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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 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
NASA NTRS1996

Momentum Transfer Studies and Studies of Linear and Nonlinear Optical Properties of Metal Colloids and Semiconductor Quantum Dots

Phase 1 of this work involved design work on a momentum transfer device. The progress on design and testing will be presented. Phase 2 involved the systematic study of the MPD thruster for dual uses. Though it was designed as a thruster for space vehicles, the characteristics of the plasma make it an excellent candidate for industrial applications. This project sought to characterize the system for use in materials processing and characterization. The surface modification on ZnCdTe, CdTe, and ZnTe will be presented. Phase 3 involved metal colloids and semiconductor quantum dots. One aspect of this project involves a collaborative effort with the Solid State Division of ORNL. The thrust behind this research is to develop ion implantation for synthesizing novel materials (quantum dots wires and wells, and metal colloids) for applications in all optical switching devices, up conversion, and the synthesis of novel refractory materials. The ions of interest are Au, Ag, Cd, Se, In, P, Sb, Ga, and As. The specific materials of interest are: CdSe, CdTe, InAs, GaAs, InP, GaP, InSb, GaSb, and InGaAs. A second aspect of this research program involves using porous glass (25-200 A) for fabricating materials of finite size. The results of some of this work will also be reported.

Collins, W. E.↗
DOE OSTI2018

Origin of Broad Emission Spectra in InP Quantum Dots: Contributions from Structural and Electronic Disorder

The ensemble emission spectra of colloidal InP quantum dots are broader than achievable spectra of cadmium- and lead-based quantum dots, despite similar single-particle line widths and significant efforts invested in the improvement of synthetic protocols. Here, we seek to explain the origin of persistently broad ensemble emission spectra of colloidal InP quantum dots by investigating the nature of the electronic states responsible for luminescence. We identify a correlation between red-shifted emission spectra and anomalous broadening of the excitation spectra of luminescent InP colloids, suggesting a trap-associated emission pathway in highly emissive core shell quantum dots. Time-resolved pump probe experiments find that s are largely untrapped on photoluminescence relevant time scales pointing to emission from recombination of localized holes with free electrons. Two-dimensional electronic spectroscopy on InP quantum dots reveals multiple emissive states and increased electron phonon coupling associated with hole localization. These localized hole states near the valence band edge are hypothesized to arise from incomplete surface passivation and structural disorder associated with lattice defects. We confirm the presence and effect of lattice disorder by X-ray absorption spectroscopy and Raman scattering measurements. Participation of localized electronic states that are associated with various classes of lattice defects gives rise to phonon-coupled defect related emission. These findings explain the origins of the persistently broad emission spectra of colloidal InP quantum dots and suggest future strategies to narrow ensemble emission lines comparable to what is observed for cadmium-based materials.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Colloidal Synthesis Path to 2D Crystalline Quantum Dot Superlattices

By combining colloidal nanocrystal synthesis, self-assembly, and solution phase epitaxial growth techniques, we developed a general method for preparing single dot thick atomically attached quantum dot (QD) superlattices with high-quality translational and crystallographic orientational order along with state-of-the-art uniformity in the attachment thickness. The procedure begins with colloidal synthesis of hexagonal prism shaped core/shell QDs (e.g., CdSe/CdS), followed by liquid subphase self-assembly and immobilization of superlattices on a substrate. Solution phase epitaxial growth of additional semiconductor material fills in the voids between the particles, resulting in a QD-in-matrix structure. The photoluminescence emission spectra of the QD-in-matrix structure retains characteristic 0D electronic confinement. Importantly, annealing of the resulting structures removes inhomogeneities in the QD–QD inorganic bridges, which our atomistic electronic structure calculations demonstrate would otherwise lead to Anderson-type localization. The piecewise nature of this procedure allows one to independently tune the size and material of the QD core, shell, QD–QD distance, and the matrix material. These four choices can be tuned to control many properties (degree of quantum confinement, quantum coupling, band alignments, etc.) depending on the specific applications. Lastly, cation exchange reactions can be performed on the final QD-in-matrix, as demonstrated herein with a CdSe/CdS to HgSe/HgS conversion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Sub–single-exciton lasing using charged quantum dots coupled to a distributed feedback cavity

Colloidal semiconductor quantum dots (QDs) are attractive materials for realizing highly flexible, solution-processable optical gain media, but they are difficult to use in lasing because of complications associated with extremely short optical-gain lifetimes limited by nonradiative Auger recombination. By combining compositional grading of the QD’s interior for hindering Auger decay with postsynthetic charging for suppressing parasitic ground-state absorption, we can reduce the lasing threshold to values below the single-exciton-per-dot limit. As a favorable departure from traditional multi-exciton–based lasing schemes, our approach should facilitate the development of solution-processable lasing devices and thereby help to extend the reach of lasing technologies into areas not accessible with traditional, epitaxially grown semiconductor materials.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Peculiarities of the nonlinear absorption of colloidal solutions of CdSe/ZnS quantum dots under stationary single-photon excitation of excitons

Peculiarities of the nonlinear absorption of a colloidal solution of CdSe/ZnS quantum dots with various sizes under resonant stationary excitation of the ground electron–hole (exciton) transition have been revealed by the pump and probe technique. The detected peculiarities of the nonlinear change in absorption are explained by the coexistence and competition of the effects of state filling and charge-induced Stark and temperature long-wavelength shift of the absorption spectra.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

In situ spectroscopic characterization of a solution-phase X-type ligand exchange at colloidal lead sulphide quantum dot surfaces

Here, we employed quantitative NMR spectroscopy and spectrophotometric absorbance titration to study a quantum dot X-type ligand exchange reaction. We find that the exchange is highly cooperative, where at low extents of exchange the change in free energy of the reaction, Δ G XC , is ~11 kJ mol –1 while at higher extents of exchange Δ G XC saturates to ~–4 kJ mol –1 . A modified Fowler binding isotherm is developed to describe the reaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Ultrafast Symmetry Control in Photoexcited Quantum Dots

Symmetry control is essential for realizing unconventional properties, such as ferroelectricity, nonlinear optical responses, and complex topological order, thus it holds promise for the design of emerging quantum and photonic systems. Nevertheless, fast and reversible control of symmetry in materials remains a challenge, especially for nanoscale systems. Here, reversible symmetry changes are unveiled in colloidal lead chalcogenide quantum dots on picosecond timescales. Using a combination of ultrafast electron diffraction and total X-ray scattering, in conjunction with atomic-scale structural modeling and first-principles calculations, it is revealed that symmetry-broken lead sulfide quantum dots restore to a centrosymmetric phase upon photoexcitation. The symmetry restoration is driven by photoexcited electronic carriers, which suppress lead off-centering for about 100 ps. Furthermore, the change in symmetry is closely correlated with the electronic properties, and the bandgap transiently red-shifts in the symmetry-restored quantum dots. Overall, this study elucidates reversible symmetry changes in colloidal quantum dots, and more broadly defines a new methodology to optically control symmetry in nanoscale systems on ultrafast timescales.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Self-diffraction of ultrashort laser pulses under resonant excitation of excitons in a colloidal solution of CdSe/ZnS quantum dots

We report self-diffraction processes of two types under resonant excitation of the fundamental electron – hole (exciton) transition in a strongly absorbing colloidal solution of CdSe/ZnS quantum dots (QDs) by high-power picosecond laser pulses. In the first case the absorption saturation (bleaching) at the exciton transition frequency and the Stark shift of exciton absorption line lead to the formation of a transparency channel and self-diffraction of the laser beam from the thus induced round diaphragm. In the second case, self-diffraction of two laser beams, intersecting in a cell with a colloidal QD solution, occurs on the diffraction grating induced by these beams. The physical processes responsible for the nonlinear optical properties of CdSe/ZnS QDs and the found selfaction effects are analysed. (nonlinear optical phenomena)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Nanotechnology: Colourful Particles for Spectrometry

In 1857 Michael Faraday gave a well-attended lecture at the Royal Institution of Great Britain, in which he presented his pioneering experimental work that investigated the interaction of light with matter. Faraday’s study probed the fundamental properties of light as it was reflected and absorbed by progressively smaller particles. Very fine gold particles dispersed in liquid were shown to produce vivid colors not seen in larger particles. Faraday did not know he had created colloidal suspensions of quantum dots, but his insight correctly concluded that the distinct colors were somehow due to the minute size of the gold particles. This great experimental physicist had actually glimpsed a special condition where the particle’s quantum nature was expressed. This work set the future course for nanoscience and quantum theory, but it would take another 125 years before the physical basis of this phenomenon would be explained by quantum size effects. It is now known that when quantum dots are exposed to UV light, some of the electrons are excited as they gain energy, however they remain confined to discrete energy levels not observed in larger particles and solid materials. When the electrons relax and lose their energy, the quantum dot emits light at a specific color that varies with the size of the quantum dot. Bao and Bawendi have cleverly exploited the unique optical properties intrinsic to colloidal quantum dots to develop an innovative compact optical spectrometer that could be integrated with a smart phone camera or as a versatile miniature handheld sensing tool.

Colloidal quantum dots↗
DOE OSTI2015

Optical and structural properties of ensembles of colloidal Ag{sub 2}S quantum dots in gelatin

The size dependences of the absorption and luminescence spectra of ensembles of hydrophilic colloidal Ag{sub 2}S quantum dots produced by the sol-gel method and dispersed in gelatin are analyzed. By X-ray diffraction analysis and transmission electron microscopy, the formation of core/shell nanoparticles is detected. The characteristic feature of the nanoparticles is the formation of crystalline cores, 1.5–2.0 nm in dimensions, and shells of gelatin and its complexes with the components of synthesis. The observed slight size dependence of the position of infrared photoluminescence bands (in the range 1000–1400 nm) in the ensembles of hydrophilic colloidal Ag{sub 2}S quantum dots is explained within the context of the model of the radiative recombination of electrons localized at structural and impurity defects with free holes.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Unsaturated Ligands Seed an Order to Disorder Transition in Mixed Ligand Shells of CdSe/CdS Quantum Dots

A phase transition within the ligand shell of core/shell quantum dots is studied in the prototypical system of colloidal CdSe/CdS quantum dots with a ligand shell composed of bound oleate (OA) and octadecylphosphonate (ODPA). The ligand shell composition is tuned using a ligand exchange procedure and quantified through proton NMR spectroscopy. Temperature-dependent photoluminescence spectroscopy reveals a signature of a phase transition within the organic ligand shell. Surprisingly, the ligand order to disorder phase transition triggers an abrupt increase in the photoluminescence quantum yield (PLQY) and full-width at half-maximum (FWHM) with increasing temperature. The temperature and width of the phase transition show a clear dependence on ligand shell composition, such that QDs with higher ODPA fractions have sharper phase transitions that occur at higher temperatures. In order to gain a molecular understanding of the changes in ligand ordering, Fourier transform infrared and vibrational sum frequency generation spectroscopies are performed. These measurements confirm that an order/disorder transition in the ligand shell tracks with the photoluminescence changes that accompany the ligand phase transition. The phase transition is simulated through a lattice model that suggests that the ligand shell is well-mixed and does not have completely segregated domains of OA and ODPA. Finally, we show that the unsaturated chains of OA seed disorder within the ligand shell.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Optical nonlinearities of colloidal InP@ZnS core-shell quantum dots probed by Z-scan and two-photon excited emission

Spectrally resolved nonlinear optical properties of colloidal InP@ZnS core-shell quantum dots of various sizes were investigated with the Z-scan technique and two-photon fluorescence excitation method using a femtosecond laser system tunable in the range from 750 nm to 1600 nm. In principle, both techniques should provide comparable results and can be interchangeably used for determination of the nonlinear optical absorption parameters, finding maximal values of the cross sections and optimizing them. We have observed slight differences between the two-photon absorption cross sections measured by the two techniques and attributed them to the presence of non-radiative paths of absorption or relaxation. The most significant value of two-photon absorption cross section σ{sub 2} for 4.3 nm size InP@ZnS quantum dot was equal to 2200 GM, while the two-photon excitation action cross section σ{sub 2}Φ was found to be 682 GM at 880 nm. The properties of these cadmium-free colloidal quantum dots can be potentially useful for nonlinear bioimaging.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Light-emitting nanocomposite particles

A method of making an inorganic light emitting layer includes combining a solvent for semiconductor nanoparticle growth, a solution of core/shell quantum dots, and semiconductor nanoparticle precursor(s); growing semiconductor nanoparticles to form a crude solution of core/shell quantum dots, semiconductor nanoparticles, and semiconductor nanoparticles that are connected to the core/shell quantum dots; forming a single colloidal dispersion of core/shell quantum dots, semiconductor nanoparticles, and semiconductor nanoparticles that are connected to the core/shell quantum dots; depositing the colloidal dispersion to form a film; and annealing the film to form the inorganic light emitting layer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2013

Composite system based on CdSe/ZnS quantum dots and GaAs nanowires

The possibility of fabricating a composite system based on colloidal CdSe/ZnS quantum dots and GaAs nanowires is demonstrated and the structural and emission properties of this system are investigated by electron microscopy and photoluminescence spectroscopy techniques. The good wettability and developed surface of the nanowire array lead to an increase in the surface density of quantum dots and, as a consequence, in the luminosity of the system in the 600-nm wavelength region. The photoluminescence spectrum of the quantum dots exhibits good temperature stability in the entire range 10-295 K. The impact of surface states on energy relaxation and the role of exciton states in radiative recombination in the quantum dots are discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Asymmetrically strained quantum dots with non-fluctuating single-dot emission spectra and subthermal room-temperature linewidths

The application of colloidal semiconductor quantum dots as single-dot light sources still requires overcoming several challenges. Recently, there has been considerable progress in suppressing intensity fluctuations (blinking) by encapsulating an emitting core into a thick protective shell. However, these nanostructures still show considerable fluctuations in both emission energy and linewidth. Here we demonstrate type-I core/shell heterostructures that overcome these deficiencies. They are made by combining wurtzite semiconductors with a large, directionally anisotropic lattice mismatch, which results in strong asymmetric compression of the emitting core. This modifies the structure of band-edge excitonic states and leads to accelerated radiative decay, reduced exciton-phonon interactions, and suppressed coupling to fluctuating electrostatic environment. As a result, individual asymmetrically strained dots exhibit highly stable emission energy (<1 meV standard deviation) and a subthermal room-temperature linewidth (~20 meV), concurrent with nearly nonblinking behaviour, high emission quantum yields, and a widely tunable emission colour.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Singlet-Oxygen Sensitization by Associates of Methylene Blue with Colloidal Ag{sub 2}S Quantum Dots Passivated by Thioglycolic Acid

Luminescence studies of singlet-oxygen photosensitization by methylene blue molecules in various solvents, as well as by hybrid associates of this dye with colloidal Ag{sub 2}S quantum dots with average sizes of 2.0, 2.4, and 2.7 nm, are performed. The conditions for simultaneous singlet-oxygen photosensitization and detection of the IR luminescence of colloidal Ag{sub 2}S quantum dots passivated by thioglycolic acid are determined.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2014

Magneto-optical controlled transmittance alteration of PbS quantum dots by moderately applied magnetic fields at room temperature

We observed changes of the transmitted monochromatic light passing through a colloidal PbS quantum dot film on glass owing to an applied moderate (smaller than 1 T) magnetic field under ambient conditions. The observed alterations show a square dependence on the magnetic field increase that cannot be achieved with bulk semiconductors. The findings point to so far not recognized application potentials of quantum dots.

77 NANOSCIENCE AND NANOTECHNOLOGY↗