Room-temperature direct synthesis of semi-conductive PbS nanocrystal inks for optoelectronic applications.

Lead sulphide (PbS) nanocrystals (NCs) are promising materials for low-cost, high-performance optoelectronic devices. So far, PbS NCs have to be first synthesized with long-alkyl chain organic surface ligands and then be ligand-exchanged with shorter ligands (two-steps) to enable charge transport. However, the initial synthesis of insulated PbS NCs show no necessity and the ligand-exchange process is tedious and extravagant. Herein, we have developed a direct one-step, scalable synthetic method for iodide capped PbS (PbS-I) NC inks. The estimated cost for PbS-I NC inks is decreased to less than 6 $·g-1, compared with 16 $·g-1 for conventional methods. Furthermore, based on these PbS-I NCs, photodetector devices show a high detectivity of 1.4 × 1011 Jones and solar cells show an air-stable power conversion efficiency (PCE) up to 10%. This scalable and low-cost direct preparation of high-quality PbS-I NC inks may pave a path for the future commercialization of NC based optoelectronics.

Electroluminescence Generation in PbS Quantum Dot Light-Emitting Field-Effect Transistors with Solid-State Gating.

The application of light-emitting field-effect transistors (LEFET) is an elegant way of combining electrical switching and light emission in a single device architecture instead of two. This allows for a higher degree of miniaturization and integration in future optoelectronic applications. Here, we report on a LEFET based on lead sulfide quantum dots processed from solution. Our device shows state-of-the-art electronic behavior and emits near-infrared photons with a quantum yield exceeding 1% when cooled. We furthermore show how LEFETs can be used to simultaneously characterize the optical and electrical material properties on the same device and use this benefit to investigate the charge transport through the quantum dot film.

Electron Mobility of 24 cm2 V-1 s-1 in PbSe Colloidal-Quantum-Dot Superlattices.

Colloidal quantum dots (CQDs) are nanoscale building blocks for bottom-up fabrication of semiconducting solids with tailorable properties beyond the possibilities of bulk materials. Achieving ordered, macroscopic crystal-like assemblies has been in the focus of researchers for years, since it would allow exploitation of the quantum-confinement-based electronic properties with tunable dimensionality. Lead-chalcogenide CQDs show especially strong tendencies to self-organize into 2D superlattices with micrometer-scale order, making the array fabrication fairly simple. However, most studies concentrate on the fundamentals of the assembly process, and none have investigated the electronic properties and their dependence on the nanoscale structure induced by different ligands. Here, it is discussed how different chemical treatments on the initial superlattices affect the nanostructure, the optical, and the electronic-transport properties. Transistors with average two-terminal electron mobilities of 13 cm2 V-1 s-1 and contactless mobility of 24 cm2 V-1 s-1 are obtained for small-area superlattice field-effect transistors. Such mobility values are the highest reported for CQD devices wherein the quantum confinement is substantially present and are comparable to those reported for heavy sintering. The considerable mobility with the simultaneous preservation of the optical bandgap displays the vast potential of colloidal QD superlattices for optoelectronic applications.

High-Efficiency PbS Quantum-Dot Solar Cells with Greatly Simplified Fabrication Processing via "Solvent-Curing".

PbS quantum-dot (QD) solar cells are promising candidates for low-cost solution-processed photovoltaics. However, the device fabrication usually requires ten more times film deposition and rinsing steps, which is not ideal for scalable manufacturing. Here, a greatly simplified deposition processing is demonstrated by replacing methanol with acetonitrile (ACN) as the rinsing solvent. It is discovered that ACN can effectively "cure" the film cracks generated from the volume loss during the solid-state ligand-exchange process, which enables the deposition of thick and dense films with much fewer deposition steps. Meanwhile, due to the aprotic nature of ACN, fewer trap states can be introduced during the rinsing process. As a result, with only three deposition steps for the active layer, a CPVT-certified 11.21% power conversion efficiency is obtained, which is the highest efficiency ever reported for PbS QD solar cells employing a solid-state ligand-exchange process. More importantly, the simple film-deposition processing provides an opportunity for the future application of QDs in low-cost printing of optoelectronic devices.

Comparing Halide Ligands in PbS Colloidal Quantum Dots for Field-Effect Transistors and Solar Cells.

Capping colloidal quantum dots (CQDs) with atomic ligands is a powerful approach to tune their properties and improve the charge carrier transport in CQD solids. Efficient passivation of the CQD surface, which can be achieved with halide ligands, is crucial for application in optoelectronic devices. Heavier halides, i.e., I- and Br-, have been thoroughly studied as capping ligands in the last years, but passivation with fluoride ions has not received sufficient consideration. In this work, effective coating of PbS CQDs with fluoride ligands is demonstrated and compared to the results obtained with other halides. The electron mobility in field-effect transistors of PbS CQDs treated with different halides shows an increase with the size of the atomic ligand (from 3.9 × 10-4 cm2/(V s) for fluoride-treated to 2.1 × 10-2 cm2/(V s) for iodide-treated), whereas the hole mobility remains unchanged in the range between 1 × 10-5 cm2/(V s) and 10-4cm2/(V s). This leads to a relatively more pronounced p-type behavior of the fluoride- and chloride-treated films compared to the iodide-treated ones. Cl-- and F--capped PbS CQDs solids were then implemented as p-type layer in solar cells; these devices showed similar performance to those prepared with 1,2-ethanedithiol in the same function. The relatively stronger p-type character of the fluoride- and chloride-treated PbS CQD films broadens the utility of such materials in optoelectronic devices.

An All-Solution-Based Hybrid CMOS-Like Quantum Dot/Carbon Nanotube Inverter.

The development of low-cost, flexible electronic devices is subordinated to the advancement in solution-based and low-temperature-processable semiconducting materials, such as colloidal quantum dots (QDs) and single-walled carbon nanotubes (SWCNTs). Here, excellent compatibility of QDs and SWCNTs as a complementary pair of semiconducting materials for fabrication of high-performance complementary metal-oxide-semiconductor (CMOS)-like inverters is demonstrated. The n-type field effect transistors (FETs) based on I- capped PbS QDs (Vth = 0.2 V, on/off = 105 , SS-th = 114 mV dec-1 , µe = 0.22 cm2 V-1 s-1 ) and the p-type FETs with tailored parameters based on low-density random network of SWCNTs (Vth = -0.2 V, on/off > 105 , SS-th = 63 mV dec-1 , µh = 0.04 cm2 V-1 s-1 ) are integrated on the same substrate in order to obtain high-performance hybrid inverters. The inverters operate in the sub-1 V range (0.9 V) and have high gain (76 V/V), large maximum-equal-criteria noise margins (80%), and peak power consumption of 3 nW, in combination with low hysteresis (10 mV).

High gain hybrid graphene-organic semiconductor phototransistors.

Hybrid phototransistors of graphene and the organic semiconductor poly(3-hexylthiophene-2,5-diyl) (P3HT) are presented. Two types of phototransistors are demonstrated with a charge carrier transit time that differs by more than 6 orders of magnitude. High transit time devices are fabricated using a photoresist-free recipe to create large-area graphene transistors made out of graphene grown by chemical vapor deposition. Low transit time devices are fabricated out of mechanically exfoliated graphene on top of mechanically exfoliated hexagonal boron nitride using standard e-beam lithography. Responsivities exceeding 10(5) A/W are obtained for the low transit time devices.