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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

A Mechanistic Understanding of Nonclassical Crystal Growth in Hydrothermally Synthesized Sodium Yttrium Fluoride Nanowires

Sodium yttrium fluoride (NaYF 4 ) is an important upconverting material with many potential uses in chemistry, materials science, and biology, which can be synthesized hydrothermally in both cubic (α) and hexagonal (β) crystallographic polymorphs. Understanding the mechanisms underlying the phase conversion between the cubic and hexagonal polymorphs is of great interest to help inform future synthetic efforts, for example in the design of atomically precise quantum materials with well-defined sizes and morphologies. In this work, we use a combination of analytical transmission electron microscopy (TEM), scanning transmission electron microscopy (STEM), powder X-ray diffraction (XRD), in situ liquid cell TEM, atom probe tomography (APT), and extended X-ray absorption fine structure (EXAFS) measurements to show that the hexagonal NaYF 4 nanowires form through a nonclassical crystal growth mechanism involving the formation and subsequent oriented attachment of mesocrystals consisting of cubic (α) phase units. Additionally, EXAFS measurements suggest that substitutional Yb 3+ point defects within NaYF 4 are distributed evenly throughout the crystal lattice without clustering and also that they may exhibit selective substitution into one of the two possible trivalent yttrium sites in the unit cell for hydrothermally synthesized β-NaYF 4 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Laser Refrigeration of Ytterbium-Doped Sodium–Yttrium–Fluoride Nanowires

Sodium yttrium fluoride (ß-NaYF4) nanowires (NWs) with a hexagonal crystal structure are synthesized using a low-cost hydrothermal process and are shown to undergo laser refrigeration based on an upconversion process leading to anti-Stokes (blueshifted) photoluminescence. Single-beam laser trapping combined with forward light scattering is used to investigate cryophotonic laser refrigeration of individual NWs through analysis of their local Brownian dynamics.

Zhou, Xuezhe↗
DOE OSTI2022

Chemically Tunable Aspect Ratio Control and Laser Refrigeration of Hexagonal Sodium Yttrium Fluoride Upconverting Materials

Hexagonal sodium yttrium fluoride with Na 3x Y 2-x F 6 stoichiometry (β-NaYF) is a promising material for luminescence upconversion applications due to the narrow crystal field splitting of the Yb(III) ion’s lower 2 F 7/2 manifold. However, growing single crystals of β-NaYF remains an outstanding challenge due to thermal expansion stresses that cause cracking during melt growth. Here, we demonstrate a novel hydrothermal synthesis of β-NaYF with the ability to tune the aspect ratio from microplatelets to microrods with aspect ratios that match computationally predicted cavity (Mie) resonances. These crystals have a root-mean-square roughness below 1 nm after calcination, which makes them ideal for optical cavities. The β-NaYF microcrystals are doped with 10% Yb(III) cations and are used to build optomechanical laser-refrigeration devices consisting of a hexagonal β-NaYF crystal located at the end of a cantilever. Laser refrigeration of these devices by >12.5 °C is observed using calibrated measurements of both the cantilever’s fundamental eigenfrequency and a Boltzmann fit to crystal field luminescence from the Yb(III) ions.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Chemically Driven Multistep Crystallization in the Synthesis of Sodium Yttrium Fluoride Via a Porous, Electrochemically Active Intermediate

Two-step crystallization mechanisms based on liquid–liquid phase separations followed by crystallization are commonly observed both in the laboratory and in nature. While this pathway quite often occurs as a result of a chemical reaction, the subsequent nucleation and growth are often considered as separate, discrete events from the reaction itself. We show this mechanism in the aqueous synthesis sodium yttrium fluoride, but by using a combination of experimental techniques and computational modeling, we show an additional step of solid-state chemical diffusion that is essential to the nucleation mechanism. In this system, we observe at least four distinct steps in the crystallization process, including (1) the segregation of aqueous ions into a dense liquid phase, (2) the formation of a metastable amorphous aggregate, (3) the continuous, gradual solid-state diffusion of sodium and fluoride ions into the amorphous aggregate toward a NaYF4 stoichiometry, and (4) the crystallization of a stable cubic sodium yttrium fluoride phase. Unlike previous descriptions of nucleation and growth, we find that the stoichiometry of the final solid phase evolves throughout the crystallization process rather than being determined at the time of the initial separation from solution. Further, this emphasizes that the chemical reaction cannot be assumed to be a separate event from the phase separation and growth, especially in compounds with variable stoichiometry. We also find that the amorphous aggregate that forms prior to the ion incorporation step adopts a porous, gel-like structure, which we isolated and showed to be electrochemically active, allowing for its potential use as a battery anode in lithium and sodium ion batteries, among other potential applications.

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

Laser refrigeration of optically levitated sodium yttrium fluoride nanocrystals

Solid state laser refrigeration can cool optically levitated nanocrystals in an optical dipole trap, allowing for internal temperature control by mitigating photothermal heating. This work demonstrates cooling of ytterbium-doped cubic sodium yttrium fluoride nanocrystals to 252 K on average with the most effective crystal cooling to 241 K. The amount of cooling increases linearly with the intensity of the cooling laser and is dependent on the pressure of the gas surrounding the nanocrystal. Furthermore, cooling optically levitated nanocrystals allows for crystals prone to heating to be studied at lower pressures than currently achievable and for temperature control and stabilization of trapped nanocrystals

36 MATERIALS SCIENCE↗
NASA NTRS1987

Efficient holmium:yttrium lithium fluoride laser longitudinally pumped by a semiconductor laser array

Optical pumping of a holmium:yttrium lithium floride (Ho:YLF) crystal with a 790-nm continuous-wave diode-laser array has generated 56 mW of 2.1-micron laser radiation with an optical-to-optical conversion slope efficiency of 33 percent while the crystal temperature is held at 77 K. The lasing threshold occurs at 7 mW of input power, and laser operation continues up to a crystal temperature of 124 K.

Hemmati, H.↗
DOE OSTI2016

Controllable synthesis and tunable luminescence of glass ceramic containing Mn{sup 2+}:ZnAl{sub 2}O{sub 4} and Pr{sup 3+}:YF{sub 3} nano-crystals

Highlights: • Glass ceramic containing ZnAl{sub 2}O{sub 4} and YF{sub 3} nano-crystals is fabricated. • Mn{sup 2+} and Pr{sup 3+} are selectively incorporated into ZnAl{sub 2}O{sub 4} and YF{sub 3}, respectively. • The luminescence color can be tuned by adjusting the excitation wavelength. - Abstract: Glass ceramic containing spinel ZnAl{sub 2}O{sub 4}:Mn{sup 2+} and orthorhombic YF{sub 3}:Pr{sup 3+} nano-crystals has been successfully prepared by a melt-quenching technique. X-ray diffraction and transmission electron microscopy demonstrated that two nano-phases, i.e. ZnAl{sub 2}O{sub 4} and YF{sub 3}, were homogeneously distributed among the glass matrix. Importantly, the selective incorporation of Pr{sup 3+} ions into the Y{sup 3+} nine-fold coordinated sites of YF{sub 3} and the segregation of Mn{sup 2+} dopants in the Zn{sup 2+} tetrahedral sites of ZnAl{sub 2}O{sub 4} were confirmed based on the excitation/emission spectra and the crystal field calculation. Under blue light excitation, both Pr{sup 3+} and Mn{sup 2+} in the glass ceramic can be simultaneously excited, and emit red and green luminescence, respectively, owing to the suppression of energy transfer between them. The luminescence color of the obtained glass ceramic can be easily tuned by adjusting the excitation wavelength. These results indicate the potential application of the glass ceramic as converting phosphor to generate white-light after coupling with the blue LED chip.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Mediation of Colloidal Encounter Dynamics by Surface Roughness

Rigorous understanding on the self-assembly of colloidal nanocrystals is crucial to develop tailored nanostructured materials for energy storage, sensing, and optical fields. Despite extensive studies on the self-assembly, a mechanistic understanding of self-assembly under an external field still remains an ongoing challenge. Here, in this work, we used optical tweezers that impose an external attractive force field, resulting in the self-assembly of alpha-phase sodium yttrium fluoride nanocrystals. The dynamic force that is strongly dependent on the surface roughness of the nanocrystals is shown to be a decisive factor for a direct contact between the nanocrystals, manifested by the roughness-dependent hydrodynamic resistivity and Langevin dynamic simulations. Our study provides direct evidence that the role of dynamics is equally important in understanding the self-assembly, which has been rarely observed in the self-assembly in contrast with many studies on the equilibrium forces. These results may have further impact in other fields, such as having explanatory power for the probability of nonclassical crystal growth or the structure of viral spike proteins that affect the probability of viruses binding with cells.

Felsted, Robert G. [Univ. of Washington, Seattle, ↗
DOE OSTI2014

Multifunctional gold coated rare-earth hydroxide fluoride nanotubes for simultaneous wastewater purification and quantitative pollutant determination

Highlights: • The morphology and properties of Ce-doped yttrium hydroxide fluoride nanotubes (YHF:Ce NTs) were investigated. • YHF:Ce NTs were conjugated with Au nanoparticles to produce Au-YHF:Ce nanocomposites. • Au-YHF:Ce NTs showed excellent capability and efficiency in removing Congo red from solutions. • Au-YHF:Ce NTs were utilized to determine the concentration of Congo red based on SERS. - Abstract: Ce-doped yttrium hydroxide fluoride nanotubes (YHF:Ce NTs) with large surface area are synthesized and conjugated with Au nanoparticles (NPs) to produce Au-YHF:Ce nanocomposites. The Au-YHF:Ce NTs have a hollow structure, rough surface, polymer coating, and good surface-enhanced Raman spectroscopy (SERS) properties. They are applied to wastewater treatment to remove Congo red as a typical pollutant. The materials not only remove pollutants rapidly from the wastewater, but also detect trace amounts of the pollutants quantitatively. The multifunctional Au-YHF:Ce NTs have commercial potential as nano-absorbents and nano-detectors in water treatment and environmental monitoring.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Fast synthesis of sub-10 nm β-NaYF4:Yb3+, Er3+@NaYF4 core-shell upconversion nanocrystals mediated by oleate ligands

Highlights: • Fast synthesize ultra-small β-NaYF{sub 4}:Yb{sup 3+}, Er{sup 3+} UCNCs with 0 min reaction or down to 5.3 nm. • Highly bright sub-10 nm β-NaYF{sub 4}:Yb{sup 3+}, Er{sup 3+} core-shell NCs were obtained. • OA{sup −} ligands cannot only promote the α-to-β phase transition, but also inhibit the crystal growth. • OA{sup −} ligands manipulated phase transition and size evaluation is also applicable to other UCNCs. - Abstract: We developed a facile approach for the fast synthesis of ultrasmall and monodisperse β-NaYF{sub 4}:Yb{sup 3+}, Er{sup 3+} nanocrystals down to 5.3 nm with the assistant of oleate ligands, based on which the highly bright sub-10 nm β-NaYF{sub 4}:Yb{sup 3+}, Er{sup 3+}@NaYF{sub 4} core-shell nanocrystals with three order of magnitude increased upconversion emission were successfully obtained by a seed-mediated growth method. The reaction time and temperature dependent experimental results implied that the introduciton of extra oleate ligands can both promote the α-to-β phase transition and impeded the crystal growth of NaYF{sub 4}, which is due to the oleate ligand induced orderly arrangement of Y{sup 3+} and capping effect, respectively. It is expected that the oleate ligands mediated phase transition and size evaluation, demonstrated here in NaYF{sub 4}:Yb{sup 3+}, Er{sup 3+} NCs, is also applicable to other lanthanide-doped upconversion nanocrystals.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2015

Nanostructured crystals of fluorite phases Sr{sub 1−x}R{sub x}F{sub 2+x} (R Are Rare Earth Elements) and their ordering: 10. Ordering under spontaneous crystallization and annealing of Sr{sub 1−x}R{sub x}F{sub 2+x} Alloys (R = Tb-Lu, Y) with 23.8–36.1 mol % RF{sub 3}

The products of spontaneous crystallization (at a cooling rate of ∼200 K/min) of Sr{sub 1−x}R{sub x}F{sub 2+x} melts in the homogeneity range of the fluorite phase have been investigated. Thirty-two irrational compositions with 23.8–36.1 mol % RF{sub 3} and eight rational Sr{sub 2}RF{sub 7} compositions are obtained. With respect to the RF{sub 3} content, these compositions form five groups: (1) Sr{sub 0.762}R{sub 0.238}F{sub 2.238} (23.8% RF{sub 3}), (2) Sr{sub 0.744}R{sub 0.256}F{sub 2.256} (25.6%), (3) Sr{sub 0.718}R{sub 0.282}F{sub 2.282} (28.2%), (4) Sr{sub 2}RF{sub 7} (33.3%), and (5) Sr{sub 0.639}R{sub 0.361}F{sub 2.361} (36.1%). R = Tb-Lu, Y for all groups. Quenching melts of group 5 with R = Tb, Dy, and Ho leads to the formation of ordered phases with the trigonal distortion of the rhβ-Na{sub 7}Zr{sub 6}F{sub 31} type, while for melts of group 5 with R = Lu, quenching yields a phase of the trigonal rhα′-Sr{sub 4}Lu{sub 3}F{sub 17} type. In group 5 with R = Y, Er, Tm, or Yb and in groups 1–4 with all REEs, fluorite phases are formed. Annealing at 900 ± 20°C for 96 h with subsequent cooling at a rate of ∼200 K/min expands the variety of ordered phases: a phase with a new r type of orthorhombic distortion is formed in group 1 with R = Lu, in group 2 with R = Tm or Lu, and in group 3 with R = Ho-Lu, Y; a t-Sr{sub 2}RF{sub 7} phase with tetragonal distortion is formed in group 4 with R = Tb-Er, Y; and a phase of trigonal rhα′ type is formed in group 5 with R = Y, Yb, or Lu. A fluorite phase arises in group 1 with R = Tb-Lu, Y as a result of quenching and annealing. The tendency to ordering becomes more pronounced with an increase in the RF{sub 3} content and REE atomic number. The annealing conditions do not provide equilibrium or the completely ordered state of all alloys.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Ionic conductivity of binary fluorides of potassium and rare earth elements

The ionic conductivity s of KYF{sub 4} and K{sub 2}RF{sub 5} single crystals (R = Gd, Ho, Er) and KNdF{sub 4} and K{sub 2}RF{sub 5} ceramic samples (R = Dy, Er) has been studied in the temperature range of 340–500°C. A comparative analysis of the σ values for these objects has been performed. Binary fluorides of potassium and rare earth elements were synthesized by the hydrothermal method (temperature 480°C, pressure 100–150 MPa) in the R{sub 2}O{sub 3}–KF–H{sub 2}O systems. The σ values of tetraf luorides are 3 × 10{sup –5} S/cm (KYF{sub 4} single crystal) and 3 × 10{sup –6} S/cm (KNdF{sub 4} ceramics) at 435°C. A K{sub 2}ErF{sub 5} single crystal with σ = 1.2 × 10{sup –4} S/cm at 435°C has the maximum value of ionic conductivity among pentafluorides. The anisotropy of ionic transport was found in K{sub 2}HoF{sub 5} single crystals, σ{sub ∥c}/σ{sub ⊥c} = 2.5, where σ{sub ∥c} and σ{sub ⊥c} are, respectively, the conductivities along the crystallographic c axis and in the perpendicular direction.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Planar fluoride waveguides for amplifiers and lasers

We have produced planar optical waveguides having a crystalline CaF{sub 2} – YF{sub 3} – NdF{sub 3} mixed yttrofluorite core and two reflective claddings in order to improve waveguide excitation efficiency. Under diode pumping, lasing has been achieved at a wavelength of 1064 nm with a slope efficiency near 15%. (lasers)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Correlation between the Molecular Refractions of Crystals and the Ionic Radii of the Cations in the Rare-Earth Trifluoride Homologous Series

We have identified linear correlations between the molecular refractions R{sub mol} (cm{sup 3}/mol) of crystals and the ionic radii r{sub i} (Å) of the cations in the RF{sub 3} rare-earth trifluoride homologous series: R{sub mol} = 8.33r{sub i} + 0.102 for R = La–Nd and R{sub mol} = 13.03r{sub i}–4.42 for R = Sm–Lu. The fact that the RF{sub 3} rare-earth trifluorides can be divided into two groups is related to the morphotropic transition from the LaF{sub 3} (tysonite) structure to the β-YF{sub 3} structure. The correlation found here for RF{sub 3} crystals with the β-YF{sub 3} structure because the electronic structure of Y (4d{sup 1}5s{sup 2}) differs from that of Sm–Lu (4f{sup 6–14}5d{sup 0–1}6s{sup 2}) in that it has no 4f electrons.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Laser performance of in-band pumped Er : LiYF{sub 4} and Er : LiLuF{sub 4} crystals

Spectroscopic properties of Er : LiLuF{sub 4} and Er : LiYF{sub 4} crystals in the spectral region near 1.5 μm and the lasing characteristics of these crystals under in-band pumping at a wavelength of 1522 nm are studied. With the Er : LiLuF{sub 4} crystal, the maximum slope efficiency with respect to the absorbed pump power was 44% at a wavelength of 1609 nm. Continuous-wave operation of an inband pumped Er : LiYF{sub 4} laser is obtained for the first time. The output power at a wavelength of 1606 nm was 58 mW with a slope efficiency of 21%. (lasers)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗