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At least 703 records · Page 39
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

Preparation and optical characteristics of layered perovskite-type lead-bromide-incorporated azobenzene chromophores

Lead bromide-based layered perovskite powders with azobenzene derivatives were prepared by a homogeneous precipitation method. From the diffuse reflectance (DR) and photoluminescence (PL) spectra of the hybrid powder materials, the present hybrids exhibited sharp absorption and PL peaks originating from excitons produced in the PbBr{sub 4}{sup 2-} layer. When the present hybrid powder was irradiated with UV light at 350 nm, the absorption band from the trans-azobenzene chromophore, observed around 350 nm, decreased, while the absorption band from the cis-azobenzene chromophore, observed around 450 nm, increased. These results indicate that azobenzene chromophores in the present hybrid materials exhibit reversible photoisomerization. Moreover, it was found that the PL intensity from the exciton also varied due to photoisomerization of the azobenzene chromophores in the present hybrid. Thus, for the first time we succeeded in preparing the azobenzene derivative lead-bromide-based layered perovskite with photochromism before and after UV light irradiation. - Graphical abstract: For the first time, we succeeded in preparing the azobenzene derivative lead-bromide-based layered perovskite with photochromism before and after UV light irradiation. Highlights: Black-Right-Pointing-Pointer PbBr-based layered perovskite with azobenezene derivatives could be synthesized by a homogeneous precipitation method. Black-Right-Pointing-Pointer Azobenzene derivatives incorporated the present hybrid that exhibited reversible photoisomerization under UV and/or visible light irradiation. Black-Right-Pointing-Pointer PL property of the present hybrid could also be varied by photoisomerization.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Transformations of lead 1,3-propylenediaminetetraacetate to its MOF products for the selective adsorption of methanol

Water soluble coordination polymer of potassium lead 1,3-propylenediaminetetraacetate {K_4[Pb_2(1,3-pdta)_2]·6H_2O}{sub n} (1) and its insoluble products {[Pb(1,3-H_2pdta)(H_2O)]·2H_2O}{sub n} (2), {[Pb_2(1,3-pdta)(H_2O)_4]·4H_2O}{sub n} (3) and [Pb{sub 2}(1,3-pdta)(H{sub 2}O){sub 2}]{sub n} (4) were obtained from the direct reactions of lead nitrate with 1,3-propylenediaminetetraacetic acid in different conditions (1,3-H{sub 4}pdta=1,3-propylenediaminetetraacetic acid). The former 1 could be converted to the insoluble products of {[Pb_2(1,3-pdta)(H_2O)_4]·4H_2O}{sub n} (3) and [Pb{sub 2}(1,3-pdta)(H{sub 2}O){sub 2}]{sub n} (4) in weak acidic solution. The complexes have been full characterized by EA, FT-IR, solution and solid state {sup 13}C NMR spectra, thermogravimetric and structural analyses. Interestingly, 3 contains a unique (H{sub 2}O){sub 26} cluster and a 5.2 Å pore after eliminating the guest water molecules, which exhibits reversible adsorption for methanol. This is confirmed by PXRD and solid state {sup 13}C NMR analyses. Nano-confined methanol in microporous structure has been observed based on the large downfield shift of {sup 13}C NMR signal (Δδ 9.72 ppm), attributing to the methyl group in methanol. - Graphical abstract: Water soluble coordination polymer K{sub 4n}[Pb{sub 2}(1,3-pdta){sub 2}]{sub n}·6nH{sub 2}O (1) is converted to its insoluble product [Pb{sub 2}(1,3-pdta)(H{sub 2}O){sub 4}]{sub n}·4nH{sub 2}O (3), which contains a unique (H{sub 2}O){sub 26} cluster and exhibits reversible adsorption for methanol. - Highlights: • Water-soluble coordination polymer was constructed by lead propylenediaminetetraacetate. • Its MOF product has a unique (H{sub 2}O){sub 26} cluster. • The product exhibits reversible adsorption for methanol.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2012

Rapid sonochemical preparation of shape-selective lead iodide

Graphical abstract: SEM morphologies of various PbI2 products obtained with the iodine concentration of 6.7 g/L and irradiation time of 1 minute at the reaction temperatures of 35 °C (a), 25 °C (b), and 15 °C (c). Highlights: ► PbI{sub 2} with various morphologies were rapidly formed at room temperature. ► We could well control the morphologies of PbI{sub 2} by changing reaction conditions. ► The PbI{sub 2} films could better resist rolling in a liquid media. -- Abstract: Lead iodide (PbI{sub 2}) films/crystals with various nano/micro morphologies (e.g., Nanoflake, block and microrod) were rapidly synthesized by taking advantage of a simple sonochemical method. The PbI{sub 2} crystals with uniform nanoflake structures could be fabricated directly on lead foils with the irradiation time as short as 36 s via interfacial reaction between lead foils and elemental iodine in ethanol at ambient temperature. It was found experimentally that the morphologies of the resulting thin films/crystals could be well controlled by the adjustment of several parameters including irradiation time, reaction solvents, iodine concentration, ultrasonic power, and reaction temperature. Most importantly, the resultant PbI{sub 2} films are stable enough to resist rolling under the drastic ultrasound irradiation in a liquid media. This method is believed to be the fastest way for in situ fabrication of morphology-controlled semiconductor films on various metal substrates for subsequent applications related to the other metal iodide or metal sulfide semiconductor films.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Probing lead acetate in solution using X-ray diffraction

Here, for the purpose of water purification involving toxic metal sensing and removal, high energy X-ray diffraction experiments have been performed on lead acetate Pb(Ac) 2 solutions, liquid and amorphous glutathione disulfide (GSSG), and their mixtures. The data have been interpreted using Empirical Potential Structure Refinement and pair distribution function analysis. At the highest concentration of 1 M Pb(Ac) 2 in water, the lead molecules are found to cluster and the second shell in the water structure becomes slightly more ordered as the water molecules become compressed. Liquid and amorphous GSSG are found to hydrogen bond primarily via OH-O interactions, while NH-O bonds are much more distorted. Aqueous solutions of Pb(Ac) 2 + GSSG show the closest Pb-O (carboxyl) and Pb-N (amine) bonds both at a distance of 2.5 ± 0.1 Å at a concentration of 1 M Pb(Ac) 2 in water. At 0.75 M Pb(Ac) 2 in water, strong Pb-S bonds are found at a distance of 2.8 ± 0.1 Å. The implications for lead removal using capacitive deionization are discussed.

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

Miniature DC electromagnetic pumps of molten lead and sodium to support development of Gen-IV nuclear reactors

This work developed designs of submerged, dual-regions, miniature DC-EM pumps for circulating molten lead and liquid sodium at ≤500 °C without active cooling for use in ex-pile and in-pile test loops to support of materials and fuel developments for Gen-IV sodium and molten lead fast nuclear reactor. These pumps with two pumping regions are 57 mm, 66.8 mm, 95.4 mm, and 133.5 mm in diameter and have two Alnico 5 permanent magnets with Hiperco-50 pole pieces for focusing the magnetic field lines in the flow duct. The Equivalent Circuit Model (ECM) linked to the Finite Element Method Magnetics (FEMM) software in MATLAB platform calculated the pumps characteristics for a wide range of parameters. Also determined are the pumps dimensions for the highest cumulative pumping power and peak efficiency. These dimensions are the height, width, and length of the flow duct, the thickness of the Alnico magnets, the length of current electrodes, and the separation distance between the two pumping regions. For molten lead, the pumping power increases from 368 W to 728 W, and the peak efficiency from 14.7% to 31.6% with increased pump diameter from 57 mm to 133.5 mm. In conclusion, for liquid sodium, both the pumping power and peak efficiency are higher, increasing from 392 W to 767 W and from 44.3 to 51.2%, respectively, with increased pump diameter from 57 mm to 133.5 mm.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2020

Thermodynamics of cesium lead halide (CsPbX 3 , x= I, Br, Cl) perovskites

Inorganic cesium lead halide (CsPbX 3 , X = I, Br, Cl) perovskites have sparked broad interest for photovoltaic applications, which, however, may be plagued by chemical and thermodynamic instabilities. This work reports calorimetric studies on the formation enthalpies of CsPbX 3 perovskites, confirming decreasing thermodynamic stability in the order CsPbCl 3 , CsPbBr 3 and CsPbI 3 . Cesium lead iodide (CsPbI 3 ), one of the most studied inorganic lead halide perovskites, is shown to be only barely stable from a thermodynamic perspective. This order of increasing instability is consistent with the variation of Goldschmidt tolerance factor. The perovskites are high temperature entropy-stabilized phases with respect to low temperature polymorphs, with the thermodynamics of phase transitions reflecting the above thermodynamic trends.

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

P-Type Doping of Mixed Tin–Lead Halide Perovskites Using Electron Transfer to Mo(tfd-COCF3) 3 and F 4 TCNQ

Mixed tin-lead halide perovskites are emerging as promising candidates to address the toxicity issues of lead-based perovskites and to provide additional bandgap tunability for optoelectronic applications. Electron-transfer doping offers a prospective pathway to modulate electronic properties of metal-halide perovskites, while not disturbing the underlying crystal structure. However, limited research exists comparing molecular dopants for these systems. Here, our study investigates the p-type electron-transfer doping of the mixed tin-lead halide perovskite MAPb 0.5 Sn 0.5 I 3 (MA = methylammonium) using a sequential deposition approach (perovskite film followed by dopant incorporation) and the molecular dopants F 4 TCNQ and Mo(tfd-COCF 3 ) 3 . Up to 3 orders of magnitude higher carrier density and up to 2 orders of magnitude greater conductivity are achieved relative to the undoped samples, with F 4 TCNQ and Mo(tfd-COCF 3 ) 3 demonstrating similar doping efficiencies (associated with the ratio of mobile charges added to the number of dopant molecules incorporated) of 0.031(3) % and 0.024(3) %, respectively. Differences in the doping effectiveness for a given molarity doping solution likely follow from variations in dopant incorporation within the film during the spin coating deposition step.

14 SOLAR ENERGY↗
DOE OSTI2020

Lead-Free Cs 4 CuSb 2 Cl 12 Layered Double Perovskite Nanocrystals

Concerns about the toxicity of lead-based perovskites have aroused great interest for the development of alternative lead-free perovskite-type materials. Recently, theoretical calculations predict that Pb 2+ cations can be substituted by a combination of Cu 2+ and Sb 3+ cations to form a vacancy-ordered layered double perovskite structure with superior optoelectronic properties. However, accessibilities to this class of perovskite-type materials remain inadequate, hindering their practical implementations in various applications. Here, we report the first colloidal synthesis of Cs 4 CuSb 2 Cl 12 perovskite-type nanocrystals (NCs). The resulting NCs exhibit a layered double perovskite structure with ordered vacancies and a direct bandgap of 1.79 eV. A composition-structure-property relationship has been established by investigating a series of Cs 4 Cu x Ag 2-2x Sb 2 Cl 12 perovskite-type NCs (0 ≤ x ≤ 1). The composition-induced crystal structure transformation, thus the electronic bandgap evolution has been explored by experimental observations and further confirmed by theoretical calculations. Taking advantages of both the unique electronic structure and solution processability, we demonstrate that the Cs 4 CuSb 2 Cl 12 NCs can be solution-processed as high-speed photodetectors with ultrafast photo-response and narrow bandwidth. We anticipate that our study will prompt future research to design and fabricate novel and high-performance lead-free perovskite-type NCs for a range of applications.

25 ENERGY STORAGE↗
DOE OSTI2011

Mechanisms of laser induced modification of lead and barium vanadate glasses

We report on our investigations on the mechanisms for structural and morphological change in lead and barium vanadate glasses modified by 785 nm laser irradiation. The fundamental process is thermal in nature, leading to phase decomposition, phase changes, and mass transport in the center of the irradiated region, as well as the formation of lead-or barium-rich debris zones. Crystallization is also a consequence of the exposure to the laser light. We further report on preirradiation experiments in which low-power exposure above a determined energy threshold results in structural changes that bridge the gap between the amorphous state and the ultimate crystalline arrangement. Finally, we discuss the application of the laser irradiation in the making of vanadate microspheres.

36 MATERIALS SCIENCE↗
DOE OSTI2011

Effects of porosity on dielectric and piezoelectric properties of porous lead zirconate titanate ceramics

We report porous lead zirconate titanate ceramics fabricated by tert-butyl alcohol-based gel-casting process which show a very high thickness electromechanical coupling coefficient (0.77), high hydrostatic figure of merit (9594x10{sup -15} m{sup 2}/N), and low acoustic impedance (3.7 Mrayls). We show that the porosity effectively affects the performance of the samples in two ways: (1) a higher porosity simplifies the resonance behavior, leading to more efficient energy transduction; (2) its replacement of active ceramic phase leads to low relative permittivity, high hydrostatic figure of merit, and low acoustic impedance. It was confirmed the properties could be tailored by controlling the porosity.

36 MATERIALS SCIENCE↗
DOE OSTI2012

Incorporation of lead and titanium into a porous alumina membrane during Pb(Zr{sub 0.52}Ti{sub 0.48})O{sub 3} nanotube synthesis

We report the identification and characteristics of lead aluminate (Pb{sub 2}Al{sub 2}O{sub 5} or PbAl{sub 12}O{sub 19})/aluminum titanate (Al{sub 2}TiO{sub 5}) formed as a result of the interaction between a Pb(Zr{sub 0.52}Ti{sub 0.48})O{sub 3} (PZT) precursor and a porous alumina membrane (PAM) during PZT nanotube synthesis. The surface morphology and composition of PZT nanotubes were examined as a function of the etching time and annealing temperature, and the diffusion of elements over nanometer length scales during PZT nanotube formation was investigated based on analysis using field emission transmission electron microscopy, scanning transmission electron microscopy, and energy dispersive x-ray microscopy. As the annealing temperature increased, the volume of lead aluminate/aluminum titanate increased, suggesting that considerable diffusion of Pb and Ti occurred and, in turn, dramatically affected the nanotube characteristics. The diffusion of Pb and Ti was clearly evident, resulting in the formation of a distinct lead aluminate/aluminum titanate at the PZT nanotube/PAM interface.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2014

Vibrational lifetimes of hydrogen on lead films: An ab initio molecular dynamics with electronic friction (AIMDEF) study

Using density functional theory and Ab Initio Molecular Dynamics with Electronic Friction (AIMDEF), we study the adsorption and dissipative vibrational dynamics of hydrogen atoms chemisorbed on free-standing lead films of increasing thickness. Lead films are known for their oscillatory behaviour of certain properties with increasing thickness, e.g., energy and electron spillout change in discontinuous manner, due to quantum size effects [G. Materzanini, P. Saalfrank, and P. J. D. Lindan, Phys. Rev. B 63, 235405 (2001)]. Here, we demonstrate that oscillatory features arise also for hydrogen when chemisorbed on lead films. Besides stationary properties of the adsorbate, we concentrate on finite vibrational lifetimes of H-surface vibrations. As shown by AIMDEF, the damping via vibration-electron hole pair coupling dominates clearly over the vibration-phonon channel, in particular for high-frequency modes. Vibrational relaxation times are a characteristic function of layer thickness due to the oscillating behaviour of the embedding surface electronic density. Implications derived from AIMDEF for frictional many-atom dynamics, and physisorbed species will also be given.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Lead-silicate glass optical microbubble resonator

Microbubble whispering gallery resonators have the potential to become key components in a variety of active and passive photonic circuit devices by offering a range of significant functionalities. Here, we report on the fabrication, optical characterization, and theoretical analysis of lead-silicate glass and optical microbubble resonators. Evanescent field coupling to the microbubbles was achieved using a 1 μm diameter, silica microfiber at a wavelength of circa 775 nm. High Q-factor modes were efficiently excited in both single-stem and two-stem, lead-silicate glass, and microbubble resonators, with bubble diameters of 38 μm (single-stem) and 48 μm (two-stem). Whispering gallery mode resonances with Q-factors as high as 2.3 × 10{sup 5} (single-stem) and 7 × 10{sup 6} (two-stem) were observed. By exploiting the high-nonlinearity of the lead-silicate glass, this work will act as a catalyst for studying a range of nonlinear optical effects in microbubbles, such as Raman scattering and four-wave mixing, at low optical powers.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Enhanced torsional actuation and stress coupling in Mn-modified 0.93(Na 0.5 Bi 0.5 TiO 3 )-0.07BaTiO 3 lead-free piezoceramic system

This paper is concerned with the development of a piezoelectric d 15 shear-induced torsion actuator made of a lead-free piezoceramic material exhibiting giant piezoelectric shear stress coefficient (e 15 ) and piezoelectric transverse shear actuation force comparable to that of leadbased shear-mode piezoceramics. The Mn-modified 0.93(Na 0.5 Bi 0.5 TiO 3 )-0.07BaTiO 3 (NBT-BTMn) composition exhibited excellent properties as a torsional transducer with piezoelectric shear stress coefficient on the order of 11.6 C m –2 . The torsional transducer, consisting of two oppositely polarized NBT-BT-Mn d 15 mode piezoceramic shear patches, provided a rate of twist of 0.08 mm m –1 V –1 under quasi-static 150 V drive. The high value of piezoelectric shear d 15 coefficient in NBT-BT-Mn sample further demonstrated its potential in practical applications. Lastly, these results confirm that the lead-free piezoceramics can be as effective as their lead-based counterparts.

36 MATERIALS SCIENCE↗
DOE OSTI2011

Fission and quasifission modes in heavy-ion-induced reactions leading to the formation of Hs{sup *}

Mass and energy distributions of binary reaction products obtained in the reactions {sup 22}Ne+{sup 249}Cf,{sup 26}Mg+{sup 248}Cm, {sup 36}S+{sup 238}U, and {sup 58}Fe+{sup 208}Pb have been measured. All reactions lead to Hs isotopes. At energies below the Coulomb barrier the bimodal fission of Hs{sup *}, formed in the reaction {sup 26}Mg+{sup 248}Cm, is observed. In the reaction {sup 36}S+{sup 238}U, leading to the formation of a similar compound nucleus, the main part of the symmetric fragments arises from the quasifission process. At energies above the Coulomb barrier fusion-fission is the main process leading to the formation of symmetric fragments for both reactions with Mg and S ions. In the case of the {sup 58}Fe+{sup 208}Pb reaction the quasifission process dominates at all measured energies.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2012

Lead (II) selenite halides Pb{sub 3}(SeO{sub 3}){sub 2}X{sub 2} (X = Br, I): Synthesis and crystal structure

Two lead selenite halides, Pb{sub 3}(SeO{sub 3}){sub 2}Br{sub 2} and Pb{sub 3}(SeO{sub 3}){sub 2}I{sub 2}, have been prepared by solid-phase synthesis and structurally characterized. These compounds are isotypic and can be considered 3D with a microporous framework composed of lead polyhedra (distorted Archimedean antiprisms formed by oxygen and halogen atoms). The framework contains channels oriented in the [010] direction. These channels contain selenium atoms, which are bound with framework oxygen atoms belonging to different lead polyhedra.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2011

Critical magnetic field of surface superconductivity in lead

The critical superconductivity field H{sub c3} is measured on lead single crystals. It is shown that the temperature dependence of H{sub c3}/H{sub c} in the vicinity of superconducting transition temperature T{sub c} is essentially nonlinear. Relative changes in the value of H{sub c3}/H{sub c} reach approximately 30%, which cannot be described by the Ginzburg-Landau theory. The experimental temperature dependences lead to the conclusion that the surface superconducting transition temperature noticeably exceeds the superconducting transition temperature in the bulk of the semiconductor. The differences in the critical temperatures and in the Ginzburg-Landau parameters for lead are estimated.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

The Formation of Hollow Lead Structures on the Surface of PbSe Films Treated in Argon Plasma

Conditions for ion sputtering of a PbSe/CaF{sub 2}/Si(111) epitaxial system in high-density inductively coupled plasma of high-frequency low-pressure discharge in argon have been established that ensure the formation of submicron-sized hollow lead structures on a lead-selenide surface. The surface was plasma-treated for time periods within 60–240 s at low energy (20–30 eV) of Ar{sup +} ions, which is close to their sputtering threshold energy. The properties of the obtained material were studied by the techniques of scanning electron microscopy and energy-dispersive X-ray microanalysis. It is shown that the characteristic size, shape, and density of surface structures can be varied within broad limits depending on the time of plasma treatment and temperature of the material surface. Physical processes responsible for the formation of hollow lead structures under the proposed conditions of plasma sputtering are considered.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗