Solution-Deposited Organic–Inorganic Hybrid Multilayer Gate Dielectrics. Design, Synthesis, Microstructures, and Electrical Properties with Thin-Film Transistors

Abstract

We report here on the rational synthesis, processing, and dielectric properties of novel layer-by-layer organic/inorganic hybrid multilayer dielectric films enabled by polarizable π-electron phosphonic acid building blocks and ultrathin ZrO(2) layers. These new zirconia-based self-assembled nanodielectric (Zr-SAND) films (5-12 nm thick) are readily fabricated via solution processes under ambient atmosphere. Attractive Zr-SAND properties include amenability to accurate control of film thickness, large-area uniformity, well-defined nanostructure, exceptionally large electrical capacitance (up to 750 nF/cm(2)), excellent insulating properties (leakage current densities as low as 10(-7) A/cm(2)), and excellent thermal stability. Thin-film transistors (TFTs) fabricated with pentacene and PDIF-CN(2) as representative organic semiconductors and zinc-tin-oxide (Zn-Sn-O) as a representative inorganic semiconductor function well at low voltages (<±4.0 V). Furthermore, the TFT performance parameters of representative organic semiconductors deposited on Zr-SAND films, functionalized on the surface with various alkylphosphonic acid self-assembled monolayers, are investigated and shown to correlate closely with the alkylphosphonic acid chain dimensions.

Forming nanomaterials as layered functional structures toward materials nanoarchitectonics

“…They expect that a rational combination of the luminescent property of polyoxometalate clusters with the electric response of reduced graphene oxide films could lead to logic-gate devices with dual optical and electrical output functions. Ha et al 44 demonstrated preparation of self-assembled nanodielectrics with alternate structures of organic and inorganic layers, where polarizable, phosphonic acid-functionalized organic precursors and ultrathin layers of high-k inorganic oxide materials were used ( Figure 10). The ultrathin dielectric materials obtained were adherent, insulating, high-capacitance and thermally stable.…”

Molecular Motions in Functional Self-Assembled Nanostructures

“…Ever since the pioneering studies in 1993 [124,125], organic-inorganic mono- and multilayer films gained significant attention for their tunable thicknesses, processing ease and insulating properties leading to their integration in organic transistors [6,7,44,126,127]. Especially, recently developed self-assembled nanodielectrics (SANDs) were found to exhibit promising properties for a variety of opto-electronic applications, including thin-film transistors (TFTs) (Figure 6) [7,126–128].…”

A Ladder-Type Organosilicate Copolymer Gate Dielectric Materials for Organic Thin-Film Transistors

“…To this end, many studies on the development and application of new dielectric materials with low leakage current, high dielectric constant, and facile process have been reported [39][40][41][42][43][44][45][46][47][48]. Among them, organic-inorganic hybrid dielectrics might synergistically combine the advantages of both materials, i.e., the excellent mechanical and electrical properties of inorganics and the flexibility and large area solution processibility of organics [41][42][43][44].…”

“…Among them, organic-inorganic hybrid dielectrics might synergistically combine the advantages of both materials, i.e., the excellent mechanical and electrical properties of inorganics and the flexibility and large area solution processibility of organics [41][42][43][44]. One of the representative examples is organosilicate materials, a type of silica containing organic groups.…”