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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 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Hybrid Carbon Dioxide Reduction Photocatalysts Consisting of Macrocyclic Cobalt(III) Complexes Deposited on Semiconductor Surfaces

Hybrid photocatalysts can be prepared by coupling metal ligand complexes with light-harvesting semiconductors. It is often challenging and time consuming to derivatize ligands with anchoring groups to effectively attach onto surfaces. In this study, we synthesized hybrid carbon dioxide reduction photocatalysts by directly depositing two macrocyclic Co(III) complexes on three different semiconductor surfaces (TiO 2 , N-Ta 2 O 5 and C 3 N 4 ). The resulting hybrid photocatalysts were characterized with various techniques and tested in CO 2 reduction reactions under different light conditions. Excellent visible-light CO 2 -reduction activity was obtained using C 3 N 4 as the light-harvesting semiconductor. Furthermore, density functional theory calculations were conducted to help understand interactions between the cobalt complexes with a model TiO 2 surface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Advanced Thermoluminescence Spectroscopy as a Research Tool for Semiconductor and Photonic Materials: A Review and Perspective

Thermoluminescence (TL) or thermally stimulated luminescence (TSL) spectroscopy is based on liberating charge carriers from traps in the bandgap by providing enough thermal energy to overcome the potential barrier of the traps. It provides a powerful tool to measure the positions of the localized states/traps in the bandgap. Despite that, its applications in semiconductors are very limited. Herein, the basics of TL spectroscopy and the recent advances in the technique with focus on cryogenic thermally stimulated photoemission spectroscopy (C‐TSPS) which extends TL measurements to cryogenic regime and allows the detection of very low concentrations of shallow and deep localized states is discussed. One goal herein is to introduce the reader to the use of TL and C‐TSPS in the characterization of semiconductors, explaining how it can be applied and demonstrating its advantages as a powerful tool for measuring shallow donor/acceptor ionization energies in semiconductors and as a method for characterizing compensating defects. The article also discusses interesting potential applications of C‐TSPS in new research areas such as corrosion and formation of oxide layers on metal surfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2023

The Migdal effect in semiconductors for dark matter with masses below ~ 100 MeV

Dark matter scattering off a nucleus has a small probability of inducing an observable ionization through the inelastic excitation of an electron, called the Migdal effect. We use an effective field theory to extend the computation of the Migdal effect in semiconductors to regions of small momentum transfer to the nucleus, where the final state of the nucleus is no longer well described by a plane wave. Our analytical result can be fully quantified by the measurable dynamic structure factor of the semiconductor, which accounts for the vibrational degrees of freedom (phonons) in a crystal. We show that, due to the sum rules obeyed by the structure factor, the inclusive Migdal rate and the shape of the electron recoil spectrum is well captured by approximating the nuclei in the crystal as free ions; however, the exclusive differential rate with respect to energy depositions to the crystal depends on the phonon dynamics encoded in the dynamic structure function of the specific material. Our results now allow the Migdal effect in semiconductors to be evaluated even for the lightest dark matter candidates (m χ ≳ 1 MeV) that can kinematically excite electrons.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

The dependence of aluminum lattice orientation on semiconductor lattice parameter in planar InAs/Al hybrid heterostructures

We present a detailed study of 7-nm thick Al layers epitaxially grown on In x Al 1-x As or Al 1-x Ga x Sb y As 1-y (0 0 1) semiconductors using high-resolution transmission electron microscopy (HRTEM) and synchrotron X-ray diffraction (XRD). These techniques provide high spatial and high reciprocal space resolution information about Al lattice orientations and interfacial structure, highlighting the existence of a strong correlation between the surface lattice parameter of the semiconductor and the normal orientation of the aluminum film. The normal orientation of Al layers is found to be [1 1 1] when the in-plane semiconductor surface lattice parameter, a S , is smaller than 5.98 Å, and is [1 1 0] when aS is larger than this value. In the transition between these lattice parameters where one orientation is preferred, both orientations may be observed. Concomitant with the change in normal orientation is an inversion in the strain state of the aluminum film. When the normal orientation is [1 1 1], the Al film is compressively strained; while for [1 1 0] normal orientations, the Al in-plane strain is tensile. An energy balance model, accounting for surface, interfacial, side-face, and strain energy, and the registry of lattice planes across the semiconductor/aluminum interface provide explanations for the observed normal orientation and strain inversion.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Design optimization of semiconductor piezoresistors with Schottky diode contacts

A modeling theory is developed to predict the performance of piezoresistors which incorporate Schottky diode electrical contacts. This new theory allows the design of high performance gauges which can be fabricated using NonLithographically-Based Microfabrication (NLBM) techniques. These semiconductor piezoresistors can be designed in customizable sizes and fabricated in parallel in order to integrate position sensing into MEMS flexural positioners. Customizable nanopositioning platforms will enable advances in a range of nano-scale fabrication and metrology applications. A semiconductor piezoresistor with Schottky diode contacts was fabricated and attached to a titanium flexure. This device is shown to match predicted electrical performance within about 8% and to show a gauge factor of 116, within 2% of the predicted value. Performance limits for Schottky diode semiconductor piezoresistors are identified to be about 127dB full noise dynamic range for a quarter bridge over a 10kHz sensor bandwidth on a 600µm width titanium flexure, making them ideal for sensing on meso-/micro-scale flexural positioners. Methods of reaching these performance bound are suggested and their impact on the sensor dynamic range are studied.

42 ENGINEERING↗
DOE OSTI2022

Semiconductor-dielectric-metal solar absorbers with high spectral selectivity

An ideal solar thermal absorber has a sharp transition between high and low absorptance at the wavelength where the blackbody emissive power begins to exceed the solar irradiance. However, most real selective absorbers have a fairly broad transition, leading to both solar absorption and thermal emission losses. Here, we model, fabricate, and characterize a highly selective semiconductor-dielectric-metal (Ga0.46In0.54As - MgF2 - Ag) solar absorber with an extremely sharp transition from high to low absorptance. The thin semiconductor serves as a selective filter, absorbing photons with wavelengths shorter than the bandgap and transmitting those with longer wavelengths. The highly reflective dielectric-metal rear mirror allows the structure to have very low emittance for longer wavelengths. These characteristics provide the absorber with a measured solar absorptance >91% below the bandgap wavelength and infrared emittance <5% at 100 degrees C above the bandgap wavelength. This transition wavelength can be tuned by modifying the semiconductor composition, and modeling indicates that the absorber's optical properties should be stable at high temperatures, making the structure a good candidate for unconcentrated to highly concentrated solar thermal energy conversion.

14 SOLAR ENERGY↗
DOE OSTI2020

Tuning the Mechanical Properties of a Polymer Semiconductor by Modulating Hydrogen Bonding Interactions

Conjugation breakers (CBs) with different H-bonding chemistry and linker flexibility are designed and incorporated into a Diketopyrrolopyrrole (DPP)-based conjugated polymer backbone. The effects of H-bonding interactions on polymer semiconductor morphology, mechanical properties and electrical performance are systematically investigated. We observe that CBs with H-bonding self-association constant >0.7 or denser packing tendency are able to induce higher polymer chain aggregation and crystallinity in as-casted thin film, resulting in higher modulus and crack on-set strain. Additionally, the rDoC (relative degree of crystallinity) of the stretched thin film with the highest crack on-set strain only suffers a small decrease, suggesting the main energy dissipation mechanism is the breakage of H-bonding interactions. By contrast, other less stretchable polymer films dissipate strain energy through the breakage of crystalline domains, indicated by drastic decrease in rDoC. Furthermore, we evaluate their electrical performance under mechanical strain in fully stretchable field-effect transistors. The polymer with the highest crack on-set strain has the least degradation in mobility as a function of strain. Overall, these observations suggest that we can aptly tune the mechanical properties in polymer semiconductors by modulating intermolecular interactions, such as H-bonding chemistry and linker flexibility. Such understanding provides molecular design guidelines for future stretchable semiconductors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Two-Dimensional Copper Iodide-Based Inorganic–Organic Hybrid Semiconductors: Synthesis, Structures, and Optical and Transport Properties

A group of copper iodide-based hybrid semiconductors with the general formula of 2D-CuI(L) 0.5 (L = organic ligands) are synthesized and structurally characterized. All compounds are two-dimensional (2D) networks made of one-dimensional (1D) copper iodide staircase chains that are interconnected by bidentate nitrogen-containing ligands. Results from optical absorption and emission experiments and density functional theory (DFT) calculations reveal that their photoluminescence (PL) can be systematically tuned by adjusting the lowest unoccupied molecular orbital (LUMO) energies of the organic ligands. Charge carrier transport measurements were carried out for the first time on single crystals of selected 2D-CuI(L) 0.5 structures, and the results show that they possess p-type conductivity with a Hall mobility of ~1 cm 2 V -1 s -1 for 2D-CuI(pm) 0.5 and 0.13 cm 2 V -1 s -1 for 2D-CuI(pz) 0.5 , respectively. These values are comparable to or higher than the mobilities of typical highly luminescent organic semiconductors. Finally, this work suggests that robust, high-dimensional copper iodide hybrid semiconductors are promising candidates to be considered as a new type of emissive layer for light-emitting diode (LED) devices.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Cubic Crystal Structure Formation and Optical Properties within the Ag–B II –M IV –X (B II = Sr, Pb; M IV = Si, Ge, Sn; X = S, Se) Family of Semiconductors

Quaternary chalcogenide semiconductors are promising materials for energy conversion and nonlinear optical applications, with properties tunable primarily by varying the elemental composition and crystal structure. Here, we first analyze the connections among several cubic crystal structure types, as well as the orthorhombic Ag 2 PbGeS 4 -type structure, reported for select members within the Ag–B II –M IV –X (B II = Sr, Pb; M IV = Si, Ge, Sn; X = S, Se) compositional space. Focusing on the Ag–Pb–Si–S and Ag–Sr–Sn–S systems, we show that one structure type, with the formulas Ag 2 Pb 3 Si 2 S 8 and Ag 2 Sr 3 Sn 2 S 8 , is favored. We have prepared powder and single-crystal samples of Ag 2 Pb 3 Si 2 S 8 and Ag 2 Sr 3 Sn 2 S 8 , showing that each takes on the noncentrosymmetric cubic space group I$\bar{43}$d and is isostructural to the previously reported compound Ag 2 Sr 3 Ge 2 Se 8 . Through hybrid density functional theory calculations, these cubic compounds are demonstrated to be (quasi-)direct band gap semiconductors with high densities of states at the band maxima. Furthermore, the band-gap energies are measured by reflectance spectroscopy as 1.95(3) and 2.66(4) eV for Ag 2 Pb 3 Si 2 S 8 and Ag 2 Sr 3 Sn 2 S 8 , respectively. We further measure the optical properties and show the electronic band structures of three other isostructural A I –B II –M IV –X-type materials, i.e., Ag 2 Sr 3 Si 2 S 8 , Ag 2 Sr 3 Ge 2 S 8 , and Ag 2 Sr 3 Ge 2 Se 8 , showing that the band gaps can be predictably tuned by element substitution. Detailed visual analyses of the different structures and of their relationships with other members of the Ag–B II –M IV –X compositional family provide a basis for a broader understanding of the structure formation and optoelectronic properties within the quaternary chalcogenide semiconductor family.

14 SOLAR ENERGY↗
DOE OSTI2020

Monolayer Semiconductor Auger Detector

Auger recombination in semiconductors is a many-body phenomenon in which the recombination of electrons and holes is accompanied by excitation of other charge carriers. The excess energy of the excited carriers is normally rapidly converted to heat, making Auger processes difficult to probe directly. In this paper, we employ a technique in which the Auger-excited carriers are detected by their ability to tunnel out of the semiconductor through a thin barrier, generating a current. We use vertical van der Waals heterostructures with monolayer WSe 2 as the semiconductor, with hexagonal boron nitride as the tunnel barrier, and a graphite collector electrode. The Auger processes combined with resonant absorption produce characteristic negative photoconductance. We detect holes Auger-excited by both neutral and charged excitons and find that the Auger scattering is surprisingly strong under weak excitation. Our work expands the range of techniques available for probing relaxation processes in 2D materials.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Evaluating Brightness and Stability of Cathodoluminescence from Colloidal Semiconductor Nanocrystals

Cathodoluminescence offers promise as a technique for correlation of atomic structure with electronic structure at the level of individual nanoparticles or even defects, with the ability to analyze complex nanostructures at length-scales far below those typically available to optical spectroscopy. Unlike other forms of electron microscopy, cathodoluminescence offers direct insights into the electronic structure of the visualized sample. Despite reports more than 10 years ago of individual nanoparticle cathodoluminescence, effective cathodoluminescence collection from colloidal semiconductor materials is relatively rare and remains challenging due to the instability of materials under the conditions of electron beam irradiation. In this work, to clarify the roadblocks for cathodoluminescence analysis of colloidal nanocrystals, we attempt a comprehensive study of the cathodoluminescence properties of semiconductor quantum shells, which have a thin concentric CdSe shell surrounding CdS nanoparticles, then surrounded by a further concentric CdS shell. These same materials were recently demonstrated to show promising scintillation performance in radioluminescence measurements, including high brightness (up to 100 ph/keV) and excellent durability. Comparative quantum yield measurements are designed to assess the brightness of semiconductor nanocrystal films, which show that the quantum shells are much less bright under electron irradiation compared to X-ray photons. Instability of CL emission is assigned to charging effects on the samples—and not thermal effects—through a series of voltage, current, dwell time, and atmospheric pressure experiments.

cathodoluminescence↗
DOE OSTI2024

Computational Insights into Phase Equilibria Between Wide-Gap Semiconductors and Contact Materials

Novel wide-band-gap semiconductors are needed for next-generation power electronics, but there is a gap between a promising material and a functional device. Finding stable (metal) contacts is one of the major challenges that is currently dealt with mainly via trial and error. Herein, we computationally investigate the thermochemistry and phase coexistence at the junction between three wide-gap semiconductors, ..beta..-Ga2O3, GeO2, and GaN, and possible contact materials. The pool of possible contacts includes 47 elemental metals and a set of 4 common, n-type transparent conducting oxides (ZnO, TiO2, SnO2, and In2O3). We use first-principles thermodynamics to model the Gibbs free energies of chemical reactions as a function of gas pressure (pO2/pN2) and equilibrium temperature. We deduce whether a semiconductor/contact interface will be stable at relevant conditions or a chemical reaction between them is to be expected, possibly influencing the long-term reliability and performance of devices. We generally find that most elemental metals tend to oxidize or nitridize and form various interface oxide/nitride layers. Exceptions include select late- and post-transition metals and, in the case of GaN, also the alkali metals, which are predicted to exhibit stable coexistence, although in many cases at relatively low gas partial pressures. Similar is true for the transparent conducting oxides, for which, in most cases, we predict a preference toward forming ternary oxides when in contact with ..beta..-Ga2O3 and GeO2. The only exception is SnO2, which we find to form stable contacts with both oxides. Finally, we show how the same approach can be used to predict gas partial pressure vs temperature phase diagrams to help direct synthesis of ternary compounds. We believe these results provide a valuable guidance in selecting contact materials to wide-gap semiconductors and suitable growth conditions.

contact materials↗
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

Coloring Tetrahedral Semiconductors: Synthesis and Photoluminescence Enhancement of Ternary II-III 2 -VI 4 Colloidal Nanocrystals

Ternary tetrahedral II-III 2 -VI 4 semiconductors, where II is Zn or Cd, III In or Ga, and VI S, Se, or Te, are of interest in UV radiation detectors in medicine and space physics as well as CO 2 photoreduction under visible light. We synthesize colloidal II-III 2 -VI 4 semiconductor nanocrystals from readily available precursors and ascertain their ternary nature by structural and spectroscopic methods, including 77 Se solid-state NMR spectroscopy. The pyramidally shaped nanocrystals range between 2 and 12 nm and exhibit optical gaps of 2–3.9 eV. In the presence of excess anions on the particle surface, treatment with Lewis acidic, Z-type ligands results in better passivation and enhanced photoluminescence. Electronic structure calculations reveal the most stable, lowest energy polymorphs and coloring patterns. This work will pave the way toward more environmentally friendly, ternary semiconductors for optoelectronics and electrocatalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Impact of Photon Recycling, Grain Boundaries, and Nonlinear Recombination on Energy Transport in Semiconductors

Energy carrier transport and recombination in semiconductors can be directly monitored with optical microscopy, revealing key insights into fundamental photophysics and informs efficient optoelectronic device design. Oftentimes, energy transport is measured by monitoring a time-resolved expanding carrier profile after optical excitation under a focused laser beam. Although this approach has gained widespread adoption, the presence of competing dynamic processes, such as diffusion and photon recycling, has made it difficult to accurately extract and understand important semiconductor properties. Here, we develop and apply a new framework for modeling energy transport in both excitonic and free carrier semiconductors. Here, we demonstrate that processes such as nonlinear recombination and photon recycling can have a significant impact on the apparent energy carrier profiles, especially for excitonic materials with short radiative lifetimes. Additionally, we find that film microstructure can lead to unique transport profiles that strongly depends on material boundary behavior and the difference between feature size and diffusion length. Here, these findings provide a deeper understanding of energy transport in semiconducting materials and provide new strategies for the design and optimization of electronic and optoelectronic devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Slow light in a 2D semiconductor plasmonic structure

Spectrally narrow optical resonances can be used to generate slow light, i.e., a large reduction in the group velocity. In a previous work, we developed hybrid 2D semiconductor plasmonic structures, which consist of propagating optical frequency surface-plasmon polaritons interacting with excitons in a semiconductor monolayer. Here, we use coupled exciton-surface plasmon polaritons (E-SPPs) in monolayer WSe 2 to demonstrate slow light with a 1300 fold decrease of the SPP group velocity. Specifically, we use a high resolution two-color laser technique where the nonlinear E-SPP response gives rise to ultra-narrow coherent population oscillation (CPO) resonances, resulting in a group velocity on order of 105 m/s. Our work paves the way toward on-chip actively switched delay lines and optical buffers that utilize 2D semiconductors as active elements.

42 ENGINEERING↗
DOE OSTI2023

Epitaxial growth of highly symmetrical branched noble metal-semiconductor heterostructures with efficient plasmon-induced hot-electron transfer

Epitaxial growth is one of the most commonly used strategies to precisely tailor heterostructures with well-defined compositions, morphologies, crystal phases, and interfaces for various applications. However, as epitaxial growth requires a small interfacial lattice mismatch between the components, it remains a challenge for the epitaxial synthesis of heterostructures constructed by materials with large lattice mismatch and/or different chemical bonding, especially the noble metal-semiconductor heterostructures. Here, we develop a noble metal-seeded epitaxial growth strategy to prepare highly symmetrical noble metal-semiconductor branched heterostructures with desired spatial configurations, i.e., twenty CdS (or CdSe) nanorods epitaxially grown on twenty exposed (111) facets of Ag icosahedral nanocrystal, albeit a large lattice mismatch (more than 40%). Importantly, a high quantum yield (QY) of plasmon-induced hot-electron transferred from Ag to CdS was observed in epitaxial Ag-CdS icosapods (18.1%). This work demonstrates that epitaxial growth can be achieved in heterostructures composed of materials with large lattice mismatches. The constructed epitaxial noble metal-semiconductor interfaces could be an ideal platform for investigating the role of interfaces in various physicochemical processes.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Coupling of electronic transition to ferroelectric order in a 2D semiconductor

A ferroelectric material often exhibits a soft transverse optical (TO) phonon mode which governs its phase transition. Charge coupling to this ferroelectric soft mode may further mediate emergent physical properties, including superconductivity and defect tolerance in semiconductors. However, direct experimental evidence for such coupling is scarce. Here we show that a photogenerated coherent phonon couples strongly to the electronic transition above the bandgap in the van der Waals (vdW) two-dimensional (2D) ferroelectric semiconductor NbOI 2 . Using terahertz time-domain spectroscopy and first-principles calculations, we identify this mode as the TO phonon responsible for ferroelectric order. This exclusive coupling occurs only with the above-gap electronic transition and is absent in the valence band as revealed by resonant inelastic X-ray scattering. Our findings suggest a new role of the soft TO phonon mode in electronic and optical properties of ferroelectric semiconductors.

36 MATERIALS SCIENCE↗