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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Chemical Control of Charge Trapping and Charge Transfer Processes at the Organic-Inorganic Interface within Quantum Dot-Organic Complexes

Within the research program funded through the Early Career Research Award we designed complexes of colloidal semiconductor quantum dots (QDs) and organic molecules in which the interfacial chemistry controls the electronic structure and dynamics of the excitonic state of the QD. The program included two main projects; (1) investigation of the mechanisms by which organic surfactants control the quantum confinement of excitonic charge carriers; and (2) development of models for electron transfer between QDs and adsorbed molecules as a function of interfacial chemistry. This project was extremely successful in that our achievements in those two areas addressed the great majority of questions we outlined in the original proposal and answered questions I did not think to ask in that original proposal. Our work led to the discovery of “exciton delocalizing ligands”, which change the electronic structure of colloidal semiconductor nanocrystals by altering, with small synthetic modifications to their surfaces, their most defining characteristic – the quantum confinement of their excited states. It also led to detailed, quantitative descriptions of how the surface chemistry of a QD dictates, thermodynamically and kinetically, the probability of exchange of electrons between the QD and a small molecule. We used two of the three major techniques in the proposal (transient photoluminescence and transient absorption). Electrogenerated chemiluminescence was also proposed, but was too technically difficult with these systems to be useful. Instead, NMR spectroscopy emerged as a major analytical tool in our studies. With the fundamental advancements we made with this project, we believe that we can design QDs to be the next great class of visible-light photocatalysts.

14 SOLAR ENERGY↗
DOE OSTI2013

Quantum Dots Promise to Significantly Boost Solar Cell Efficiencies (Fact Sheet)

In the search for a third generation of solar-cell technologies, a leading candidate is the use of 'quantum dots' -- tiny spheres of semiconductor material measuring only about 2-10 billionths of a meter in diameter. Quantum dots have the potential to dramatically increase the efficiency of converting sunlight into energy -- perhaps even doubling it in some devices -- because of their ability to generate more than one bound electron-hole pair, or exciton, per incoming photon. NREL has produced quantum dots using colloidal suspensions; then, using molecular self-assembly, they have been fabricated into the first-ever quantum-dot solar cells. While these devices operate with only 4.4% efficiency, they demonstrate the capability for low-cost manufacturing.

14 SOLAR ENERGY↗
DOE OSTI2020

3D Volumetric Structural Hierarchy Induced by Colloidal Polymerization of a Quantum-Dot Ionic Liquid Monomer Conjugate

Hierarchically structured emissive quantum dot (CdS/CdSe) poly(ionic liquid) composites are synthesized through colloidal polymerization within a lyotropic liquid crystal, yielding a solvent-responsive nanoparticle (NP) composite possessing four ordered structural motifs. The composite is prepared by coassembling an amphiphilic ionic liquid (IL) monomer, 3-decyl-1-vinylimidazolium chloride, [C 10 VIm + ][Cl - ], and IL monomer, 3-(10-mercaptodecyl)-1-vinylimidazolium bromide surface-functionalized quantum dots, QD-[SC 10 VIm + ][Br - ], in 30 wt % water. Photo (UV)-initiated free radical polymerization serves to form a colloidal copolymer that collimates pairs of QDs within the core of large cylinders (average diameter = 21 nm and length = 422 nm), as evidenced by ultrasmall-angle X-ray scattering (USAXS). As revealed by continuous wave terahertz multispectral reconstructive 3-D imaging, the subsurface structure along the cylinder axis undergoes dynamic rearrangement between 2D hexagonal and cubic packing. The polymerized ionic liquid sheath surrounding the QDs is composed of concentric hexagonally perforated lamellae (HPL) with an interlamellar repeat distance of 3 nm, as determined by small-angle X-ray scattering (SAXS). The encapsulated QDs retain crystallinity (TEM and WAXS) and emission characteristics (photoluminescence spectroscopy, lambda(EM) = 638 nm). Phenomenological time-dependent Ginzburg-Landau calculations verify the mesoscale cylinders arise from the topological constraints imposed by the in-plane perforations of the polymerized ionic liquid as it wraps around the hard (unmalleable) spherical QDs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Nonradiative Energy Transfer from Individual CdSe/ZnS Quantum Dots to Single-Layer and Few-Layer Tin Disulfide

We study the combination of zero-dimensional (0D) colloidal CdSe/ZnS quantum dots with tin disulfide (SnS 2 ), a two-dimensional (2D)-layered metal dichalcogenide, results in 0D–2D hybrids with enhanced light absorption properties. These 0D–2D hybrids, when exposed to light, exhibit intrahybrid nonradiative energy transfer from photoexcited CdSe/ZnS quantum dots to SnS 2 . Using single nanocrystal spectroscopy, we find that the rate for energy transfer in 0D–2D hybrids increases with added number of SnS 2 layers, a positive manifestation toward the potential functionality of such 2D-based hybrids in applications such as photovoltaics and photon sensing.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Atomic layer deposition effect on the electrical properties of Al{sub 2}O{sub 3}-passivated PbS quantum dot field-effect transistors

We have investigated the effect of atomic layer deposition (ALD) on the electrical properties of colloidal PbS quantum dot field-effect transistors (PbS QD-FETs). Low-temperature Al{sub 2}O{sub 3} ALD process was used to fill up the pore spaces of PbS QD films containing 1, 2-ethanedithiol ligands. Upon deposition of Al{sub 2}O{sub 3} on PbS film, the PbS QD-FETs showed ambipolar behavior. The treated film retained this property for over 2 months, despite of exposure to air. This change in the electrical properties of the PbS QD-FETs is attributed to the formation of electron channels in the Al{sub 2}O{sub 3}-passivated PbS film. We conclude that these electron transport channels in the Al{sub x}O{sub y}-PbS film are formed due to substitution of the Pb sites by Al metal and chemical reduction of Pb{sup 2+} ions, as determined by an analysis of the depth profile of the film using secondary ion mass spectrometry and X-ray photoelectron spectroscopy.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2015

Optical power limiting in ensembles of colloidal Ag{sub 2}S quantum dots

The effect of power limiting for optical radiation at a wavelength of 660 nm with a pulse duration of 10 ms and operation threshold of 2.2 – 3.1 mJ cm{sup -2} is observed in ensembles of colloidal Ag{sub 2}S quantum dots (QDs). Using the z-scanning method in an open-aperture scheme it is found that the power is limited mainly due to reverse saturable absorption caused by two-photon optical transitions that involve energy levels of Ag{sub 2}S photoluminescence centres, related to structural impurity defects in colloidal Ag{sub 2}S QDs. At the same time, the z-scanning in a closed-aperture scheme demonstrates the formation of a thermal dynamic lens. (nonlinear optical phenomena)

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2026

Advances in Colloidal InP-Based Quantum Dots for Photocatalytic Hydrogen Evolution

Photocatalytic materials for hydrogen generation are typically categorized into UV-absorbing metal oxides and visible-range semiconductors such as chalcogenides or perovskites, which often incorporate toxic elements. To address environmental concerns of the latter group, indium phosphide (InP)-based quantum dots (QDs) have recently emerged as a less toxic alternative. These nanocrystals (NCs) benefit from a broadband and tunable absorption spectrum, which is well matched for solar photochemistry, and offer suitable electronic characteristics to drive photoinduced charge separation. This perspective provides a comprehensive summary of the recent advancements in developing InP-based NCs with a focus on photocatalytic hydrogen production. We discuss synthetic strategies that enhance the catalytic activity of these materials and highlight key challenges that must be addressed to enhance their performance. Finally, we explore future research directions aimed at improving photocatalytic efficiency and integrating InP-based QDs into practical solar-to-fuel conversion systems.

Hydrogen↗
DOE OSTI2016

Solution-Processed, High-Speed, and High-Quantum-Efficiency Quantum Dot Infrared Photodetectors

For over a decade, much effort has been focused on passivation of the high density of localized electronic trap states in colloidal semiconductor quantum dots (QDs), which lead to reduced performance in solar cell, light-emitting diode, laser, and photoconductor applications. However, here we take advantage of the naturally occurring high density of trap states to demonstrate solution-processed high-speed PbSe quantum dot near-infrared photodetectors. Carrier transport dynamics studies reveal multiple trapping and release transport dynamics in band tail states. A sandwich microstrip transmission line photodetector utilizing these QD films was fabricated to achieve high performance by allowing carriers to be swept to the electrodes before they fall into the band tail states. As a result, this device demonstrates external quantum efficiency, responsivity, and response time (full width at half-maximum) of 54%, 0.36 A/W, and 74 ps, respectively.

36 MATERIALS SCIENCE↗
DOE OSTI2012

Photoinduced Surface Oxidation and Its Effect on the Exciton Dynamics of CdSe Quantum Dots

With increased interest in semiconductor nanoparticles for use in quantum dot solar cells there comes a need to understand the long-term photostability of such materials. Colloidal CdSe quantum dots (QDs) were suspended in toluene and stored in combinations of light/dark and N{sub 2}/O{sub 2} to simulate four possible benchtop storage environments. CdSe QDs stored in a dark, oxygen-free environment were observed to better retain their optical properties over the course of 90 days. The excited state lifetimes, determined through femtosecond transient absorption spectroscopy, of air-equilibrated samples exposed to light exhibit a decrease in average lifetime (0.81 ns) when compared to samples stored in a nitrogen/dark environment (8.3 ns). A photoetching technique commonly used for controlled reduction of QD size was found to induce energetic trap states to CdSe QDs and accelerate the rate of electron-hole recombination. X-ray absorption near edge structure (XANES) analysis confirms surface oxidation, the extent of which is shown to be dependent on the thickness of the ligand shell.

14 SOLAR ENERGY↗
DOE OSTI2017

Nanoimprinted High-Refractive Index Active Photonic Nanostructures Based on Quantum Dots for Visible Light

A novel method to realizing printed active photonic devices was developed using nanoimprint lithography (NIL), combining a printable high-refractive index material and colloidal CdSe/CdS quantum dots (QDs) for applications in the visible region. Active media QDs were applied in two different ways: embedded inside a printable high-refractive index matrix to form an active printable hybrid nanocomposite, and used as a uniform coating on top of printed photonic devices. As a proof-of-demonstration for printed active photonic devices, two-dimensional (2-D) photonic crystals as well as 1D and 2D photonic nanocavities were successfully fabricated following a simple reverse-nanoimprint process. We observed enhanced photoluminescence from the 2D photonic crystal and the 1D nanocavities. Outstandingly, the process presented in this study is fully compatible with large-scale manufacturing where the patterning areas are only limited by the size of the corresponding mold. This work shows that the integration of active media and functional materials is a promising approach to the realization of integrated photonics for visible light using high throughput technologies. We believe that this work represents a powerful and cost-effective route for the development of numerous nanophotonic structures and devices that will lead to the emergence of new applications.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Optically Excited Lasing in a Cavity‐Based, High‐Current‐Density Quantum Dot Electroluminescent Device

Abstract Laser diodes based on solution‐processable materials can benefit numerous technologies including integrated electronics and photonics, telecommunications, and medical diagnostics. An attractive system for implementing these devices is colloidal semiconductor quantum dots (QDs). The progress towards a QD laser diode has been hampered by rapid nonradiative Auger decay of optical‐gain‐active multicarrier states, fast device degradation at high current densities required for laser action, and unfavorable competition between optical gain and optical losses in a multicomponent device stack. Here we resolve some of these challenges and demonstrate optically excited lasing from fully functional high‐current density electroluminescent (EL) devices with an integrated optical resonator. This advance has become possible due to excellent optical gain properties of continuously graded QDs and a refined device architecture, which allows for highly efficient light amplification in a thin, EL‐active QD layer.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Influence of interfacial oxide on the optical properties of single layer CdTe/CdS quantum dots in porous silicon scaffolds

Using a combination of continuous wave and time-resolved spectroscopy, we study the effects of interfacial conditions on the radiative lifetimes and photoluminescence intensities of sub-monolayer colloidal CdTe/CdS quantum dots (QDs) embedded in a three-dimensional porous silicon (PSi) scaffold. The PSi matrix was thermally oxidized under different conditions to change the interfacial oxide thickness. QDs embedded in a PSi matrix with ∼0.4 nm of interfacial oxide exhibited reduced photoluminescence intensity and nearly five times shorter radiative lifetimes (∼16 ns) compared to QDs immobilized within completely oxidized, porous silica (PSiO{sub 2}) frameworks (∼78 ns). The exponential dependence of QD lifetime on interfacial oxide thickness in the PSi scaffolds suggests charge transfer plays an important role in the exciton dynamics.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Photoinduced Degradation of the Optical Properties of Colloidal Ag{sub 2}S and CdS Quantum Dots Passivated by Thioglycolic Acid

The results of studying degradation of the optical properties of colloidal Ag{sub 2}S and CdS quantum dots (QDs) 2.6–3.2 nm in size passivated by thioglycolic acid (TGA) are presented. The photoluminescence intensity of colloidal Ag{sub 2}S QDs has been found to decrease under laser irradiation at a wavelength of 445 nm, beginning with the effective power of 10 mW. The observed effect is interpreted as a photochemical reaction of formation of new nonradiative-recombination channels in Ag{sub 2}S QDs upon excitation. It is established for colloidal CdS QDs passivated by TGA that a decrease in the optical density in the entire absorption spectrum and the luminescence intensity is accompanied by precipitation of the colloidal particles in a cell and related to photodegradation of the passivating shell.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2018

Perovskite Quantum Dots: A New Absorber for Perovskite-Perovskite Tandem Solar Cells: Preprint

The nanoscale phase stabilization of CsPbI3 quantum dots allows for the advantageous manipulation of its phase diagram. We show that these all inorganic halide perovskite nanocrystals can be used to fabricate colloidal perovskite quantum dot solar cells with incredibly low voltage losses. Despite recently emerging on the photovoltaic scene, CsPbI3 quantum dot solar cells have already achieved approximately 85% of their Shockley-Quessier limit open-circuit voltage, among the lowest voltage loss achieved for any material with a band gap of 1.7 eV, excepting III-V semiconductors. The low losses in these devices recently led to a world record certified quantum dot solar cell efficiency of 13.4%. While single junction thin film perovskite solar cells have surpassed 22% power conversion efficiency, perovskite-perovskite tandem solar cells offer the potential for power conversion efficiencies exceeding 30%. However, to accomplish this ambitious goal, perovskite solar cells must be designed with incredibly low losses and the appropriate band gaps, which differ from the ideal band gap for single junction perovskite solar cells. In this respect, the incredibly low voltage loss and tunable band gap of CsPbI3 quantum dots make them ideally suited for all-perovskite tandem solar cell applications.

14 SOLAR ENERGY↗
DOE OSTI2024

Strain-graded quantum dots with spectrally pure, stable and polarized emission

Structural deformation modifies the bandgap, exciton fine structure and phonon energy of semiconductors, providing an additional knob to control their optical properties. The impact can be exploited in colloidal semiconductor quantum dots (QDs), wherein structural stresses can be imposed in three dimensions while defect formation is suppressed by controlling surface growth kinetics. Yet, the control over the structural deformation of QDs free from optically active defects has not been reached. Here, we demonstrate strain-graded CdSe-ZnSe core-shell QDs with compositionally abrupt interface by the coherent pseudomorphic heteroepitaxy. Resulting QDs tolerate mutual elastic deformation of varying magnitudes at the interface with high structural fidelity, allowing for spectrally stable and pure emission of photons at accelerated rates with near unity luminescence efficiency. We capitalize on the asymmetric strain effect together with the quantum confinement effect to expand emission envelope of QDs spanning the entire visible region and exemplify their use in photonic applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2018

Perovskite Quantum Dots. A New Absorber for Perovskite-Perovskite Tandem Solar Cells

The nanoscale properties of CsPbI 3 quantum dots allows for the advantageous manipulation of its phase diagram. We show that these all-inorganic halide perovskite nanocrystals can be used to fabricate colloidal perovskite quantum dot solar cells with low voltage losses. Despite only recently emerging on the photovoltaic scene, CsPbI 3 quantum dot solar cells have already achieved approximately 85% of their Shockley-Quessier limit open-circuit voltage, among the lowest voltage loss achieved for any material with a band gap of 1.7 eV, excepting III-V semiconductors. The low losses in these devices recently led to a world record certified quantum dot solar cell efficiency of 13.4%. While single junction thin film perovskite solar cells have surpassed 22% power conversion efficiency, perovskite-perovskite tandem solar cells offer the potential for power conversion efficiencies exceeding 30%. However, to accomplish this ambitious goal, perovskite solar cells must be designed with low losses and the appropriate band gaps, which differ from the ideal band gap for single junction perovskite solar cells. In this respect, the incredibly low voltage loss and tunable band gap of CsPbI 3 quantum dots make them ideally suited for all-perovskite tandem solar cell applications.

14 SOLAR ENERGY↗
DOE OSTI2017

Synthesis and Spectroscopy of Silver-Doped PbSe Quantum Dots

Electronic impurity doping of bulk semiconductors is an essential component of semiconductor science and technology. Yet there are only a handful of studies demonstrating control of electronic impurities in semiconductor nanocrystals. Here, we studied electronic impurity doping of colloidal PbSe quantum dots (QDs) using a postsynthetic cation exchange reaction in which Pb is exchanged for Ag. We found that varying the concentration of dopants exposed to the as-synthesized PbSe QDs controls the extent of exchange. The electronic impurity doped QDs exhibit the fundamental spectroscopic signatures associated with injecting a free charge carrier into a QD under equilibrium conditions, including a bleach of the first exciton transition and the appearance of a quantum-confined, low-energy intraband absorption feature. Photoelectron spectroscopy confirms that Ag acts as a p-type dopant for PbSe QDs and infrared spectroscopy is consistent with k • p calculations of the size-dependent intraband transition energy. We find that to bleach the first exciton transition by an average of 1 carrier per QD requires that approximately 10% of the Pb be replaced by Ag. Here, we hypothesize that the majority of incorporated Ag remains at the QD surface and does not interact with the core electronic states of the QD. Instead, the excess Ag at the surface promotes the incorporation of <1% Ag into the QD core where it causes p-type doping behavior.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Detection of CdSe quantum dot photoluminescence for security label on paper

CdSe quantum dot has great potential in various applications especially for emitting devices. One example potential application of CdSe quantum dot is security label for anti-counterfeiting. In this work, we present a practical approach of security label on paper using one and two colors of colloidal CdSe quantum dot, which is used as stamping ink on various types of paper. Under ambient condition, quantum dot is almost invisible. The quantum dot security label can be revealed by detecting emission of quantum dot using photoluminescence and cnc machine. The recorded quantum dot emission intensity is then analyzed using home-made program to reveal quantum dot pattern stamp having the word ’RAHASIA’. We found that security label using quantum dot works well on several types of paper. The quantum dot patterns can survive several days and further treatment is required to protect the quantum dot. Oxidation of quantum dot that occurred during this experiment reduced the emission intensity of quantum dot patterns.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗