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Pietryga, Jeffrey Michael

Publications and source records attributed to Pietryga, Jeffrey Michael.

PbE (E = S, Se) Colloidal Quantum Dot-Layered 2D Material Hybrid Photodetectors

Hybrid lead chalcogenide (PbE) (E = S, Se) quantum dot (QD)-layered 2D systems are an emerging class of photodetectors with unique potential to expand the range of current technologies and easily integrate into current complementary metal-oxide-semiconductor (CMOS)-compatible architectures. Herein, we review recent advancements in hybrid PbE QD-layered 2D photodetectors and place them in the context of key findings from studies of charge transport in layered 2D materials and QD films that provide lessons to be applied to the hybrid system. Photodetectors utilizing a range of layered 2D materials including graphene and transition metal dichalcogenides sensitized with PbE QDs in various device architectures are presented. Figures of merit such as responsivity (R) and detectivity (D*) are reviewed for a multitude of devices in order to compare detector performance. Finally, a look to the future considers possible avenues for future device development, including potential new materials and device treatment/fabrication options.

36 MATERIALS SCIENCE↗

Cubic SnGe nanoalloys: beyond thermodynamic composition limit

A general synthetic route is reported leading to cubic phase Sn x Ge 1-x alloy nanocrystals with a composition varying from essentially pure Ge to 95% Sn. Overcoating of alloys with a sulfide layer increases their thermal stability to 500 °C and makes the alloy nanocrystals amenable to easy ligand exchange.

36 MATERIALS SCIENCE↗

The role of surface ligands in quantum-dot devices: Villain or unsung hero?

For over three decades, the study of nanocrystal quantum dots (QDs), which are solution-synthesized nanometer-scale bits of semiconductor materials, has produced singular advances in both our understanding of quantum confinement effects, and in our ability to make use of them in tech-relevant materials. Accordingly, QDs have found their way into the marketplace, specifically as high-performance fluorophores for, e.g., displays and biolabeling. In such applications, optimization of the QD surface, including the passivating ligands, is key to keeping photo-excited carriers from leaving the QD interior before recombining, resulting in a high fluorescence efficiency. Increasingly, attention has turned to realize the promise of QDs for optoelectronic applications (e.g., solar cells, LEDs, sensors) which require charge carriers to controllably enter, exit and/or travel through QDs, a much more challenging problem. In this scenario, the role of the QD surface must be completely reimagined, from being an impenetrable wall to being a gateway, or even a ramp. In this talk, I’ll explore the inherent contrast between QD fluorophore and device applications, and describe how ligands, originally thought only to be impediments to QD electronic devices, may actually give the savvy QD device designer control over function and performance in a manner unknown in bulk semiconductor devices. Finally, I’ll survey recent efforts at Los Alamos to develop a universal tool box for deposition of conductive QD films that may finally allow the manufacturing of economical, high-performance devices for a wide range of applications.

36 MATERIALS SCIENCE↗

Phase-Transfer Ligand Exchange of Lead Chalcogenide Quantum Dots for Direct Deposition of Thick, Highly Conductive Films

Here, the use of semiconductor nanocrystal quantum dots (QDs) in optoelectronic devices typically requires postsynthetic chemical surface treatments to enhance electronic coupling between QDs and allow for efficient charge transport in QD films. Despite their importance in solar cells and infrared (IR) light-emitting diodes and photodetectors, advances in these chemical treatments for lead chalcogenide (PbE; E = S, Se, Te) QDs have lagged behind those of, for instance, II–VI semiconductor QDs. Here, we introduce a method for fast and effective ligand exchange for PbE QDs in solution, resulting in QDs completely passivated by a wide range of small anionic ligands. Due to electrostatic stabilization, these QDs are readily dispersible in polar solvents, in which they form highly concentrated solutions that remain stable for months. QDs of all three Pb chalcogenides retain their photoluminescence, allowing for a detailed study of the effect of the surface ionic double layer on electronic passivation of QD surfaces, which we find can be explained using the hard/soft acid–base theory. Importantly, we prepare highly conductive films of PbS, PbSe, and PbTe QDs by directly casting from solution without further chemical treatment, as determined by field-effect transistor measurements. This method allows for precise control over the surface chemistry, and therefore the transport properties of deposited films. It also permits single-step deposition of films of unprecedented thickness via continuous processing techniques, as we demonstrate by preparing a dense, smooth, 5.3-μm-thick PbSe QD film via doctor-blading. As such, it offers important advantages over laborious layer-by-layer methods for solar cells and photodetectors, while opening the door to new possibilities in ionizing-radiation detectors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Engineered core/shell quantum dots as phosphors for solid-state lighting

Light-emitting diodes (LEDs) for solid state light ing (SSL) typically combine a blue or near- ultraviolet drive LED with one or more dow nconverting phosphors to produce “white” light. Further advances in both efficiency and wh ite-light quality will re quire new phosphors with narrow-band, highly efficient emission, particul arly in the red. A team led by principal investigator Dr. Victor Klim ov of Los Alamos National Labo ratory proposes to develop engineered semiconductor nanocrystal quantum dots (QDs) that combine optimal luminescent properties with long-term stability under ty pical downconverting conditions to enable new performance levels in SSL. The white LED phosphor industry is estimated to have sales of roughly $400 million in 2018 and would significantly benefit from the development of bright and narrow red-emitting QD phosphors because they woul d enable warmer whites without wasting energy by emission of light beyond the response of the human eye. In order to capitalize on the market opportunity, the LANL team is partnering with a local company called UbiQD that will facilitate US manufacturing.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗