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At least 1,675 records · Page 93
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Photonic Crystal Waveguides for >90% Light Trapping Efficiency in Luminescent Solar Concentrators

Luminescent solar concentrators are currently limited in their potential concentration factor and solar conversion efficiency by the inherent escape cone losses present in conventional planar dielectric waveguides. Here, we demonstrate that photonic crystal slab waveguides tailored for luminescent solar concentrator applications can exhibit >90% light trapping efficiency. This is achieved by use of quantum dot luminophores embedded within the waveguide that absorb light at photon energies corresponding to photonic crystal leaky modes that couple to incoming sunlight. The luminophores then emit at lower photon energies into photonic crystal bound modes that enable highly efficient light trapping in slab waveguides of wavelength-scale thickness. Photonic crystal waveguides thus nearly eliminate escape cone losses, and overcome the performance limitations of previously proposed wavelength-selective dielectric multilayer filters. We describe designs for hole-array and rod-array photonic crystals comprised of hydrogenated amorphous silicon carbide using CdSe/CdS quantum dots. Our analysis suggests that photonic crystal waveguide luminescent solar concentrators using these materials these can achieve light trapping efficiency above 92% and a concentration factor as high as 100.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Broadband Liquid Crystal Tunable Metasurfaces in the Visible: Liquid Crystal Inhomogeneities Across the Metasurface Parameter Space

Optical metasurfaces—planar nanostructured devices that can arbitrarily tailor the wavefront of light—may be reconfigured by changing their dielectric environment. The application of external stimuli to liquid crystals is a particularly promising means of tuning the optical properties of embedded metasurfaces because of liquid crystals' large and broadband optical anisotropy. However, the detailed behavior of liquid crystals immediately adjacent to the nanostructured meta-atoms elements is often overlooked, despite the optics of the device depending sensitively on this behavior (e.g., the spectral position of the meta-atom resonances). This is of increasing concern as the wavelength of operation further approaches the short-wavelength end of the visible spectrum and, therefore, the length scale of the inhomogeneities in the liquid crystal director field. In this manuscript, we undertake a fully comprehensive study, across the metasurface geometrical parameter space, of broadband (450-700 nm) all-dielectric liquid crystal tunable metasurfaces operating in the visible. Here, through combined experimental characterization, liquid crystal modeling, and optical simulations, we reveal and quantify the improved accuracy with which the optical properties of the liquid crystal tunable metasurfaces may be described, and identify the underlying physical mechanism: the three-dimensional spatial overlap of the liquid crystal director field and metasurface optical near fields in the vicinity of the meta-atoms.

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

Polarity-Tolerant Chloride Binding in Foldamer Capsules by Programmed Solvent-Exclusion

Persistent anion binding in a wide range of solution environments is a key challenge that continues to motivate and demand new strategies in synthetic receptor design. Though strong binding in low-polarity solvents has become routine, our ability to maintain high affinities in high-polarity solvents has not yet reached the standard set by nature. Anions are bound and transported regularly in aqueous environments by proteins that use secondary and tertiary structure to isolate anion binding sites from water. Inspired by this principle of solvent exclusion, we created a sequence-defined foldameric capsule whose global minimum conformation displays a helical folded state and is preorganized for 1:1 anion complexation. The high stability of the folded geometry and its ability to exclude solvent were supported by solid-state and solution phase studies. This capsule then withstood a 4-fold increase in solvent dielectric constant (εr) from dichloromethane (9) to acetonitrile (36) while maintaining a high and solvent-independent affinity of 10 5 M –1 ; ΔG ~ 28 kJ mol –1 . This behavior is unusual. More typical of solvent-dependent behavior, Cl – affinities were seen to plummet in control compounds, such as aryl-triazole macrocycles and pentads, with their solvent-exposed binding cavities susceptible to dielectric screening. Finally, dimethyl sulfoxide denatures the foldamer by putative solvent binding, which then lowers the foldamer’s Cl – affinity to normal levels. Furthermore, the design of this capsule demonstrates a new prototype for the development of potent receptors that can operate in polar solvents and has the potential to help manage hydrophilic anions present in the hydrosphere and biosphere.

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

Chemical Design of Pb-Free Relaxors for Giant Capacitive Energy Storage

Dielectric capacitors have captured substantial attention for advanced electrical and electronic systems. Developing dielectrics with high energy density and high storage efficiency is challenging owing to the high compositional diversity and the lack of general guidelines. Herein, we propose a map that captures the structural distortion ($\delta$) and tolerance factor (t) of perovskites to design Pb-free relaxors with extremely high capacitive energy storage. Our map shows how to select ferroelectric with large $\delta$ and paraelectric components to form relaxors with a t value close to 1 and thus obtaining eliminated hysteresis and large polarization under a high electric breakdown. Taking the Bi 0.5 Na 0.5 TiO 3 -based solid solution as an example, we demonstrate that composition-driven predominant order-disorder characteristic of local atomic polar displacements endows the relaxor with a slushlike structure and strong local polar fluctuations at several nanoscale. This leads to a giant recoverable energy density of 13.6 J cm -3 , along with an ultrahigh efficiency of 94%, which is far beyond the current performance boundary reported in Pb-free bulk ceramics. In conclusion, our work provides a solution through rational chemical design for obtaining Pb-free relaxors with outstanding energy-storage properties.

25 ENERGY STORAGE↗
DOE OSTI2023

Framework-Topology-Controlled Singlet Fission in Metal–Organic Frameworks

Singlet fission (SF) has been explored as a viable route to improve photovoltaic performance by producing more excitons. Efficient SF is achieved through a high degree of interchromophoric coupling that facilitates electron super exchange to generate triplet pairs. However, strongly coupled chromophores often form excimers that can serve as an SF intermediate or a low-energy trap site. The succeeding decoherence process, however, requires an optimum electronic coupling to facilitate the isolation of triplet production from the initially prepared correlated triplet pair. Conformational flexibility and dielectric modulation can provide a means to tune the SF mechanism and efficiency by modulating the interchromophoric electronic interaction. Such a strategy cannot be easily adopted in densely stacked traditional organic solids. Here, we show that the assembly of the SF-active chromophores around well-defined pores of solution-stable metal-organic frameworks (MOFs) can be a great platform for a modular SF process. A series of three new MOFs, built out from 9,10-bis(ethynylenephenyl)anthracene-derived struts, show a topology-defined packing density and conformational flexibility of the anthracene core to dictate the SF mechanism. Various steady-state and transient spectroscopic data suggest that the initially prepared singlet population can prefer either an excimer-mediated SF or a direct SF (both through a virtual charge-transfer (CT) state). Finally, these solution-stable frameworks offer the tunability of the dielectric environment to facilitate the SF process by stabilizing the CT state. Given that MOFs are a great platform for various photophysical and photochemical developments, generating a large population of long-lived triplets can expand their utilities in various photon energy conversion schemes.

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

A molecular design approach towards elastic and multifunctional polymer electronics

Next-generation wearable electronics require enhanced mechanical robustness and device complexity. Besides previously reported softness and stretchability, desired merits for practical use include elasticity, solvent resistance, facile patternability and high charge carrier mobility. Here, we show a molecular design concept that simultaneously achieves all these targeted properties in both polymeric semiconductors and dielectrics, without compromising electrical performance. This is enabled by covalently-embedded in-situ rubber matrix (iRUM) formation through good mixing of iRUM precursors with polymer electronic materials, and finely-controlled composite film morphology built on azide crosslinking chemistry which leverages different reactivities with C–H and C=C bonds. The high covalent crosslinking density results in both superior elasticity and solvent resistance. When applied in stretchable transistors, the iRUM-semiconductor film retained its mobility after stretching to 100% strain, and exhibited record-high mobility retention of 1 cm 2 V -1 s -1 after 1000 stretching-releasing cycles at 50% strain. The cycling life was stably extended to 5000 cycles, five times longer than all reported semiconductors. Furthermore, we fabricated elastic transistors via consecutively photo-patterning of the dielectric and semiconducting layers, demonstrating the potential of solution-processed multilayer device manufacturing. The iRUM represents a molecule-level design approach towards robust skin-inspired electronics.

42 ENGINEERING↗
DOE OSTI2024

Photonic time-crystalline behaviour mediated by phonon squeezing in T a 2 NiSe 5

Photonic time crystals refer to materials whose dielectric properties are periodic in time, analogous to a photonic crystal whose dielectric properties is periodic in space. Here, we theoretically investigate photonic time-crystalline behaviour initiated by optical excitation above the electronic gap of the excitonic insulator candidate Ta 2 NiSe 5 . We show that after electron photoexcitation, electron-phonon coupling leads to an unconventional squeezed phonon state, characterised by periodic oscillations of phonon fluctuations. Squeezing oscillations lead to photonic time crystalline behaviour. The key signature of the photonic time crystalline behaviour is terahertz (THz) amplification of reflectivity in a narrow frequency band. The theory is supported by experimental results on Ta 2 NiSe 5 where photoexcitation with short pulses leads to enhanced THz reflectivity with the predicted features. We explain the key mechanism leading to THz amplification in terms of a simplified electron-phonon Hamiltonian motivated by ab-initio DFT calculations. Our theory suggests that the pumped Ta 2 NiSe 5 is a gain medium, demonstrating that squeezed phonon noise may be used to create THz amplifiers in THz communication applications.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Machine learning the electric field response of condensed phase systems using perturbed neural network potentials

Abstract The interaction of condensed phase systems with external electric fields is of major importance in a myriad of processes in nature and technology, ranging from the field-directed motion of cells (galvanotaxis), to geochemistry and the formation of ice phases on planets, to field-directed chemical catalysis and energy storage and conversion systems including supercapacitors, batteries and solar cells. Molecular simulation in the presence of electric fields would give important atomistic insight into these processes but applications of the most accurate methods such as ab-initio molecular dynamics (AIMD) are limited in scope by their computational expense. Here we introduce Perturbed Neural Network Potential Molecular Dynamics (PNNP MD) to push back the accessible time and length scales of such simulations. We demonstrate that important dielectric properties of liquid water including the field-induced relaxation dynamics, the dielectric constant and the field-dependent IR spectrum can be machine learned up to surprisingly high field strengths of about 0.2 V Å −1 without loss in accuracy when compared to ab-initio molecular dynamics. This is remarkable because, in contrast to most previous approaches, the two neural networks on which PNNP MD is based are exclusively trained on molecular configurations sampled from zero-field MD simulations, demonstrating that the networks not only interpolate but also reliably extrapolate the field response. PNNP MD is based on rigorous theory yet it is simple, general, modular, and systematically improvable allowing us to obtain atomistic insight into the interaction of a wide range of condensed phase systems with external electric fields.

Science & Technology - Other Topics↗
DOE OSTI2025

Emergent topological polarization textures in relaxor ferroelectrics

Relaxor ferroelectrics underpin high-performance actuators and sensors, yet the nature of polar heterogeneities driving their broadband dielectric response remains debated. Using a unified, multimodal structural refinement framework— simultaneously fitting complementary X-ray and neutron total scattering, X-ray absorption spectra, and diffuse scattering—we reconstruct 3D mesoscale polarization maps in the classic relaxor system PbMg 1/3 Nb 2/3 O 3 –PbTiO 3 . We uncover self-organized swirling polarization textures with half-skyrmion (meron) vortices, challenging models of independent polar nanoregions. These textures, characterized by smooth changes in the polarization direction, originate from overlapping volumes in which the projections of locally correlated polarization vectors onto each volume’s long axis share the same sign. Vortex cores correlate strongly with local charge and strain gradients imposed by compositional heterogeneities. In this work, our results suggest that chemical disorder, acting via depolarizing and strain fields, stabilizes topological vortex textures of the polarization field, offering a route for engineering new dielectric and ferroelectric functionalities.

Eremenko, Maksim [National Institute of Standards ↗
DOE OSTI2025

Dynamic realization of emergent high-dimensional optical vortices

The dimensionality of vortical structures has recently been extended beyond two dimensions, providing additional topological complexity and robustness for high-capacity information processing and turbulence control. The generation of high-dimensional vortical structures has mostly been demonstrated in classical systems through the complex interference of fluidic, acoustic, or electromagnetic waves. However, natural materials rarely support three- or higher-dimensional vortical structures and their physical interactions. Here, we experimentally demonstrate a high-dimensional gradient thickness optical cavity (GTOC) in which the optical coupling of planar metal-dielectric multilayers implements topological interactions across multiple dimensions. At non-trivial topological phases, high-dimensional GTOC induces high-dimensional vortical structures in generalized parameter space in three, four dimensions, and beyond. These emergent high-dimensional vortical structures are observed under electro-optic tomography as optical vortex dynamics in two-dimensional real-space, employing the optical thicknesses of dielectric layers as synthetic dimensions. Our findings hold significant promise for emulating high-dimensional physics and developing active topological photonic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Experimental evidence of plasmarons and effective fine structure constant in electron-doped graphene/h-BN heterostructure

Electron-electron interaction is fundamental in condensed matter physics and can lead to composite quasiparticles called plasmarons, which strongly renormalize the dispersion and carry information of electron-electron coupling strength as defined by the effective fine structure constant $α$ $^{*}_{ee}$. Although h-BN with unique dielectric properties has been widely used as an important substrate for graphene, so far there is no experimental report of plasmarons in graphene/h-BN yet. Here, we report direct experimental observation of plasmaron dispersion in graphene/h-BN heterostructures through angle-resolved photoemission spectroscopy (ARPES) measurements upon in situ electron doping. Characteristic diamond-shaped dispersion is observed near the Dirac cone in both 0° (aligned) and 13.5° (twisted) graphene/h-BN, and the electron-electron interaction strength $α$ $^{*}_{ee}$ is extracted to be $α$ $^{*}_{ee}$ ≈ 0.9 ± 0.1, highlighting the important role of electron-electron interaction. Our results suggest graphene/h-BN as an ideal platform for investigating strong electron-electron interaction with weak dielectric screening, and lays fundamental physics for gate-tunable nano-electronics and nano-plasmonics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
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 OSTI2024

Giant energy storage and power density negative capacitance superlattices

Dielectric electrostatic capacitors, because of their ultrafast charge-discharge, are desirable for high-power energy storage applications. Along with ultrafast operation, on-chip integration can enable miniaturized energy storage devices for emerging autonomous microelectronics and microsystems. Moreover, state-of-the-art miniaturized electrochemical energy storage systems-microsupercapacitors and microbatteries-currently face safety, packaging, materials and microfabrication challenges preventing on-chip technological readiness, leaving an opportunity for electrostatic microcapacitors. Here, in this study, we report record-high electrostatic energy storage density (ESD) and power density, to our knowledge, in HfO 2 -ZrO 2 -based thin film microcapacitors integrated into silicon, through a three-pronged approach. First, to increase intrinsic energy storage, atomic-layer-deposited antiferroelectric HfO 2 -ZrO 2 films are engineered near a field-driven ferroelectric phase transition to exhibit amplified charge storage by the negative capacitance effect, which enhances volumetric ESD beyond the best-known back-end-of-the-line-compatible dielectrics (115 J cm -3 ). Second, to increase total energy storage, antiferroelectric superlattice engineering scales the energy storage performance beyond the conventional thickness limitations of HfO 2 -ZrO 2 -based (anti)ferroelectricity (100-nm regime). Third, to increase the storage per footprint, the superlattices are conformally integrated into three-dimensional capacitors, which boosts the areal ESD nine times and the areal power density 170 times that of the best-known electrostatic capacitors: 80 mJ cm -2 and 300 kW cm -2 , respectively. This simultaneous demonstration of ultrahigh energy density and power density overcomes the traditional capacity-speed trade-off across the electrostatic-electrochemical energy storage hierarchy. Furthermore, the integration of ultrahigh-density and ultrafast-charging thin films within a back-end-of-the-line-compatible process enables monolithic integration of on-chip microcapacitors, which can unlock substantial energy storage and power delivery performance for electronic microsystems.

25 ENERGY STORAGE↗
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 OSTI2025

PAH101: A GW+BSE Dataset of 101 Polycyclic Aromatic Hydrocarbon (PAH) Molecular Crystals

Abstract The excited-state properties of molecular crystals are important for applications in organic electronic devices. TheGWapproximation and Bethe-Salpeter equation (GW+BSE) is the state-of-the-art method for calculating the excited-state properties of crystalline solids with periodic boundary conditions. We present the PAH101 dataset ofGW+BSE calculations for 101 molecular crystals of polycyclic aromatic hydrocarbons (PAHs) with up to ~500 atoms in the unit cell. To the best of our knowledge, this is the firstGW+BSE dataset for molecular crystals. The data records include theGWquasiparticle band structure, the fundamental band gap, the static dielectric constant, the first singlet exciton energy (optical gap), the first triplet exciton energy, the dielectric function, and optical absorption spectra for light polarized along the three lattice vectors. The dataset can be used to (i) discover materials with desired electronic/optical properties, (ii) identify correlations between DFT andGW+BSE quantities, and (iii) train machine learned models to help in materials discovery efforts.

Science & Technology - Other Topics↗
DOE OSTI2024

Control of work functions of nanophotonic components

Work function is an essential material’s property playing important roles in electronics, photovoltaics, and more recently, in nanophotonics. We have studied effects of organic, and inorganic dielectric materials on work functions of Au films in single layered, and multilayered structures. We found that measured work function of metallic surfaces can be affected by dielectric materials situated 10–100 nm away from the metallic surface. We have found that, (i) the glass underneath ~ 50 nm gold slab reduces the work function of gold, (ii) Rh590:PMMA increases the work function of a gold film deposited on top of the polymer, and (iii) reduces it if Rh590:PMMA is deposited on top of Au. (iv) With increase of the Rh590 concentration in PMMA, n, the work function first decreases (at n < 64 g/l), and then increases (at n > 64 g/l). (v) The work function of a Fabry–Perot cavity or an MIM waveguide is almost the same as that of single Au films of comparable thickness. The experimental results can be qualitatively explained in terms of a simple model taking into account adhesion of charged molecules to a metallic surface, and formation of a double layer of charges accelerating or decelerating electrons exiting the metal and decreasing or increasing the work function.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Solid-state thermometry via ionic–electronic coupling in two-dimensional heterostructures

The coupling of ionic and electronic transport in solid-state systems offers new opportunities for realizing compact, energy-efficient sensing technologies, yet practical implementations remain limited. In this article, we introduce a two-dimensional iontronic platform based on field-effect transistors that integrate monolayer MoS 2 channels with van der Waals bimetallic thiophosphates ( AB P 2 X 6 , A = Li, Cu, Ag and so on; B = In, Sc and so on; and X = S and Se) as ionic gate dielectrics to realize on-chip thermometry. Specifically, we exploit thermally activated ion migration within the gate dielectric leading to conductance modulation in the MoS 2 channel for temperature sensing. We achieve ~1–2 °C resolution, fast electronic readout and subpicojoule energy consumption in an ultracompact footprint (~1 µm 2 ). Beyond thermometry, these results establish bimetallic thiophosphates as a versatile platform for solid-state iontronics and broaden the functional design space of van der Waals heterostructures for sensing, actuation and adaptive electronics.

42 ENGINEERING↗