Abstract

Assemblies of colloidal quantum dots (CQDs) are attractive for a broad range of applications because of the ability to exploit the quantum confinement effect and the large surface-to-volume ratio due to their small dimensions. Each application requires different types of assemblies based on which properties are intended to be utilized. Greater control of assembly formation and optimization of the related carrier transport characteristics are vital to advance the utilization of these materials. Here, we demonstrate on-demand control of the assembly morphology and electrical properties of highly crosslinked CQD solids through the augmentation of various assembly methods. Employment of electric-double-layer (EDL) gating on these assembly structures (i.e., an amorphous assembly, a hierarchical porous assembly, and a compact superlattice assembly) reveals their intrinsic carrier transport and accumulation characteristics. Demonstrations of high electron mobility with a high current modulation ratio reaching 105 in compact QD films and of a record-high areal capacitance of 400 μF/cm2 in an electric-double-layer supercapacitor with very thin (<100 nm) QD hierarchical porous assemblies signify the versatility of CQDs as building blocks for various modern electronic devices.

Highlights

  • Colloidal quantum dot (CQD) solids render flexible and low cost solution-processed materials with unique sizedependent properties

  • In summary, we have demonstrated a strong relationship of the QD assembly morphology with the electrical properties

  • Different deposition techniques can generate various QD assembly structures, as shown for the spincoating, dip-coating, and liquid/air interfacial assembly methods, which provided us with a variety of assemblies: amorphous-like, hierarchical porous, and compact wellordered assembly structures

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Summary

Introduction

Colloidal quantum dot (CQD) solids render flexible and low cost solution-processed materials with unique sizedependent properties. The small size of the individual constituent QDs leads to the quantum confinement effect of the carrier wavefunction, which is reflected in the size dependency of the electronic band gaps and the formation of discrete energy levels[1]. These CQDs have a sizeable surface-to-volume ratio. Each device requires different types of nanocrystal assemblies based on which the merits will be exploited. The assembly requirements for devices that need high electronic coupling between the QDs can be significantly different from those that require high accumulated charge carrier density

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