High Performance PbS Quantum Dot/Graphene Hybrid Solar Cell with Efficient Charge Extraction.

Hybrid colloidal quantum dot (CQD) solar cells are fabricated from multilayer stacks of lead sulfide (PbS) CQD and single layer graphene (SG). The inclusion of graphene interlayers is shown to increase power conversion efficiency by 9.18%. It is shown that the inclusion of conductive graphene enhances charge extraction in devices. Photoluminescence shows that graphene quenches emission from the quantum dot suggesting spontaneous charge transfer to graphene. CQD photodetectors exhibit increased photoresponse and improved transport properties. We propose that the CQD/SG hybrid structure is a route to make CQD thin films with improved charge extraction, therefore resulting in improved solar cell efficiency

Chemically triggered formation of two-dimensional epitaxial quantum dot superlattices

Two dimensional superlattices of epitaxially connected quantum dots enable size-quantization effects to be combined with high charge carrier mobilities, an essential prerequisite for highly performing QD devices based on charge transport. Here, we demonstrate that surface active additives known to restore nanocrystal stoichiometry can trigger the formation of epitaxial superlattices of PbSe and PbS quantum dots. More specifically, we show that both chalcogen-adding (sodium sulfide) and lead oleate displacing (amines) additives induce small area epitaxial superlattices of PbSe quantum dots. In the latter case, the amine basicity is a sensitive handle to tune the superlattice symmetry, with strong and weak bases yielding pseudohexagonal or quasi-square lattices, respectively. Through density functional theory calculations and in situ titrations monitored by nuclear magnetic resonance spectroscopy, we link this observation to the concomitantly different coordination enthalpy and ligand displacement potency of the amine. Next to that, an initial similar to 10% reduction of the initial ligand density prior to monolayer formation and addition of a mild, lead oleate displacing chemical trigger such as aniline proved key to induce square superlattices with long-range, square micrometer order; an effect that is the more pronounced the larger the quantum dots. Because the approach applies to PbS quantum dots as well, we conclude that it offers a reproducible and rational method for the formation of highly ordered epitaxial quantum dot superlattices

Reduction of moisture sensitivity of PbS quantum dot solar cells by incorporation of reduced graphene oxide

PbS nanocrystals are an important narrow-gap material for solar cells and photodetectors. Nevertheless, their application may be limited because device performance can be affected by atmospheric conditions. Indeed, the presence of oxygen and/or water can degrade the active layers, possibly leading to device failure. Strategies to address this issue are therefore actively explored. Here we report a solution-processed PbS quantum dot solar cell, consisting of a PbS-silane functionalized reduced graphene oxide (PbS-rGO) layer on top of the PbS absorber film, which enhances device stability, especially when the solar cells are exposed to moisture. Power conversion efficiency (PCE) measurements demonstrate a slower degradation under continuous illumination for solar cells with PbS-rGO. When storing the samples under saturated water vapor, differences are even more remarkable: with PbS-rGO the solar cells essentially maintain their initial PCE, while the PCE of the PbS reference devices is reduced by 50% after 5 days. Scanning electron microscopy, energy dispersive X-ray and X-ray photoelectron spectroscopy reveal the damage to the PbS films and the formation of PbSOX crystals in the PbS reference devices. Such crystals are not observed in the PbS-rGO devices, further supporting the importance of the PbSrGO barrier layer

High Efficiency Colloidal Quantum Dot Infrared Light Emitting Diodes via Engineering at the Supra-Nanocrystalline Level

Colloidal quantum dot (CQD) light-emitting diodes (LEDs) deliver a compelling performance in the visible, yet infrared CQD LEDs underperform their visible-emitting counterparts, largely due to their low photoluminescence quantum efficiency. Here we employ a ternary blend of CQD thin film that comprises a binary host matrix that serves to electronically passivate as well as to cater for an efficient and balanced carrier supply to the emitting quantum dot species. In doing so, we report infrared PbS CQD LEDs with an external quantum efficiency of ~7.9% and a power conversion efficiency of ~9.3%, thanks to their very low density of trap states, on the order of 1014 cm−3, and very high photoluminescence quantum efficiency in electrically conductive quantum dot solids of more than 60%. When these blend devices operate as solar cells they deliver an open circuit voltage that approaches their radiative limit thanks to the synergistic effect of the reduced trap-state density and the density of state modification in the nanocomposite.Peer ReviewedPostprint (author's final draft

Plasmonic light trapping leads to responsivity increase in colloidal quantum dot photodetectors

We report broadband responsivity enhancement in PbS colloidal quantum dot (CQDs) photoconductive photodetectors due to absorption increase offered by a plasmonic scattering layer of Ag metal nanoparticles. Responsivity enhancements are observed in the near infrared with a maximum 2.4-fold increase near the absorption band edge of 1 lm for 400 nm thick devices. Additionally, we study the effect of the mode structure on the efficiency of light trapping provided by random nanoparticle scattering in CQD films and provide insights for plasmonic scattering enhancement in CQD thin films.This research has been partially supported by Fundacio´ Privada Cellex Barcelona. We also acknowledge support from European Commission’s Seventh Framework Programme for Research under contract PIRG06-GA-2009-256355

Reducing charge trapping in PbS colloidal quantum dot solids

Understanding and improving charge transport in colloidal quantum dot solids is crucial for the development of efficient solar cells based on these materials. In this paper, we report high performance field-effect transistors based on lead-sulfide colloidal quantum dots (PbS CQDs) crosslinked with 3-mercaptopropionic acid (MPA). Electron mobility up to 0.03 cm(2)/Vs and on/off ratio above 10(5) was measured; the later value is the highest in the literature for CQD Field effect transistors with silicon-oxide gating. This was achieved by using high quality material and preventing trap generation during fabrication and measurement. We show that air exposure has a reversible p-type doping effect on the devices, and that intrinsically MPA is an n-type dopant for PbS CQDs. (C) 2014 AIP Publishing LLC

Interdot Lead Halide Excess Management in PbS Quantum Dot Solar Cells

Light-harvesting devices made from lead sulfide quantum dot (QD) absorbers are one of the many promising technologies of third-generation photovoltaics. Their simple, solution-based fabrication, together with a highly tunable and broad light absorption makes their application in newly developed solar cells, particularly promising. In order to yield devices with reduced voltage and current losses, PbS QDs need to have strategically passivated surfaces, most commonly achieved through lead iodide and bromide passivation. The interdot spacing is then predominantly filled with residual amorphous lead halide species that remain from the ligand exchange, thus hindering efficient charge transport and reducing device stability. Herein, it is demonstrated that a post-treatment by iodide-based 2-phenylethlyammonium salts and intermediate 2D perovskite formation can be used to manage the lead halide excess in the PbS QD active layer. This treatment results in improved device performance and increased shelf-life stability, demonstrating the importance of interdot spacing management in PbS QD photovoltaics