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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 577 records · Page 32
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Strain-Driven Nanoscale Phase Competition near the Antipolar–Nonpolar Phase Boundary in Bi 0.7 La 0.3 FeO 3 Thin Films

Complex-oxide materials tuned to be near phase boundaries via chemistry/composition, temperature, pressure, etc. are known to exhibit large susceptibilities. Here, we observe a strain-driven nanoscale phase competition in epitaxially constrained Bi 0.7 La 0.3 FeO 3 thin films near the antipolar-nonpolar phase boundary and explore the evolution of the structural, dielectric, (anti)ferroelectric, and magnetic properties with strain. We find that compressive and tensile strains can stabilize an antipolar PbZrO 3 -like Pbam phase and a nonpolar Pnma orthorhombic phase, respectively. Heterostructures grown with little to no strain exhibit a self-assembled nanoscale mixture of the two orthorhombic phases, wherein the relative fraction of each phase can be modified with film thickness. Subsequent investigation of the dielectric and (anti)ferroelectric properties reveals an electric-field-driven phase transformation from the nonpolar phase to the antipolar phase. X-ray linear dichroism reveals that the antiferromagnetic-spin axes can be effectively modified by the strain-induced phase transition. This evolution of antiferromagnetic-spin axes can be leveraged in exchange coupling between the antiferromagnetic Bi 0.7 La 0.3 FeO 3 and a ferromagnetic Co0.9Fe0.1 layer to tune the ferromagnetic easy axis of the Co 0.9 Fe 0.1 . These results demonstrate that besides chemical alloying, epitaxial strain is an alternative and effective way to modify subtle phase relations and tune physical properties in rare earth-alloyed BiFeO 3 . Furthermore, the observation of antiferroelectric-antiferromagnetic properties in the Pbam Bi 0.7 La 0.3 FeO 3 phase could be of significant scientific interest and great potential in magnetoelectric devices because of its dual antiferroic nature.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Direct Deposition of Crystalline Ta 3 N 5 Thin Films on FTO for PEC Water Splitting

Tantalum Nitride is a promising photoanode material for solar water splitting, but the further study and practical use is constrained by the harsh conditions of the synthesis from Ta metal. Here we report the direct deposition of crystalline Ta 3 N 5 on FTO substrate via a custom-built ALD system. A combination of TaCl 5 (Ta-precursor) and ammonia (N-source) were sequentially pulsed into the ALD reactor with the substrate heated to 550 °C to deposit compact and thin films of Ta 3 N 5 with controllable thicknesses on FTO substrates. Importantly, it is shown that the FTO is chemically and structurally stable under the reducing conditions of ammonia at 550 °C. These electrodes produced an exceptional photocurrent onset potential of ~ 0.3 V vs. RHE with a maximum photocurrent of ~ 2.4 mA cm -2 at 1.23 V vs RHE. Results of photoelectrochemical investigations as a function of film thickness and illumination direction reveal that the performance of Ta 3 N 5 is controlled by a hole diffusion length of ~50 nm. These results are crucial for the successful integration of Ta 3 N 5 in efficient unassisted water splitting applications.

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

Reaction of Pb(II) and Zn(II) with Ethyl Linoleate To Form Structured Hybrid Inorganic–Organic Complexes: A Model for Degradation in Historic Paint Films

To investigate soap formation in drying oils in historic paints, the reaction between metal acetates (K + , Zn 2+ , Pb 2+ ) and ethyl linoleate (EL) was studied using optical microscopy, X-ray powder diffraction, and electron microscopy. Pb(II) and Zn(II) react rapidly with EL to form highly structured, spherulitic, luminescent crystallites that aggregate. Evidence from Fourier transform infrared (FTIR) and scanning electron microscopy/energy dispersive X-ray analysis and high-resolution synchrotron powder X-ray diffraction indicates that these are organic–inorganic hybrid complexes or coordination polymers. FTIR absorbance peaks at ca. 1540 cm –1 for Pb(II) and ca. 1580 cm –1 for Zn(II) are consistent with the formation of carboxylate complexes. The complexes formed offer insight into the degradation processes observed in oil paint films, suggesting that soap formation is rapid when metal ions are solubilized and can occur with unsaturated fatty acids that are present in fresh oils. These complexes may account for the atypical luminescence observed in lead-containing cured oil paint films.

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

Dynamically Disordered Lattice in a Layered Pb-I-SCN Perovskite Thin Film Probed by Two-Dimensional Infrared Spectroscopy

The dynamically flexible lattices in lead-halide perovskites may play important roles in extending carrier recombination lifetime in 3D perovskite solar-cell absorbers and in exciton self-trapping in 2D perovskite white-light phosphors. Here, two-dimensional infrared (2D IR) spectroscopy was applied to study a recently reported Pb-I-SCN layered perovskite. The Pb-ISCN perovskite was spin-coated on a SiO 2 surface as a thin film, with a thickness of ~100 nm, where the S 12 CN – anions were isotopically diluted with the ratio of S 12 CN:S 13 CN=5:95 or 1:99 to avoid vibrational coupling and excitation transfer between adjacent SCN – anions. The minor S 12 CN – component was the principal vibrational probe that reported on the structural evolution through 2D IR spectroscopy. Spectral diffusion was observed with a time constant of 4.1 ± 0.3 ps. Spectral diffusion arises from small structural changes that result in sampling of frequencies within the distribution of frequencies that comprise the inhomogeneously broadened absorption spectrum of the in the Pb-I-SCN layered perovskite. These transitions among discrete local structures are distinct from oscillatory phonon motions of the lattice. To accurately evaluate the structural dynamics through measurement of spectral diffusion, the vibrational coupling between adjacent SCN – anions had to be carefully treated. Although the inorganic layers of typical 2D perovskites are structurally isolated from each other, the 2D IR data demonstrated that the layers of the Pb-I-SCN perovskite are vibrationally coupled. When both S 12 CN – and S 13 CN – were pumped simultaneously, cross-peaks between S 12 CN and S 13 CN vibrations and an oscillating 2D band shape of the S 12 CN – vibration were observed. Both observables demonstrate vibrational coupling between the closest SCN – anions, which reside in different inorganic layers. The thin films and the isotopic dilution produced exceedingly small vibrational echo signal fields; measurements were made possible using the near-Brewster’s angle reflection pump-probe geometry.

14 SOLAR ENERGY↗
DOE OSTI2013

Adsorption and Reaction of Methanol over CeO X (100) Thin Films

Methanol was adsorbed on oxidized and reduced CeO X (100) thin films to probe the active sites and reaction selectivity of these surfaces compared to those of CeO X (111). Roughly twice as much methoxy was formed on oxidized CeO 2 (100) compared to that formed on CeO 2 (111). In addition to more methoxy, hydroxyl is also more stable on CeO 2 (100). Unlike on CeO 2 (111), however, methanol on CeO 2 (100) produced CO, CO 2 , and H 2 in addition to water and formaldehyde. The behavior of CeO 2 (100) is related to its surface structure, which provides greater access to Ce cations and therefore more active adsorption sites and more highly undercoordinated Ce and O. The undercoordinated O may explain the enhanced dehydrogenation activity leading to CO and H 2 formation. The reduction of ceria leads to increased methanol uptake on both CeO 2 – X (100) and CeO 2 – X (111). However, although the uptake doubled on reduced CeO 2 – X (111) compared to the oxidized surface, it increased by only 10% on reduced CeO 2 – X (100) compared to that on fully oxidized CeO 2 (100). Reduction of both surfaces leads to a greater production of CO and H 2 . Reaction on all surfaces progresses rapidly from methoxy to products. Lastly, there is no spectroscopic evidence of formyl or formate intermediates. On CeO X (100), carbonate is detected that decomposes into CO 2 at high temperature.

Albrecht, P↗
DOE OSTI2012

Charge Trapping in Bright and Dark States of Coupled PbS Quantum Dot Films

Analysis of photoluminescence (PL) from chemically treated lead sulfide (PbS) quantum dot (QD) films versus temperature reveals the effects of QD size and ligand binding on the motion of carriers between bright and dark trap states. For strongly coupled QDs, the PL exhibits temperature-dependent quenching and shifting consistent with charges residing in a shallow exponential tail of quasi-localized states below the band gap. The depth of the tail varies from 15 to 40 meV, similar to or smaller than exponential band tail widths measured for polycrystalline Si. The trap state distribution can be manipulated with QD size and surface treatment, and its characterization should provide a clearer picture of charge separation and percolation in disordered QD films than what currently exists.

14 SOLAR ENERGY↗
DOE OSTI2016

Thin-film ferroelectric materials and their applications

Ferroelectric materials, because of their robust spontaneous electrical polarization, are widely used in various applications. Recent advances in modelling, synthesis and characterization techniques are spurring unprecedented advances in the study of these materials. In this Review, we focus on thin-film ferroelectric materials and, in particular, on the possibility of controlling their properties through the application of strain engineering in conventional and unconventional ways. We explore how the study of ferroelectric materials has expanded our understanding of fundamental effects, enabled the discovery of novel phases and physics, and allowed unprecedented control of materials properties. We discuss several exciting possibilities for the development of new devices, including those in electronic, thermal and photovoltaic applications, and transduction sensors and actuators. We conclude with a brief survey of the different directions that the field may expand to over the coming years.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Enhanced photoelectrochemical efficiency and stability using a conformal TiO 2 film on a black silicon photoanode

Black silicon (b-Si) is a surface-nanostructured Si with extremely efficient light absorption capability and is therefore of interest for solar energy conversion. However, intense charge recombination and low electrochemical stability limit the use of b-Si in photoelectrochemical solar-fuel production. Here we report that a conformal, ultrathin, amorphous TiO 2 film deposited by low-temperature atomic layer deposition (ALD) on top of b-Si can simultaneously address both of these issues. Combined with a Co(OH) 2 thin film as the oxygen evolution catalyst, this b-Si/TiO 2 /Co(OH) 2 heterostructured photoanode was able to produce a saturated photocurrent density of 32.3 mA cm –2 at an external potential of 1.48 V versus reversible reference electrode (RHE) in 1 M NaOH electrolyte. The enhanced photocurrent relative to planar Si and unprotected b-Si photoelectrodes was attributed to the enhanced charge separation efficiency as a result of the effective passivation of defective sites on the b-Si surface. The 8-nm ALD TiO 2 layer extends the operational lifetime of b-Si from less than half an hour to four hours.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Spectral control of nonclassical light pulses using an integrated thin-film lithium niobate modulator

Abstract Manipulating the frequency and bandwidth of nonclassical light is essential for implementing frequency-encoded/multiplexed quantum computation, communication, and networking protocols, and for bridging spectral mismatch among various quantum systems. However, quantum spectral control requires a strong nonlinearity mediated by light, microwave, or acoustics, which is challenging to realize with high efficiency, low noise, and on an integrated chip. Here, we demonstrate both frequency shifting and bandwidth compression of heralded single-photon pulses using an integrated thin-film lithium niobate (TFLN) phase modulator. We achieve record-high electro-optic frequency shearing of telecom single photons over terahertz range (±641 GHz or ±5.2 nm), enabling high visibility quantum interference between frequency-nondegenerate photon pairs. We further operate the modulator as a time lens and demonstrate over eighteen-fold (6.55 nm to 0.35 nm) bandwidth compression of single photons. Our results showcase the viability and promise of on-chip quantum spectral control for scalable photonic quantum information processing.

Optics↗