Synthetic methods produce libraries of colloidal nanocrystals with tunable physical properties by tailoring the nanocrystal size, shape, and composition. Here, we exploit colloidal nanocrystal diversity and design the materials, interfaces, and processes to construct all-nanocrystal electronic devices using solution-based processes. Metallic silver and semiconducting cadmium selenide nanocrystals are deposited to form high-conductivity and high-mobility thin-film electrodes and channel layers of field-effect transistors. Insulating aluminum oxide nanocrystals are assembled layer by layer with polyelectrolytes to form high-dielectric constant gate insulator layers for low-voltage device operation. Metallic indium nanocrystals are codispersed with silver nanocrystals to integrate an indium supply in the deposited electrodes that serves to passivate and dope the cadmium selenide nanocrystal channel layer. We fabricate all-nanocrystal field-effect transistors on flexible plastics with electron mobilities of 21.7 square centimeters per volt-second.

Integration of graphene into macroscopic architectures represents the first step toward creating a new class of graphene-based nanodevices. We report a novel yet simple approach to fabricate graphene fibers, a porous and monolithic macrostructure, from chemical vapor deposition grown graphene films. Graphene is first self-assembled from a 2D film to a 1D fiberlike structure in an organic solvent (e.g., ethanol, acetone) and then dried to give the porous and crumpled structure. The method developed here is scalable and controllable, delivering tunable morphology and pore structure by controlling the evaporation of solvents with suitable surface tension. The fibers are 20-50 μm thick, with a typical electrical conductivity of ∼1000 S/m. The cyclic voltammetric studies show typical capacitive behavior for the porous graphene fibers with good rate stability and capacitance values ranging from 0.6 to 1.4 mF/cm(2). Decorated with only 1-3 wt % MnO(2), the graphene/MnO(2) composites exhibit remarkable enhancement of combined performance both with respect to discharge capacitance (up to 12.4 mF/cm(2)) and cycling stability. This special structure could facilitate chemical doping and electrochemical energy storage and find applications in catalyst supports, sensors, supercapacitors, Li ion batteries, etc.

We study charge injection and transport in PbSe nanocrystal thin films. By engineering the contact metallurgy and nanocrystal ligand exchange chemistry and surface passivation, we demonstrate partial Fermi-level pinning at the metal-nanocrystal interface and an insulator-to-metal transition with increased coupling and doping, allowing us to design high conductivity and mobility PbSe nanocrystal films. We construct complementary nanocrystal circuits from n-type and p-type transistors realized from a single nanocrystal material by selecting the contact metallurgy.

The synthesis of colloidal III–V quantum dots (QDs), particularly of the arsenides and antimonides, has been limited by the lack of stable and available group V precursors. In this work, we exploit accessible InCl3- and pnictogen chloride-oleylamine as precursors to synthesize III–V QDs. Through coreduction reactions of the precursors, we achieve size- and stoichiometry-tunable binary InAs and InSb as well as ternary alloy InAs1–x Sb x QDs. On the basis of structural, analytical, optical, and electrical characterization of the QDs and their thin-film assemblies, we study the effects of alloying on their particle formation and optoelectronic properties. We introduce a hydrazine-free hybrid ligand-exchange process to improve carrier transport in III–V QD thin films and realize InAs QD field-effect transistors with electron mobility > 5 cm2/(V s). We demonstrate that III–V QD thin films are promising candidate materials for infrared devices and show InAs1–x Sb x QD photoconductors with superior short-wavelength infrared (SWIR) photoresponse than those of the binary QD devices.

Flexible all-solid-state supercapacitors based on graphene fibers are demonstrated in this study. Surface-deposited oxide nanoparticles are used as pseudo-capacitor electrodes to achieve high capacitance. This supercapacitor electrode has an areal capacitance of 42 mF cm(-2), which is comparable to the capacitance for fiber-based supercapacitors reported to date. During the bending and cycling of the fiber-based supercapacitor, the stability could be maintained without sacrificing the electrochemical performance, which provides a novel and simple way to develop flexible, lightweight and efficient graphene-based devices.