Highly versatile near-infrared emitters based on an atomically defined HgS interlayer embedded into a CdSe/CdS quantum dot.

The availability of colloidal quantum dots with highly efficient, fast and 'non-blinking' near-infrared emission would benefit numerous applications, from advanced optical communication and quantum networks to biomedical diagnostics. Here, we report high-quality near-infrared emitters that are based on well known CdSe/CdS heterostructures. By incorporating an HgS interlayer at the quantum dot core/shell interface, we convert normally visible emitters into highly efficient near-infrared fluorophores. Employing thermodynamically controlled sequential deposition of metal and chalcogen ions, we achieve atomic-level precision in defining the thickness of the HgS interlayer (H). This manifests in 'quantized' jumps of the photoluminescence spectrum when H changes in discrete, atomic steps. The synthesized structures show highly efficient photoluminescence, tunable from 700 to 1,370 nm, and fast radiative rates of ~1/60 ns-1. The emission from individual CdSe/HgS/CdS colloidal quantum dots is virtually blinking free and exhibits nearly perfect single-photon purity. In addition, when incorporated into a light-emitting-diode architecture, these quantum dots demonstrate strong electroluminescence with a sub-bandgap turn-on voltage.

High-Performance Ultra-Short Channel Field-Effect Transistor Using Solution-Processable Colloidal Nanocrystals.

We demonstrate high-mobility solution-processed inorganic field-effect transistors (FETs) with ultra-short channel (USC) length using semiconductor CdSe nanocrystals (NCs). Capping of the NCs with hybrid inorganic-organic CdCl3--butylamine ligands enables coarsening of the NCs during annealing at a moderate temperature, resulting in the devices having good transport characteristics with electron mobilities in the saturation regime reaching 8 cm2 V-1 s-1. Solution-based processing of the NCs and fabrication of thin films involve neither harsh conditions nor the use of hydrazine. Employing photolithographic methods, we fabricated FETs with a vertical overlap of source and drain electrodes to achieve a submicrometer channel length. To the best of our knowledge, this is the first report on an USC FET based on colloidal semiconductor NCs. Because of a short channel length, the FETs show a normalized transconductance of 4.2 m V-1 s-1 with a high on/off ratio of 105.

Emerging Hierarchical Aerogels: Self-Assembly of Metal and Semiconductor Nanocrystals.

Aerogels assembled from colloidal metal or semiconductor nanocrystals (NCs) feature large surface area, ultralow density, and high porosity, thus rendering them attractive in various applications, such as catalysis, sensors, energy storage, and electronic devices. Morphological and structural modification of the aerogel backbones while maintaining the aerogel properties enables a second stage of the aerogel research, which is defined as hierarchical aerogels. Different from the conventional aerogels with nanowire-like backbones, those hierarchical aerogels are generally comprised of at least two levels of architectures, i.e., an interconnected porous structure on the macroscale and a specially designed configuration at local backbones at the nanoscale. This combination "locks in" the inherent properties of the NCs, so that the beneficial genes obtained by nanoengineering are retained in the resulting monolithic hierarchical aerogels. Herein, groundbreaking advances in the design, synthesis, and physicochemical properties of the hierarchical aerogels are reviewed and organized in three sections: i) pure metallic hierarchical aerogels, ii) semiconductor hierarchical aerogels, and iii) metal/semiconductor hybrid hierarchical aerogels. This report aims to define and demonstrate the concept, potential, and challenges of the hierarchical aerogels, thereby providing a perspective on the further development of these materials.

Transfer of Inorganic-Capped Nanocrystals into Aqueous Media.

We report on a novel and simple approach to surface ligand design of CdSe-based nanocrystals (NCs) with biocompatible, heterobifunctional polyethylene glycol (PEG) molecules. This method provides high transfer yields of the NCs into aqueous media with preservation of the narrow and symmetric emission bands of the initial organic-capped NCs regardless of their interior crystal structure and surface chemistry. The PEG-functionalized NCs show small sizes, high photoluminescence quantum yields of up to 75%, as well as impressive optical and colloidal stability. This universal approach is applied to different fluorescent nanomaterials (CdSe/CdS, CdSe/CdSCdxZn1-xS, and CdSe/CdS/ZnS), extending the great potential of organic-capped NCs for biological applications.

Hybrid N-Butylamine-Based Ligands for Switching the Colloidal Solubility and Regimentation of Inorganic-Capped Nanocrystals.

We report on a simple and effective technique of tuning the colloidal solubility of inorganic-capped CdSe and CdSe/CdS core/shell nanocrystals (NCs) from highly polar to nonpolar media using n-butylamine molecules. The introduction of the short and volatile organic amine mainly results in a modification of the labile diffusion region of the inorganic-capped NCs, enabling a significant extension of their dispersibility and improving the ability to form long-range assemblies. Moreover, the hybrid n-butylamine/inorganic capping can be thermally decomposed under mild heat treatment, making this approach of surface functionalization well-compatible with a low-temperature, solution-processed device fabrication. Particularly, a field-effect transistor-based on n-butylamine/Ga-I-complex-capped 4.5 nm CdSe NC solids shows excellent transport characteristics with electron mobilities up to 2 cm2/(V·s) and a high current modulation value (>104) at a low operation voltage (<2 V).

3D Assembly of All-Inorganic Colloidal Nanocrystals into Gels and Aerogels.

We report an efficient approach to assemble a variety of electrostatically stabilized all-inorganic semiconductor nanocrystals (NCs) by their linking with appropriate ions into multibranched gel networks. These all-inorganic non-ordered 3D assemblies benefit from strong interparticle coupling, which facilitates charge transport between the NCs with diverse morphologies, compositions, sizes, and functional capping ligands. Moreover, the resulting dry gels (aerogels) are highly porous monolithic structures, which preserve the quantum confinement of their building blocks. The inorganic semiconductor aerogel made of 4.5 nm CdSe colloidal NCs capped with I(-) ions and bridged with Cd(2+) ions had a large surface area of 146 m(2) g(-1) .