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Results for “Optical Response”

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 OSTI2022

Comparative Analysis of the Near‐ and Far‐Field Optical Response of Thin Plasmonic Nanostructures

Abstract Nanostructures made of metallic materials support collective oscillations of their conduction electrons, commonly known as surface plasmons. These modes, whose characteristics are determined by the material and morphology of the nanostructure, couple strongly to light and confine it into subwavelength volumes. Of particular interest are metallic nanostructures for which the size along one dimension approaches the nanometer or even the subnanometer scale, since such morphologies can lead to stronger light–matter interactions and higher degrees of confinement than regular three‐dimensional nanostructures. Here, the plasmonic response of metallic nanodisks of varying thicknesses and aspect ratios is investigated under far‐ and near‐field excitation conditions. It is found that, for far‐field excitation, the strength of the plasmonic response of the nanodisk increases with its thickness, as expected from the increase in the number of conduction electrons in the system. However, for near‐field excitation, the plasmonic response becomes stronger as the thickness of the nanodisk is reduced. This behavior is attributed to the higher efficiency with which a near‐field source couples to the plasmons supported by thinner nanodisks. The results of this work advance the understanding of the plasmonic response of thin metallic nanostructures, thus increasing their potential for the development of novel applications.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Surface-Induced Deprotonation of Thiol Ligands Impacts the Optical Response of CdS Quantum Dots

Cadmium chalcogenide quantum dots (QDs) passivated by thiol-based ligands exhibit several advantages in their applications in lighting, sensing, and imaging technologies. However, their emission is sensitive to thiol concentrations, pH conditions, and temperatures. Using calculations based on the density functional theory, we identify conditions for thiol/thiolate equilibrium at the CdS QD surface that either eliminate or introduce optically inactive hole trap states favoring or disfavoring the emission. Our calculations indicate much weaker interactions between the QD and protonated species (thiols), compared to their deprotonated counterparts (thiolates). Additionally, the surface of CdS QD facilitates the partial deprotonation of thiols, leading to the formation of an additional stable networking conformation where the proton is shared between the ligand and the QD surface. Thiolates strongly reduce the optical intensity of low-energy transitions in CdS QDs, contributing thiolate-localized hole trap states at the QD band gap. However, networking between the thiols and the surface, as well as the presence of native ligands such as primary amines, stabilize such trap states brightening the lowest optical transitions. This explains the increased emission of thiol-passivated QDs at lower concentrations in neutral or acidic solutions. Surface-mediated bias toward deprotonated species and their contribution to optically inactive states also rationalizes irreversible emission quenching and bleaching in the CdSe/CdS QDs exposed to high temperatures or intensive laser pulse.

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

Flat Bands and Chiral Optical Response of Moiré Insulators

Here, we present a low-energy model describing the reconstruction of the electronic spectrum in twisted bilayers of honeycomb crystals with broken sublattice symmetry. The resulting moiré patterns are classified into two families with different symmetry. In both cases, flat bands appear at relatively large angles without any magic-angle condition. Transitions between them give rise to sharp resonances in the optical absorption spectrum at frequencies well below the gap of the monolayer. Owing to their chiral symmetry, twisted bilayers display circular dichroism, that is, different absorption of left and right circularly polarized light. This optical activity is a nonlocal property determined by the stacking. In hexagonal boron nitride, sensitivity to the stacking leads to strikingly different circular dichroism in the two types of moirés. Our calculations exemplify how subtle properties of the electronic wave functions, encoded in current correlations between the layers, control physical observables of moiré materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

In-plane and out-of-plane optical response of the nodal-line semimetals ZrGeS and ZrGeSe

Polarization-dependent reflectivity measurements were carried out over a broad frequency range on single-crystalline ZrGeSe and ZrGeS compounds, which are closely related to the prototype nodal-line semimetal ZrSiS. These measurements revealed the strongly anisotropic character of both ZrGeSe and ZrGeS, with a reduced plasma frequency for the out-of-plane direction E∥c as compared with the in-plane direction E ∥ ab. For E ∥ ab, the optical conductivity spectrum consists of two Drude terms followed by a shoulder or plateaulike behavior and a distinct U shape at higher energies, while for E ∥ c, one Drude term is followed by a peaklike behavior, and the U shape of the profile is less developed. Under external pressure, two prominent excitations appear in the out-of-plane optical conductivity spectrum of ZrGeSe, whose frequency position and oscillator strength show a weak anomaly at ~3 GPa. Overall, the pressure-induced changes in the profile of the E∥c conductivity spectrum are much enhanced >~3 GPa. We compare our results to those recently reported for ZrSiS in a quantitative manner.

36 MATERIALS SCIENCE↗
DOE OSTI2024

TiN‐Au/HfO 2 ‐Au Multilayer Thin Films with Tunable Hyperbolic Optical Response

Abstract Hyperbolic metamaterials (HMM) possess significant anisotropic physical properties and tunability and thus find many applications in integrated photonic devices. HMMs consisting of metal and dielectric phases in either multilayer or vertically aligned nanocomposites (VAN) form are demonstrated with different hyperbolic properties. Herein, self‐assembled HfO 2 ‐Au/TiN‐Au multilayer thin films, combining both the multilayer and VAN designs, are demonstrated. Specifically, Au nanopillars embedded in HfO 2 and TiN layers forming the alternative layers of HfO 2 ‐Au VAN and TiN‐Au VAN. The HfO 2 and TiN layer thickness is carefully controlled by varying laser pulses during pulsed laser deposition (PLD). Interestingly, tunable anisotropic physical properties can be achieved by adjusting the bi‐layer thickness and the number of the bi‐layers. Type II optical hyperbolic dispersion can be obtained from high layer thickness structure (e.g., 20 nm), while it can be transformed into Type I optical hyperbolic dispersion by reducing the thickness to a proper value (e.g., 4 nm). This new nanoscale hybrid metamaterial structure with the three‐phase VAN design shows great potential for tailorable optical components in future integrated devices.

Chemistry↗
DOE OSTI2022

Optical Response of Periodic Arrays of Graphene Nanodisks

Doped graphene nanostructures are a promising platform for photonics due to their exceptionally strong and tunable plasmonic resonances. When placed in a periodic array configuration, the plasmons supported by the individual nanostructures interact with each other and, under the appropriate conditions, can give rise to a collective mode known as a lattice resonance. Here, for this study, we perform a comprehensive analysis of the response of periodic arrays of graphene nanodisks and identify the conditions under which the system is able to support lattice resonances. We find that the ratio between the period of the array and the wavelength of the plasmon completely determines the behavior of the system. As a consequence, strong lattice resonances are achieved for micron-size nanodisks in the terahertz regime. We develop a theoretical model valid beyond the electrostatic approximation and use it to derive closed analytical expressions for the strength, the wavelength, and the width of the optical resonance of the arrays. The theoretical framework developed in this work paves the way for facile design and discovery of emerging properties of periodic arrays of graphene nanostructures that could enable applications in photonics and plasmonics.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Direct Observation of the Pressure-Induced Structural Variation in Gold Nanoclusters and the Correlated Optical Response

The ability to gradually modify the atomic structures of nanomaterials and directly identify such structural variation is important in nanoscience research. Here, we present the first example of a high-pressure single-crystal X-ray diffraction analysis of atomically precise metal nanoclusters. The pressure-dependent, subangstrom structural evolution of an ultrasmall gold nanoparticle, Au 25 S 18 , has been directly identified. We found that a 0.1 Å decrease of the Au–Au bond length could induce a blue-shift of 30 nm in the photoluminescence spectra of gold nanoclusters. From theoretical calculations, the origins of the blue-shift and enhanced photoluminescence under pressure are investigated, which are ascribed to molecular orbital symmetry and conformational locking, respectively. Here, the combination of the high-pressure in situ X-ray results with both theoretical and experimental optical spectra provides a direct and generalizable avenue to unveil the underlying structure–property relations for nanoclusters and nanoparticles which cannot be obtained through traditional physical chemistry measurements.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2020

Collective modes in excitonic insulators: Effects of electron-phonon coupling and signatures in the optical response

Here, we consider a two-band spinless model describing an excitonic insulator (EI) on the two-dimensional square lattice with anisotropic hopping parameters and electron-phonon (el-ph) coupling, inspired by the EI candidate Ta 2 NiSe 5 . We systematically study the nature of the collective excitations in the ordered phase which originates from the interband Coulomb interaction and the el-ph coupling. When the ordered phase is stabilized only by the Coulomb interaction (pure EI phase), its collective response exhibits a massless phase mode in addition to the amplitude mode. We show that in the BEC regime, the signal of the amplitude mode becomes less prominent and that the anisotropy in the phase-mode velocities is reduced. Through coupling to the lattice, the phase mode acquires a mass and the signal of the amplitude mode becomes less prominent. Importantly, the character of the softening mode at the boundary between the normal semiconductor phase and the ordered phase depends on the parameters. In particular, we point out that even for el-ph coupling smaller than the Coulomb interaction, the mode that softens to zero at the boundary can have a phonon character. We also discuss how the collective modes can be observed in the optical conductivity. Furthermore, we study the effects of nonlocal interactions on the collective modes and show the possibility of realizing a coexistence of an in-gap mode and an above-gap mode split off from the single-amplitude mode in the system with local interactions only.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Controlling the Magneto-Optical Response in Ultrathin Films of EuO 1– x via Interface Engineering with Ferroelectric BaTi 2 O 5

Utilizing pulsed laser deposition, a film of EuO 1–x was deposited onto a Si(001) substrate with MgO buffer and compared to the same heterostructure with an additional BaTi 2 O 5 thin film on top of the EuO 1–x surface. X-ray diffraction (XRD) indicates the films crystallize into a preferred EuO(111) orientation; it also reveals the clear presence of EuSi 2 , which suggests Si or Eu diffuses across the MgO buffer layer. EuO 1–x films exhibit a ferromagnetic (FM) signature and temperature-dependent exchange bias, indicated by MOKE measurements, suggesting the presence of a magnetic order well above the EuO Curie temperature with possible origins in charge carrier density near the interface. In comparison, an antiferromagnetic character persists well above the EuO Curie temperature of 69 K and the enhanced Curie temperature of 150 K for BaTi 2 O 5 films grown on the EuO 1–x films. Furthermore, the antiferromagnetic behavior is not seen in thicker EuO 1–x thin films when integrated with other ferroelectric (FE) phases of the BaO–TiO 2 system, suggesting an origin in the perturbed charge population at the BaTi 2 O 5 /EuO 1–x interface.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Correlating structural changes in thermoresponsive hydrogels to the optical response of embedded plasmonic nanoparticles

Stimuli-responsive microgels, composed of small beads with soft, deformable polymer networks swollen through a combination of synthetic control over the polymer and its interaction with water, form a versatile platform for development of multifunctional and biocompatible sensors. The interfacial structural variation of such materials at a nanometer length scale is essential to their function, but not yet fully comprehended. Here, we take advantage of the plasmonic response of a gold nanorod embedded in a thermoresponsive microgel (AuNR@PNIPMAm) to monitor structural changes in the hydrogel directly near the nanorod surface. By direct comparison of the plasmon response against measurements of the hydrogel structure from dynamic light scattering and nuclear magnetic resonance, we find that the microgel shell of batch-polymerized AuNR@PNIPMAm exhibits a heterogeneous volume phase transition reflected by different onset temperatures for changes in the hydrodyanmic radius (R H ) and plasmon resonance, respectively. The new approach of contrasting plasmonic response (a measure of local surface hydrogel structure) with R H and relaxation times paves a new path to gain valuable insight for the design of plasmonic sensors based on stimuli-responsive hydrogels.

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

Hugoniot states and optical response of soda lime glass shock compressed to 120 GPa

In contrast to relatively pure silica glass (fused silica-FS), commercial silica-rich glasses contain significant fractions of additional oxide components. In particular, soda-lime glass (SLG) consists of approximately 71% SiO 2 by weight, which raises the question: what is the effect of additional cations on the shock compression response of silica-rich glasses? To address this concern, plate impact experiments were conducted to determine the high-pressure Hugoniot states for shocked SLG (37 to 120 GPa) and compared with recently reported results on FS. Using laser interferometry, particle velocity profiles were measured at the impact surface and the SLG/LiF window interface. In all experiments, the transmitted profiles show a single shock wave, with no features indicative of a phase transformation. The Hugoniot states determined from the wave profiles are described well using a linear shock velocity–particle velocity relation. Interferometry measurements (using 1550-nm wavelength laser) at the impact surface show that SLG is transparent when shocked to 55 GPa, transparent for tens of nanoseconds after impact between 55 and 81 GPa, and opaque beyond 81 GPa. From impact surface measurements, a linear relationship between the apparent and true particle velocity was observed, resulting in a linear relationship between the refractive index (at 1550 nm) and density. At 120 GPa, the SLG density is nearly twice its ambient value, indicating that SLG can achieve highly dense amorphous states. When compared to FS, shocked SLG is much less compressible and likely does not transform to a crystalline phase. A plausible explanation for this difference is indicated.

58 GEOSCIENCES↗