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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 685 records · Page 38
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Split-pane electrochromic window control based on an embedded photometric device with real-time daylighting computing

Well-designed electrochromic (EC) glazing control can improve the energy performance of buildings and visual comfort of occupants in highly glazed buildings. Here in this paper, we designed and demonstrated a compact integrated EC glazing automation system to control tint states of a split-pane EC window according to variations of sky conditions. The control is based on monitoring the luminance distribution of the sky and real-time lighting computation for a building interior, using an embedded photometric device (EPD). It optimizes tint states of EC glazing to offer sufficient daylight provision and temper discomfort glare for occupants, which potentially mitigates excessive solar heat gain. ’In-situ’ experiments were conducted in a full-scale testbed to demonstrate the daylighting performance under various sky conditions. Finally, experimental results showed 83% of the working time for work-plane illuminance (WPI) and 95% of the time for daylight glare probability (DGP) were constrained in comfort range (WPIϵ[500, 2000] lux, DGP ≤ 0.35) by the automated EC glazing (controlled by EPD) under clear skies; 68% of the time for WPI and 94% of the time for DGP in confined range under clear skies with thin clouds; 62% of the time for WPI and 85% of the time for DGP in confined range under partly cloudy skies.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2013

Stability, electronic structures and transport properties of armchair (10, 10) BN/C nanotubes

Using the first-principle calculations, the stability and electronic properties of two novel types of four-segment armchair (10, 10) BN/C hybrid nanotubes ((BN){sub 5}C{sub 5}(BN){sub 5}C{sub 5}NT and (BN){sub 5}C{sub 5}(NB){sub 5}C{sub 5}NT) as well as two-segment armchair (10, 10) BN/C hybrid nanotubes ((BN{sub 20−n}C{sub n}NTs) are systematically investigated. When n increases from 1 to 4, the band gap of (BN){sub 20−n}C{sub n}NTs gradually decreases to a narrow one. When 4≤n≤17, the electronic structure of carbon segment in (BN){sub 20−n}C{sub n}NTs behaves as zigzag graphene nanoribbons whose band gap is modulated by an inherent electric field of the BN segment. ZGNR-like segments in (BN){sub 5}C{sub 5}(BN){sub 5}C{sub 5}NT and (BN){sub 5}C{sub 5}(NB){sub 5}C{sub 5}NT behave as narrow gap semiconductor and metal, respectively, due to their different chemical environment. Moreover, the (BN){sub 5}C{sub 5}(NB){sub 5}C{sub 5}NT can separate electron and hole carriers, indicating its potential application in solar cell materials. Obvious transport enhancement around the Fermi level is found in the four-segment nanotubes, especially a 6G{sub 0} transmission peak in the metallic (BN){sub 5}C{sub 5}(NB){sub 5}C{sub 5}NT. - Graphical abstract: Structural diagram of four-segment (BN){sub 5}C{sub 5}(NB){sub 5}C{sub 5}NT and its typical two-probe system. The band structures and transport spectra of (BN){sub 5}C{sub 5}(NB){sub 5}C{sub 5}NT are shown in upper and lower panels. Highlights: ► Transport properties of two types of four-segment BNC hybrid nanotubes are studied. ► Transport enhancements are realized in the four-segment BNC hybrid nanotubes. ► Electron and hole separation is found in four-segment BNC hybrid nanotubes.

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

Sol-gel preparation and characterization of Er3+ doped TiO2 luminescent nanoparticles

Highlights: • Sol-gel derived Er{sup 3+} doped TiO{sub 2} nanoparticles for potential use in solar cells and bio imaging. • Influence of Er{sup 3+} doping into TiO{sub 2} with various Er{sup 3+} concentration on structural, optical, and luminescence properties. • Down-and up-conversion luminescence behaviour of Er{sup 3+} doped titanium dioxide. - Abstract: The present paper reports on down-and up-conversion luminescence behaviour of sol-gel derived erbium doped titanium dioxide with anatase structure. Through combined structural, optical and electron microscope analysis, effective and influence of Er{sup 3+} doping into TiO{sub 2} lattice has been demonstrated using X-Ray diffraction (XRD), scanning electron microscope (SEM), transmission electron microscope (TEM), and optical reflectance spectra. XRD results showed only anatase diffraction peaks of TiO{sub 2}, indicating the formation of a pure anatase phase even after Er{sup 3+} incorporation into TiO{sub 2} lattice. Selected Area Electron Diffraction (SAED) confirmed that the synthesized TiO{sub 2} nanoparticles are polycrystalline in nature which correlated well with XRD findings. Upon excitation at 320 nm, two down-conversion contributions at 378 nm and 435 nm attributed to indirect band gap and defect-related emissions, respectively were observed from both pure and Er{sup 3+} doped TiO{sub 2} nanoparticles. On the other hand, strong green up-conversion emission centred at 544 nm ascribed to {sup 4}S{sub 3/2 }→ {sup 4}I{sub 15/2} transition of Er{sup 3+} was observed under 980 nm laser excitation for all Er{sup 3+} doped TiO{sub 2} samples. This result analysis brings insight on understanding of structural, optical and luminescence properties of Er{sup 3+} doped TiO{sub 2} nanoparticles for use in solar cells and bio imaging devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2018

A rapid molecular precursor solid-state route to crystalline Fe 2 GeS 4 nanoparticles

Iron germanium sulfide (Fe 2 GeS 4 ) recently emerged as a potential thin film solar photovoltaic absorber. The introduction of the third element—germanium (Ge)—viewed as a solution for overcoming multiple barriers of a photovoltaic pyrite, confers stability to Fe 2 GeS 4 at elevated temperatures, typically required for accomplishing grain growth in Gen 2 thin film PV. A facile synthesis of Fe 2 GeS 4 nanoparticles from molecular precursors, comprising mechanical mixing of starting materials followed by a two-hour annealing in a sulfur-rich atmosphere is presented herein. Further processing of the resulting Fe 2 GeS 4 nanopowders at elevated temperatures demonstrates high thermal stability of Fe 2 GeS 4 (up to 500 °C), in comparison with pyrite, which shows onset of pyrrhotite upon heating above 160 °C. Based on the secondary crystalline phases formed, here we propose a mechanism of decomposition of Fe 2 GeS 4 at high temperatures. Films fabricated with Fe 2 GeS 4 were further annealed and revealed that Fe 2 GeS 4 withstands high temperatures in thin film.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Polymorphism and Optoelectronic Properties in Crystalline Supramolecular Polymers

Supramolecular polymers can emulate some of the physical properties of covalent polymers but offer new opportunities given the possibility of designing monomers that will form highly ordered assemblies with defined shapes. Internally ordered supramolecular polymers formed through nucleation–elongation self-assembly are well-known but highly crystalline examples which exhibit important properties such as light harvesting, charge transport, and ferroelectricity are not common. We report here on a detailed study of supramolecular polymers formed in water by carboxylated naphtho-p-quinodimethane amphiphiles. We found that supramolecular polymerization of these amphiphiles in aqueous media yields crystalline assemblies with morphologies that included ribbons, helically rolled ribbons, and twisted filaments. This polymorphism was found to be controlled exclusively by repulsive electrostatic interactions controlled by the degree of protonation of the carboxylic head groups which also dictates the nature of supramolecular packing. Substoichiometric amounts of base lead to highly crystalline ribbons due to a decreased surface charge density and less electrostatic repulsion. Increasing deprotonation results in helically rolled ribbons with a different polymorph crystal lattice, whereas excessive deprotonation leads to twisted filaments with maximum surface charge density. Ribbons, helical rolled ribbons, and twisted filaments revealed an increasing red shift in their visible absorption maxima. These crystalline assemblies could be potential candidates for solar energy materials and photocatalytic systems.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Vacancy Control in TiNb 2 O 7 : Implications for Energy Applications

Rapid global electrification, including for transportation, has dramatically increased demand for long-lasting and faster-charging batteries. Titanium niobium oxide (TiNb 2 O 7 ) is one of the most promising anode materials for high-power lithium-ion batteries (LIBs). However, the intrinsic low electronic conductivity of TiNb 2 O 7 is a significant drawback. Herein, an almost 10 orders of magnitude increase in conductivity is achieved via reduction of TiNb 2 O 7 in H 2 at 900 °C. The observed dramatic increase in electron conductivity upon reduction is unprecedented and opens new possibilities to produce niobium-based conductive materials for next-generation energy storage. Upon extended reduction, TiNb 2 O 7 converts into a distorted rutile TiNb 2 O 6 structure, which can be reoxidized back into the crystallographic shear phase. In addition, TiNb 2 O 7 can be thermally reduced in an inert atmosphere and reoxidized by CO 2 with excellent oxygen exchange capacity. Thus, the TiNb 2 O 7 Wadsley–Roth phase demonstrates outstanding potential for solar-driven thermochemical CO 2 splitting at 1400 °C. In conclusion, these findings manifest that controlling defect chemistry paves the way for developing advanced materials for LIBs and solar-driven thermochemical fuel production.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Design of Metastable Tin Titanium Nitride Semiconductor Alloys

Here, we report on design of optoelectronic properties in previously unreported metastable tin titanium nitride alloys with spinel crystal structure. Theoretical calculations predict that Ti alloying in metastable Sn 3 N 4 compound should improve hole effective mass by up to 1 order of magnitude, while other optical bandgaps remains in the 1–2 eV range up to x ~ 0.35 Ti composition. Experimental synthesis of these metastable alloys is predicted to be challenging due to high required nitrogen chemical potential (Δμ N ≥ +1.0 eV) but proven to be possible using combinatorial cosputtering from metal targets in the presence of nitrogen plasma. Characterization experiments confirm that thin films of such (Sn 1–x Ti x ) 3 N 4 alloys can be synthesized up to x = 0.45 composition, with suitable optical band gaps (1.5–2.0 eV), moderate electron densities (10 17 to 10 18 cm –3 ), and improved photogenerated hole transport (by 5×). Overall, this study shows that it is possible to design the metastable nitride materials with properties suitable for potential use in solar energy conversion applications.

14 SOLAR ENERGY↗
DOE OSTI2020

Pressure Effects on the Electronic and Optical Properties in Low-Dimensional Metal Halide Perovskites

Metal halide perovskites have shown enormous potential in perovskite solar cells and light-emitting diodes and made unprecedented progress in the past decade. Additionally, pressure engineering as an effective technique can systematically modify the electronic structures and physical properties of functional materials. Low-dimensional metal halide perovskites (0D, 1D, and 2D) with a variety of compositions have soft lattices that allow pressure to drastically modulate their structures and properties. High-pressure investigations have obtained a comprehensive understanding of their structure–property relationships. Simultaneously, discoveries of novel pressure-driven properties, such as metallization and partially retained band gap narrowing have contributed significantly to the further development of such materials. In this work, we mainly highlight the effect of pressure on the properties and structures of low-dimensional metal halide perovskites, which is essential for designing new perovskite materials and advancing applications.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Ultrafast Triplet Generation at the Lead Halide Perovskite/Rubrene Interface

Triplet sensitization of rubrene by bulk lead halide perovskites has recently resulted in efficient infrared-to-visible photon upconversion via triplet-triplet annihilation. Notably, this process can occur under solar relevant fluxes, potentially paving the way toward integration with photovoltaic devices. In order to further improve the upconversion efficiency, the fundamental photophysical pathways at the perovskite/rubrene interface must be clearly understood to maximize charge extraction. Here, we utilize ultrafast transient absorption spectroscopy to elucidate the processes underlying triplet generation at the perovskite/rubrene interface. In this work, our results point to a triplet generation mechanism based on hot carriers; thermally excited charge carriers in the perovskite cool more rapidly in the presence of rubrene, suggesting rapid extraction of these thermally excited carriers on the picosecond time scale. Subsequent triplet formation in rubrene is observed on a subnanosecond time scale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Bright Silicon Nanocrystals from a Liquid Precursor: Quasi-Direct Recombination with High Quantum Yield

Silicon nanocrystals (SiNCs) with bright bandgap photoluminescence (PL) are of current interest for a range of potential applications, from solar windows to biomedical contrast agents. Here, we use the liquid precursor cyclohexasilane (Si 6 H 12 ) for the plasma synthesis of colloidal SiNCs with exemplary core emission. Here, through size separation executed in an oxygen-shielded environment, we achieve PL quantum yields (QYs) approaching 70% while exposing intrinsic constraints on efficient core emission from smaller SiNCs. Time-resolved PL spectra of these fractions in response to femtosecond pulsed excitation reveal a zero-phonon radiative channel that anticorrelates with QY, which we model using advanced computational methods applied to a 2 nm SiNC. Our results offer additional insight into the photophysical interplay of the nanocrystal surface, quasi-direct recombination, and efficient SiNC core PL.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Mechanistic details for cobalt catalyzed photochemical hydrogen production in aqueous solution: Efficiencies of the photochemical and non-photochemical steps

The use of sunlight to drive chemical reactions that lead to the reduction of water to produce hydrogen is a potential avenue of solar energy utilization. There are many individual steps that take place in this process. This paper reports the investigation of a particular system that involves light absorbing molecules, electron donating agents and a catalyst for water reduction to hydrogen. We evaluated the efficiency of the light induced formation of a strong electron donor, the use of this donor to reduce the catalyst and finally the efficiency of the catalyst to produce hydrogen from water. From this, the sources of loss of efficiency could be clearly identified and used in the design of better systems to produce hydrogen from water.

14 SOLAR ENERGY↗
DOE OSTI2014

Faradaurate-940: Synthesis, Mass Spectrometry, STEM, PDF, and SAXS Study of Au~940(SR)~160 Nanocrystals

Obtaining monodisperse nanocrystals, and determining its composition to the atomic level and its atomic structure is highly desirable, but is generally lacking. Here, we report the discovery and comprehensive characterization of a 3-nm plasmonic nanocrystal with a composition of Au940 20(SCH2CH2Ph)160 4, which is, the largest mass spectrometrically characterized gold thiolate nanoparticle produced to date. The compositional assignment has been made using electrospray ionization (ESI) and matrix assisted laser desorption ionization (MALDI) mass spectrometry (MS). The MS results show an unprecedented size monodispersity, where the number of Au atoms vary by only 40 atoms (940 20). The mass spectrometrically-determined size and composition are supported by aberration-corrected scanning transmission electron microscopy (STEM) and synchrotron-based methods such as atomic pair distribution function (PDF) and small angle X-ray scattering (SAXS). Lower resolution STEM images show an ensemble of particles 1000 s per frame visually demonstrating monodispersity. Modelling of SAXS on statistically significant nanoparticle population approximately 1012 individual nanoparticles - shows that the diameter is 3.0 0.2nm, supporting mass spectrometry and electron microscopy results on monodispersity. Atomic PDF based on high energy X-ray diffraction experiments show decent match with either a Marks decahedral or truncated octrahedral structure. Atomic resolution STEM images of single particles and its FFT suggest face-centered cubic (fcc) arrangement. UV-visible spectroscopy data shows that the 940-atom size supports a surface plasmon resonance peak at 505 nm. These monodisperse plasmonic nanoparticles minimize averaging effects and has potential application in solar cells, nano-optical devices, catalysis and drug delivery.

Kumara, Chanaka↗
DOE OSTI2015

An allosteric photoredox catalyst inspired by photosynthetic machinery

Biological photosynthetic machinery allosterically regulate light harvesting via conformational and electronic changes at the antenna protein complexes as a response to specific chemical inputs. Fundamental limitations in current approaches to regulating inorganic light-harvesting mimics prevent their use in catalysis. Here we show that a light-harvesting antenna/reaction centre mimic can be regulated by utilizing a coordination framework incorporating antenna hemilabile ligands and assembled via a high-yielding, modular approach. As in nature, allosteric regulation is afforded by coupling the conformational changes to the disruptions in the electrochemical landscape of the framework upon recognition of specific coordinating analytes. The hemilabile ligands enable switching using remarkably mild and redox-inactive inputs, allowing one to regulate the photoredox catalytic activity of the photosynthetic mimic reversibly and in situ . Furthermore, we demonstrate that bioinspired regulatory mechanisms can be applied to inorganic light-harvesting arrays displaying switchable catalytic properties and with potential uses in solar energy conversion and photonic devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

High-performance light-driven heterogeneous CO 2 catalysis with near-unity selectivity on metal phosphides

Akin to single-site homogeneous catalysis, a long sought-after goal is to achieve reaction site precision in heterogeneous catalysis for chemical control over patterns of activity, selectivity and stability. Herein, we report on metal phosphides as a class of material capable of realizing these attributes and unlock their potential in solar-driven CO 2 hydrogenation. Selected as an archetype, Ni 12 P 5 affords a structure based upon highly dispersed nickel nanoclusters integrated into a phosphorus lattice that harvest light intensely across the entire solar spectral range. Motivated by its panchromatic absorption and unique linearly bonded nickel-carbonyl-dominated reaction route, Ni 12 P 5 is found to be a photothermal catalyst for the reverse water gas shift reaction, offering a CO production rate of 960 ± 12 mmol g cat –1 h –1 , near 100% selectivity and long-term stability. Successful extension of this idea to Co2P analogs implies that metal phosphide materials are poised as a universal platform for high-rate and highly selective photothermal CO 2 catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Plasmon-enhanced ultralow-threshold solid-state triplet fusion upconversion

Triplet fusion upconversion has potential applications in solar cells, photoredox catalysis, additive manufacturing and bioimaging. However, solid-state upconversion systems have struggled to measure up to their solution-phase counterparts, often requiring enormous optical power densities to operate at the maximum efficiency. Here we substantially improve the performance of upconversion films through excitation with surface plasmons that propagate along a planar silver-film interface, leading to an absorption enhancement that reduces the intensity threshold I th by a factor of 19 and enhances the external quantum efficiency by a factor of 17. From this, we achieve I th values as low as 3.4 mW cm −2 and an external quantum efficiency up to 0.094%. To demonstrate real-world viability, we couple the upconversion film to plasmons generated by the near-field of excitons in an organic light-emitting diode. As a result, this scheme is then used to fabricate a white-emitting organic light-emitting diode where blue emission sources from plasmon-excited upconversion, achieving a high colour rendering index of 86.2 and setting precedent for blue emission in the absence of high-energy polarons or triplets.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Overcoming Carrier Concentration Limits in Polycrystalline CdTe Thin Films with In Situ Doping

Abstract Thin film materials for photovoltaics such as cadmium telluride (CdTe), copper-indium diselenide-based chalcopyrites (CIGS), and lead iodide-based perovskites offer the potential of lower solar module capital costs and improved performance to microcrystalline silicon. However, for decades understanding and controlling hole and electron concentration in these polycrystalline films has been extremely challenging and limiting. Ionic bonding between constituent atoms often leads to tenacious intrinsic compensating defect chemistries that are difficult to control. Device modeling indicates that increasing CdTe hole density while retaining carrier lifetimes of several nanoseconds can increase solar cell efficiency to 25%. This paper describes in-situ Sb, As, and P doping and post-growth annealing that increases hole density from historic 10 14 limits to 10 16 –10 17 cm −3 levels without compromising lifetime in thin polycrystalline CdTe films, which opens paths to advance solar performance and achieve costs below conventional electricity sources.

14 SOLAR ENERGY↗
DOE OSTI2013

New Insights into Dynamics and Morphology of P3HT:PCBM Active Layers in Bulk Heterojunctions

Organic photovoltaics (OPVs) are topic of extensive research for their potential application in solar cells. Recent work has led to the development of a coarse-grained model for studying poly(3-hexylthiophene) (P3HT) and [6,6]-phenyl-C 61 -butyric acid methyl ester (PCBM) blends with molecular simulations. Here we provide further validation of the force field and use it to study the thermal annealing process of P3HT:PCBM blends. A key finding of our study is that, in contrast to a previous report, the annealing process does not converge at the short time scales reported. Rather, we find that the self assembly of the blends is characterized by three rate dependent stages that require much longer simulations to approach convergence. Using state-of-the- art high performance computing, we are able to study annealing at length and time scales commensurate with devices used in experiments. Our simulations show different phase segregated morphologies dependent on the P3HT chain length and PCBM volume fraction in the blend. For short chain lengths, we observed a smectic morphology containing alternate P3HT and PCBM domains. In contrast, a phase segregated morphology containing domains of P3HT and PCBM distributed randomly in space is found for longer chain lengths. Theoretical arguments justifying stabilization of these morphologies due to shape anisotropy of P3HT (rod-like) and PCBM (sphere-like) are presented. Furthermore, results on structure factor, miscibility of P3HT and PCBM, domain spacing and kinetics of phase segregation in the blends are presented in detail. Qualitative comparison of these results with small-angle neutron scattering experiments from literature is presented and an excellent agreement is found.

14 SOLAR ENERGY↗