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DOE OSTI2013

Facile synthesis of QD-anchored composite particles with magnetite cluster cores ({sup n}Fe{sub 3}O{sub 4}@SiO{sub 2}@QDs)

Highlights: ► Triple layered Fe{sub 3}O{sub 4}/SiO{sub 2}/QDs were designed as fluorescent magnetic nanocomposites. ► Magnetite cluster-embedded silica exhibited strong and controllable magnetism. ► Effective conjugation between QDs and magnetic silica occurred at pH3. - Abstract: Magnetism-controlled fluorescent composite particles ({sup n}Fe{sub 3}O{sub 4}@SiO{sub 2}@QDs) were prepared as QD-anchored silica nanoparticles with magnetite cluster cores. First, citrate-capped magnetites (C-Fe{sub 3}O{sub 4}) were prepared by the co-precipitation method and subsequently complexed with 3-aminopropyl-trimethoxysilane (APTMS) at room temperature, consequently leading to the formation of magnetite clusters (A-{sup n}Fe{sub 3}O{sub 4}) with alkoxy terminated interfaces. The sol–gel reaction between A-{sup n}Fe{sub 3}O{sub 4} and tetraethoxysilane (TEOS) produced the core-shell {sup n}Fe{sub 3}O{sub 4}@SiO{sub 2}. The resulting core-shell particles exhibited superparamagnetic properties and controllable magnetism simply by adjusting the thickness of nonmagnetic silica layer. After then, amine-terminated {sup n}Fe{sub 3}O{sub 4}@SiO{sub 2} (NH{sub 2}–{sup n}Fe{sub 3}O{sub 4}@SiO{sub 2}) was conjugated with carboxy quantum dots (QDs) using an EDC coupling agent. The QD conjugation with NH{sub 2}–{sup n}Fe{sub 3}O{sub 4}@SiO{sub 2} of lower pH exhibited the higher photoluminescence (PL) intensity, and the resulting composite particles ({sup n}Fe{sub 3}O{sub 4}@SiO{sub 2}@QDs) can be a useful biomedical agent. This chemical strategy can be further applied to prepare the core-shell magnetic nanostructure with various oxide layers for specific applications.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Dimensional control of defect dynamics in perovskite oxide superlattices

Point defects play a critical role in the structural, physical, and interfacial properties of perovskite oxide superlattices. However, understanding of the fundamental properties of point defects in superlattices, especially their transport properties, is rather limited. Here, we report predictions of the stability and dynamics of oxygen vacancies in SrTiO 3 /PbTiO 3 oxide superlattices using first-principles calculations in combination with the kinetic Monte Carlo method. By varying the stacking period, i.e., changing of n in n STO/ n PTO, we discover a crossover from three-dimensional diffusion to primarily two-dimensional planar diffusion. Such planar diffusion may lead to novel designs of ionic conductors. We show that the dominant vacancy position may vary in the superlattices, depending on the superlattice structure and stacking period, contradicting the common assumption that point defects reside at interfaces. Moreover, we predict a significant increase in room-temperature ionic conductivity for 3STO/3PTO relative to the bulk phases. As a result, considering the variety of cations that can be accommodated in perovskite superlattices and the potential mismatch of spin, charge, and orbitals at the interfaces, this paper identifies a pathway to control defect dynamics for technological applications.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Coherent terahertz radiation with 2.8-octave tunability through chip-scale photomixed microresonator optical parametric oscillation

High-spectral-purity frequency-agile room-temperature sources in the terahertz spectrum are foundational elements for imaging, sensing, metrology, and communications. Here we present a chip-scale optical parametric oscillator based on an integrated nonlinear microresonator that provides broadly tunable single-frequency and multi-frequency oscillators in the terahertz regime. Through optical-to-terahertz down-conversion using a plasmonic nanoantenna array, coherent terahertz radiation spanning 2.8-octaves is achieved from 330 GHz to 2.3 THz, with ≈20 GHz cavity-mode-limited frequency tuning step and ≈10 MHz intracavity-mode continuous frequency tuning range at each step. By controlling the microresonator intracavity power and pump-resonance detuning, tunable multi-frequency terahertz oscillators are also realized. Furthermore, by stabilizing the microresonator pump power and wavelength, sub-100 Hz linewidth of the terahertz radiation with 10 –15 residual frequency instability is demonstrated. The room-temperature generation of both single-frequency, frequency-agile terahertz radiation and multi-frequency terahertz oscillators in the chip-scale platform offers unique capabilities in metrology, sensing, imaging and communications.

42 ENGINEERING↗

NASA NTRSDate not supplied

A Multiphysics Study to Improve Specific Energy of Primary Batteries for Low Temperature Operation for Deep Space Missions

Several lander missions on the outer planets such as Europa, Enceladus, and Titan require electrical power to operate scientific and communication equipment. The traditional power generation methods, such as a photovoltaic array, are not feasible as their efficiency drops significantly at these vast distances. The novel radioisotope power systems are not practical today based on current lander designs and the effectiveness of these systems. To perform in situ science on distant planets, a high specific energy battery (>700 Wh/kg) needs to operate for about 480 hours under cold temperatures (-40C or 0C) [1]. While a primary battery such as Li-CFx can provide high specific energy at room temperature, its specific capacity decreases significantly at low temperatures. One of the causes for this drop is low ion and electrical conductivity, and slower reaction kinetics. Slower transport and facile kinetics lead to an increase in the battery’s resistance and higher voltage drops during the cell operation, thus reducing specific capacity. Both the transport and kinetics show a strong dependence on temperature. Thus, a small temperature rise can lead to an increase in the reaction rate and ion conductivity; since the temperature, cell resistance, and specific capacity are interdependent. A conventional battery model accounts for ohmic, thermodynamic, and, electrochemical, and chemical decomposition heating. The ohmic heating can be controlled by designing a resistive microstructure and varying the ratios of the active materials [2]. The kinetics can be improved by increasing the surface area, reducing the particle size, or adding a catalyst. These parameters are often optimized to achieve high specific energy at room temperatures. A similar optimization study is not available at low temperatures and for a primary (high specific energy) battery. For this presentation, we will explore the effect of geometrical, microstructural, and material properties on optimal specific capacity at low temperatures through multiphysics simulations. The ion transport resistance depends on the porosity and the tortuosity of an electrode and the separator.

M. Mehta↗

DOE OSTI2020

Bi-directional tuning of thermal transport in SrCoO x with electrochemically induced phase transitions

Unlike the wide-ranging dynamic control of electrical conductivity, there does not exist an analogous ability to tune thermal conductivity by means of electric potential. The traditional picture assumes that atoms inserted into a material’s lattice act purely as a source of scattering for thermal carriers, which can only reduce thermal conductivity. In contrast, here we show that the electrochemical control of oxygen and proton concentration in an oxide provides a new ability to bi-directionally control thermal conductivity. On electrochemically oxygenating the brownmillerite SrCoO 2.5 to the perovskite SrCoO 3–δ , the thermal conductivity increases by a factor of 2.5, whereas protonating it to form hydrogenated SrCoO 2.5 effectively reduces the thermal conductivity by a factor of four. This bi-directional tuning of thermal conductivity across a nearly 10 ± 4-fold range at room temperature is achieved by using ionic liquid gating to trigger the ‘tri-state’ phase transitions in a single device. We elucidated the effects of these anionic and cationic species, and the resultant changes in lattice constants and lattice symmetry on thermal conductivity by combining chemical and structural information from X-ray absorption spectroscopy with thermoreflectance thermal conductivity measurements and ab initio calculations. This ability to control multiple ion types, multiple phase transitions and electronic conductivity that spans metallic through to insulating behaviour in oxides by electrical means provides a new framework for tuning thermal transport over a wide range.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Benefits of Leapfrogging to Superefficiency and Low Global Warming Potential Refrigerants in Room Air Conditioning

Hydrofluorocarbons (HFCs) emitted from uses such as refrigerants and thermal insulating foam, are now the fastest growing greenhouse gases (GHGs), with global warming potentials (GWP) thousands of times higher than carbon dioxide (CO2). Because of the short lifetime of these molecules in the atmosphere, mitigating the amount of these short-lived climate pollutants (SLCPs) provides a faster path to climate change mitigation than control of CO2 alone. This has led to proposals from Africa, Europe, India, Island States, and North America to amend the Montreal Protocol on Substances that Deplete the Ozone Layer (Montreal Protocol) to phase-down high-GWP HFCs. Simultaneously, energy efficiency market transformation programs such as standards, labeling and incentive programs are endeavoring to improve the energy efficiency for refrigeration and air conditioning equipment to provide life cycle cost, energy, GHG, and peak load savings. In this paper we provide an estimate of the magnitude of such GHG and peak electric load savings potential, for room air conditioning, if the refrigerant transition and energy efficiency improvement policies are implemented either separately or in parallel. We find that implementing HFC refrigerant transition and energy efficiency improvement policies in parallel for room air conditioning, roughly doubles the benefit of either policy implemented separately. We estimate that shifting the 2030 world stock of room air conditioners from the low efficiency technology using high-GWP refrigerants to higher efficiency technology and low-GWP refrigerants in parallel would save between 340-790 gigawatts (GW) of peak load globally, which is roughly equivalent to avoiding 680-1550 peak power plants of 500MW each. This would save 0.85 GT/year annually in China equivalent to over 8 Three Gorges dams and over 0.32 GT/year annually in India equivalent to roughly twice India’s 100GW solar mission target. While there is some uncertainty associated with emissions and growth projections, moving to efficient room air conditioning (~30% more efficient than current technology) in parallel with low-GWP refrigerants in room air conditioning could avoid up to ~25 billion tonnes of CO2 in 2030, ~33 billion in 2040, and ~40 billion in 2050, i.e. cumulative savings up to 98 billion tonnes of CO2 by 2050. Therefore, superefficient room ACs using low-GWP refrigerants merit serious consideration to maximize peak load reduction and GHG savings.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2018

Locally Controlled Cu-Ion Transport in Layered Ferroelectric CuInP 2 S 6

Metal thiophosphates are gaining attention in the context of quasi-two-dimensional van der Waals functional materials. Alkali thiophosphates are investigated as ion conductors for solid electrolytes, and transition-metal thiophosphates are explored as a new class of ferroelectric materials. For the latter, a representative copper indium thiophosphate is ferrielectric at room temperature and, despite low polarization, exhibits giant negative electrostrictive coefficients. In this work, we reveal that ionic conductivity in this material enables localized extraction of Cu ions from the lattice with a biased scanning probe microscopy tip, which is surprisingly reversible. The ionic conduction is tracked through local volume changes with a scanning probe microscopy tip providing a current-free probing technique, which can be explored for other thiophosphates of interest. Nearly 90 nm-tall crystallites can be formed and erased reversibly on the surface of this material as a result of ionic motion, the size of which can be sensitively controlled by both magnitude and frequency of the electric field, as well as the ambient temperature. These experimental results and density functional theory calculations point to a remarkable resilience of CuInP 2 S 6 to large-scale ionic displacement and Cu vacancies, in part enabled by the metastability of Cu-deficient phases. Moreover, we have found that the piezoelectric response of CuInP 2 S 6 is enhanced by about 45% when a slight ionic modification is carried out with applied field. This new mode of modifying the lattice of CuInP 2 S 6 , and more generally ionically conducting thiophosphates, posits new prospects for their applications in van der Waals heterostructures, possibly in the context of catalytic or electronic functionalities.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Engineering collinear magnetization in hexagonal LuFeO 3 and magnetoelectric control of skyrmions in hexagonal 2D epilayers

Cubic, perovskite-structure ABO 3- and A 1–x A’ x BO 3 -type oxides have been investigated extensively while their hexagonal structure versions have not, even though they are multiferroic and can form heterostructures with hexagonal 2D materials. In particular, multiferroic 2D epilayers may lead to strong magnetoelectric coupling. Hexagonal RFeO 3 ferrites, where R is a rare-earth element (Lu, Yb, etc.), are excellent candidates, but their ferromagnetism isweak. In this paper, we employ density-functional-theory (DFT) calculations and first show that heavy electron doping of hexagonal LuFeO 3 (h-LFO), namely Lu 1–x Hf x FeO 3 (h-LHFO), leads to spin-disproportionation of the Fe sublattices and, especially for x = 1/2 and 2/3, to robust, room-temperature, out-of-plane, collinear ferrimagnetism that is stabilized by a Jahn-Teller metal-to-insulator transition. We then show that h-LHFO/h-2D heterostructures, where h-2D is the FE/ FM monolayer MnSTe, stabilize skyrmions without an external magnetic field and control their chirality by an external electric field through the h-LHFO polarization, opening up a new realm for magnetoelectric applications.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Understanding and control of bipolar self-doping in copper nitride

Semiconductor materials that can be doped both n-type and p-type are desirable for diode-based applications and transistor technology. Copper nitride (Cu{sub 3}N) is a metastable semiconductor with a solar-relevant bandgap that has been reported to exhibit bipolar doping behavior. However, deeper understanding and better control of the mechanism behind this behavior in Cu{sub 3}N is currently lacking in the literature. In this work, we use combinatorial growth with a temperature gradient to demonstrate both conduction types of phase-pure, sputter-deposited Cu{sub 3}N thin films. Room temperature Hall effect and Seebeck effect measurements show n-type Cu{sub 3}N with 10{sup 17} electrons/cm{sup 3} for low growth temperature (≈35 °C) and p-type with 10{sup 15} holes/cm{sup 3}–10{sup 16} holes/cm{sup 3} for elevated growth temperatures (50 °C–120 °C). Mobility for both types of Cu{sub 3}N was ≈0.1 cm{sup 2}/Vs–1 cm{sup 2}/Vs. Additionally, temperature-dependent Hall effect measurements indicate that ionized defects are an important scattering mechanism in p-type films. By combining X-ray absorption spectroscopy and first-principles defect theory, we determined that V{sub Cu} defects form preferentially in p-type Cu{sub 3}N, while Cu{sub i} defects form preferentially in n-type Cu{sub 3}N, suggesting that Cu{sub 3}N is a compensated semiconductor with conductivity type resulting from a balance between donor and acceptor defects. Based on these theoretical and experimental results, we propose a kinetic defect formation mechanism for bipolar doping in Cu{sub 3}N that is also supported by positron annihilation experiments. Overall, the results of this work highlight the importance of kinetic processes in the defect physics of metastable materials and provide a framework that can be applied when considering the properties of such materials in general.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2015

Benefits of Leapfrogging to Superefficiency and Low Global Warming Potential Refrigerants in Room Air Conditioning

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2013

Structure and microwave dielectric properties of Ba{sub 3}(VO{sub 4}){sub 2}–Zn{sub 2−x}SiO{sub 4−x} ceramic composites

Highlights: ► New Ba{sub 3}(VO{sub 4}){sub 2}–Zn{sub 1.87}SiO{sub 3.87} microwave dielectric composite ceramic was reported. ► The single-phase willemite was obtained by controlling of ZnO deficiency. ► The composite with 40 wt% Zn{sub 1.87}SiO{sub 3.87} exhibited excellent τ{sub f} value of 0.4 ppm/°C. - Abstract: Microwave dielectric ceramic composites with compositions of (1 − y)Ba{sub 3}(VO{sub 4}){sub 2}–yZn{sub 2−x}SiO{sub 4−x} (y = 0.4–0.6, x = 0.13) have been prepared by firing mixtures of Ba{sub 3}(VO{sub 4}){sub 2} and Zn{sub 1.87}SiO{sub 3.87}. The X-ray diffraction (XRD) analysis revealed that Zn{sub 2}SiO{sub 4} with a willemite phase can be obtained by appropriately controlling the ZnO deficiency. The starting Zn{sub 1.87}SiO{sub 3.87} powder should be thus composed of the ZnSiO{sub 4} crystal phase and redundant SiO{sub 2} amorphous phase at room temperature. The scanning electron microscopy studies demonstrated the coexistence of Zn{sub 2}SiO{sub 4} and Ba{sub 3}(VO{sub 4}){sub 2} phases in the sintered bodies, as further confirmed by the XRD and Raman results. The near-zero temperature coefficients of the resonant frequency (τ{sub f}) could be achieved by adjusting the relative content of the two phases owing to their opposite τ{sub f} values. The existence of a slight amount of secondary phases, element interdiffusion and non-stoichiometry such as Zn deficiency altogether made the predicted property values deviate from the experimentally measured ones. The composite ceramics with 40 wt% Zn{sub 1.87}SiO{sub 3.87} sintered at 1100 °C exhibited desirable microwave dielectric properties of the quality factor Q × f ∼ 23,000 GHz, dielectric constant ε{sub r} ∼ 9.3, and τ{sub f} ∼ 0.4 ppm/°C.

36 MATERIALS SCIENCE↗

DOE OSTI2011

Deformation of Olivine at Subduction Zone Conditions Determined from In situ Measurements with Synchrotron Radiation

We report measurements of the deformation stress for San Carlos olivine at pressures of 3-5 GPa, temperatures of 25-1150 C, and strain rates of 10{sup -7}-10{sup -5} s{sup -1}. We determine a deformation stress of approximately 2.5 GPa that is relatively temperature and strain rate independent in the temperature range of 400-900 C. The deformation experiments have been carried out on a deformation DIA (D-DIA) apparatus, Sam85, at X17B2, NSLS. Powder samples are used in these experiments. Enstatite (MgSiO{sub 3}) (3-5% total quality of sample) is used as the buffer to control the activity of silica. Ni foil is used in some experiments to buffer the oxygen fugacity. Water content is confirmed by IR spectra of the recovered samples. Samples are compressed at room temperature and are then annealed at 1200 C for at least 2 h before deformation. The total (plastic and elastic) strains (macroscopic) are derived from the direct measurements of the images taken by X-ray radiograph technique. The differential stresses are derived from the diffraction determined elastic strains. In the regime of 25-400 C, there is a small decrease of stress at steady state as temperature increases; in the regime of 400 C to the 'transition temperature', the differential stress at steady state ({approx}2.5 GPa) is relatively insensitive to the changes of temperature and strain rate; however, it drastically decreases to about 1 GPa and becomes temperature-dependent above the transition temperature and thereafter. The transition temperature is near 900 C. Above the transition temperature, the flow agrees with power law creep measurements of previous investigations. The anisotropy of differential stress in individual planes indicates that the deformation of olivine at low temperature is dominated by [0 0 1](1 0 0). Accounting to a slower strain rate in the natural system, the transition temperature for the olivine in the slab is most likely in the range of 570-660 C.

58 GEOSCIENCES↗

DOE OSTI2024

Steric and Electronic Influence of Excited-State Decay in Cu(I) MLCT Chromophores

For the past eleven years, a dedicated effort in our research group focused on fundamentally advancing the photophysical properties of cuprous bis-phenanthroline-based metal-to-ligand charge transfer (MLCT) excited states. We rationalized that by gaining control over the numerous factors limiting the more widespread use of Cu I MLCT photosensitizers, they would be readily adopted in numerous light-activated applications given the earth-abundance of copper and the extensive library of 1,10-phenanthrolines developed over the last century. Significant progress has been achieved by recognizing valuable structure-property concepts developed by other researchers in tandem with detailed ultrafast and conventional time-scale investigations, in-silico-inspired molecular designs to predict spectroscopic properties, and applying novel synthetic methodologies. Ultimately, we achieved a plateau in exerting cooperative steric influence to control Cu I MLCT excited state decay. This led to combining sterics with π-conjugation and/or inductive electronic effects to further exert control over molecular photophysical properties. The lessons gleaned from our studies of homoleptic complexes were recently extended to heteroleptic bis(phenanthrolines) featuring enhanced visible light absorption properties and long-lived room-temperature photoluminescence. Furthermore, this Account navigates the reader through our intellectual journey of decision-making, molecular and experimental design, and data interpretation in parallel with appropriate background information related to the quantitative characterization of molecular photophysics using Cu I MLCT chromophores as prototypical examples.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Green Emitting Single-Crystalline Bulk Assembly of Metal Halide Clusters with Near-Unity Photoluminescence Quantum Efficiency

Abstract not provided

Zhou, Chenkun↗

DOE OSTI2014

Stochastic formation of magnetic vortex structures in asymmetric disks triggered by chaotic dynamics

The non-trivial spin configuration in a magnetic vortex is a prototype for fundamental studies of nanoscale spin behaviour with potential applications in magnetic information technologies. Arrays of magnetic vortices interfacing with perpendicular thin films have recently been proposed as enabler for skyrmionic structures at room temperature, which has opened exciting perspectives on practical applications of skyrmions. An important milestone for achieving not only such skyrmion materials but also general applications of magnetic vortices is a reliable control of vortex structures. However, controlling magnetic processes is hampered by stochastic behaviour, which is associated with thermal fluctuations in general. Here we show that the dynamics in the initial stages of vortex formation on an ultrafast timescale plays a dominating role for the stochastic behaviour observed at steady state. Our results show that the intrinsic stochastic nature of vortex creation can be controlled by adjusting the interdisk distance in asymmetric disk arrays.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Ultranarrow bright single-photon emitters in diamond with strong broadband phonon decoupling

Single-photon emitters are fundamental building blocks for quantum information processing, communication and sensing. However, unwanted interactions with bulk phonons in their host environment strongly limit their coherence and controllability. We report single color centers in nanodiamonds that are strongly and comprehensively decoupled from the bulk phononic environment. The color centers feature record-narrow linewidths down to 0.3 nm at room temperature and stable, bright emission, exceeding 10 Mcps in saturation. Notably, the bulk phonon sideband is almost entirely suppressed, revealing the presence of a single localized vibrational mode outside the diamond phonon band. Our observations and simulations point towards a unique mechanism for phonon decoupling in common wide-gap materials, based on a strongly radiative orbital transition coupled to a localized vibrational mode. The new color center enables qualitatively higher performance for applications in quantum networks and nanoscale sensing, and the exploration of new physical resources associated with vibrational states.

Sahoo, Swetapadma [ORNL]↗

DOE OSTI2012

Magnetically active vacancy related defects in irradiated GaN layers

We present the studies of magnetic properties of 2 MeV {sup 4}He{sup +}-irraadiated GaN grown by metal-organic chemical-vapor deposition. Particle irradiation allowed controllable introduction of Ga-vacancy in the samples. The magnetic moments with concentrations changing between 4.3 and 8.3 Multiplication-Sign 10{sup 17}cm{sup -3} showing superparamagnetic blocking at room temperature are observed. The appearance of clear hysteresis curve at T=5K with coercive field of about H{sub C} Almost-Equal-To 270 Oe suggests that the formation of more complex Ga vacancy related defects is promoted with increasing Ga vacancy content. The small concentration of the observed magnetically active defects with respect to the total Ga-vacancy concentration suggests that the presence of the oxygen/hydrogen-related vacancy complexes is the source of the observed magnetic moments.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Electrochemically deposited BiTe-based nanowires for thermoelectric applications

Nanostructured materials systems such as thin-films and nanowires (NWs) are promising for thermoelectric power generation and refrigeration compared to traditional counterparts in bulk, due to their enhanced thermoelectric figures-of-merit. BiTe and its derivative compounds, in particular, are well-known for their near-room temperature thermoelectric performance. In this work, both the binary and ternary BiTe-based nanowires namely, BiTe and BiSbTe, were synthesized using template-assisted electrodeposition. Diameters of the nanowires were controlled by the pore sizes of the anodised alumina (AAO) templates used. Systematic study on the compositional change as a function of applied potential was carried out via Linear Sweep Voltanmetry (LSV). Chemical compositions of the nanowires were studied using Energy Dispersive X-ray Spectrometry (EDXS) and their microstructures evaluated using diffraction and imaging techniques. Results from chemical analysis on the nanowires indicated that while the Sb content in BiSbTe nanowires increased with more negative deposition potentials, the formation of Te{sup 0} and Bi{sub 2}Te{sub 3} were favorable at more positive potentials.

36 MATERIALS SCIENCE↗