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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 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Exploring the influence of interfacial solvation on electrochemical CO 2 reduction using plasmon‐enhanced vibrational sum frequency generation spectroscopy

Although interfacial solvation plays an important role in determining carbon dioxide reduction (CO 2 R) kinetics, present understanding of the potential dependent properties of the electrochemical double layer under conditions relevant for CO 2 R remains limited. This article summarizes the development and recent applications of plasmon-enhanced vibrational sum frequency generation (VSFG) spectroscopy to study the effects of cation hydration and interfacial solvation on CO 2 R using CO as a vibrational Stark reporter. Results show that electrolyte cations retain their entire solvation shell upon adsorption to inactive sites, while active sites retain only a single water layer between the gold surface and the cation. Measurements also show that the total interfacial electric field can be separated into two contributions: one from the electrochemical double layer (Stern field) and another from the polar solvation environment (Onsager field). Surprisingly, correlating VSFG spectra with reaction kinetics reveals that it is the solvation-mediated Onsager field that governs the chemical reactivity at the electrode/electrolyte interface. Measuring the interfacial water spectra during electrocatalysis also provides evidence for the proton source during H2 evolution, which competes with CO 2 R in aqueous electrolyte. These findings highlight the importance of directly probing cation hydration and interfacial solvation, which mediates reaction kinetics at electrochemical interfaces.

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

Effects of ion adsorption on graphene oxide films and interfacial water structure: A molecular-scale description

Herein we discuss graphene oxide as a promising, emerging separation material, as it is durable, dispersible in water, and has naturally forming functional groups. Bulk studies using graphene oxide flakes have demonstrated impressive metal adsorption. However, little interfacial information about water and metal organization near graphene oxide is available. A mechanistic understanding of water and ions interactions with graphene oxide films is critical toward advanced separations, including improved sorption efficiency and membrane regeneration. We study metal ion and local water organization near graphene oxide thin films formed at the air/water interface. These films are not typical membranes and allow us to determine nanoscale information about the graphene oxide-water interface. We accomplish this with x-ray reflectivity (XR), x-ray fluorescence near total reflection (XFNTR), and vibrational sum frequency generation spectroscopy (SFG). These interface-specific techniques provide the electron density profile normal to the interface, number of adsorbed ions, and information about the orientational ordering and hydrogen-bonding network of interfacial water, respectively. Via XFNTR and SFG, we find that trivalent yttrium ions preferentially adsorb to graphene oxide and affect its structure, compared to divalent strontium and monovalent cesium ions. Two different interfacial water populations can be described, based on their hydrogen bonding strength, and the adsorbed ions affect these populations differently. These results provide fundamental information about ion and water organization at the interface and help address the large computational-experimental agreement gap for graphene oxide systems. Additionally, they are relevant for improved soft-scaffold graphene oxide membranes and downstream applications.

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

Damping coating with a constraint layer

A coating is applied to a base material. The coating comprises a viscoelastic layer having a surface in which cavities are formed; and a constraint layer. The viscoelastic layer is disposed on the base material, and the constraint layer is disposed on, and partially bonded, at an interface, to the viscoelastic layer over the surface in which the cavities are formed. The cavities are filled with particles configured for vibration and frictional interaction at the partially bonded interface between the partially bonded viscoelastic layer and the constraint layer. A turbine blade having an airfoil with the subject coating is also provided.

Zhang, James↗
DOE OSTI2022

Variable Daily Autocorrelation Functions of High-Frequency Seismic Data on Mars

Abstract High-frequency seismic data on Mars are dominated by wind-generated lander vibrations, which are radiated partially to the subsurface. Autocorrelation functions (ACFs) of seismic data on Mars filtered between 1 and 5 Hz show clear phases at ∼1.3, ∼2.6, and ∼3.9 s. Daily temporal changes of their arrival times (dt/t) correlate well with the daily changes of ground temperature, with ∼5% daily variation and ∼50 min apparent phase delay. The following two mechanisms could explain the observations: (1) the interference of two predominant spectral peaks at ∼3.3 and ∼4.1 Hz, assumed to be both lander resonance modes, generate the apparent arrivals in the ACFs; (2) the interference of the lander vibration and its reflection from an interface ∼200 m below the lander generate the 3.3 Hz spectral peak and ∼1.3 s arrival in the ACFs. The driving mechanism of the resolved dt/t that most likely explains the ∼50 min delay is thermoelastic strain at a near-surface layer, affecting the lander–ground coupling and subsurface structures. The two outlined mechanisms suggest, respectively, up to ∼10% changes in ground stiffness at 1–5 Hz and ∼15% velocity changes in the top ∼20 m layer. These are upper bound values considering also other possible contributions. The presented methodology and results contribute to analysis of ACFs with limited data and the understanding of subsurface materials on Mars.

Geochemistry & Geophysics↗
DOE OSTI2022

The Unexpected Role of Cations in the Self-Assembly of Positively Charged Amphiphiles at Liquid/Liquid Interfaces

Conventional wisdom suggests that cations play a minimal role in the assembly of cationic amphiphiles. Here, we show that at liquid/liquid (L/L) interfaces, specific cation effects can modulate the assemblies of hydrophobic tails in an oil phase despite being attached to cationic headgroups in the aqueous phase. In this work, we used oligo-dimethylsiloxane (ODMS) methyl imidazolium amphiphiles to identify these specific interactions at hexadecane/aqueous interfaces. Small cations, such as Li + , bind to the O atoms in the ODMS tail and pin it to the interface, thereby imposing a kinked conformation-as evidenced by vibrational sum frequency generation spectroscopy and molecular dynamics simulations. While larger Cs + ions more readily partition to the interface, they do not form analogous complexes. Our data not only point to ways for controlling amphiphile structure at L/L interfaces but also suggest a means for the separation of Li + , or related applications, in soft-matter electronics.

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

Negative refraction in hyperbolic hetero-bicrystals

We visualized negative refraction of phonon polaritons, which occurs at the interface between two natural crystals. The polaritons—hybrids of infrared photons and lattice vibrations—form collimated rays that display negative refraction when passing through a planar interface between the two hyperbolic van der Waals materials: molybdenum oxide (MoO 3 ) and isotopically pure hexagonal boron nitride (h 11 BN). At a special frequency ω 0 , these rays can circulate along closed diamond-shaped trajectories. We have shown that polariton eigenmodes display regions of both positive and negative dispersion interrupted by multiple gaps that result from polaritonic-level repulsion and strong coupling.

Science & Technology - Other Topics↗
DOE OSTI2025

Vibrational sum frequency generation spectroscopy reveals the inertness of chromium oxide (001) surfaces

Nanoengineered metal oxides such as Cr(III)-oxide (chromia) films have diverse potential applications in corrosion inhibition, remediation, energy generation, catalysis, data storage, and biological and environmental systems. Concerns about material degradation or oxidation to toxic chromate necessitate an understanding of chromia/aqueous interfaces, beginning with their hydroxylation and hydration behavior. Vibrational sum-frequency generation spectroscopy (vSFG) provides specific molecular-level information about water at the oxide/aqueous junction with high surface selectivity. To overcome the strong absorber problem typical of certain metal oxides in the UV–visible range during nonlinear optical studies, we employed molecular beam epitaxy to deposit transparent, epitaxial nanofilms of Cr 2 O 3 with (001) crystalline orientation on sapphire (Al 2 O 3 (001)) substrates, as confirmed by atomic force microscopy and X-ray diffraction. vSFG spectra of the air and water interfaces of the Cr 2 O 3 (001) films reveal hydroxyl features corresponding to both dissociated and molecular water on the surface. In contrast to the dangling hydroxyls found on the bare Al 2 O 3 (001) substrate, the hydroxyl groups on the deposited Cr 2 O 3 (001) nanofilm do not readily undergo isotopic H/D exchange when exposed to varying forms of D 2 O under ambient conditions. When considering the chemistries of the corresponding trivalent cations in aqueous solution, the finding is at variance with their similar acidities and proton exchange dynamics but consistent with markedly slower inner-sphere water ligand exchange of hexaquo Cr 3+ . This finding challenges the idea that proton and water exchange at the water/Cr₂O₃(001) interface are solely correlated, driven by the strength of metal-bridging oxygen bonds and surface hydroxyl distribution, without direct causation.

Boamah-Agyemang, Mavis D. [Pacific Northwest Natio↗
DOE OSTI2025

A nonlinear optical perspective on the chemistry at liquid/liquid interfaces

In this review, we discuss some of the subtle (and not-so-subtle) rules that govern chemistry and transport at liquid/liquid (L/L) interfaces. An overview of the importance of L/L interfaces is provided with context about why these interfaces are so challenging to study. Emphasis is placed on the use of vibrational sum-frequency generation (SFG), a surface-specific spectroscopy, to probe these interfaces at and away from equilibrium. Highlights from our laboratory’s work probing these interfaces in the context of chemical separations and soft-matter electronics are discussed. In conclusion, revealing the rules that govern self-assembly, chemical recognition, and transport at these dynamic, highly heterogeneous interfaces can allow formulation of avenues to control chemical and physical transformations, impacting a range of basic and applied fields.

Doughty, Benjamin L. [Oak Ridge National Laborator↗
DOE OSTI2024

Interfacial Nanostructure and Hydrogen Bond Networks of Choline Chloride and Glycerol Mixtures Probed with X-ray and Vibrational Spectroscopies

The molecular distribution at the liquid-vapor interface and evolution of the hydrogen bond interactions in mixtures of glycerol and choline chloride are investigated using X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy. Nanoscale depth profiles of supersaturated deep eutectic solvent (DES) mixtures up to ~2 nm measured by ambient-pressure XPS show the enhancement of choline cation (Ch + ) concentration by a factor of 2 at the liquid-vapor interface compared to the bulk. In addition, Raman spectral analysis of a wide range of DES mixtures reveals the conversion of gauche-conformer Ch + into the anti-conformer in relatively lower ChCl concentrations. Finally, the depletion of Ch + from the interface (probing depth = 0.4 nm) is demonstrated by aerosol-based velocity map imaging XPS measurements of glyceline and water mixtures. The nanostructure of liquid-vapor interfaces and structural rearrangement by hydration can provide critical insight into the molecular origin of the deep eutectic behavior and gas-capturing application of DESs.

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

Electro-optic transduction in silicon via gigahertz-frequency nanomechanics

Interfacing electronics with optical fiber networks is key to the long-distance transfer of classical and quantum information. Piezo-optomechanical transducers enable such interfaces by using gigahertz-frequency acoustic vibrations as mediators for converting microwave photons to optical photons via the combination of optomechanical and piezoelectric interactions. However, despite successful demonstrations, efficient quantum transduction remains out of reach due to the challenges associated with hybrid material integration and increased loss from piezoelectric materials when operating in the quantum regime. Here, we demonstrate an alternative approach in which we actuate 5-GHz phonons in a conventional silicon-on-insulator platform. In our experiment, microwave photons resonantly drive a phononic crystal oscillator via the electrostatic force realized in a charge-biased narrow-gap capacitor. The mechanical vibrations are subsequently transferred via a phonon waveguide to an optomechanical cavity, where they transform into optical photons in the sideband of a pump laser field. Operating at room temperature and atmospheric pressure, we measure a microwave-to-optical photon conversion efficiency of 1.72±0.14×10 −7 in a 3.3 MHz bandwidth. Our results mark a stepping stone towards quantum transduction with integrated devices made from crystalline silicon, which promise efficient high-bandwidth operation and integration with superconducting qubits. Additionally, the lack of need for piezoelectricity or other intrinsic nonlinearities makes our approach applicable to a wide range of materials for potential applications beyond quantum technologies.

42 ENGINEERING↗
DOE OSTI2022

Structural measurement of electron-phonon coupling and electronic thermal transport across a metal-semiconductor interface

Scattering of energetic charge carriers and their coupling to lattice vibrations (phonons) in dielectric materials and semiconductors are crucial processes that determine the functional limits of optoelectronics, photovoltaics, and photocatalysts. The strength of these energy exchanges is often described by the electron-phonon coupling coefficient, which is difficult to measure due to the microscopic time- and length-scales involved. In the present study, we propose an alternate means to quantify the coupling parameter along with thermal boundary resistance and electron conductivity by performing a high angular-resolution time-resolved X-ray diffraction measurement of propagating lattice deformation following laser excitation of a nanoscale, polycrystalline metal film on a semiconductor substrate. Our data present direct experimental evidence for identifying the ballistic and diffusive transport components occurring at the interface, where only the latter participates in thermal diffusion. This approach provides a robust measurement that can be applied to investigate microscopic energy transport in various solid-state materials.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Trapping light in air with membrane metasurfaces for vibrational strong coupling

Optical metasurfaces can manipulate electromagnetic waves in unprecedented ways at ultra-thin engineered interfaces. Specifically, in the mid-infrared (mid-IR) region, metasurfaces have enabled numerous biochemical sensing, spectroscopy, and vibrational strong coupling (VSC) applications via enhanced light-matter interactions in resonant cavities. However, mid-IR metasurfaces are usually fabricated on solid supporting substrates, which degrade resonance quality factors (Q) and hinder efficient sample access to the near-field electromagnetic hotspots. Besides, typical IR-transparent substrate materials with low refractive indices, such as CaF 2 , NaCl, KBr, and ZnSe, are usually either water-soluble, expensive, or not compatible with low-cost mass manufacturing processes. Here, we present novel free-standing Si-membrane mid-IR metasurfaces with strong light-trapping capabilities in accessible air voids. We employ the Brillouin zone folding technique to excite tunable, high-Q quasi-bound states in the continuum (qBIC) resonances with our highest measured Q-factor of 722. Leveraging the strong field localizations in accessible air cavities, we demonstrate VSC with multiple quantities of PMMA molecules and the qBIC modes at various detuning frequencies. Our new approach of fabricating mid-IR metasurfaces into semiconductor membranes enables scalable manufacturing of mid-IR photonic devices and provides exciting opportunities for quantum-coherent light-matter interactions, biochemical sensing, and polaritonic chemistry. The authors introduce a mid-IR metasurface fabricated by decorating a free-standing Si-membrane with air holes. The enhanced light-matter interactions in such air cavities enable vibrational strong coupling and advanced biochemical sensing.

infrared spectroscopy↗
DOE OSTI2024

Synergistic Assembly of Charged Oligomers and Amino Acids at the Air–Water Interface: An Avenue toward Surface-Directed CO 2 Capture

Interfaces are considered a major bottleneck in the capture of CO 2 from air. Efforts to design surfaces to enhance CO 2 capture probabilities are challenging due to the remarkably poor understanding of chemistry and self-assembly taking place at these interfaces. In this report we leverage surface-specific vibrational spectroscopy, Langmuir trough techniques, and simulations to mechanistically elucidate how cationic oligomers can drive surface localization of amino acids (AAs) that serve as CO 2 capture agents speeding up the apparent rate of absorption. We demonstrate how tuning these interfaces provides a means to facilitate CO 2 capture chemistry to occur at the interface, while lowering surface tension and improving transport/reaction probabilities. We show that in the presence of interfacial AA-rich aggregates, one can improve capture probabilities vs that of a bare interface, which holds promise in addressing climate change through the removal of CO 2 via tailored interfaces and associated chemistries.

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

Contribution of the Hydroxyl Group on Interfacial Heat Conduction of Monohydric Alcohols: A Molecular Dynamics Study

Monohydric alcohols have been used as promising phase change materials (PCMs) for low-temperature latent heat storage. However, the heat storage/retrieval rates are limited due to the low thermal conductivity of such alcohols. In this work, nonequilibrium molecular dynamics (NEMD) simulations were performed to study the microscopic heat conduction in example monohydric alcohols, i.e., 1-dodecanol (C12H26O), 1-tetradecanol (C14H30O), and 1-hexadecanol (C16H34O). A simplified ideal crystal model was proposed to exploit the potential for improving the thermal conductivity of monohydric alcohols. The effect of ideal crystalline structures, especially the contribution of the hydroxyl group, on the microscopic heat conduction process was analyzed. The thermal conductivity of the ideal crystals of the various monohydric alcohols was predicted to be more than twice as compared to that of their respective solids. The major thermal resistance in the ideal crystals was found around the molecular interfaces, as a result of the excellent heat conduction performance along the linear molecular chains. The calculated vibrational density of states (VDOS) and interfacial heat transfer were then investigated. When the interfaces are surrounded by hydroxyl groups as walls, strong hydrogen bond (HB) interactions were observed. The interfacial heat transfer coefficient of the ideal crystalline structures of 1-tetradecanol was found to reach up to ~735.6 MW/m2 W. It was elucidated that the high interfacial heat transfer rate is clearly related to the stronger intermolecular interactions.

Engineering↗
DOE OSTI2026

Interfacial Inversion of Stealth Surfactants

Amphiphilic macromolecular surfactants segregate to liquid–liquid interfaces, thereby reducing the interfacial tension and free energy. Here, we investigated “stealth surfactants” in the form of core–shell bottlebrush polymers comprised of pH-responsive diblock copolymer side chains forming a hydrophilic core and a hydrophobic shell, enabling solubility in oil. At liquid–liquid interfaces, these polymers undergo a structural “inversion”, with hydrophilic blocks segregating into the aqueous phase and hydrophobic blocks residing in the oil phase. The reconfiguration kinetics and surfactant properties are influenced by multiple factors, including the molecular weights of the backbone and side chain components, the hydrophilic-to-hydrophobic balance of the side chains, and the pH of the aqueous phase. An observed nonmonotonic dependence of interfacial tension with time is attributed to a progressive structural inversion, where the projected area of the macromolecule onto the interface decreases. To validate this inversion hypothesis, interfacial properties were characterized by sum-frequency generation vibrational spectroscopy, which revealed configurational changes of the core–shell bottlebrush polymers at the fluid interface and revealed a pH-dependent interfacial coverage. Coarse-grained molecular dynamics simulations supported these experimental findings, showing that the pH-responsive core and hydrophobic shell assume a time-averaged configuration with orientations parallel and perpendicular to the plane of the interface, respectively. These findings open routes to design multistimuli-responsive polymeric surfactants and compatibilizers, expanding their potential applications in advanced interfacial systems.

Stealth surfactants↗
DOE OSTI2025

Electrical Transport Interplay with Charge Density Waves, Magnetization, and Disorder Tuned by 2D van der Waals Interface Modification via Elemental Intercalation and Substitution in ZrTe 3 , 2H-TaS 2 , and Cr 2 Si 2 Te 6 Crystals

Electrical transport in 2D materials exhibits unique behaviors due to reduced dimensionality, broken symmetries, and quantum confinement. It serves as both a sensitive probe for the emergence of coherent electronic phases and a tool to actively manipulate many-body correlated states. Exploring their interplay and interdependence is crucial but remains underexplored. This review integratively cross-examines the atomic and electronic structures and transport properties of van der Waals-layered crystals ZrTe 3 , 2H-TaS 2 , and Cr 2 Si 2 Te 6 , providing a comprehensive understanding and uncovering new discoveries and insights. A common observation from these crystals is that modifying the atomic and electronic interface structures of 2D van der Waals interfaces using heteroatoms significantly influences the emergence and stability of coherent phases, as well as phase-sensitive transport responses. In ZrTe 3 , substitution and intercalation with Se, Hf, Cu, or Ni at the 2D vdW interface alter phonon–electron coupling, valence states, and the quasi-1D interface Fermi band, affecting the onset of CDW and SC, manifested as resistance upturns and zero-resistance states. We conclude here that these phenomena originate from dopant-induced variations in the lattice spacing of the quasi-1D Te chains of the 2D vdW interface, and propose an unconventional superconducting mechanism driven by valence fluctuations at the van Hove singularity, arising from quasi-1D lattice vibrations. Short-range in-plane electronic heterostructures at the vdW interface of Cr 2 Si 2 Te 6 result in a narrowed band gap. The sharp increase in in-plane resistance is found to be linked to the emergence and development of out-of-plane ferromagnetism. The insertion of 2D magnetic layers such as Mn, Fe, and Co into the vdW gap of 2H-TaS 2 induces anisotropic magnetism and associated transport responses to magnetic transitions. Overall, 2D vdW interface modification offers control over collective electronic behavior, transport properties, and their interplays, advancing fundamental science and nanoelectronic devices.

2D van der Waals interfaces↗
DOE OSTI2025

Defects vibrations engineering for enhancing interfacial thermal transport in polymer composites

To push upper boundaries of thermal conductivity in polymer composites, understanding of thermal transport mechanisms is crucial. Despite extensive simulations, systematic experimental investigation on thermal transport in polymer composites is limited. To better understand thermal transport processes, we design polymer composites with perfect fillers (graphite) and defective fillers (graphite oxide), using polyvinyl alcohol (PVA) as a matrix model. Measured thermal conductivities of ~1.38 ± 0.22 W m -1 K -1 in PVA/defective filler composites is higher than those of ~0.86 ± 0.21 W m -1 K -1 in PVA/perfect filler composites, while measured thermal conductivities in defective fillers are lower than those of perfect fillers. We identify how thermal transport occurs across heterogeneous interfaces. Thermal transport measurements, neutron scattering, quantum mechanical modeling, and molecular dynamics simulations reveal that vibrational coupling between PVA and defective fillers at PVA/filler interfaces enhances thermal conductivity, suggesting that defects in polymer composites improve thermal transport by promoting this vibrational coupling.

42 ENGINEERING↗
DOE OSTI2025

Vibration Fixture Design and Testing for Rigid - Y Cable Mount on MMRTG F4

INL is responsible for the fueling and testing of Radioisotope Thermoelectric Generators for NASA space missions. For the upcoming NASA mission "DRAGONFLY," INL is tasked with fueling and testing the Multi-Mission Radioisotope Thermoelectric Generator F4 (MMRTG F4). This involves conducting various tests, such as vibration testing and mass properties testing. For these tests, an interface is required between the MMRTG and the testing equipment, provided by cables mounted on a legacy bracket. Due to design changes in the cooling lines, a new cable – the Rigid Y cable – is to be used. The test described in this poster was to verify if the Rigid Y cable would survive the vibration tests. The results will determine the procedure for conducting the vibration tests on the MMRTG F4.

42 - ENGINEERING↗