Date of Award

Winter 2006

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Micro and Nanoscale Systems

First Advisor

Yi Su

Abstract

In this study, resistor-type, diode-type, and transistor-type organic memory devices were investigated, aiming at the low-cost plastic integrated circuit applications. A series of solution-processing techniques including spin-coating, inkjet printing, and self-assembly were employed to fabricate these devices.

The organic resistive memory device is based on a novel molecular complex film composed of tetracyanoquinodimethane (TCNQ) and a soluble methanofullerene derivative [6,6]-phenyl C61-butyric acid methyl ester (PCBM). It has an Al/molecules/Al sandwich structure. The molecular layer was formed by spin-coating technique instead of expensive vacuum deposition method. The current-voltage characteristics show that the device switches from the initial 'low' conduction state to 'high' conduction state upon application of external electric field at room temperature and return to 'low' conduction state when a high current pulse is applied. The on/off ratio is over 106. Each state has been found to remain stable for more than five months, even after the external electric field is removed. The PCBM nanodots wrapped by TCNQ molecules can form potential wells for charge trapping, and are believed to be responsible for the memory effects.

A rewritable diode memory device was achieved in an improved configuration, i.e., ITO-PEDOT:PSS-PCBM/TCNQ-Al, where a semiconductor polymer PEDOT:PSS is used to form p+-N heterojunction with PCBM/TCNQ. It exhibits a diode characteristic (low conductive) before switching to a high-conductive Poole-Frenkel regime upon applying a positive external bias to ITO. The on/off ratio at +1.0 V is up to 105. Simulation results from Taurus-Medici are in qualitative agreement with the experimental results and the proposed charge storage model.

The transistor-type memory device is fabricated on a heavily doped n-type silicon (n+-Si) substrate with a 100 nm thick thermally-grown oxide layer. The n+-Si serves as the gate electrode, while the oxide layer functions as the control gate dielectric. Gold nanoparticles as the charge storage units are deposited on the substrate by electrostatic self-assembly method. A self-assembled multilayer of polyelectrolytes, together with a thin spin-coated poly(4-vinyl phenol) layer, covers the gold nanoparticles and separates them from the poly(3-hexyl thiophene) channel. Conducting polymer PEDOT:PSS is inkjet printed to form the source/drain electrodes. The device exhibits significant hysteresis behavior in its Ids-Vgs characteristics. The charge storage in gold nanodots (diameter = 16 nm) was confirmed by comparing with devices having no gold nanoparticles, although the effects of interfacial traps may be also significant. The data retention time of the transistor memory is about 60 seconds, which needs to be further improved. It appears that this is the first demonstration of memory effects in an organic transistor caused by charge storage in metal nanodots in the gate dielectric. Therefore, the approach reported in this work offers a new direction to make low-cost organic transistor memories.

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