications for the presence of neutral F4TCNQ. Only upon completing the dedoping at 120 °C are both the conductivity and the microstructure of pristine P3HT recovered. We demonstrate that the temperature-induced dedoping provides valuable information on the microstructure of doped organic semiconductors, which remains inaccessible otherwise because of the intrinsic structural and energetic complexity of such systems.
The advent of two-dimensional materials has opened a plethora of opportunities in accessing ultrascaled device dimensions for future logic and memory applications. In this work, we demonstrate that a single layer of large-area chemical vapor deposition-grown molybdenum disulfide (MoS2) sandwiched between two metal electrodes can be tuned to show multilevel nonvolatile resistive memory states with resistance values separated by 5 orders of magnitude. The switching process is unipolar and thermochemically driven requiring significant Joule heating in the reset process. Temperature-dependent electrical measurements coupled with semiclassical charge transport models suggest that the transport in these devices varies significantly in the initial (pristine) state, high resistance state, and low resistance state. In the initial state, the transport is a one-step direct tunneling (at low voltage biases) and Fowler Nordeim tunneling (at higher bias) with an effective barrier height of 0.33 eV, which closely matches the Schottky barrier at the MoS2/Au interface. In the high resistive state, trap-assisted tunneling provides a reasonable fit to experimental data for a trap height of 0.82 eV. Density functional theory calculations suggest the possibility of single- and double-sulfur vacancies as the microscopic origins of these trap sites. The temperature-dependent behavior of the set and reset process are explained by invoking the probability of defect (sulfur vacancy) creation and mobility of sulfur ions. Finally, conductive atomic force microscopy measurements confirm that the multifilamentary resistive memory effects are inherent to a single-crystalline MoS2 triangle and not necessarily dependent on grain boundaries. The insights suggested in this work are envisioned to open up possibilities for ultrascaled, multistate, resistive memories for next-generation digital memory and neuromorphic applications.
In this work a technology to fabricate low-voltage amorphous gallium-indium-zinc oxide thin film transistors ͑TFTs͒ based integrated circuits on 25 m foils is presented. High performance TFTs were fabricated at low processing temperatures ͑Ͻ150°C͒ with field effect mobility around 17 cm 2 / V s. The technology is demonstrated with circuit building blocks relevant for radio frequency identification applications such as high-frequency functional code generators and efficient rectifiers. The integration level is about 300 transistors.
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