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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 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Wide bandgap semiconductor materials and devices

The technological and societal impacts of electronic devices based on Ge, Si, and compound semiconductors like GaAs have been profound, fueling the decades long quest in identifying ever-larger bandgap semiconductors to untap new applications and possibilities. Specifically, an increase in the bandgap leads to shorter wavelength emission and an increased breakdown electric field, which has direct consequences for solid-state lighting like light-emitting diodes (LEDs) and laser diodes (LDs) from the visible (blue-green, blue, and violet) and beyond (UV and deep-UV) spectral range and for radically improved power devices supported by a higher intrinsic breakdown strength. Wide bandgap (WBG) semiconductors represent the frontier of materials that satisfy these criteria and include group IV, III–V, and II–VI material families like SiC (3.2 eV), GaN (3.4 eV), and ZnO (3.4 eV), respectively. With even larger bandgaps exceeding 4 eV, ultrawide bandgap (UWBG) semiconductors include diamond, III-nitrides incorporating Al and B (e.g., AlN, BN, and AlGaN), and sesquioxides like Ga 2 O 3 and (Al,Ga) 2 O 3 . These materials span widely varying stages of technological maturity, with SiC and GaN platforms among the most mature with commercially available devices in RF and high-power electronics, while other platforms such as Ga 2 O 3 rapidly advancing and poised to enable new UV and deep-UV optoelectronic devices. This Special Topic on Wide Bandgap Semiconductor Materials and Devices covers broad research subtopics on WBG and UWBG materials that span bulk crystals, epitaxy and substrate technologies, fundamental defect science, and doping, as well as electronic and optoelectronic device fabrication and characterization. Here, we highlight works from the collection, which we categorize by material platform of SiC, III-nitrides, and Ga 2 O 3 and related alloys.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Optical property investigations of polystyrene capped Ca{sub 2}P{sub 2}O{sub 7}:Dy{sup 3+} persistent phosphor

Highlights: • Synthesis of polymer capped pyrophosphate phosphors by citrate gel method. • Radiative lifetime is calculated from parameters of Judd-Ofelt theory and ICP-AES. • Reaction mechanism is discussed leading to high photoluminescence efficiency. • PL emission spectrum reveals broad band emission suitable for solid state lighting. - Abstract: By virtue of enhanced photosensivity, good optical response and better thermal stability, organic–inorganic hybrid materials are contemplated as one of the alternatives for designing advanced optoelectronic devices and innovative photonic applications. A novel inorganic organic hybrid Ca{sub 2}P{sub 2}O{sub 7}:Dy{sup 3+} phosphor has been fabricated by Pechini method. The optical property of synthesized phosphor is successfully altered by the in corporation of polystyrene sulfonic acid as capping agent in the colloidal solution. The phase purity and the average particle size of the prepared phosphor were calculated from X-ray diffraction (XRD) employing Debye Scherrer method. The morphological and chemical investigations were carried out through scanning electron microscopy (SEM) and energy dispersive spectroscopy (EDS) analysis. The radiative transitions are explained on the basis of Judd-Ofelt theory and on the basis of derived parameters, the radiative lifetime of persistent hybrid Ca{sub 2}P{sub 2}O{sub 7}:Dy{sup 3+} phosphor is calculated as 5.33 ms. This paper explores the mechanism leading to high photoluminescence efficiency using organic capping additives. The photoluminescence (PL) graphs reveal broad band emission at 482 nm (blue) and 573 nm (yellow) corresponding to {sup 4}F{sub 9/2}-{sup 6}H{sub 15/2} and {sup 4}F{sub 9/2}-{sup 6}H{sub 13/2} transitions of Dy{sup 3+}, respectively. The Commission International De I-Eclairage (CIE) chromaticity co-ordinates were calculated from emission spectra and the values (x, y) were approaching to standard value of white emission. The synthesized pyrophosphate phosphors can thereby account in multiple potential applications including white light emitting diodes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Self‐Trapped and Free Exciton Dynamics in Vacuum‐Deposited Cesium Copper Iodide Thin Films

Abstract Highly photoluminescent, lead‐free perovskites are of interest for displays and solid‐state light‐emitting devices. In this report, streak camera‐based time‐resolved emission and transient absorption spanning visible to deep‐ultraviolet (UV) wavelengths are utilized to study self‐trapped and free exciton dynamics in vacuum‐deposited cesium copper halide thin films of CsCu 2 I 3 and Cs 3 Cu 2 I 5 . Self‐trapped exciton emission of CsCu 2 I 3 exhibits more noticeable changes with time in the peak position and width than Cs 3 Cu 2 I 5 . UV‐to‐blue emission is detectable for both compositions, where free exciton emission is distinct for CsCu 2 I 3 . Transient absorption shows loss of ground‐state bleach signals at early time delays for both, and the bleach signal shifts toward higher energy as time delay increases, likely due to strains induced by the newly created self‐trapped excitons. Global analysis performed on the transient absorption results yields time constants in these materials that build an overall dynamic scheme. This work aids in building a complete picture regarding light emission in these promising materials.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Uranium Doped Gallium Nitride Epitaxial Thin Films

Gallium nitride (GaN) is near ubiquitous in modern day technologies, forming the backbone of solid-state lighting and high-power electronics. Engineering the physical properties of GaN has been investigated to some degree by the incorporation or doping of most of the elements of the periodic table, but the actinides remain unexplored. Molecular beam epitaxy is used to demonstrate uranium doping of GaN single crystals. High structural quality of the host matrix is maintained despite partial elemental segregation of the uranium dopant into 1D structures at the levels presented here. Electronic transport measurements reveal relatively high conductivity, which persists down to cryogenic temperature and is characterized by the formation of narrow gaps in the electronic band structures very close to the Fermi level. Photoluminescence measurements reveal that the U-doped GaN exhibits optical behavior similar to that of the GaN substrate. The addition of actinide materials to a non-centrosymmetric, optically active, radiation-hard, and electronically tunable host matrix opens a world of possibilities for investigating and leveraging elements with high electron correlations in the pursuit of novel devices.

36 - MATERIALS SCIENCE↗
DOE OSTI2018

Unexpectedly Strong Auger Recombination in Halide Perovskites

The emergence of halide perovskites for photovoltaic applications has triggered great interest in these materials for solid-state light emission. Higher order electron–hole recombination processes can critically affect the efficiency of such devices. In the present work, the Auger recombination coefficients are computed in the prototypical halide perovskite, CH 3 NH 3 PbI 3 (MAPbI 3 ), using first-principles calculations. It is demonstrated that Auger recombination is responsible for the exceptionally high third-order recombination coefficient observed in experiment. The large Auger coefficient is attributed to a coincidental resonance between the bandgap and interband transitions to a complex of higher-lying conduction bands. It is also found that the distortions of PbI 6 octahedra contribute significantly to the high Auger coefficient, offering potential avenues for materials design.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Applications of plasma-enhanced metalorganic chemical vapor deposition

The use of plasma enhancement for growth of III-V compound semiconductor materials by metalorganic chemical vapor deposition (MOCVD) is examined, to improve control of microstructure, develop understanding of the underlying growth mechanisms, and expand the range of materials combinations for photovoltaic and solid-state lighting applications. Whereas plasma is commonly used with group-IV materials, such as silicon, few studies have examined the impact of plasma-enhanced MOCVD (PE-MOCVD) for III-V materials growth. PE-MOCVD provides improved decomposition of metalorganic precursors, which is driven by hydrogen plasma to augment hydride reactions and thermal pyrolysis, but plasma generation requires low reactor pressure. We have demonstrated elemental Al films grown by PE-MOCVD, which show distinct crystallographic texturing, and assume epitaxial microstructure upon post-growth annealing. We also demonstrate PE-MOCVD of GaAs at temperatures as low as 300 °C. With increasing radio-frequency power, the GaAs growth rate shows a transition from power limited to mass-transport limited. PE-MOCVD grown Ga 0.5 In 0.5 P shows no detectable spontaneous atomic ordering, which offers a mechanism to form order/disorder unicompositional heterostructures, without temperature change or impurity incorporation. In its current implementation, PE-MOCVD grown films have shown microstructural degradation, that we attribute to direct plasma exposure during growth. Improvements in the system design and growth sequences are at the focus of on-going efforts.

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

Fluorescence properties of Tb{sup 3+} and Sm{sup 3+} activated novel LiAl{sub 7}B{sub 4}O{sub 17} host via solution combustion synthesis

Graphical abstract: - Highlights: • New LiAl{sub 7}B{sub 4}O{sub 17}:Tb{sup 3+}, Sm{sup 3+} phosphors were synthesized first time by solution combustion method. • The LiAl{sub 7}B{sub 4}O{sub 17}:Tb{sup 3+} emissions; 489, 544, 586 and 623 nm (λ{sub ex} = 234 nm). • Also for LiAl{sub 7}B{sub 4}O{sub 17}:Sm{sup 3+}; 564, 601 and 649 nm (λ{sub ex} = 403 nm). • Synthesized materials were characterized by powder XRD, FE-SEM. • Concentration quenching mechanism and critical transfer distance of Tb{sup 3+} and Sm{sup 3+} in the prepared sample has been investigated. - Abstract: Novel LiAl{sub 7}B{sub 4}O{sub 17} (LABO) phosphor activated with trivalent rare earth ions (RE = Tb, Sm) was synthesized by using solution combustion synthesis. The powder X-ray diffraction (XRD), field emission-scanning electron microscope (FE-SEM), photoluminescence (PL), critical transfer distance (R{sub c}) and quenching mechanism studies were employed to characterize the samples. Under ultraviolet irradiation of the LiAl{sub 7}B{sub 4}O{sub 17}: Tb{sup 3+}, Sm{sup 3+} phosphors exhibit the typical green ({sup 5}D{sub 4} → {sup 7}F{sub j} = 6, 5, 4 and 3) emission band of the Tb{sup 3+} ions, as well as an orange-red and red ({sup 4}G{sub 5/2} → {sup 6}H{sub J=5/2,} {sub 7/2,} {sub 9/2}) emission bands of the Sm{sup 3+} ions. These results suggest that Tb{sup 3+} and Sm{sup 3+} activated LABO phosphor could be promising in vision of the necessity for solid state lighting applications.

36 MATERIALS SCIENCE↗
DOE OSTI2018

The GdF3 phosphors with enhanced multicolor luminescence via multi-channel excitation and energy migration procedure

Highlights: • Core-shell structured GdF{sub 3} phosphors were synthesized by hydrothermal method. • SiO{sub 2} coating layers prevent aggregation and sintering during thermal annealing. • The annealed CSS nanophosphors were highly dispersible. • The inserted PMA significantly enhances multicolor luminescence. • The annealed CSS phosphors exhibit enhanced multicolor luminescence properties. - Abstract: A collection of GdF{sub 3} core-shell structured (CSS) phosphors were synthesized by hydrothermal method. The as-prepared (AP) phosphors were coated with SiO{sub 2} layers to avoid aggregation and sintering during thermal annealing at 800 °C, after which the SiO{sub 2} layers were etched off and the annealed phosphors became highly dispersible. The annealed CSS phosphor aGdF{sub 3}:Eu{sup 3+}@GdF{sub 3}:Ce{sup 3+},Dy{sup 3+} shows excellent multicolor luminescence performance with the aid of dual-channel excitation and energy migration (EM) procedure of Gd{sup 3+} ions. By inserting pyromellitic acid (PMA) organic ligands into the interfaces between annealed core and AP shell layer regions, the so-called antenna effect of organic ligands of PMA forms a new excitation channel, which makes the CSS phosphor aGdF{sub 3}:Eu{sup 3+}@PMA@GdF{sub 3}:Ce{sup 3+},Dy{sup 3+} exhibit significantly enhanced multicolor luminescence via multi-channel excitation and EM process. The prepared CSS phosphors in this work are excellent candidates for applications in solid-state lighting.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Determining the Conduction Band-Edge Potential of Solar-Cell-Relevant Nb{sub 2}O{sub 5} Fabricated by Atomic Layer Deposition

Often key to boosting photovoltages in photo electrochemical and related solar-energy-conversion devices is the preferential slowing of rates of charge recombination especially recombination at semiconductor/solution, semiconductor/polymer, or semiconductor/perovskite interfaces. In devices featuring TiO2 as the semiconducting component, a common approach to slowing recombination is to install an ultrathin metal oxide barrier layer or trap-passivating layer atop the semiconductor, with the needed layer often being formed via atomic layer deposition (ALD). A particularly promising barrier layer material is Nb2O5. Its conduction-band-edge potential Ecg is low enough that charge injection from an adsorbed molecular, polymeric, or solid-state light absorber and into the semiconductor can still occur, but high enough that charge recombination is inhibited. While a few measurements of Ecg have been reported for conventionally synthesized, bulk Nb2O5, none have been described for ALD-fabricated versions. Here, we specifically determine the conduction-band-edge energy of ALD-fabricated Nb2O5 relative to that of TiO2. We find that, while the value for ALD-Nb2O5 is indeed higher than that for TiO2, the difference is less than anticipated based on measurements of conventionally synthesized Nb2O5 and is dependent on the thermal history of the material. The implications of the findings for optimization of competing interfacial rate processes, and therefore photovoltages, are briefly discussed.

Hoffeditz, William L.↗
DOE OSTI2017

Electronic and Optical Properties of Two-Dimensional GaN from First-Principles

Gallium nitride (GaN) is a vital commercial semiconductor for solid-state lighting applications. Atomically thin GaN, a recently synthesized two-dimensional material, is of particular interest because the extreme quantum confinement enables additional control of its light-emitting properties. We performed first-principles calculations based on density functional and many-body perturbation theory to investigate the electronic, optical, and excitonic properties of monolayer and bilayer two-dimensional (2D) GaN as a function of strain. These findings demonstrate that light emission from monolayer 2D GaN is blueshifted into the deep ultraviolet range, which is promising for sterilization and water-purification applications. Light emission from bilayer 2D GaN occurs at a similar wavelength to its bulk counterpart due to the cancellation of the effect of quantum confinement on the optical gap by the quantum-confined Stark shift. Polarized light emission at room temperature is possible via uniaxial in-plane strain, which is desirable for energy-efficient display applications. We compare the electronic and optical properties of freestanding two-dimensional GaN to atomically thin GaN wells embedded within AlN barriers in order to understand how the functional properties are influenced by the presence of barriers. Our results offer microscopic understanding of the electronic and optical characteristics of GaN at the few-layer regime.

36 MATERIALS SCIENCE↗
DOE OSTI2015

A Specific Nucleophilic Ring-Opening Reaction of Aziridines as a Unique Platform for the Construction of Hydrogen Polysulfides Sensors

Hydrogen polysulfides (H 2 S n , n>1) have been recently suggested to be the actual signalling molecules that involved in sulfur-related redox biology. However the exact mechanisms of H 2 S n are still poorly understood and a major hurdle in this field is the lack of reliable and convenient methods for H 2 S n detection. In this work we report a unique ring-opening reaction of N-sulfonylaziridine by Na 2 S 2 under mild conditions. Based on this reaction a novel H 2 S n -specific fluorescent probe (AP) was developed. The probe showed high sensitivity and selectivity for H 2 S n . Notably, the fluorescent turn-on product, i.e. compound 1, exhibited excellent two-photon photophysical properties and a large Stokes shift. Moreover, the high solid state luminescent efficiency of compound 1 makes it a potential candidate for organic emitters and solid-state lighting devices.

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

Near-Unity Photoluminescence Quantum Yield in Blue-Emitting Cs 3 Cu 2 Br 5– x I x (0 ≤ x ≤ 5)

Recently, interest in developing efficient, low-cost, nontoxic, and stable metal halide emitters that can be incorporated into solid-state lighting technologies has taken hold. Here we report nontoxic, stable, and highly efficient blue-light-emitting Cs 3 Cu 2 Br 5–x I x (0 ≤ x ≤ 5). Room-temperature photoluminescence measurements show bright blue emission in the 456 to 443 nm range with near-unity quantum yield for Cs 3 Cu 2 I 5 . Here, density functional theory calculations and power-dependent PL measurements suggest that the emission results from self-trapped excitons induced by strong charge localization within the zero-dimensional cluster structure of Cs 3 Cu 2 Br 5–x I x .

0D all-inorganic metal halides↗
DOE OSTI2015

Tunable Photoluminescent Core/Shell Cu(+)-Doped ZnSe/ZnS Quantum Dots Codoped with Al(3+), Ga(3+), or In(3+).

Semiconductor quantum dots (QDs) with stable, oxidation resistant, and tunable photoluminescence (PL) are highly desired for various applications including solid-state lighting and biological labeling. However, many current systems for visible light emission involve the use of toxic Cd. Here, we report the synthesis and characterization of a series of codoped core/shell ZnSe/ZnS QDs with tunable PL maxima spanning 430-570 nm (average full width at half-maximum of 80 nm) and broad emission extending to 700 nm, through the use of Cu(+) as the primary dopant and trivalent cations (Al(3+), Ga(3+), and In(3+)) as codopants. Furthermore, we developed a unique thiol-based bidentate ligand that significantly improved PL intensity, long-term stability, and resilience to postsynthetic processing. Through comprehensive experimental and computational studies based on steady-state and time-resolved spectroscopy, electron microscopy, and density functional theory (DFT), we show that the tunable PL of this system is the result of energy level modification to donor and/or acceptor recombination pathways. By incorporating these findings with local structure information obtained from extended X-ray absorption fine structure (EXAFS) studies, we generate a complete energetic model accounting for the photophysical processes in these unique QDs. With the understanding of optical, structural, and electronic properties we gain in this study, this successful codoping strategy may be applied to other QD or related systems to tune the optical properties of semiconductors while maintaining low toxicity.

Cooper, Jason K↗
DOE OSTI2022

Colloidal Quantum Shells: An Emerging 2D Semiconductor for Energy Applications

Low-dimensional semiconductors hold strong promise for future energy applications. These nanomaterials are inexpensive to process and offer a broad spectrum of attractive quantum-mechanical properties. The notorious problem of low-dimensional nanostructures, however, lies in their limited performance under high energetic loads, when more than one exciton per particle is created. Multiple excitons undergo fast annihilation, causing efficiently roll-off in energy-intensive applications, including high-brightness LEDs, X-ray scintillators, and solar cells. In this prospective, we will highlight an emerging type of low-dimensional semiconductors that allows avoiding such multi-exciton (MX) energy losses. Recently demonstrated colloidal quantum shells benefit from the spatial separation of multiple excitons, which leads to extraordinary improvements to MX lifetimes and MX quantum yield. This makes quantum shell morphology an attractive candidate for solution-processed optical and electrical devices. In this Focus Review, we compare the optoelectronic properties of quantum shells against other low-dimensional semiconductors and discuss their emerging opportunities in solid-state lighting and energy-harvesting applications.

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

Ligand Controls Excited Charge Carrier Dynamics in Metal-Rich CdSe Quantum Dots: Computational Insights

Small metal-rich semiconducting quantum dots (QDs) are promising for solid-state lighting and single-photon emission due to their highly tunable yet narrow emission line widths. Nonetheless, the anionic ligands commonly employed to passivate these QDs exert a substantial influence on the optoelectronic characteristics, primarily owing to strong electron–phonon interactions. In this work, we combine time-domain density functional theory and nonadiabatic molecular dynamics to investigate the excited charge carrier dynamics of Cd 28 Se 17 X 22 QDs (X = HCOO – , OH – , Cl – , and SH – ) at ambient conditions. These chemically distinct but regularly used molecular groups influence the dynamic surface-ligand interfacial interactions in Cd-rich QDs, drastically modifying their vibrational characteristics. The strong electron–phonon coupling leads to substantial transient variations at the band edge states. The strength of these interactions closely depends on the physicochemical characteristics of passivating ligands. Consequently, the ligands largely control the nonradiative recombination rates and emission characteristics in these QDs. Our simulations indicate that Cd 28 Se 17 (OH) 22 has the fastest nonradiative recombination rate due to the strongest electron–phonon interactions. Conversely, QDs passivated with thiolate or chloride exhibit considerably longer carrier lifetimes and suppressed nonradiative processes. The ligand-controlled electron–phonon interactions further give rise to the broadest and narrowest intrinsic optical line widths for OH and Cl-passivated single QDs, respectively. Finally, obtained computational insights lay the groundwork for designing appropriate passivating ligands on metal-rich QDs, making them suitable for a wide range of applications, from blue LEDs to quantum emitters.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Solid-State Solvation and Enhanced Exciton Diffusion in Doped Organic Thin Films under Mechanical Pressure

Direct modification of exciton energy has been previously used to optimize the operation of organic optoelectronic devices. One demonstrated method for exciton energy modification is through the use of the solvent dielectric effects in doped molecular films. To gain a deeper appreciation of the underlying physical mechanisms, we test the solid-state solvation effect in molecular thin films under applied external pressure. We observe that external mechanical pressure increases dipole–dipole interactions, leading to shifts in the Frenkel exciton energy and enhancement of the time-resolved spectral red shift associated with the energy-transfer-mediated exciton diffusion. Measurements are performed on host:dopant molecular thin films, which show bathochromic shifts in photoluminescence (PL) under increasing pressure. This is in agreement with a simple solvation theory model of exciton energetics with a fitting parameter based on the mechanical properties of the host matrix material. We measure no significant change in exciton lifetime with increasing pressure, consistent with unchanged aggregation in molecular films under compression. However, we do observe an increase in exciton spectral thermalization rate for compressed molecular films, indicating enhanced exciton diffusion for increased dipole–dipole interactions under pressure. The results highlight the contrast between molecular energy landscapes obtained when dipole–dipole interactions are increased by the pressure technique versus the conventional dopant concentration variation methods, which can lead to extraneous effects such as aggregation at higher doping concentrations. The present work demonstrates the use of pressure-probing techniques in studying energy disorder and exciton dynamics in amorphous molecular thin films.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Photophysics of Thermally-Assisted Photobleaching in “Giant” Quantum Dots Revealed in Single Nanocrystals

Quantum dots (QDs) are steadily being implemented as down-conversion phosphors in market-ready display products to enhance color rendering, brightness, and energy efficiency. However, for adequate longevity, QDs must be encased in a protective barrier that separates them from ambient oxygen and humidity, and device architectures are designed to avoid significant heating of the QDs as well as direct contact between the QDs and the excitation source. In order to increase the utility of QDs in display technologies and to extend their usefulness to more demanding applications as, for example, alternative phosphors for solid-state lighting (SSL), QDs must retain their photoluminescence emission properties over extended periods of time under conditions of high temperature and high light flux. Doing so would simplify the fabrication costs for QD display technologies and enable QDs to be used as down-conversion materials in light-emitting diodes for SSL, where direct-on-chip configurations expose the emitters to temperatures approaching 100 °C and to photon fluxes from 0.1 W/mm 2 to potentially 10 W/mm 2 . Here, we investigate the photobleaching processes of single QDs exposed to controlled temperature and photon flux. In particular, we investigate two types of room-temperature-stable core/thick-shell QDs, known as “giant” QDs for which shell growth is conducted using either a standard layer-by-layer technique or by a continuous injection method. We determine the mechanistic pathways responsible for thermally-assisted photodegradation, distinguishing effects of hot-carrier trapping and QD charging. As a result, the findings presented here will assist in the further development of advanced QD heterostructures for maximum device lifetime stability.

36 MATERIALS SCIENCE↗