Search NASA⌕ Search

SEARCH · Search NASA

Results for “DIELECTRIC POLARIZATION”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 217 records · Page 12
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Solvent effects on triplet yields in BODIPY-based photosensitizers

Here, we employ molecular dynamics simulations and quantum rate theories to elucidate the complex condensed-phase dynamics underpinning triplet-state formation in organic photosensitizers. Using models informed by first-principles calculations complete with a molecular representation of solvents of different polarities, we elucidate the interplay of the internal and environmental interactions underlying triplet yield. We find that triplet yields depend sensitively on the dielectric stabilization of the charge transfer intermediate that facilitates a transition into the triplet manifold. Our results illustrate the importance of molecularly detailed models in understanding the excited-state internal charge-transfer dynamics of photochemically relevant organic molecules.

Coello Escalante, Leonardo [University of Californ↗
DOE OSTI2020

Extraordinarily large permittivity modulation in zinc oxide for dynamic nanophotonics

The dielectric permittivity of a material encapsulates the essential physics of light-matter interaction into the material's local response to optical excitation. Photo-induced modulation of the permittivity can enable an unprecedented level of control over the phase, amplitude, and polarization of light. Therefore, the detailed dynamic characterization of technology-relevant materials with substantially tunable optical properties and fast response times is a crucial step to realize tunable optical devices. This work reports on the extraordinarily large permittivity changes in zinc oxide thin films (up to similar to 3.6 relative change in the real part of the dielectric permittivity at 1600 nm wavelength) induced by optically generated free carriers. We demonstrate broadband reflectance modulation up to 70% in metal-backed oxide mirrors at the telecommunication wavelengths, with picosecond-scale relaxation times. The epsilon near zero points of the films can be dynamically shifted from 8.5 mm to 1.6 mm by controlling the pump fluence. Additionally, the modulation can be selectively enhanced at specific wavelengths employing metal-backed zinc oxide disks while maintaining picosecond-scale switching times. This work provides insights into the free-carrier assisted permittivity modulation in zinc oxide and could enable the realization of novel dynamic devices for beam-steering, polarizers, and spatial light modulators.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Carrier-Envelope Phase Control in Terahertz Pulse Generation Using InAs Ribbon Metasurfaces

Generation of broadband terahertz (THz) pulses with variable polarization and carrier-envelope phase can enable the tailoring of THz beam wavefronts for advanced applications in THz imaging and spectroscopy and for strong THz field optics. While metasurfaces composed of deeply subwavelength THz emitters have recently been demonstrated to define the polarization and spatial profile of the generated THz fields, precise phase control or synthesis of THz pulse waveforms remains a challenging problem. Here, we propose and demonstrate metasurfaces composed of indium arsenide (InAs) nanoscale ribbon arrays capable of generating THz pulses with variable carrier-envelope phase. We show that different THz generation mechanisms, each contributing distinct phases, can be activated in the ribbons, enabling carrier-envelope phase control spanning a range of π over a wide band of frequencies (∼1–3 THz). This is achieved solely through the ribbon array geometry using linearly polarized optical excitation of the ribbons. The arrays enable precise control of the THz phase and amplitude, opening the door to advanced structured THz wavefront synthesis using ultrathin dielectric metasurfaces.

carrier-envelope phase↗
DOE OSTI2022

Vibrational fingerprints of ferroelectric HfO 2

Hafnia (HfO 2 ) is a promising material for emerging chip applications due to its high-κ dielectric behavior, suitability for negative capacitance heterostructures, scalable ferroelectricity, and silicon compatibility. The lattice dynamics along with phononic properties such as thermal conductivity, contraction, and heat capacity are under-explored, primarily due to the absence of high quality single crystals. Herein, we report the vibrational properties of a series of HfO 2 crystals stabilized with yttrium (chemical formula HfO2: xY, where x = 20, 12, 11, 8, and 0%) and compare our findings with a symmetry analysis and lattice dynamics calculations. We untangle the effects of Y by testing our calculations against the measured Raman and infrared spectra of the cubic, antipolar orthorhombic, and monoclinic phases and then proceed to reveal the signature modes of polar orthorhombic hafnia. This work provides a spectroscopic fingerprint for several different phases of HfO 2 and paves the way for an analysis of mode contributions to high-κ dielectric and ferroelectric properties for chip technologies.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Solvent Polarity Independent Symmetry-Breaking Charge Separation in a Slip-Stacked Covalent Terrylene Monoimide Dimer

The design of organic materials capable of efficient photoinduced charge separation in low-polarity environments is a critical challenge for advancing organic photovoltaics. Symmetry-breaking charge separation (SB-CS) offers a promising route to efficient charge separation with minimal energy loss; however, in conventional organic materials this process typically relies on polar solvents to stabilize the charge-separated state. Here, we investigate a slip-stacked terrylene monoimide dimer (TMI 2 ) engineered with intrinsic electronic asymmetry to circumvent this limitation. We demonstrate through a comprehensive suite of ultrafast spectroscopic techniques that TMI 2 undergoes remarkably efficient SB-CS regardless of solvent polarity enabled by the permanent dipole moment of TMI and the accessible intramolecular charge-transfer (ICT) character of its monomer units. Furthermore, analysis of vibronic coherences reveals that the initial state mixing is actively driven by a 193 cm –1 intermolecular mode, while the final SB-CS state is marked by a distinct vibrational fingerprint of the radical ion pair product. Our findings reveal how the intrinsic electronic asymmetry of the TMI monomers that constitute TMI 2 creates an efficient charge separation pathway that precludes the need for external stabilization from a polar solvent. Here, this work establishes a powerful molecular design principle for leveraging intrinsic monomeric asymmetry to achieve efficient charge separation in low-dielectric environments, with significant implications for the development of next-generation organic optoelectronic materials.

Aromatic compounds↗
DOE OSTI2024

Tantalum pentoxide: a new material platform for high-performance dielectric metasurface optics in the ultraviolet and visible region

Dielectric metasurfaces, composed of planar arrays of subwavelength dielectric structures that collectively mimic the operation of conventional bulk optical elements, have revolutionized the field of optics by their potential in constructing high-efficiency and multi-functional optoelectronic systems on chip. The performance of a dielectric metasurface is largely determined by its constituent material, which is highly desired to have a high refractive index, low optical loss and wide bandgap, and at the same time, be fabrication friendly. Here, we present a new material platform based on tantalum pentoxide (Ta 2 O 5 ) for implementing high-performance dielectric metasurface optics over the ultraviolet and visible spectral region. This wide-bandgap dielectric, exhibiting a high refractive index exceeding 2.1 and negligible extinction coefficient across a broad spectrum, can be easily deposited over large areas with good quality using straightforward physical vapor deposition, and patterned into high-aspect-ratio subwavelength nanostructures through commonly-available fluorine-gas-based reactive ion etching. We implement a series of high-efficiency ultraviolet and visible metasurfaces with representative light-field modulation functionalities including polarization-independent high-numerical-aperture lensing, spin-selective hologram projection, and vivid structural color generation, and the devices exhibit operational efficiencies up to 80%. Our work overcomes limitations faced by scalability of commonly-employed metasurface dielectrics and their operation into the visible and ultraviolet spectral range, and provides a novel route towards realization of high-performance, robust and foundry-manufacturable metasurface optics.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Active learning of polarizable nanoparticle phase diagrams for the guided design of triggerable self-assembling superlattices

Polarizable nanoparticles are of interest in materials science because of their rich and complex phase behavior that can be used to engineer nanostructured materials with long-range crystalline order. To understand and rationally navigate the design space of polarizable nanoparticles for self-assembling highly ordered superlattices, we developed a coarse-grained computational model to describe the nanoparticle-nanoparticle interactions in implicit solvent and employ the computationally efficient image method to model many-body polarization interactions. We conducted high-throughput virtual screening over a five-dimensional particle design space spanned by temperature, particle size, particle charge, particle dielectric, and solvent dielectric using enhanced sampling molecular dynamics calculations within an active learning framework to efficiently map out the regions of thermodynamic stability of the self-assembled aggregates. We validate our predictions in comparisons against small angle x-ray scattering measurements of gold nanoparticles surface functionalized with metal chalcogenide ligands. Lastly, we use our validated phase maps to computationally design switchable nanostructured materials capable of triggered assembly and disassembly as a function of temperature and solvent dielectric with potential applications as sensors, smart windows, optoelectronic devices, and in medical diagnostics.

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

Pulse duration dependent effects of ultrafast laser induced damage on a 1030 nm multi-layer dielectric mirror for high repetition rate, high average power laser systems

High repetition rate, high peak, and average power laser systems are crucial for next-generation particle accelerators, inertial confinement fusion, and secondary particle sources. These applications demand durable laser optics, particularly interference coatings on optics lasting millions of shots at high fluence. This study focuses on designing, testing, and simulating multi-layer dielectric (MLD) mirrors for pulse durations of 260 fs, 77 fs, and 25 fs at 1030 nm wavelength and 45-degree incidence angle with p -polarization. S-on-1 laser-induced damage thresholds (LIDT) for varying pulse numbers were determined, with single-shot LIDT values of 0.98 Jcm -2 , 1.63 Jcm -2 , and 2.3 Jcm -2 for 25 fs, 77 fs, and 260 fs respectively. A strong correlation between blister shape and local fluence was observed, implying that the layer expansion in a blister depends on local fluence. We have also examined mechanisms responsible for laser-induced stress generation and energy release rates in blister formation. Damage mechanisms are further explored by finite-difference time-domain (FDTD) simulations, incorporating Keldysh strong field ionization, whose predictions were in excellent agreement with the onset of damage determined experimentally. These findings offer insights for enhancing MLD coating technology, promising more efficient and resilient laser systems for diverse scientific and industrial applications.

Noor, Mohamed Yaseen (ORCID:000000021036644X)↗
DOE OSTI2024

Imaging Valley Excitons in a 2D Semiconductor with Scanning Tunneling Microscope-Induced Luminescence

Valley excitons dominate the optoelectronic response of transition-metal dichalcogenides and are drastically affected by structural and environmental inhomogeneities localized in these materials. Critical to understanding and controlling these nanoscale excitonic changes is the ability to correlate the imaging of excitonic states with crystalline structures on the atomic scale. Here, in this study, we apply scanning tunneling microscope-induced luminescence microscopy to image valley excitons in a semiconducting transition-metal dichalcogenide monolayer decoupled by a 10 nanometer-thick hexagonal-boron-nitride flake incorporated in a lateral homojunction on an Au electrode surface. This design enables the observation of chiral excitonic emission arising from neutral and charged valley excitons of the monolayer semiconductor at ambipolar voltages with a quantum efficiency up to similar to ~10 -5 photon/electron. The measured light helicity demonstrates considerable circular polarization dependent on the sample voltage, reaching as much as 40%. The real-space luminescence imaging maps$-$at subnanometer resolution$-$of the valley excitons reveal striking spatial variations associated with localized inhomogeneities, including surface impurities and possibly nanoscale dielectric and/or potential disorders in the monolayer. Our study introduces a promising format for 2D materials to explore and tailor their optoelectronic processes at the atomic scale.

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

Ferrielectricity in the Archetypal Antiferroelectric, PbZrO 3

Antiferroelectric materials, where the transition between antipolar and polar phase is controlled by external electric fields, offer exceptional energy storage capacity with high efficiencies, giant electrocaloric effect, and superb electromechanical response. PbZrO 3 is the first discovered and the archetypal antiferroelectric material. Nonetheless, substantial challenges in processing phase pure PbZrO 3 have limited studies of the undoped composition, hindering understanding of the phase transitions in this material or unraveling the controversial origins of a low-field ferroelectric phase observed in lead zirconate thin films. Here, leveraging highly oriented PbZrO 3 thin films, a room-temperature ferrielectric phase is observed in the absence of external electric fields, with modulations of amplitude and direction of the spontaneous polarization and large anisotropy for critical electric fields required for phase transition. The ferrielectric state observations are qualitatively consistent with theoretical predictions, and correlate with very high dielectric tunability, and ultrahigh strains (up to 1.1%). This work suggests a need for re-evaluation of the fundamental science of antiferroelectricity in this archetypal material.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Zonal flow screening in negative triangularity tokamaks

Here, this paper presents a comparative study of zonal flow screening in positive and negative triangularity tokamaks. Neoclassical screening sets the strength of zonal flow shear for fixed drive and damping. Orbit calculations show that the radial excursions of trapped particles are reduced in negative triangularity tokamaks, as compared to positive triangularity. Yet surprisingly, the neoclassical dielectric susceptibility actually increases with decreasing triangularity, such that the susceptibility is higher for negative triangularity than for positive triangularity. This is because the reduction in neoclassical polarization by shrinking the banana width is offset by the increase in neoclassical polarization by the enhancement of trapped fraction for negative triangularity. As a result, the zonal flow screening length is actually enhanced for negative triangularity, as compared to positive triangularity. Hence, the zonal flow residual is smaller for negative triangularity than for positive triangularity. Results from gyrokinetic simulations support the analytic calculations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Broadband, 920-nm mirror thin film damage competition

This year’s competition proposed to survey the state-of-the-art broadband, near-IR multilayer dielectric (MLD) mirrors designed for ultra-short, pulsed laser applications. The requirements for the coatings were a minimum reflection of 99.5% at 45-degree incidence angle for S-polarization from 830 nm to 1010 nm and group delay dispersion (GDD) < ± 50 fs 2 . The participants in this effort selected the coating materials, coating design, and deposition method. Samples were damage tested at a single testing facility to enable direct comparison among the participants using a 25 ± 5 fs OPCPA laser system operating at 5 Hz. A double blind test assured sample and submitter anonymity. The damage performance results, sample rankings, details of the deposition processes, coating materials and substrate cleaning methods are shared here. We found that multilayer coatings using tantala and/or hafnia as high index materials were top performers within several coating deposition groups. Specifically, dense coatings by ion-beam sputtering (IBS), magnetron sputtering (MS), and electron-beam ion assisted deposition (e-beam IAD) exhibited highest damage initiation onset (LIDT) while e-beam coatings were low performers. In addition, damage growth onset (LDGT) was also examined and the results are reported here for all samples as this performance metric plays an important role in establishing the safe operational conditions for larger aperture, ultrashort pulsed lasers. As a result, not all coating samples in the survey met the GDD requirements stated above and associated measurements are discussed in the context of the present and past competitions focused on similar broadband, near-IR MLD coatings.

42 ENGINEERING↗
DOE OSTI2020

Tuning the charge transfer character of the multiexciton state in singlet fission

Intramolecular singlet fission (SF) produces the multiexciton correlated triplet pair state, (T 1 T 1 ), prior to the formation of free triplet excitons. The nature of the multiexciton state is complex, as generation of the (T 1 T 1 ) state may involve a charge transfer (CT) intermediate and has been shown to have both mixed electronic and spin characters. According to transient absorption spectroscopy, a linear terrylene-3,4:11,12-bis(dicarboximide) dimer (TDI 2 ) exhibits solvent-dependent excited-state dynamics. As solvent polarity increases from 1,2,4-trichlorobenzene (ε = 2.2) to chlorobenzene (ε = 5.6) to 1,2-dichlorobenzene (ε = 9.9), the SF rate in TDI2 increases and the multiexciton state, which can be thought of as a linear combination of the 1 (S 1 S 0 ), CT, and (T 1 T 1 ) states, gains more CT character. Eventually, the CT state becomes a trap state as indicated by symmetry-breaking charge separation in TDI2 in pyridine (ε = 12.3). The dielectric environment influences not only the SF rate and the relative contributions of the 1 (S 1 S 0 ), CT, and (T 1 T 1 ) states to the overall multiexciton state but also the rate at which the state mixing evolves, with faster dynamics in higher polarity solvents. More importantly, the tunability and presence of strong CT character in the multiexciton state have implications for SF applications since they often rely on electron transfer from the free triplet excitons. This enhanced CT character in the (T 1 T 1 ) state may assist with two-electron transfer directly from the (T 1 T 1 ) state, allowing for facile extraction of charges in intramolecular SF systems whose (T 1 T 1 ) states do not always efficiently dissociate to two triplet excitons.

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

Atomic-scale imaging of frequency-dependent phonon anisotropy

Directly visualizing vibrational anisotropy in individual phonon modes is essential for understanding a wide range of intriguing optical, thermal and elastic phenomena in materials. Although conventional optical and diffraction techniques have been used to estimate vibrational anisotropies, they fall short in achieving the spatial and energy resolution necessary to provide detailed information. Here, we introduce a new form of momentum-selective electron energy-loss spectroscopy, which enables the element-resolved imaging of frequency- and symmetry-dependent vibrational anisotropies with atomic resolution. Vibrational anisotropies manifest in different norms of orthogonal atomic displacements, known as thermal ellipsoids. Using the centrosymmetric strontium titanate as a model system, we observed two distinct types of oxygen vibrations with contrasting anisotropies: oblate thermal ellipsoids below 60 meV and prolate ones above 60 meV. In non-centrosymmetric barium titanate, our approach can detect subtle distortions of the oxygen octahedra by observing the unexpected modulation of q-selective signals between apical and equatorial oxygen sites near 55 meV, which originates from reduced crystal symmetry and may also be linked to ferroelectric polarization. These observations are quantitatively supported by theoretical modelling, which demonstrates the reliability of our approach. The measured frequency-dependent vibrational anisotropies shed new light on the dielectric and thermal behaviours governed by acoustic and optical phonons. Furthermore, the ability to visualize phonon eigenvectors at specific crystallographic sites with unprecedented spatial and energy resolution opens new avenues for exploring dielectric, optical, thermal and superconducting properties.

Ferroelectrics and multiferroics↗
DOE OSTI2022

A Landau–Devonshire analysis of strain effects on ferroelectric Al 1-x Sc x N

We present a thermodynamic analysis of the recently discovered nitride ferroelectric materials using the classic Landau–Devonshire approach. Electrostrictive and dielectric stiffness coefficients of Al 1-x Sc x N with a wurtzite structure (6 mm) are determined using a free energy density function assuming a hexagonal parent phase (6/mmm), with the first-order phase transition based on the dielectric stiffness relationships. The results of this analysis show that the strain sensitivity of the energy barrier is one order of magnitude larger than that of the spontaneous polarization in these wurtzite ferroelectrics, yet both are less sensitive to strain compared to classic perovskite ferroelectrics. These analysis results reported here explain experimentally reported sensitivity of the coercive field to elastic strain/stress in Al 1-x Sc x N films and would enable further thermodynamic analysis via phase field simulation and related methods.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

An SF 6 gas-insulated −500 kV DC conical insulator vacuum feedthrough

A test electrode was biased to −500 kV direct current (DC) by means of a novel SF 6 gas-insulated conical alumina insulator feedthrough. The design enables the extreme high vacuum conditions required by spin-polarized electron sources by reducing the photogun vacuum chamber volume compared to coaxial cylindrical insulators. In contrast to conventional inverted-insulator photogun designs that rely on solid dielectric interfaces for high-voltage terminations, the present design employs a pressurized SF 6 intervening volume between a conical alumina insulator and a modified commercial epoxy high-voltage cable receptacle. Here, this approach enables the use of commercially available cable hardware while extending the demonstrated operating voltage of solid feedthroughs. A maximum voltage of −500 kV was applied to a test electrode attached to the narrow end of the feedthrough inside a chamber filled with SF 6 at 170.3 kPa (10 psig) and later under vacuum to −259 kV, limited by field emission. The results demonstrate that a commercial high-voltage cable combined with a custom-designed SF 6 gas-insulated vacuum feedthrough can be used to bias photogun electrodes to −500 kV DC.

Palacios-Serrano, Gabriel [Thomas Jefferson Nation↗
DOE OSTI2024

Broadband 920-nm mirror thin film damage competition

The 2023 Laser Damage conference thin-film damage competition was devoted to a survey on the state-of-the-art broadband near-IR multilayer dielectric (MLD) mirrors designed for ultra-short pulsed laser applications. The requirements for the coatings were a minimum reflection of 99.5% at 45-deg incidence angle for S-polarization from 830 nm to 1010 nm and group delay dispersion (GDD) < ± 50fs 2 . The participants were allowed to select the coating materials, coating design, and coating deposition method. Samples were damage tested at a single testing facility to enable direct comparison among the participants using a 25 ± 5 fs optical parametric chirped-pulse amplification (OPCPA) laser system operating at 5 Hz. The testing results from this set of 37 samples showed that dense coatings by ion-beam sputtering (IBS), magnetron sputtering (MS), and electron-beam ion assisted deposition (e-beam IAD) exhibited highest damage initiation onset (laser-induced damage threshold or LIDT) while e-beam coatings were low performers. In addition, multilayer coatings using tantala and/or hafnia as high index materials were top performers. Furthermore, this competition included for the first time the measurement of the damage growth onset (laser-induced damage growth threshold or LDGT). This latter performance metric plays an important role in establishing the safe operational conditions for larger aperture ultrashort pulsed lasers. Information pertaining to the morphology of the damage sites and their evolution under subsequent exposure to different laser fluences leading to damage growth is presented. Finally, not all coating samples in the survey met the GDD requirements stated above and associated measurements are discussed in the context of the present and past thin-film damage competitions focused on similar broadband near-IR MLD coatings.

23 broadband high reflectors↗
DOE OSTI2023

Voltage‐Modulated Untwist Deformations and Multispectral Optical Effects from Ion Intercalation into Chiral Ceramic Nanoparticles

Abstract Reconfiguration of chiral ceramic nanostructures after ion intercalation should favor specific nanoscale twists leading to strong chiroptical effects. In this work, V 2 O 3 nanoparticles are shown to have “built‐in” chiral distortions caused by binding of tartaric acid enantiomers to the nanoparticle surface. As evidenced by spectroscopy/microscopy techniques and calculations of nanoscale chirality measures, the intercalation of Zn 2+ ions into the V 2 O 3 lattice results in particle expansion, untwist deformations, and chirality reduction. Coherent deformations in the particle ensemble manifest as changes in sign and positions of circular polarization bands at ultraviolet, visible, mid‐infrared (IR), near‐IR (NIR), and IR wavelengths. The g‐ factors observed for IR and NIR spectral diapasons are ≈100–400 times higher than those for previously reported dielectric, semiconductor, and plasmonic nanoparticles. Nanocomposite films layer‐by‐layer assembled (LBL) from V 2 O 3 nanoparticles reveal cyclic‐voltage‐driven modulation of optical activity. Device prototypes for IR and NIR range problematic for liquid crystals and other organic materials are demonstrated. High optical activity, synthetic simplicity, sustainable processability, and environmental robustness of the chiral LBL nanocomposites provide a versatile platform for photonic devices. Similar reconfigurations of particle shapes are expected for multiple chiral ceramic nanostructures, leading to unique optical, electrical, and magnetic properties.

36 MATERIALS SCIENCE↗