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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 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Additively manufactured strain sensors for in-pile applications

Accurate, real-time monitoring of strain in fuel, cladding, and structural components of nuclear reactors is critical to better understand radiation induced phenomena during reactor tests and operations. The data provided is crucial to verify physics-based, multiscale modeling and simulation efforts, which aim to shorten the timeline for the development of new nuclear materials. Resistive strain gauges have limited performance during in-pile experiments due to the harsh operating conditions and limited physical space between fuel and cladding components. In this work, aerosol jet printing using silver nanoparticle inks was used to fabricate interdigitated electrode capacitive strain gauges on aluminum alloy 6061 tensile specimens. Here to simulate the temperatures of a traditional light water reactor, the capacitive strain gauges were tested with a mechanical test frame up to 300 °C and compared to commercially available bondable resistive strain gauges. The printed capacitive strain gauges exhibited a gauge factor of 1.0 and showed higher reproducibility and predictability of strain sensing performance than the resistive strain gauge. The results demonstrate the potential of aerosol jet printing to fabricate strain sensors with predictable performance and reduced invasiveness for high-temperature applications with confined spacing.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Multiphysics modeling of printed surface acoustic wave thermometers

Surface acoustic wave (SAW) transducers are a class of sensors and actuators that operate on the fundamental principle of piezoelectricity. Aerosol jet printing and other additive manufacturing techniques have resulted in the low-cost fabrication of low-power and small-footprint SAW devices that are suitable for sensing in high-temperature and radioactive environments. In this work, we developed a series of temperature-dependent finite element models for a SAW transducer consisting of printed silver interdigitated transducers (IDTs) deposited onto piezoelectric lithium niobate. Modeling accuracy was evaluated experimentally from room temperature to 200 °C using an aerosol-jet-printed SAW thermometer. A time-domain study enabled visualization of the wave propagation and successfully guided the denoising of the scattering parameter measurement. Additionally, frequency-domain models using traditional modal analysis or the unique port boundary condition feature in COMSOL Multiphysics accurately predicted the temperature-driven natural frequency drift in the SAW thermometer. The finite element models developed in this study serve to facilitate the computer-aided design of future SAW transducers for applications in harsh environments.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Characterization of front contact degradation in monocrystalline and multicrystalline silicon photovoltaic modules following damp heat exposure

Reliability and durability tests play a key role in the photovoltaic (PV) industry by minimizing potential failure risks for both existing and new cell and module technologies. In this work, a detailed study of contact degradation in monocrystalline and multicrystalline PV modules is performed. The modules are subjected to a sequence of damp heat (DH) exposures followed by electrical characterization after each step. Electroluminescence (EL) imaging shows different darkening patterns for monocrystalline modules compared to multicrystalline modules; the former shows darkening near the busbars and the latter shows it across virtually the entire cell surface. The primary loss mechanism is confirmed to be resistive after comparing the current-voltage (I–V) characteristics at each DH exposure step. Representative samples have been cored out from both the degraded modules and controls for materials characterization to gain further insights into the degradation mechanism. Top-down and cross-sectional scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), and top-down high-resolution X-ray photoelectron spectroscopy (XPS) analysis performed on the cored samples confirm the degradation is due to metallization corrosion. Our study suggests that the difference in the darkening pattern can most likely be attributed to the different silver paste composition used for contacting each cell technology, particularly the composition of the glass frit.

36 MATERIALS SCIENCE↗
DOE OSTI2026

A bioinspired approach for adaptive solid-solid phase change material coatings with optimized surface features for passive thermal regulation

The necessity to reduce global energy consumption calls for innovative strategies in building thermal management. Passive thermal regulation, particularly through bio-inspired designs, offers a promising avenue by mimicking nature's efficient control of optical properties. This research introduces a novel, climate-responsive coating that integrates optimized bio-inspired surface features with a solid-solid phase change material (SS-PCM) to dynamically manage solar absorptivity without adding additional thickness, enabling both heating and cooling as needed. Drawing on the photonic architectures of the Saharan silver ant and Morpho Didius butterfly, we employed a modeling and multi-objective optimization framework to tailor these surface features. Simulations reveal that surface texture, rather than the intrinsic phase transition of the SS PCM, dominates optical control. Relative to a flat SS PCM coating, optimized isotropic random roughness and broader range features yielded the highest passive heating power increase of about 144 % and 319 % respectively suitable for cold climates. Saharan ant-inspired features enhanced passive cooling for hot climates, achieving a 21.8 % improvement. For moderate climates, Butterfly-wing-inspired surface features provided a balanced enhancement of 19 % for heating and 7 % for cooling. Across all cases, the optimized surface features reduced combined heating and cooling energy demand more effectively than the baseline coating, while preserving material thickness. These findings demonstrate that climate-adaptive, optimized bio-inspired surface features can unlock the full potential of SS PCM coatings, providing a versatile pathway to significant energy savings in buildings and other applications. The methodology establishes a framework for designing next-generation adaptive envelopes that leverage natural photonic principles for high-impact, low-cost thermal regulation.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Computational study of the adsorption of bimetallic clusters on alumina substrate

We performed computational investigation of the adsorption of bimetallic Pd 3 M 2 (where M changes from Ag, Au, Co, Cu, Mn, Ni, Pt, and Ru) cluster on the hydroxylated alumina surface. Previously, it was shown that small silver cluster can control the rate of discharge at the cathode of lithium-oxygen battery. The gap near the fermi energy was shown to control the oxygen reduction, an important reaction for LiO 2 formation. Controlling the gap would ultimately control the rate of LiO 2 formation. One can vary the size of the cluster to vary the gap, however, this "knob" provides limited variance in the gap. Alloying, in combination with size variation offer a much wider control of the gap, hence the LiO 2 formation. Using Density Functional Theory (DFT), we determined the most stable geometry of the bimetallic clusters Pd 3 M 2 and calculated the binding energies of these clusters on the alumina substrate which ranges from 0.2 eV to 0.25 eV depending upon the composition of the alloy-cluster, its orientation and the adsorption site. We also find that Pd atoms bind strongly with the substrate oxygen atoms with an average short bond-length of about 2.2 angstrom. We explored how the gap at the Fermi level of the system varies as a function of elemental composition and the calculated gap ranges from 0 meV to 90 meV. Charges distribution using Bader analysis was also performed to probe how charges are transferred between the cluster and the substrate. These preliminary results will open the door for more systematic studies of alloy clusters of different size and stoichiometry for Li-O 2 battery cathode design.

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

N -Arylimide Molecular Balances: A Comprehensive Platform for Studying Aromatic Interactions in Solution

Noncovalent interactions of aromatic surfaces play a key role in many biological processes and in determining the properties and utility of synthetic materials, sensors, and catalysts. However, the study of aromatic interactions has been challenging because these interactions are usually very weak and their trends are modulated by many factors such as structural, electronic, steric, and solvent effects. Recently, N-arylimide molecular balances have emerged as highly versatile and effective platforms for studying aromatic interactions in solution. These molecular balances can accurately measure weak noncovalent interactions in solution via their influence on the folded–unfolded conformational equilibrium. The structure (i.e., size, shape, π-conjugation, and substitution) and nature (i.e., element, charge, and polarity) of the π-surfaces and interacting groups can be readily varied, enabling the study of a wide range of aromatic interactions. These include aromatic stacking, heterocyclic aromatic stacking, and alkyl–π, chalcogen–π, silver–π, halogen–π, substituent–π, and solvent–π interactions. The ability to measure a diverse array of aromatic interactions within a single model system provides a unique perspective and insights as the interaction energies, stability trends, and solvent effects for different types of interactions can be directly compared. Some broad conclusions that have emerged from this comprehensive analysis include: (1) The strongest aromatic interactions involve groups with positive charges such as pyridinium and metal ions which interact with the electrostatically negative π-face of the aromatic surface via cation–π or metal–π interactions. Attractive electrostatic interactions can also form between aromatic surfaces and groups with partial positive charges. (2) Electrostatic interactions involving aromatic surfaces can be switched from repulsive to attractive using electron-withdrawing substituents or heterocycles. These electrostatic trends appear to span many types of aromatic interactions involving a polar group interacting with a π-surface such as halogen–π, chalcogen–π, and carbonyl–π. (3) Nonpolar groups form weak but measurable stabilizing interactions with aromatic surfaces in organic solvents due to favorable dispersion and/or solvophobic effects. Furthermore, a good predictor of the interaction strength is provided by the change in solvent-accessible surface area. (4) Solvent effects modulate the aromatic interactions in the forms of solvophobic effects and competitive solvation, which can be modeled using solvent cohesion density and specific solvent–solute interactions.

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

The Influence of Nonlocal Metal–Dielectric Environments on Physical and Chemical Processes

Plasmonic nanolayers and laminar metallic/dielectric multilayers were originally developed for optical cloaking applications and lensing applications that could potentially image objects whose size was below the diffraction limit. These assemblies were initially formed from gold or silver nanorods grown within an alumina mesh. However, more recently, assemblies with similar properties have also been prepared by sequential thin-layer deposition of alternating layers of gold and magnesium fluoride (MgF 2 ). These metal/dielectric composite materials enable control of the dielectric constant in the directions perpendicular to the layers and balance the real and imaginary dielectric constants of the assembly such that the speed and the amplitude of the waves traveling through the assembly are not attenuated. In this Account, we will also focus on a few of the applications ranging from surface wetting to fluorescence quenching to enhancement of photochemical reactions. First, we will share an introduction to processes used to create these materials, which are combinations of low refractive index metals and transparent higher index materials arranged in a scalable repeating fashion. Two fabrication methods were employed: an electrochemical deposition of Ag nanorods into an anodized alumina matrix which produced materials with an anisotropic negative refractive index material within the plane of the film and lamellar metal/dielectric layers in which the negative index perpendicular to the growth direction. These alternating layers of plasmonic metals and dielectric materials were ultimately chosen to prepare films for further testing, because of their relative ease of fabrication. We will continue with a discussion of a few of the applications of both of these nonlocal dielectric composite materials including more specialized plasmonic, composite, and hyperbolic metamaterials including fluorescence quenching, photochemical reactions, and surface wetting. In each of these applications, the unique response caused by the enhancement of the electric field and the interface between hyperbolic materials and plasmonic materials as they interact photophysically with their near neighbors is presented. In each of the applications, the enhanced electric field extends from the composite substrate layer to interact with its near neighbors and beyond. Furthermore, the presence of this extended interaction can be observed in the form of decreased emission lifetime, enhancement of photochemical reaction rates, and changes in the surface energies measured by contact angle goniometry. In this Account, all of these situations will be addressed. Finally, we will conclude with a summary and vision for the future as well as a discussion of the unique challenges and opportunities available as research active faculty at an HBCU.

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

Real-Time Detection of Hydrogen and Ammonia Isotopologues for Impurity Removal and Recovery of Tritium

To accommodate gas measurements for impurity removal and recovery of tritium, a silver-coated optical or waveguide is employed for collecting Raman scattered signals to determine relative hydrogen and ammonia isotopologue populations in real time. The data and results presented here demonstrate an analytical methodology for the analysis of four ammonia and three hydrogen isotopologues in a hydrogen–deuterium exchange reaction by gas phase Raman spectroscopy. Standard chemometric modeling techniques effectively unravel the signatures of the isotopologues involved observed here; however, a sophisticated quantum chemical approach supports the spectral assignments. An interpretation of the data presented here can emphasize the practicality and reliability of the gaseous monitoring system in complex chemical environments for the hydrogen fuel economy as well as the more distant energy source from a facility that handles tritium. There are still considerable concerns about the measurement of tritium in isotope separation and radiological impurities from gas processing. A common impurity in gas processing is ammonia, which can form readily in the presence of nitrogen and tritium. Substituted ammonia (NQ 3 ), where Q = H, D, or T, is traditionally removed through getters or diffusers along with other non-hydrogen contaminants. A preferable analytical approach is noninvasive and can be deployed for real-time process evaluation in radiological environments.

Ammonia↗
DOE OSTI2021

Iodine Vapor Reactions with Pure Metal Wires at Temperatures of 100–139 °C in Air

In this work, I 2(g) reactions with 11 metal wires (i.e., Al, Ag, Cu, In, Mo, Nb, Ni, Pd, Pt, Sn, Ta) were evaluated at three temperatures (i.e., 100 ± 3°C, 123 ± 4°C, 139 ± 5°C) with exposure times of 24 hours at each temperature. Over these temperatures, some of the metals showed increased mass gain with higher temperatures (i.e., In, Ag, Cu), Sn showed decreased iodine capture at increased temperatures, and most metals (i.e., Mo, Nb, Ni, Pd, Pt, and Ta) showed little to no mass gain at all temperatures. Silver mordenite (AgZ) was used as a standard during these studies and showed a consistent mass gain (m% I ) of 10.6 → 12.8% over this temperature range. The values of mass of iodine captured per mass of starting metal (g g -1 ) ranged widely across the study with the highest values achieved for (in descending order) Sn-T 100°C (4.37), In-T 139°C (3.34), Sn-T 123°C (1.98), In-T 123°C (1.57), Ag-T 139°C (1.19), In-T 100°C (0.97), and Cu-T 139°C (0.71). In some cases, the metal-iodide complex was not stable at the experimental temperature and it was clear some volatility had occurred during the experiment based on discoloration in the vials. These results show that some metals can have extensive reactions with I 2(g) without showing metal-iodide preferences over metal-oxide formation based on thermodynamic predictions. It is possible that materials such as these could be implemented near nuclear facilities to getter I 2(g) in the event of a nuclear accident.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Electrochemically Assisted Single Crystal Growth of Reduced Preyssler Polyoxometalates Decorated with M 2+ ( M = Co, Ni) and Cubane–Like Ni 4 O 4 Units

Polyoxometalates (POMs) are of great interest to the scientific community, and their reduction and nucleation have been well–established by multi–step techniques. The present study develops an electrochemical approach for simultaneous reduction and nucleation of polyoxometalate–containing solids. Herein we report crystal growth of reduced Preyssler polyoxotungstate–based (anionic formula [NaP 5 W 30 O 110 ] 14– ) new crystalline solids made of Preyssler anions interlinked by Co 2+ and Ni 2+ ions. Crystal nucleation and in situ reduction were achieved at room temperature using a two silver wire electrode setup in various aqueous solutions under constant applied potentials. The POM material was deposited on the cathode, and its structure was characterized by X–ray diffraction techniques. The primary structure type observed involves POMs decorated by disordered Co 2+ /Ni 2+ octahedra and fused into 1–D pillars by additional Co 2+ /Ni 2+ octahedra. Additionally, a secondary phase was observed in the Ni–based reactions, where reduced Preyssler anions are decorated by Ni 4 O 4 cubane–like units. To understand the electrochemical process, polarization curves of the electrolyte solutions are presented, suggesting an applied potential best suited for crystal growth. The work highlights the effectiveness of an electrochemical pathway where nucleation and simultaneous reduction of POMs can make novel reduced POM solids.

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

Methods to Calculate Electronic Excited-State Dynamics for Molecules on Large Metal Clusters with Many States: Ensuring Fast Overlap Calculations and a Robust Choice of Phase

Here, we present an efficient set of methods for propagating excited-state dynamics involving a large number of configuration interaction singles (CIS) or Tamm-Dancoff approximation (TDA) single-reference excited states. Specifically, (i) following Head-Gordon et al., we implement an exact evaluation of the overlap of singly-excited CIS/TDA electronic states at different nuclear geometries using a biorthogonal basis and (ii) we employ a unified protocol for choosing the correct phase for each adiabat at each geometry. For many-electron systems, the combination of these techniques significantly reduces the computational cost of integrating the electronic Schrodinger equation and imposes minimal overhead on top of the underlying electronic structure calculation. As a demonstration, we calculate the electronic excited-state dynamics for a hydrogen molecule scattering off a silver metal cluster, focusing on high-lying excited states, where many electrons can be excited collectively and crossings are plentiful. Interestingly, we find that the high-lying, plasmon-like collective excitation spectrum changes with nuclear dynamics, highlighting the need to simulate non-adiabatic nuclear dynamics and plasmonic excitations simultaneously. In the future, the combination of methods presented here should help theorists build a mechanistic understanding of plasmon-assisted charge transfer and excitation energy relaxation processes near a nanoparticle or metal surface.

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

Electron Paramagnetic Resonance Characteristics and Crystal Structure of a Tutton Salt Analogue: Copper-Doped Cadmium Creatininium Sulfate

Electron paramagnetic resonance and crystallographic studies on copper-doped cadmium creatininium sulfate (CdCrnS) were undertaken to study the characteristics of a copper-hexahydrate complex in an organic analogue of Tutton's salt. X-ray diffraction experiments determined the crystal structure of CdCrnS at both 100 and 298 K. CdCrnS, like Tutton salt, crystallizes in the monoclinic space group P2 1 /n. The unit cell contains two cadmium hexahydrate complexes, four creatininium ions, four sulfates, and four additional solvation waters. Both crystallography and EPR find that the doped copper replaces the cadmium in the structure. Single-crystal EPR measurements at room temperature determined the g and copper hyperfine (A Cu ) tensors (principal values: g = 2.437, 2.134, and 2.080 and A Cu = -327, -84.8, and 7.33 MHz). EPR spectra of the powder at room temperature gave g = 2.448, 2.125, and 2.085 and A Cu = -315, -75.0, and 35.0 MHz and at 110 K gave g = 2.462, 2.116, and 2.077 and A Cu = -340, -30.0, and 35.0 MHz. The room-temperature tensors are close to the "rigid lattice limit" values found in copper-doped Tutton salts but with a higher gmin and weaker A Cu x coupling than average. A small but measurable temperature dependency of the tensors indicated the presence of a dynamic Jahn-Teller (JT) effect. In addition, the EPR line width changed dramatically with temperature, which is like that found in all copper-doped Tutton crystals. Utilizing the model of Silver-Getz for the g-value variation gave an estimate for the energy difference (δ 12 = 640 cm -1 ) between the ground and next highest JT configurations. An empirical correlation appears to exist between δ 12 and g min and A Cu x for the copper hexahydrates studied in similar crystals. Finally, this suggests a relationship between the amount of unpaired spins in the copper d-orbital x lobe and the gap between wells of the adiabatic potential surface.

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

Spatially Resolved Mapping of Three-Dimensional Molecular Orientations with ~2 nm Spatial Resolution through Tip-Enhanced Raman Scattering

We record local optical field images of silver nanocubes (75 nm) using tip-enhanced Raman (TER) spectral imaging. The images that we observe are consistent with several recent reports from our group, but here, we demonstrate sub-2 nm spatial resolution in local optical field nanoimaging under ambient laboratory conditions. This is achieved by scanning the substrate (nanocube on Si) relative to a 4-thiobenzonitrile (TBN)-functionalized Ag-coated TER probe. The spatial resolution that we obtain necessitates that only a few molecules govern the recorded optical response; molecular orientation becomes an important consideration in such measurements. We model the orientation through geometry optimization of a TBN molecule chemisorbed onto an Ag79 cluster (sphere with a ~1 nm diameter). Using the computed orientation of the cluster-bound molecule, we then model the optical response using formalism that accounts for the orientation of the molecule relative to vector components of the local optical fields. We find optimal agreement between experiment and theory. In effect, this work reveals the parallels between single-molecule Raman scattering and high-spatial-resolution TER spectroscopy, even when the images themselves cannot be used to visualize a single molecule in real space.

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

Underlying Mechanisms of Hot Carrier-Driven Reactivity on Bimetallic Nanostructures

Bimetallic nanostructures exhibit unique catalytic activity and selectivity that is not evident for their monometallic analogs. Such nanostructures contain plasmonic metals, such as gold or silver, that afford highly efficient harvesting of electromagnetic radiation and its conversion into hot carriers. These highly energetic species are transferred to the catalytic metal sub-component of the bimetallic nanostructure, where a large spectrum of chemical reactions may be catalyzed. The strength of the electric field and the interplay between catalytic and plasmonic metals at the nanoscale are thus critically important for the catalytic activity of bimetallic nanostructures. In this study, we investigate the relationship between the catalytic activity and local electric fields sustained on the surface of gold-palladium (Au@PdNPs) and gold-platinum (Au@PtNPs) nanoplates using tip-enhanced Raman spectroscopy (TERS). We image the spatially varying magnitudes of rectified (DC) local electric fields on the surface of these nanostructures and compare them to fields sustained on the surface of monometallic nanoplates. We find substantially larger electric field magnitudes on Au@PdNPs and Au@PtNPs as compared to their monometallic analogs. These findings suggest that catalytic efficiency of bimetallic nanostructures may be mediated and potentially tuned through precise control of electric fields sustained on their surfaces.

Li, Zhandong↗
DOE OSTI2026

Low Temperature Oxygen Activation on the NiAg(100) Single-Atom Alloy Surface

Silver-catalyzed ethylene epoxidation remains the only industrially viable route for ethylene oxide (EO) production. However, this process requires chlorine and other promoters to achieve a high EO selectivity while still generating substantial CO 2 emissions. A recent theory-guided approach identified Ni, in single-atom alloy (SAA) form, as a new promoter of this reaction. Specifically, the addition of Ni to Ag nanoparticles supported on α-Al 2 O 3 at a highly diluted ratio (1 Ni per 200 Ag atoms) increased catalyst selectivity to EO by ∼25%, the same increase afforded by the ubiquitous industrial promoter chlorine. To better understand the effect of Ni, we investigated the interaction of O 2 with NiAg(100) SAA surfaces by using scanning tunneling microscopy (STM) and density functional theory (DFT). While only molecular O 2 was present when pure Ag(100) was exposed to O 2 at 78 K, a distinct NiO 2 species, indicative of O 2 dissociation at Ni atom sites, was identified on the NiAg(100) SAA under the same conditions. High-resolution STM imaging backed by DFT simulations elucidated the formation of an O−Ni−O species with the oxygen atoms in 4-fold hollow sites. These findings provide direct experimental evidence that Ni atoms are very effective at O 2 activation, even at cryogenic temperatures. This suggests that, in addition to the known role of Ni in stabilizing the unselective nucleophilic oxygen on Ag, it could also accelerate O 2 dissociation, which can be rate limiting.

Catalysts↗
DOE OSTI2020

The Prevalence of Anions at Plasmonic Nanojunctions: A Closer Look at P-Nitrothiophenol

We revisit the reductive coupling of p-nitrothiophenol (NTP) to form dimercaptoazobenzene (DMAB), herein monitored through gap-mode tip-enhanced Raman spectroscopy (TERS) and nano-imaging. We employ a plasmonic Au probe (100 nm diameter at its apex) illuminated with a 633 nm laser source (50 ?W/?m2 at the sample position) to image a NTP-coated faceted silver nanoparticle (~70 nm diameter). A detailed analysis of the recorded spectra reveals that anionic NTP species contribute to the recorded spectral images, in addition to the more thoroughly described DMAB product. Notably, the signatures of the anions are more pronounced than those of the DMAB product under our present experimental conditions. Our results thus demonstrate that anions and their spectral signatures must be considered in the analysis of plasmon-enhanced spectra and images.

Wang, Chih-Feng↗
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 OSTI2021

Imaging Plasmons with Sub-2 nm Spatial Resolution via Tip-Enhanced Four-Wave Mixing

Four-wave mixing at plasmonic tip-sample nanojunctions may be used to visualize plasmonic fields with sub-2nm spatial resolution under ambient laboratory conditions. We illustrate the latter using a gold-coated atomic force microscopy probe irradiated with a pair of near-IR femtosecond laser pulses and used to interrogate plasmonic gold nanoplates and silver nanocubes. Through diagnostic polarization-dependent tip-only measurements, we illustrate that the 4-wave mixing signal is localized to the tip apex. The apex-bound signal is further enhanced when the tip is located near plasmonic nanoparticles. Overall, this work paves the way for visualizing coherent electronic and vibrational dynamics with joint femtosecond temporal and few-nanometer spatial resolution under ambient conditions.

Wang, Chih-Feng↗