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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 OSTI2021

Mapping Molecular Adsorption Configurations with < 5 nm Spatial Resolution through Ambient Tip-Enhanced Raman Imaging

We interrogate para-mercaptobenzoic acid (MBA) molecules chemisorbed onto plasmonic silver nanocubes through tip-enhanced Raman (TER) spectral nano-imaging. Through a detailed examination of the spectra, aided by correlation analysis and density functional theory calculations, we find that MBA chemisorbs onto the plasmonic particles with at least two distinct configurations: S- and CO2-bound. High spatial resolution TER mapping allows us to distinguish between the distinct adsorption geometries with a pixel-limited (< 5 nm) spatial resolution under ambient laboratory conditions.

Gabel, Matthew L.↗
DOE OSTI2022

A Closer Look at Tip-Enhanced Raman Chemical Reaction Nanoimages

Tip-enhanced Raman spectroscopy (TERS) is a powerful technique that enables ultrahigh spatial resolution and ultrasensitive chemical imaging. This technique’s ability to track plasmon-induced/enhanced chemical reactions in real space has gained increasing popularity in recent years. Here, in this study, we expose inherent difficulties associated with assigning TERS signatures that accompany chemical transformations. Namely, distinct selection rules as well as the possibility of multiple physical processes/chemical reaction pathways complicate spectral assignments and necessitate caution in assigning the experimental observables. We illustrate the latter using 4,4'-dimercaptostilbene-functionalized plasmonic silver nanocubes, wherein we identify the TERS signatures of product formation, molecular charging, multipolar Raman scattering, and preferred molecular orientations that all lead to distinct and assignable spectral patterns.

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

Imaging Domain Walls in van der Waals Ferroelectrics Using Tip-Enhanced Second Harmonic Generation

van der Waals ferroelectrics have captured significant interest for applications in novel memory and neuromorphic computing devices. Within these materials, interfaces between regions of different ferroelectric polarizations (i.e., domain walls) exhibit distinctive behaviors. Characterization of these behaviors remains a challenge, as domain wall thickness resides at the nanoscale. Using tip-enhanced second harmonic generation (TESHG), we demonstrate nanoscale imaging of domain walls in 2D ferroelectric α-In 2 Se 3 . With a narrow-band near-IR laser, we take advantage of high-wavelength, off-resonant signal enhancement to generate robust and reproducible TESHG. In conclusion, a 16 nm spatial resolution is achieved, and we identify spectral features suggesting that nonlocal effects from domain walls persist nanometers into adjacent domains.

Mantilla, Alexander B. C. [Washington State Univ.,↗
DOE OSTI2020

Creation of Single-Photon Emitters in WSe 2 Monolayers Using Nanometer-Sized Gold Tips

Due to their tunable bandgaps and strong spin-valley locking, transition metal dichalcogenides constitute a unique platform for hosting single-photon emitters. Here, we present a versatile approach for creating bright single-photon emitters in WSe 2 monolayers by the deposition of gold nanostars. Our molecular dynamics simulations reveal that the formation of the quantum emitters is likely caused by the highly localized strain fields created by the sharp tips of the gold nanostars. The surface plasmon modes supported by the gold nanostars can change the local electromagnetic fields in the vicinity of the quantum emitters, leading to their enhanced emission intensities. Moreover, by correlating the emission energies and intensities of the quantum emitters, we are able to associate them with two types of strain fields and derive the existence of a low-lying dark state in their electronic structures. The findings here are highly relevant for the development and understanding of single-photon emitters in transition metal dichalcogenide materials.

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

Subnanometer Visualization of Spatially Varying Local Field Resonances that Drive Tip-Enhanced Optical Spectroscopy

Our knowledge of the electromagnetic fields that power modern nanoscale optical measurements, including (non)linear tip-enhanced Raman and photoluminescence, chiefly stems from numerical simulations. Aside from idealized in silico vs heterogeneous (nano)structures in the laboratory, challenges in quantitative descriptions of nanoscale light–matter interactions more generally stem from the very nature of the problem, which lies at the interface of classical and quantum theories. This is particularly the case in ultrahigh spatial resolution measurements that are sensitive to local optical field variations that take place on subnanometer length scales. Here this work approaches this challenge through extinction-based spectral nanoimaging experiments. We demonstrate <1 nm spatial resolution in hyperspectral extinction measurements that track spatially varying plasmon resonances. We describe the principles behind our experiments and highlight more general implications of our observations.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2020

Nanoscale Mass Spectrometry Multimodal Imaging via Tip-Enhanced Photothermal Desorption

Materials ranging from adhesives, pharmaceuticals, lubricants, and personal care products are traditionally studied using macroscopic characterization techniques. However, their functionality is in reality defined by details of chemical organization on often noncrystalline matter with characteristic length scales on the order of microns to nanometers. Additionally, these materials are traditionally difficult to analyze using standard vacuum-based approaches that provide nanoscale chemical characterization due to their volatile and beam-sensitive nature. Therefore, approaches that operate under ambient conditions need to be developed that allow probing of nanoscale chemical phenomena and correlated functionality. Here, we demonstrate a tool for probing and visualizing local chemical environments and correlating them to material structure and functionality using advanced multimodal chemical imaging on a combined atomic force microscopy (AFM) and mass spectrometry (MS) system using tip-enhanced photothermal desorption with atmospheric pressure chemical ionization (APCI). We demonstrate enhanced performance metrics of the technique for correlated imaging and point sampling and illustrate the applicability for the analysis of trace chemicals on a human hair, additives in adhesives on paper, and pharmaceuticals samples notoriously difficult to analyze in a vacuum environment. Overall, this approach of correlating local chemical environments to structure and functionality is key to advancing research in many fields ranging from biology, to medicine, to material science.

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

Tip-Enhanced Raman Chemical and Chemical Reaction Imaging in H 2 O with Sub-3-nm Spatial Resolution

Reproducible chemical and chemical reaction nano-imaging at solid-liquid interfaces remains challenging, particularly when resolutions on the order of a few nm are sought after. In this work, we demonstrate the latter through liquid tip-enhanced Raman (TER) measurements that target gold nanoplates functionalized with 4-mercaptobenzonitrile (MBN). In addition to chemical imaging and local optical field nano-visualization with high spatial resolution, we observe the signatures of 4-mercaptobenzoic acid, which forms as a result of plasmon-induced hydrolysis of MBN. Evidently, the solvent leads to distinct plasmon-induced/enhanced chemical reaction pathways that have not been documented. Here this work shows that such reactions that take place at solid-liquid interfaces can be tracked with a record sub-3 nm spatial resolution via TER spectral nano-imaging in liquids.

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

Distilling nanoscale heterogeneity of amorphous silicon using tip-enhanced Raman spectroscopy (TERS) via multiresolution manifold learning

Abstract Accurately identifying the local structural heterogeneity of complex, disordered amorphous materials such as amorphous silicon is crucial for accelerating technology development. However, short-range atomic ordering quantification and nanoscale spatial resolution over a large area on a-Si have remained major challenges and practically unexplored. We resolve phonon vibrational modes of a-Si at a lateral resolution of <60 nm by tip-enhanced Raman spectroscopy. To project the high dimensional TERS imaging to a two-dimensional manifold space and categorize amorphous silicon structure, we developed a multiresolution manifold learning algorithm. It allows for quantifying average Si-Si distortion angle and the strain free energy at nanoscale without a human-specified physical threshold. The multiresolution feature of the multiresolution manifold learning allows for distilling local defects of ultra-low abundance (< 0.3%), presenting a new Raman mode at finer resolution grids. This work promises a general paradigm of resolving nanoscale structural heterogeneity and updating domain knowledge for highly disordered materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Manipulating the insulator–metal transition through tip-induced hydrogenation

Manipulating the insulator–metal transition in strongly correlated materials has attracted a broad range of research activity due to its promising applications in, for example, memories, electrochromic windows and optical modulators. Electric-field-controlled hydrogenation using ionic liquids and solid electrolytes is a useful strategy to obtain the insulator–metal transition with corresponding electron filling, but faces technical challenges for miniaturization due to the complicated device architecture. Here, in this work, we demonstrate reversible electric-field control of nanoscale hydrogenation into VO 2 with a tunable insulator–metal transition using a scanning probe. The Pt-coated probe serves as an efficient catalyst to split hydrogen molecules, while the positive-biased voltage accelerates hydrogen ions between the tip and sample surface to facilitate their incorporation, leading to non-volatile transformation from insulating VO 2 into conducting H x VO 2 . Remarkably, a negative-biased voltage triggers dehydrogenation to restore the insulating VO 2 . This work demonstrates a local and reversible electric-field-controlled insulator–metal transition through hydrogen evolution and presents a versatile pathway to exploit multiple functional devices at the nanoscale.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Particle-number distribution in large fluctuations at the tip of branching random walks

Here, we investigate properties of the particle distribution near the tip of one-dimensional branching random walks at large times t , focusing on unusual realizations in which the rightmost lead particle is very far ahead of its expected position, but still within a distance smaller than the diffusion radius ~$\sqrt{t}$. Our approach consists in a study of the generating function $G_{Δx}(λ) = Σ_n$ ${λ^n}p_n(Δx)$ for the probabilities $p_n(Δx)$ of observing $\textit{n}$ particles in an interval of given size $Δ\textit{x}$ from the lead particle to its left, fixing the position of the latter. This generating function can be expressed with the help of functions solving the Fisher-Kolmogorov-Petrovsky-Piscounov (FKPP) equation with suitable initial conditions. In the infinite-time and large-$Δ\textit{x}$ limits, we find that the mean number of particles in the interval grows exponentially with $Δ\textit{x}$, and that the generating function obeys a nontrivial scaling law, depending on $Δ\textit{x}$ and λ through the combined variable $[Δx — f(λ)]^3 / Δx^2$, where $\textit{f}$(λ) ≡ – ln(1 – λ) – ln [– ln(1 – λ)]. From this property, one may conjecture that the growth of the typical particle number with the size of the interval is slower than exponential, but, surprisingly enough, only by a subleading factor at large Δ$\textit{x}$. The scaling we argue is consistent with results from a numerical integration of the FKPP equation.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Large-eddy simulations of turbulent wake flows behind helical- and straight-bladed vertical axis wind turbines rotating at low tip speed ratios

Turbulent wake flows behind helical- and straight-bladed vertical axis wind turbines (VAWTs) rotating at low tip speed ratios (TSRs) are studied numerically. The turbulent flows are simulated using the large-eddy simulation (LES) model, and the rotating turbine blades are modeled using the actuator line method. The helical VAWT has identical key parameters as the straight VAWT except for the 135° helical twist of the blades over the 0.3m vertical span. A set of LES runs are performed for two TSRs, 0.6 and 0.4, and the results are reported and analyzed. At these low TSRs, the wake behind the straight-bladed VAWT exhibits two-dimensional dominant flow motions (in the horizontal plane perpendicular to the straight blades) in the near-wake region that cause considerable spanwise expansion of the wake as it extends downstream. In contrast, the helical-bladed VAWT generates highly three-dimensional (3D) wake flow structures and upward/downward mean flow motions within the wake that cause the wake to expand mainly in the vertical direction. Turbulence statistical analyses also show that the 3D wake flow features induced by the helical blades accelerate the wake transition to turbulence and enhance the small-scale turbulent dissipation (as shown by the subgrid-scale turbulent dissipation in the LES), which leads to a more rapid decay of the wake turbulence intensity than that in the straight-bladed VAWT case at the same TSR. Finally, compared with the straight-bladed VAWT, the helical-bladed VAWT also exhibits much smaller temporal variations for the torque and power coefficients during the rotation cycle, which can be beneficial for wind power generation.

17 WIND ENERGY↗
DOE OSTI2020

Tipping points of Mississippi Delta marshes due to accelerated sea-level rise

Coastal marshes are threatened by relative sea-level (RSL) rise, yet recent studies predict marsh survival even under the high rates of RSL rise expected later in this century. However, because these studies are mostly based on short-term records, uncertainty persists about the longer-term vulnerability of coastal marshes. We present an 8500-year-long marsh record from the Mississippi Delta, showing that at rates of RSL rise exceeding 6 to 9 mm year –1 , marsh conversion into open water occurs in about 50 years. At rates of RSL rise exceeding ~3 mm year –1 , marsh drowning occurs within a few centuries. Because present-day rates of global sea-level rise already surpass this rate, submergence of the remaining ~15,000 km 2 of marshland in coastal Louisiana is probably inevitable. RSL-driven tipping points for marsh drowning vary geographically, and those for the Mississippi Delta may be lower than elsewhere. Nevertheless, our findings highlight the need for consideration of longer time windows in determining the vulnerability of coastal marshes worldwide.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Fabrication of silicon-tipped fiber-optic temperature sensors using aerogel-assisted glass soldering with precise laser heating

We demonstrate the fabrication of fiber-optic Fabry–Perot interferometer (FPI) temperature sensors by bonding a small silicon diaphragm to the tip of an optical fiber using low melting point glass powders heated by a 980 nm laser on an aerogel substrate. The heating laser is delivered to the silicon FPI using an optical fiber, while the silicon temperature is being monitored using a 1550 nm white-light system, providing localized heating with precise temperature control. The use of an aerogel substrate greatly improves the heating efficiency by reducing the thermal loss of the bonding parts to the ambient environment. A desirable temperature for bonding can be achieved with relatively small heating laser power. The bonding process is carried out in an open space at room temperature for convenient optical alignment. The precise temperature control ensures minimum perturbation to the optical alignment and no induced thermal damage to the optical parts during the bonding process. For demonstration, we fabricated a low-finesse and high-finesse silicon FPI sensor and characterized their measurement resolution and temperature capability. The results show that the fabrication method has a good potential for high-precision fabrication of fiber-optic sensors.

Sheng, Qiwen↗
DOE OSTI2025

Significantly enhanced near-field coupling via tip engineering

The ability to significantly enhance near-field coupling between light and matter at the nanoscale is crucial for advancing the fields of nanophotonics and nanopolariotonics. However, conventional probes face challenges in achieving optimal light–matter interaction. In this study, we propose a novel, to the best of our knowledge, simulation-based strategy that leverages tip engineering to dramatically amplify the scattering field through tailored double-layer geometries. By employing a core-shell structure with a thin shell layer optimized for specific dielectric permittivity and effective polarizability, we demonstrate a near-field enhancement of up to 10 times compared to conventional probes. Our findings highlight exciting new possibilities for optimizing near-field interactions through probe designs with customized resonances, paving the way for substantially improved nano-optical sensing, imaging, and detection.

Shiravi, H.↗
DOE OSTI2020

Chaperone-tip adhesin complex is vital for synergistic activation of CFA/I fimbriae biogenesis

Colonization factor CFA/I defines the major adhesive fimbriae of enterotoxigenic Escherichia coli and mediates bacterial attachment to host intestinal epithelial cells. The CFA/I fimbria consists of a tip-localized minor adhesive subunit, CfaE, and thousands of copies of the major subunit CfaB polymerized into an ordered helical rod. Biosynthesis of CFA/I fimbriae requires the assistance of the periplasmic chaperone CfaA and outer membrane usher CfaC. Although the CfaE subunit is proposed to initiate the assembly of CFA/I fimbriae, how it performs this function remains elusive. Here, we report the establishment of an in vitro assay for CFA/I fimbria assembly and show that stabilized CfaA-CfaB and CfaA-CfaE binary complexes together with CfaC are sufficient to drive fimbria formation. The presence of both CfaA-CfaE and CfaC accelerates fimbria formation, while the absence of either component leads to linearized CfaB polymers in vitro. We further report the crystal structure of the stabilized CfaA-CfaE complex, revealing features unique for biogenesis of Class 5 fimbriae.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2025

CROCUS Tipping Bucket Rain Gauge Data at Argonne National Laboratory Prairie Site

The Tipping Bucket Rain Gauge (TBRG) dataset contains data from both the Nova-Lynx 12 inch TBRG and the Met One 8-inch TBRG. The dataset contains one minute measurements for precipitation accumulation measured in that timeframe from both instruments. Each TBRG was equipped with heaters for all-season measurements. These data are helpful for identifying periods of drought, potential flooding, and general input for water budgets. TBRGs can be used to validate optical rain gauge data and disdrometer data collected during the CROCUS project. Data were collected at the Argonne Testbed for Multiscale Observational Science (ATMOS), a 20-acre prairie site at Argonne National Laboratory in Lemont, Illinois. The data is presented as daily NetCDF (.nc) files, each containing approximately 24 hours of observations. Files follow the naming convention of: the project (CROCUS), location (atmos), instrument name (tbrg), data level (raw, a1), and date (year, month, day). The NetCDF format can be accessed using common scientific software such as Python using xarray, netCDF4 or act-doe.

1-min Precipitation Accumulation↗
DOE OSTI2020

Arctic Tipping Points Triggering Global Change (LDRD Final Report)

The Arctic is warming and feedbacks in the coupled Earth system may be driving the Arctic to tipping events that could have critical downstream impacts for the rest of the globe. In this project we have focused on analyzing sea ice variability and loss in the coupled Earth system Summer sea ice loss is happening rapidly and although the loss may be smooth and reversible, it has significant consequences for other Arctic systems as well as geopolitical and economic implications. Accurate seasonal predictions of sea ice minimum extent and long-term estimates of timing for a seasonally ice-free Arctic depend on a better understanding of the factors influencing sea ice dynamics and variation in this strongly coupled system. Under this project we have investigated the most influential factors in accurate predictions of September Arctic sea ice extent using machine learning models trained separately on observational data and on simulation data from five E3SM historical ensembles. Monthly averaged data from June, July, and August for a selection of ice, ocean, and atmosphere variables were used to train a random forest regression model. Gini importance measures were computed for each input feature with the testing data. We found that sea ice volume is most important earlier in the season (June) and sea ice extent became a more important predictor closer to September. Results from this study provide insight into how feature importance changes with forecast length and illustrates differences between observational data and simulated Earth system data. We have additionally performed a global sensitivity analysis (GSA) using a fully coupled ultra- low resolution configuration E3SM. To our knowledge, this is the first global sensitivity analysis involving the fully-coupled E3SM Earth system model. We have found that parameter variations show significant impact on the Arctic climate state and atmospheric parameters related to cloud parameterizations are the most significant. We also find significant interactions between parameters from different components of E3SM. The results of this study provide invaluable insight into the relative importance of various parameters from the sea ice, atmosphere and ocean components of the E3SM (including cross-component parameter interactions) on various Arctic-focused quantities of interest (QOIs).

54 ENVIRONMENTAL SCIENCES↗