From oxide surface to organic transistor properties: the nature and the role of oxide gate surface defects

By applying various surface treatments to the oxide gate of pentacene transistors, both in vacuum (H2, O2 and Ar plasma treatments) and in aqueous solution, we were able to vary the balance between oxygen-free radicals (Si•), oxygen-centered radicals (Si−O• and Si−O−O•), and other defect types such as silanol (Si−OH), silicon hydride (Si−H), and silicate groups (Si−O−). The consequences of these modifications on the microstructure of pentacene deposited onto the gate have been studied by contact angle measurements and atomic force microscopy. The changes in the transport properties of the ultrathin devices were deduced from their electrical characteristics and from independent four-probe measurements. While the wetting properties of the oxide and in turn the pentacene growth process is mainly controlled by the Si−OH/Si−O− balance, it has been evidenced that oxygen-centered radicals act as charge transfer centers and determine to a large extent the transport properties of many thin-film transistors.

Transistors organiques ultraminces à base de pentacène

Adrian von Mühlenen

The goal of this thesis is to contribute to the understanding of charge transport in organic field-effect transistors (OFETs) made of pentacene. Organic thin-film transistors (OTFTs) with active layers thicknesses of 5, 10, 20, and 100 nm were fabricated in order to examine their structure and electrical characteristics and identify the key parameters that affect the charge transport in these devices. The conductivity of the pentacene films determined via four probe measurements suggests the presence of extrinsic charge carriers, or residual carriers, which have a large influence on device performance and electrical characteristics. The origin of these carriers is discussed in terms of a charge-transfer process occurring between the organic semiconductor and the electron acceptor states of the gate oxide surface. The gate interface is studied by varying the density of residual carriers via modification of the oxide surface by different plasma treatments with or without using subsequent deposition of various molecular monolayers. The OFETs yielded residual carrier densities ranging from 5 × 109 et 1 × 1013 cm-2 depending on the gate interface modification. The electrical characteristics such as the film conductivity and field-effect mobility are shown to be dependent on the density of residual carriers. Based on the measured density of residual carriers the OFETs are classified into two groups : devices based on doped and on un-doped pentacene. Temperature-dependent measurements of the field-effect mobility and the film conductivity performed on these devices reveal a thermally-activated character. This suggests that charge transport in the examined devices occurs via hopping between localized states. Based on the activation energies of the film conductivity and the field-effect mobility, the difference in energy between the Fermi and the transport level Δε is estimated to be between 10 and 160 meV depending on the density of residual carriers. This range of values is in agreement with thermoelectric power measurements performed on the same devices. The thermoelectric power is discussed in terms of two contributions : one that is dependent on Δε and another constant term that is independent of temperature and gate interface modification. The latter contribution was measured to be 265 ± 40 μV/K and originates from the creation of the phonon cloud associated with local changes in intermolecular interaction. This suggests that the charge carrier in the channel is dressed with a cloud of polarization, an electronic polaron.

EPFL2007

The Effect of Interface Modification on the Properties of Organic Thin-Film Transistors

Franziska Dora Fleischli

In organic thin-film transistors (OTFTs), the conducting channel is located near the interface between the organic semiconductor and the dielectric; this interface is crucial for transistor performance. The goal of this thesis is to study the effect of this interface, especially when it is modified either by surface treatments or self-assembled monolayers. For this purpose, OTFTs based on pentacene and doped silicon wafer gate electrode and gold top contacts are fabricated. The dielectric is either silicon oxide (SiO2) or polyimide (PI). The dielectric surface affects both the growth of the pentacene film on the top of it and the electric performance of the transistor. The pentacene film morphology is studied on treated and untreated SiO2 and PI surfaces by AFM and water contact angle measurements. Depending on the nature of the dielectric surface, traps or charge transfer centers are introduced which then affect the performance of the transistor. The transistor performance is determined by measuring the drain current as it is dependent upon the drain and gate voltage. The contributions of the channel and the contacts are separated by 4-probe measurements (at floating and non-floating gate). The transistors with untreated dielectrics are first characterized. The dependence on the channel length, the thickness and the morphology of the pentacene film is studied. The short channels (2 – 20 µm) are patterned by stencil masks; the long channels (100 – 600 µm) by steel masks. The results show that the transistors with a channel length of 20 µm and smaller are limited by the contacts, while the transistors with a channel length between 100 and 600 µm are dominated by the channel, and thus the traps and residual carriers in the channel. The pentacene film morphology has more influence on the contact resistance than on the channel behavior. To study the effect of the interface modifications, the transistor behavior should be dominated by the channel and the contact effects minimized; hence, long-channel transistors are used. The dielectric surfaces are treated by plasma or pH solutions prior to the pentacene deposition resulting in a variety of defects. The defects are distinguished by those which lead to a change in the film growth and those which affect the electric performance by introducing traps or charge transfer centers. To overcome the influence of the dielectric surface, the oxide dielectric is passivated by a self-assembled monolayer (SAM). The neutral SAM acts as a spacer between the dielectric and the pentacene film and thus enhances the transistor performance. The polar SAMs also introduce a dipole moment. A series of molecules with a similar length, but different end groups, are used to investigate the effect of the dipole moment. The main result of this study is that the nature and the quality of the gate and the contact interfaces are often more important for the performance of the transistors than the thin film morphology.

EPFL2010

Transistors organiques ultraminces à base de pentacène

Adrian von Mühlenen

EPFL2007

The Effect of Interface Modification on the Properties of Organic Thin-Film Transistors

Franziska Dora Fleischli

EPFL2010