Formation of SiGe nanocrystals embedded in Al2O3 for the application of write-once-read-many-times memory

NASA Astrophysics Data System (ADS)

Wu, Min-Lin; Wu, Yung-Hsien; Lin, Chia-Chun; Chen, Lun-Lun

2012-10-01

The structure of SiGe nanocrystals embedded in Al2O3 formed by sequential deposition of Al2O3/Si/Ge/Al2O3 and a subsequent annealing was confirmed by transmission electron microscopy and energy dispersive spectroscopy (EDS), and its application for write-once-read-many-times (WORM) memory devices was explored in this study. By applying a -10 V pulse for 1 s, a large amount of holes injected from Si substrate are stored in the nanocrystals and consequently, the current at +1.5 V increases by a factor of 104 as compared to that of the initial state. Even with a smaller -5 V pulse for 1 μs, a sufficiently large current ratio of 36 can still be obtained, verifying the low power operation. Since holes are stored in nanocrystals which are isolated from Si substrate by Al2O3 with good integrity and correspond to a large valence band offset with respect to Al2O3, desirable read endurance up to 105 cycles and excellent retention over 100 yr are achieved. Combining these promising characteristics, WORM memory devices are appropriate for high-performance archival storage applications.

Primordial Terrestrial Xe from the Viewpoint of CFF-Xe

NASA Astrophysics Data System (ADS)

Meshik, A. P.; Shukolyukov, Yu. A.; Jessberger, E. K.

1995-09-01

We have already reported [7, 23] on the non-linear isotope mass-fractionation of fission Xe by migration of the precursors I, Te, Sn, and Sb and simultaneous fission of heavy nuclei. Xe with anomalous isotopic pattern was found in a number of meteorites and terrestrial materials and was named CFF-Xe (Chemically Fractionated Fission Xe). It is characterized by an up eightfold ^132Xe and ^131Xe excesses coupled with smaller ^134Xe and ^129Xe excesses. The present work is aimed to estimate the role of CFF-Xe in the terrestrial lithosphere and specifically deals with the problem of the isotopic composition of primordial terrestrial Xe. Due to variations of the migration conditions the isotopic structure of CFF-Xe is not well established and is even not reproducible in the same rock [2]. Nevertheless, we have tried to estimate the composition of CFF-Xe by investigating all available isotopic data of Xe of presumable mantle origin. This is Xe in MORB [29, 1, 12] and ocean island glasses [1, 28], in diamonds [17], in volcanic rocks [29, 8, 9, 21], in volcanic glasses from pillow basalts [16, 6], continental igneous rocks [1, 24, 10, 22], carbonatites and granitoids [1] as well as Xe in natural gases [3, 24, 11, 4, 15]. All data are plotted Fig. 1 where we also suggest end members of the observed scattering. Optimized slopes of CFF-lines are shown as well as the position of the initial points which we regard as primordial terrestrial Xe (Xe0). The isotopic composition of CFF-Xe and Xe0 are given in Tab. 1. The abundances of ^124Xe and ^126Xe in mantle derived samples are very uncertain, but since ^128Xe/^130Xe in Xea and Xe0 is very similar we propose the same ^124Xe/^130Xe and ^126Xe/^130Xe ratios for both Xea and Xe0. If so, AVCC-Xe is simply Xe0 with an admixture of L-Xe, and atmospheric xenon Xea consists of Xe0, CFF-Xe and a small amount of fission Xe (92.5%Xe0 + 5.3%CFF-Xe + 2.2%XeF). Thus, a number of old problems in xenology are removed. The hypothetic components U-Xe

Nanocomposite Phosphor Consisting of CaI2:Eu2+ Single Nanocrystals Embedded in Crystalline SiO2.

PubMed

Daicho, Hisayoshi; Iwasaki, Takeshi; Shinomiya, Yu; Nakano, Akitoshi; Sawa, Hiroshi; Yamada, Wataru; Matsuishi, Satoru; Hosono, Hideo

2017-11-29

High luminescence efficiency is obtained in halide- and chalcogenide-based phosphors, but they are impractical because of their poor chemical durability. Here we report a halide-based nanocomposite phosphor with excellent luminescence efficiency and sufficient durability for practical use. Our approach was to disperse luminescent single nanocrystals of CaI 2 :Eu 2+ in a chemically stable, translucent crystalline SiO 2 matrix. Using this approach, we successfully prepared a nanocomposite phosphor by means of self-organization through a simple solid-state reaction. Single nanocrystals of 6H polytype (thr notation) CaI 2 :Eu 2+ with diameters of about 50 nm could be generated not only in a SiO 2 amorphous powder but also in a SiO 2 glass plate. The nanocomposite phosphor formed upon solidification of molten CaI 2 left behind in the crystalline SiO 2 that formed from the amorphous SiO 2 under the influence of a CaI 2 flux effect. The resulting nanocomposite phosphor emitted brilliant blue luminescence with an internal quantum efficiency up to 98% upon 407 nm violet excitation. We used cathodoluminescence microscopy, scanning transmission electron microscopy, and Rietveld refinement of the X-ray diffraction patterns to confirm that the blue luminescence was generated only by the CaI 2 :Eu 2+ single nanocrystals. The phosphor was chemically durable because the luminescence sites were embedded in the crystalline SiO 2 matrix. The phosphor is suitable for use in near-ultraviolet light-emitting diodes. The concept for this nanocomposite phosphor can be expected to be effective for improvements in the practicality of poorly durable materials such as halides and chalcogenides.

Dense Ge nanocrystals embedded in TiO2 with exponentially increased photoconduction by field effect.

PubMed

Lepadatu, A-M; Slav, A; Palade, C; Dascalescu, I; Enculescu, M; Iftimie, S; Lazanu, S; Teodorescu, V S; Ciurea, M L; Stoica, T

2018-03-20

Si and Ge nanocrystals in oxides are of a large interest for photo-effect applications due to the fine-tuning of the optical bandgap by quantum confinement in nanocrystals. In this work, dense Ge nanocrystals suitable for enhanced photoconduction were fabricated from 60% Ge in TiO 2 amorphous layers by low temperature rapid thermal annealing at 550 °C. An exponential increase of the photocurrent with the applied voltage was observed in coplanar structure of Ge nanocrystals composite films deposited on oxidized Si wafers. The behaviour was explained by field effect control of the Fermi level at the Ge nanocrystals-TiO 2 layer/substrate interfaces. The blue-shift of the absorption gap from bulk Ge value to 1.14 eV was evidenced in both photocurrent spectra and optical reflection-transmission experiments, in good agreement with quantum confinement induced bandgap broadening in Ge nanocrystal with sizes of about 5 nm as found from HRTEM and XRD investigations. A nonmonotonic spectral dependence of the refractive index is associated to the Ge nanocrystals formation. The nanocrystal morphology is also in good agreement with the Coulomb gap hopping mechanism of T -1/2 -type explaining the temperature dependence of the dark conduction.

Trapping time of excitons in Si nanocrystals embedded in a SiO2 matrix

NASA Astrophysics Data System (ADS)

de Jong, E. M. L. D.; de Boer, W. D. A. M.; Yassievich, I. N.; Gregorkiewicz, T.

2017-05-01

Silicon (Si) nanocrystals (NCs) are of great interest for many applications, ranging from photovoltaics to optoelectonics. The photoluminescence quantum yield of Si NCs dispersed in SiO2 is limited, suggesting the existence of very efficient processes of nonradiative recombination, among which the formation of a self-trapped exciton state on the surface of the NC. In order to improve the external quantum efficiency of these systems, the carrier relaxation and recombination need to be understood more thoroughly. For that purpose, we perform transient-induced absorption spectroscopy on Si NCs embedded in a SiO2 matrix over a broad probe range for NCs of average sizes from 2.5 to 5.5 nm. The self-trapping of free excitons on surface-related states is experimentally and theoretically discussed and found to be dependent on the NC size. These results offer more insight into the self-trapped exciton state and are important to increase the optical performance of Si NCs.

Ge nanocrystals embedded in ultrathin Si3N4 multilayers with SiO2 barriers

NASA Astrophysics Data System (ADS)

Bahariqushchi, R.; Gundogdu, Sinan; Aydinli, A.

2017-04-01

Multilayers of germanium nanocrystals (NCs) embedded in thin films of silicon nitride matrix separated with SiO2 barriers have been fabricated using plasma enhanced chemical vapor deposition (PECVD). SiGeN/SiO2 alternating bilayers have been grown on quartz and Si substrates followed by post annealing in Ar ambient from 600 to 900 °C. High resolution transmission electron microscopy (HRTEM) as well as Raman spectroscopy show good crystallinity of Ge confined to SiGeN layers in samples annealed at 900 °C. Strong compressive stress for SiGeN/SiO2 structures were observed through Raman spectroscopy. Size, as well as NC-NC distance were controlled along the growth direction for multilayer samples by varying the thickness of bilayers. Visible photoluminescence (PL) at 2.3 and 3.1 eV with NC size dependent intensity is observed and possible origin of PL is discussed.

124Xe(n,γ)125Xe and 124Xe(n,2n)123Xe measurements for National Ignition Facility

NASA Astrophysics Data System (ADS)

Bhike, Megha; Ludin, Nurin; Tornow, Werner

2015-05-01

The cross section for the 124Xe(n,γ)125Xe reaction has been measured for the first time for neutron energies above 100 keV. In addition, the 124Xe(n,2n)123Xe reaction has been studied between threshold and 14.8 MeV. The results of these measurements provide sensitive diagnostic tools for investigating properties of the inertial confinement fusion plasma in Deuterium-Tritium (DT) capsules at the National Ignition Facility (NIF) located at Lawrence Livermore National Laboratory.

Formation of SiGe nanocrystals embedded in Al{sub 2}O{sub 3} for the application of write-once-read-many-times memory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Min-Lin; Wu, Yung-Hsien; Lin, Chia-Chun

2012-10-15

The structure of SiGe nanocrystals embedded in Al{sub 2}O{sub 3} formed by sequential deposition of Al{sub 2}O{sub 3}/Si/Ge/Al{sub 2}O{sub 3} and a subsequent annealing was confirmed by transmission electron microscopy and energy dispersive spectroscopy (EDS), and its application for write-once-read-many-times (WORM) memory devices was explored in this study. By applying a -10 V pulse for 1 s, a large amount of holes injected from Si substrate are stored in the nanocrystals and consequently, the current at +1.5 V increases by a factor of 10{sup 4} as compared to that of the initial state. Even with a smaller -5 V pulsemore » for 1 {mu}s, a sufficiently large current ratio of 36 can still be obtained, verifying the low power operation. Since holes are stored in nanocrystals which are isolated from Si substrate by Al{sub 2}O{sub 3} with good integrity and correspond to a large valence band offset with respect to Al{sub 2}O{sub 3}, desirable read endurance up to 10{sup 5} cycles and excellent retention over 100 yr are achieved. Combining these promising characteristics, WORM memory devices are appropriate for high-performance archival storage applications.« less

Strong visible electroluminescence from silicon nanocrystals embedded in a silicon carbide film

DOE Office of Scientific and Technical Information (OSTI.GOV)

Huh, Chul, E-mail: chuh@etri.re.kr; Kim, Tae-Youb; Ahn, Chang-Geun

2015-05-25

We report the strong visible light emission from silicon (Si) nanocrystals (NCs) embedded in a Si carbide (SiC) film. Compared to Si NC light-emitting diode (LED) by employing the Si nitride (SiN{sub x}) film as a surrounding matrix, the turn-on voltage of the Si NC LED with the SiC film was significantly decreased by 4 V. This was attributed to a smaller barrier height for injecting the electrons into the Si NCs due to a smaller band gap of SiC film than a SiN{sub x} film. The electroluminescence spectra increases with increasing forward voltage, indicating that the electrons are efficiently injectedmore » into the Si NCs in the SiC film. The light output power shows a linear increase with increasing forward voltage. The light emission originated from the Si NCs in a SiC film was quite uniform. The power efficiency of the Si NC LED with the SiC film was 1.56 times larger than that of the Si NC LED with the SiN{sub x} film. The Si NCs in a SiC film show unique advantages and are a promising candidate for application in optical devices.« less

Ti12Xe: A twelve-coordinated Xe-containing molecule

NASA Astrophysics Data System (ADS)

Miao, Junjian; Xu, Wenwu; Zhu, Beien; Gao, Yi

2017-08-01

A twelve-coordinated Xe-containing molecule Ti12Xe has been predicted by DFT calculations with quasi-icosahedral symmetry. Structural and NBO analyses show the chemical bonding exists between the central Xe atom and peripheral Ti atoms, which leads to the high stability of the molecule to a considerable degree. First principle molecular dynamics simulations further reveal the particularly high thermal stability of Ti12Xe up to 1500 K. This unique species may disclose new physics and chemistry of xenon element and stir interest in the Xe-transition metal cluster physics and chemistry.

Matrix effect on vibrational frequencies: Experiments and simulations for HCl and HNgCl (Ng = Kr and Xe)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kalinowski, Jaroslaw; Räsänen, Markku; Lignell, Antti

2014-03-07

We study the environmental effect on molecules embedded in noble-gas (Ng) matrices. The experimental data on HXeCl and HKrCl in Ng matrices is enriched. As a result, the H−Xe stretching bands of HXeCl are now known in four Ng matrices (Ne, Ar, Kr, and Xe), and HKrCl is now known in Ar and Kr matrices. The order of the H−Xe stretching frequencies of HXeCl in different matrices is ν(Ne) < ν(Xe) < ν(Kr) < ν(Ar), which is a non-monotonous function of the dielectric constant, in contrast to the “classical” order observed for HCl: ν(Xe) < ν(Kr) < ν(Ar) < ν(Ne).more » The order of the H−Kr stretching frequencies of HKrCl is consistently ν(Kr) < ν(Ar). These matrix effects are analyzed theoretically by using a number of quantum chemical methods. The calculations on these molecules (HCl, HXeCl, and HKrCl) embedded in single Ng{sup ′} layer cages lead to very satisfactory results with respect to the relative matrix shifts in the case of the MP4(SDQ) method whereas the B3LYP-D and MP2 methods fail to fully reproduce these experimental results. The obtained order of frequencies is discussed in terms of the size available for the Ng hydrides in the cages, probably leading to different stresses on the embedded molecule. Taking into account vibrational anharmonicity produces a good agreement of the MP4(SDQ) frequencies of HCl and HXeCl with the experimental values in different matrices. This work also highlights a number of open questions in the field.« less

Phase diagrams of ferroelectric nanocrystals strained by an elastic matrix

NASA Astrophysics Data System (ADS)

Nikitchenko, A. I.; Azovtsev, A. V.; Pertsev, N. A.

2018-01-01

Ferroelectric crystallites embedded into a dielectric matrix experience temperature-dependent elastic strains caused by differences in the thermal expansion of the crystallites and the matrix. Owing to the electrostriction, these lattice strains may affect polarization states of ferroelectric inclusions significantly, making them different from those of a stress-free bulk crystal. Here, using a nonlinear thermodynamic theory, we study the mechanical effect of elastic matrix on the phase states of embedded single-domain ferroelectric nanocrystals. Their equilibrium polarization states are determined by minimizing a special thermodynamic potential that describes the energetics of an ellipsoidal ferroelectric inclusion surrounded by a linear elastic medium. To demonstrate the stability ranges of such states for a given material combination, we construct a phase diagram, where the inclusion’s shape anisotropy and temperature are used as two parameters. The ‘shape-temperature’ phase diagrams are calculated numerically for PbTiO3 and BaTiO3 nanocrystals embedded into representative dielectric matrices generating tensile (silica glass) or compressive (potassium silicate glass) thermal stresses inside ferroelectric inclusions. The developed phase maps demonstrate that the joint effect of thermal stresses and matrix-induced elastic clamping of ferroelectric inclusions gives rise to several important features in the polarization behavior of PbTiO3 and BaTiO3 nanocrystals. In particular, the Curie temperature displays a nonmonotonic variation with the ellipsoid’s aspect ratio, being minimal for spherical inclusions. Furthermore, the diagrams show that the polarization orientation with respect to the ellipsoid’s symmetry axis is controlled by the shape anisotropy and the sign of thermal stresses. Under certain conditions, the mechanical inclusion-matrix interaction qualitatively alters the evolution of ferroelectric states on cooling, inducing a structural transition

Observation of Quantum Confinement in Monodisperse Methylammonium Lead Halide Perovskite Nanocrystals Embedded in Mesoporous Silica.

PubMed

Malgras, Victor; Tominaka, Satoshi; Ryan, James W; Henzie, Joel; Takei, Toshiaki; Ohara, Koji; Yamauchi, Yusuke

2016-10-13

Hybrid organic-inorganic metal halide perovskites have fascinating electronic properties and have already been implemented in various devices. Although the behavior of bulk metal halide perovskites has been widely studied, the properties of perovskite nanocrystals are less well-understood because synthesizing them is still very challenging, in part because of stability. Here we demonstrate a simple and versatile method to grow monodisperse CH 3 NH 3 PbBr x I x-3 perovskite nanocrystals inside mesoporous silica templates. The size of the nanocrystal is governed by the pore size of the templates (3.3, 3.7, 4.2, 6.2, and 7.1 nm). In-depth structural analysis shows that the nanocrystals maintain the perovskite crystal structure, but it is slightly distorted. Quantum confinement was observed by tuning the size of the particles via the template. This approach provides an additional route to tune the optical bandgap of the nanocrystal. The level of quantum confinement was modeled taking into account the dimensions of the rod-shaped nanocrystals and their close packing inside the channels of the template. Photoluminescence measurements on CH 3 NH 3 PbBr clearly show a shift from green to blue as the pore size is decreased. Synthesizing perovskite nanostructures in templates improves their stability and enables tunable electronic properties via quantum confinement. These structures may be useful as reference materials for comparison with other perovskites, or as functional materials in all solid-state light-emitting diodes.

Laser-induced growth of nanocrystals embedded in porous materials

PubMed Central

2013-01-01

Space localization of the linear and nonlinear optical properties in a transparent medium at the submicron scale is still a challenge to yield the future generation of photonic devices. Laser irradiation techniques have always been thought to structure the matter at the nanometer scale, but combining them with doping methods made it possible to generate local growth of several types of nanocrystals in different kinds of silicate matrices. This paper summarizes the most recent works developed in our group, where the investigated nanoparticles are either made of metal (gold) or chalcogenide semiconductors (CdS, PbS), grown in precursor-impregnated porous xerogels under different laser irradiations. This review is associated to new results on silver nanocrystals in the same kind of matrices. It is shown that, depending on the employed laser, the particles can be formed near the sample surface or deep inside the silica matrix. Photothermal and/or photochemical mechanisms may be invoked to explain the nanoparticle growth, depending on the laser, precursor, and matrix. One striking result is that metal salt reduction, necessary to the production of the corresponding nanoparticles, can efficiently occur due to the thermal wrenching of electrons from the matrix itself or due to multiphoton absorption of the laser light by a reducer additive in femtosecond regime. Very localized semiconductor quantum dots could also be generated using ultrashort pulses, but while PbS nanoparticles grow faster than CdS particles due to one-photon absorption, this better efficiency is counterbalanced by a sensitivity to oxidation. In most cases where the reaction efficiency is high, particles larger than the pores have been obtained, showing that a fast diffusion of the species through the interconnected porosity can modify the matrix itself. Based on our experience in these techniques, we compare several examples of laser-induced nanocrystal growth in porous silica xerogels, which allows

Alkyl Passivation and Amphiphilic Polymer Coating of Silicon Nanocrystals for Diagnostic Imaging

PubMed Central

Hessel, Colin M.; Rasch, Michael R.; Hueso, Jose L.; Goodfellow, Brian W.; Akhavan, Vahid A.; Puvanakrishnan, Priyaveena; Tunnell, James W.

2011-01-01

We show a method to produce biocompatible polymer-coated silicon (Si) nanocrystals for medical imaging. Silica-embedded Si nanocrystals are formed by HSQ thermolysis. The nanocrystals are then liberated from the oxide and terminated with Si-H bonds by HF etching, followed by alkyl monolayer passivation by thermal hydrosilylation. The Si nanocrystals have an average diameter of 2.1 ± 0.6 nm and photoluminesce (PL) with a peak emission wavelength of 650 nm, which lies within the transmission window of 650–900 nm that is useful for biological imaging. The hydrophobic Si nanocrystals are then coated with an amphiphilic polymer for dispersion in aqueous media with pH ranging between 7 and 10 and ionic strength between 30 mM and 2 M, while maintaining a bright and stable PL and a hydrodynamic radius of only 20 nm. Fluorescence imaging of polymer-coated Si nanocrystals in a biological tissue host is demonstrated, showing the potential for in vivo imaging. PMID:20818646

Hydrodynamic predictions for 5.44 TeV Xe+Xe collisions

NASA Astrophysics Data System (ADS)

Giacalone, Giuliano; Noronha-Hostler, Jacquelyn; Luzum, Matthew; Ollitrault, Jean-Yves

2018-03-01

We argue that relativistic hydrodynamics is able to make robust predictions for soft particle production in Xe+Xe collisions at the CERN Large Hadron Collider (LHC). The change of system size from Pb+Pb to Xe+Xe provides a unique opportunity to test the scaling laws inherent to fluid dynamics. Using event-by-event hydrodynamic simulations, we make quantitative predictions for several observables: mean transverse momentum, anisotropic flow coefficients, and their fluctuations. Results are shown as a function of collision centrality.

14N NQR lineshape in nanocrystals: An ab initio investigation of urea

PubMed Central

Gregorovič, Alan

2017-01-01

14N nuclear quadrupole resonance (NQR) lineshapes mostly contain information of low interest, although in nanocrystals they may display some unexpected behaviour. In this work, we present an ab initio computational study of the 14N NQR lineshapes in urea nanocrystals as a function of the nanocrystal size and geometry, focusing on the surface induced broadening of the lineshapes. The lineshapes were obtained through a calculation of the electric field gradient for each nitrogen site in the nanocrystal separately, taking into account the individual crystal field by embedding the molecule of interest in a suitable lattice of point multipoles representing other urea molecules in the nanocrystal. The small influence of distant molecules is found with a series expansion, using the in-crystal Sternheimer shieldings which we also calculated ab initio. We have considered nanocrystals with two geometries: a sphere and a cube, with characteristic sizes between 5 and 100 nm. Our calculations suggest that there is a dramatic difference between the linewidths for the two geometries. For spheres, we find a steep drop in linewidths at ∼10 nm; at 5 nm the linewidth is ∼11 kHz, whereas for sizes above 20 nm the linewidth is practically negligible (<100 Hz). For cubes, on the other hand, we find a steady 1/size decrease, from 12 kHz at 10 nm to 1.2 kHz at 100 nm. This analysis is important for 14N NQR spectroscopy of crystalline pharmaceuticals, where nanoparticles are increasingly more often embedded in some sort of matrix. Although this is only a theoretical analysis, we believe that this work can serve as a guidance for the forthcoming experimental analysis. PMID:28527464

High performance SONOS flash memory with in-situ silicon nanocrystals embedded in silicon nitride charge trapping layer

NASA Astrophysics Data System (ADS)

Lim, Jae-Gab; Yang, Seung-Dong; Yun, Ho-Jin; Jung, Jun-Kyo; Park, Jung-Hyun; Lim, Chan; Cho, Gyu-seok; Park, Seong-gye; Huh, Chul; Lee, Hi-Deok; Lee, Ga-Won

2018-02-01

In this paper, SONOS-type flash memory device with highly improved charge-trapping efficiency is suggested by using silicon nanocrystals (Si-NCs) embedded in silicon nitride (SiNX) charge trapping layer. The Si-NCs were in-situ grown by PECVD without additional post annealing process. The fabricated device shows high program/erase speed and retention property which is suitable for multi-level cell (MLC) application. Excellent performance and reliability for MLC are demonstrated with large memory window of ∼8.5 V and superior retention characteristics of 7% charge loss for 10 years. High resolution transmission electron microscopy image confirms the Si-NC formation and the size is around 1-2 nm which can be verified again in X-ray photoelectron spectroscopy (XPS) where pure Si bonds increase. Besides, XPS analysis implies that more nitrogen atoms make stable bonds at the regular lattice point. Photoluminescence spectra results also illustrate that Si-NCs formation in SiNx is an effective method to form deep trap states.

Inner-shell photoionization and core-hole decay of Xe and XeF2.

PubMed

Southworth, Stephen H; Wehlitz, Ralf; Picón, Antonio; Lehmann, C Stefan; Cheng, Lan; Stanton, John F

2015-06-14

Photoionization cross sections and partial ion yields of Xe and XeF2 from Xe 3d(5/2), Xe 3d(3/2), and F 1s subshells in the 660-740 eV range are compared to explore effects of the F ligands. The Xe 3d-ϵf continuum shape resonances dominate the photoionization cross sections of both the atom and molecule, but prominent resonances appear in the XeF2 cross section due to nominal excitation of Xe 3d and F 1s electrons to the lowest unoccupied molecular orbital (LUMO), a delocalized anti-bonding MO. Comparisons of the ion products from the atom and molecule following Xe 3d photoionization show that the charge-state distribution of Xe ions is shifted to lower charge states in the molecule along with production of energetic F(+) and F(2+) ions. This suggests that, in decay of a Xe 3d core hole, charge is redistributed to the F ligands and the system dissociates due to Coulomb repulsion. The ion products from excitation of the F 1s-LUMO resonance are different and show strong increases in the yields of Xe(+) and F(+) ions. The subshell ionization thresholds, the LUMO resonance energies, and their oscillator strengths are calculated by relativistic coupled-cluster methods and agree well with measurements.

Inner-shell photoionization and core-hole decay of Xe and XeF 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Southworth, Stephen H.; Wehlitz, Ralf; Picón, Antonio

2015-06-14

Photoionization cross sections and partial ion yields of Xe and XeF2 from Xe 3d5/2, Xe 3d3/2, and F 1s subshells in the 660–740 eV range are compared to explore effects of the F ligands. The Xe 3d-ϵf continuum shape resonances dominate the photoionization cross sections of both the atom and molecule, but prominent resonances appear in the XeF2 cross section due to nominal excitation of Xe 3d and F 1s electrons to the lowest unoccupied molecular orbital (LUMO), a delocalized anti-bonding MO. Comparisons of the ion products from the atom and molecule following Xe 3d photoionization show that the charge-statemore » distribution of Xe ions is shifted to lower charge states in the molecule along with production of energetic F+ and F2+ ions. This suggests that, in decay of a Xe 3d core hole, charge is redistributed to the F ligands and the system dissociates due to Coulomb repulsion. The ion products from excitation of the F 1s-LUMO resonance are different and show strong increases in the yields of Xe+ and F+ ions. The subshell ionization thresholds, the LUMO resonance energies, and their oscillator strengths are calculated by relativistic coupled-cluster methods and agree well with measurements.« less

Tuning Li-Ion Diffusion in α-LiMn 1–x Fe x PO 4 Nanocrystals by Antisite Defects and Embedded β-Phase for Advanced Li-Ion Batteries

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hu, Jiangtao; Xiao, Yinguo; Tang, Hanting

Olivine-structured LiMn1-xFexPO4 has become a promising candidate for cathode materials owing to its higher working voltage of 4.1 V and thus larger energy density than that of LiFePO4, which has been used for electric vehicles batteries with the advantage of high safety but disadvantage of low energy density due to its lower working voltage of 3.4 V. One drawback of LiMn1-xFexPO4 electrode is its relatively low electronic and Li-ionic conductivity with Li-ion one-dimensional diffusion. Herein, olivine-structured α-LiMn0.5Fe0.5PO4 nanocrystals were synthesized with optimized Li-ion diffusion channels in LiMn1-xFexPO4 nanocrystals by inducing high concentrations of Fe2+-Li+ antisite defects, which showed impressive capacitymore » improvements of approaching 162, 127, 73, and 55 mAh g-1 at 0.1, 10, 50, and 100 C, respectively, and a long-term cycling stability of maintaining about 74% capacity after 1000 cycles at 10 C. By using high-resolution transmission electron microscopy imaging and joint refinement of hard X-ray and neutron powder diffraction patterns, we revealed that the extraordinary high-rate performance could be achieved by suppressing the formation of electrochemically inactive phase (β-LiMn1-xFexPO4, which is first reported in this work) embedded in α-LiMn0.5Fe0.5PO4. Because of the coherent orientation relationship between β- and α- phases, the β-phase embedded would impede the Li+ diffusion along the [100] and/or [001] directions that was activated by the high density of Fe2+-Li+ antisite (4.24%) in α-phase. Thus, by optimizing concentrations of Fe2+-Li+ antisite defects and suppressing β-phase-embedded olivine structure, Li-ion diffusion properties in LiMn1-xFexPO4 nanocrystals can be tuned by generating new Li+ tunneling. These findings may provide insights into the design and generation of other advanced electrode materials with improved rate performance.« less

Tuning Li-Ion Diffusion in α-LiMn 1–xFe xPO 4 Nanocrystals by Antisite Defects and Embedded β-Phase for Advanced Li-Ion Batteries

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hu, Jiangtao; Xiao, Yinguo; Tang, Hanting

Olivine-structured LiMn 1–xFe xPO 4 has become a promising candidate for cathode materials owing to its higher working voltage of 4.1 V and thus larger energy density than that of LiFePO 4, which has been used for electric vehicles batteries with the advantage of high safety but disadvantage of low energy density due to its lower working voltage of 3.4 V. One drawback of LiMn 1–xFe xPO 4 electrode is its relatively low electronic and Li-ionic conductivity with Li-ion one-dimensional diffusion. In this paper, olivine-structured α-LiMn 0.5Fe 0.5PO 4 nanocrystals were synthesized with optimized Li-ion diffusion channels in LiMn 1–xFemore » xPO 4 nanocrystals by inducing high concentrations of Fe 2+–Li + antisite defects, which showed impressive capacity improvements of approaching 162, 127, 73, and 55 mAh g –1 at 0.1, 10, 50, and 100 C, respectively, and a long-term cycling stability of maintaining about 74% capacity after 1000 cycles at 10 C. By using high-resolution transmission electron microscopy imaging and joint refinement of hard X-ray and neutron powder diffraction patterns, we revealed that the extraordinary high-rate performance could be achieved by suppressing the formation of electrochemically inactive phase (β-LiMn 1–xFe xPO 4, which is first reported in this work) embedded in α-LiMn 0.5Fe 0.5PO 4. Because of the coherent orientation relationship between β- and α-phases, the β-phase embedded would impede the Li + diffusion along the [100] and/or [001] directions that was activated by the high density of Fe 2+–Li + antisite (4.24%) in α-phase. Thus, by optimizing concentrations of Fe 2+–Li + antisite defects and suppressing β-phase-embedded olivine structure, Li-ion diffusion properties in LiMn 1–xFe xPO 4 nanocrystals can be tuned by generating new Li + tunneling. Finally, these findings may provide insights into the design and generation of other advanced electrode materials with improved rate performance.« less

Tuning Li-Ion Diffusion in α-LiMn 1–xFe xPO 4 Nanocrystals by Antisite Defects and Embedded β-Phase for Advanced Li-Ion Batteries

DOE PAGES

Hu, Jiangtao; Xiao, Yinguo; Tang, Hanting; ...

2017-07-13

Olivine-structured LiMn 1–xFe xPO 4 has become a promising candidate for cathode materials owing to its higher working voltage of 4.1 V and thus larger energy density than that of LiFePO 4, which has been used for electric vehicles batteries with the advantage of high safety but disadvantage of low energy density due to its lower working voltage of 3.4 V. One drawback of LiMn 1–xFe xPO 4 electrode is its relatively low electronic and Li-ionic conductivity with Li-ion one-dimensional diffusion. In this paper, olivine-structured α-LiMn 0.5Fe 0.5PO 4 nanocrystals were synthesized with optimized Li-ion diffusion channels in LiMn 1–xFemore » xPO 4 nanocrystals by inducing high concentrations of Fe 2+–Li + antisite defects, which showed impressive capacity improvements of approaching 162, 127, 73, and 55 mAh g –1 at 0.1, 10, 50, and 100 C, respectively, and a long-term cycling stability of maintaining about 74% capacity after 1000 cycles at 10 C. By using high-resolution transmission electron microscopy imaging and joint refinement of hard X-ray and neutron powder diffraction patterns, we revealed that the extraordinary high-rate performance could be achieved by suppressing the formation of electrochemically inactive phase (β-LiMn 1–xFe xPO 4, which is first reported in this work) embedded in α-LiMn 0.5Fe 0.5PO 4. Because of the coherent orientation relationship between β- and α-phases, the β-phase embedded would impede the Li + diffusion along the [100] and/or [001] directions that was activated by the high density of Fe 2+–Li + antisite (4.24%) in α-phase. Thus, by optimizing concentrations of Fe 2+–Li + antisite defects and suppressing β-phase-embedded olivine structure, Li-ion diffusion properties in LiMn 1–xFe xPO 4 nanocrystals can be tuned by generating new Li + tunneling. Finally, these findings may provide insights into the design and generation of other advanced electrode materials with improved rate performance.« less

Light-induced changes in silicon nanocrystal based solar cells: Modification of silicon-hydrogen bonding on silicon nanocrystal surface under illumination

NASA Astrophysics Data System (ADS)

Kim, Ka-Hyun; Johnson, Erik V.; Cabarrocas, Pere Roca i.

2016-07-01

Hydrogenated polymorphous silicon (pm-Si:H) is a material consisting of a small volume fraction of nanocrystals embedded in an amorphous matrix. pm-Si:H solar cells demonstrate interesting initial degradation behaviors such as rapid initial change in photovoltaic parameters and self-healing after degradation during light-soaking. The precise dynamics of the light-induced degradation was studied in a series of light-soaking experiments under various illumination conditions such as AM1.5G and filtered 570 nm yellow light. Hydrogen effusion experiment before and after light-soaking further revealed that the initial degradation of pm-Si:H solar cells originate from the modification of silicon-hydrogen bonding on the surface of silicon nanocrystals in pm-Si:H.

Comprehensive sets of 124Xe(n ,γ )125Xe and 124Xe(n ,2 n )123Xe cross-section data for assessment of inertial-confinement deuterium-tritium fusion plasma

NASA Astrophysics Data System (ADS)

Bhike, Megha; Fallin, B.; Gooden, M. E.; Ludin, N.; Tornow, W.

2015-01-01

Measurements of the neutron radiative-capture cross section of 124Xe have been performed for the first time for neutron energies above 100 keV. In addition, data for the 124Xe(n ,2 n )123Xe reaction cross section have been obtained from threshold to 14.8 MeV to cover the entire energy range of interest, while previous data existed only at around 14 MeV. The results of these measurements provide the basis for an alternative and sensitive diagnostic tool for investigating properties of the inertial confinement fusion plasma in deuterium-tritium (DT) capsules at the National Ignition Facility located at Lawrence Livermore National Laboratory. Here, areal density ρ R (density × radius) of the fuel, burn asymmetry, and fuel-ablator mix are of special interest. The 124Xe(n ,γ )125Xe reaction probes the down-scattered neutrons, while the 124Xe(n ,2 n )123Xe reaction provides a measure of the 14 MeV direct neutrons.

Size-Dependent Photon Emission from Organometal Halide Perovskite Nanocrystals Embedded in an Organic Matrix

PubMed Central

2015-01-01

In recent years, organometal halide perovskite materials have attracted significant research interest in the field of optoelectronics. Here, we introduce a simple and low-temperature route for the formation of self-assembled perovskite nanocrystals in a solid organic matrix. We demonstrate that the size and photoluminescence peak of the perovskite nanocrystals can be tuned by varying the concentration of perovskite in the matrix material. The physical origin of the blue shift of the perovskite nanocrystals’ emission compared to its bulk phase is also discussed. PMID:25949773

Hg-Xe exciplex formation in mixed Xe/Ar matrices: molecular dynamics and luminescence study.

PubMed

Lozada-García, Rolando; Rojas-Lorenzo, Germán; Crépin, Claudine; Ryan, Maryanne; McCaffrey, John G

2015-03-19

Luminescence of Hg((3)P1) atoms trapped in mixed Ar/Xe matrices containing a small amount of Xe is reported. Broad emission bands, strongly red-shifted from absorption are recorded which are assigned to strong complexes formed between the excited mercury Hg* and xenon atoms. Molecular dynamics calculations are performed on simulated Xe/Ar samples doped with Hg to follow the behavior of Hg* in the mixed rare gas matrices leading to exciplex formation. The role of Xe atoms in the first solvation shell (SS1) around Hg was investigated in detail, revealing the formation of two kinds of triatomic exciplexes; namely, Xe-Hg*-Xe and Ar-Hg*-Xe. The first species exists only when two xenon atoms are present in SS1 with specific geometries allowing the formation of a linear or quasi-linear exciplex. In the other geometries, or in the presence of only one Xe in SS1, a linear Ar-Hg*-Xe exciplex is formed. The two kinds of exciplexes have different emission bands, the most red-shifted being that involving two Xe atoms, whose emission is very close to that observed in pure Xe matrices. Simulations give a direct access to the analysis of the experimental absorption, emission, and excitation spectra, together with the dynamics of exciplexes formation.

Electron energy-loss spectroscopy of single nanocrystals: mapping of tin allotropes.

PubMed

Roesgaard, Søren; Ramasse, Quentin; Chevallier, Jacques; Fyhn, Mogens; Julsgaard, Brian

2018-05-25

Using monochromated electron energy-loss spectroscopy (EELS), we are able to map different allotropes in Sn-nanocrystals embedded in Si. It is demonstrated that α-Sn and β-Sn, as well as an interface related plasmon, can be distinguished in embedded Sn-nanostructures. The EELS data is interpreted by standard non-negative matrix factorization followed by a manual Lorentzian decomposition. The decomposition allows for a more physical understanding of the EELS mapping without reducing the level of information. Extending the analysis from a reference system to smaller nanocrystals demonstrates that allotrope determination in nanoscale systems down below 5 nm is possible. Such local information proves the use of monochromated EELS mapping as a powerful technique to study nanoscale systems. This possibility enables investigation of small nanostructures that cannot be investigated through other means, allowing for a better understanding and thus leading to realizations that can result in nanomaterials with improved properties.

Electron energy-loss spectroscopy of single nanocrystals: mapping of tin allotropes

NASA Astrophysics Data System (ADS)

Roesgaard, Søren; Ramasse, Quentin; Chevallier, Jacques; Fyhn, Mogens; Julsgaard, Brian

2018-05-01

Using monochromated electron energy-loss spectroscopy (EELS), we are able to map different allotropes in Sn-nanocrystals embedded in Si. It is demonstrated that α-Sn and β-Sn, as well as an interface related plasmon, can be distinguished in embedded Sn-nanostructures. The EELS data is interpreted by standard non-negative matrix factorization followed by a manual Lorentzian decomposition. The decomposition allows for a more physical understanding of the EELS mapping without reducing the level of information. Extending the analysis from a reference system to smaller nanocrystals demonstrates that allotrope determination in nanoscale systems down below 5 nm is possible. Such local information proves the use of monochromated EELS mapping as a powerful technique to study nanoscale systems. This possibility enables investigation of small nanostructures that cannot be investigated through other means, allowing for a better understanding and thus leading to realizations that can result in nanomaterials with improved properties.

Inner-shell photoionization and core-hole decay of Xe and XeF{sub 2}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Southworth, Stephen H.; Picón, Antonio; Lehmann, C. Stefan

2015-06-14

Photoionization cross sections and partial ion yields of Xe and XeF{sub 2} from Xe 3d{sub 5/2}, Xe 3d{sub 3/2}, and F 1s subshells in the 660–740 eV range are compared to explore effects of the F ligands. The Xe 3d-ϵf continuum shape resonances dominate the photoionization cross sections of both the atom and molecule, but prominent resonances appear in the XeF{sub 2} cross section due to nominal excitation of Xe 3d and F 1s electrons to the lowest unoccupied molecular orbital (LUMO), a delocalized anti-bonding MO. Comparisons of the ion products from the atom and molecule following Xe 3d photoionizationmore » show that the charge-state distribution of Xe ions is shifted to lower charge states in the molecule along with production of energetic F{sup +} and F{sup 2+} ions. This suggests that, in decay of a Xe 3d core hole, charge is redistributed to the F ligands and the system dissociates due to Coulomb repulsion. The ion products from excitation of the F 1s-LUMO resonance are different and show strong increases in the yields of Xe{sup +} and F{sup +} ions. The subshell ionization thresholds, the LUMO resonance energies, and their oscillator strengths are calculated by relativistic coupled-cluster methods and agree well with measurements.« less

Doped and codoped silicon nanocrystals: The role of surfaces and interfaces

NASA Astrophysics Data System (ADS)

Marri, Ivan; Degoli, Elena; Ossicini, Stefano

2017-12-01

Si nanocrystals have been extensively studied because of their novel properties and their potential applications in electronic, optoelectronic, photovoltaic, thermoelectric and biological devices. These new properties are achieved through the combination of the quantum confinement of carriers and the strong influence of surface chemistry. As in the case of bulk Si the tuning of the electronic, optical and transport properties is related to the possibility of doping, in a controlled way, the nanocrystals. This is a big challenge since several studies have revealed that doping in Si nanocrystals differs from the one of the bulk. Theory and experiments have underlined that doping and codoping are influenced by a large number of parameters such as size, shape, passivation and chemical environment of the silicon nanocrystals. However, the connection between these parameters and dopant localization as well as the occurrence of self-purification effects are still not clear. In this review we summarize the latest progress in this fascinating research field considering free-standing and matrix-embedded Si nanocrystals both from the theoretical and experimental point of view, with special attention given to the results obtained by ab-initio calculations and to size-, surface- and interface-induced effects.

Photoproduction of light vector mesons in Xe-Xe ultraperipheral collisions at the LHC and the nuclear density of Xe-129

NASA Astrophysics Data System (ADS)

Guzey, V.; Kryshen, E.; Zhalov, M.

2018-07-01

We make predictions for cross sections of ρ and ϕ vector meson photoproduction in ultraperipheral Xe-Xe collisions at √{sNN } = 5.44TeV. Analyzing the momentum transfer distribution of ρ mesons in this process, we explore the feasibility of extracting the nuclear density of 129Xe, which is needed in searches for dark matter with Xenon-based detectors.

Adsorption and excess fission Xe - Adsorption of Xe on vacuum crushed minerals

NASA Technical Reports Server (NTRS)

Bernatowicz, T. J.; Kramer, F. E.; Podosek, F. A.; Honda, M.

1982-01-01

It is hypothesized that adsorption is not likely to provide a sufficiently precise mechanism for the concentration of excess fission Xe in the entire lunar regolith, in view of laboratory analogs of the lunar soil and calculations of the residence times of noble gases in the present day regolith. Lunar cold trap and episodic degassing models are difficult to reconcile, however, with the generality of excess fission Xe in all gas-rich highland breccias. It is concluded that the high Xe concentration in such highland breccias is not the result of Xe adsorption prior to the trapping of this component.

I-Xe systematics in LL chondrites

NASA Technical Reports Server (NTRS)

Bernatowicz, T. J.; Podosek, F. A.; Swindle, T. D.; Honda, M.

1988-01-01

A stepwise heating analysis of Ar and Xe data from five neutron-irradiated whole rock LL chondrites (Soko Banja, Alta Ameen, Tuxtuac, Guidder, and Olivenza) is presented, emphasizing the complicated thermal history of ordinary chondrites. None of the present meteorites show a well-defined (Ar-40)-(Ar-39) apparent age plateau comprised of more than two release fractions. Most of the samples are found to yield well-defined high-temperature correlations between Xe-129/Xe-130 and Xe-128/Xe-130, and thus determinations of I-129/I-127 and Xe-129/Xe-130 at the time of isotopic closure for Xe. As in the case of other ordinary chondrites, the I-Xe systematics for LL chondrites correlate neither with a metamorphic grade nor with chronologies based opon other methods.

Xe-129 - Xe-128 and Ar-40 - Ar-39 chronology of two Antarctic enstatite meteorites

NASA Technical Reports Server (NTRS)

Honda, M.; Bernatowicz, T. J.; Podosek, F. A.

1983-01-01

Xe-129 - Xe-128 and Ar-40 - Ar-39 analyses has been performed on two Antarctic enstatite meteorites, the chondrite Y-691 and the aubrite (enstatite achondrite) ALH-78113. Both meteorites have complex Ar-40 - Ar-39 release patterns to which no unambiguous age assignment is possible. Both give apparently satisfactory Xe-129 - Xe-128 correlations corresponding to unusual ages. The I-Xe age of the chondrite Y-691 is 16 Ma after Bjurbole, not unusual for chondrites in general but 10 Ma later than previously known ages for enstatite chondrites. The I-Xe age of the aubrite ALH-78113 is 210 Ma after Bjurbole, the latest age (rather than a limit) so far observed by the I-Xe technique, but this age assignment must be considered tentative because of the possibility that it is significantly influenced by terrestrial I contamination.

Fabrication of Si heterojunction solar cells using P-doped Si nanocrystals embedded in SiNx films as emitters

PubMed Central

2013-01-01

Si heterojunction solar cells were fabricated on p-type single-crystal Si (sc-Si) substrates using phosphorus-doped Si nanocrystals (Si-NCs) embedded in SiNx (Si-NCs/SiNx) films as emitters. The Si-NCs were formed by post-annealing of silicon-rich silicon nitride films deposited by electron cyclotron resonance chemical vapor deposition. We investigate the influence of the N/Si ratio in the Si-NCs/SiNx films on their electrical and optical properties, as well as the photovoltaic properties of the fabricated heterojunction devices. Increasing the nitrogen content enhances the optical gap E04 while deteriorating the electrical conductivity of the Si-NCs/SiNx film, leading to an increased short-circuit current density and a decreased fill factor of the heterojunction device. These trends could be interpreted by a bi-phase model which describes the Si-NCs/SiNx film as a mixture of a high-transparency SiNx phase and a low-resistivity Si-NC phase. A preliminary efficiency of 8.6% is achieved for the Si-NCs/sc-Si heterojunction solar cell. PMID:24188725

Nanocrystal structures

DOEpatents

Eisler, Hans J [Stoneham, MA; Sundar, Vikram C [Stoneham, MA; Walsh, Michael E [Everett, MA; Klimov, Victor I [Los Alamos, NM; Bawendi, Moungi G [Cambridge, MA; Smith, Henry I [Sudbury, MA

2008-12-30

A structure including a grating and a semiconductor nanocrystal layer on the grating, can be a laser. The semiconductor nanocrystal layer can include a plurality of semiconductor nanocrystals including a Group II-VI compound, the nanocrystals being distributed in a metal oxide matrix. The grating can have a periodicity from 200 nm to 500 nm.

Nanocrystal structures

DOEpatents

Eisler, Hans J.; Sundar, Vikram C.; Walsh, Michael E.; Klimov, Victor I.; Bawendi, Moungi G.; Smith, Henry I.

2006-12-19

A structure including a grating and a semiconductor nanocrystal layer on the grating, can be a laser. The semiconductor nanocrystal layer can include a plurality of semiconductor nanocrystals including a Group II–VI compound, the nanocrystals being distributed in a metal oxide matrix. The grating can have a periodicity from 200 nm to 500 nm.

Atomic Layer Deposited Oxide-Based Nanocomposite Structures with Embedded CoPtx Nanocrystals for Resistive Random Access Memory Applications.

PubMed

Wang, Lai-Guo; Cao, Zheng-Yi; Qian, Xu; Zhu, Lin; Cui, Da-Peng; Li, Ai-Dong; Wu, Di

2017-02-22

Al 2 O 3 - or HfO 2 -based nanocomposite structures with embedded CoPt x nanocrystals (NCs) on TiN-coated Si substrates have been prepared by combination of thermal atomic layer deposition (ALD) and plasma-enhanced ALD for resistive random access memory (RRAM) applications. The impact of CoPt x NCs and their average size/density on the resistive switching properties has been explored. Compared to the control sample without CoPt x NCs, ALD-derived Pt/oxide/100 cycle-CoPt x NCs/TiN/SiO 2 /Si exhibits a typical bipolar, reliable, and reproducible resistive switching behavior, such as sharp distribution of RRAM parameters, smaller set/reset voltages, stable resistance ratio (≥10 2 ) of OFF/ON states, better switching endurance up to 10 4 cycles, and longer data retention over 10 5 s. The possible resistive switching mechanism based on nanocomposite structures of oxide/CoPt x NCs has been proposed. The dominant conduction mechanisms in low- and high-resistance states of oxide-based device units with embedded CoPt x NCs are Ohmic behavior and space-charge-limited current, respectively. The insertion of CoPt x NCs can effectively improve the formation of conducting filaments due to the CoPt x NC-enhanced electric field intensity. Besides excellent resistive switching performances, the nanocomposite structures also simultaneously present ferromagnetic property. This work provides a flexible pathway by combining PEALD and TALD compatible with state-of-the-art Si-based technology for multifunctional electronic devices applications containing RRAM.

Si Nanocrystal-Embedded SiO x nanofoils: Two-Dimensional Nanotechnology-Enabled High Performance Li Storage Materials.

PubMed

Yoo, Hyundong; Park, Eunjun; Bae, Juhye; Lee, Jaewoo; Chung, Dong Jae; Jo, Yong Nam; Park, Min-Sik; Kim, Jung Ho; Dou, Shi Xue; Kim, Young-Jun; Kim, Hansu

2018-05-02

Silicon (Si) based materials are highly desirable to replace currently used graphite anode for lithium ion batteries. Nevertheless, its usage is still a big challenge due to poor battery performance and scale-up issue. In addition, two-dimensional (2D) architectures, which remain unresolved so far, would give them more interesting and unexpected properties. Herein, we report a facile, cost-effective, and scalable approach to synthesize Si nanocrystals embedded 2D SiO x nanofoils for next-generation lithium ion batteries through a solution-evaporation-induced interfacial sol-gel reaction of hydrogen silsesquioxane (HSiO 1.5 , HSQ). The unique nature of the thus-prepared centimeter scale 2D nanofoil with a large surface area enables ultrafast Li + insertion and extraction, with a reversible capacity of more than 650 mAh g -1 , even at a high current density of 50 C (50 A g -1 ). Moreover, the 2D nanostructured Si/SiO x nanofoils show excellent cycling performance up to 200 cycles and maintain their initial dimensional stability. This superior performance stems from the peculiar nanoarchitecture of 2D Si/SiO x nanofoils, which provides short diffusion paths for lithium ions and abundant free space to effectively accommodate the huge volume changes of Si during cycling.

Novel silica stabilization method for the analysis of fine nanocrystals using coherent X-ray diffraction imaging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Monteforte, Marianne; Estandarte, Ana K.; Chen, Bo

2016-06-23

High-energy X-ray Bragg coherent diffraction imaging (BCDI) is a well established synchrotron-based technique used to quantitatively reconstruct the three-dimensional morphology and strain distribution in nanocrystals. The BCDI technique has become a powerful analytical tool for quantitative investigations of nanocrystals, nanotubes, nanorods and more recently biological systems. BCDI has however typically failed for fine nanocrystals in sub-100?nm size regimes ? a size routinely achievable by chemical synthesis ? despite the spatial resolution of the BCDI technique being 20?30?nm. The limitations of this technique arise from the movement of nanocrystals under illumination by the highly coherent beam, which prevents full diffraction datamore » sets from being acquired. A solution is provided here to overcome this problem and extend the size limit of the BCDI technique, through the design of a novel stabilization method by embedding the fine nanocrystals into a silica matrix. Chemically synthesized FePt nanocrystals of maximum dimension 20?nm and AuPd nanocrystals in the size range 60?65?nm were investigated with BCDI measurement at beamline 34-ID-C of the APS, Argonne National Laboratory. Novel experimental methodologies to elucidate the presence of strain in fine nanocrystals are a necessary pre-requisite in order to better understand strain profiles in engineered nanocrystals for novel device development.« less

Novel silica stabilization method for the analysis of fine nanocrystals using coherent X-ray diffraction imaging.

PubMed

Monteforte, Marianne; Estandarte, Ana K; Chen, Bo; Harder, Ross; Huang, Michael H; Robinson, Ian K

2016-07-01

High-energy X-ray Bragg coherent diffraction imaging (BCDI) is a well established synchrotron-based technique used to quantitatively reconstruct the three-dimensional morphology and strain distribution in nanocrystals. The BCDI technique has become a powerful analytical tool for quantitative investigations of nanocrystals, nanotubes, nanorods and more recently biological systems. BCDI has however typically failed for fine nanocrystals in sub-100 nm size regimes - a size routinely achievable by chemical synthesis - despite the spatial resolution of the BCDI technique being 20-30 nm. The limitations of this technique arise from the movement of nanocrystals under illumination by the highly coherent beam, which prevents full diffraction data sets from being acquired. A solution is provided here to overcome this problem and extend the size limit of the BCDI technique, through the design of a novel stabilization method by embedding the fine nanocrystals into a silica matrix. Chemically synthesized FePt nanocrystals of maximum dimension 20 nm and AuPd nanocrystals in the size range 60-65 nm were investigated with BCDI measurement at beamline 34-ID-C of the APS, Argonne National Laboratory. Novel experimental methodologies to elucidate the presence of strain in fine nanocrystals are a necessary pre-requisite in order to better understand strain profiles in engineered nanocrystals for novel device development.

Diffraction peak profiles of surface relaxed spherical nanocrystals

NASA Astrophysics Data System (ADS)

Perez-Demydenko, C.; Scardi, P.

2017-09-01

A model is proposed for surface relaxation of spherical nanocrystals. Besides reproducing the primary effect of changing the average unit cell parameter, the model accounts for the inhomogeneous atomic displacement caused by surface relaxation and its effect on the diffraction line profiles. Based on three parameters with clear physical meanings - extension of the sub-coordination effect, maximum radial displacement due to sub-coordination, and effective hydrostatic pressure - the model also considers elastic anisotropy and provides parametric expressions of the diffraction line profiles directly applicable in data analysis. The model was tested on spherical nanocrystals of several fcc metals, matching atomic positions with those provided by Molecular Dynamics (MD) simulations based on embedded atom potentials. Agreement was also verified between powder diffraction patterns generated by the Debye scattering equation, using atomic positions from MD and the proposed model.

Time-dependent characteristics of the dielectric barrier discharge in Xe-Cl2 mixture and kinetics of the XeCl∗ molecules

NASA Astrophysics Data System (ADS)

Avtaeva, Svetlana

2014-04-01

Time-dependent characteristics of the dielectric barrier discharge in Xe-Cl2 mixture at chlorine concentration of 0.5% and kinetic processes governing the generation of XeCl∗ molecules are studied using the 1D fluid model. It is shown that at low voltage amplitude (5 kV) a one-peak mode of the discharge is observed and at high voltage amplitude (7 kV) a two-peak mode of the discharge appears. The radiation power of the XeCl∗ band increases with amplitude of the supply voltage. It is demonstrated that the harpoon reaction Xe∗ + Cl2 → XeCl∗ + Cl provides the greatest contribution into generation of XeCl∗ exciplex molecules during short current pulses and the ion-ion recombination Xe+ 2 + Cl- → XeCl* + Xe provides the greatest contribution during afterglow. Quenching of XeCl∗ molecules is a result of the radiative decay XeCl∗ → Xe + Cl + hv (308 nm). During current spike the great contribution into quenching of XeCl∗ provides also the dissociative ionization e + XeCl∗ → Xe+ + Cl + 2e.

High rectifying behavior in Al/Si nanocrystal-embedded SiOxNy/p-Si heterojunctions

NASA Astrophysics Data System (ADS)

Jacques, E.; Pichon, L.; Debieu, O.; Gourbilleau, F.; Coulon, N.

2011-05-01

We examine the electrical properties of MIS devices made of Al/Si nanocrystal-SiOxNy/p-Si. The J-V characteristics of the devices present a high rectifying behavior. Temperature measurements show that the forward current is thermally activated following the thermal diffusion model of carriers. At low reverse bias, the current is governed by thermal emission amplified by the Poole-Frenkel effect of carriers from defects located at the silicon nanocrystals/SiOxNy interfaces, whereas tunnel conduction in silicon oxynitride matrix dominates at high reverse bias. The devices exhibit a rectification ratio >104 for the current measured at V = ± 1 V. Study reveals that thermal annealing in forming gas (H2/N2) improves the electrical properties of the devices due to the passivation of defects.

Synthesis and Doping of Silicon Nanocrystals for Versatile Nanocrystal Inks

NASA Astrophysics Data System (ADS)

Kramer, Nicolaas Johannes

The impact of nanotechnology on our society is getting larger every year. Electronics are becoming smaller and more powerful, the "Internet of Things" is all around us, and data generation is increasing exponentially. None of this would have been possible without the developments in nanotechnology. Crystalline semiconductor nanoparticles (nanocrystals) are one of the latest developments in the field of nanotechnology. This thesis addresses three important challenges for the transition of silicon nanocrystals from the lab bench to the marketplace: A better understanding of the nanocrystal synthesis was obtained, the electronic properties of the nanocrystals were characterized and tuned, and novel silicon nanocrystal inks were formed and applied using simple coating technologies. Plasma synthesis of nanocrystals has numerous advantages over traditional solution-based synthesis methods. While the formation of nanoparticles in low pressure nonthermal plasmas is well known, the heating mechanism leading to their crystallization is poorly understood. A combination of comprehensive plasma characterization with a nanoparticle heating model presented here reveals the underlying plasma physics leading to crystallization. The model predicts that the nanoparticles reach temperatures as high as 900 K in the plasma as a result of heating reactions on the nanoparticle surface. These temperatures are well above the gas temperature and sufficient for complete nanoparticle crystallization. Moving the field of plasma nanoparticle synthesis to atmospheric pressures is important for lowering its cost and making the process attractive for industrial applications. The heating and charging model for silicon nanoparticles was adapted in Chapter 3 to study plasmas maintained over a wide range of pressures (10 -- 105 Pa). The model considers three collisionality regimes and determines the dominant contribution of each regime under various plasma conditions. Strong nanoparticle cooling at

Simulation of ultraviolet- and soft X-ray-pulse generation as a result of cooperative recombination of excitons in diamond nanocrystals embedded in a polymer film

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kukushkin, V. A., E-mail: vakuk@appl.sci-nnov.ru

2013-11-15

Using numerical simulation, it is shown that the recombination of free excitons photoexcited in diamond nanocrystals embedded in a polymer film can occur in the cooperative mode. It is found that this mode can be implemented despite the fact that diamond is an 'indirect' semiconductor. It is shown that the power of the generated radiation at the pulse peak during the cooperative recombination of free excitons can exceed that of the incoherent spontaneous emission of the same initial number of free excitons by more than an order of magnitude. Finally, it is shown that the process under consideration can bemore » used to generate picosecond pulses of ultraviolet and soft X-ray electromagnetic field at a wavelength of 235 nm.« less

Optical properties of p–i–n structures based on amorphous hydrogenated silicon with silicon nanocrystals formed via nanosecond laser annealing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krivyakin, G. K.; Volodin, V. A., E-mail: volodin@isp.nsc.ru; Kochubei, S. A.

Silicon nanocrystals are formed in the i layers of p–i–n structures based on a-Si:H using pulsed laser annealing. An excimer XeCl laser with a wavelength of 308 nm and a pulse duration of 15 ns is used. The laser fluence is varied from 100 (below the melting threshold) to 250 mJ/cm{sup 2} (above the threshold). The nanocrystal sizes are estimated by analyzing Raman spectra using the phonon confinement model. The average is from 2.5 to 3.5 nm, depending on the laser-annealing parameters. Current–voltage measurements show that the fabricated p–i–n structures possess diode characteristics. An electroluminescence signal in the infrared (IR)more » range is detected for the p–i–n structures with Si nanocrystals; the peak position (0.9–1 eV) varies with the laser-annealing parameters. Radiative transitions are presumably related to the nanocrystal–amorphous-matrix interface states. The proposed approach can be used to produce light-emitting diodes on non-refractory substrates.« less

XeNA: an automated 'open-source' (129)Xe hyperpolarizer for clinical use.

PubMed

Nikolaou, Panayiotis; Coffey, Aaron M; Walkup, Laura L; Gust, Brogan M; Whiting, Nicholas; Newton, Hayley; Muradyan, Iga; Dabaghyan, Mikayel; Ranta, Kaili; Moroz, Gregory D; Rosen, Matthew S; Patz, Samuel; Barlow, Michael J; Chekmenev, Eduard Y; Goodson, Boyd M

2014-06-01

Here we provide a full report on the construction, components, and capabilities of our consortium's "open-source" large-scale (~1L/h) (129)Xe hyperpolarizer for clinical, pre-clinical, and materials NMR/MRI (Nikolaou et al., Proc. Natl. Acad. Sci. USA, 110, 14150 (2013)). The 'hyperpolarizer' is automated and built mostly of off-the-shelf components; moreover, it is designed to be cost-effective and installed in both research laboratories and clinical settings with materials costing less than $125,000. The device runs in the xenon-rich regime (up to 1800Torr Xe in 0.5L) in either stopped-flow or single-batch mode-making cryo-collection of the hyperpolarized gas unnecessary for many applications. In-cell (129)Xe nuclear spin polarization values of ~30%-90% have been measured for Xe loadings of ~300-1600Torr. Typical (129)Xe polarization build-up and T1 relaxation time constants were ~8.5min and ~1.9h respectively under our spin-exchange optical pumping conditions; such ratios, combined with near-unity Rb electron spin polarizations enabled by the high resonant laser power (up to ~200W), permit such high PXe values to be achieved despite the high in-cell Xe densities. Importantly, most of the polarization is maintained during efficient HP gas transfer to other containers, and ultra-long (129)Xe relaxation times (up to nearly 6h) were observed in Tedlar bags following transport to a clinical 3T scanner for MR spectroscopy and imaging as a prelude to in vivo experiments. The device has received FDA IND approval for a clinical study of chronic obstructive pulmonary disease subjects. The primary focus of this paper is on the technical/engineering development of the polarizer, with the explicit goals of facilitating the adaptation of design features and operative modes into other laboratories, and of spurring the further advancement of HP-gas MR applications in biomedicine. Copyright © 2014 Elsevier Inc. All rights reserved.

Two-photon pumped amplified spontaneous emission based on all-inorganic perovskite nanocrystals embedded with gold nanorods

NASA Astrophysics Data System (ADS)

Liu, Shaoying; Fang, Xiaohui; Wang, Yimeng; Zhang, Xinping

2018-07-01

CsPbBr3 nanocrystals have attracted great interest owing to their high fluorescence quantum efficiency, adjustable photoluminescence wavelength, and good stability. We report a device that consists of disordered gold nanorods underneath a film of CsPbBr3 nanocrystals. Two-photon pumping using femtosecond laser pulses at 800 nm enables amplified spontaneous emission (ASE) at about 523 nm. In this work, a narrow peak with linewidth of 5 nm is observed when the pump fluence reaches a low threshold of 0.65 mJ/cm2. The results show that plasmonic resonance of gold nanorods improves the emission transition rate and enables low threshold ASE.

Hyperpolarized 131Xe NMR spectroscopy

PubMed Central

Stupic, Karl F.; Cleveland, Zackary I.; Pavlovskaya, Galina E.; Meersmann, Thomas

2011-01-01

Hyperpolarized (hp) 131Xe with up to 2.2% spin polarization (i.e., 5000-fold signal enhancement at 9.4 T) was obtained after separation from the rubidium vapor of the spin-exchange optical pumping (SEOP) process. The SEOP was applied for several minutes in a stopped-flow mode, and the fast, quadrupolar-driven T1 relaxation of this spin I = 3/2 noble gas isotope required a rapid subsequent rubidium removal and swift transfer into the high magnetic field region for NMR detection. Because of the xenon density dependent 131Xe quadrupolar relaxation in the gas phase, the SEOP polarization build-up exhibits an even more pronounced dependence on xenon partial pressure than that observed in 129Xe SEOP. 131Xe is the only stable noble gas isotope with a positive gyromagnetic ratio and shows therefore a different relative phase between hp signal and thermal signal compared to all other noble gases. The gas phase 131Xe NMR spectrum displays a surface and magnetic field dependent quadrupolar splitting that was found to have additional gas pressure and gas composition dependence. The splitting was reduced by the presence of water vapor that presumably influences xenon-surface interactions. The hp 131Xe spectrum shows differential line broadening, suggesting the presence of strong adsorption sites. Beyond hp 131Xe NMR spectroscopy studies, a general equation for the high temperature, thermal spin polarization, P, for spin I⩾1/2 nuclei is presented. PMID:21051249

Chemi-luminescence measurements of hyperthermal Xe{sup +}/Xe{sup 2+}+ NH{sub 3} reactions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Prince, Benjamin D.; Steiner, Colby P.; Chiu, Yu-Hui

2012-04-14

Luminescence spectra are recorded for the reactions of Xe{sup +}+ NH{sub 3} and Xe{sup 2+}+ NH{sub 3} at energies ranging from 11.5 to 206 eV in the center-of-mass (E{sub cm}) frame. Intense features of the luminescence spectra are attributed to the NH (A {sup 3}{Pi}{sub i}-X {sup 3}{Sigma}{sup -}), hydrogen Balmer series, and Xe I emission observable for both primary ions. Evidence for charge transfer products is only found through Xe I emission for both primary ions and NH{sup +} emission for Xe{sup 2+} primary ions. For both primary ions, the absolute NH (A-X) cross section increases with collision energymore » before leveling off at a constant value, approximately 9 x 10{sup -18} cm{sup 2}, at about 50 eV while H-{alpha} emission increases linearly with collision energy. The nascent NH (A) populations derived from the spectral analysis are found to be independent of collision energy and have a constant rotational temperature of 4200 K.« less

Metal-organic frameworks for Xe/Kr separation

DOEpatents

Ryan, Patrick J.; Farha, Omar K.; Broadbelt, Linda J.; Snurr, Randall Q.; Bae, Youn-Sang

2014-07-22

Metal-organic framework (MOF) materials are provided and are selectively adsorbent to xenon (Xe) over another noble gas such as krypton (Kr) and/or argon (Ar) as a result of having framework voids (pores) sized to this end. MOF materials having pores that are capable of accommodating a Xe atom but have a small enough pore size to receive no more than one Xe atom are desired to preferentially adsorb Xe over Kr in a multi-component (Xe--Kr mixture) adsorption method. The MOF material has 20% or more, preferably 40% or more, of the total pore volume in a pore size range of 0.45-0.75 nm which can selectively adsorb Xe over Kr in a multi-component Xe--Kr mixture over a pressure range of 0.01 to 1.0 MPa.

Metal-organic frameworks for Xe/Kr separation

DOEpatents

Ryan, Patrick J.; Farha, Omar K.; Broadbelt, Linda J.; Snurr, Randall Q.; Bae, Youn-Sang

2013-08-27

Metal-organic framework (MOF) materials are provided and are selectively adsorbent to xenon (Xe) over another noble gas such as krypton (Kr) and/or argon (Ar) as a result of having framework voids (pores) sized to this end. MOF materials having pores that are capable of accommodating a Xe atom but have a small enough pore size to receive no more than one Xe atom are desired to preferentially adsorb Xe over Kr in a multi-component (Xe--Kr mixture) adsorption method. The MOF material has 20% or more, preferably 40% or more, of the total pore volume in a pore size range of 0.45-0.75 nm which can selectively adsorb Xe over Kr in a multi-component Xe--Kr mixture over a pressure range of 0.01 to 1.0 MPa.

Xenon in the Protoplanetary Disk (PPD-Xe)

NASA Astrophysics Data System (ADS)

Marti, K.; Mathew, K. J.

2015-06-01

Relationships among solar system Xe components as observed in the solar wind, in planetary atmospheres, and in meteorites are investigated using isotopic correlations. The term PPD-Xe is used for components inferred to have been present in the molecular cloud material that formed the protoplanetary disk (PPD). The evidence of the lack of simple relationships between terrestrial atmospheric Xe and solar or meteoritic components is confirmed. Xe isotopic correlations indicate a heterogeneous PPD composition with variable mixing ratios of the nucleosynthetic component Xe-HL. Solar Xe represents a bulk PPD component, and the isotopic abundances did not change from the time of incorporation into the interior of Mars through times of regolith implantations to the present.

XeNA: An automated ‘open-source’ 129Xe hyperpolarizer for clinical use

PubMed Central

Nikolaou, Panayiotis; Coffey, Aaron M.; Walkup, Laura L.; Gust, Brogan M.; Whiting, Nicholas; Newton, Hayley; Muradyan, Iga; Dabaghyan, Mikayel; Ranta, Kaili; Moroz, Gregory D.; Rosen, Matthew S.; Patz, Samuel; Barlow, Michael J.; Chekmenev, Eduard Y.; Goodson, Boyd M.

2014-01-01

Here we provide a full report on the construction, components, and capabilities of our consortium’s “open-source” large-scale (~1 L/hr) 129Xe hyperpolarizer for clinical, pre-clinical, and materials NMR/MRI (Nikolaou et al., Proc. Natl. Acad. Sci. USA, 110, 14150 (2013)). The ‘hyperpolarizer’ is automated and built mostly of off-the-shelf components; moreover, it is designed to be cost-effective and installed in both research laboratories and clinical settings with materials costing less than $125,000. The device runs in the xenon-rich regime (up to 1800 Torr Xe in 0.5 L) in either stopped-flow or single-batch mode—making cryo-collection of the hyperpolarized gas unnecessary for many applications. In-cell 129Xe nuclear spin polarization values of ~30-90% have been measured for Xe loadings of ~300-1600 Torr. Typical 129Xe polarization build-up and T1 relaxation time constants were ~8.5 min and ~1.9 hr respectively under our SEOP conditions; such ratios, combined with near-unity Rb electron spin polarizations enabled by the high resonant laser power (up to ~200 W), permits such high PXe values to be achieved despite the high in-cell Xe densities. Importantly, most of the polarization is maintained during efficient HP gas transfer to other containers, and ultra-long 129Xe relaxation times (up to nearly 6 hr) were observed in Tedlar bags following transport to a clinical 3 T scanner for MR spectroscopy and imaging as a prelude to in vivo experiments. The device has received FDA IND approval for a clinical study of COPD subjects. The primary focus of this paper is on the technical / engineering development of the polarizer, with the explicit goals of facilitating the adaptation of design features and operative modes into other laboratories, and of spurring the further advancement of HP-gas MR applications in biomedicine. PMID:24631715

High-spin structures in 132Xe and 133Xe and evidence for isomers along the N =79 isotones

NASA Astrophysics Data System (ADS)

Vogt, A.; Siciliano, M.; Birkenbach, B.; Reiter, P.; Hadyńska-Klek, K.; Wheldon, C.; Valiente-Dobón, J. J.; Teruya, E.; Yoshinaga, N.; Arnswald, K.; Bazzacco, D.; Blazhev, A.; Bracco, A.; Bruyneel, B.; Chakrawarthy, R. S.; Chapman, R.; Cline, D.; Corradi, L.; Crespi, F. C. L.; Cromaz, M.; de Angelis, G.; Eberth, J.; Fallon, P.; Farnea, E.; Fioretto, E.; Fransen, C.; Freeman, S. J.; Fu, B.; Gadea, A.; Gelletly, W.; Giaz, A.; Görgen, A.; Gottardo, A.; Hayes, A. B.; Hess, H.; Hetzenegger, R.; Hirsch, R.; Hua, H.; John, P. R.; Jolie, J.; Jungclaus, A.; Karayonchev, V.; Kaya, L.; Korten, W.; Lee, I. Y.; Leoni, S.; Liang, X.; Lunardi, S.; Macchiavelli, A. O.; Menegazzo, R.; Mengoni, D.; Michelagnoli, C.; Mijatović, T.; Montagnoli, G.; Montanari, D.; Müller-Gatermann, C.; Napoli, D.; Pearson, C. J.; Podolyák, Zs.; Pollarolo, G.; Pullia, A.; Queiser, M.; Recchia, F.; Regan, P. H.; Régis, J.-M.; Saed-Samii, N.; Şahin, E.; Scarlassara, F.; Seidlitz, M.; Siebeck, B.; Sletten, G.; Smith, J. F.; Söderström, P.-A.; Stefanini, A. M.; Stezowski, O.; Szilner, S.; Szpak, B.; Teng, R.; Ur, C.; Warner, D. D.; Wolf, K.; Wu, C. Y.; Zell, K. O.

2017-08-01

The transitional nuclei 132Xe and 133Xe are investigated after multinucleon-transfer (MNT) and fusion-evaporation reactions. Both nuclei are populated (i) in 136Xe+208Pb MNT reactions employing the high-resolution Advanced GAmma Tracking Array (AGATA) coupled to the magnetic spectrometer PRISMA, (ii) in the 136Xe+198Pt MNT reaction employing the GAMMASPHERE spectrometer in combination with the gas-detector array CHICO, and (iii) as an evaporation residue after a 130Te(α ,x n )134 -x nXe fusion-evaporation reaction employing the HORUS γ -ray array at the University of Cologne. The high-spin level schemes are considerably extended above the Jπ=(7-) and (10+) isomers in 132Xe and above the 11 /2- isomer in 133Xe. The results are compared to the high-spin systematics of the Z =54 as well as the N =78 and N =79 chains. Furthermore, evidence is found for a long-lived (T1 /2≫1 μ s ) isomer in 133Xe which closes a gap along the N =79 isotones. Shell-model calculations employing the SN100PN and PQM130 effective interactions reproduce the experimental findings and provide guidance to the interpretation of the observed high-spin features.

High-spin structures in Xe 132 and Xe 133 and evidence for isomers along the N = 79 isotones

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vogt, A.; Siciliano, M.; Birkenbach, B.

In this study, the transitional nuclei 132Xe and 133Xe are investigated after multinucleon-transfer (MNT) and fusion-evaporation reactions. Both nuclei are populated (i) in 136Xe + 208Pb MNT reactions employing the high-resolution Advanced GAmma Tracking Array (AGATA) coupled to the magnetic spectrometer PRISMA, (ii) in the 136Xe + 198Pt MNT reaction employing the GAMMASPHERE spectrometer in combination with the gas-detector array CHICO, and (iii) as an evaporation residue after a 130Te (α,xn) 134-xnXe fusion-evaporation reaction employing the HORUS γ -ray array at the University of Cologne. The high-spin level schemes are considerably extended above the J π = (7 -) andmore » (10 +) isomers in 132Xe and above the 11/2 - isomer in 133Xe. The results are compared to the high-spin systematics of the Z = 54 as well as the N = 78 and N = 79 chains. Furthermore, evidence is found for a long-lived (T 1/2 » 1 μs) isomer in 133Xe which closes a gap along the N = 79 isotones. Finally, shell-model calculations employing the SN100PN and PQM130 effective interactions reproduce the experimental findings and provide guidance to the interpretation of the observed high-spin features.« less

High-spin structures in Xe 132 and Xe 133 and evidence for isomers along the N = 79 isotones

DOE PAGES

Vogt, A.; Siciliano, M.; Birkenbach, B.; ...

2017-08-24

In this study, the transitional nuclei 132Xe and 133Xe are investigated after multinucleon-transfer (MNT) and fusion-evaporation reactions. Both nuclei are populated (i) in 136Xe + 208Pb MNT reactions employing the high-resolution Advanced GAmma Tracking Array (AGATA) coupled to the magnetic spectrometer PRISMA, (ii) in the 136Xe + 198Pt MNT reaction employing the GAMMASPHERE spectrometer in combination with the gas-detector array CHICO, and (iii) as an evaporation residue after a 130Te (α,xn) 134-xnXe fusion-evaporation reaction employing the HORUS γ -ray array at the University of Cologne. The high-spin level schemes are considerably extended above the J π = (7 -) andmore » (10 +) isomers in 132Xe and above the 11/2 - isomer in 133Xe. The results are compared to the high-spin systematics of the Z = 54 as well as the N = 78 and N = 79 chains. Furthermore, evidence is found for a long-lived (T 1/2 » 1 μs) isomer in 133Xe which closes a gap along the N = 79 isotones. Finally, shell-model calculations employing the SN100PN and PQM130 effective interactions reproduce the experimental findings and provide guidance to the interpretation of the observed high-spin features.« less

High energy XeBr electric discharge laser

DOEpatents

Sze, Robert C.; Scott, Peter B.

1981-01-01

A high energy XeBr laser for producing coherent radiation at 282 nm. The XeBr laser utilizes an electric discharge as the excitation source to minimize formation of molecular ions thereby minimizing absorption of laser radiation by the active medium. Additionally, HBr is used as the halogen donor which undergoes harpooning reactions with Xe.sub.M * to form XeBr*.

High energy XeBr electric discharge laser

DOEpatents

Sze, R.C.; Scott, P.B.

A high energy XeBr laser for producing coherent radiation at 282 nm is disclosed. The XeBr laser utilizes an electric discharge as the excitation source to minimize formation of molecular ions thereby minimizing absorption of laser radiation by the active medium. Additionally, HBr, is used as the halogen donor which undergoes harpooning reactions with Xe/sub M/ to form XeBr.

Xenon in the protoplanetary disk (PPD-XE)

DOE PAGES

Marti, K.; Mathew, K. J.

2015-06-18

Relationships among solar system Xe components as observed in the solar wind (SW), in planetary atmospheres and in meteorites are investigated using isotopic correlations. The term PPD-Xe is used for components inferred to have been present in the molecular cloud material that formed the protoplanetary disk (PPD). The evidence of the lack of simple relationships between terrestrial atmospheric Xe and solar or meteoritic components is confirmed. Xe isotopic correlations indicate a heterogeneous PPD composition with variable mixing ratios of the nucleosynthetic component Xe-HL. Solar Xe represents a bulk PPD component, and the isotopic abundances did not change from the timemore » of incorporation into the interior of Mars, through times of regolith implantations to the present.« less

Weaving a two-dimensional fishing net from titanoniobate nanosheets embedded with Fe3O4 nanocrystals for highly efficient capture and isotope labeling of phosphopeptides

NASA Astrophysics Data System (ADS)

Chen, Xueqin; Li, Siyuan; Zhang, Xiaoxia; Min, Qianhao; Zhu, Jun-Jie

2015-03-01

Qualitative and quantitative characterization of phosphopeptides by means of mass spectrometry (MS) is the main goal of MS-based phosphoproteomics, but suffers from their low abundance in the large haystack of various biological molecules. Herein, we introduce two-dimensional (2D) metal oxides to tackle this biological separation issue. A nanocomposite composed of titanoniobate nanosheets embedded with Fe3O4 nanocrystals (Fe3O4-TiNbNS) is constructed via a facile cation-exchange approach, and adopted for the capture and isotope labeling of phosphopeptides. In this nanoarchitecture, the 2D titanoniobate nanosheets offer enlarged surface area and a spacious microenvironment for capturing phosphopeptides, while the Fe3O4 nanocrystals not only incorporate a magnetic response into the composite but, more importantly, also disrupt the restacking process between the titanoniobate nanosheets and thus preserve a greater specific surface for binding phosphopeptides. Owing to the extended active surface, abundant Lewis acid sites and excellent magnetic controllability, Fe3O4-TiNbNS demonstrates superior sensitivity, selectivity and capacity over homogeneous bulk metal oxides, layered oxides, and even restacked nanosheets in phosphopeptide enrichment, and further allows in situ isotope labeling to quantify aberrantly-regulated phosphopeptides from sera of leukemia patients. This composite nanosheet greatly contributes to the MS analysis of phosphopeptides and gives inspiration in the pursuit of 2D structured materials for separation of other biological molecules of interests.Qualitative and quantitative characterization of phosphopeptides by means of mass spectrometry (MS) is the main goal of MS-based phosphoproteomics, but suffers from their low abundance in the large haystack of various biological molecules. Herein, we introduce two-dimensional (2D) metal oxides to tackle this biological separation issue. A nanocomposite composed of titanoniobate nanosheets embedded with Fe3

129 Xe chemical shift in human blood and pulmonary blood oxygenation measurement in humans using hyperpolarized 129 Xe NMR.

PubMed

Norquay, Graham; Leung, General; Stewart, Neil J; Wolber, Jan; Wild, Jim M

2017-04-01

To evaluate the dependency of the 129 Xe-red blood cell (RBC) chemical shift on blood oxygenation, and to use this relation for noninvasive measurement of pulmonary blood oxygenation in vivo with hyperpolarized 129 Xe NMR. Hyperpolarized 129 Xe was equilibrated with blood samples of varying oxygenation in vitro, and NMR was performed at 1.5 T and 3 T. Dynamic in vivo NMR during breath hold apnea was performed at 3 T on two healthy volunteers following inhalation of hyperpolarized 129 Xe. The 129 Xe chemical shift in RBCs was found to increase nonlinearly with blood oxygenation at 1.5 T and 3 T. During breath hold apnea, the 129 Xe chemical shift in RBCs exhibited a periodic time modulation and showed a net decrease in chemical shift of ∼1 ppm over a 35 s breath hold, corresponding to a decrease of 7-10 % in RBC oxygenation. The 129 Xe-RBC signal amplitude showed a modulation with the same frequency as the 129 Xe-RBC chemical shift. The feasibility of using the 129 Xe-RBC chemical shift to measure pulmonary blood oxygenation in vivo has been demonstrated. Correlation between 129 Xe-RBC signal and 129 Xe-RBC chemical shift modulations in the lung warrants further investigation, with the aim to better quantify temporal blood oxygenation changes in the cardiopulmonary vascular circuit. Magn Reson Med 77:1399-1408, 2017. © 2016 The Authors Magnetic Resonance in Medicine published by Wiley Periodicals, Inc. on behalf of International Society for Magnetic Resonance in Medicine. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited. © 2016 The Authors Magnetic Resonance in Medicine published by Wiley Periodicals, Inc. on behalf of International Society for Magnetic Resonance in Medicine.

High-spin structure of 134Xe

NASA Astrophysics Data System (ADS)

Vogt, A.; Birkenbach, B.; Reiter, P.; Blazhev, A.; Siciliano, M.; Valiente-Dobón, J. J.; Wheldon, C.; Bazzacco, D.; Bowry, M.; Bracco, A.; Bruyneel, B.; Chakrawarthy, R. S.; Chapman, R.; Cline, D.; Corradi, L.; Crespi, F. C. L.; Cromaz, M.; de Angelis, G.; Eberth, J.; Fallon, P.; Farnea, E.; Fioretto, E.; Freeman, S. J.; Gadea, A.; Geibel, K.; Gelletly, W.; Gengelbach, A.; Giaz, A.; Görgen, A.; Gottardo, A.; Hayes, A. B.; Hess, H.; Hua, H.; John, P. R.; Jolie, J.; Jungclaus, A.; Korten, W.; Lee, I. Y.; Leoni, S.; Liang, X.; Lunardi, S.; Macchiavelli, A. O.; Menegazzo, R.; Mengoni, D.; Michelagnoli, C.; Mijatović, T.; Montagnoli, G.; Montanari, D.; Napoli, D.; Pearson, C. J.; Pellegri, L.; Podolyák, Zs.; Pollarolo, G.; Pullia, A.; Radeck, F.; Recchia, F.; Regan, P. H.; Şahin, E.; Scarlassara, F.; Sletten, G.; Smith, J. F.; Söderström, P.-A.; Stefanini, A. M.; Steinbach, T.; Stezowski, O.; Szilner, S.; Szpak, B.; Teng, R.; Ur, C.; Vandone, V.; Ward, D.; Warner, D. D.; Wiens, A.; Wu, C. Y.

2016-05-01

Detailed spectroscopic information on the N ˜82 nuclei is necessary to benchmark shell-model calculations in the region. The nuclear structure above long-lived isomers in 134Xe is investigated after multinucleon transfer (MNT) and actinide fission. Xenon-134 was populated as (i) a transfer product in 238U+ 136Xe and 208Pb+ 136Xe MNT reactions and (ii) as a fission product in the 238U+ 136Xe reaction employing the high-resolution Advanced Gamma Tracking Array (AGATA). Trajectory reconstruction has been applied for the complete identification of beamlike transfer products with the magnetic spectrometer PRISMA. The 198Pt 136Xe MNT reaction was studied with the γ -ray spectrometer GAMMASPHERE in combination with the gas detector array Compact Heavy Ion Counter (CHICO). Several high-spin states in 134Xe on top of the two long-lived isomers are discovered based on γ γ -coincidence relationships and information on the γ -ray angular distributions as well as excitation energies from the total kinetic energy loss and fission fragments. The revised level scheme of 134Xe is extended up to an excitation energy of 5.832 MeV with tentative spin-parity assignments up to 16+. Previous assignments of states above the 7- isomer are revised. Latest shell-model calculations employing two different effective interactions reproduce the experimental findings and support the new spin and parity assignments.

Biological Studies with Laser-Polarized ^129Xe

NASA Astrophysics Data System (ADS)

Tseng, C. H.; Oteiza, E. R.; Wong, G. A.; Walsworth, R. L.; Albert, M. S.; Nascimben, L.; Peled, S.; Sakai, K.; Jolesz, F. A.

1996-05-01

We have studied several biological systems using laser-polarized ^129Xe. In certain tissues magnetic resonance imaging (MRI) using inhaled laser-polarized noble gases may provide images superior to those from conventional proton MRI. High resolution laser-polarized ^3He images of air spaces in the human lung were recently obtained by the Princeton/Duke group. However, ^3He is not very soluble in tissue. Therefore, we are using laser polarized ^129Xe (tissue-soluble), with the long term goal of biomedical functional imaging. We have investigated multi-echo and multi-excitation magnetic resonance detection schemes to exploit the highly non-thermal ^129Xe magnetization produced by the laser polarization technique. We have inhalated live rats with laser-polarized ^129Xe gas and measured three distinct ^129Xe tissue resonances that last 20 to 40 sec. As a demonstration, we obtained a laser polarized ^129Xe image of the human oral cavity. Currently we are measuring the polarization lifetime of ^129Xe dissolved in human blood, the biological transporting medium. These studies and other recent developments will be reported.

Emission characteristics of Xe-RbBr plasma

NASA Astrophysics Data System (ADS)

Heneral, A. A.; Avtaeva, S. V.

2017-12-01

The luminescence spectra of the longitudinal pulsed-periodic discharge in Xe-RbBr gas-vapour mixtures at low pressures are experimentally studied. Conditions for obtaining strong UV radiation of XeBr* exiplex molecules in the spectral range of 200-425 nm are found. The greatest output of the XeBr* UV radiation is provided at temperature of the gas-discharge tube walls of ~1000 K. The maximum UV emission power of the whole plasma volume is 4.8 W. Formation of XeBr* exciplex molecules in the pulsed-periodic discharge in Xe-RbBr gas-vapour mixtures at low pressures is discussed.

X-ray structural analysis of two-dimensional assembling lead sulfide nanocrystals of different sizes

NASA Astrophysics Data System (ADS)

Ushakova, Elena V.; Golubkov, Valery V.; Litvin, Aleksandr P.; Parfenov, Peter S.; Cherevkov, Sergei A.; Fedorov, Anatoly V.; Baranov, Alexander V.

2016-08-01

We report on the structural investigation of self-organized assemblies of PbS nanocrystals (NCs) of different sizes, which were deposited on a glass substrate or embedded in a porous matrix. Regardless of the NC size and the type of the substrate and matrix, the assemblies were ordered in two-dimensional superlattices with densely packed NCs.

Titanium-tungsten nanocrystals embedded in a SiO(2)/Al(2)O(3) gate dielectric stack for low-voltage operation in non-volatile memory.

PubMed

Yang, Shiqian; Wang, Qin; Zhang, Manhong; Long, Shibing; Liu, Jing; Liu, Ming

2010-06-18

Titanium-tungsten nanocrystals (NCs) were fabricated by a self-assembly rapid thermal annealing (RTA) process. Well isolated Ti(0.46)W(0.54) NCs were embedded in the gate dielectric stack of SiO(2)/Al(2)O(3). A metal-oxide-semiconductor (MOS) capacitor was fabricated to investigate its application in a non-volatile memory (NVM) device. It demonstrated a large memory window of 6.2 V in terms of flat-band voltage (V(FB)) shift under a dual-directional sweeping gate voltage of - 10 to 10 V. A 1.1 V V(FB) shift under a low dual-directional sweeping gate voltage of - 4 to 4 V was also observed. The retention characteristic of this MOS capacitor was demonstrated by a 0.5 V memory window after 10(4) s of elapsed time at room temperature. The endurance characteristic was demonstrated by a program/erase cycling test.

The 129Xe nuclear shielding surfaces for Xe interacting with linear molecules CO2, N2, and CO

NASA Astrophysics Data System (ADS)

de Dios, Angel C.; Jameson, Cynthia J.

1997-09-01

We have calculated the intermolecular nuclear magnetic shielding surfaces for 129Xe in the systems Xe-CO2, Xe-N2, and Xe-CO using a gauge-invariant ab initio method at the coupled Hartree-Fock level with gauge-including atomic orbitals (GIAO). Implementation of a large basis set (240 basis functions) on the Xe gives very small counterpoise corrections which indicates that the basis set superposition errors in the calculated shielding values are negligible. These are the first intermolecular shielding surfaces for Xe-molecule systems. The surfaces are highly anisotropic and can be described adequately by a sum of inverse even powers of the distance with explicit angle dependence in the coefficients expressed by Legendre polynomials P2n(cos θ), n=0-3, for Xe-CO2 and Xe-N2. The Xe-CO shielding surface is well described by a similar functional form, except that Pn(cos θ), n=0-4 were used. When averaged over the anisotropic potential function these shielding surfaces provide the second virial coefficient of the nuclear magnetic resonance (NMR) chemical shift observed in gas mixtures. The energies from the self-consistent field (SCF) calculations were used to construct potential surfaces, using a damped dispersion form. These potential functions are compared with existing potentials in their predictions of the second virial coefficients of NMR shielding, the pressure virial coefficients, the density coefficient of the mean-square torque from infrared absorption, and the rotational constants and other average properties of the van der Waals complexes. Average properties of the van der Waals complexes were obtained by quantum diffusion Monte Carlo solutions of the vibrational motion using the various potentials and compared with experiment.

Pseudopotential SCF-MO studies of hypervalent compounds. II. XeF+5 and XeF6

NASA Astrophysics Data System (ADS)

Rothman, Michael J.; Bartell, Lawrence S.; Ewig, Carl S.; Van Wazer, John R.

1980-07-01

New evidence bearing upon the anomalous properties of xenon hexafluoride has been obtained via the ab initio molecular orbital approach applied successfully to the di- and tetrafluorides in paper I. Structures of both XeF+5 and XeF6 are governed by a stereochemically active lone pair. In the case of the square-pyramidal cation the Fax-Xe-Feq angle calculated for the bare ion is within 2° of the value observed in the crystalline complex. For the hexafluoride, however, the calculated deformation from Oh symmetry is appreciably greater than that deduced from electron diffraction intensities. Nevertheless, the results of calculations are in sufficient conformity with the Bartell-Gavin, Pitzer-Bernstein interpretation and at variance with the ''electronic-isomers'' interpretation to leave little doubt about the answer. With increasing fluorination in the XeFn series the HOMO-LUMO energy difference decreases and the second-order Jahn-Teller effect is enhanced. Increasing fluorination (and increased positive charge on Xe) also shortens bond lengths; calculated shortenings parallel observed shortenings. The deformation of XeF6 from Oh is along t1u bend and stretch coordinates to a C3v structure with long bonds adjacent to the lone pair, as expected according to the valence-shell-electron-pair-repulsion model. Pure t2g deformations are destabilizing but anharmonic t1u-t2g coupling significantly stabilizes the deformation. Steric aspects of the structure and force field are diagnosed and found to be minor. Values for the force constants f44, f55, f¯4444, f¯444'4', and f¯445 are derived and found to be of the magnitude forecast in the Bartell-Gavin and Pitzer-Bernstein treatments except that the calculations do not reproduce the delicate balances believed to lead to almost free pseudorotation in XeF6.

Surface chemical modification of nanocrystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Helms, Brett Anthony; Milliron, Delia Jane; Rosen, Evelyn Louise

Nanocrystals comprising organic ligands at surfaces of the plurality of nanocrystals are provided. The organic ligands are removed from the surfaces of the nanocrystals using a solution comprising a trialkyloxonium salt in a polar aprotic solvent. The removal of the organic ligands causes the nanocrystals to become naked nanocrystals with cationic surfaces.

Nanocrystal floating gate memory with solution-processed indium-zinc-tin-oxide channel and colloidal silver nanocrystals

NASA Astrophysics Data System (ADS)

Hu, Quanli; Ha, Sang-Hyub; Lee, Hyun Ho; Yoon, Tae-Sik

2011-12-01

A nanocrystal (NC) floating gate memory with solution-processed indium-zinc-tin-oxide (IZTO) channel and silver (Ag) NCs embedded in thin gate dielectric layer (SiO2(30 nm)/Al2O3(3 nm)) was fabricated. Both the IZTO channel and colloidal Ag NC layers were prepared by spin-coating and subsequent annealing, and dip-coating process, respectively. A threshold voltage shift up to ~0.9 V, corresponding to the electron density of 6.5 × 1011 cm-2, at gate pulsing <=10 V was achieved by the charging of high density NCs. These results present the successful non-volatile memory characteristics of an oxide-semiconductor transistor fabricated through solution processes.

White up-conversion emission in Ho3+/Tm3+/Yb3+ tri-doped glass ceramics embedding BaF2 nanocrystals

NASA Astrophysics Data System (ADS)

Li, Chenxia; Xu, Shiqing; Ye, Rengguang; Deng, Degang; Hua, Youjie; Zhao, Shilong; Zhuang, Songlin

2011-04-01

Ho3+/Tm3+/Yb3+ tri-doped glass ceramics with white light emitting have been developed and demonstrated. Pumped by 980 nm laser diode (LD), intensive red, green and blue up-conversions (UC) were obtained. The green emission is assigned to Ho3+ ion and the blue emission is assigned to Tm3+ ion, whereas the red emission is the combination contribution of the Ho3+ and Tm3+ ions. The RGB intensities could be adjusted by tuning the rare-earth ion concentration and pump power intensity. Thus, multicolor of the luminescence, including perfect white light with CIE-X=0.329 and CIE-Y=0.342 in the 1931 CIE chromaticity diagram can be obtained in 0.15 Ho3+/0.2Tm3+/3Yb3+ tri-doped glass ceramics embedding BaF2 nanocrystals pumped by a single infrared laser diode source of 980 nm at 500 mW. The up-conversion luminescence mechanism of Yb3+ sensitize Ho3+ and Tm3+ ions and the energy transfer from Ho3+ to Tm3+ in oxy-fluoride silicate glass ceramics were analyzed.

Molecular dynamics averaging of Xe chemical shifts in liquids.

PubMed

Jameson, Cynthia J; Sears, Devin N; Murad, Sohail

2004-11-15

The Xe nuclear magnetic resonance chemical shift differences that afford the discrimination between various biological environments are of current interest for biosensor applications and medical diagnostic purposes. In many such environments the Xe signal appears close to that in water. We calculate average Xe chemical shifts (relative to the free Xe atom) in solution in eleven liquids: water, isobutane, perfluoro-isobutane, n-butane, n-pentane, neopentane, perfluoroneopentane, n-hexane, n-octane, n-perfluorooctane, and perfluorooctyl bromide. The latter is a liquid used for intravenous Xe delivery. We calculate quantum mechanically the Xe shielding response in Xe-molecule van der Waals complexes, from which calculations we develop Xe (atomic site) interpolating functions that reproduce the ab initio Xe shielding response in the complex. By assuming additivity, these Xe-site shielding functions can be used to calculate the shielding for any configuration of such molecules around Xe. The averaging over configurations is done via molecular dynamics (MD). The simulations were carried out using a MD technique that one of us had developed previously for the simulation of Henry's constants of gases dissolved in liquids. It is based on separating a gaseous compartment in the MD system from the solvent using a semipermeable membrane that is permeable only to the gas molecules. We reproduce the experimental trends in the Xe chemical shifts in n-alkanes with increasing number of carbons and the large chemical shift difference between Xe in water and in perfluorooctyl bromide. We also reproduce the trend for a given solvent of decreasing Xe chemical shift with increasing temperature. We predict chemical shift differences between Xe in alkanes vs their perfluoro counterparts.

Syntheses, Raman spectra, and X-ray crystal structures of [XeF(5)][mu-F(OsO(3)F(2))(2)] and [M][OsO(3)F(3)] (M = XeF(5)(+), Xe(2)F(11)(+)).

PubMed

Hughes, Michael J; Mercier, Hélène P A; Schrobilgen, Gary J

2010-04-05

Stoichiometric amounts of XeF(6) and (OsO(3)F(2))(infinity) react at 25-50 degrees C to form salts of the known XeF(5)(+) and Xe(2)F(11)(+) cations, namely, [XeF(5)][mu-F(OsO(3)F(2))(2)], [XeF(5)][OsO(3)F(3)], and [Xe(2)F(11)][OsO(3)F(3)]. Although XeF(6) is oxophilic toward a number of transition metal and main-group oxides and oxide fluorides, fluoride/oxide metathesis was not observed. The series provides the first examples of noble-gas cations that are stabilized by metal oxide fluoride anions and the first example of a mu-F(OsO(3)F(2))(2)(-) salt. Both [XeF(5)][mu-F(OsO(3)F(2))(2)] and [Xe(2)F(11)][OsO(3)F(3)] are orange solids at room temperature. The [XeF(5)][OsO(3)F(3)] salt is an orange liquid at room temperature that solidifies at 5-0 degrees C. When the salts are heated at 50 degrees C under 1 atm of N(2) for more than 2 h, significant XeF(6) loss occurs. The X-ray crystal structures (-173 degrees C) show that the salts exist as discrete ion pairs and that the osmium coordination spheres in OsO(3)F(3)(-) and mu-F(OsO(3)F(2))(2)(-) are pseudo-octahedral OsO(3)F(3)-units having facial arrangements of oxygen and fluorine atoms. The mu-F(OsO(3)F(2))(2)(-) anion is comprised of two symmetry-related OsO(3)F(2)-groups that are fluorine-bridged to one another. Ion pairing results from secondary bonding interactions between the fluorine/oxygen atoms of the anions and the xenon atom of the cation, with the Xe...F/O contacts occurring opposite the axial fluorine and from beneath the equatorial XeF(4)-planes of the XeF(5)(+) and Xe(2)F(11)(+) cations so as to avoid the free valence electron lone pairs of the xenon atoms. The xenon atoms of [XeF(5)][mu-F(OsO(3)F(2))(2)] and [Xe(2)F(11)][OsO(3)F(3)] are nine-coordinate and the xenon atom of [XeF(5)][OsO(3)F(3)] is eight-coordinate. Quantum-chemical calculations at SVWN and B3LYP levels of theory were used to obtain the gas-phase geometries, vibrational frequencies, and NBO bond orders, valencies, and NPA charges of

Toward calculations of the 129Xe chemical shift in Xe@C60 at experimental conditions: relativity, correlation, and dynamics.

PubMed

Straka, Michal; Lantto, Perttu; Vaara, Juha

2008-03-27

We calculate the 129Xe chemical shift in endohedral Xe@C60 with systematic inclusion of the contributing physical effects to model the real experimental conditions. These are relativistic effects, electron correlation, the temperature-dependent dynamics, and solvent effects. The ultimate task is to obtain the right result for the right reason and to develop a physically justified methodological model for calculations and simulations of endohedral Xe fullerenes and other confined Xe systems. We use the smaller Xe...C6H6 model to calibrate density functional theory approaches against accurate correlated wave function methods. Relativistic effects as well as the coupling of relativity and electron correlation are evaluated using the leading-order Breit-Pauli perturbation theory. The dynamic effects are treated in two ways. In the first approximation, quantum dynamics of the Xe atom in a rigid cage takes advantage of the centrosymmetric potential for Xe within the thermally accessible distance range from the center of the cage. This reduces the problem of obtaining the solution of a diatomic rovibrational problem. In the second approach, first-principles classical molecular dynamics on the density functional potential energy hypersurface is used to produce the dynamical trajectory for the whole system, including the dynamic cage. Snapshots from the trajectory are used for calculations of the dynamic contribution to the absorption 129Xe chemical shift. The calculated nonrelativistic Xe shift is found to be highly sensitive to the optimized molecular structure and to the choice of the exchange-correlation functional. Relativistic and dynamic effects are significant and represent each about 10% of the nonrelativistic static shift at the minimum structure. While the role of the Xe dynamics inside of the rigid cage is negligible, the cage dynamics turns out to be responsible for most of the dynamical correction to the 129Xe shift. Solvent effects evaluated with a polarized

Temperature profiles for laser-induced heating of nanocrystals embedded in glass matrices

NASA Astrophysics Data System (ADS)

Bhatnagar, Promod K.; Nagpal, Swati

2001-05-01

Quantum confined nanostructures are very important because of their application towards optoelectronic devices. Commercial colored glass filters, which have large semiconductor particles, are being used to manufacture nanocrystals by suitable heat treatments. The progress in this area has been hampered by high size dispersion of these dots in the glass matrix which leads to reduction in higher order susceptibility thereby reducing non-linearity. In the present paper attempt has been made to theoretically model the temperature profiles of a laser irradiated CdS doped Borosilicate sample. Laser being used has a beam diameter of 1.5 mm and energy for 10 nsec pulse is 10 mJ. Two different particle radii of 5 nm and 10 nm have been considered. It is found that larger particles reach higher temperatures for the same pulse characteristics. This is because smaller particles have larger surface to volume ratio and hence dissipates out heat faster to the surrounding. Hence bigger particles will reach dissolution temperature faster than smaller particle and particle beyond a certain size should dissolve in the glass matrix when a sample is heat treated by laser. This could lead to a reduction in size dispersion of the nanocrystals. Also photodarkening effect found in semiconductor doped glasses is a big handicap for practical application of these materials in fast optical switching and non-linear optical devices. Photodarkening effect has been established to be a photochemical effect and it is important to study the temperature profiles around a particle since it will effect the impurity migration.

Synthesis and Study of Fe-Doped Bi₂S₃ Semimagnetic Nanocrystals Embedded in a Glass Matrix.

PubMed

Silva, Ricardo S; Mikhail, Hanna D; Guimarães, Eder V; Gonçalves, Elis R; Cano, Nilo F; Dantas, Noelio O

2017-07-11

Iron-doped bismuth sulphide (Bi 2- x Fe x S₃) nanocrystals have been successfully synthesized in a glass matrix using the fusion method. Transmission electron microscopy images and energy dispersive spectroscopy data clearly show that nanocrystals are formed with an average diameter of 7-9 nm, depending on the thermic treatment time, and contain Fe in their chemical composition. Magnetic force microscopy measurements show magnetic phase contrast patterns, providing further evidence of Fe incorporation in the nanocrystal structure. The electron paramagnetic resonance spectra displayed Fe 3+ typical characteristics, with spin of 5/2 in the 3d⁵ electronic state, thereby confirming the expected trivalent state of Fe ions in the Bi₂S₃ host structure. Results from the spin polarized density functional theory simulations, for the bulk Fe-doped Bi₂S₃ counterpart, corroborate the experimental fact that the volume of the unit cell decreases with Fe substitutionally doping at Bi1 and Bi2 sites. The Bader charge analysis indicated a pseudo valency charge of 1.322| e | on Fe Bi ₁ and 1.306| e | on Fe Bi ₂ ions, and a spin contribution for the magnetic moment of 5.0 µ B per unit cell containing one Fe atom. Electronic band structures showed that the (indirect) band gap changes from 1.17 eV for Bi₂S₃ bulk to 0.71 eV (0.74 eV) for Bi₂S₃:Fe Bi1 (Bi₂S₃:Fe Bi2 ). These results are compatible with the 3d⁵ high-spin state of Fe 3+ , and are in agreement with the experimental results, within the density functional theory accuracy.

Living Nanocrystals: Synthesis of Precisely Defined Metal Oxide Nanocrystals Through a Continuous Growth Process

NASA Astrophysics Data System (ADS)

Jansons, Adam Wayne

Colloidal nanocrystals offer new and improved performance in applications as well as less environmental impact when compared to traditional device fabrication methods. The important properties that enable improved applications are a direct result of nanocrystal structure. While there have been many great advances in the production of colloidal nanocrystals over the past three decades, precise, atomic-level control of the size, composition, and structure of the inorganic core remains challenging. Rather than dictate these material aspects through traditional synthetic routes, this dissertation details the development and exploitation of a colloidal nanocrystal synthetic method inspired by polymerization reactions. Living polymerization reactions offer precise control of polymer size and structure and have tremendously advanced polymer science, allowing the intuitive production of polymers and block co-polymers of well-defined molecular weights. Similarly, living nanocrystal synthetic methods allow an enhanced level of structural control, granting the synthesis of binary, doped, and core/shell nanocrystals of well-defined size, composition, and structure. This improved control in turn grants enhanced nanocrystal property performance and deepens our understanding of structure/property relationships. This dissertation defines living nanocrystal growth and demonstrates the potential of the living methods in the colloidal production of oxide nanocrystals. After a brief introduction, living growth is defined and discussed in the context of synthetic prerequisites, attributes, and outcomes. Living growth is also compared to more traditional colloidal nanocrystal synthetic methods. The following chapters then demonstrate the precise control living approaches offer in three separate studies; the first highlights sub-nanometer control of nanocrystal size from 2-22+ nm in diameter. Next the improvement in nanocrystal composition is illustrated using several transition metal

Nanocrystal/sol-gel nanocomposites

DOEpatents

Klimov, Victor L.; Petruska, Melissa A.

2010-05-25

The present invention is directed to a process for preparing a solid composite having colloidal nanocrystals dispersed within a sol-gel matrix, the process including admixing colloidal nanocrystals with an amphiphilic polymer including hydrophilic groups selected from the group consisting of --COOH, --OH, --SO.sub.3H, --NH.sub.2, and --PO.sub.3H.sub.2 within a solvent to form an alcohol-soluble colloidal nanocrystal-polymer complex, admixing the alcohol-soluble colloidal nanocrystal-polymer complex and a sol-gel precursor material, and, forming the solid composite from the admixture. The present invention is also directed to the resultant solid composites and to the alcohol-soluble colloidal nanocrystal-polymer complexes.

A room-temperature-operated Si LED with β-FeSi2 nanocrystals in the active layer: μW emission power at 1.5 μm

NASA Astrophysics Data System (ADS)

Shevlyagin, A. V.; Goroshko, D. L.; Chusovitin, E. A.; Balagan, S. A.; Dotsenko, S. A.; Galkin, K. N.; Galkin, N. G.; Shamirzaev, T. S.; Gutakovskii, A. K.; Latyshev, A. V.; Iinuma, M.; Terai, Y.

2017-03-01

This article describes the development of an Si-based light-emitting diode with β-FeSi2 nanocrystals embedded in the active layer. Favorable epitaxial conditions allow us to obtain a direct band gap type-I band alignment Si/β-FeSi2 nanocrystals/Si heterostructure with optical transition at a wavelength range of 1500-1550 nm at room temperature. Transmission electron microscopy data reveal strained, defect-free β-FeSi2 nanocrystals of diameter 6 and 25 nm embedded in the Si matrix. Intense electroluminescence was observed at a pumping current density as low as 0.7 A/cm2. The device reached an optical emission power of up to 25 μW at 9 A/cm2 with an external quantum efficiency of 0.009%. Watt-Ampere characteristic linearity suggests that the optical power margin of the light-emitting diode has not been exhausted. Band structure calculations explain the luminescence as being mainly due to radiative recombination in the large β-FeSi2 nanocrystals resulting from the realization of an indirect-to-direct band gap electronic configuration transformation arising from a favorable deformation of nanocrystals. The direct band gap structure and the measured short decay time of the luminescence of several tens of ns give rise to a fast operation speed for the device. Thus a method for developing a silicon-based photonic integrated circuit, combining complementary metal-oxide-semiconductor technology functionality and near-infrared light emission, is reported here.

Nanocrystals Technology for Pharmaceutical Science.

PubMed

Cheng, Zhongyao; Lian, Yumei; Kamal, Zul; Ma, Xin; Chen, Jianjun; Zhou, Xinbo; Su, Jing; Qiu, Mingfeng

2018-05-17

Nanocrystals technology is a promising method for improving the dissolution rate and enhancing the bioavailability of poorly soluble drugs. In recent years, it has been developing rapidly and applied to drug research and engineering. Nanocrystal drugs can be formulated into various dosage forms. This review mainly focused on the nanocrystals technology and its application in pharmaceutical science. Firstly, different preparation methods of nanocrystal technology and the characterization of nanocrystal drugs are briefly described. Secondly, the application of nanocrystals technology in pharmaceutical science is mainly discussed followed by the introduction of sustained release formulations. Then, the scaling up process, marketed nanocrystal drug products and regulatory aspects about nanodrugs are summarized. Finally, the specific challenges and opportunities of nanocrystals technology for pharmaceutical science are summarized and discussed. This review will provide a comprehensive guide for scientists and engineers in the field of pharmaceutical science and biochemical engineering. Copyright© Bentham Science Publishers; For any queries, please email at epub@benthamscience.org.

Fabrication of all-inorganic nanocrystal solids through matrix encapsulation of nanocrystal arrays.

PubMed

Kinder, Erich; Moroz, Pavel; Diederich, Geoffrey; Johnson, Alexa; Kirsanova, Maria; Nemchinov, Alexander; O'Connor, Timothy; Roth, Dan; Zamkov, Mikhail

2011-12-21

A general strategy for low-temperature processing of colloidal nanocrystals into all-inorganic films is reported. The present methodology goes beyond the traditional ligand-interlinking scheme and relies on encapsulation of morphologically defined nanocrystal arrays into a matrix of a wide-band gap semiconductor, which preserves optoelectronic properties of individual nanoparticles while rendering the nanocrystal film photoconductive. Fabricated solids exhibit excellent thermal stability, which is attributed to the heteroepitaxial structure of nanocrystal-matrix interfaces, and show compelling light-harvesting performance in prototype solar cells. © 2011 American Chemical Society

Energy Transfer Efficiency from ZnO-Nanocrystals to Eu3+ Ions Embedded in SiO₂ Film for Emission at 614 nm.

PubMed

Mangalam, Vivek; Pita, Kantisara

2017-08-10

In this work, we study the energy transfer mechanism from ZnO nanocrystals (ZnO-nc) to Eu 3+ ions by fabricating thin-film samples of ZnO-nc and Eu 3+ ions embedded in a SiO₂ matrix using the low-cost sol-gel technique. The time-resolved photoluminescence (TRPL) measurements from the samples were analyzed to understand the contribution of energy transfer from the various ZnO-nc emission centers to Eu 3+ ions. The decay time obtained from the TRPL measurements was used to calculate the energy transfer efficiencies from the ZnO-nc emission centers, and these results were compared with the energy transfer efficiencies calculated from steady-state photoluminescence emission results. The results in this work show that high transfer efficiencies from the excitonic and Zn defect emission centers is mostly due to the energy transfer from ZnO-nc to Eu 3+ ions which results in the radiative emission from the Eu 3+ ions at 614 nm, while the energy transfer from the oxygen defect emissions is most probably due to the energy transfer from ZnO-nc to the new defects created due to the incorporation of the Eu 3+ ions.

Magneto-optical Faraday rotation of semiconductor nanoparticles embedded in dielectric matrices.

PubMed

Savchuk, Andriy I; Stolyarchuk, Ihor D; Makoviy, Vitaliy V; Savchuk, Oleksandr A

2014-04-01

Faraday rotation has been studied for CdS, CdTe, and CdS:Mn semiconductor nanoparticles synthesized by colloidal chemistry methods. Additionally these materials were prepared in a form of semiconductor nanoparticles embedded in polyvinyl alcohol films. Transmission electron microscopy and atomic force microscopy analyses served as confirmation of nanocrystallinity and estimation of the average size of the nanoparticles. Spectral dependence of the Faraday rotation for the studied nanocrystals and nanocomposites is correlated with a blueshift of the absorption edge due to the confinement effect in zero-dimensional structures. Faraday rotation spectra and their temperature behavior in Mn-doped nanocrystals demonstrates peculiarities, which are associated with s, p-d exchange interaction between Mn²⁺ ions and band carriers in diluted magnetic semiconductor nanostructures.

SEP-Kr and SEP-Xe in Lunar Ilmenite and the Ar/Kr/Xe Ratio in the Solar Wind

NASA Astrophysics Data System (ADS)

Wieler, R.; Baur, H.; Signer, P.

1992-07-01

We analyzed all five noble gases in an ilmenite sample from lunar soil 71501 by closed system stepped etching (CSSE), thus extending our CSSE studies of solar noble gases (Wieler et al., 1986; Benkert et al., 1988) to Kr and Xe. He, Ne, Ar isotopes: We observe the familiar presence of two solar noble gas components: step 1 shows ^4He/^3He = 2250, ^20Ne/^22Ne = 13.8, and ^36Ar/^38Ar=5.46. The first two ratios are essentially identical to modern solar wind values (SWC; Geiss, 1973), indicating an isotopically unfractionated SW noble gas reservoir in lunar ilmenite. The Ne data-points of later steps fall on a straight line and reach the SEP-Ne point (^20Ne/^22Ne = 11.3). The slope of this line indicates mass dependent fractionation between SW-Ne and SEP-Ne. SEP-He (^4He/^3He = 4650 +-100) and SEP-Ar (^36Ar/^38Ar = 4.89+-0.05) are also observed (latter two numbers slightly revised compared to Wieler et al., 1992). Kr, Xe isotopes: Kr in those two steps that release pure SW-Ne is very slightly lighter than atmospheric Kr (^86Kr/^84Kr = 0.3041; see also Wieler et al., 1992). We interpret this to be SW-Kr in soil 71501. Steps containing (isotopically heavier) SEP-Ne likewise release heavier Kr, interpreted accordingly as SEP-Kr (^86Kr/^84Kr = 0.323). Similarly, a light Xe component is released first (SW-Xe, ^136Xe/^132Xe = 0.3003), followed by heavier SEP-Xe (^136Xe/^132Xe = 0.319). The data are consistent with both Kr and Xe in SW and SEP components to be related by mass fractionation. The relation first proposed by Benkert et al. (1988) between a ratio R(m(sub)2,m(sub)1) of two isotopes with masses m(sub)2>m(sub)1 in SW and SEP now holds for all five noble gases: (R(sub)SW-R(sub)SEP)/R(sub)SW = (2+-0.13)*(m(sub)2- m(sub)1)/m(sub)2. Since m(sub)2~m(sub)1, this relation may also be written as: R(sub)SEP/R(sub)SW ~ (m(sub)1/m(sub)2)^2 (Geiss and Bochsler, 1991). Element ratios: ^4He/^36Ar and ^20Ne/^36Ar rise from values several times below SWC to essentially SWC ratios in

Silicon nanocrystal inks, films, and methods

DOEpatents

Wheeler, Lance Michael; Kortshagen, Uwe Richard

2015-09-01

Silicon nanocrystal inks and films, and methods of making and using silicon nanocrystal inks and films, are disclosed herein. In certain embodiments the nanocrystal inks and films include halide-terminated (e.g., chloride-terminated) and/or halide and hydrogen-terminated nanocrystals of silicon or alloys thereof. Silicon nanocrystal inks and films can be used, for example, to prepare semiconductor devices.

Unified random access memory (URAM) by integration of a nanocrystal floating gate for nonvolatile memory and a partially depleted floating body for capacitorless 1T-DRAM

NASA Astrophysics Data System (ADS)

Ryu, Seong-Wan; Han, Jin-Woo; Kim, Chung-Jin; Kim, Sungho; Choi, Yang-Kyu

2009-03-01

This paper describes a unified memory (URAM) that utilizes a nanocrystal SOI MOSFET for multi-functional applications of both nonvolatile memory (NVM) and capacitorless 1T-DRAM. By using a discrete storage node (Ag nanocrystal) as the floating gate of the NVM, high defect immunity and 2-bit/cell operation were achieved. The embedded nanocrystal NVM also showed 1T-DRAM operation (program/erase time = 100 ns) characteristics, which were realized by storing holes in the floating body of the SOI MOSFET, without requiring an external capacitor. Three-bit/cell operation was accomplished for different applications - 2-bits for nonvolatility and 1-bit for fast operation.

Fenofibrate Nanocrystals Embedded in Oral Strip-Films for Bioavailability Enhancement

PubMed Central

Barvaliya, Manish; Zhang, Lu; Anovadiya, Ashish; Brahmbhatt, Harshad; Paul, Parimal; Tripathi, Chandrabhanu

2018-01-01

The aim of the present study was to make a fenofibrate (FNB) nanocrystal (NC) by wet media milling, characterizations and formulates into oral strip-films (OSFs). Mechanical properties, redispersion study, and solid-state characterizations results suggested that reduction of drug crystal size at nanoscale and incorporation into OSFs does not affect the solid-state properties of the drug. In vitro dissolution kinetics showed enhanced dissolution rate was easily manipulated by changing the thickness of the OSF. In situ UV-imaging was used to monitor drug dissolution qualitatively and quantitatively in real time. Results confirm that the intrinsic dissolution rates and surface drug concentration measured with this device were in agreement with the USP-IV dissolution profiles. In vivo pharmacokinetics in rabbits showed a significant difference in the pharmacokinetics parameter (1.4 fold increase bioavailability) of FNB NC-loaded OSFs as compared to the marketed formulation “Tricor” and as-received (pristine) drug. This approach of drug nanocrystallization and incorporation into OSFs may have significant applications in cost-effective tools for bioavailability enhancement of FNB. PMID:29438297

Production of pure 133mXe for CTBTO

NASA Astrophysics Data System (ADS)

Peräjärvi, K.; Eronen, T.; Gorelov, D.; Hakala, J.; Jokinen, A.; Kettunen, H.; Kolhinen, V.; Laitinen, M.; Moore, I. D.; Penttilä, H.; Rissanen, J.; Saastamoinen, A.; Toivonen, H.; Turunen, J.; Äystö, J.

2014-01-01

Underground nuclear weapon detonations release gaseous species into the atmosphere. The most interesting isotopes/isomers from the detection point of view are 131mXe, 133mXe, 133Xe and 135Xe. We have developed a method that employs high-precision Penning trap mass spectrometry at the JYFLTRAP facility, the University of Jyväskylä, to produce pure calibration samples of these isotopes/isomers. Among developments this work required a new mass resolution record of a few parts-per-million. Here the status and future plans of the project are reviewed.

I-Xe Dating: Comparison of I-Xe and Pb-Pb Ages of Richardton Chondrules and Separated Mineral Phases

NASA Technical Reports Server (NTRS)

Pravdivtseva, O. V.; Amelin, Y.; Hohenberg, C. M.; Meshik, A. P.

2002-01-01

I-Xe and Pb-Pb ages of individual Richardton chondrules and different mineral phases were compared in order to test the absolute I-Xe age normalization. Additional information is contained in the original extended abstract.

Thermomechanical Properties of Lignin-Based Electrospun Nanofibers and Films Reinforced with Cellulose Nanocrystals: A Dynamic Mechanical and Nanoindentation Study

Treesearch

Mariko Ago; Joseph E. Jakes; Orlando J. Rojas

2013-01-01

We produced defect-free electrospun fibers from aqueous dispersions of lignin, poly(vinyl alcohol) (PVA), and cellulose nanocrystals (CNCs), which were used as reinforcing nanoparticles. The thermomechanical performance of the lignin-based electrospun fibers and the spin-coated thin films was improved when they were embedded with CNCs. Isochronal dynamic mechanical...

Atomistic simulation of the thermal conductivity in amorphous SiO2 matrix/Ge nanocrystal composites

NASA Astrophysics Data System (ADS)

Kuryliuk, Vasyl V.; Korotchenkov, Oleg A.

2017-04-01

We use nonequilibrium molecular dynamics computer simulations with the Tersoff potential aiming to provide a comprehensive picture of the thermal conductivity of amorphous SiO2 (a-SiO2) matrix with embedded Ge nanocrystals (nc-Ge). The modelling predicts the a-SiO2 matrix thermal conductivity in a temperature range of 50 < T < 500 K yielding a fair agreement with experiment at around room temperature. It is worth noticing that the predicted room-temperature thermal conductivity in a-SiO2 is in very good agreement with the experimental result, which is in marked contrast with the thermal conductivity calculated employing the widely used van Beest-Kramer-van Santen (BKS) potential. We show that the thermal conductivity of composite nc-Ge/a-SiO2 systems decreases steadily with increasing the volume fraction of Ge inclusions, indicative of enhanced interface scattering of phonons imposed by embedded Ge nanocrystals. We also observe that increasing the volume fractions above a certain threshold value results in a progressively increased thermal conductivity of the nanocomposite, which can be explained by increasing volume fraction of a better thermally conducting Ge. Finally, non-equilibrium molecular dynamics simulations with the Tersoff potential are promising for computing the thermal conductivity of nanocomposites based on amorphous SiO2 and can be readily scaled to more complex composite structures with embedded nanoparticles, which thus help design nanocomposites with desired thermal properties.

Temperature-Ramped 129Xe Spin-Exchange Optical Pumping

PubMed Central

2015-01-01

We describe temperature-ramped spin-exchange optical pumping (TR-SEOP) in an automated high-throughput batch-mode 129Xe hyperpolarizer utilizing three key temperature regimes: (i) “hot”—where the 129Xe hyperpolarization rate is maximal, (ii) “warm”—where the 129Xe hyperpolarization approaches unity, and (iii) “cool”—where hyperpolarized 129Xe gas is transferred into a Tedlar bag with low Rb content (<5 ng per ∼1 L dose) suitable for human imaging applications. Unlike with the conventional approach of batch-mode SEOP, here all three temperature regimes may be operated under continuous high-power (170 W) laser irradiation, and hyperpolarized 129Xe gas is delivered without the need for a cryocollection step. The variable-temperature approach increased the SEOP rate by more than 2-fold compared to the constant-temperature polarization rate (e.g., giving effective values for the exponential buildup constant γSEOP of 62.5 ± 3.7 × 10–3 min–1 vs 29.9 ± 1.2 × 10–3 min–1) while achieving nearly the same maximum %PXe value (88.0 ± 0.8% vs 90.1% ± 0.8%, for a 500 Torr (67 kPa) Xe cell loading—corresponding to nuclear magnetic resonance/magnetic resonance imaging (NMR/MRI) enhancements of ∼3.1 × 105 and ∼2.32 × 108 at the relevant fields for clinical imaging and HP 129Xe production of 3 T and 4 mT, respectively); moreover, the intercycle “dead” time was also significantly decreased. The higher-throughput TR-SEOP approach can be implemented without sacrificing the level of 129Xe hyperpolarization or the experimental stability for automation—making this approach beneficial for improving the overall 129Xe production rate in clinical settings. PMID:25008290

Photoionization and Photofragmentation of the Endohedral Xe C60+ Molecular Ion

NASA Astrophysics Data System (ADS)

Aryal, Nagendra Bahadur

An experimental study of photoionization and fragmentation of the Xe C 60+ endohedral molecular ion is presented in the photon energy range of the well-known Xe 4d giant resonance, and evidence of redistribution of the Xe 4d oscillator strength in photon energy due to multipath interference is reported. Experiments were conducted at undulator beamline 10.0.1 of the Advanced Light Source (ALS) using the merged-beams technique. Prior to these measurements, macroscopic samples containing endohedral Xe C60 were prepared using a setup developed at the ALS. Endohedral Xe C60 yields as high as 2.5x10 -4 were synthesized and a pure Xe C60+ ion beam current of up to 5.5 pA was obtained for the merged-beams experiments. Cross sections were measured in the photon energy range 60 - 150 eV in 0.5 eV steps for single, double, and triple photoionization of endohedral Xe C 60+ accompanied by the loss of n pairs of carbon atoms yielding Xe C60-2n2+ (n = 0, 1), Xe C60-2n 3+ (n = 0, 1, 2, 3), and Xe C584+ photoion products. Reference absolute cross-section measurements were made for empty C60+ for the corresponding reaction channels. The spectroscopic measurements with Xe C60+ were placed onto an absolute scale by normalization to the reference cross sections for C60+ in ranges of photon energies where the Xe 4d contributions were negligible. Results for single photoionization and fragmentation of Xe C60+ show no evidence of the presence of the caged Xe atom. The measurements of double and triple photoionization with fragmentation of Xe C60+ exhibit prominent signatures of the Xe 4d resonance and together account for 6.6 +/- 1.5 of the total Xe 4d oscillator strength of 10. Compared to that for a free Xe atom, the Xe oscillator strength in Xe C60+ is redistributed in photon energy due to multipath interference of outgoing Xe 4d photoelectron waves that may be transmitted or reflected by the spherical C60+ molecular cage, yielding so-called confinement resonances. The experimental

Semiconductor nanocrystal-based phagokinetic tracking

DOEpatents

Alivisatos, A Paul; Larabell, Carolyn A; Parak, Wolfgang J; Le Gros, Mark; Boudreau, Rosanne

2014-11-18

Methods for determining metabolic properties of living cells through the uptake of semiconductor nanocrystals by cells. Generally the methods require a layer of neutral or hydrophilic semiconductor nanocrystals and a layer of cells seeded onto a culture surface and changes in the layer of semiconductor nanocrystals are detected. The observed changes made to the layer of semiconductor nanocrystals can be correlated to such metabolic properties as metastatic potential, cell motility or migration.

About 129Xe ∗ in meteoritic nanodiamonds

NASA Astrophysics Data System (ADS)

Fisenko, A. V.; Semjonova, L. F.

2008-08-01

The analysis of excess 129Xe in meteoritic nanodiamonds and the kinetics of its release during stepwise pyrolysis allow to suggest that (1) in the solar nebula 129I atoms were adsorbed onto nanodiamond grains and (or) chemisorbed by forming covalent bonds with carbon atoms. Most 129I atoms existed in a surface connected state, but a minor amount of them was in nanopores of the grains. At radioactive decay of 129I the formed 129Xe ( 129Xe ∗) was trapped by diamond grains due to nuclear recoil. (2) During thermal metamorphism or aqueous alteration, the surface-sited 129I atoms were basically lost. On the basis of these assumptions and calculated concentrations of 129Xe ∗ in meteoritic nanodiamonds it is shown that the minimum closing time of the I-Xe system for meteorites of different chemical classes and low petrologic types may be about one million years relative to the minimally thermally metamorphized CO3 meteorite ALHA 77307. With increasing metamorphic grade the closing time of the I-Xe system increases and can range up to several ten millions years. This tendency is in agreement with an onion-shell model of structure and cooling history of meteorite parent bodies where the temperature increases in the direction from surface to center of the asteroids.

Recoil distance lifetime measurements in 122,124Xe

NASA Astrophysics Data System (ADS)

Govil, I. M.; Kumar, A.; Iyer, H.; Li, H.; Garg, U.; Ghugre, S. S.; Johnson, T.; Kaczarowski, R.; Kharraja, B.; Naguleswaran, S.; Walpe, J. C.

1998-02-01

Lifetimes of the lower-excited states in 122,124Xe are measured using the recoil-distance Doppler-shift technique. The reactions 110Pd(16O,4n)122Xe and 110Pd(18O,4n)124Xe at a beam energy of 66 MeV were used for this experiment. The lifetimes of the 2+, 4+, 6+, and 8+ states of the ground state band were extracted using the computer code LIFETIME including the corrections due to the side feeding and the nuclear deorientation effects. The lifetime of the 2+ state in 122Xe agrees with the recoil distance method (RDM) measurements but for the 124Xe it does not agree with the RDM measurements but agrees with the Coulomb-excitation experiment. The measured B(E2) values for both the nuclei are compared with the standard algebraic and the multishell models.

NMR of laser-polarized 129Xe in blood foam

NASA Technical Reports Server (NTRS)

Tseng, C. H.; Peled, S.; Nascimben, L.; Oteiza, E.; Walsworth, R. L.; Jolesz, F. A.

1997-01-01

Laser-polarized 129Xe dissolved in a foam preparation of fresh human blood was investigated. The NMR signal of 129Xe dissolved in blood was enhanced by creating a foam in which the dissolved 129Xe exchanged with a large reservoir of gaseous laser-polarized 129Xe. The dissolved 129Xe T1 in this system was found to be significantly shorter in oxygenated blood than in deoxygenated blood. The T1 of 129Xe dissolved in oxygenated blood foam was found to be approximately 21 (+/-5) s, and in deoxygenated blood foam to be greater than 40 s. To understand the oxygenation trend, T1 measurements were also made on plasma and hemoglobin foam preparations. The measurement technique using a foam gas-liquid exchange interface may also be useful for studying foam coarsening and other liquid physical properties.

New constraints on Xe incorporation mechanisms in olivine from first-principles calculations

NASA Astrophysics Data System (ADS)

Crépisson, Céline; Blanchard, Marc; Lazzeri, Michele; Balan, Etienne; Sanloup, Chrystèle

2018-02-01

Storage of Xe at depth in silicate minerals has recently been proposed to explain the low Xe abundance in the Earth's and Mars' atmospheres compared to other noble gases (the so-called 'Missing Xenon' issue). Evidences for incorporation, and thus reactivity of Xe in olivine at high pressure and high temperature are based on variations in cell parameters and the appearance of a new Raman band. To constrain the, so far only hypothetical, Xe incorporation mechanism in olivine, we theoretically investigated models of Xe-bearing olivine using density functional theory. Three types of incorporation mechanisms are tested: Xe for Si and Xe for Mg substitutions, and interstitial Xe. Xe for Si substitution, implying an oxidation of Xe, is found to be the only mechanism consistent with experimental observations, leading to an increase of cell parameter a and the appearance of a new Raman band around 720-750 cm-1 associated with Xesbnd O stretching vibrations. Raman spectroscopy makes it possible to identify Xe incorporation site, even at low Xe content, due to high Xe polarizability. An estimation of Xe content in olivine, based on present work and previous in situ experimental results, shows that up to 0.4 at.% Xe could be stored in olivine at depth.

Silicon nanocrystals as handy biomarkers

NASA Astrophysics Data System (ADS)

Fujioka, Kouki; Hoshino, Akiyoshi; Manabe, Noriyoshi; Futamura, Yasuhiro; Tilley, Richard; Yamamoto, Kenji

2007-02-01

Quantum dots (QDs) have brighter and longer fluorescence than organic dyes. Therefore, QDs can be applied to biotechnology, and have capability to be applied to medical technology. Currently, among the several types of QDs, CdSe with a ZnS shell is one of the most popular QDs to be used in biological experiments. However, when the CdSe QDs were applied to clinical technology, potential toxicological problems due to CdSe core should be considered. To eliminate the problem, silicon nanocrystals, which have the potential of biocompatibility, could be a candidate of alternate probes. Silicon nanocrystals have been synthesized using several techniques such as aerosol, electrochemical etching, laser pyrolysis, plasma deposition, and colloids. Recently, the silicon nanocrystals were reported to be synthesized in inverse micelles and also stabilized with 1-heptene or allylamine capping. Blue fluorescence of the nanocrystals was observed when excited with a UV light. The nanocrystals covered with 1-heptene are hydrophobic, whereas the ones covered with allylamine are hydrophilic. To test the stability in cytosol, the water-soluble nanocrystals covered with allylamine were examined with a Hela cell incorporation experiment. Bright blue fluorescence of the nanocrystals was detected in the cytosol when excited with a UV light, implying that the nanocrystals were able to be applied to biological imaging. In order to expand the application range, we synthesized and compared a series of silicon nanocrystals, which have variable surface modification, such as alkyl group, alcohol group, and odorant molecules. This study will provide a wider range of optoelectronic applications and bioimaging technology.

High-j neutron excitations outside 136Xe

NASA Astrophysics Data System (ADS)

Talwar, R.; Kay, B. P.; Mitchell, A. J.; Adachi, S.; Entwisle, J. P.; Fujita, Y.; Gey, G.; Noji, S.; Ong, H. J.; Schiffer, J. P.; Tamii, A.

2017-08-01

The ν 0 h9 /2 and ν 0 i13 /2 strength at 137Xe, a single neutron outside the N =82 shell closure, has been determined using the 136Xe(α ,3He)137Xe reaction carried out at 100 MeV. We confirm the recent observation of the second 13 /2+ state and reassess previous data on the 9 /2- states, obtaining spectroscopic factors. These new data provide additional constraints on predictions of the same single-neutron excitations at 133Sn.

Switchable Ni–Mn–Ga Heusler nanocrystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zayak, Alexey T.; Beckman, Scott P.; Tiago, Murilo L.

2008-10-02

Here, we examined bulk-like Heusler nanocrystals using real-space pseudopotentials constructed within density functional theory. The nanocrystals were made of various compositions of Ni-Mn-Ga in the size range from 15 up to 169 atoms. Among these compositions, the closest to the stoichiometric Ni 2MnGa were found to be the most stable. The Ni-based nanocrystals retained a tendency for tetragonal distortion, which is inherited from the bulk properties. Surface effects suppress the tetragonal structure in the smaller Ni-based nanocrystals, while bigger nanocrystals develop a bulk-like tetragonal distortion. We suggest the possibility of switchable Ni-Mn-Ga nanocrystals, which could be utilized for magnetic nano-shape-memorymore » applications.« less

Charge Transport in Semiconductor Nanocrystal Solids

NASA Astrophysics Data System (ADS)

Talapin, Dmitri; Shevchenko, Elena; Lee, Jong Soo; Urban, Jeffrey; Mitzi, David; Murray, Christopher

2007-03-01

Self-assembly of chemically-synthesized nanocrystals can yield complex long-range ordered structures which can be used as model systems for studying transport phenomena in low-dimensional materials [1]. Treatment of close-packed PbSe nanocrystal arrays with hydrazine enhanced exchange coupling between the nanocrystals and improved conductance by more than ten orders of magnitude compared to native nanocrystal films [2]. The conductivity of PbSe nanocrystal solids can be switched between n- and p-type transports by controlling the saturation of electronic states at nanocrystal surfaces. Nanocrystal arrays form the n- and p-channels of field-effect transistors with electron and hole mobilities of 2.5 cm^2V-1s-1 and 0.3 cm^2V-1s-1, respectively, and current modulation Ion/Ioff˜10^3-10^4. The field-effect mobility in PbSe nanocrystal arrays is higher than the mobility of organic transistors while the easy switch between n- and p-transport allows realization of complimentary circuits and p-n junctions for nanocrystal-based solar cells and thermoelectric devices. [1] E. V. Shevchenko, D. V. Talapin, N. A. Kotov, S. O'Brien, C. B. Murray. Nature 439, 55 (2006). [2] D. V. Talapin, C. B. Murray. Science 310, 86 (2005).

Nanocrystal synthesis

DOEpatents

Tisdale, William; Prins, Ferry; Weidman, Mark; Beck, Megan

2016-11-01

A method of preparing monodisperse MX semiconductor nanocrystals can include contacting an M-containing precursor with an X donor to form a mixture, where the molar ratio between the M containing precursor and the X donor is large. Alternatively, if additional X donor is added during the reaction, a smaller ratio between the M containing precursor and the X donor can be used to prepare monodisperse MX semiconductor nanocrystals.

Biomolecular Assembly of Gold Nanocrystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Micheel, Christine Marya

2005-05-20

Over the past ten years, methods have been developed to construct discrete nanostructures using nanocrystals and biomolecules. While these frequently consist of gold nanocrystals and DNA, semiconductor nanocrystals as well as antibodies and enzymes have also been used. One example of discrete nanostructures is dimers of gold nanocrystals linked together with complementary DNA. This type of nanostructure is also known as a nanocrystal molecule. Discrete nanostructures of this kind have a number of potential applications, from highly parallel self-assembly of electronics components and rapid read-out of DNA computations to biological imaging and a variety of bioassays. My research focused inmore » three main areas. The first area, the refinement of electrophoresis as a purification and characterization method, included application of agarose gel electrophoresis to the purification of discrete gold nanocrystal/DNA conjugates and nanocrystal molecules, as well as development of a more detailed understanding of the hydrodynamic behavior of these materials in gels. The second area, the development of methods for quantitative analysis of transmission electron microscope data, used computer programs written to find pair correlations as well as higher order correlations. With these programs, it is possible to reliably locate and measure nanocrystal molecules in TEM images. The final area of research explored the use of DNA ligase in the formation of nanocrystal molecules. Synthesis of dimers of gold particles linked with a single strand of DNA possible through the use of DNA ligase opens the possibility for amplification of nanostructures in a manner similar to polymerase chain reaction. These three areas are discussed in the context of the work in the Alivisatos group, as well as the field as a whole.« less

All-in-One Cellulose Nanocrystals for 3D Printing of Nanocomposite Hydrogels.

PubMed

Wang, Jieping; Chiappone, Annalisa; Roppolo, Ignazio; Shao, Feng; Fantino, Erika; Lorusso, Massimo; Rentsch, Daniel; Dietliker, Kurt; Pirri, Candido Fabrizio; Grützmacher, Hansjörg

2018-02-23

Cellulose nanocrystals (CNCs) with >2000 photoactive groups on each can act as highly efficient initiators for radical polymerizations, cross-linkers, as well as covalently embedded nanofillers for nanocomposite hydrogels. This is achieved by a simple and reliable method for surface modification of CNCs with a photoactive bis(acyl)phosphane oxide derivative. Shape-persistent and free-standing 3D structured objects were printed with a mono-functional methacrylate, showing a superior swelling capacity and improved mechanical properties. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Electron transfer between colloidal ZnO nanocrystals.

PubMed

Hayoun, Rebecca; Whitaker, Kelly M; Gamelin, Daniel R; Mayer, James M

2011-03-30

Colloidal ZnO nanocrystals capped with dodecylamine and dissolved in toluene can be charged photochemically to give stable solutions in which electrons are present in the conduction bands of the nanocrystals. These conduction-band electrons are readily monitored by EPR spectroscopy, with g* values that correlate with the nanocrystal sizes. Mixing a solution of charged small nanocrystals (e(-)(CB):ZnO-S) with a solution of uncharged large nanocrystals (ZnO-L) caused changes in the EPR spectrum indicative of quantitative electron transfer from small to large nanocrystals. EPR spectra of the reverse reaction, e(-)(CB):ZnO-L + ZnO-S, showed that electrons do not transfer from large to small nanocrystals. Stopped-flow kinetics studies monitoring the change in the UV band-edge absorption showed that reactions of 50 μM nanocrystals were complete within the 5 ms mixing time of the instrument. Similar results were obtained for the reaction of charged nanocrystals with methyl viologen (MV(2+)). These and related results indicate that the electron-transfer reactions of these colloidal nanocrystals are quantitative and very rapid, despite the presence of ~1.5 nm long dodecylamine capping ligands. These soluble ZnO nanocrystals are thus well-defined redox reagents suitable for studies of electron transfer involving semiconductor nanostructures.

Mechanochemical approach for the capping of mixed core CdS/ZnS nanocrystals: Elimination of cadmium toxicity.

PubMed

Bujňáková, Zdenka; Baláž, Matej; Dutková, Erika; Baláž, Peter; Kello, Martin; Mojžišová, Gabriela; Mojžiš, Ján; Vilková, Mária; Imrich, Ján; Psotka, Miroslav

2017-01-15

The wet mechanochemical procedure for the capping of the CdS and CdS/ZnS quantum dot nanocrystals is reported. l-cysteine and polyvinylpyrrolidone (PVP) were used as capping agents. When using l-cysteine, the dissolution of cadmium(II) was almost none for CdS/ZnS nanocrystals. Moreover, prepared CdS- and CdS/ZnS-cysteine nanosuspensions exhibited unimodal particle size distributions with very good stability, which was further supported by the zeta potential measurements. The Fourier-transform infrared (FTIR) and nuclear magnetic resonance (NMR) spectroscopy showed the successful embedment of cysteine into the structure of the nanocrystals. Additionally, the optical properties were examined, and the results showed that the cysteine nanosuspension has promising fluorescence properties. On the other hand, PVP was not determined to be a very suitable capping agent for the present system. In this case, the release of cadmium(II) was higher in comparison to the l-cysteine capped samples. The nanosuspensions were successfully used for in vitro studies on selected cancer cell lines. Using fluorescence microscopy, it was evidenced that the nanocrystals enter the cell and that they can serve as imaging agents in biomedical applications. Copyright © 2016. Published by Elsevier Inc.

Experimental ion mobility measurements in Xe-CF4 mixtures

NASA Astrophysics Data System (ADS)

Cortez, A. F. V.; Kaja, M. A.; Escada, J.; Santos, M. A. G.; Veenhof, R.; Neves, P. N. B.; Santos, F. P.; Borges, F. I. G. M.; Conde, C. A. N.

2018-04-01

In this paper we present the results of the ion mobility measurements made in gaseous mixtures of xenon with carbon tetrafluoride (Xe-CF4) for pressures ranging from 6 to 10 Torr (8-10.6 mbar) and for low reduced electric fields in the 10 to 25 Td range (2.4-6.1 kVṡcm‑1ṡbar‑1), at room temperature. The time-of-arrival spectra revealed one or two peaks depending on the gas relative abundances, which were attributed to CF3+ and to Xe2+ ions. However, for Xe concentrations above 60%, only one peak remains (Xe2+). The reduced mobilities obtained from the peak centroid of the time-of-arrival spectra are presented for Xe concentrations in the 5%-95% range.

Stable Chloro- and Bromoxenate Cage Anions; [X3(XeO3)3]3- and [X4(XeO3)4]4- (X = Cl or Br).

PubMed

Goettel, James T; Haensch, Veit G; Schrobilgen, Gary J

2017-06-28

The number of isolable compounds which contain different noble-gas-element bonds is limited for xenon and even more so for krypton. Examples of Xe-Cl bonds are rare, and prior to this work, no Xe-Br bonded compound had been isolated in macroscopic quantities. The syntheses, isolation, and characterization of the first compounds to contain Xe-Br bonds and their chlorine analogues are described in the present work. The reactions of XeO 3 with [N(CH 3 ) 4 ]Br and [N(C 2 H 5 ) 4 ]Br have provided two bromoxenate salts, [N(C 2 H 5 ) 4 ] 3 [Br 3 (XeO 3 ) 3 ] and [N(CH 3 ) 4 ] 4 [Br 4 (XeO 3 ) 4 ], in which the cage anions have Xe-Br bond lengths that range from 3.0838(3) to 3.3181(8) Å. The isostructural chloroxenate anions (Xe-Cl bond lengths, 2.9316(2) to 3.101(4) Å) were synthesized by analogy with their bromine analogues. The bromo- and chloroxenate salts are stable in the atmosphere at room temperature and were characterized in the solid state by Raman spectroscopy and low-temperature single-crystal X-ray diffraction, and in the gas phase by quantum-chemical calculations. They are the only known examples of cage anions that contain a noble-gas element. The Xe-Br and Xe-Cl bonds are very weakly covalent and can be viewed as σ-hole interactions, similar to those encountered in halogen bonding. However, the halogen atoms in these cases are valence electron lone pair donors, and the σ* Xe-O orbitals are lone pair acceptors.

Predictions for multiplicities and flow harmonics in 5.44 TeV Xe+Xe collisions at the CERN Large Hadron Collider

NASA Astrophysics Data System (ADS)

Eskola, K. J.; Niemi, H.; Paatelainen, R.; Tuominen, K.

2018-03-01

We present the event-by-event next-to-leading-order perturbative-QCD + saturation + viscous hydrodynamics (EKRT) model predictions for the centrality dependence of the charged hadron multiplicity in the pseudorapidity interval |η |≤0.5 , and for the centrality dependence of the charged hadron flow harmonics vn{2 } obtained from two-particle cumulants, in √{sN N}=5.44 TeV Xe+Xe collisions at the CERN Large Hadron Collider. Our prediction for the 0-5 % central charged multiplicity is d Nch/d η =1218 ±46 . We also predict vn{2 } in Xe+Xe collisions to increase more slowly from central towards peripheral collisions than those in a Pb+Pb system. We find that at 10 ,⋯,50 % centralities v2{2 } is smaller and v3{2 } is larger than in the Pb+Pb system while v4{2 } is of the same magnitude in both systems. We also find that the ratio of flow harmonics in Xe+Xe collisions and in Pb+Pb collisions shows a slight sensitivity to the temperature dependence of the shear-viscosity-to-entropy ratio. As we discuss here, the new nuclear mass-number systematics especially in the flow harmonics serves as a welcome further constraint for describing the space-time evolution of a heavy-ion system and for determining the shear viscosity and other transport properties of strongly interacting matter.

Improved search for two-neutrino double electron capture on 124Xe and 126Xe using particle identification in XMASS-I

NASA Astrophysics Data System (ADS)

Xmass Collaboration; Abe, K.; Hiraide, K.; Ichimura, K.; Kishimoto, Y.; Kobayashi, K.; Kobayashi, M.; Moriyama, S.; Nakahata, M.; Norita, T.; Ogawa, H.; Sato, K.; Sekiya, H.; Takachio, O.; Takeda, A.; Tasaka, S.; Yamashita, M.; Yang, B. S.; Kim, N. Y.; Kim, Y. D.; Itow, Y.; Kanzawa, K.; Kegasa, R.; Masuda, K.; Takiya, H.; Fushimi, K.; Kanzaki, G.; Martens, K.; Suzuki, Y.; Xu, B. D.; Fujita, R.; Hosokawa, K.; Miuchi, K.; Oka, N.; Takeuchi, Y.; Kim, Y. H.; Lee, K. B.; Lee, M. K.; Fukuda, Y.; Miyasaka, M.; Nishijima, K.; Nakamura, S.

2018-05-01

We conducted an improved search for the simultaneous capture of two K-shell electrons on the ^{124}Xe and ^{126}Xe nuclei with emission of two neutrinos using 800.0 days of data from the XMASS-I detector. A novel method to discriminate γ-ray/X-ray or double electron capture signals from β-ray background using scintillation time profiles was developed for this search. No significant signal was found when fitting the observed energy spectra with the expected signal and background. Therefore, we set the most stringent lower limits on the half-lives at 2.1 × 10^{22} and 1.9 × 10^{22} years for ^{124}Xe and ^{126}Xe, respectively, with 90% confidence level. These limits improve upon previously reported values by a factor of 4.5.

Phase separation in SiGe nanocrystals embedded in SiO{sub 2} matrix during high temperature annealing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mogaddam, N. A. P.; Turan, R.; Alagoz, A. S.

2008-12-15

SiGe nanocrystals have been formed in SiO{sub 2} matrix by cosputtering Si, Ge, and SiO{sub 2} independently on Si substrate. Effects of the annealing time and temperature on structural and compositional properties are studied by transmission electron microscopy, x-ray diffraction (XRD), and Raman spectroscopy measurements. It is observed that Ge-rich Si{sub (1-x)}Ge{sub x} nanocrystals do not hold their compositional uniformity when annealed at high temperatures for enough long time. A segregation process leading to separation of Ge and Si atoms from each other takes place. This process has been evidenced by a double peak formation in the XRD and Ramanmore » spectra. We attributed this phase separation to the differences in atomic size, surface energy, and surface diffusion disparity between Si and Ge atoms leading to the formation of nonhomogenous structure consist of a Si-rich SiGe core covered by a Ge-rich SiGe shell. This experimental observation is consistent with the result of reported theoretical and simulation methods.« less

A novel approach for the fabrication of all-inorganic nanocrystal solids: Semiconductor matrix encapsulated nanocrystal arrays

NASA Astrophysics Data System (ADS)

Moroz, Pavel

Growing fossil fuels consumption compels researchers to find new alternative pathways to produce energy. Along with new materials for the conversion of different types of energy into electricity innovative methods for efficient processing of energy sources are also introduced. The main criteria for the success of such materials and methods are the low cost and compelling performance. Among different types of materials semiconductor nanocrystals are considered as promising candidates for the role of the efficient and cheap absorbers for solar energy applications. In addition to the anticipated cost reduction, the integration of nanocrystals (NC) into device architectures is inspired by the possibility of tuning the energy of electrical charges in NCs via nanoparticle size. However, the stability of nanocrystals in photovoltaic devices is limited by the stability of organic ligands which passivate the surface of semiconductors to preserve quantum confinement. The present work introduces a new strategy for low-temperature processing of colloidal nanocrystals into all-inorganic films: semiconductor matrix encapsulated nanocrystal arrays (SMENA). This methodology goes beyond the traditional ligand-interlinking scheme and relies on the encapsulation of morphologically-defined nanocrystal arrays into a matrix of a wide-band gap semiconductor, which preserves optoelectronic properties of individual nanoparticles. Fabricated solids exhibit excellent thermal stability, which is attributed to the heteroepitaxial structure of nanocrystal-matrix interfaces. The main characteristics and properties of these solids were investigated and compared with ones of traditionally fabricated nanocrystal films using standard spectroscopic, optoelectronic and electronic techniques. As a proof of concept, we. We also characterized electron transport phenomena in different types of nanocrystal films using all-optical approach. By measuring excited carrier lifetimes in either ligand-linked or

Photo-sensitive Ge nanocrystal based films controlled by substrate deposition temperature

NASA Astrophysics Data System (ADS)

Stavarache, Ionel; Maraloiu, Valentin Adrian; Negrila, Catalin; Prepelita, Petronela; Gruia, Ion; Iordache, Gheorghe

2017-10-01

Lowering the temperature of crystallization by deposition of thin films on a heated substrate represents the easiest way to find new means to develop and improve new working devices based on nanocrystals embedded in thin films. The improvements are strongly related with the increasing of operation speed, substantially decreasing the energy consumption and reducing unit fabrication costs of the respective semiconductor devices. This approach avoids major problems, such as those related to diffusion or difficulties in controlling nanocrystallites size, which appear during thermal treatments at high temperatures after deposition. This article reports on a significant progress given by structuring Ge nanocrystals (Ge-NCs) embedded in silicon dioxide (SiO2) thin films by heating the substrate at 400 °C during co-deposition of Ge and SiO2 by magnetron sputtering. As a proof-of-concept, a Si/Ge-NCs:SiO2 photo-sensitive structure was fabricated thereof and characterized. The structure shows superior performance on broad operation bandwidth from visible to near-infrared, as strong rectification properties in dark, significant current rise in the inversion mode when illuminated, high responsivity, high photo-detectivity of 1014 Jones, quick response and significant conversion efficiency with peak value reaching 850% at -1 V and about 1000 nm. This simple preparation approach brings an important contribution to the effort of structuring Ge nanocrystallites in SiO2 thin films at a lower temperature for the purpose of using these materials for devices in optoelectronics, solar cells and electronics on flexible substrates.

Xe-126 Excesses: Monoisotopic Anomalies in Regolith Samples?

NASA Technical Reports Server (NTRS)

Mathew, K. J.; Marti, K.; Levskii, L. K.

2003-01-01

We present new Xe isotopic signatures of Pesyanoe regolith samples which document excesses of 126Xe and we explore the possibility that it formed by low-energy reactions on transient Te-rich coatings.

Half-life of Xe120

NASA Astrophysics Data System (ADS)

Phillips, A. A.; Andreoiu, C.; Ball, G. C.; Bandyopadhyay, D.; Behr, J. A.; Chupp, T. E.; Finlay, P.; Garrett, P. E.; Grinyer, G. F.; Hackman, G.; Hayden, M. E.; Hyland, B.; Nuss-Warren, S. R.; Pearson, M. R.; Schumaker, M. A.; Smith, M. B.; Svensson, C. E.; Tardiff, E. R.; Valiente-Dobón, J. J.; Warner, T.

2006-08-01

We have measured the half-life of Xe120 using a high-purity germanium (HPGe) detector to monitor the 176, 178, and 762 keV γ rays from Xe120 β+ decay. The result, 46±0.6 min, differs significantly from the value 40±1 min reported by Andersson [Ark. Fys. 28, 37 (1964)]. We have also measured the half-lives of Cs120 and I120 to be 60±0.7 s and 82.1±0.6 min, respectively, both of which are consistent with previous measurements.

Analysis of XeC1 Emission in a Hollow Cathode Discharge.

DTIC Science & Technology

1981-06-01

excited homopolar molecule, e.g., Xe2 , Hg2 The term exciplex refers to an electronically excited heteropolar complex, e.g., KrF , XeOH , XeCl , which...HCI Products, k9 = 5.4 x 10 cm /sec. (25) Figure 9 summarizes the main energy pathways for XeCI exciplex formation via three body recombination and

Simulations of Xe and U diffusion in UO2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andersson, Anders D.; Vyas, Shyam; Tonks, Michael R.

2012-09-10

Diffusion of xenon (Xe) and uranium (U) in UO{sub 2} is controlled by vacancy mechanisms and under irradiation the formation of mobile vacancy clusters is important. Based on the vacancy and cluster diffusion mechanisms established from density functional theory (DFT) calculations, we derive continuum thermodynamic and diffusion models for Xe and U in UO{sub 2}. In order to capture the effects of irradiation, vacancies (Va) are explicitly coupled to the Xe and U dynamics. Segregation of defects to grain boundaries in UO{sub 2} is described by combining the bulk diffusion model with models of the interaction between Xe atoms andmore » vacancies with grain boundaries, which were derived from atomistic calculations. The diffusion and segregation models were implemented in the MOOSE-Bison-Marmot (MBM) finite element (FEM) framework and the Xe/U redistribution was simulated for a few simple microstructures.« less

Linearly arranged polytypic CZTSSe nanocrystals

PubMed Central

Fan, Feng-Jia; Wu, Liang; Gong, Ming; Chen, Shi You; Liu, Guang Yao; Yao, Hong-Bin; Liang, Hai-Wei; Wang, Yi-Xiu; Yu, Shu-Hong

2012-01-01

Even colloidal polytypic nanostructures show promising future in band-gap tuning and alignment, researches on them have been much less reported than the standard nano-heterostructures because of the difficulties involved in synthesis. Up to now, controlled synthesis of colloidal polytypic nanocrsytals has been only realized in II-VI tetrapod and octopod nanocrystals with branched configurations. Herein, we report a colloidal approach for synthesizing non-branched but linearly arranged polytypic I2-II-IV-VI4 nanocrystals, with a focus on polytypic non-stoichiometric Cu2ZnSnSxSe4−x nanocrystals. Each synthesized polytypic non-stoichiometric Cu2ZnSnSxSe4−x nanocrystal is consisted of two zinc blende-derived ends and one wurtzite-derived center part. The formation mechanism has been studied and the phase composition can be tuned through adjusting the reaction temperature, which brings a new band-gap tuning approach to Cu2ZnSnSxSe4-x nanocrystals. PMID:23233871

Xe isotope detection and discrimination using beta spectroscopy with coincident gamma spectroscopy

NASA Astrophysics Data System (ADS)

Reeder, P. L.; Bowyer, T. W.

1998-02-01

Beta spectroscopic techniques show promise of significant improvements for a beta-gamma coincidence counter that is part of a system for analyzing Xe automatically separated from air. The previously developed counting system for 131mXe, 133mXe, 133gXe, and 135gXe can be enhanced to give additional discrimination between these Xe isotopes by using the plastic scintillation sample cell as a beta spectrometer to resolve the conversion electron peaks. The automated system will be a key factor in monitoring the Comprehensive Test Ban Treaty.

Live 129I-129Xe dating

NASA Technical Reports Server (NTRS)

Marti, K.

1986-01-01

A technique of cosmic ray exposure age dating using cosmic ray produced I-129 and Xe-129 components is discussed. The live I-129 - Xe-129 method provides an ideal monitor for cosmic ray flux variations on the 10(7)y - 10(8)y time-scale. It is based on low-energy neutron reactions on Te, and these data, when coupled to those from other methods, may facilitate the detection of complex exposure histories.

Numerical model of a single nanocrystal devoted to the study of disordered nanocrystal floating gates of new flash memories

NASA Astrophysics Data System (ADS)

Leroy, Yann; Armeanu, Dumitru; Cordan, Anne-Sophie

2011-05-01

The improvement of our model concerning a single nanocrystal that belongs to a nanocrystal floating gate of a flash memory is presented. In order to extend the gate voltage range applicability of the model, the 3D continuum of states of either metallic or semiconducting electrodes is discretized into 2D subbands. Such an approach gives precise information about the mechanisms behind the charging or release processes of the nanocrystal. Then, the self-energy and screening effects of an electron within the nanocrystal are evaluated and introduced in the model. This enables a better determination of the operating point of the nanocrystal memory. The impact of those improvements on the charging or release time of the nanocrystal is discussed.

Room temperature enhanced red emission from novel Eu(3+) doped ZnO nanocrystals uniformly dispersed in nanofibers.

PubMed

Zhang, Yongzhe; Liu, Yanxia; Li, Xiaodong; Wang, Qi Jie; Xie, Erqing

2011-10-14

Achieving red emission from ZnO-based materials has long been a goal for researchers in order to realize, for instance, full-color display panels and solid-state light-emitting devices. However, the current technique using Eu(3+) doped ZnO for red emission generation has a significant drawback in that the energy transfer from ZnO to Eu(3+) is inefficient, resulting in a low intensity red emission. In this paper, we report an efficient energy transfer scheme for enhanced red emission from Eu(3+) doped ZnO nanocrystals by fabricating polymer nanofibers embedded with Eu(3+) doped ZnO nanocrystals to facilitate the energy transfer. In the fabrication, ZnO nanocrystals are uniformly dispersed in polymer nanofibers prepared by the high electrical field electrospinning technique. Enhanced red emission without defect radiation from the ZnO matrix is observed. Three physical mechanisms for this observation are provided and explained, namely a small ZnO crystal size, uniformity distribution of ZnO nanocrystals in polymers (PVA in this case), and strong bonding between ZnO and polymer through the -OH group bonding. These explanations are supported by high resolution transmission emission microscopy measurements, resonant Raman scattering characterizations, photoluminescence spectra and photoluminescence excitation spectra measurements. In addition, two models exploring the 'accumulation layer' and 'depletion layer' are developed to explain the reasons for the more efficient energy transfer in our ZnO nanocrystal system compared to that in the previous reports. This study provides an important approach to achieve enhanced energy transfer from nanocrystals to ions which could be widely adopted in rare earth ion doped materials. These discoveries also provide more insights into other energy transfer problems in, for example, dye-sensitized solar cells and quantum dot solar cells.

Direct Measurements of Magnetic Polarons in Cd 1–xMn x Se Nanocrystals from Resonant Photoluminescence

DOE PAGES

Rice, W. D.; Liu, W.; Pinchetti, V.; ...

2017-04-07

In semiconductors, quantum confinement can greatly enhance the interaction between band carriers (electrons and holes) and dopant atoms. One manifestation of this enhancement is the increased stability of exciton magnetic polarons in magnetically doped nanostructures. In the limit of very strong 0D confinement that is realized in colloidal semiconductor nanocrystals, a single exciton can exert an effective exchange field B ex on the embedded magnetic dopants that exceeds several tesla. Here we use the very sensitive method of resonant photoluminescence (PL) to directly measure the presence and properties of exciton magnetic polarons in colloidal Cd 1–xMn xSe nanocrystals. Despite smallmore » Mn 2+ concentrations (x = 0.4–1.6%), large polaron binding energies up to ~26 meV are observed at low temperatures via the substantial Stokes shift between the pump laser and the resonant PL maximum, indicating nearly complete alignment of all Mn 2+ spins by B exex ≈ 10 T in these nanocrystals, in good agreement with theoretical estimates. Further, the emission line widths provide direct insight into the statistical fluctuations of the Mn 2+ spins. In conclusion, these resonant PL studies provide detailed insight into collective magnetic phenomena, especially in lightly doped nanocrystals where conventional techniques such as nonresonant PL or time-resolved PL provide ambiguous results.« less

Direct Measurements of Magnetic Polarons in Cd 1–xMn x Se Nanocrystals from Resonant Photoluminescence

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rice, W. D.; Liu, W.; Pinchetti, V.

In semiconductors, quantum confinement can greatly enhance the interaction between band carriers (electrons and holes) and dopant atoms. One manifestation of this enhancement is the increased stability of exciton magnetic polarons in magnetically doped nanostructures. In the limit of very strong 0D confinement that is realized in colloidal semiconductor nanocrystals, a single exciton can exert an effective exchange field B ex on the embedded magnetic dopants that exceeds several tesla. Here we use the very sensitive method of resonant photoluminescence (PL) to directly measure the presence and properties of exciton magnetic polarons in colloidal Cd 1–xMn xSe nanocrystals. Despite smallmore » Mn 2+ concentrations (x = 0.4–1.6%), large polaron binding energies up to ~26 meV are observed at low temperatures via the substantial Stokes shift between the pump laser and the resonant PL maximum, indicating nearly complete alignment of all Mn 2+ spins by B exex ≈ 10 T in these nanocrystals, in good agreement with theoretical estimates. Further, the emission line widths provide direct insight into the statistical fluctuations of the Mn 2+ spins. In conclusion, these resonant PL studies provide detailed insight into collective magnetic phenomena, especially in lightly doped nanocrystals where conventional techniques such as nonresonant PL or time-resolved PL provide ambiguous results.« less

Concentration Independent Calibration of β-γ Coincidence Detector Using 131mXe and 133Xe

DOE Office of Scientific and Technical Information (OSTI.GOV)

McIntyre, Justin I.; Cooper, Matthew W.; Carman, April J.

Absolute efficiency calibration of radiometric detectors is frequently difficult and requires careful detector modeling and accurate knowledge of the radioactive source used. In the past we have calibrated the b-g coincidence detector of the Automated Radioxenon Sampler/Analyzer (ARSA) using a variety of sources and techniques which have proven to be less than desirable.[1] A superior technique has been developed that uses the conversion-electron (CE) and x-ray coincidence of 131mXe to provide a more accurate absolute gamma efficiency of the detector. The 131mXe is injected directly into the beta cell of the coincident counting system and no knowledge of absolute sourcemore » strength is required. In addition, 133Xe is used to provide a second independent means to obtain the absolute efficiency calibration. These two data points provide the necessary information for calculating the detector efficiency and can be used in conjunction with other noble gas isotopes to completely characterize and calibrate the ARSA nuclear detector. In this paper we discuss the techniques and results that we have obtained.« less

Connecting the Particles in the Box - Controlled Fusion of Hexamer Nanocrystal Clusters within an AB6 Binary Nanocrystal Superlattice

PubMed Central

Treml, Benjamin E.; Lukose, Binit; Clancy, Paulette; Smilgies, Detlef-M; Hanrath, Tobias

2014-01-01

Binary nanocrystal superlattices present unique opportunities to create novel interconnected nanostructures by partial fusion of specific components of the superlattice. Here, we demonstrate the binary AB6 superlattice of PbSe and Fe2O3 nanocrystals as a model system to transform the central hexamer of PbSe nanocrystals into a single fused particle. We present detailed structural analysis of the superlattices by combining high-resolution X-ray scattering and electron microscopy. Molecular dynamics simulations show optimum separation of nanocrystals in agreement with the experiment and provide insights into the molecular configuration of surface ligands. We describe the concept of nanocrystal superlattices as a versatile ‘nanoreactor' to create and study novel materials based on precisely defined size, composition and structure of nanocrystals into a mesostructured cluster. We demonstrate ‘controlled fusion' of nanocrystals in the clusters in reactions initiated by thermal treatment and pulsed laser annealing. PMID:25339169

High-efficiency near-infrared enabled planar perovskite solar cells by embedding upconversion nanocrystals.

PubMed

Meng, Fan-Li; Wu, Jiao-Jiao; Zhao, Er-Fei; Zheng, Yan-Zhen; Huang, Mei-Lan; Dai, Li-Ming; Tao, Xia; Chen, Jian-Feng

2017-11-30

Integration of the upconversion effect in perovskite solar cells (PSCs) is a facile approach towards extending the spectral absorption from the visible to the near infrared (NIR) range and reducing the non-absorption loss of solar photons. However, the big challenge for practical application of UCNCs in planar PSCs is the poor compatibility between UCNCs and the perovskite precursor. Herein, we have subtly overcome the tough compatibility issue using a ligand-exchange strategy. For the first time, β-NaYF 4 :Yb,Er UCNCs have been embedded in situ into a CH 3 NH 3 PbI 3 layer to fabricate NIR-enabled planar PSCs. The CH 3 NH 3 I-capped UCNCs generated from the ligand-exchange were mixed with the perovskite precursor and served as nucleation sites for the UCNC-mediated heteroepitaxial growth of perovskite; moreover, the in situ embedding of UCNCs into the perovskite layer was realized during a spin-coating process. The resulting UCNC-embedded perovskite layer attained a uniform pinhole-free morphology with enlarged crystal grains and enabled NIR absorption. It also contributed to the energy transfer from the UCNCs to the perovskite and electron transport to the collecting electrode surface. The device fabricated using the UCNC-embedded perovskite film achieved an average power-conversion efficiency of 18.60% (19.70% for the best) under AM 1.5G and 0.37% under 980 nm laser, corresponding to 54% and 740-fold increase as compared to that of its counterpart without UCNCs.

The Surface Chemistry of Metal Chalcogenide Nanocrystals

NASA Astrophysics Data System (ADS)

Anderson, Nicholas Charles

The surface chemistry of metal chalcogenide nanocrystals is explored through several interrelated analytical investigations. After a brief discussion of the nanocrystal history and applications, molecular orbital theory is used to describe the electronic properties of semiconductors, and how these materials behave on the nanoscale. Quantum confinement plays a major role in dictating the optical properties of metal chalcogenide nanocrystals, however surface states also have an equally significant contribution to the electronic properties of nanocrystals due to the high surface area to volume ratio of nanoscale semiconductors. Controlling surface chemistry is essential to functionalizing these materials for biological imaging and photovoltaic device applications. To better understand the surface chemistry of semiconducting nanocrystals, three competing surface chemistry models are presented: 1.) The TOPO model, 2.) the Non-stoichiometric model, and 3.) the Neutral Fragment model. Both the non-stoichiometric and neutral fragment models accurately describe the behavior of metal chalcogenide nanocrystals. These models rely on the covalent bond classification system, which divides ligands into three classes: 1.) X-type, 1-electron donating ligands that balance charge with excess metal at the nanocrystal surface, 2.) L-type, 2-electron donors that bind metal sites, and 3.) Z-type, 2-electron acceptors that bind chalcogenide sites. Each of these ligand classes is explored in detail to better understand the surface chemistry of metal chalcogenide nanocrystals. First, chloride-terminated, tri-n-butylphosphine (Bu 3P) bound CdSe nanocrystals were prepared by cleaving carboxylate ligands from CdSe nanocrystals with chlorotrimethylsilane in Bu3P solution. 1H and 31P{1H} nuclear magnetic resonance spectra of the isolated nanocrystals allowed assignment of distinct signals from several free and bound species, including surface-bound Bu3P and [Bu3P-H]+[Cl]- ligands as well as a Bu

Composite material including nanocrystals and methods of making

DOEpatents

Bawendi, Moungi G.; Sundar, Vikram C.

2010-04-06

Temperature-sensing compositions can include an inorganic material, such as a semiconductor nanocrystal. The nanocrystal can be a dependable and accurate indicator of temperature. The intensity of emission of the nanocrystal varies with temperature and can be highly sensitive to surface temperature. The nanocrystals can be processed with a binder to form a matrix, which can be varied by altering the chemical nature of the surface of the nanocrystal. A nanocrystal with a compatibilizing outer layer can be incorporated into a coating formulation and retain its temperature sensitive emissive properties.

Composite material including nanocrystals and methods of making

DOEpatents

Bawendi, Moungi G [Boston, MA; Sundar, Vikram C [New York, NY

2008-02-05

Temperature-sensing compositions can include an inorganic material, such as a semiconductor nanocrystal. The nanocrystal can be a dependable and accurate indicator of temperature. The intensity of emission of the nanocrystal varies with temperature and can be highly sensitive to surface temperature. The nanocrystals can be processed with a binder to form a matrix, which can be varied by altering the chemical nature of the surface of the nanocrystal. A nanocrystal with a compatibilizing outer layer can be incorporated into a coating formulation and retain its temperature sensitive emissive properties

Quantum confinement of nanocrystals within amorphous matrices

NASA Astrophysics Data System (ADS)

Lusk, Mark T.; Collins, Reuben T.; Nourbakhsh, Zahra; Akbarzadeh, Hadi

2014-02-01

Nanocrystals encapsulated within an amorphous matrix are computationally analyzed to quantify the degree to which the matrix modifies the nature of their quantum-confinement power—i.e., the relationship between nanocrystal size and the gap between valence- and conduction-band edges. A special geometry allows exactly the same amorphous matrix to be applied to nanocrystals of increasing size to precisely quantify changes in confinement without the noise typically associated with encapsulating structures that are different for each nanocrystal. The results both explain and quantify the degree to which amorphous matrices redshift the character of quantum confinement. The character of this confinement depends on both the type of encapsulating material and the separation distance between the nanocrystals within it. Surprisingly, the analysis also identifies a critical nanocrystal threshold below which quantum confinement is not possible—a feature unique to amorphous encapsulation. Although applied to silicon nanocrystals within an amorphous silicon matrix, the methodology can be used to accurately analyze the confinement softening of other amorphous systems as well.

Synthesis of ligand-stabilized metal oxide nanocrystals and epitaxial core/shell nanocrystals via a lower-temperature esterification process.

PubMed

Ito, Daisuke; Yokoyama, Shun; Zaikova, Tatiana; Masuko, Keiichiro; Hutchison, James E

2014-01-28

The properties of metal oxide nanocrystals can be tuned by incorporating mixtures of matrix metal elements, adding metal ion dopants, or constructing core/shell structures. However, high-temperature conditions required to synthesize these nanocrystals make it difficult to achieve the desired compositions, doping levels, and structural control. We present a lower temperature synthesis of ligand-stabilized metal oxide nanocrystals that produces crystalline, monodisperse nanocrystals at temperatures well below the thermal decomposition point of the precursors. Slow injection (0.2 mL/min) of an oleic acid solution of the metal oleate complex into an oleyl alcohol solvent at 230 °C results in a rapid esterification reaction and the production of metal oxide nanocrystals. The approach produces high yields of crystalline, monodisperse metal oxide nanoparticles containing manganese, iron, cobalt, zinc, and indium within 20 min. Synthesis of tin-doped indium oxide (ITO) can be accomplished with good control of the tin doping levels. Finally, the method makes it possible to perform epitaxial growth of shells onto nanocrystal cores to produce core/shell nanocrystals.

High-speed all-optical logic inverter based on stimulated Raman scattering in silicon nanocrystal.

PubMed

Sen, Mrinal; Das, Mukul K

2015-11-01

In this paper, we propose a new device architecture for an all-optical logic inverter (NOT gate), which is cascadable with a similar device. The inverter is based on stimulated Raman scattering in silicon nanocrystal waveguides, which are embedded in a silicon photonic crystal structure. The Raman response function of silicon nanocrystal is evaluated to explore the transfer characteristic of the inverter. A maximum product criterion for the noise margin is taken to analyze the cascadability of the inverter. The time domain response of the inverter, which explores successful inversion operation at 100 Gb/s, is analyzed. Propagation delay of the inverter is on the order of 5 ps, which is less than the delay in most of the electronic logic families as of today. Overall dimension of the device is around 755  μm ×15  μm, which ensures integration compatibility with the matured silicon industry.

Nanocrystal/sol-gel nanocomposites

DOEpatents

Petruska, Melissa A [Los Alamos, NM; Klimov, Victor L [Los Alamos, NM

2007-06-05

The present invention is directed to solid composites including colloidal nanocrystals within a sol-gel host or matrix and to processes of forming such solid composites. The present invention is further directed to alcohol soluble colloidal nanocrystals useful in formation of sol-gel based solid composites.

Nanocrystal/sol-gel nanocomposites

DOEpatents

Petruska, Melissa A [Los Alamos, NM; Klimov, Victor L [Los Alamos, NM

2012-06-12

The present invention is directed to solid composites including colloidal nanocrystals within a sol-gel host or matrix and to processes of forming such solid composites. The present invention is further directed to alcohol soluble colloidal nanocrystals useful in formation of sol-gel based solid composites

Barium titanate nanocrystals and nanocrystal thin films: Synthesis, ferroelectricity, and dielectric properties

NASA Astrophysics Data System (ADS)

Huang, Limin; Chen, Zhuoying; Wilson, James D.; Banerjee, Sarbajit; Robinson, Richard D.; Herman, Irving P.; Laibowitz, Robert; O'Brien, Stephen

2006-08-01

Advanced applications for high k dielectric and ferroelectric materials in the electronics industry continues to demand an understanding of the underlying physics in decreasing dimensions into the nanoscale. We report the synthesis, processing, and electrical characterization of thin (<100nm thick) nanostructured thin films of barium titanate (BaTiO3) built from uniform nanoparticles (<20nm in diameter). We introduce a form of processing as a step toward the ability to prepare textured films based on assembly of nanoparticles. Essential to this approach is an understanding of the nanoparticle as a building block, combined with an ability to integrate them into thin films that have uniform and characteristic electrical properties. Our method offers a versatile means of preparing BaTiO3 nanocrystals, which can be used as a basis for micropatterned or continuous BaTiO3 nanocrystal thin films. We observe the BaTiO3 nanocrystals crystallize with evidence of tetragonality. We investigated the preparation of well-isolated BaTiO3 nanocrystals smaller than 10nm with control over aggregation and crystal densities on various substrates such as Si, Si /SiO2, Si3N4/Si, and Pt-coated Si substrates. BaTiO3 nanocrystal thin films were then prepared, resulting in films with a uniform nanocrystalline grain texture. Electric field dependent polarization measurements show spontaneous polarization and hysteresis, indicating ferroelectric behavior for the BaTiO3 nanocrystalline films with grain sizes in the range of 10-30nm. Dielectric measurements of the films show dielectic constants in the range of 85-90 over the 1KHz -100KHz, with low loss. We present nanocrystals as initial building blocks for the preparation of thin films which exhibit highly uniform nanostructured texture and grain sizes.

Colloidal inorganic nanocrystals: Nucleation, growth and biological applications

NASA Astrophysics Data System (ADS)

Lynch, Jared James

Colloidal inorganic nanocrystals are a class of material whose size ranges from a few nanometers to a hundred nanometers in dimension. These nanocrystals have size dependent properties that differ significantly from the bulk material counterparts. Due to their unique physical properties colloidal inorganic nanocrystals have several promising applications in a diverse range of areas, such as biomedical diagnosis, catalysis, plasmonics, high-density data storage and solar energy conversion. This dissertation presents the study of the formation of iron oxide nanocrystals under the influence of solvent and Ar gas bubbles, the phase transfer of metal oxide nanocrystals into water using inorganic ions, and the doping of semiconductor CdS/ZnS core/shell nanocrystals with copper and silver ions. First, the formation of iron oxide nanocrystals is investigated in the presence of boiling solvent or Ar bubbles. Using a non-injection based synthesis method, the thermal decomposition of iron oleate was studied under various reaction conditions, and the role of the bubbles on the nucleation and growth of iron oxide nanocrystals was determined. Kinetics studies were used to elucidate how latent heat transfer from the bubbles allows for "active monomers" to form preferentially from exothermic reactions taking place during nucleation. General insights into colloidal inorganic nanocrystal formation are discussed. Second, a non-injection based synthesis for CdS/ZnS core/shell nanocrystals is used to make high quality semiconductor particles which are intentionally doped with Cu or Ag ions. The Ag ions effect on the optical properties of the CdS/ZnS nanocrystals is investigated. The absorption and fluorescence of the samples is measured as a function of time and temperature. Proposed mechanisms for the observations are given and thoroughly discussed. Comparisons between previous results for Cu doped CdS/ZnS nanocrystals are also made to further understand how doping of semiconductor

Self-assembly of water-soluble nanocrystals

DOEpatents

Fan, Hongyou [Albuquerque, NM; Brinker, C Jeffrey [Albuquerque, NM; Lopez, Gabriel P [Albuquerque, NM

2012-01-10

A method for forming an ordered array of nanocrystals where a hydrophobic precursor solution with a hydrophobic core material in an organic solvent is added to a solution of a surfactant in water, followed by removal of a least a portion of the organic solvent to form a micellar solution of nanocrystals. A precursor co-assembling material, generally water-soluble, that can co-assemble with individual micelles formed in the micellar solution of nanocrystals can be added to this micellar solution under specified reaction conditions (for example, pH conditions) to form an ordered-array mesophase material. For example, basic conditions are used to precipitate an ordered nanocrystal/silica array material in bulk form and acidic conditions are used to form an ordered nanocrystal/silica array material as a thin film.

Xe incorporation in crust and upper mantle minerals: new experimental and theoretical evidences

NASA Astrophysics Data System (ADS)

Celine, C.; Sanloup, C.; Blanchard, M.; Lazzeri, M.; Balan, E.; Hudspeth, J.

2017-12-01

Storage of Xe in silicate minerals has been proposed to explain the `Missing Xenon' issue, i.e. the low Xe abundance in the Earth's and Mars' atmospheres compared to other noble gases [1]. However, data about Xe incorporation in minerals remain scarce due to high Xe volatility preventing studies at ambient conditions. Xe incorporations in olivine [2] and quartz [3] have been proposed based on experimental evidences at high pressures and temperatures. Nevertheless, Xe incorporation mechanisms remained so far only hypothetical. We present here new in situ X-ray diffraction data in diamond-anvil cell showing Xe incorporation in widespread silicate minerals of the continental crust (feldspars and quartz) and of the upper mantle (olivine) at relevant pressure and temperature conditions. Significant variations in cell parameters are retrieved in Xe-rich minerals as well as new peaks, implying change in the crystal structures linked to Xe incorporation. Theoretical calculations have been performed (using the density functional theory) to propose Xe incorporation sites able to reproduce experimental observations. In olivine, a Xe for Si substitutions is proposed, with up to 0.4 at% Xe potentially stored in olivine at depth. These new constraints on Xe incorporation at depths in silicate minerals, often neglected, could be crucial in the `Missing Xenon' issue. [1] Anders and Owen (1977) Science 198, 453-465, [2] Sanloup et al. (2011) Geochim. Cosmochim. Acta 75, 6271-6284, [3] Sanloup et al., (2005) Science, 310, 1174-1177

Nanocrystal thin film fabrication methods and apparatus

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kagan, Cherie R.; Kim, David K.; Choi, Ji-Hyuk

Nanocrystal thin film devices and methods for fabricating nanocrystal thin film devices are disclosed. The nanocrystal thin films are diffused with a dopant such as Indium, Potassium, Tin, etc. to reduce surface states. The thin film devices may be exposed to air during a portion of the fabrication. This enables fabrication of nanocrystal-based devices using a wider range of techniques such as photolithography and photolithographic patterning in an air environment.

Mass and Double-Beta-Decay Q Value of Xe136

NASA Astrophysics Data System (ADS)

Redshaw, Matthew; Wingfield, Elizabeth; McDaniel, Joseph; Myers, Edmund G.

2007-02-01

The atomic mass of Xe136 has been measured by comparing cyclotron frequencies of single ions in a Penning trap. The result, with 1 standard deviation uncertainty, is M(Xe136)=135.907 214 484 (11) u. Combined with previous results for the mass of Ba136 [Audi, Wapstra, and Thibault, Nucl. Phys. A 729, 337 (2003)NUPABL0375-947410.1016/j.nuclphysa.2003.11.003], this gives a Q value (M[Xe136]-M[Ba136])c2=2457.83(37)keV, sufficiently precise for ongoing searches for the neutrinoless double-beta decay of Xe136.

Tunable Room-Temperature Synthesis of Coinage Metal Chalcogenide Nanocrystals from N -Heterocyclic Carbene Synthons

DOE PAGES

Lu, Haipeng; Brutchey, Richard L.

2017-01-23

Here we present a new toolset of precursors for semiconductor nanocrystal synthesis, N-heterocyclic carbene (NHC)-metal halide complexes, which enables a tunable molecular platform for the preparation of coinage metal chalcogenide quantum dots (QDs). Phase-pure and highly monodisperse coinage metal chalcogenide (Ag 2E, Cu 2-xE; E = S, Se) QDs are readily synthesized from the direct reaction of an NHC-MBr synthon (where M = Ag, Cu) with alkylsilyl chalcogenide reagents at room temperature. We demonstrate that the size of the resulting QDs is well tailored by the electron-donating ability of the L-type NHC ligands, which are further confirmed to be themore » only organic capping ligands on the QD surface, imparting excellent colloidal stability. Local superstructures of the NHC-capped Ag 2S QDs are observed by TEM, further demonstrating their potential for synthesizing monodisperse ensembles and mediating self-assembly.« less

Tunable Room-Temperature Synthesis of Coinage Metal Chalcogenide Nanocrystals from N -Heterocyclic Carbene Synthons

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lu, Haipeng; Brutchey, Richard L.

Here we present a new toolset of precursors for semiconductor nanocrystal synthesis, N-heterocyclic carbene (NHC)-metal halide complexes, which enables a tunable molecular platform for the preparation of coinage metal chalcogenide quantum dots (QDs). Phase-pure and highly monodisperse coinage metal chalcogenide (Ag 2E, Cu 2-xE; E = S, Se) QDs are readily synthesized from the direct reaction of an NHC-MBr synthon (where M = Ag, Cu) with alkylsilyl chalcogenide reagents at room temperature. We demonstrate that the size of the resulting QDs is well tailored by the electron-donating ability of the L-type NHC ligands, which are further confirmed to be themore » only organic capping ligands on the QD surface, imparting excellent colloidal stability. Local superstructures of the NHC-capped Ag 2S QDs are observed by TEM, further demonstrating their potential for synthesizing monodisperse ensembles and mediating self-assembly.« less

Nanocrystals for electronics.

PubMed

Panthani, Matthew G; Korgel, Brian A

2012-01-01

Semiconductor nanocrystals are promising materials for low-cost large-area electronic device fabrication. They can be synthesized with a wide variety of chemical compositions and size-tunable optical and electronic properties as well as dispersed in solvents for room-temperature deposition using various types of printing processes. This review addresses research progress in large-area electronic device applications using nanocrystal-based electrically active thin films, including thin-film transistors, light-emitting diodes, photovoltaics, and thermoelectrics.

Xe/Kr Selectivity Measurements using AgZ-PAN at Various Temperatures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Garn, Troy Gerry; Greenhalgh, Mitchell Randy; Watson, Tony Leroy

2015-05-01

In preparation for planned FY-15 Xe/Kr multi-column testing, a series of experiments were performed to determine the selectivity of Xe over Kr using the silver converted mordenite-polyacrylonitrile (AgZ-PAN) sorbent. Results from these experiments will be used for parameter selection guidelines to define test conditions for Kr gas capture purity evaluations later this year. The currently configured experimental test bed was modified by installing a new cooling apparatus to permit future multi-column testing with independent column temperature control. The modified test bed will allow for multi-column testing to facilitate a Xe separation followed by a Kr separation using engineered form sorbents.more » Selectivity experiments were run at temperatures of 295, 250 and 220 K. Two feed gas compositions of 1000 ppmv Xe, 150 ppmv Kr in either a He or an air balance were used. AgZ-PAN sorbent selectivity was calculated using Xe and Kr capacity determinations. AgZ-PAN sorbent selectivities for Xe over Kr of 72 were calculated at room temperature (295 K) using the feed gas with a He balance and 34 using the feed gas with an air balance. As the test temperatures were decreased the selectivity of Xe over Kr also decreased due to an increase in both Xe and Kr capacities. At 220 K, the sorbent selectivities for Xe over Kr were 22 using the feed gas with a He balance and 28 using the feed gas with an air balance. The selectivity results indicate that AgZ-PAN used in the first column of a multi-column configuration will provide adequate partitioning of Xe from Kr in the tested temperature range to produce a more pure Kr end product for collection.« less

Coordination of XeF2 to calcium and cadmium hexafluorophosphates(V).

PubMed

Bunic, Tina; Tavcar, Gasper; Tramsek, Melita; Zemva, Boris

2006-02-06

[M(XeF2)5](PF6)2 (M = Ca, Cd) complexes were prepared by the reaction of MF2 and XeF2 under pressure of gaseous PF5 in anhydrous HF as solvent. The coordination sphere of the Ca atom consists of nine fluorine atoms: three from two PF6(-) units (one bidentate and one monodentate) and one from each of six XeF2 molecules. The coordination sphere of the Cd atom consists of eight fluorine atoms: one from each of two PF6(-) units and one from each of six XeF2 molecules. Two of the XeF2 ligands about M in each compound are bridging ligands and are each linked to two M, generating infinite (-M-F-Xe-F-M-F-Xe-F-) chains along the b-axis in the Ca salt and along the c-axis in the Cd compound. The Cd2+ cation is smaller and more electronegative than the Ca2+ cation. These differences account for the higher F ligand coordination in the Ca2+ salt and for other structural features that distinguish them. The different stoichiometry of the PF6(-) salts when compared with their AsF6(-) analogues, which have the composition [M(XeF2)4](AsF6)2 (M = Ca, Cd), is in accord with the lower F ligand charge in the AsF6(-) when compared with that in the PF6(-) compound. Indeed, the AsF6(-) ligand charges appear to be similar to those in the XeF2-bridged species.

Electronic displays using optically pumped luminescent semiconductor nanocrystals

DOEpatents

Weiss, Shimon; Schlamp, Michael C.; Alivisatos, A. Paul

2010-04-13

A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit light of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

Electronic displays using optically pumped luminescent semiconductor nanocrystals

DOEpatents

Weiss, Shimon; Schlamp, Michael C.; Alivisatos, A. Paul

2005-03-08

A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit light of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

Electronic displays using optically pumped luminescent semiconductor nanocrystals

DOEpatents

Weiss, Shimon; Schlamp, Michael C.; Alivisatos, A. Paul

2015-06-23

A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit light of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

Electronic displays using optically pumped luminescent semiconductor nanocrystals

DOEpatents

Weiss, Shimon; Schlamp, Michael C; Alivisatos, A. Paul

2014-02-11

A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit light of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

Electronic displays using optically pumped luminescent semiconductor nanocrystals

DOEpatents

Weiss, Shimon; Schlamp, Michael C.; Alivisatos, Paul A.

2015-11-10

A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit tight of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

Electronic displays using optically pumped luminescent semiconductor nanocrystals

DOEpatents

Weiss, Shimon [Pinole, CA; Schlamp, Michael C [Plainsboro, NJ; Alivisatos, A Paul [Oakland, CA

2011-09-27

A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit light of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

Electronic displays using optically pumped luminescent semiconductor nanocrystals

DOEpatents

Weiss, Shimon; Schlam, Michael C; Alivisatos, A. Paul

2014-03-25

A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit tight of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

Electronic displays using optically pumped luminescent semiconductor nanocrystals

DOEpatents

Weiss, Shimon; Schlamp, Michael C.; Alivisatos, A. Paul

2017-06-06

A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit tight of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

Charge transport in metal oxide nanocrystal-based materials

NASA Astrophysics Data System (ADS)

Runnerstrom, Evan Lars

There is probably no class of materials more varied, more widely used, or more ubiquitous than metal oxides. Depending on their composition, metal oxides can exhibit almost any number of properties. Of particular interest are the ways in which charge is transported in metal oxides: devices such as displays, touch screens, and smart windows rely on the ability of certain metal oxides to conduct electricity while maintaining visible transparency. Smart windows, fuel cells, and other electrochemical devices additionally rely on efficient transport of ionic charge in and around metal oxides. Colloidal synthesis has enabled metal oxide nanocrystals to emerge as a relatively new but highly tunable class of materials. Certain metal oxide nanocrystals, particularly highly doped metal oxides, have been enjoying rapid development in the last decade. As in myriad other materials systems, structure dictates the properties of metal oxide nanocrystals, but a full understanding of how nanocrystal synthesis, the processing of nanocrystal-based materials, and the structure of nanocrystals relate to the resulting properties of nanocrystal-based materials is still nascent. Gaining a fundamental understanding of and control over these structure-property relationships is crucial to developing a holistic understanding of metal oxide nanocrystals. The unique ability to tune metal oxide nanocrystals by changing composition through the introduction of dopants or by changing size and shape affords a way to study the interplay between structure, processing, and properties. This overall goal of this work is to chemically synthesize colloidal metal oxide nanocrystals, process them into useful materials, characterize charge transport in materials based on colloidal metal oxide nanocrystals, and develop ways to manipulate charge transport. In particular, this dissertation characterizes how the charge transport properties of metal oxide nanocrystal-based materials depend on their processing and

Copper Selenide Nanocrystals for Photothermal Therapy

PubMed Central

Hessel, Colin M.; Pattani, Varun; Rasch, Michael; Panthani, Matthew G.; Koo, Bonil; Tunnell, James W.; Korgel, Brian A.

2011-01-01

Ligand-stabilized copper selenide (Cu2−xSe) nanocrystals, approximately 16 nm in diameter, were synthesized by a colloidal hot injection method and coated with amphiphilic polymer. The nanocrystals readily disperse in water and exhibit strong near infrared (NIR) optical absorption with a high molar extinction coefficient of 7.7 × 107 cm−1 M−1 at 980 nm. When excited with 800 nm light, the Cu2−xSe nanocrystals produce significant photothermal heating with a photothermal transduction efficiency of 22%, comparable to nanorods and nanoshells of gold (Au). In vitro photothermal heating of Cu2−xSe nanocrystals in the presence of human colorectal cancer cell (HCT-116) led to cell destruction after 5 minutes of laser irradiation at 33 W/cm2, demonstrating the viabilitiy of Cu2−xSe nanocrystals for photothermal therapy applications. PMID:21553924

Magnetic Resonance Imaging with laser polarized 129Xe

NASA Astrophysics Data System (ADS)

Swanson, Scott D.; Rosen, Matthew S.; Agranoff, Bernard W.; Coulter, Kevin P.; Welsh, Robert C.; Chupp, Timothy E.

1998-01-01

Magnetic Resonance Imaging with laser-polarized 129Xe can be utilized to trace blood flow and perfusion in tissue for a variety of biomedical applications. Polarized xenon gas introduced in to the lungs dissolves in the blood and is transported to organs such as the brain where it accumulates in the tissue. Spectroscopic studies combined with imaging have been used to produce brain images of 129Xe in the rat head. This work establishes that nuclear polarization produced in the gas phases survives transport to the brain where it may be imaged. Increases in polarization and delivered volume of 129Xe will allow clinical measurements of regional blood flow.

Hyperpolarized 129Xe MRI of the Human Lung

PubMed Central

Mugler, John P.; Altes, Talissa A.

2012-01-01

By permitting direct visualization of the airspaces of the lung, MR imaging using hyperpolarized gases provides unique strategies for evaluating pulmonary structure and function. Although the vast majority of research in humans has been performed using hyperpolarized 3He, recent contraction in the supply of 3He and consequent increases in price have turned attention to the alternative agent, hyperpolarized 129Xe. Compared to 3He, 129Xe yields reduced signal due to its smaller magnetic moment. Nonetheless, taking advantage of advances in gas-polarization technology, recent studies in humans using techniques for measuring ventilation, diffusion, and partial pressure of oxygen have demonstrated results for hyperpolarized 129Xe comparable to those previously demonstrated using hyperpolarized 3He. In addition, xenon has the advantage of readily dissolving in lung tissue and blood following inhalation, which makes hyperpolarized 129Xe particularly attractive for exploring certain characteristics of lung function, such as gas exchange and uptake, which cannot be accessed using 3He. Preliminary results from methods for imaging 129Xe dissolved in the human lung suggest that these approaches will provide new opportunities for quantifying relationships among gas delivery, exchange, and transport, and thus show substantial potential to broaden our understanding of lung disease. Finally, recent changes in the commercial landscape of the hyperpolarized-gas field now make it possible for this innovative technology to move beyond the research lab. PMID:23355432

Development Considerations for Nanocrystal Drug Products.

PubMed

Chen, Mei-Ling; John, Mathew; Lee, Sau L; Tyner, Katherine M

2017-05-01

Nanocrystal technology has emerged as a valuable tool for facilitating the delivery of poorly water-soluble active pharmaceutical ingredients (APIs) and enhancing API bioavailability. To date, the US Food and Drug Administration (FDA) has received over 80 applications for drug products containing nanocrystals. These products can be delivered by different routes of administration and are used in a variety of therapeutic areas. To aid in identifying key developmental considerations for these products, a retrospective analysis was performed on the submissions received by the FDA to date. Over 60% of the submissions were for the oral route of administration. Based on the Biopharmaceutics Classification System (BCS), most nanocrystal drugs submitted to the FDA are class II compounds that possess low aqueous solubility and high intestinal permeability. Impact of food on drug bioavailability was reduced for most nanocrystal formulations as compared with their micronized counterparts. For all routes of administration, dose proportionality was observed for some, but not all, nanocrystal products. Particular emphasis in the development of nanocrystal products was placed on the in-process tests and controls at critical manufacturing steps (such as milling process), mitigation and control of process-related impurities, and the stability of APIs or polymorphic form (s) during manufacturing and upon storage. This emphasis resulted in identifying challenges to the development of these products including accurate determination of particle size (distribution) of drug substance and/or nanocrystal colloidal dispersion, identification of polymorphic form (s), and establishment of drug substance/product specifications.

Cellulose nanocrystals: synthesis, functional properties, and applications

PubMed Central

George, Johnsy; Sabapathi, SN

2015-01-01

Cellulose nanocrystals are unique nanomaterials derived from the most abundant and almost inexhaustible natural polymer, cellulose. These nanomaterials have received significant interest due to their mechanical, optical, chemical, and rheological properties. Cellulose nanocrystals primarily obtained from naturally occurring cellulose fibers are biodegradable and renewable in nature and hence they serve as a sustainable and environmentally friendly material for most applications. These nanocrystals are basically hydrophilic in nature; however, they can be surface functionalized to meet various challenging requirements, such as the development of high-performance nanocomposites, using hydrophobic polymer matrices. Considering the ever-increasing interdisciplinary research being carried out on cellulose nanocrystals, this review aims to collate the knowledge available about the sources, chemical structure, and physical and chemical isolation procedures, as well as describes the mechanical, optical, and rheological properties, of cellulose nanocrystals. Innovative applications in diverse fields such as biomedical engineering, material sciences, electronics, catalysis, etc, wherein these cellulose nanocrystals can be used, are highlighted. PMID:26604715

Luminescent Characteristics of a Pulsed Discharge Plasma in Xe-KBr Mixture

NASA Astrophysics Data System (ADS)

Heneral, A. A.; Zhmenyak, Y. V.

2018-03-01

A mixture of xenon with a nontoxic halogen carrier Xe-KBr is used to create a plasma radiation source at the 282-nm transition of the XeBr* molecule excited by a high-voltage pulsed-periodic discharge. The luminescence spectra of the plasma of a longitudinal pulsed-periodic discharge in the Xe-KBr mixture at low pressures are studied experimentally. The most intense UV bands of exciplex XeBr* molecules are recorded in the spectral range of 250-350 nm. The spectral, temporal, and energetic characteristics of the radiation source are presented, as well as the dependence of the XeBr* exciplex molecule formation efficiency on the discharge excitation conditions. The optimal conditions for the excitation of UV radiation in the pulsed-periodic discharge plasma are determined.

Hydrothermal synthesis of tungsten doped tin dioxide nanocrystals

NASA Astrophysics Data System (ADS)

Zhou, Cailong; Li, Yufeng; Chen, Yiwen; Lin, Jing

2018-01-01

Tungsten doped tin dioxide (WTO) nanocrystals were synthesized through a one-step hydrothermal method. The structure, composition and morphology of WTO nanocrystals were characterized by x-ray diffraction, x-ray photoelectron spectroscopy, energy dispersive x-ray spectroscopy, UV-vis diffuse reflectance spectra, zeta potential analysis and high-resolution transmission electron microscopy. Results show that the as-prepared WTO nanocrystals were rutile-type structure with the size near 13 nm. Compared with the undoped tin dioxide nanocrystals, the WTO nanocrystals possessed better dispersity in ethanol phase and formed transparent sol.

Xe isotopic constraints on cycling of deep Earth volatiles

NASA Astrophysics Data System (ADS)

Parai, R.; Mukhopadhyay, S.

2017-12-01

The modern deep Earth volatile budget reflects primordial volatiles delivered during accretion, radiogenic ingrowth of volatile species (e.g., 40Ar produced by 40K decay), outgassing in association with mantle processing, and regassing via subduction. The noble gases are unique volatile tracers in that they are chemically inert, but are thought to be trapped within hydrous alteration phases in downwelling lithologies. Noble gases thus provide a tracer of volatile transport between the deep Earth and surface reservoirs. Constraints on the fluxes of noble gases between deep Earth and surface reservoirs over time can accordingly be used to provide insight into temperature conditions at subduction zones, limits on volatile cycling, and the evolving distribution of major volatile species in terrestrial reservoirs over time. Xe isotope systematics in mantle-derived rocks show that 80-90% of the mantle Xe budget is derived from recycling of atmospheric Xe, indicating that atmospheric Xe is retained in subducting slabs beyond depths of magma generation in subduction zones over Earth history. We present an integrated model of Xe cycling between the mantle and atmosphere in association with mantle processing over Earth history. We test a wide variety of outgassing and regassing rates and take the evolution of the atmospheric Xe isotopic composition [e.g., 1] into account. Models in which the deep Earth transitions from a net outgassing to net regassing regime best satisfy Xe isotopic constraints from mantle-derived rocks [2-6]. [1] Avice et al., 2017; Nature Communications, 8; [2] Mukhopadhyay, 2012, Nature 486, 101-104; [3] Parai et al., 2012, EPSL 359-360, 227-239; [4] Parai and Mukhopadhay, 2015, G-cubed 16, 719-735; [5] Peto et al., 2013, EPSL 369-370, 13-23; [6] Tucker et al., 2012, EPSL 355-356, 244-254.

Chalcogenide Aerogels as Sorbents for Noble Gases (Xe, Kr)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Subrahmanyam, Kota S.; Spanopoulos, Ioannis; Chun, Jaehun

High surface MoSx and SbSx chalcogels were studied for Xe/Kr gas separation. The intrinsic soft character of the chalcogel framework is a unique property among the large family of porous materials and offers a potential new approach towards the selective separation of Xe over Kr. Among these chalcogels, MoSx shows the highest Xe and Kr uptake, reaching 0.69 mmol g-1 (1.05 mmol cm-3) and 0.28 mmol g-1 (0.42 mmol cm-3) respectively, at 273 K and 1 bar. The corresponding isosteric heat of adsorption at zero coverage (Qst0) is 22.8 and 18.6 kJ mol-1 and both are the highest among themore » selected chalcogels. The IAST (10:90) Xe/Kr selectivity at 273 K for MoSx is 6.0 while for SbSx chalcogels varies in the range 2.0-2.8. The higher formal charge of molybdenum, Mo4+, in MoSx versus that of antimony, Sb3+, in SbSx coupled with its larger atomic size could induce higher polarizability in the MoSx framework and therefore higher Xe/Kr selectivity.« less

Stellar laboratories . VIII. New Zr iv-vii, Xe iv-v, and Xe vii oscillator strengths and the Al, Zr, and Xe abundances in the hot white dwarfs G191-B2B and RE 0503-289

NASA Astrophysics Data System (ADS)

Rauch, T.; Gamrath, S.; Quinet, P.; Löbling, L.; Hoyer, D.; Werner, K.; Kruk, J. W.; Demleitner, M.

2017-03-01

Context. For the spectral analysis of high-resolution and high-signal-to-noise spectra of hot stars, state-of-the-art non-local thermodynamic equilibrium (NLTE) model atmospheres are mandatory. These are strongly dependent on the reliability of the atomic data that is used for their calculation. Aims: To search for zirconium and xenon lines in the ultraviolet (UV) spectra of G191-B2B and RE 0503-289, new Zr iv-vii, Xe iv-v, and Xe vii oscillator strengths were calculated. This allows, for the first time, determination of the Zr abundance in white dwarf (WD) stars and improvement of the Xe abundance determinations. Methods: We calculated Zr iv-vii, Xe iv-v, and Xe vii oscillator strengths to consider radiative and collisional bound-bound transitions of Zr and Xe in our NLTE stellar-atmosphere models for the analysis of their lines exhibited in UV observations of the hot WDs G191-B2B and RE 0503-289. Results: We identified one new Zr iv, 14 new Zr v, and ten new Zr vi lines in the spectrum of RE 0503-289. Zr was detected for the first time in a WD. We measured a Zr abundance of -3.5 ± 0.2 (logarithmic mass fraction, approx. 11 500 times solar). We identified five new Xe vi lines and determined a Xe abundance of -3.9 ± 0.2 (approx. 7500 times solar). We determined a preliminary photospheric Al abundance of -4.3 ± 0.2 (solar) in RE 0503-289. In the spectra of G191-B2B, no Zr line was identified. The strongest Zr iv line (1598.948 Å) in our model gave an upper limit of -5.6 ± 0.3 (approx. 100 times solar). No Xe line was identified in the UV spectrum of G191-B2B and we confirmed the previously determined upper limit of -6.8 ± 0.3 (ten times solar). Conclusions: Precise measurements and calculations of atomic data are a prerequisite for advanced NLTE stellar-atmosphere modeling. Observed Zr iv-vi and Xe vi-vii line profiles in the UV spectrum of RE 0503-289 were simultaneously well reproduced with our newly calculated oscillator strengths. Based on observations

Optical determination of crystal phase in semiconductor nanocrystals

PubMed Central

Lim, Sung Jun; Schleife, André; Smith, Andrew M.

2017-01-01

Optical, electronic and structural properties of nanocrystals fundamentally derive from crystal phase. This is especially important for polymorphic II–VI, III–V and I-III-VI2 semiconductor materials such as cadmium selenide, which exist as two stable phases, cubic and hexagonal, each with distinct properties. However, standard crystallographic characterization through diffraction yields ambiguous phase signatures when nanocrystals are small or polytypic. Moreover, diffraction methods are low-throughput, incompatible with solution samples and require large sample quantities. Here we report the identification of unambiguous optical signatures of cubic and hexagonal phases in II–VI nanocrystals using absorption spectroscopy and first-principles electronic-structure theory. High-energy spectral features allow rapid identification of phase, even in small nanocrystals (∼2 nm), and may help predict polytypic nanocrystals from differential phase contributions. These theoretical and experimental insights provide simple and accurate optical crystallographic analysis for liquid-dispersed nanomaterials, to improve the precision of nanocrystal engineering and improve our understanding of nanocrystal reactions. PMID:28513577

Method of synthesizing pyrite nanocrystals

DOEpatents

Wadia, Cyrus; Wu, Yue

2013-04-23

A method of synthesizing pyrite nanocrystals is disclosed which in one embodiment includes forming a solution of iron (III) diethyl dithiophosphate and tetra-alkyl-ammonium halide in water. The solution is heated under pressure. Pyrite nanocrystal particles are then recovered from the solution.

Ultrasonication of Bismuth Telluride Nanocrystals Fabricated by Solvothermal Method

NASA Technical Reports Server (NTRS)

Chu, Sang-Hyon; Choi, Sang H.; Kim, Jae-Woo; King, Glen C.; Elliott, James R.

2006-01-01

The objective of this study is to evaluate the effect of ultrasonication on bismuth telluride nanocrystals prepared by solvothermal method. In this study, a low dimensional nanocrystal of bismuth telluride (Bi2Te3) was synthesized by a solvothermal process in an autoclave at 180 C and 200 psi. During the solvothermal reaction, organic surfactants effectively prevented unwanted aggregation of nanocrystals in a selected solvent while controlling the shape of the nanocrystal. The atomic ratio of bismuth and tellurium was determined by energy dispersive spectroscopy (EDS). The cavitational energy created by the ultrasonic probe was varied by the ultrasonication process time, while power amplitude remained constant. The nanocrystal size and its size distribution were measured by field emission scanning electron microscopy (FESEM) and a dynamic light scattering system. When the ultrasonication time increased, the average size of bismuth telluride nanocrystal gradually increased due to the direct collision of nanocrystals. The polydispersity of the nanocrystals showed a minimum when the ultrasonication was applied for 5 min. Keywords: bismuth telluride, nanocrystal, low-dimensional, ultrasonication, solvothermal

Optical properties of silicon nanocrystals synthesized in supercritical fluids

NASA Astrophysics Data System (ADS)

Pell, Lindsay; Korgel, Brian A.

2002-11-01

We developed a supercritical solution phase synthesis of silicon nanocrystals. High temperature and pressure (500°C, >140 bar) conditions allow a wet chemical approach to this challenging synthesis. Diphenylsilane was used as a silicon precursor and long chain thiols and alcohols were used to sterically stabilize the luminescent nanocrystals. Moderate size separation was achieved via size exclusion chromatography using crosslinked styrene divinylbenzene beads. Size separated fractions of silicon nanocrystals exhibit quantum efficiencies of 12% while polydisperse samples have quantum efficiencies of 5%. Nanocrystal size distributions have been determined with transmission electron microscopy and further characterized with atomic force microscopy (AFM). These silicon nanocrystals have size tunable photoluminescence as indicated by their ensemble spectroscopy and further verified through AFM and single nanocrystal photoluminescence spectroscopy. Fluorescence intermittency (characteristic of single CdSe nanocrystals) is present in our isolated silicon nanocrystals and is one of the criteria used to distinguish single crystals from clusters of particles.

High-temperature crystallization of nanocrystals into three-dimensional superlattices

DOE PAGES

Wu, Liheng; Willis, Joshua J.; McKay, Ian Salmon; ...

2017-07-31

Crystallization of colloidal nanocrystals into superlattices represents a practical bottom-up process with which to create ordered metamaterials with emergent functionalities. With precise control over the size, shape and composition of individual nanocrystals, various single-and multi-component nanocrystal superlattices have been produced, the lattice structures and chemical compositions of which can be accurately engineered. Nanocrystal superlattices are typically prepared by carefully controlling the assembly process through solvent evaporation or destabilization or through DNA-guided crystallization. Slow solvent evaporation or cooling of nanocrystal solutions (over hours or days) is the key element for successful crystallization processes. Here we report the rapid growth (seconds) ofmore » micrometre-sized, face-centred-cubic, three-dimensional nanocrystal superlattices during colloidal synthesis at high temperatures (more than 230 degrees Celsius). Using in situ small-angle X-ray scattering, we observe continuous growth of individual nanocrystals within the lattices, which results in simultaneous lattice expansion and fine nanocrystal size control due to the superlattice templates. Thermodynamic models demonstrate that balanced attractive and repulsive interparticle interactions dictated by the ligand coverage on nanocrystal surfaces and nanocrystal core size are responsible for the crystallization process. The interparticle interactions can also be controlled to form different superlattice structures, such as hexagonal close-packed lattices. In conclusion, the rational assembly of various nanocrystal systems into novel materials is thus facilitated for both fundamental research and for practical applications in the fields of magnetics, electronics and catalysis.« less

High-temperature crystallization of nanocrystals into three-dimensional superlattices.

PubMed

Wu, Liheng; Willis, Joshua J; McKay, Ian Salmon; Diroll, Benjamin T; Qin, Jian; Cargnello, Matteo; Tassone, Christopher J

2017-08-10

Crystallization of colloidal nanocrystals into superlattices represents a practical bottom-up process with which to create ordered metamaterials with emergent functionalities. With precise control over the size, shape and composition of individual nanocrystals, various single- and multi-component nanocrystal superlattices have been produced, the lattice structures and chemical compositions of which can be accurately engineered. Nanocrystal superlattices are typically prepared by carefully controlling the assembly process through solvent evaporation or destabilization or through DNA-guided crystallization. Slow solvent evaporation or cooling of nanocrystal solutions (over hours or days) is the key element for successful crystallization processes. Here we report the rapid growth (seconds) of micrometre-sized, face-centred-cubic, three-dimensional nanocrystal superlattices during colloidal synthesis at high temperatures (more than 230 degrees Celsius). Using in situ small-angle X-ray scattering, we observe continuous growth of individual nanocrystals within the lattices, which results in simultaneous lattice expansion and fine nanocrystal size control due to the superlattice templates. Thermodynamic models demonstrate that balanced attractive and repulsive interparticle interactions dictated by the ligand coverage on nanocrystal surfaces and nanocrystal core size are responsible for the crystallization process. The interparticle interactions can also be controlled to form different superlattice structures, such as hexagonal close-packed lattices. The rational assembly of various nanocrystal systems into novel materials is thus facilitated for both fundamental research and for practical applications in the fields of magnetics, electronics and catalysis.

High-temperature crystallization of nanocrystals into three-dimensional superlattices

NASA Astrophysics Data System (ADS)

Wu, Liheng; Willis, Joshua J.; McKay, Ian Salmon; Diroll, Benjamin T.; Qin, Jian; Cargnello, Matteo; Tassone, Christopher J.

2017-08-01

Crystallization of colloidal nanocrystals into superlattices represents a practical bottom-up process with which to create ordered metamaterials with emergent functionalities. With precise control over the size, shape and composition of individual nanocrystals, various single- and multi-component nanocrystal superlattices have been produced, the lattice structures and chemical compositions of which can be accurately engineered. Nanocrystal superlattices are typically prepared by carefully controlling the assembly process through solvent evaporation or destabilization or through DNA-guided crystallization. Slow solvent evaporation or cooling of nanocrystal solutions (over hours or days) is the key element for successful crystallization processes. Here we report the rapid growth (seconds) of micrometre-sized, face-centred-cubic, three-dimensional nanocrystal superlattices during colloidal synthesis at high temperatures (more than 230 degrees Celsius). Using in situ small-angle X-ray scattering, we observe continuous growth of individual nanocrystals within the lattices, which results in simultaneous lattice expansion and fine nanocrystal size control due to the superlattice templates. Thermodynamic models demonstrate that balanced attractive and repulsive interparticle interactions dictated by the ligand coverage on nanocrystal surfaces and nanocrystal core size are responsible for the crystallization process. The interparticle interactions can also be controlled to form different superlattice structures, such as hexagonal close-packed lattices. The rational assembly of various nanocrystal systems into novel materials is thus facilitated for both fundamental research and for practical applications in the fields of magnetics, electronics and catalysis.

Light-emitting Ga-oxide nanocrystals in glass: a new paradigm for low-cost and robust UV-to-visible solar-blind converters and UV emitters.

PubMed

Sigaev, Vladimir N; Golubev, Nikita V; Ignat'eva, Elena S; Paleari, Alberto; Lorenzi, Roberto

2014-01-01

Wide-bandgap nanocrystals are an inexhaustible source of tuneable functions potentially addressing most of the demand for new light emitting systems. However, the implementation of nanocrystal properties in real devices is not straightforward if a robust and stable optical component is required as a final result. The achievement of efficient light emission from dense dispersions of Ga-oxide nanocrystals in UV-grade glass can be a breakthrough in this regard. Such a result would permit the fabrication of low cost UV-to-visible converters for monitoring UV-emitting events on a large-scale - from invisible hydrogen flames to corona dispersions. From this perspective, γ-Ga₂O₃ nanocrystals are developed by phase separation in Ga-alkali-germanosilicate glasses, obtaining optical materials based on a UV transparent matrix. Band-to-band UV-excitation of light emission from donor-acceptor pair (DAP) recombination is investigated for the first time in embedded γ-Ga₂O₃. The analysis of the decay kinetics gives unprecedented evidence that nanosized confinement of DAP recombination can force a nanophase to the efficient response of exactly balanced DAPs. The results, including a proof of concept of UV-to-visible viewer, definitely demonstrate the feasibility of workable glass-based fully inorganic nanostructured materials with emission properties borrowed from Ga₂O₃ single-crystals and tailored by the nanocrystal size.

Transition-Metal Decorated Aluminum Nanocrystals.

PubMed

Swearer, Dayne F; Leary, Rowan K; Newell, Ryan; Yazdi, Sadegh; Robatjazi, Hossein; Zhang, Yue; Renard, David; Nordlander, Peter; Midgley, Paul A; Halas, Naomi J; Ringe, Emilie

2017-10-24

Recently, aluminum has been established as an earth-abundant alternative to gold and silver for plasmonic applications. Particularly, aluminum nanocrystals have shown to be promising plasmonic photocatalysts, especially when coupled with catalytic metals or oxides into "antenna-reactor" heterostructures. Here, a simple polyol synthesis is presented as a flexible route to produce aluminum nanocrystals decorated with eight varieties of size-tunable transition-metal nanoparticle islands, many of which have precedence as heterogeneous catalysts. High-resolution and three-dimensional structural analysis using scanning transmission electron microscopy and electron tomography shows that abundant nanoparticle island decoration in the catalytically relevant few-nanometer size range can be achieved, with many islands spaced closely to their neighbors. When coupled with the Al nanocrystal plasmonic antenna, these small decorating islands will experience increased light absorption and strong hot-spot generation. This combination makes transition-metal decorated aluminum nanocrystals a promising material platform to develop plasmonic photocatalysis, surface-enhanced spectroscopies, and quantum plasmonics.

Mass and Double-Beta-Decay Q Value of {sup 136}Xe

DOE Office of Scientific and Technical Information (OSTI.GOV)

Redshaw, Matthew; Wingfield, Elizabeth; McDaniel, Joseph

The atomic mass of {sup 136}Xe has been measured by comparing cyclotron frequencies of single ions in a Penning trap. The result, with 1 standard deviation uncertainty, is M({sup 136}Xe)=135.907 214 484 (11) u. Combined with previous results for the mass of {sup 136}Ba [Audi, Wapstra, and Thibault, Nucl. Phys. A 729, 337 (2003)], this gives a Q value (M[{sup 136}Xe]-M[{sup 136}Ba])c{sup 2}=2457.83(37) keV, sufficiently precise for ongoing searches for the neutrinoless double-beta decay of {sup 136}Xe.

High-Bandgap Silicon Nanocrystal Solar Cells: Device Fabrication, Characterization, and Modeling

NASA Astrophysics Data System (ADS)

Löper, Philipp; Canino, Mariaconcetta; Schnabel, Manuel; Summonte, Caterina; Janz, Stefan; Zacharias, Margit

Silicon nanocrystals (Si NCs) embedded in Si-based dielectrics provide a Si-based high-bandgap material (1.7 eV) and enable the construction of crystalline Si tandem solar cells. This chapter focusses on Si NC embedded in silicon carbide, because silicon carbide offers electrical conduction through the matrix material. The material development is reviewed, and optical modeling is introduced as a powerful method to monitor the four material components, amorphous and crystalline silicon as well as amorphous and crystalline silicon carbide. In the second part of this chapter, recent device developments for the photovoltaic characterization of Si NCs are examined. The controlled growth of Si NCs involves high-temperature annealing which deteriorates the properties of any previously established selective contacts. A membrane-based device is presented to overcome these limitations. In this approach, the formation of both selective contacts is carried out after high-temperature annealing and is therefore not affected by the latter. We examine p-i-n solar cells with an intrinsic region made of Si NCs embedded in silicon carbide. Device failure due to damaged insulation layers is analyzed by light beam-induced current measurements. An optical model of the device is presented for improving the cell current. A characterization scheme for Si NC p-i-n solar cells is presented which aims at determining the fundamental transport and recombination properties, i.e., the effective mobility lifetime product, of the nanocrystal layer at device level. For this means, an illumination-dependent analysis of Si NC p-i-n solar cells is carried out within the framework of the constant field approximation. The analysis builds on an optical device model, which is used to assess the photogenerated current in each of the device layers. Illumination-dependent current-voltage curves are modelled with a voltage-dependent current collection function with only two free parameters, and excellent

Nuclear structure studies in highly neutron-deficient (114,116)Xe

NASA Astrophysics Data System (ADS)

Degraaf, James Hendrick

Lifetimes of nuclear states in 114Xe and 116Xe were measured for the first time; these nuclei represent the most neutron-deficient isotopes of xenon for which lifetimes have now been measured. The fusion-evaporation reactions 58Ni(60Ni, 2p)116Xe at 223 MeV beam energy and 58Ni(58Ni, 2p)114Xe at 215 MeV beam energy were used. Lifetimes were measured using the Recoil Distance Method (RDM) with the 8π gamma-ray spectrometer at Chalk River Laboratories. The new measurements of the B(E2;2+/to 0+) strength in these nuclei, coupled with the recent measurements for heavier xenon isotopes, are well described within the framework of the O(6) symmetry limit of the Interacting Boson Approximation. The octupole nature of the negative parity side-band was also studied, and the lifetime measurements indicate a change from a K/approx 3 structure in heavier xenon isotopes to a K/approx 0,/ 1 structure in 114Xe.

Xe adsorption site distributions on Pt(111), Pt(221) and Pt(531)

NASA Astrophysics Data System (ADS)

Gellman, Andrew J.; Baker, L.; Holsclaw, B. S.

2016-04-01

The ideal structures of the Pt(111), Pt(221) and Pt(531) surfaces expose adsorption sites that can be qualitatively described as terrace sites on Pt(111), both step and terrace sites on Pt(221), and kink sites on Pt(531). The real surface structures of these surfaces can be complicated by imperfections such as misorientation, reconstruction and thermal roughening, all of which will influence their distributions of adsorption sites. Xe adsorption sites on the Pt(111), Pt(221) and Pt(531) surfaces have been probed using both photoemission of adsorbed Xe (PAX) and temperature programmed desorption (TPD) of Xe. Both PAX and Xe TPD are sensitive to the adsorption sites of the Xe and serve as complementary means of assessing the distributions of adsorption sites on these three Pt surfaces. The adsorption of Xe is sufficiently sensitive to detect the presence of residual steps on the Pt(111) surface at a density of 1.5% step atoms per Pt atom. On the Pt(221) surface, PAX and Xe TPD reveal adsorption at both terrace and step sites simultaneously. Although the ideal structure of the Pt(531) surface has no well-defined steps or terraces, Xe adsorption indicates that its adsorption sites are best described as a distribution of both step and kink sites with roughly twice as many steps sites as kinks.

Engineering Plasmonic Nanocrystal Coupling through Template-Assisted Self-Assembly

NASA Astrophysics Data System (ADS)

Greybush, Nicholas J.

The construction of materials from nanocrystal building blocks represents a powerful new paradigm for materials design. Just as nature's materials orchestrate intricate combinations of atoms from the library of the periodic table, nanocrystal "metamaterials" integrate individual nanocrystals into larger architectures with emergent collective properties. The individual nanocrystal "meta-atoms" that make up these materials are themselves each a nanoscale atomic system with tailorable size, shape, and elemental composition, enabling the creation of hierarchical materials with predesigned structure at multiple length scales. However, an improved fundamental understanding of the interactions among individual nanocrystals is needed in order to translate this structural control into enhanced functionality. The ability to form precise arrangements of nanocrystals and measure their collective properties is therefore essential for the continued development of nanocrystal metamaterials. In this dissertation, we utilize template-assisted self-assembly and spatially-resolved spectroscopy to form and characterize individual nanocrystal oligomers. At the intersection of "top-down" and "bottom-up" nanoscale patterning schemes, template-assisted self-assembly combines the design freedom of lithography with the chemical control of colloidal synthesis to achieve unique nanocrystal configurations. Here, we employ shape-selective templates to assemble new plasmonic structures, including heterodimers of Au nanorods and upconversion phosphors, a series of hexagonally-packed Au nanocrystal oligomers, and triangular formations of Au nanorods. Through experimental analysis and numerical simulation, we elucidate the means through which inter-nanocrystal coupling imparts collective optical properties to the plasmonic assemblies. Our self-assembly and measurement strategy offers a versatile platform for exploring optical interactions in a wide range of material systems and application areas.

Hyperpolarized (129)Xe T (1) in oxygenated and deoxygenated blood

NASA Technical Reports Server (NTRS)

Albert, M. S.; Balamore, D.; Kacher, D. F.; Venkatesh, A. K.; Jolesz, F. A.

2000-01-01

The viability of the new technique of hyperpolarized (129)Xe MRI (HypX-MRI) for imaging organs other than the lungs depends on whether the spin-lattice relaxation time, T(1), of (129)Xe is sufficiently long in the blood. In previous experiments by the authors, the T(1) was found to be strongly dependent upon the oxygenation of the blood, with T(1) increasing from about 3 s in deoxygenated samples to about 10 s in oxygenated samples. Contrarily, Tseng et al. (J. Magn. Reson. 1997; 126: 79-86) reported extremely long T(1) values deduced from an indirect experiment in which hyperpolarized (129)Xe was used to create a 'blood-foam'. They found that oxygenation decreased T(1). Pivotal to their experiment is the continual and rapid exchange of hyperpolarized (129)Xe between the gas phase (within blood-foam bubbles) and the dissolved phase (in the skin of the bubbles); this necessitated a complicated analysis to extract the T(1) of (129)Xe in blood. In the present study, the experimental design minimizes gas exchange after the initial bolus of hyperpolarized (129)Xe has been bubbled through the sample. This study confirms that oxygenation increases the T(1) of (129)Xe in blood, from about 4 s in freshly drawn venous blood, to about 13 s in blood oxygenated to arterial levels, and also shifts the red blood cell resonance to higher frequency. Copyright 2000 John Wiley & Sons, Ltd. Abbreviations used BOLD blood oxygen level dependent NOE nuclear overhouses effect PO(2) oxygen partial pressure RBC red blood cells RF radio frequency SNR signal-to-noise ratio.

CdSe/CdS semiconductor quantum rods as robust fluorescent probes for paraffin-embedded tissue imaging.

PubMed

Zacheo, Antonella; Quarta, Alessandra; Mangoni, Antonella; Pompa, Pier Paolo; Mastria, Rosanna; Capogrossi, Maurizio C; Rinaldi, Ross; Pellegrino, Teresa

2011-09-01

Immunofluorescence techniques on formalin fixed paraffin-embedded sections allow for the evaluation of the expression and spatial distribution of specific markers in patient tissue specimens or for monitoring the fate of labeled cells after in vivo injection. This technique suffers however from the auto-fluorescence background signal of the embedded tissue that eventually confounds the analysis. Here we show that rod-like semiconductor nanocrystals (QRs), intramuscularly injected in living mice, could be clearly detected by confocal microscopy in formalin fixed paraffin-embedded tissue sections. Despite the low amount of QRs amount injected (25 picomoles), these were clearly visible after 24 h in the muscle sections and their fluorescence signal was stronger than that of CdSe/ZnS quantum dots (QDs) similarly functionalized and in the case of QRs only, the signal lasted even after 21 days after the injection. © 2011 IEEE

Neutron Inelastic Scattering on 134Xe at En = 5 - 8 MeV

NASA Astrophysics Data System (ADS)

Kidd, Mary; Tornow, Werner; Finch, Sean; Krishichayan, Fnu; Bhike, Megha

2017-09-01

Neutrinoless double-beta decay (0 νββ) studies are both the best way to determine the Majorana nature of the neutrino and determine its effective mass. The two main experiments searching for 0 νββ -decay of 136Xe (Q value = 2457.8 keV) are Kamland-Zen and EXO-200. Though both experiments have enriched 136Xe targets, these targets still contain significant quantities of 134Xe. Recently, a new nuclear level was discovered in 134Xe that decays to the ground state emitting a 2485.7 keV gamma ray. The γ-ray production cross section for this branch was found to be on the order of 10 mb for incident neutron energies of 2.5-4.5 MeV. Here, we have extended the investigation of this level to higher incident neutron energies, and further explore the potential neutron-induced backgrounds on both 134Xe and 136Xe for extended neutron energies. We will report our preliminary results for neutron inelastic scattering on 134Xe in applications to 0 νββ decay searches. NSF PHY-1614348, DE-FG02-97ER41033.

Nanocrystal Targeting In Vivo

DTIC Science & Technology

2002-08-01

Shearwater Polymers , Huntsville, AL) was thiolated with iminothiolane. Thiolated PEG was directly added to a solution of mercaptoacetic acid- coated qdots...Nanocrystal targeting in vivo Maria E. Åkerman*†‡, Warren C. W. Chan†‡, Pirjo Laakkonen*, Sangeeta N. Bhatia†, and Erkki Ruoslahti*§ *Cancer Research...set out to explore the feasibility of in vivo targeting by using semiconductor quantum dots (qdots). Qdots are small (᝺ nm) inorganic nanocrystals

Colloidal nanocrystals and method of making

DOEpatents

Kahen, Keith

2015-10-06

A tight confinement nanocrystal comprises a homogeneous center region having a first composition and a smoothly varying region having a second composition wherein a confining potential barrier monotonically increases and then monotonically decreases as the smoothly varying region extends from the surface of the homogeneous center region to an outer surface of the nanocrystal. A method of producing the nanocrystal comprises forming a first solution by combining a solvent and at most two nanocrystal precursors; heating the first solution to a nucleation temperature; adding to the first solution, a second solution having a solvent, at least one additional and different precursor to form the homogeneous center region and at most an initial portion of the smoothly varying region; and lowering the solution temperature to a growth temperature to complete growth of the smoothly varying region.

Measuring the Valence of Nanocrystal Surfaces

DOE Office of Scientific and Technical Information (OSTI.GOV)

Owen, Jonathan Scharle

2016-11-30

The goal of this project is to understand and control the interplay between nanocrystal stoichiometry, surface ligand binding and exchange, and the optoelectronic properties of semiconductor nanocrystals in solution and in thin solid films. We pursued three research directions with this goal in mind: 1) We characterized nanocrystal stoichiometry and its influence on the binding of L-type and X-type ligands, including the thermodynamics of binding and the kinetics of ligand exchange. 2) We developed a quantitative understanding of the relationship between surface ligand passivation and photoluminescence quantum yield. 3) We developed methods to replace the organic ligands on the nanocrystalmore » with halide ligands and controllably deposit these nanocrystals into thin films, where electrical measurements were used to investigate the electrical transport and internanocrystal electronic coupling.« less

Programming A Molecular Relay for Ultrasensitive Biodetection through 129 Xe NMR

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Yanfei; Roose, Benjamin W.; Philbin, John P.

2015-12-21

We reported a supramolecular strategy for detecting specific proteins in complex media by using hyperpolarized 129Xe NMR. A cucurbit[6]uril (CB[6])-based molecular relay was programmed for three sequential equilibrium conditions by designing a two-faced guest (TFG) that initially binds CB[6] and blocks the CB[6]–Xe interaction. Moreover, the protein analyte recruits the TFG and frees CB[6] for Xe binding. TFGs containing CB[6]- and carbonic anhydrase II (CAII)-binding domains were synthesized in one or two steps. X-ray crystallography confirmed TFG binding to Zn 2+ in the deep CAII active-site cleft, which precludes simultaneous CB[6] binding. The molecular relay was reprogrammed to detect avidinmore » by using a different TFG. Finally, Xe binding by CB[6] was detected in buffer and in E. coli cultures expressing CAII through ultrasensitive 129Xe NMR spectroscopy.« less

Optical Properties of CdSe/ZnS Nanocrystals

PubMed Central

Gaigalas, Adolfas K; DeRose, Paul; Wang, Lili; Zhang, Yu-Zhong

2014-01-01

Measurements are presented of the absorbance, fluorescence emission, fluorescence quantum yield, and fluorescence lifetime of CdSe/ZnS nanocrystals, also known as quantum dots (QDs). The study included three groups of nanocrystals whose surfaces were either passivated with organic molecules, modified further with carboxyl groups, or conjugated with CD14 mouse anti-human antibodies. The surface modifications had observable effects on the optical properties of the nanocrystals. The oscillator strength (OS) of the band edge transition was about 1.0 for the nanocrystals emitting at 565 nm, 605 nm, and 655 nm. The OS could not be determined for QDs with emission at 700 nm and 800 nm. The fluorescence lifetimes varied from 26 ns for nanocrystals emitting near 600 nm to 150 ns for nanocrystals emitting near 800 nm. The quantum yield ranged between 0.4 and 0.9 for the nanocrystals in this study. A brightness index (BI) was used to evaluate the suitability of the nanocrystal labels for flow cytometer measurements. Most QD labels are at least as bright as fluorescein for applications in flow cytometer assays with 488 nm excitation. For optimal brightness the QDs should be excited with 405 nm light. We observed a strong dependence of the QD absorbance at 250 nm on the surface modification of the QD. PMID:26601047

GraXe, graphene and xenon for neutrinoless double beta decay searches

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gómez-Cadenas, J.J.; Martín-Albo, J.; Monrabal, F.

2012-02-01

We propose a new detector concept, GraXe (to be pronounced as grace), to search for neutrinoless double beta decay in {sup 136}XE. GraXe combines a popular detection medium in rare-event searches, liquid xenon, with a new, background-free material, graphene. In our baseline design of GraXe, a sphere made of graphene-coated titanium mesh and filled with liquid xenon (LXe) enriched in the {sup 136}XE isotope is immersed in a large volume of natural LXe instrumented with photodetectors. Liquid xenon is an excellent scintillator, reasonably transparent to its own light. Graphene is transparent over a large frequency range, and impermeable to themore » xenon. Event position could be deduced from the light pattern detected in the photosensors. External backgrounds would be shielded by the buffer of natural LXe, leaving the ultra-radiopure internal volume virtually free of background. Industrial graphene can be manufactured at a competitive cost to produce the sphere. Enriching xenon in the isotope {sup 136}XE is easy and relatively cheap, and there is already near one ton of enriched xenon available in the world (currently being used by the EXO, KamLAND-Zen and NEXT experiments). All the cryogenic know-how is readily available from the numerous experiments using liquid xenon. An experiment using the GraXe concept appears realistic and affordable in a short time scale, and its physics potential is enormous.« less

Nanocrystal dispersed amorphous alloys

NASA Technical Reports Server (NTRS)

Perepezko, John H. (Inventor); Allen, Donald R. (Inventor); Foley, James C. (Inventor)

2001-01-01

Compositions and methods for obtaining nanocrystal dispersed amorphous alloys are described. A composition includes an amorphous matrix forming element (e.g., Al or Fe); at least one transition metal element; and at least one crystallizing agent that is insoluble in the resulting amorphous matrix. During devitrification, the crystallizing agent causes the formation of a high density nanocrystal dispersion. The compositions and methods provide advantages in that materials with superior properties are provided.

MARMOT simulations of Xe segregation to grain boundaries in UO2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Andersson, Anders D.; Tonks, Michael; Casillas, Luis

2012-06-20

Diffusion of Xe and U in UO{sub 2} is controlled by vacancy mechanisms and under irradiation the formation of mobile vacancy clusters is important. We derive continuum thermodynamic and diffusion models for Xe and U in UO{sub 2} based on the vacancy and cluster diffusion mechanisms established from recent density functional theory (DFT) calculations. Segregation of defects to grain boundaries in UO{sub 2} is described by combining the diffusion model with models of the interaction between Xe atoms and vacancies with grain boundaries derived from separate atomistic calculations. The diffusion and segregation models are implemented in the MOOSE/MARMOT (MBM) finitemore » element (FEM) framework and we simulate Xe redistribution for a few simple microstructures. In this report we focus on segregation to grain boundaries. The U or vacancy diffusion model as well as the coupled diffusion of vacancies and Xe have also been implemented, but results are not included in this report.« less

128Xe Lifetime Measurement Using the Coulex-Plunger Technique in Inverse Kinematics

NASA Astrophysics Data System (ADS)

Konstantinopoulos, T.; Lagoyannis, A.; Harissopulos, S.; Dewald, A.; Rother, W.; Ilie, G.; Jones, P.; Rakhila, P.; Greenlees, P.; Grahn, T.; Julin, R.; Balabanski, D. L.

2008-05-01

The lifetimes of the lowest collective yrast and non-yrast states in 128Xe were measured in a Coulomb excitation experiment using the recoil distance method (RDM) in inverse kinematics. Hereby, the Cologne plunger apparatus was employed together with the JUROGAM spectrometer. Excited states in 128Xe were populated using a 128Xe beam impinging on a natFe target with E(128Xe)~525 MeV. Recoils were detected by means of an array of solar cells placed at forward angles. Recoil-gated γ-spectra were measured at different plunger distances.

Enhanced oral bioavailability of glycyrrhetinic acid via nanocrystal formulation.

PubMed

Lei, Yaya; Kong, Yindi; Sui, Hong; Feng, Jun; Zhu, Rongyue; Wang, Wenping

2016-10-01

The purpose of this study was to prepare solid nanocrystals of glycyrrhetinic acid (GA) for improved oral bioavailability. The anti-solvent precipitation-ultrasonication method followed by freeze-drying was adopted for the preparation of GA nanocrystals. The physicochemical properties, drug dissolution and pharmacokinetic of the obtained nanocrystals were investigated. GA nanocrystals showed a mean particle size of 220 nm and shaped like short rods. The analysis results from differential scanning calorimetry and X-ray powder diffraction indicated that GA remained in crystalline state despite a huge size reduction. The equilibrium solubility and dissolution rate of GA nanocrystal were significantly improved in comparison with those of the coarse GA or the physical mixture. The bioavailability of GA nanocrystals in rats was 4.3-fold higher than that of the coarse GA after oral administration. With its rapid dissolution and absorption performance, the solid nanocrystal might be a more preferable formulation for oral administration of poorly soluble GA.

Nanocrystal assembly for tandem catalysis

DOEpatents

Yang, Peidong; Somorjai, Gabor; Yamada, Yusuke; Tsung, Chia-Kuang; Huang, Wenyu

2014-10-14

The present invention provides a nanocrystal tandem catalyst comprising at least two metal-metal oxide interfaces for the catalysis of sequential reactions. One embodiment utilizes a nanocrystal bilayer structure formed by assembling sub-10 nm platinum and cerium oxide nanocube monolayers on a silica substrate. The two distinct metal-metal oxide interfaces, CeO.sub.2--Pt and Pt--SiO.sub.2, can be used to catalyze two distinct sequential reactions. The CeO.sub.2--Pt interface catalyzed methanol decomposition to produce CO and H.sub.2, which were then subsequently used for ethylene hydroformylation catalyzed by the nearby Pt--SiO.sub.2 interface. Consequently, propanal was selectively produced on this nanocrystal bilayer tandem catalyst.

Isolating and moving single atoms using silicon nanocrystals

DOEpatents

Carroll, Malcolm S.

2010-09-07

A method is disclosed for isolating single atoms of an atomic species of interest by locating the atoms within silicon nanocrystals. This can be done by implanting, on the average, a single atom of the atomic species of interest into each nanocrystal, and then measuring an electrical charge distribution on the nanocrystals with scanning capacitance microscopy (SCM) or electrostatic force microscopy (EFM) to identify and select those nanocrystals having exactly one atom of the atomic species of interest therein. The nanocrystals with the single atom of the atomic species of interest therein can be sorted and moved using an atomic force microscope (AFM) tip. The method is useful for forming nanoscale electronic and optical devices including quantum computers and single-photon light sources.

Interfacial interactions between calcined hydroxyapatite nanocrystals and substrates.

PubMed

Okada, Masahiro; Furukawa, Keiko; Serizawa, Takeshi; Yanagisawa, Yoshihiko; Tanaka, Hidekazu; Kawai, Tomoji; Furuzono, Tsutomu

2009-06-02

Interfacial interactions between calcined hydroxyapatite (HAp) nanocrystals and surface-modified substrates were investigated by measuring adsorption behavior and adhesion strength with a quartz crystal microbalance (QCM) and a contact-mode atomic force microscope (AFM), respectively. The goal was to develop better control of HAp-nanocrystal coatings on biomedical materials. HAp nanocrystals with rodlike or spherical morphology were prepared by a wet chemical process followed by calcination at 800 degrees C with an antisintering agent to prevent the formation of sintered polycrystals. The substrate surface was modified by chemical reaction with a low-molecular-weight compound, or graft polymerization with a functional monomer. QCM measurement showed that the rodlike HAp nanocrystals adsorbed preferentially onto anionic COOH-modified substrates compared to cationic NH2- or hydrophobic CH3-modified substrates. On the other hand, the spherical nanocrystals adsorbed onto NH2- and COOH-modified substrates, which indicates that the surface properties of the HAp nanocrystals determined their adsorption behavior. The adhesion strength, which was estimated from the force required to move the nanocrystal in contact-mode AFM, on a COOH-grafted substrate prepared by graft polymerization was almost 9 times larger than that on a COOH-modified substrate prepared by chemical reaction with a low-molecular-weight compound, indicating that the long-chain polymer grafted on the substrate mitigated the surface roughness mismatch between the nanocrystal and the substrate. The adhesion strength of the nanocrystal bonded covalently by the coupling reaction to a Si(OCH3)-grafted substrate prepared by graft polymerization was approximately 1.5 times larger than that when adsorbed on the COOH-grafted substrate.

XeCl Avalanche discharge laser employing Ar as a diluent

DOEpatents

Sze, Robert C.

1981-01-01

A XeCl avalanche discharge exciplex laser which uses a gaseous lasing starting mixture of: (0.2%-0.4% chlorine donor/2.5%-10% Xe/97.3%-89.6% Ar). The chlorine donor normally comprises HCl but can also comprise CCl.sub.4 BCl.sub.3. Use of Ar as a diluent gas reduces operating pressures over other rare gas halide lasers to near atmospheric pressure, increases output lasing power of the XeCl avalanche discharge laser by 30% to exceed KrF avalanche discharge lasing outputs, and is less expensive to operate.

Submicron polymer particles containing fluorescent semiconductor nanocrystals CdSe/ZnS for bioassays.

PubMed

Generalova, Alla N; Sizova, Svetlana V; Zdobnova, Tatiana A; Zarifullina, Margarita M; Artemyev, Michail V; Baranov, Alexander V; Oleinikov, Vladimir A; Zubov, Vitaly P; Deyev, Sergey M

2011-02-01

This study aimed to design a panel of uniform particulate biochemical reagents and to test them in specific bioassays. These reagents are polymer particles of different sizes doped with semiconductor nanocrystals and conjugated with either full-size antibodies or recombinant mini-antibodies (4D5 scFv fragment) designed by genetic engineering approaches. A panel of highly fluorescent polymer particles (150-800 nm) were formed by embedding CdSe/ZnS nanocrystals (quantum dots) into preformed polyacrolein and poly(acrolein-co-styrene) particles. Morphology, content and fluorescence characteristics of the prepared materials were studied by laser correlation spectroscopy, spectrophotometry, optical and fluorescent microscopy and fluorimetry. The obtained fluorescent particles sensitized by anti-Yersinia pestis antibodies were used for rapid agglutination glass test suitable for screening analysis of Y. pestis antigen and for microtiter particle agglutination, which, owing to its speed and simplicity, is very beneficial for diagnostic detection of Y. pestis antigen. Recombinant 4D5 scFv antibodies designed and conjugated with polymer particles containing quantum dots provide multipoint highly specific binding with cancer marker HER2/neu on the surface of SKOV-3 cell.

Iron Oxide Nanocrystals for Magnetic Hyperthermia Applications

PubMed Central

Armijo, Leisha M.; Brandt, Yekaterina I.; Mathew, Dimple; Yadav, Surabhi; Maestas, Salomon; Rivera, Antonio C.; Cook, Nathaniel C.; Withers, Nathan J.; Smolyakov, Gennady A.; Adolphi, Natalie; Monson, Todd C.; Huber, Dale L.; Smyth, Hugh D. C.; Osiński, Marek

2012-01-01

Magnetic nanocrystals have been investigated extensively in the past several years for several potential applications, such as information technology, MRI contrast agents, and for drug conjugation and delivery. A specific property of interest in biomedicine is magnetic hyperthermia—an increase in temperature resulting from the thermal energy released by magnetic nanocrystals in an external alternating magnetic field. Iron oxide nanocrystals of various sizes and morphologies were synthesized and tested for specific losses (heating power) using frequencies of 111.1 kHz and 629.2 kHz, and corresponding magnetic field strengths of 9 and 25 mT. Polymorphous nanocrystals as well as spherical nanocrystals and nanowires in paramagnetic to ferromagnetic size range exhibited good heating power. A remarkable 30 °C temperature increase was observed in a nanowire sample at 111 kHz and magnetic field of 25 mT (19.6 kA/m), which is very close to the typical values of 100 kHz and 20 mT used in medical treatments. PMID:28348300

Photon-induced formation of CdS nanocrystals in selected areas of polymer matrices

DOE Office of Scientific and Technical Information (OSTI.GOV)

Athanassiou, Athanassia; Cingolani, Roberto; Tsiranidou, Elsa

2007-10-08

We demonstrate light-induced formation of semiconductor quantum dots in TOPAS registered polymer matrix with very high control of their size and their spatial localization. Irradiation with UV laser pulses of polymer films embedding Cd thiolate precursors results in the formation of cadmium sulfide nanocrystals well confined in the irradiation area, through a macroscopically nondestructive procedure for the host matrix. With increasing number of laser pulses, we accomplish the formation of nanoparticles with gradually increasing dimensions, resulting in the dynamic change of the spectra emitted by the formed nanocomposite areas. The findings are supported by x-ray diffraction and transmission electron microscopymore » measurements.« less

Imaging Human Brain Perfusion with Inhaled Hyperpolarized 129Xe MR Imaging.

PubMed

Rao, Madhwesha R; Stewart, Neil J; Griffiths, Paul D; Norquay, Graham; Wild, Jim M

2018-02-01

Purpose To evaluate the feasibility of directly imaging perfusion of human brain tissue by using magnetic resonance (MR) imaging with inhaled hyperpolarized xenon 129 ( 129 Xe). Materials and Methods In vivo imaging with 129 Xe was performed in three healthy participants. The combination of a high-yield spin-exchange optical pumping 129 Xe polarizer, custom-built radiofrequency coils, and an optimized gradient-echo MR imaging protocol was used to achieve signal sensitivity sufficient to directly image hyperpolarized 129 Xe dissolved in the human brain. Conventional T1-weighted proton (hydrogen 1 [ 1 H]) images and perfusion images by using arterial spin labeling were obtained for comparison. Results Images of 129 Xe uptake were obtained with a signal-to-noise ratio of 31 ± 9 and demonstrated structural similarities to the gray matter distribution on conventional T1-weighted 1 H images and to perfusion images from arterial spin labeling. Conclusion Hyperpolarized 129 Xe MR imaging is an injection-free means of imaging the perfusion of cerebral tissue. The proposed method images the uptake of inhaled xenon gas to the extravascular brain tissue compartment across the intact blood-brain barrier. This level of sensitivity is not readily available with contemporary MR imaging methods. © RSNA, 2017.

Targeted Molecular Imaging of Cancer Cells Using MS2-Based 129 Xe NMR

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jeong, Keunhong; Netirojjanakul, Chawita; Munch, Henrik K.

Targeted, selective, and highly sensitive 129Xe NMR nanoscale biosensors have been synthesized using a spherical MS2 viral capsid, Cryptophane A molecules, and DNA aptamers. The biosensors showed strong binding specificity toward targeted lymphoma cells (Ramos line). Hyperpolarized 129Xe NMR signal contrast and hyper-CEST 129Xe MRI image contrast indicated its promise as highly sensitive hyperpolarized 129Xe NMR nanoscale biosensor for future applications in cancer detection in vivo.

Optima XE Single Wafer High Energy Ion Implanter

DOE Office of Scientific and Technical Information (OSTI.GOV)

Satoh, Shu; Ferrara, Joseph; Bell, Edward

2008-11-03

The Optima XE is the first production worthy single wafer high energy implanter. The new system combines a state-of-art single wafer endstation capable of throughputs in excess of 400 wafers/hour with a production-proven RF linear accelerator technology. Axcelis has been evolving and refining RF Linac technology since the introduction of the NV1000 in 1986. The Optima XE provides production worthy beam currents up to energies of 1.2 MeV for P{sup +}, 2.9 MeV for P{sup ++}, and 1.5 MeV for B{sup +}. Energies as low as 10 keV and tilt angles as high as 45 degrees are also available., allowingmore » the implanter to be used for a wide variety of traditional medium current implants to ensure high equipment utilization. The single wafer endstation provides precise implant angle control across wafer and wafer to wafer. In addition, Optima XE's unique dose control system allows compensation of photoresist outgassing effects without relying on traditional pressure-based methods. We describe the specific features, angle control and dosimetry of the Optima XE and their applications in addressing the ever-tightening demands for more precise process controls and higher productivity.« less

Application of precipitation methods for the production of water-insoluble drug nanocrystals: production techniques and stability of nanocrystals.

PubMed

Xia, Dengning; Gan, Yong; Cui, Fude

2014-01-01

This review focuses on using precipitation (bottom-up) method to produce water-insoluble drug nanocrystals, and the stability issues of nanocrystals. The precipitation techniques for production of ultra-fine particles have been widely researched for last few decades. In these techniques, precipitation of solute is achieved by addition of a non-solvent for solute called anti-solvent to decrease the solvent power for the solute dissolved in a solution. The anti-solvent can be water, organic solvents or supercritical fluids. In this paper, efforts have been made to review the precipitation techniques involving the anti-solvent precipitation by simple mixing, impinging jet mixing, multi-inlet vortex mixing, the using of high-gravity, ultrasonic waves and supercritical fluids. The key to the success of yielding stable nanocrystals in these techniques is to control the nucleation kinetics and particle growth through mixing during precipitation based on crystallization theories. The stability issues of the nanocrystals, such as sedimentation, Ostwald ripening, agglomeration and cementing of crystals, change of crystalline state, and the approaches to stabilizing nanocrystals are also discussed in detail.

Optical properties of implanted Xe color centers in diamond

NASA Astrophysics Data System (ADS)

Sandstrom, Russell; Ke, Li; Martin, Aiden; Wang, Ziyu; Kianinia, Mehran; Green, Ben; Gao, Wei-bo; Aharonovich, Igor

2018-03-01

Optical properties of color centers in diamond have been the subject of intense research due to their promising applications in quantum photonics. In this work we study the optical properties of Xe related color centers implanted into nitrogen rich (type IIA) and an ultrapure, electronic grade diamond. The Xe defect has two zero phonon lines at ∼794 nm and 811 nm, which can be effectively excited using both green and red excitation, however, its emission in the nitrogen rich diamond is brighter. Near resonant excitation is performed at cryogenic temperatures and luminescence is probed under strong magnetic field. Our results are important towards the understanding of the Xe related defect and other near infrared color centers in diamond.

Enhanced luminescence of Cu-In-S nanocrystals by surface modification.

PubMed

Kim, Young-Kuk; Cho, Young-Sang; Chung, Kookchae; Choi, Chul-Jin; Shin, Pyung-Woo

2012-04-01

We have synthesized highly luminescent Cu-In-S nanocrystals by heating the mixture of metal carboxylates and alkylthiol under inert atmosphere. We modified the surface of CIS nanocrystals with zinc carboxylate and subsequent injection of alkylthiol. As a result of the surface modification, highly luminescent CIS@ZnS core/shell nanocrystals were synthesized. The luminescence quantum yield (QY) of best CIS@ZnS nanocrystals was above 50%, which is more than 10 times higher than the initial QY of CIS nanocrystals before surface modification (QY = 3%). Detailed study on the luminescence mechanism implies that etching of the surface of nanocrystals by dissociated carboxylate group (CH3COO-) and formation of epitaxial shell by Zn with sulfur from alkylthiol efficiently removed the surface defects which are major non-radiative recombination sites in semiconductor nanocrystals. In this study, we developed a novel surface modification route for monodispersed highly luminescent Cu-In-S nanocrystals with less toxic and highly stable precursors.

Composite CD-MOF nanocrystals-containing microspheres for sustained drug delivery.

PubMed

Li, Haiyan; Lv, Nana; Li, Xue; Liu, Botao; Feng, Jing; Ren, Xiaohong; Guo, Tao; Chen, Dawei; Fraser Stoddart, J; Gref, Ruxandra; Zhang, Jiwen

2017-06-08

Metal-organic frameworks (MOFs), which are typically embedded in polymer matrices as composites, are emerging as a new class of carriers for sustained drug delivery. Most of the MOFs and the polymers used so far in these composites, however, are not pharmaceutically acceptable. In the investigation reported herein, composites of γ-cyclodextrin (γ-CD)-based MOFs (CD-MOFs) and polyacrylic acid (PAA) were prepared by a solid in oil-in-oil (s/o/o) emulsifying solvent evaporation method. A modified hydrothermal protocol has been established which produces efficiently at 50 °C in 6 h micron (5-10 μm) and nanometer (500-700 nm) diameter CD-MOF particles of uniform size with smooth surfaces and powder X-ray diffraction patterns that are identical with those reported in the literature. Ibuprofen (IBU) and Lansoprazole (LPZ), both insoluble in water and lacking in stability, were entrapped with high drug loading in nanometer-sized CD-MOFs by co-crystallisation (that is more effective than impregnation) without causing MOF crystal degradation during the loading process. On account of the good dispersion of drug-loaded CD-MOF nanocrystals inside polyacrylic acid (PAA) matrices and the homogeneous distribution of the drug molecules within these crystals, the composite microspheres exhibit not only spherical shapes and sustained drug release over a prolonged period of time, but they also demonstrate reduced cell toxicity. The cumulative release rate for IBU (and LPZ) follows the trend: IBU-γ-CD complex microspheres (ca. 80% in 2 h) > IBU microspheres > IBU-CD-MOF/PAA composite microspheres (ca. 50% in 24 h). Importantly, no burst release of IBU (and LPZ) was observed from the CD-MOF/PAA composite microspheres, suggesting an even distribution of the drug as well as strong drug carrier interactions inside the CD-MOF. In summary, these composite microspheres, composed of CD-MOF nanocrystals embedded in a biocompatible polymer (PAA) matrix, constitute an efficient and

Robust and Bright Photoluminescence from Colloidal Nanocrystal/Al2O3 Composite Films Fabricated by Atomic Layer Deposition.

PubMed

Palei, Milan; Caligiuri, Vincenzo; Kudera, Stefan; Krahne, Roman

2018-06-22

Colloidal nanocrystals are a promising fluorescent class of materials whose spontaneous emission features can be tuned over a broad spectral range via their composition, geometry, and size. However, toward embedding nanocrystal films in elaborated device geometries, one significant drawback is the sensitivity of their emission properties on further fabrication processes like lithography, metal or oxide deposition, etc. In this work, we demonstrate how bright-emitting and robust thin films can be obtained by combining nanocrystal deposition from solutions via spin coating with subsequent atomic layer deposition of alumina. For the resulting composite films, the layer thickness can be controlled on the nanoscale and their refractive index can be finely tuned by the amount of deposited alumina. Ellipsometry is used to measure the real and imaginary part of the dielectric permittivity, which gives direct access to the wavelength dependent refractive index and absorbance of the film. Detailed analysis of the photophysics of thin films of core-shell nanocrystals with different shapes and different shell thicknesses allows to correlate the behavior of the photoluminescence and of the decay lifetime to the changes in the nonradiative rate that are induced by the alumina deposition. We show that the photoemission properties of such composite films are stable in wavelength and intensity over several months and that the photoluminescence completely recovers from heating processes up to 240 °C. The latter is particularly interesting since it demonstrates robustness to the typical heat treatment that is needed in several process steps like resist-based lithography and deposition by thermal or electron beam evaporation of metals or oxides.

Hollow nanocrystals and method of making

DOEpatents

Alivisatos, A Paul [Oakland, CA; Yin, Yadong [Moreno Valley, CA; Erdonmez, Can Kerem [Berkeley, CA

2011-07-05

Described herein are hollow nanocrystals having various shapes that can be produced by a simple chemical process. The hollow nanocrystals described herein may have a shell as thin as 0.5 nm and outside diameters that can be controlled by the process of making.

2-Hydroxypropyltrimethylammonium xylan adsorption onto rod-like cellulose nanocrystal.

PubMed

Sim, Jae Hyun; Dong, Shuping; Röemhild, Katrin; Kaya, Abdulaziz; Sohn, Daewon; Tanaka, Keiji; Roman, Maren; Heinze, Thomas; Esker, Alan R

2015-02-15

Chemical incompatibility and relatively weak interaction between lignocellulosic fibers and synthetic polymers have made studies of wood fiber-thermoplastic composite more challenging. In this study, adsorption of 2-hydroxypropyltrimethylammonium xylans onto rod-like cellulose nanocrystals are investigated by zeta-potential measurements, and polarized and depolarized dynamic light scattering as a factor for better understanding of lignocellulosic fibers and cellulose nanocrystals. Zeta-potential measurements show xylan derivative adsorption onto cellulose nanocrystals. Decay time distributions of the ternary system and binary system from dynamic light scattering show that aggregates exist in the binary system and they disappear in the ternary system. At low 2-hydroxypropyltrimethylammonium xylan concentrations relative to that of cellulose nanocrystal, xylan derivatives adsorbed onto some of the cellulose nanocrystal. Hence, more xylan derivatives adsorbed onto cellulose nanocrystal increased with increasing xylan derivative concentration. Also, the concentration dependence of the ratio of the rotational diffusion coefficient to the translational diffusion coefficient revealed a strong adsorptive interaction between xylan derivatives and the cellulose nanocrystals. Copyright © 2014 Elsevier Inc. All rights reserved.

Controlling upconversion nanocrystals for emerging applications

NASA Astrophysics Data System (ADS)

Zhou, Bo; Shi, Bingyang; Jin, Dayong; Liu, Xiaogang

2015-11-01

Lanthanide-doped upconversion nanocrystals enable anti-Stokes emission with pump intensities several orders of magnitude lower than required by conventional nonlinear optical techniques. Their exceptional properties, namely large anti-Stokes shifts, sharp emission spectra and long excited-state lifetimes, have led to a diversity of applications. Here, we review upconversion nanocrystals from the perspective of fundamental concepts and examine the technical challenges in relation to emission colour tuning and luminescence enhancement. In particular, we highlight the advances in functionalization strategies that enable the broad utility of upconversion nanocrystals for multimodal imaging, cancer therapy, volumetric displays and photonics.

Nuclear Structure of 124Xe Studied with β+/EC-Decay

NASA Astrophysics Data System (ADS)

Radich, A. J.; Garrett, P. E.; Allmond, J. M.; Andreoiu, C.; Ball, G. C.; Bianco, L.; Bildstein, V.; Chagnon-Lessard, S.; Cross, D. S.; Diaz Varela, A.; Dunlop, R.; Finlay, P.; Garnsworthy, A. B.; Hackman, G.; Hadinia, B.; Jigmeddorj, B.; Laffoley, A. T.; Leach, K. G.; Michetti-Wilson, J.; Orce, J. N.; Rajabali, M. M.; Rand, E.; Starosta, K.; Sumithrarachchi, C. S.; Svensson, C. E.; Triambak, S.; Wang, Z. M.; Wood, J. L.; Wong, J.; Williams, S. J.; Yates, S. W.

The nuclear structure of 124Xe was investigated using γ-ray spectroscopy following the β+/EC-decay of 124Cs. A very high-statistics data set was collected and γγ coincidence data was analyzed, greatly adding to the 124Xe level scheme. A new decay branch from the high-spin isomer of 124Cs was observed as well as weak E2 transitions into excited 0+ states in 124Xe. B(E2) transition strengths of such low-spin transitions are very important in determining collective properties, which are currently poorly characterized in the region of neutron-deficient xenon isotopes.

XeCl avalanche discharge laser employing Ar as a diluent

DOEpatents

Sze, R.C.

1979-10-10

A XeCl avalanche discharge exciplex laser which uses a gaseous lasing starting mixture of: 0.2 to 0.4% chlorine donor/2.5% to 10% Xe/97.3% to 89.6% Ar) is provided. The chlorine donor normally comprises HCl but can also comprise CCl/sub 4/ BCl/sub 3/. Use of Ar as a diluent gas reduces operating pressures over other rare gas halide lasers to near atmospheric pressure, increases output lasing power of the XeCl avalanche discharge laser by 30% to exceed KrF avalanche discharge lasing outputs, and is less expensive to operate.

Zirconia nanocrystals as submicron level biological label

NASA Astrophysics Data System (ADS)

Smits, K.; Liepins, J.; Gavare, M.; Patmalnieks, A.; Gruduls, A.; Jankovica, D.

2012-08-01

Inorganic nanocrystals are of increasing interest for their usage in biology and pharmacology research. Our interest was to justify ZrO2 nanocrystal usage as submicron level biological label in baker's yeast Saccharomyces cerevisia culture. For the first time (to our knowledge) images with sub micro up-conversion luminescent particles in biologic media were made. A set of undoped as well as Er and Yb doped ZrO2 samples at different concentrations were prepared by sol-gel method. The up-conversion luminescence for free standing and for nanocrystals with baker's yeast cells was studied and the differences in up-conversion luminescence spectra were analyzed. In vivo toxic effects of ZrO2 nanocrystals were tested by co-cultivation with baker's yeast.

Theoretical Calculations of XeF Ground State Kinetics.

DTIC Science & Technology

1988-03-01

potential parameters for XeF are taken from Tellinghuisen et al. 3 The values of the Lennard - Jones parameters for HeF...parameters for the Morse potential and the Lennard - Jones potentials are listed in Table 1. These parameters for the Lennard - Jones potentials produce the...relaxation and dissociation. 13 ~ o Table 1. Potential Parameters. Morse Function (XeF)3 De = 3.35 kcal/mol ae=1.726 a.u.-1 re =4.367 a.u. Lennard Jones

Doping effect in Si nanocrystals

NASA Astrophysics Data System (ADS)

Li, Dongke; Xu, Jun; Zhang, Pei; Jiang, Yicheng; Chen, Kunji

2018-06-01

Intentional doping in semiconductors is a fundamental issue since it can control the conduction type and ability as well as modify the optical and electronic properties. To realize effective doping is the basis for developing semiconductor devices. However, by reducing the size of a semiconductor, like Si, to the nanometer scale, the doping effects become complicated due to the coupling between the quantum confinement effect and the surfaces and/or interfaces effect. In particular, by introducing phosphorus or boron impurities as dopants into material containing Si nanocrystals with a dot size of less than 10 nm, it exhibits different behaviors and influences on the physical properties from its bulk counterpart. Understanding the doping effects in Si nanocrystals is currently a challenge in order to further improve the performance of the next generation of nano-electronic and photonic devices. In this review, we present an overview of the latest theoretical studies and experimental results on dopant distributions and their effects on the electronic and optical properties of Si nanocrystals. In particular, the advanced characterization techniques on dopant distribution, the carrier transport process as well as the linear and nonlinear optical properties of doped Si nanocrystals, are systematically summarized.

Stress evolution of Ge nanocrystals in dielectric matrices.

PubMed

Bahariqushchi, Rahim; Raciti, Rosario; Kasapoğlu, Ahmet Emre; Gür, Emre; Sezen, Meltem; Kalay, Eren; Mirabella, Salvatore; Aydinli, A

2018-05-04

Germanium nanocrystals (Ge NCs) embedded in single and multilayer silicon oxide and silicon nitride matrices have been synthesized using plasma enhanced chemical vapor deposition followed by conventional furnace annealing or rapid thermal processing in N 2 ambient. Compositions of the films were determined by Rutherford backscattering spectrometry and x-ray photoelectron spectroscopy. The formation of NCs under suitable process conditions was observed with high resolution transmission electron microscope micrographs and Raman spectroscopy. Stress measurements were done using Raman shifts of the Ge optical phonon line at 300.7 cm -1 . The effect of the embedding matrix and annealing methods on Ge NC formation were investigated. In addition to Ge NCs in single layer samples, the stress on Ge NCs in multilayer samples was also analyzed. Multilayers of Ge NCs in a silicon nitride matrix separated by dielectric buffer layers to control the size and density of NCs were fabricated. Multilayers consisted of SiN y :Ge ultrathin films sandwiched between either SiO 2 or Si 3 N 4 by the proper choice of buffer material. We demonstrated that it is possible to tune the stress state of Ge NCs from compressive to tensile, a desirable property for optoelectronic applications. We also observed that there is a correlation between the stress and the crystallization threshold in which the compressive stress enhances the crystallization, while the tensile stress suppresses the process.

Stress evolution of Ge nanocrystals in dielectric matrices

NASA Astrophysics Data System (ADS)

Bahariqushchi, Rahim; Raciti, Rosario; Emre Kasapoğlu, Ahmet; Gür, Emre; Sezen, Meltem; Kalay, Eren; Mirabella, Salvatore; Aydinli, A.

2018-05-01

Germanium nanocrystals (Ge NCs) embedded in single and multilayer silicon oxide and silicon nitride matrices have been synthesized using plasma enhanced chemical vapor deposition followed by conventional furnace annealing or rapid thermal processing in N2 ambient. Compositions of the films were determined by Rutherford backscattering spectrometry and x-ray photoelectron spectroscopy. The formation of NCs under suitable process conditions was observed with high resolution transmission electron microscope micrographs and Raman spectroscopy. Stress measurements were done using Raman shifts of the Ge optical phonon line at 300.7 cm-1. The effect of the embedding matrix and annealing methods on Ge NC formation were investigated. In addition to Ge NCs in single layer samples, the stress on Ge NCs in multilayer samples was also analyzed. Multilayers of Ge NCs in a silicon nitride matrix separated by dielectric buffer layers to control the size and density of NCs were fabricated. Multilayers consisted of SiN y :Ge ultrathin films sandwiched between either SiO2 or Si3N4 by the proper choice of buffer material. We demonstrated that it is possible to tune the stress state of Ge NCs from compressive to tensile, a desirable property for optoelectronic applications. We also observed that there is a correlation between the stress and the crystallization threshold in which the compressive stress enhances the crystallization, while the tensile stress suppresses the process.

Optical properties of implanted Xe color centers in diamond

DOE PAGES

Sandstrom, Russell; Ke, Li; Martin, Aiden; ...

2017-12-20

Optical properties of color centers in diamond have been the subject of intense research due to their promising applications in quantum photonics. Here in this work we study the optical properties of Xe related color centers implanted into nitrogen rich (type IIA) and an ultrapure, electronic grade diamond. The Xe defect has two zero phonon lines at 794 nm and 811 nm, which can be effectively excited using both green and red excitation, however, its emission in the nitrogen rich diamond is brighter. Near resonant excitation is performed at cryogenic temperatures and luminescence is probed under strong magnetic field. Finally,more » our results are important towards the understanding of the Xe related defect and other near infrared color centers in diamond.« less

Optical properties of implanted Xe color centers in diamond

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sandstrom, Russell; Ke, Li; Martin, Aiden

Optical properties of color centers in diamond have been the subject of intense research due to their promising applications in quantum photonics. Here in this work we study the optical properties of Xe related color centers implanted into nitrogen rich (type IIA) and an ultrapure, electronic grade diamond. The Xe defect has two zero phonon lines at 794 nm and 811 nm, which can be effectively excited using both green and red excitation, however, its emission in the nitrogen rich diamond is brighter. Near resonant excitation is performed at cryogenic temperatures and luminescence is probed under strong magnetic field. Finally,more » our results are important towards the understanding of the Xe related defect and other near infrared color centers in diamond.« less

Single-exciton optical gain in semiconductor nanocrystals.

PubMed

Klimov, Victor I; Ivanov, Sergei A; Nanda, Jagjit; Achermann, Marc; Bezel, Ilya; McGuire, John A; Piryatinski, Andrei

2007-05-24

Nanocrystal quantum dots have favourable light-emitting properties. They show photoluminescence with high quantum yields, and their emission colours depend on the nanocrystal size--owing to the quantum-confinement effect--and are therefore tunable. However, nanocrystals are difficult to use in optical amplification and lasing. Because of an almost exact balance between absorption and stimulated emission in nanoparticles excited with single electron-hole pairs (excitons), optical gain can only occur in nanocrystals that contain at least two excitons. A complication associated with this multiexcitonic nature of light amplification is fast optical-gain decay induced by non-radiative Auger recombination, a process in which one exciton recombines by transferring its energy to another. Here we demonstrate a practical approach for obtaining optical gain in the single-exciton regime that eliminates the problem of Auger decay. Specifically, we develop core/shell hetero-nanocrystals engineered in such a way as to spatially separate electrons and holes between the core and the shell (type-II heterostructures). The resulting imbalance between negative and positive charges produces a strong local electric field, which induces a giant ( approximately 100 meV or greater) transient Stark shift of the absorption spectrum with respect to the luminescence line of singly excited nanocrystals. This effect breaks the exact balance between absorption and stimulated emission, and allows us to demonstrate optical amplification due to single excitons.

All-inorganic Germanium nanocrystal films by cationic ligand exchange

DOE PAGES

Wheeler, Lance M.; Nichols, Asa W.; Chernomordik, Boris D.; ...

2016-01-21

In this study, we introduce a new paradigm for group IV nanocrystal surface chemistry based on room temperature surface activation that enables ionic ligand exchange. Germanium nanocrystals synthesized in a gas-phase plasma reactor are functionalized with labile, cationic alkylammonium ligands rather than with traditional covalently bound groups. We employ Fourier transform infrared and 1H nuclear magnetic resonance spectroscopies to demonstrate the alkylammonium ligands are freely exchanged on the germanium nanocrystal surface with a variety of cationic ligands, including short inorganic ligands such as ammonium and alkali metal cations. This ionic ligand exchange chemistry is used to demonstrate enhanced transport inmore » germanium nanocrystal films following ligand exchange as well as the first photovoltaic device based on an all-inorganic germanium nanocrystal absorber layer cast from solution. This new ligand chemistry should accelerate progress in utilizing germanium and other group IV nanocrystals for optoelectronic applications.« less

Structure and transformation of tactoids in cellulose nanocrystal suspensions

NASA Astrophysics Data System (ADS)

Wang, Pei-Xi; Hamad, Wadood Y.; MacLachlan, Mark J.

2016-05-01

Cellulose nanocrystals obtained from natural sources are of great interest for many applications. In water, cellulose nanocrystals form a liquid crystalline phase whose hierarchical structure is retained in solid films after drying. Although tactoids, one of the most primitive components of liquid crystals, are thought to have a significant role in the evolution of this phase, they have evaded structural study of their internal organization. Here we report the capture of cellulose nanocrystal tactoids in a polymer matrix. This method allows us to visualize, for the first time, the arrangement of cellulose nanocrystals within individual tactoids by electron microscopy. Furthermore, we can follow the structural evolution of the liquid crystalline phase from tactoids to iridescent-layered films. Our insights into the early nucleation events of cellulose nanocrystals give important information about the growth of cholesteric liquid crystalline phases, especially for cellulose nanocrystals, and are crucial for preparing photonics-quality films.

One-step DNA-programmed growth of luminescent and biofunctionalized nanocrystals

NASA Astrophysics Data System (ADS)

Ma, Nan; Sargent, Edward H.; Kelley, Shana O.

2009-02-01

Colloidal semiconductor nanocrystals are widely used as lumiphores in biological imaging because their luminescence is both strong and stable, and because they can be biofunctionalized. During synthesis, nanocrystals are typically passivated with hydrophobic organic ligands, so it is then necessary either to replace these ligands or encapsulate the nanocrystals with hydrophilic moieties to make the lumiphores soluble in water. Finally, biological labels must be added to allow the detection of nucleic acids, proteins and specific cell types. This multistep process is time- and labour-intensive and thus out of reach of many researchers who want to use luminescent nanocrystals as customized lumiphores. Here, we show that a single designer ligand-a chimeric DNA molecule-can controllably program both the growth and the biofunctionalization of the nanocrystals. One part of the DNA sequence controls the nanocrystal passivation and serves as a ligand, while another part controls the biorecognition. The synthetic protocol reported here is straightforward and produces a homogeneous dispersion of nanocrystal lumiphores functionalized with a single biomolecular receptor. The nanocrystals exhibit strong optical emission in the visible region, minimal toxicity and have hydrodynamic diameters of ~6 nm, which makes them suitable for bioimaging. We show that the nanocrystals can specifically bind DNA, proteins or cells that have unique surface recognition markers.

An intense radiation in mid-infrared of Xe

NASA Astrophysics Data System (ADS)

He, Shan; Liu, Dong; Guo, Jingwei; Sang, Fengting

2017-01-01

Recently, the optically pumped rare gas lasers have been attracted extensive attention. Rare gas laser systems with Ne (2p53p), Ar (3p54p), and Kr (4p55p) atoms have been investigated. However, there are sparse studies based on Xe. In this work, new phenomena, intensive mid-infrared amplified spontaneous emissions (ASEs), are found after two-photon excitation of Xe from the ground state to the 6p[1/2]0 state. Simultaneously, substantial 6p[1/2]1 atoms are populated. The thresholds of ASE peak 1 and the generation of 6p[1/2]1 atoms are both about 1.5 mJ. It indicates that there should exist the relationship between these two phenomena. The ASE signals show broadband spectra. Therefore, it must be yielded by the superposition of Xe2* excimer transitions. The mid-infrared ASEs lead to excimers correlating to the 6s'[1/2]1 enormously generated. Then these excimers dissociate to produce substantial 6p[1/2]1 atoms. Under some circumstance, the ratio of the 6p[1/2]1 to 6p[1/2]0 atoms reaches about 80%. It indicates that the 6p[1/2]0 atoms strongly tend to decay through the emissions between the excimer states. Using these emissions, continuous-tunable mid-infrared laser with metastable Xe can be promisingly produced.

Plasmonic Properties of Silicon Nanocrystals Doped with Boron and Phosphorus.

PubMed

Kramer, Nicolaas J; Schramke, Katelyn S; Kortshagen, Uwe R

2015-08-12

Degenerately doped silicon nanocrystals are appealing plasmonic materials due to silicon's low cost and low toxicity. While surface plasmonic resonances of boron-doped and phosphorus-doped silicon nanocrystals were recently observed, there currently is poor understanding of the effect of surface conditions on their plasmonic behavior. Here, we demonstrate that phosphorus-doped silicon nanocrystals exhibit a plasmon resonance immediately after their synthesis but may lose their plasmonic response with oxidation. In contrast, boron-doped nanocrystals initially do not exhibit plasmonic response but become plasmonically active through postsynthesis oxidation or annealing. We interpret these results in terms of substitutional doping being the dominant doping mechanism for phosphorus-doped silicon nanocrystals, with oxidation-induced defects trapping free electrons. The behavior of boron-doped silicon nanocrystals is more consistent with a strong contribution of surface doping. Importantly, boron-doped silicon nanocrystals exhibit air-stable plasmonic behavior over periods of more than a year.

Si nanocrystals-based multilayers for luminescent and photovoltaic device applications

NASA Astrophysics Data System (ADS)

Lu, Peng; Li, Dongke; Cao, Yunqing; Xu, Jun; Chen, Kunji

2018-06-01

Low dimensional Si materials have attracted much attention because they can be developed in many kinds of new-generation nano-electronic and optoelectronic devices, among which Si nanocrystals-based multilayered material is one of the most promising candidates and has been extensively studied. By using multilayered structures, the size and distribution of nanocrystals as well as the barrier thickness between two adjacent Si nanocrystal layers can be well controlled, which is beneficial to the device applications. This paper presents an overview of the fabrication and device applications of Si nanocrystals, especially in luminescent and photovoltaic devices. We first introduce the fabrication methods of Si nanocrystals-based multilayers. Then, we systematically review the utilization of Si nanocrystals in luminescent and photovoltaic devices. Finally, some expectations for further development of the Si nanocrystals-based photonic and photovoltaic devices are proposed. Project supported by the National Natural Science Foundation of China (Nos. 11774155, 11274155).

Spontaneous and induced emission of XeCl* excimer molecules under pumping of Xe - CCl4 and Ar - Xe - CCl4 gas mixtures with a low CCl4 content by fast electrons and uranium fission fragments

NASA Astrophysics Data System (ADS)

Mis'kevich, A. I.; Guo, J.; Dyuzhov, Yu A.

2013-11-01

The spontaneous and induced emission of XeCl* excimer molecules upon excitation of Xe - CCl4 and Ar - Xe - CCl4 gas mixtures with a low CCl4 content by high-energy charged particles [a pulsed high-energy electron beam and products of neutron nuclear reaction 235U(n, f)] has been experimentally studied. The electron energy was 150 keV, and the pump current pulse duration and amplitude were 5 ns and 5 A, respectively. The energy of fission fragments did not exceed 100 MeV, the duration of the neutron pump pulse was 200 μs, and the specific power contribution to the gas was about 300 W cm-3. Electron beam pumping in a cell 4 cm long with a cavity having an output mirror transmittance of 2.7% gives rise to lasing on the B → X transition in the XeCl* molecule (λ = 308 nm) with a gain α = 0.0085 cm-1 and fluorescence efficiency η ≈ 10%. Pumping by fission fragments in a 250-cm-long cell with a cavity formed by a highly reflecting mirror and a quartz window implements amplified spontaneous emission (ASE) with an output power of 40 - 50 kW sr-1 and a base ASE pulse duration of ~200 ms.

Extraordinary Interfacial Stitching between Single All-Inorganic Perovskite Nanocrystals

PubMed Central

2018-01-01

All-inorganic cesium lead halide perovskite nanocrystals are extensively studied because of their outstanding optoelectronic properties. Being of a cubic shape and typically featuring a narrow size distribution, CsPbX3 (X = Cl, Br, and I) nanocrystals are the ideal starting material for the development of homogeneous thin films as required for photovoltaic and optoelectronic applications. Recent experiments reveal spontaneous merging of drop-casted CsPbBr3 nanocrystals, which is promoted by humidity and mild-temperature treatments and arrested by electron beam irradiation. Here, we make use of atom-resolved annular dark-field imaging microscopy and valence electron energy loss spectroscopy in a state-of-the-art low-voltage monochromatic scanning transmission electron microscope to investigate the aggregation between individual nanocrystals at the atomic level. We show that the merging process preserves the elemental composition and electronic structure of CsPbBr3 and takes place between nanocrystals of different sizes and orientations. In particular, we reveal seamless stitching for aligned nanocrystals, similar to that reported in the past for graphene flakes. Because the crystallographic alignment occurs naturally in drop-casted layers of CsPbX3 nanocrystals, our findings constitute the essential first step toward the development of large-area nanosheets with band gap energies predesigned by the nanocrystal choice—the gateway to large-scale photovoltaic applications of inorganic perovskites. PMID:29355301

Extraordinary Interfacial Stitching between Single All-Inorganic Perovskite Nanocrystals.

PubMed

Gomez, Leyre; Lin, Junhao; de Weerd, Chris; Poirier, Lucas; Boehme, Simon C; von Hauff, Elizabeth; Fujiwara, Yasufumi; Suenaga, Kazutomo; Gregorkiewicz, Tom

2018-02-14

All-inorganic cesium lead halide perovskite nanocrystals are extensively studied because of their outstanding optoelectronic properties. Being of a cubic shape and typically featuring a narrow size distribution, CsPbX 3 (X = Cl, Br, and I) nanocrystals are the ideal starting material for the development of homogeneous thin films as required for photovoltaic and optoelectronic applications. Recent experiments reveal spontaneous merging of drop-casted CsPbBr 3 nanocrystals, which is promoted by humidity and mild-temperature treatments and arrested by electron beam irradiation. Here, we make use of atom-resolved annular dark-field imaging microscopy and valence electron energy loss spectroscopy in a state-of-the-art low-voltage monochromatic scanning transmission electron microscope to investigate the aggregation between individual nanocrystals at the atomic level. We show that the merging process preserves the elemental composition and electronic structure of CsPbBr 3 and takes place between nanocrystals of different sizes and orientations. In particular, we reveal seamless stitching for aligned nanocrystals, similar to that reported in the past for graphene flakes. Because the crystallographic alignment occurs naturally in drop-casted layers of CsPbX 3 nanocrystals, our findings constitute the essential first step toward the development of large-area nanosheets with band gap energies predesigned by the nanocrystal choice-the gateway to large-scale photovoltaic applications of inorganic perovskites.

Theoretical study of the NMR chemical shift of Xe in supercritical condition.

PubMed

Lacerda, Evanildo G; Sauer, Stephan P A; Mikkelsen, Kurt V; Coutinho, Kaline; Canuto, Sylvio

2018-02-20

In this work we investigate the level of theory necessary for reproducing the non-linear variation of the 129 Xe nuclear magnetic resonance (NMR) chemical shift with the density of Xe in supercritical conditions. In detail we study how the 129 Xe chemical shift depends under supercritical conditions on electron correlation, relativistic and many-body effects. The latter are included using a sequential-QM/MM methodology, in which a classical MD simulation is performed first and the chemical shift is then obtained as an average of quantum calculations of 250 MD snapshots conformations carried out for Xe n clusters (n = 2 - 8 depending on the density). The analysis of the relativistic effects is made at the level of 4-component Hartree-Fock calculations (4c-HF) and electron correlation effects are considered using second order Møller-Plesset perturbation theory (MP2). To simplify the calculations of the relativistic and electron correlation effects we adopted an additive scheme, where the calculations on the Xe n clusters are carried out at the non-relativistic Hartree-Fock (HF) level, while electron correlation and relativistic corrections are added for all the pairs of Xe atoms in the clusters. Using this approach we obtain very good agreement with the experimental data, showing that the chemical shift of 129 Xe in supercritical conditions is very well described by cluster calculations at the HF level, with small contributions from relativistic and electron correlation effects.

Hyperpolarized 129Xe MRI: A Viable Functional Lung Imaging Modality?

PubMed Central

Patz, Samuel; Hersman, F. William; Muradian, Iga; Hrovat, Mirko I.; Ruset, Iulian C.; Ketel, Stephen; Jacobson, Francine; Topulos, George P.; Hatabu, Hiroto; Butler, James P.

2008-01-01

The majority of researchers investigating hyperpolarized gas MRI as a candidate functional lung imaging modality have used 3He as their imaging agent of choice rather than 129Xe. This preference has been predominantly due to, 3He providing stronger signals due to higher levels of polarization and higher gyromagnetic ratio, as well as its being easily available to more researchers due to availability of polarizers (USA) or ease of gas transport (Europe). Most researchers agree, however, that hyperpolarized 129Xe will ultimately emerge as the imaging agent of choice due to its unlimited supply in nature and its falling cost. Our recent polarizer technology delivers vast improvements in hyperpolarized 129Xe output. Using this polarizer, we have demonstrated the unique property of xenon to measure alveolar surface area noninvasively. In this article, we describe our human protocols and their safety, and our results for the measurement of the partial pressure of pulmonary oxygen (pO2) by observation of 129Xe signal decay. We note that the measurement of pO2 by observation of 129Xe signal decay is more complex than that for 3He because of an additional signal loss mechanism due to interphase diffusion of 129Xe from alveolar gas spaces to septal tissue. This results in measurements of an equivalent pO2 that accounts for both traditional T1 decay from pO2 and that from interphase diffusion. We also provide an update on new technological advancements that form the foundation for an improved compact design polarizer as well as improvements that provide another order-of-magnitude scale-up in xenon polarizer output. PMID:17890035

Nimodipine nanocrystals for oral bioavailability improvement: preparation, characterization and pharmacokinetic studies.

PubMed

Fu, Qiang; Sun, Jin; Zhang, Dong; Li, Mo; Wang, Yongjun; Ling, Guixia; Liu, Xiaohong; Sun, Yinghua; Sui, Xiaofan; Luo, Cong; Sun, Le; Han, Xiaopeng; Lian, He; Zhu, Meng; Wang, Siling; He, Zhonggui

2013-09-01

This study intended to develop nimodipine (NMD) nanocrystals with different sizes for oral administration and to investigate the relationship between dissolution and pharmacokinetics for NMD nanocrystals and Nimotop(®). NMD nanocrystals were prepared by combination of microprecipitation and high pressure homogenization and were further lyophilized. The particle size, morphology and aqueous solubility of the NMD nanocrystals were determined. With Nimotop(®) as the control, the dissolution rate was evaluated and the pharmacokinetic study was undertaken in beagle dogs. NMD nanocrystals with mean diameters of about 159.0, 503.0 and 833.3 nm were prepared, respectively. The lyophilization didn't affect the particle sizes of the redispersed nanocrystals. The aqueous solubility was significantly improved and displayed a size-dependent manner. The nanocrystals exhibited lower dissolution patterns than Nimotop(®) under non-sink condition, but bioavailability of the two nanocrystals (159.0 and 833.3 nm) was equivalent, about 2.6-fold higher than Nimotop(®). In conclusion, oral nanocrystal drug delivery system was a promising strategy in improving the oral bioavailability of poorly soluble or insoluble drugs. But we could not establish a favorable in vitro in vivo correlation for NMD nanocrystals and Nimotop(®) and thus the oral absorption mechanism of the NMD nanocrystals required further study. Copyright © 2013 Elsevier B.V. All rights reserved.

Magnetic dipole strength in 128Xe and 134Xe in the spin-flip resonance region

NASA Astrophysics Data System (ADS)

Massarczyk, R.; Rusev, G.; Schwengner, R.; Dönau, F.; Bhatia, C.; Gooden, M. Â. E.; Kelley, J. Â. H.; Tonchev, A. Â. P.; Tornow, W.

2014-11-01

The magnetic dipole strength in the energy region of the spin-flip resonance is investigated in 128Xe and 134Xe using quasimonoenergetic and linearly polarized γ -ray beams at the High-Intensity γ -Ray Source facility in Durham, North Carolina, USA. Absorption cross sections were deduced for the magnetic and electric and dipole strength distributions separately for various intervals of excitation energy, including the strength of states in the unresolved quasicontinuum. The magnetic dipole strength distributions show structures resembling a resonance in the spin-flip region around an excitation energy of 8 MeV. The electric dipole strength distributions obtained from the present experiments are in agreement with the ones deduced from an earlier experiment using broad-band bremsstrahlung instead of a quasimonoenergetic beam. The experimental magnetic and electric dipole strength distributions are compared with phenomenological approximations and with predictions of a quasiparticle random phase approximation in a deformed basis.

Noble gas bond and the behaviour of XeO3 under pressure.

PubMed

Hou, Chunju; Wang, Xianlong; Botana, Jorge; Miao, Maosheng

2017-10-18

Over the past few decades, the concept of hydrogen bonds, in which hydrogen is electrophilic, has been extended to halogen bonds, chalcogen bonds and pnicogen bonds. Herein, we show that such a non-covalent bonding also exists in noble gas compounds. Using first principles calculations, we illustrate the OXe-O bond in molecular crystal XeO 3 and its effect on the behavior of this compound under pressure. Our calculations show that the covalent Xe-O bond lengths were elongated with increasing pressure and correspondingly the Xe-O stretching vibration frequencies were red shifted, which is similar to the change of H-bonds under pressure. The OXe-O bond and related hopping of O between neighboring Xe sites also correspond to the structural changes in the XeO 3 compounds at about 2 GPa. Our study extends the concept of hydrogen bonding to include all p-block elements and show a new bonding type for Noble gas elements in which it acts as an electrophilic species.

Neutron-induced Backgrounds in 134Xe for Large-Scale Neutrinoless Double-Beta Decay Experiments

NASA Astrophysics Data System (ADS)

Moriguchi, Nina; Kidd, Mary; Tornow, Werner

2016-09-01

136Xe is used in large neutrinoless double-beta (0 νββ) decay experiments, such as KamLAND- Zen and EXO 200. Though highly purified, 136Xe still contains a significant amount of 134Xe. Recently, a new nuclear energy level was found in 134Xe. If 134Xe decays from this proposed excited state, it will emit a 2485.7 keV gamma ray. Because this energy lies near the region of interest of 136Xe νββ decay experiments (Q value 2457.8 keV), it could make a significant contribution to the background. A purified gaseous sample of 134Xe will be irradiated with neutrons of an incident energy of 4.0 MeV at Triangle Universities Nuclear Laboratory and monitored with high-purity germanium detectors. The spectra obtained from these detectors will be analyzed for the presence of the 2581 keV gamma ray. We will report on the status of this experiment. Future plans include expanding this measurement to higher initial neutron energies. Tennesse Tech University CISE Grant program.

Kr/Xe Separation over a Chabazite Zeolite Membrane

DOE Office of Scientific and Technical Information (OSTI.GOV)

Feng, Xuhui; Zong, Zhaowang; Elsaidi, Sameh K.

2016-08-10

Cryogenic distillation, the current conventional technology to separate Krypton and Xenon from air, and from nuclear reprocessing technologies, is an energy-intensive and expensive process. Membrane technology could potentially make this challenging industrial separation less energy intensive and economically viable. We demonstrate that chabazite zeolite SAPO-34 membranes effectively separated Kr/Xe gas mixtures at industrially relevant compositions. Control over membrane thickness and average crystal size led to industrial range permeances and high separation selectivities. Specifically, SAPO-34 membranes can separate Kr/Xe mixtures with Kr permeances as high as 361.4 GPU and separation selectivities of 34.8 for molar compositions close to typical concentrations ofmore » these two gases in air. In addition, SAPO-34 membranes separated Kr/Xe mixtures with Kr permeances as high as 525.7 GPU and separation selectivities up to 45.1 for molar compositions as might be encountered in nuclear reprocessing technologies. Molecular sieving and differences in diffusivities were identified as the dominant separation mechanisms.« less

Colloidal Nanocrystals with Near-infrared Optical Properties: Synthesis, Characterization, and Applications

NASA Astrophysics Data System (ADS)

Panthani, Matthew George

2011-07-01

Colloidal nanocrystals with optical properties in the near-infrared (NIR) are of interest for many applications such as photovoltaic (PV) energy conversion, bioimaging, and therapeutics. For PVs and other electronic devices, challenges in using colloidal nanomaterials often deal with the surfaces. Because of the high surface-to-volume ratio of small nanocrystals, surfaces and interfaces play an enhanced role in the properties of nanocrystal films and devices. Organic ligand-capped CuInSe2 (CIS) and Cu(InXGa 1-X)Se2 (CIGS) nanocrystals were synthesized and used as the absorber layer in prototype solar cells. By fabricating devices from spray-coated CuInSe nanocrystals under ambient conditions, solar-to-electric power conversion efficiencies as high as 3.1% were achieved. Many treatments of the nanocrystal films were explored. Although some treatments increased the conductivity of the nanocrystal films, the best devices were from untreated CIS films. By modifying the reaction chemistry, quantum-confined CuInSe XS2-X (CISS) nanocrystals were produced. The potential of the CISS nanocrystals for targeted bioimaging was demonstrated via oral delivery to mice and imaging of nanocrystal fluorescence. The size-dependent photoluminescence of Si nanocrystals was measured. Si nanocrystals supported on graphene were characterized by conventional transmission electron microscopy and spherical aberration (Cs)-corrected scanning transmission electron microscopy (STEM). Enhanced imaging contrast and resolution was achieved by using Cs-corrected STEM with a graphene support. In addition, clear imaging of defects and the organic-inorganic interface was enabled by utilizing this technique.

Inorganic Chemistry Solutions to Semiconductor Nanocrystal Problems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Alvarado, Samuel R.; Guo, Yijun; Ruberu, T. Purnima A.

2014-03-15

The optoelectronic and chemical properties of semiconductor nanocrystals heavily depend on their composition, size, shape and internal structure, surface functionality, etc. Available strategies to alter these properties through traditional colloidal syntheses and ligand exchange methods place a premium on specific reaction conditions and surfactant combinations. In this invited review, we apply a molecular-level understanding of chemical precursor reactivity to reliably control the morphology, composition and intimate architecture (core/shell vs. alloyed) of semiconductor nanocrystals. We also describe our work aimed at achieving highly selective, low-temperature photochemical methods for the synthesis of semiconductor–metal and semiconductor–metal oxide photocatalytic nanocomposites. In addition, we describemore » our work on surface modification of semiconductor nanocrystal quantum dots using new approaches and methods that bypass ligand exchange, retaining the nanocrystal's native ligands and original optical properties, as well as on spectroscopic methods of characterization useful in determining surface ligand organization and chemistry. Using recent examples from our group and collaborators, we demonstrate how these efforts have lead to faster, wider and more systematic application of semiconductor nanocrystal-based materials to biological imaging and tracking, and to photocatalysis of unconventional substrates. We believe techniques and methods borrowed from inorganic chemistry (including coordination, organometallic and solid state chemistry) have much to offer in reaching a better understanding of the synthesis, functionalization and real-life application of such exciting materials as semiconductor nanocrystals (quantum dots, rods, tetrapods, etc.).« less

Formation of noble metal nanocrystals in the presence of biomolecules

NASA Astrophysics Data System (ADS)

Burt, Justin Lockheart

One of the most promising, yet least studied routes for producing biocompatible nanostructures involves synthesis in the presence of biomolecules. I hypothesized that globular proteins could provide a suitable framework to regulate the formation of noble metal nanocrystals. As proof of concept, I designed two novel synthesis protocols utilizing bovine serum albumin (BSA) protein to regulate the formation of gold nanocrystals. In the first case, the standard protocol for polyol reduction was modified by replacing ethylene glycol with glycerin, replacing synthetic polymers with BSA as protecting agent, and decreasing the reaction temperature. In the second case, the Brust-Schiffrin two-phase reduction was modified by replacing alkylthiols with BSA as protecting agent, which facilitated a strictly aqueous phase synthesis. Due to superior product yield and rapid reduction at room temperature, the aqueous protocol became the foundation for subsequent studies. I extended this approach to produce well-dispersed ˜2nm silver, gold, and platinum nanocrystals. Having demonstrated the feasibility of BSA-functionalized nanocrystals, some potential uses were explored. BSA-functionalized silver nanocrystals were employed in a broader study on the interaction of silver nanocrystals with HIV. BSA-functionalized gold nanocrystals were utilized for in vivo dosage of a contrast enhancing agent to bacteria. BSA-functionalized platinum nanocrystals were studied as hydrogenation catalysts. Since many intriguing uses for protein-functionalized nanocrystals involve incorporation into biosystems, I sought to enhance biocompatibility by using ascorbic acid as reducing agent. Initial experiments revealed elongated and branched nanocrystals. Such structures were not observed in previous synthesis protocols with BSA, so I hypothesized ascorbic acid was driving their formation. To test my assertion, I reduced ionic gold in an aqueous solution of ascorbic acid, thereby discovering a new method

Swift heavy ion irradiation of Pt nanocrystals: II. Structural changes and H desorption

DOE Office of Scientific and Technical Information (OSTI.GOV)

Giulian, R.; Araujo, L.L.; Kluth, P.

2014-09-24

The structural properties and H desorption from embedded Pt nanocrystals (NCs) following irradiation with swift heavy ions were investigated as a function of energy and fluence. From x-ray absorption near-edge spectroscopy analysis, Pt-H bonding was identified in NCs annealed in a forming gas (95% N{sub 2} + 5% H{sub 2}) ambient. The H content decreased upon irradiation and the desorption process was NC-size dependent such that larger NCs required a higher fluence to achieve a H-free state. Pt-H bonding and NC dissolution both perturbed the NC structural parameters (coordination number, bond-length and mean-square relative displacement) as determined with extended x-raymore » absorption fine structure measurements.« less

Size-Dependent Melting Behavior of Colloidal In, Sn, and Bi Nanocrystals

PubMed Central

Liu, Minglu; Wang, Robert Y.

2015-01-01

Colloidal nanocrystals are a technologically important class of nanostructures whose phase change properties have been largely unexplored. Here we report on the melting behavior of In, Sn, and Bi nanocrystals dispersed in a polymer matrix. This polymer matrix prevents the nanocrystals from coalescing with one another and enables previously unaccessed observations on the melting behavior of colloidal nanocrystals. We measure the melting temperature, melting enthalpy, and melting entropy of colloidal nanocrystals with diameters of approximately 10 to 20 nm. All of these properties decrease as nanocrystal size decreases, although the depression rate for melting temperature is comparatively slower than that of melting enthalpy and melting entropy. We also observe an elevated melting temperature during the initial melt-freeze cycle that we attribute to surface stabilization from the organic ligands on the nanocrystal surface. Broad endothermic melting valleys and very large supercoolings in our calorimetry data suggest that colloidal nanocrystals exhibit a significant amount of surface pre-melting and low heterogeneous nucleation probabilities during freezing. PMID:26573146

Vacuum ultraviolet emission characteristics from He-Ne-Xe gas discharge in an alternating current plasma display panel cell

NASA Astrophysics Data System (ADS)

Seo, Jeong Hyun; Jeong, Heui Seob; Lee, Joo Yul; Yoon, Cha Keun; Kim, Joong Kyun; Whang, Ki-Woong

2000-08-01

We measured the time integrated vacuum ultraviolet (VUV) emission spectra of He-Ne-Xe gas mixture from a surface type alternating current (ac) plasma display panel cell. The measured emission lines are the resonance line (147 nm) from Xe*(1s4), the first continuum (150 nm) and the second continuum (173 nm) from Xe dimer excited states. The relative intensities of VUV spectral lines from Xe* and Xe2* are dependent on the He/Ne mixing ratio as well as the Xe partial and total pressure. The intensity of 147 nm VUV increases with the Ne content increase and Xe2* molecular emission increases with the He content increase. Infrared (IR) spectra and the time variation of VUV were measured to explain the reaction pathway and the effect of the mixing ratio of He/Ne on the spectral intensity. A detailed study for the decay time shows that the decay time of 147 nm has two time constants and the radiation of 150 and 173 nm results mainly from Xe*(1s5). The IR spectra shows that the contribution from Xe**(>6 s) to Xe*(1s5) and Xe*(1s4) in He-Xe is different from that of Ne-Xe. The change of IR intensity explains the spectral intensity variations of He-Xe and Ne-Xe discharge.

Metal halide solid-state surface treatment for nanocrystal materials

DOEpatents

Luther, Joseph M.; Crisp, Ryan; Beard, Matthew C.

2016-04-26

Methods of treating nanocrystal and/or quantum dot devices are described. The methods include contacting the nanocrystals and/or quantum dots with a solution including metal ions and halogen ions, such that the solution displaces native ligands present on the surface of the nanocrystals and/or quantum dots via ligand exchange.

Hyperfine frequencies of {sup 87}Rb and {sup 133}Cs atoms in Xe gas

DOE Office of Scientific and Technical Information (OSTI.GOV)

McGuyer, B. H.; Xia, T.; Jau, Y.-Y.

2011-09-15

The microwave resonant frequencies of ground-state {sup 87}Rb and {sup 133}Cs atoms in Xe buffer gas are shown to have a relatively large nonlinear dependence on the Xe pressure, presumably because of RbXe or CsXe van der Waals molecules. The nonlinear shifts for Xe are opposite in sign to the previously measured shifts for Ar and Kr, even though all three gases have negative linear shifts. The Xe data show striking discrepancies with the previous theory for nonlinear shifts. Most of this discrepancy is eliminated by accounting for the spin-rotation interaction, {gamma}N{center_dot}S, in addition to the hyperfine-shift interaction, {delta} Amore » I{center_dot}S, in the molecules. To the limit of our experimental accuracy, the shifts of {sup 87}Rb and {sup 133}Cs in He, Ne, and N{sub 2} were linear with pressure.« less

Cellulose nanocrystals with tunable surface charge for nanomedicine

NASA Astrophysics Data System (ADS)

Hosseinidoust, Zeinab; Alam, Md Nur; Sim, Goeun; Tufenkji, Nathalie; van de Ven, Theo G. M.

2015-10-01

Crystalline nanoparticles of cellulose exhibit attractive properties as nanoscale carriers for bioactive molecules in nanobiotechnology and nanomedicine. For applications in imaging and drug delivery, surface charge is one of the most important factors affecting the performance of nanocarriers. However, current methods of preparation offer little flexibility for controlling the surface charge of cellulose nanocrystals, leading to compromised colloidal stability under physiological conditions. We report a synthesis method that results in nanocrystals with remarkably high carboxyl content (6.6 mmol g-1) and offers continuous control over surface charge without any adjustment to the reaction conditions. Six fractions of nanocrystals with various surface carboxyl contents were synthesized from a single sample of softwood pulp with carboxyl contents varying from 6.6 to 1.7 mmol g-1 and were fully characterized. The proposed method resulted in highly stable colloidal nanocrystals that did not aggregate when exposed to high salt concentrations or serum-containing media. Interactions of these fractions with four different tissue cell lines were investigated over a wide range of concentrations (50-300 μg mL-1). Darkfield hyperspectral imaging and confocal microscopy confirmed the uptake of nanocrystals by selected cell lines without any evidence of membrane damage or change in cell density; however a charge-dependent decrease in mitochondrial activity was observed for charge contents higher than 3.9 mmol g-1. A high surface carboxyl content allowed for facile conjugation of fluorophores to the nanocrystals without compromising colloidal stability. The cellular uptake of fluoresceinamine-conjugated nanocrystals exhibited a time-dose dependent relationship and increased significantly with doubling of the surface charge.Crystalline nanoparticles of cellulose exhibit attractive properties as nanoscale carriers for bioactive molecules in nanobiotechnology and nanomedicine. For

Development of Xe and Kr empirical potentials for CeO 2, ThO 2, UO 2 and PuO 2, combining DFT with high temperature MD

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cooper, M. W. D.; Kuganathan, N.; Burr, P. A.

In this study, the development of embedded atom method (EAM) many-body potentials for actinide oxides and associated mixed oxide (MOX) systems has motivated the development of a complementary parameter set for gas-actinide and gas-oxygen interactions. A comprehensive set of density functional theory (DFT) calculations were used to study Xe and Kr incorporation at a number of sites in CeO 2, ThO 2, UO 2 and PuO 2. These structures were used to fit a potential, which was used to generate molecular dynamics (MD) configurations incorporating Xe and Kr at 300 K, 1500 K, 3000 K and 5000 K. Subsequent matchingmore » to the forces predicted by DFT for these MD configurations was used to refine the potential set. This fitting approach ensured weighted fitting to configurations that are thermodynamically significant over a broad temperature range, while avoiding computationally expensive DFT-MD calculations. The resultant gas potentials were validated against DFT trapping energies and are suitable for simulating combinations of Xe and Kr in solid solutions of CeO 2, ThO 2, UO 2 and PuO 2, providing a powerful tool for the atomistic simulation of conventional nuclear reactor fuel UO 2 as well as advanced MOX fuels.« less

Development of Xe and Kr empirical potentials for CeO 2, ThO 2, UO 2 and PuO 2, combining DFT with high temperature MD

DOE PAGES

Cooper, M. W. D.; Kuganathan, N.; Burr, P. A.; ...

2016-08-23

In this study, the development of embedded atom method (EAM) many-body potentials for actinide oxides and associated mixed oxide (MOX) systems has motivated the development of a complementary parameter set for gas-actinide and gas-oxygen interactions. A comprehensive set of density functional theory (DFT) calculations were used to study Xe and Kr incorporation at a number of sites in CeO 2, ThO 2, UO 2 and PuO 2. These structures were used to fit a potential, which was used to generate molecular dynamics (MD) configurations incorporating Xe and Kr at 300 K, 1500 K, 3000 K and 5000 K. Subsequent matchingmore » to the forces predicted by DFT for these MD configurations was used to refine the potential set. This fitting approach ensured weighted fitting to configurations that are thermodynamically significant over a broad temperature range, while avoiding computationally expensive DFT-MD calculations. The resultant gas potentials were validated against DFT trapping energies and are suitable for simulating combinations of Xe and Kr in solid solutions of CeO 2, ThO 2, UO 2 and PuO 2, providing a powerful tool for the atomistic simulation of conventional nuclear reactor fuel UO 2 as well as advanced MOX fuels.« less

Microscopic theory of cation exchange in CdSe nanocrystals.

PubMed

Ott, Florian D; Spiegel, Leo L; Norris, David J; Erwin, Steven C

2014-10-10

Although poorly understood, cation-exchange reactions are increasingly used to dope or transform colloidal semiconductor nanocrystals (quantum dots). We use density-functional theory and kinetic Monte Carlo simulations to develop a microscopic theory that explains structural, optical, and electronic changes observed experimentally in Ag-cation-exchanged CdSe nanocrystals. We find that Coulomb interactions, both between ionized impurities and with the polarized nanocrystal surface, play a key role in cation exchange. Our theory also resolves several experimental puzzles related to photoluminescence and electrical behavior in CdSe nanocrystals doped with Ag.

Conjugated polymer/nanocrystal nanocomposites for renewable energy applications in photovoltaics and photocatalysis.

PubMed

Su, Yu-Wei; Lin, Wei-Hao; Hsu, Yung-Jung; Wei, Kung-Hwa

2014-11-01

Conjugated polymer/nanocrystal composites have attracted much attention for use in renewable energy applications because of their versatile and synergistic optical and electronic properties. Upon absorbing photons, charge separation occurs in the nanocrystals, generating electrons and holes for photocurrent flow or reduction/oxidation (redox) reactions under proper conditions. Incorporating these nanocrystals into conjugated polymers can complement the visible light absorption range of the polymers for photovoltaics applications or allow the polymers to sensitize or immobilize the nanocrystals for photocatalysis. Here, the current developments of conjugated polymer/nanocrystal nanocomposites for bulk heterojunction-type photovoltaics incorporating Cd- and Pb-based nanocrystals or quantum dots are reviewed. The effects of manipulating the organic ligands and the concentration of the nanocrystal precursor, critical factors that affect the shape and aggregation of the nanocrystals, are also discussed. In the conclusion, the mechanisms through which conjugated polymers can sensitize semiconductor nanocrystals (TiO2 , ZnO) to ensure efficient charge separation, as well as how they can support immobilized nanocrystals for use in photocatalysis, are addressed. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Cation Exchange Reactions for Improved Quality and Diversity of Semiconductor Nanocrystals

NASA Astrophysics Data System (ADS)

Beberwyck, Brandon James

Observing the size and shape dependent physical properties of semiconductor nanocrystals requires synthetic methods capable of not only composition and crystalline phase control but also molecular scale uniformity for a particle consisting of tens to hundreds of thousands of atoms. The desire for synthetic methods that produce uniform nanocrystals of complex morphologies continues to increase as nanocrystals find roles in commercial applications, such as biolabeling and display technologies, that are simultaneously restricting material compositions. With these constraints, new synthetic strategies that decouple the nanocrystal's chemical composition from its morphology are necessary. This dissertation explores the cation exchange reaction of colloidal semiconductor nanocrystals, a template-based chemical transformation that enables the interconversion of nanocrystals between a variety of compositions while maintaining their size dispersity and morphology. Chapter 1 provides an introduction to the versatility of this replacement reaction as a synthetic method for semiconductor nanocrystals. An overview of the fundamentals of the cation exchange reaction and the diversity of products that are achievable is presented. Chapter 2 examines the optical properties of nanocrystal heterostructures produced through cation exchange reactions. The deleterious impact of exchange on the photoluminescence is correlated to residual impurities and a simple annealing protocol is demonstrated to achieve photoluminescence yields comparable to samples produced by conventional methods. Chapter 3 investigates the extension of the cation exchange reaction beyond ionic nanocrystals. Covalent III-V nanocrystal of high crystallinity and low size dispersity are synthesized by the cation exchange of cadmium pnictide nanocrystals with group 13 ions. Lastly, Chapter 4 highlights future studies to probe cation exchange reactions in colloidal semiconductor nanocrystals and progress that needs to be

An optimized microfabricated platform for the optical generation and detection of hyperpolarized 129Xe

PubMed Central

Kennedy, Daniel J.; Seltzer, Scott J.; Jiménez-Martínez, Ricardo; Ring, Hattie L.; Malecek, Nicolas S.; Knappe, Svenja; Donley, Elizabeth A.; Kitching, John; Bajaj, Vikram S.; Pines, Alexander

2017-01-01

Low thermal-equilibrium nuclear spin polarizations and the need for sophisticated instrumentation render conventional nuclear magnetic resonance (NMR) spectroscopy and imaging (MRI) incompatible with small-scale microfluidic devices. Hyperpolarized 129Xe gas has found use in the study of many materials but has required very large and expensive instrumentation. Recently a microfabricated device with modest instrumentation demonstrated all-optical hyperpolarization and detection of 129Xe gas. This device was limited by 129Xe polarizations less than 1%, 129Xe NMR signals smaller than 20 nT, and transport of hyperpolarized 129Xe over millimeter lengths. Higher polarizations, versatile detection schemes, and flow of 129Xe over larger distances are desirable for wider applications. Here we demonstrate an ultra-sensitive microfabricated platform that achieves 129Xe polarizations reaching 7%, NMR signals exceeding 1 μT, lifetimes up to 6 s, and simultaneous two-mode detection, consisting of a high-sensitivity in situ channel with signal-to-noise of 105 and a lower-sensitivity ex situ detection channel which may be useful in a wider variety of conditions. 129Xe is hyperpolarized and detected in locations more than 1 cm apart. Our versatile device is an optimal platform for microfluidic magnetic resonance in particular, but equally attractive for wider nuclear spin applications benefitting from ultra-sensitive detection, long coherences, and simple instrumentation. PMID:28266629

An optimized microfabricated platform for the optical generation and detection of hyperpolarized 129Xe

DOE PAGES

Kennedy, Daniel J.; Seltzer, Scott J.; Jiménez-Martínez, Ricardo; ...

2017-03-07

Low thermal-equilibrium nuclear spin polarizations and the need for sophisticated instrumentation render conventional nuclear magnetic resonance (NMR) spectroscopy and imaging (MRI) incompatible with small-scale microfluidic devices. Hyperpolarized 129Xe gas has found use in the study of many materials but has required very large and expensive instrumentation. Recently a microfabricated device with modest instrumentation demonstrated all-optical hyperpolarization and detection of 129Xe gas. This device was limited by 129Xe polarizations less than 1%, 129Xe NMR signals smaller than 20 nT, and transport of hyperpolarized 129Xe over millimeter lengths. Higher polarizations, versatile detection schemes, and flow of 129Xe over larger distances are desirablemore » for wider applications. Here we demonstrate an ultra-sensitive microfabricated platform that achieves 129Xe polarizations reaching 7%, NMR signals exceeding 1 μT, lifetimes up to 6 s, and simultaneous two-mode detection, consisting of a high-sensitivity in situ channel with signal-to-noise of 10 5 and a lower-sensitivity ex situ detection channel which may be useful in a wider variety of conditions. 129Xe is hyperpolarized and detected in locations more than 1 cm apart. Our versatile device is an optimal platform for microfluidic magnetic resonance in particular, but equally attractive for wider nuclear spin applications benefitting from ultra-sensitive detection, long coherences, and simple instrumentation.« less

Study of high-j neutron excitations outside 136Xe

NASA Astrophysics Data System (ADS)

Talwar, R.; Kay, B. P.; Mitchell, A. J.; Adachi, S.; Entwisle, J. P.; Fujita, Y.; Gey, G.; Noji, S.; Ong, H. J.; Schiffer, J. P.; Tamii, A.

2017-09-01

The character of single-neutron excitations outside of N = 82 has been studied using nucleon transfer reactions in terms of the energy centroid of their strength as well as the fragmentation of this strength among the actual states of the nucleus. However, extending the systematic study of the N = 83 isotones to 137Xe has been challenging due to xenon being a gas at room temperature. Though several attempts have been made, a quantitative determination of the spectroscopic factors for the neutron 9/2- and 13/2+ excitations in 137Xe is still lacking. In the present work, we report on a study of the 136Xe(α,3He)137Xe reaction carried out at 100 MeV to probe the l = 5 , 9/2- and l = 6 , 13/2+ single-neutron excitations. The experimental technique and results will be presented discussing them in context of the evolution of these single-neutron excitations and the influence of the tensor interaction on the neutron single-particle states as the proton orbits are filling. This work has been supported by the U.S. Department of Energy, Office of Science, Office of Nuclear Physics, under Contract Number DE-AC02-06CH11357, the Australian Research Council Discovery Project 120104176, and the UK Science and Technology Facilities.

Biomimetic synthesis of noble metal nanocrystals

NASA Astrophysics Data System (ADS)

Chiu, Chin-Yi

At the nanometer scale, the physical and chemical properties of materials heavily depend on their sizes and shapes. This fact has triggered considerable efforts in developing controllable nanomaterial synthesis. The controlled growth of colloidal nanocrystal is a kinetic process, in which high-energy facets grow faster and then vanish, leading to a nanocrystal enclosed by low-energy facets. Identifying a surfactant that can selectively bind to a particular crystal facet and thus lower its surface energy, is critical and challenging in shape controlled synthesis of nanocrystals. Biomolecules exhibiting exquisite molecular recognition properties can be exploited to precisely engineer nanostructured materials. In the first part of my thesis, we employed the phage display technique to select a specific multifunctional peptide sequence which can bind on Pd surface and mediate Pd crystal nucleation and growth, achieving size controlled synthesis of Pd nanocrystals in aqueous solution. We further demonstrated a rational biomimetic approach to the predictable synthesis of nanocrystals enclosed by a particular facet in the case of Pt. Specifically, Pt {100} and Pt {111} facet-specific peptides were identified and used to synthesize Pt nanocubes and Pt nano-tetrahedrons, respectively. The mechanistic studies of Pt {111} facet-specific peptide had led us to study the facet-selective adsorption of aromatic molecules on noble metal surfaces. The discoveries had achieved the development of design strategies to select facet-selective molecules which can synthesize nanocrystals with expected shapes in both Pt and Pd system. At last, we exploited Pt facet-specific peptides and controlled the molecular interaction to produce one- and three- dimensional nanostructures composed of anisotropic nanoparticles in synthetic conditions without supramolecular pre-organization, demonstrating the full potential of biomolecules in mediating material formation process. My research on biomimetic

Experimental ion mobility measurements in Xe-CO2

NASA Astrophysics Data System (ADS)

Cortez, A. F. V.; Santos, M. A. G.; Veenhof, R.; Patra, R. N.; Neves, P. N. B.; Santos, F. P.; Borges, F. I. G. M.; Conde, C. A. N.

2017-06-01

Data on ion mobility is important to improve the performance of large volume gaseous detectors. In the present work the method, experimental setup and results for the ion mobility measurements in Xe-CO2 mixtures are presented. The results for this mixture show the presence of only one peak for all gas ratios of Xe-CO2, low reduced electric fields, E/N, 10-25 Td (2.4-6.1 kV·cm-1·bar-1), low pressures 6-8 Torr (8-10.6 mbar), at room temperature.

Size- and shape-dependent surface thermodynamic properties of nanocrystals

NASA Astrophysics Data System (ADS)

Fu, Qingshan; Xue, Yongqiang; Cui, Zixiang

2018-05-01

As the fundamental properties, the surface thermodynamic properties of nanocrystals play a key role in the physical and chemical changes. However, it remains ambiguous about the quantitative influence regularities of size and shape on the surface thermodynamic properties of nanocrystals. Thus by introducing interface variables into the Gibbs energy and combining Young-Laplace equation, relations between the surface thermodynamic properties (surface Gibbs energy, surface enthalpy, surface entropy, surface energy and surface heat capacity), respectively, and size of nanocrystals with different shapes were derived. Theoretical estimations of the orders of the surface thermodynamic properties of nanocrystals agree with available experimental values. Calculated results of the surface thermodynamic properties of Au, Bi and Al nanocrystals suggest that when r > 10 nm, the surface thermodynamic properties linearly vary with the reciprocal of particle size, and when r < 10 nm, the effect of particle size on the surface thermodynamic properties becomes greater and deviates from linear variation. For nanocrystals with identical equivalent diameter, the more the shape deviates from sphere, the larger the surface thermodynamic properties (absolute value) are.

Genetics Home Reference: fragile XE syndrome

MedlinePlus

... are so mild that the individuals function normally. Learning disabilities are the most common sign of impaired cognitive function in people with fragile XE syndrome . The learning disabilities are likely a result of communication and behavioral ...

Trampoline motions in Xe-graphite(0 0 0 1) surface scattering

NASA Astrophysics Data System (ADS)

Watanabe, Yoshimasa; Yamaguchi, Hiroki; Hashinokuchi, Michihiro; Sawabe, Kyoichi; Maruyama, Shigeo; Matsumoto, Yoichiro; Shobatake, Kosuke

2005-09-01

We have investigated Xe scattering from the graphite(0 0 0 1) surface at hyperthermal incident energies using a molecular beam-surface scattering technique and molecular dynamics simulations. For all incident conditions, the incident Xe atom conserves the momentum parallel to the surface and loses approximately 80% of the normal incident energy. The weak interlayer potential of graphite disperses the deformation over the wide range of a graphene sheet. The dynamic corrugation induced by the collision is smooth even at hyperthermal incident energy; the graphene sheet moves like a trampoline net and the Xe atom like a trampoliner.

Gain measurements of the Ca-Xe charge exchange system. [for UV lasers

NASA Technical Reports Server (NTRS)

Michels, C. J.; Chubb, D. L.

1978-01-01

Charge-exchange-pumped Ca(+) was studied for possible positive laser gain at 370.6 and 315.9 nm using an Xe MPD arc as the Xe(+) source. The present paper describes the MPD arc, the calcium injection system, the diagnostics for gain, and spontaneous emission measurements and results. No positive gain measurements were observed. A small Xe-Ca charge exchange cross section compared to He-metal laser systems charge exchange cross sections is the most probable reason why the result was negative.

ZIF-Derived Nitrogen-Doped Porous Carbons for Xe Adsorption and Separation

NASA Astrophysics Data System (ADS)

Zhong, Shan; Wang, Qian; Cao, Dapeng

2016-02-01

Currently, finding high capacity adsorbents with large selectivity to capture Xe is still a great challenge. In this work, nitrogen-doped porous carbons were prepared by programmable temperature carbonization of zeolitic imidazolate framework-8 (ZIF-8) and ZIF-8/xylitol composite precursors and the resultant samples are marked as Carbon-Z and Carbon-ZX, respectively. Further adsorption measurements indicate that ZIF-derived nitrogen-doped Carbon-ZX exhibits extremely high Xe capacity of 4.42 mmol g-1 at 298 K and 1 bar, which is higher than almost all other pristine MOFs such as CuBTC, Ni/DOBDC, MOF-5 and Al-MIL-53, and even more than three times of the matrix ZIF-8 at similar conditions. Moreover, Carbon-ZX also shows the highest Xe/N2 selectivity about ~120, which is much larger than all other reported MOFs. These remarkable features illustrate that ZIF-derived nitrogen-doped porous carbon is an excellent adsorbent for Xe adsorption and separation at room temperature.

Synthesis of the missing oxide of xenon, XeO2, and its implications for Earth's missing xenon.

PubMed

Brock, David S; Schrobilgen, Gary J

2011-04-27

The missing Xe(IV) oxide, XeO(2), has been synthesized at 0 °C by hydrolysis of XeF(4) in water and 2.00 M H(2)SO(4(aq)). Raman spectroscopy and (16/18)O isotopic enrichment studies indicate that XeO(2) possesses an extended structure in which Xe(IV) is oxygen bridged to four neighboring oxygen atoms to give a local square-planar XeO(4) geometry based on an AX(4)E(2) valence shell electron pair repulsion (VSEPR) arrangement. The vibrational spectra of Xe(16)O(2) and Xe(18)O(2) amend prior vibrational assignments of xenon doped SiO(2) and are in accordance with prior speculation that xenon depletion from the Earth's atmosphere may occur by xenon insertion at high temperatures and high pressures into SiO(2) in the Earth's crust.

Search for the permanent electric dipole moment of 129Xe

NASA Astrophysics Data System (ADS)

Sachdeva, Natasha; Chupp, Timothy; Gong, Fei; Babcock, Earl; Salhi, Zahir; Burghoff, Martin; Fan, Isaac; Killian, Wolfgang; Knappe-Grüneberg, Silvia; Schabel, Allard; Seifert, Frank; Trahms, Lutz; Voigt, Jens; Degenkolb, Skyler; Fierlinger, Peter; Krägeloh, Eva; Lins, Tobias; Marino, Michael; Meinel, Jonas; Niessen, Benjamin; Stuiber, Stefan; Terrano, William; Kuchler, Florian; Singh, Jaideep

2017-09-01

CP-violation in Beyond-the-Standard-Model physics, necessary to explain the baryon asymmetry, gives rise to permanent electric dipole moments (EDMs). EDM measurements of the neutron, electron, paramagnetic and diamagnetic atoms constrain CP-violating parameters. The current limit for the 129Xe EDM is 6 ×10-27 e . cm (95 % CL). The HeXeEDM experiment at FRM-II (Munich Research Reactor) and BMSR-2 (Berlin Magnetically Shielded Room) uses a stable magnetic field in a magnetically shielded room and 3He comagnetometer with potential to improve the limit by two orders of magnitude. Polarized 3He and 129Xe free precession is detected with SQUID magnetometers in the presence of applied electric and magnetic fields. Conclusions from recent measurements will be presented.

Inhibition of palm oil oxidation by zeolite nanocrystals.

PubMed

Tan, Kok-Hou; Awala, Hussein; Mukti, Rino R; Wong, Ka-Lun; Rigaud, Baptiste; Ling, Tau Chuan; Aleksandrov, Hristiyan A; Koleva, Iskra Z; Vayssilov, Georgi N; Mintova, Svetlana; Ng, Eng-Poh

2015-05-13

The efficiency of zeolite X nanocrystals (FAU-type framework structure) containing different extra-framework cations (Li(+), Na(+), K(+), and Ca(2+)) in slowing the thermal oxidation of palm oil is reported. The oxidation study of palm oil is conducted in the presence of zeolite nanocrystals (0.5 wt %) at 150 °C. Several characterization techniques such as visual analysis, colorimetry, rheometry, total acid number (TAN), FT-IR spectroscopy, (1)H NMR spectroscopy, and Karl Fischer analyses are applied to follow the oxidative evolution of the oil. It was found that zeolite nanocrystals decelerate the oxidation of palm oil through stabilization of hydroperoxides, which are the primary oxidation product, and concurrently via adsorption of the secondary oxidation products (alcohols, aldehydes, ketones, carboxylic acids, and esters). In addition to the experimental results, periodic density functional theory (DFT) calculations are performed to elucidate further the oxidation process of the palm oil in the presence of zeolite nanocrystals. The DFT calculations show that the metal complexes formed with peroxides are more stable than the complexes with alkenes with the same ions. The peroxides captured in the zeolite X nanocrystals consequently decelerate further oxidation toward formation of acids. Unlike the monovalent alkali metal cations in the zeolite X nanocrystals (K(+), Na(+), and Li(+)), Ca(2+) reduced the acidity of the oil by neutralizing the acidic carboxylate compounds to COO(-)(Ca(2+))1/2 species.

Si-nanocrystal-based nanofluids for nanothermometry

NASA Astrophysics Data System (ADS)

Cardona-Castro, M. A.; Morales-Sánchez, A.; Licea-Jiménez, L.; Alvarez-Quintana, J.

2016-06-01

The measurement of local temperature in nanoscale volumes is becoming a technological frontier. Photoluminescent nanoparticles and nanocolloids are the natural choice for nanoscale temperature probes. However, the influence of a surrounding liquid on the cryogenic behavior of oxidized Si-nanocrystals (Si-NCs) has never been investigated. In this work, the photoluminescence (PL) of oxidized Si-NCs/alcohol based nanocolloids is measured as a function of the temperature and the molecule length of monohydric alcohols above their melting-freezing point. The results unveil a progressive blue shift on the emission peak which is dependent on the temperature as well as the dielectric properties of the surrounding liquid. Such an effect is analyzed in terms of thermal changes of the Si-NCs bandgap, quantum confinement and the polarization effects of the embedding medium; revealing an important role of the dielectric constant of the surrounding liquid. These results are relevant because they offer a general insight to the fundamental behavior of photoluminescent nanocolloids under a cooling process and moreover, enabling PL tuning based on the dielectric properties of the surrounding liquid. Hence, the variables required to engineer PL of nanofluids are properly identified for use as temperature sensors at the nanoscale.

Osteoblasts Growth Behaviour on Bio-Based Calcium Carbonate Aragonite Nanocrystal

PubMed Central

Zakaria, Zuki Abu Bakar

2014-01-01

Calcium carbonate (CaCO3) nanocrystals derived from cockle shells emerge to present a good concert in bone tissue engineering because of their potential to mimic the composition, structure, and properties of native bone. The aim of this study was to evaluate the biological response of CaCO3 nanocrystals on hFOB 1.19 and MC3T3 E-1 osteoblast cells in vitro. Cell viability and proliferation were assessed by MTT and BrdU assays, and LDH was measured to determine the effect of CaCO3 nanocrystals on cell membrane integrity. Cellular morphology was examined by SEM and fluorescence microscopy. The results showed that CaCO3 nanocrystals had no toxic effects to some extent. Cell proliferation, alkaline phosphatase activity, and protein synthesis were enhanced by the nanocrystals when compared to the control. Cellular interactions were improved, as indicated by SEM and fluorescent microscopy. The production of VEGF and TGF-1 was also affected by the CaCO3 nanocrystals. Therefore, bio-based CaCO3 nanocrystals were shown to stimulate osteoblast differentiation and improve the osteointegration process. PMID:24734228

Laser generation of XeCl exciplex molecules in a longitudinal repetitively pulsed discharge in a Xe - CsCl mixture

NASA Astrophysics Data System (ADS)

Boichenko, A. M.; Klenovskii, M. S.

2015-12-01

By using the previously developed kinetic model, we have carried out simulations to study the possibility of laser generation of XeCl exciplex molecules in the working medium based on a mixture of Xe with CsCl vapours, excited by a longitudinal repetitively pulsed discharge. The formation mechanism of exciplex molecules in this mixture is fundamentally different from the formation mechanisms in the traditional mixtures of exciplex lasers. The conditions that make the laser generation possible are discussed. For these conditions, with allowance for available specific experimental conditions of the repetitively pulsed discharge excitation, we have obtained the calculated dependences of the power and efficiency of generation on the reflectivity of mirrors in a laser cavity.

Chelating ligands for nanocrystals' surface functionalization.

PubMed

Querner, Claudia; Reiss, Peter; Bleuse, Joël; Pron, Adam

2004-09-22

A new family of ligands for the surface functionalization of CdSe nanocrystals is proposed, namely alkyl or aryl derivatives of carbodithioic acids (R-C(S)SH). The main advantages of these new ligands are as follows: they nearly quantitatively exchange the initial surface ligands (TOPO) in very mild conditions; they significantly improve the resistance of nanocrystals against photooxidation because of their ability of strong chelate-type binding to metal atoms; their relatively simple preparation via Grignard intermediates facilitates the development of new bifunctional ligands containing, in addition to the anchoring carbodithioate group, a second function, which enables the grafting of molecules or macromolecules of interest on the nanocrystal surface. To give an example of this approach, we report, for the first time, the grafting of an electroactive oligomer from the polyaniline family-aniline tetramer-on CdSe nanocrystals after their functionalization with 4-formyldithiobenzoic acid. The grafting proceeds via a condensation reaction between the aldehyde group of the ligand and the terminal primary amine group of the tetramer. The resulting organic/inorganic hybrid exhibits complete extinction of the fluorescence of its constituents, indicating efficient charge or energy transfer between the organic and the inorganic semiconductors.

Near-infrared light emitting device using semiconductor nanocrystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Supran, Geoffrey J.S.; Song, Katherine W.; Hwang, Gyuweon

A near-infrared light emitting device can include semiconductor nanocrystals that emit at wavelengths beyond 1 .mu.m. The semiconductor nanocrystals can include a core and an overcoating on a surface of the core.

Plasmonic engineering of spontaneous emission from silicon nanocrystals.

PubMed

Goffard, Julie; Gérard, Davy; Miska, Patrice; Baudrion, Anne-Laure; Deturche, Régis; Plain, Jérôme

2013-01-01

Silicon nanocrystals offer huge advantages compared to other semi-conductor quantum dots as they are made from an abundant, non-toxic material and are compatible with silicon devices. Besides, among a wealth of extraordinary properties ranging from catalysis to nanomedicine, metal nanoparticles are known to increase the radiative emission rate of semiconductor quantum dots. Here, we use gold nanoparticles to accelerate the emission of silicon nanocrystals. The resulting integrated hybrid emitter is 5-fold brighter than bare silicon nanocrystals. We also propose an in-depth analysis highlighting the role of the different physical parameters in the photoluminescence enhancement phenomenon. This result has important implications for the practical use of silicon nanocrystals in optoelectronic devices, for instance for the design of efficient down-shifting devices that could be integrated within future silicon solar cells.

Angle Performance on Optima XE

DOE Office of Scientific and Technical Information (OSTI.GOV)

David, Jonathan; Satoh, Shu

2011-01-07

Angle control on high energy implanters is important due to shrinking device dimensions, and sensitivity to channeling at high beam energies. On Optima XE, beam-to-wafer angles are controlled in both the horizontal and vertical directions. In the horizontal direction, the beam angle is measured through a series of narrow slits, and any angle adjustment is made by steering the beam with the corrector magnet. In the vertical direction, the beam angle is measured through a high aspect ratio mask, and any angle adjustment is made by slightly tilting the wafer platen during implant.Using a sensitive channeling condition, we were ablemore » to quantify the angle repeatability of Optima XE. By quantifying the sheet resistance sensitivity to both horizontal and vertical angle variation, the total angle variation was calculated as 0.04 deg. (1{sigma}). Implants were run over a five week period, with all of the wafers selected from a single boule, in order to control for any crystal cut variation.« less

One-Step Synthesis of Monodisperse In-Doped ZnO Nanocrystals

NASA Astrophysics Data System (ADS)

Wang, Qing Ling; Yang, Ye Feng; He, Hai Ping; Chen, Dong Dong; Ye, Zhi Zhen; Jin, Yi Zheng

2010-05-01

A method for the synthesis of high quality indium-doped zinc oxide (In-doped ZnO) nanocrystals was developed using a one-step ester elimination reaction based on alcoholysis of metal carboxylate salts. The resulting nearly monodisperse nanocrystals are well-crystallized with typically crystal structure identical to that of wurtzite type of ZnO. Structural, optical, and elemental analyses on the products indicate the incorporation of indium into the host ZnO lattices. The individual nanocrystals with cubic structures were observed in the 5% In-ZnO reaction, due to the relatively high reactivity of indium precursors. Our study would provide further insights for the growth of doped oxide nanocrystals, and deepen the understanding of doping process in colloidal nanocrystal syntheses.

Flexible and low-voltage integrated circuits constructed from high-performance nanocrystal transistors.

PubMed

Kim, David K; Lai, Yuming; Diroll, Benjamin T; Murray, Christopher B; Kagan, Cherie R

2012-01-01

Colloidal semiconductor nanocrystals are emerging as a new class of solution-processable materials for low-cost, flexible, thin-film electronics. Although these colloidal inks have been shown to form single, thin-film field-effect transistors with impressive characteristics, the use of multiple high-performance nanocrystal field-effect transistors in large-area integrated circuits has not been shown. This is needed to understand and demonstrate the applicability of these discrete nanocrystal field-effect transistors for advanced electronic technologies. Here we report solution-deposited nanocrystal integrated circuits, showing nanocrystal integrated circuit inverters, amplifiers and ring oscillators, constructed from high-performance, low-voltage, low-hysteresis CdSe nanocrystal field-effect transistors with electron mobilities of up to 22 cm(2) V(-1) s(-1), current modulation >10(6) and subthreshold swing of 0.28 V dec(-1). We fabricated the nanocrystal field-effect transistors and nanocrystal integrated circuits from colloidal inks on flexible plastic substrates and scaled the devices to operate at low voltages. We demonstrate that colloidal nanocrystal field-effect transistors can be used as building blocks to construct complex integrated circuits, promising a viable material for low-cost, flexible, large-area electronics.

Na + Xe collisions in the presence of two nonresonant lasers

NASA Technical Reports Server (NTRS)

De Vries, P. L.; Chang, C. H.; George, T. F.; Laskowski, B.; Stallcop, J. R.

1980-01-01

Na+Xe collisions in the presence of two distinct laser fields (rhodamine 110 and Nd:glass) are investigated with reference to the response to nonresonant radiation of alkali metals collisionally perturbed by a buffer gas. It is found that the excited Na-asterisk (4s)+Xe state is produced with a measurable cross section due to two-photon absorption with field intensities as low as 10 MW/sq cm.

Octacosanol educes physico-chemical attributes, release and bioavailability as modified nanocrystals.

PubMed

Sen Gupta, Surashree; Ghosh, Mahua

2017-10-01

Octacosanol is a lesser known nutraceutical with the potential for treatment of several inflammatory diseases, high cholesterol, Parkinson's symptoms and tumour growth along with the capacity to improve athletic performance. But its lipophilicity and large structure inhibits extended solubility in water resulting in poor absorption and a low bioavailability. In the present work, sodium salt of octacosyl sulfate was synthesized. It displayed improved water solubility. Its nanocrystals, synthesized by means of nanoprecipitation technique, enhanced diffusion velocity, antioxidant capacity, shelf-life, penetrability and bioavailability. Particle size of the nanocrystals ranged between 197 and 220nm. Both modified octacosanol and its nanocrystals displayed maximum lipid peroxidation activities at a concentration 1000ppm, but nanocrystals demonstrated higher prevention. From freeze-thaw cycles it was evident that normal octacosanol crystals were far more prone to temperature variations than the nanocrystals. A pronounced increase in release/diffusion rate and bioavailability was observed for the nanocrystals of the modified octacosanol. In vitro release kinetics, bioavailability and bioequivalence were studied. Relative bioavailability for gastric passage and pancreatic passage of nanocrystals was 2.58 times and 1.81 times that of normal crystals respectively. Furthermore the nanocrystals displayed a superior in vitro release rate, while following a non-Fickian mode. Copyright © 2017 Elsevier B.V. All rights reserved.

Nonlinear characterization of silver nanocrystals incorporated tellurite glasses for fiber development

NASA Astrophysics Data System (ADS)

Zhou, Zhiguang; Tan, Wenjiang; Si, Jinhai; Zhan, Huan; He, Jianli; Lin, Aoxiang

2011-12-01

To develop high nonlinear optical fibers for all-optical switching applications, 7.5 wt% AgNO3 was incorporated into tellurite glasses with composition of 75TeO2-20ZnO-5Na2CO3 (TZN75) under precisely-controlled experimental conditions to form 7.5Ag-TZN75 glass. Surface Plasmon resonance absorption peak of Ag nanocrystals embedded in 7.5Ag-TZN75 glass was found to center at 552 nm. By degenerated four-wave mixing method, the non-resonant nonlinear refractive index, n2, of 7.5Ag-TZN75 glass was measured to be 7.54×10-19 m2•W-1 at 1500 nm, about 3 times of the reference TZN75 glass without any dopant and 27 times of the silicate glasses and fibers, and the response time is about 1 picosecond.

Uncovering the intrinsic size dependence of hydriding phase transformations in nanocrystals.

PubMed

Bardhan, Rizia; Hedges, Lester O; Pint, Cary L; Javey, Ali; Whitelam, Stephen; Urban, Jeffrey J

2013-10-01

A quantitative understanding of nanocrystal phase transformations would enable more efficient energy conversion and catalysis, but has been hindered by difficulties in directly monitoring well-characterized nanoscale systems in reactive environments. We present a new in situ luminescence-based probe enabling direct quantification of nanocrystal phase transformations, applied here to the hydriding transformation of palladium nanocrystals. Our approach reveals the intrinsic kinetics and thermodynamics of nanocrystal phase transformations, eliminating complications of substrate strain, ligand effects and external signal transducers. Clear size-dependent trends emerge in nanocrystals long accepted to be bulk-like in behaviour. Statistical mechanical simulations show these trends to be a consequence of nanoconfinement of a thermally driven, first-order phase transition: near the phase boundary, critical nuclei of the new phase are comparable in size to the nanocrystal itself. Transformation rates are then unavoidably governed by nanocrystal dimensions. Our results provide a general framework for understanding how nanoconfinement fundamentally impacts broad classes of thermally driven solid-state phase transformations relevant to hydrogen storage, catalysis, batteries and fuel cells.

Multicolour synthesis in lanthanide-doped nanocrystals through cation exchange in water

NASA Astrophysics Data System (ADS)

Han, Sanyang; Qin, Xian; An, Zhongfu; Zhu, Yihan; Liang, Liangliang; Han, Yu; Huang, Wei; Liu, Xiaogang

2016-10-01

Meeting the high demand for lanthanide-doped luminescent nanocrystals across a broad range of fields hinges upon the development of a robust synthetic protocol that provides rapid, just-in-time nanocrystal preparation. However, to date, almost all lanthanide-doped luminescent nanomaterials have relied on direct synthesis requiring stringent controls over crystal nucleation and growth at elevated temperatures. Here we demonstrate the use of a cation exchange strategy for expeditiously accessing large classes of such nanocrystals. By combining the process of cation exchange with energy migration, the luminescence properties of the nanocrystals can be easily tuned while preserving the size, morphology and crystal phase of the initial nanocrystal template. This post-synthesis strategy enables us to achieve upconversion luminescence in Ce3+ and Mn2+-activated hexagonal-phased nanocrystals, opening a gateway towards applications ranging from chemical sensing to anti-counterfeiting.

Low-frequency Raman scattering in a Xe hydrate.

PubMed

Adichtchev, S V; Belosludov, V R; Ildyakov, A V; Malinovsky, V K; Manakov, A Yu; Subbotin, O S; Surovtsev, N V

2013-09-12

The physics of gas hydrates are rich in interesting phenomena such as anomalies for thermal conductivity, self-preservation effects for decomposition, and others. Some of these phenomena are presumably attributed to the resonance interaction of the rattling motions of guest molecules or atoms with the lattice modes. This can be expected to induce some specific features in the low-frequency (THz) vibrational response. Here we present results for low-frequency Raman scattering in a Xe hydrate, supported by numerical calculations of vibrational density of states. A number of narrow lines, located in the range from 18 to 90 cm(-1), were found in the Raman spectrum. Numerical calculations confirm that these lines correspond to resonance modes of the Xe hydrate. Also, low-frequency Raman scattering was studied during gas hydrate decomposition, and two scenarios were observed. The first one is the direct decomposition of the Xe hydrate to water and gas. The second one is the hydrate decomposition to ice and gas with subsequent melting of ice. In the latter case, a transient low-frequency Raman band is observed, which is associated with low-frequency bands (e.g., boson peak) of disordered solids.

Organization of 'nanocrystal molecules' using DNA

NASA Astrophysics Data System (ADS)

Alivisatos, A. Paul; Johnsson, Kai P.; Peng, Xiaogang; Wilson, Troy E.; Loweth, Colin J.; Bruchez, Marcel P.; Schultz, Peter G.

1996-08-01

PATTERNING matter on the nanometre scale is an important objective of current materials chemistry and physics. It is driven by both the need to further miniaturize electronic components and the fact that at the nanometre scale, materials properties are strongly size-dependent and thus can be tuned sensitively1. In nanoscale crystals, quantum size effects and the large number of surface atoms influence the, chemical, electronic, magnetic and optical behaviour2-4. 'Top-down' (for example, lithographic) methods for nanoscale manipulation reach only to the upper end of the nanometre regime5; but whereas 'bottom-up' wet chemical techniques allow for the preparation of mono-disperse, defect-free crystallites just 1-10 nm in size6-10, ways to control the structure of nanocrystal assemblies are scarce. Here we describe a strategy for the synthesis of'nanocrystal molecules', in which discrete numbers of gold nanocrystals are organized into spatially defined structures based on Watson-Crick base-pairing interactions. We attach single-stranded DNA oligonucleotides of defined length and sequence to individual nanocrystals, and these assemble into dimers and trimers on addition of a complementary single-stranded DNA template. We anticipate that this approach should allow the construction of more complex two-and three-dimensional assemblies.

Experimental ion mobility measurements in Xe-CH4

NASA Astrophysics Data System (ADS)

Perdigoto, J. M. C.; Cortez, A. F. V.; Veenhof, R.; Neves, P. N. B.; Santos, F. P.; Borges, F. I. G. M.; Conde, C. A. N.

2017-09-01

Data on ion mobility is important to improve the performance of large volume gaseous detectors. In the present work, the method, experimental setup and results for the ion mobility measurements in Xe-CH4 mixtures are presented. The results for this mixture show the presence of two distinct groups of ions. The nature of the ions depend on the mixture ratio since they are originated by both Xe and CH4. The results here presented were obtained for low reduced electric fields, E/N, 10-25 Td (2.4-6.1 kV ṡ cm-1 ṡ bar-1), at low pressure (8 Torr) (10.6 mbar), and at room temperature.

Shaped nanocrystal particles and methods for making the same

DOEpatents

Alivisatos, A Paul [Oakland, CA; Scher, Erik C [Menlo Park, CA; Manna, Liberato [Berkeley, CA

2011-11-22

Shaped nanocrystal particles and methods for making shaped nanocrystal particles are disclosed. One embodiment includes a method for forming a branched, nanocrystal particle. It includes (a) forming a core having a first crystal structure in a solution, (b) forming a first arm extending from the core having a second crystal structure in the solution, and (c) forming a second arm extending from the core having the second crystal structure in the solution.

Shaped nanocrystal particles and methods for making the same

DOEpatents

Alivisatos, A. Paul; Scher, Erik C; Manna, Liberato

2013-12-17

Shaped nanocrystal particles and methods for making shaped nanocrystal particles are disclosed. One embodiment includes a method for forming a branched, nanocrystal particle. It includes (a) forming a core having a first crystal structure in a solution, (b) forming a first arm extending from the core having a second crystal structure in the solution, and (c) forming a second arm extending from the core having the second crystal structure in the solution.

Shaped nanocrystal particles and methods for working the same

DOEpatents

Alivisatos, A. Paul; Sher, Eric C.; Manna, Liberato

2007-12-25

Shaped nanocrystal particles and methods for making shaped nanocrystal particles are disclosed. One embodiment includes a method for forming a branched, nanocrystal particle. It includes (a) forming a core having a first crystal structure in a solution, (b) forming a first arm extending from the core having a second crystal structure in the solution, and (c) forming a second arm extending from the core having the second crystal structure in the solution.

Gold nanocrystals with DNA-directed morphologies.

PubMed

Ma, Xingyi; Huh, June; Park, Wounjhang; Lee, Luke P; Kwon, Young Jik; Sim, Sang Jun

2016-09-16

Precise control over the structure of metal nanomaterials is important for developing advanced nanobiotechnology. Assembly methods of nanoparticles into structured blocks have been widely demonstrated recently. However, synthesis of nanocrystals with controlled, three-dimensional structures remains challenging. Here we show a directed crystallization of gold by a single DNA molecular regulator in a sequence-independent manner and its applications in three-dimensional topological controls of crystalline nanostructures. We anchor DNA onto gold nanoseed with various alignments to form gold nanocrystals with defined topologies. Some topologies are asymmetric including pushpin-, star- and biconcave disk-like structures, as well as more complex jellyfish- and flower-like structures. The approach of employing DNA enables the solution-based synthesis of nanocrystals with controlled, three-dimensional structures in a desired direction, and expands the current tools available for designing and synthesizing feature-rich nanomaterials for future translational biotechnology.

Engineering of Organic Nanocrystals by Electrocrystallization

NASA Astrophysics Data System (ADS)

Kilani, Mohamed

This work discusses the experimental and theoretical methods used to control the morphology of nanocrystals. The hypothesis of the thermodynamic/kinetic control of the morphology was verified. We applied the electrocrystallization to make K(def)TCP nanocrystals and we tuned the electrochemical parameters to determine their influence on the nanocrystals morphologies. The characterization was mainly performed with AFM and FE-SEM. We presented in this work the possibility to control the morphology of K(def)TCP using the electrochemical parameters. The obtained shapes ranged from nanorods to rhombohedral shape, which is reported for the first time. The observed growth behavior was modeled and simulated with a method based on Monte-Carlo techniques. The simulation results show a qualitative match with the experimental findings. This work contributes to the understanding of the crystal growth behavior and the thermodynamic/kinetic morphology transition using electrocrystallization.

Gold nanocrystals with DNA-directed morphologies

NASA Astrophysics Data System (ADS)

Ma, Xingyi; Huh, June; Park, Wounjhang; Lee, Luke P.; Kwon, Young Jik; Sim, Sang Jun

2016-09-01

Precise control over the structure of metal nanomaterials is important for developing advanced nanobiotechnology. Assembly methods of nanoparticles into structured blocks have been widely demonstrated recently. However, synthesis of nanocrystals with controlled, three-dimensional structures remains challenging. Here we show a directed crystallization of gold by a single DNA molecular regulator in a sequence-independent manner and its applications in three-dimensional topological controls of crystalline nanostructures. We anchor DNA onto gold nanoseed with various alignments to form gold nanocrystals with defined topologies. Some topologies are asymmetric including pushpin-, star- and biconcave disk-like structures, as well as more complex jellyfish- and flower-like structures. The approach of employing DNA enables the solution-based synthesis of nanocrystals with controlled, three-dimensional structures in a desired direction, and expands the current tools available for designing and synthesizing feature-rich nanomaterials for future translational biotechnology.

Photophysical properties of wavelength-tunable methylammonium lead halide perovskite nanocrystals

DOE PAGES

Freppon, Daniel J.; Men, Long; Burkhow, Sadie J.; ...

2016-11-25

Here we present the time-correlated luminescence of isolated nanocrystals of five methylammonium lead mixed-halide perovskite compositions (CH 3NH 3PbBr 3$-$xI x) that were synthesized with varying iodide and bromide anion loading. All analyzed nanocrystals had a spherical morphology with diameters in the range of 2 to 32 nm. The luminescence maxima of CH 3NH 3PbBr 3$-$xI x nanocrystals were tuned to wavelengths ranging between 498 and 740 nm by varying the halide loading. Both CH 3NH 3PbI 3 and CH 3NH 3PbBr 3 nanocrystals exhibited no luminescence intermittency for more than 90% of the 250 s analysis time, as definedmore » by a luminescence intensity three standard deviations above the background. The mixed halide CH 3NH 3PbBr 0.75I 0.25, CH 3NH 3PbBr 0.50I 0.50, and CH 3NH 3PbBr 0.25I 0.75 nanocrystals exhibited luminescence intermittency in 18%, 4% and 26% of the nanocrystals, respectively. Irrespective of luminescence intermittency, luminescence intensities were classified for each nanocrystal as: (a) constant, (b) multimodal, (c) photobrightening, and (d) photobleaching. Finally, based on their photophysics, the CH 3NH 3PbBr 3$-$xI x nanocrystals can be expected to be useful in a wide-range of applications where low and non-intermittent luminescence is desirable, for example as imaging probes and in films for energy conversion devices.« less

Photophysical properties of wavelength-tunable methylammonium lead halide perovskite nanocrystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Freppon, Daniel J.; Men, Long; Burkhow, Sadie J.

Here we present the time-correlated luminescence of isolated nanocrystals of five methylammonium lead mixed-halide perovskite compositions (CH 3NH 3PbBr 3$-$xI x) that were synthesized with varying iodide and bromide anion loading. All analyzed nanocrystals had a spherical morphology with diameters in the range of 2 to 32 nm. The luminescence maxima of CH 3NH 3PbBr 3$-$xI x nanocrystals were tuned to wavelengths ranging between 498 and 740 nm by varying the halide loading. Both CH 3NH 3PbI 3 and CH 3NH 3PbBr 3 nanocrystals exhibited no luminescence intermittency for more than 90% of the 250 s analysis time, as definedmore » by a luminescence intensity three standard deviations above the background. The mixed halide CH 3NH 3PbBr 0.75I 0.25, CH 3NH 3PbBr 0.50I 0.50, and CH 3NH 3PbBr 0.25I 0.75 nanocrystals exhibited luminescence intermittency in 18%, 4% and 26% of the nanocrystals, respectively. Irrespective of luminescence intermittency, luminescence intensities were classified for each nanocrystal as: (a) constant, (b) multimodal, (c) photobrightening, and (d) photobleaching. Finally, based on their photophysics, the CH 3NH 3PbBr 3$-$xI x nanocrystals can be expected to be useful in a wide-range of applications where low and non-intermittent luminescence is desirable, for example as imaging probes and in films for energy conversion devices.« less

The Use of Cellulose Nanocrystals for Potential Application in Topical Delivery of Hydroquinone.

PubMed

Taheri, Azade; Mohammadi, Mina

2015-07-01

Nanotechnology-based drug delivery systems can enhance drug permeation through the skin and improve the drug stability. The biodegradability and biocompatibility of cellulose nanocrystals have made these nanoparticles good candidates to use in biomedical applications. The hyperpigmentation is a common skin disorder that could be caused by number of reasons such as sun exposure and pregnancy. Hydroquinone could inhibit the production of melanin and eliminate the discolorations of skin. This study is aimed at introducing cellulose nanocrystals as suitable carriers for drug delivery to skin. Prepared cellulose nanocrystals were characterized by dynamic light scattering and atomic force microscopy. The size of cellulose nanocrystals determined using dynamic light scattering was 301 ± 10 nm. Hydroquinone-cellulose nanocrystal complex was prepared by incubating of hydroquinone solution in cellulose nanocrystals suspension. The size of hydroquinone-cellulose nanocrystal complex determined using dynamic light scattering was 310 ± 10 nm. The hydroquinone content of the hydroquinone-cellulose complex was determined using UV/vis spectroscopy. Hydroquinone was bound to cellulose nanocrystals representing 79.3 ± 2% maximum binding efficiency when 1.1 mg hydroquinone was added to 1 mL of cellulose nanocrystals suspension (2 mg cellulose nanocrystal). The hydroquinone-cellulose nanocrystal complex showed an approximately sustained release profile of hydroquinone. Approximately, 80% of bound hydroquinone released in 4 h. © 2014 John Wiley & Sons A/S.

The electroluminescence of Xe-Ne gas mixtures: A Monte Carol simulation study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Santos, F.P.; Dias, T.H.V.T.; Rachinhas, P.J.B.M.

1998-04-01

The authors have performed a Monte Carlo simulation of the drift of electrons through a mixture of gaseous xenon with the lighter noble gas neon at a total pressure of 1 atm. The electroluminescence characteristics and other transport parameters are investigated as a function of the reduced electric field and composition of the mixture. For Xe-Ne mixtures with 5, 10, 20, 40, 70, 90, and 100% of Xe, they present results for electroluminescence yield and excitation efficiency, average electron energy, electron drift velocity, reduced mobility, reduced diffusion coefficients, and characteristic energies over a range of reduced electric fields which excludemore » electron multiplication. For the 5% Xe mixture, they also assess the influence of electron multiplication on the electroluminescence yield. The present study of Xe-Ne mixtures was motivated by an interest in using them as a filling for gas proportional scintillation counters in low-energy X-ray applications. In this energy range, the X rays will penetrate further into the detector due to the presence of Ne, and this will lead to an improvement in the collection of primary electrons originating near the detector window and may represent an advantage over the use of pure Xe.« less

State of the art of nanocrystals technology for delivery of poorly soluble drugs

NASA Astrophysics Data System (ADS)

Zhou, Yuqi; Du, Juan; Wang, Lulu; Wang, Yancai

2016-09-01

Formulation of nanocrystals is a distinctive approach which can effectively improve the delivery of poorly water-soluble drugs, thus enticing the development of the nanocrystals technology. The characteristics of nanocrystals resulted in an exceptional drug delivery conductance, including saturation solubility, dissolution velocity, adhesiveness, and affinity. Nanocrystals were treated as versatile pharmaceuticals that could be delivered through almost all routes of administration. In the current review, oral, pulmonary, and intravenous routes of administration were presented. Also, the targeting of drug nanocrystals, as well as issues of efficacy and safety, were also discussed. Several methods were applied for nanocrystals production including top-down production strategy (media milling, high-pressure homogenization), bottom-up production strategy (antisolvent precipitation, supercritical fluid process, and precipitation by removal of solvent), and the combination approaches. Moreover, this review also described the evaluation and characterization of the drug nanocrystals and summarized the current commercial pharmaceutical products utilizing nanocrystals technology.

Creating ligand-free silicon germanium alloy nanocrystal inks.

PubMed

Erogbogbo, Folarin; Liu, Tianhang; Ramadurai, Nithin; Tuccarione, Phillip; Lai, Larry; Swihart, Mark T; Prasad, Paras N

2011-10-25

Particle size is widely used to tune the electronic, optical, and catalytic properties of semiconductor nanocrystals. This contrasts with bulk semiconductors, where properties are tuned based on composition, either through doping or through band gap engineering of alloys. Ideally, one would like to control both size and composition of semiconductor nanocrystals. Here, we demonstrate production of silicon-germanium alloy nanoparticles by laser pyrolysis of silane and germane. We have used FTIR, TEM, XRD, EDX, SEM, and TOF-SIMS to conclusively determine their structure and composition. Moreover, we show that upon extended sonication in selected solvents, these bare nanocrystals can be stably dispersed without ligands, thereby providing the possibility of using them as an ink to make patterned films, free of organic surfactants, for device fabrication. The engineering of these SiGe alloy inks is an important step toward the low-cost fabrication of group IV nanocrystal optoelectronic, thermoelectric, and photovoltaic devices.

Level Anticrossing of Impurity States in Semiconductor Nanocrystals

PubMed Central

Baimuratov, Anvar S.; Rukhlenko, Ivan D.; Turkov, Vadim K.; Ponomareva, Irina O.; Leonov, Mikhail Yu.; Perova, Tatiana S.; Berwick, Kevin; Baranov, Alexander V.; Fedorov, Anatoly V.

2014-01-01

The size dependence of the quantized energies of elementary excitations is an essential feature of quantum nanostructures, underlying most of their applications in science and technology. Here we report on a fundamental property of impurity states in semiconductor nanocrystals that appears to have been overlooked—the anticrossing of energy levels exhibiting different size dependencies. We show that this property is inherent to the energy spectra of charge carriers whose spatial motion is simultaneously affected by the Coulomb potential of the impurity ion and the confining potential of the nanocrystal. The coupling of impurity states, which leads to the anticrossing, can be induced by interactions with elementary excitations residing inside the nanocrystal or an external electromagnetic field. We formulate physical conditions that allow a straightforward interpretation of level anticrossings in the nanocrystal energy spectrum and an accurate estimation of the states' coupling strength. PMID:25369911

Anomalous Suppression of Valley Splittings in Lead Salt Nanocrystals

NASA Astrophysics Data System (ADS)

Poddubny, Alexander; Nestoklon, Mikhail; Goupalov, Serguei

2012-02-01

Atomistic sp^3d^5s^* tight-binding theory of PbSe and PbS nanocrystals is developed. It is demonstrated, that the valley splittings of confined electrons and holes strongly and peculiarly depend on the geometry of a nanocrystal. When the nanocrystal lacks a microscopic center of inversion and has Td symmetry, the splittings are strongly suppressed as compared to the more symmetric nanocrystals with Oh symmetry, having an inversion center. This effect is quite unusual because typically a higher symmetry of a physical system implies a higher degeneracy of its energy levels, while in our case the suppression of the splittings occurs in NCs having lower symmetry. Nevertheless, we were able to explain this puzzling behavior using mathematical apparatus of the group theory.

Colloidal synthesis of biocompatible iron disulphide nanocrystals.

PubMed

Santos-Cruz, J; Nuñez-Anita, R E; Mayén-Hernández, S A; Martínez-Alvarez, O; Acosta-Torres, L S; de la Fuente-Hernández, J; Campos-González, E; Vega-González, M; Arenas-Arrocena, M C

2018-08-01

The aim of this research was to synthesis biocompatible iron disulphide nanocrystals at different reaction temperatures using the colloidal synthesis methodology. Synthesis was conducted at the 220-240 °C range of reaction temperatures at intervals of 5 °C in an inert argon atmosphere. The toxicity of iron disulphide nanocrystals was evaluated in vitro using mouse fibroblast cell line. Two complementary assays were conducted: the first to evaluate cell viability of the fibroblast via an MTT assay and the second to determine the preservation of fibroblast nuclei integrity through DAPI staining, which labels nuclear DNA in fluorescence microscopes. Through TEM and HRTEM, we observed a cubic morphology of pyrite iron disulphide nanocrystals ranging in sizes 25-50 nm (225 °C), 50-70 nm (230 °C) and >70 nm (235 °C). Through X-ray diffraction, we observed a mixture of pyrite and pyrrohotite in the samples synthesized at 225 °C and 240 °C, showing the best photocatalytic activity at 80% and 65%, respectively, for the degradation of methylene blue after 120 minutes. In all experimental groups, iron disulphide nanocrystals were biocompatible, i.e. no statistically significant differences were observed between experimental groups as shown in a one-way ANOVA and Tukey's test. Based on all of these results, we recommend non-cytotoxic semiconductor iron sulphide nanocrystals for biomedical applications.

Change of Nuclear Configurations in the Neutrinoless Double-β Decay of 130Te → 130Xe and 136Xe → 136Ba

DOE PAGES

Entwisle, J. P.; Kay, B. P.; Tamii, A.; ...

2016-06-13

The change in the configuration of valence protons between the initial and final states in the neutrinoless double-beta decay of Te-130 -> Xe-130 and of Xe-136 -> Ba-136 has been determined by measuring the cross sections of the (d,He-3) reaction with 101-MeV deuterons. Together with our recent determination of the relevant neutron configurations involved in the process, a quantitative comparison with the latest shell-model and interacting-boson-model calculations reveals significant discrepancies. These are the same calculations used to determine the nuclear matrix elements governing the rate of neutrinoless double-beta decay in these systems.

Gadolinium embedded iron oxide nanoclusters as T1-T2 dual-modal MRI-visible vectors for safe and efficient siRNA delivery

NASA Astrophysics Data System (ADS)

Wang, Xiaoyong; Zhou, Zijian; Wang, Zhiyong; Xue, Yunxin; Zeng, Yun; Gao, Jinhao; Zhu, Lei; Zhang, Xianzhong; Liu, Gang; Chen, Xiaoyuan

2013-08-01

This report illustrates a new strategy of designing a T1-T2 dual-modal magnetic resonance imaging (MRI)-visible vector for siRNA delivery and MRI. Hydrophobic gadolinium embedded iron oxide (GdIO) nanocrystals are self-assembled into nanoclusters in the water phase with the help of stearic acid modified low molecular weight polyethylenimine (stPEI). The resulting water-dispersible GdIO-stPEI nanoclusters possess good stability, monodispersity with narrow size distribution and competitive T1-T2 dual-modal MR imaging properties. The nanocomposite system is capable of binding and delivering siRNA for knockdown of a gene of interest while maintaining its magnetic properties and biocompatibility. This new gadolinium embedded iron oxide nanocluster provides an important platform for safe and efficient gene delivery with non-invasive T1-T2 dual-modal MRI monitoring capability.This report illustrates a new strategy of designing a T1-T2 dual-modal magnetic resonance imaging (MRI)-visible vector for siRNA delivery and MRI. Hydrophobic gadolinium embedded iron oxide (GdIO) nanocrystals are self-assembled into nanoclusters in the water phase with the help of stearic acid modified low molecular weight polyethylenimine (stPEI). The resulting water-dispersible GdIO-stPEI nanoclusters possess good stability, monodispersity with narrow size distribution and competitive T1-T2 dual-modal MR imaging properties. The nanocomposite system is capable of binding and delivering siRNA for knockdown of a gene of interest while maintaining its magnetic properties and biocompatibility. This new gadolinium embedded iron oxide nanocluster provides an important platform for safe and efficient gene delivery with non-invasive T1-T2 dual-modal MRI monitoring capability. Electronic supplementary information (ESI) available. See DOI: 10.1039/c3nr02797j

Metal Nanoparticles Embedded in Cellulose Nanocrystal Based Films: Material Properties and Post-use Analysis.

PubMed

Lizundia, Erlantz; Goikuria, Uribarri; Vilas, José Luis; Cristofaro, Francesco; Bruni, Giovanna; Fortunati, Elena; Armentano, Ilaria; Visai, Livia; Torre, Luigi

2018-04-25

The dispersion of nanoparticles having different size-, shape-, and composition-dependent properties is an exciting approach to design and synthesize multifunctional materials and devices. This work shows a detailed investigation of the preparation and properties of free-standing nanocomposite films based on cellulose nanocrystals (CNC) loaded with three different types of metal nanoparticles. CNC-based nanocomposites having zinc oxide (ZnO), titanium dioxide (TiO 2 ), and silver oxide (Ag 2 O) have been obtained through evaporation-induced self-assembly (EISA) in acqueous solution. Morphological and optical characteristics, chemical properties, wettability, and antimicrobial assays of the produced films were conducted. Furthermore, disintegrability in composting condition of CNC based nanocomposites was here investigated for the first time. The morphological observations revealed the formation of a chiral nematic structure with uniformly distributed nanoparticles. The bionanocomposite films based on the metal nanoparticles had effective antimicrobial activity, killing both Escherichia coli RB ( E. coli RB) and Staphylococcus aureus 8325-4 ( S. aureus 8325-4). The simplicity method of film preparation, the large quantity of cellulose in the world, and the free-standing nature of the nanocomposite films offer highly advantageous characteristics that can for the new development of multifunctional materials.

Shape-controlled synthesis of metal nanocrystals: simple chemistry meets complex physics?

PubMed

Xia, Younan; Xiong, Yujie; Lim, Byungkwon; Skrabalak, Sara E

2009-01-01

Nanocrystals are fundamental to modern science and technology. Mastery over the shape of a nanocrystal enables control of its properties and enhancement of its usefulness for a given application. Our aim is to present a comprehensive review of current research activities that center on the shape-controlled synthesis of metal nanocrystals. We begin with a brief introduction to nucleation and growth within the context of metal nanocrystal synthesis, followed by a discussion of the possible shapes that a metal nanocrystal might take under different conditions. We then focus on a variety of experimental parameters that have been explored to manipulate the nucleation and growth of metal nanocrystals in solution-phase syntheses in an effort to generate specific shapes. We then elaborate on these approaches by selecting examples in which there is already reasonable understanding for the observed shape control or at least the protocols have proven to be reproducible and controllable. Finally, we highlight a number of applications that have been enabled and/or enhanced by the shape-controlled synthesis of metal nanocrystals. We conclude this article with personal perspectives on the directions toward which future research in this field might take.

Nanocrystal sensitized photovoltaics and photodetectors with performance enhanced using ligand engineering

NASA Astrophysics Data System (ADS)

Schut, David M.; Williams, George M., Jr.; Arteaga, Stefan; Allen, Thomas L.; Novet, Thomas

2011-06-01

Nanocrystal quantum dot photovoltaics and photodetectors with performance optimized by engineering the nanocrystals size and the optoelectronic properties of the nanocrystal's chemical coating are reported. Due to the large surface-to-volume ratio inherent to nanocrystals, the surface effects of ligands used to chemically coat and passivate nanocrystals play a significant role in device performance. However, the optoelectronic properties of ligands are difficult to ascertain, as the band structure of the ligand-capped nanoparticle system is complex and difficult to model. Using density-of-states measurements, we demonstrate that modeling of electropositive and electronegative substituents and use of the Hammett equation, are useful tools in optimizing nanocrystal detector performance. A new particle, the Janus-II nanoparticles, developed using 'charge-donating' and 'charge-withdrawing' ligands distributed over opposite surfaces of the nanocrystal, is described. The polarizing ligands of the Janus-II nanoparticle form a degeneracy-splitting dipole, which reduces the overlap integral between excitonic states, and thus reduces the probability of carrier recombination, allowing carrier extraction to take place more efficiently. This is shown to allow increased photodetection efficiencies and to allow the capture of multiple exciton events in working photodetectors.

Formic acid-assisted synthesis of palladium nanocrystals and their electrocatalytic properties.

PubMed

Wang, Qinchao; Wang, Yiqian; Guo, Peizhi; Li, Qun; Ding, Ruixue; Wang, Baoyan; Li, Hongliang; Liu, Jingquan; Zhao, X S

2014-01-14

Palladium (Pd) nanocrystals have been synthesized by using formic acid as the reducing agent at room temperature. When the concentration of formic acid was increased continuously, the size of Pd nanocrystals first decreased to a minimum and then increased slightly again. The products have been investigated by a series of techniques, including X-ray diffraction, high-resolution transmission electron microscopy (HRTEM), UV-vis absorption, and electrochemical measurements. The formation of Pd nanocrystals is proposed to be closely related to the dynamical imbalance of the growth and dissolution rate of Pd nanocrystals associated with the adsorption of formate ions onto the surface of the intermediates. It is found that small Pd nanocrystals showed blue-shifted adsorption peaks compared with large ones. Pd nanocrystals with the smallest size display the highest electrocatalytic activity for the electrooxidation of formic acid and ethanol on the basis of cyclic voltammetry and chronoamperometric data. It is suggested that both the electrochemical active surface area and the small size effect are the key roles in determining the electrocatalytic performances of Pd nanocrystals. A "dissolution-deposition-aggregation" process is proposed to explain the variation of the electrocatalytic activity during the electrocatalysis according to the HRTEM characterization.

Nuclear magnetic relaxation studies of semiconductor nanocrystals and solids

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sachleben, Joseph Robert

1993-09-01

Semiconductor nanocrystals, small biomolecules, and 13C enriched solids were studied through the relaxation in NMR spectra. Surface structure of semiconductor nanocrystals (CdS) was deduced from high resolution 1H and 13C liquid state spectra of thiophenol ligands on the nanocrystal surfaces. The surface coverage by thiophenol was found to be low, being 5.6 and 26% for nanocrystal radii of 11.8 and 19.2 Å. Internal motion is estimated to be slow with a correlation time > 10 -8 s -1. The surface thiophenol ligands react to form a dithiophenol when the nanocrystals were subjected to O 2 and ultraviolet. A method formore » measuring 14N- 1H J-couplings is demonstrated on pyridine and the peptide oxytocin; selective 2D T 1 and T 2 experiments are presented for measuring relaxation times in crowded spectra with overlapping peaks in 1D, but relaxation effects interfere. Possibility of carbon-carbon cross relaxation in 13C enriched solids is demonstrated by experiments on zinc acetate and L-alanine.« less

Nuclear magnetic relaxation studies of semiconductor nanocrystals and solids

NASA Astrophysics Data System (ADS)

Sachleben, J. R.

1993-09-01

Semiconductor nanocrystals, small biomolecules, and C-13 enriched solids were studied through the relaxation in NMR spectra. Surface structure of semiconductor nanocrystals (CdS) was deduced from high resolution H-1 and C-13 liquid state spectra of thiophenol ligands on the nanocrystal surfaces. The surface coverage by thiophenol was found to be low, being 5.6 and 26% for nanocrystal radii of 11.8 and 19.2 angstrom. Internal motion is estimated to be slow with a correlation time greater than 10(exp -8) s(exp -1). The surface thiophenol ligands react to form a dithiophenol when the nanocrystals were subjected to O2 and ultraviolet. A method for measuring (N-14)-(H-1) J-couplings is demonstrated on pyridine and the peptide oxytocin; selective 2D T(sub 1) and T(sub 2) experiments are presented for measuring relaxation times in crowded spectra with overlapping peaks in 1D, but relaxation effects interfere. Possibility of carbon-carbon cross relaxation in C-13 enriched solids is demonstrated by experiments on zinc acetate and L-alanine.

Potentiometric Titrations for Measuring the Capacitance of Colloidal Photodoped ZnO Nanocrystals.

PubMed

Brozek, Carl K; Hartstein, Kimberly H; Gamelin, Daniel R

2016-08-24

Colloidal semiconductor nanocrystals offer a unique opportunity to bridge molecular and bulk semiconductor redox phenomena. Here, potentiometric titration is demonstrated as a method for quantifying the Fermi levels and charging potentials of free-standing colloidal n-type ZnO nanocrystals possessing between 0 and 20 conduction-band electrons per nanocrystal, corresponding to carrier densities between 0 and 1.2 × 10(20) cm(-3). Potentiometric titration of colloidal semiconductor nanocrystals has not been described previously, and little precedent exists for analogous potentiometric titration of any soluble reductants involving so many electrons. Linear changes in Fermi level vs charge-carrier density are observed for each ensemble of nanocrystals, with slopes that depend on the nanocrystal size. Analysis indicates that the ensemble nanocrystal capacitance is governed by classical surface electrical double layers, showing no evidence of quantum contributions. Systematic shifts in the Fermi level are also observed with specific changes in the identity of the charge-compensating countercation. As a simple and contactless alternative to more common thin-film-based voltammetric techniques, potentiometric titration offers a powerful new approach for quantifying the redox properties of colloidal semiconductor nanocrystals.

Nanocrystal for ocular drug delivery: hope or hype.

PubMed

Sharma, Om Prakash; Patel, Viral; Mehta, Tejal

2016-08-01

The complexity of the structure and nature of the eye emanates a challenge for drug delivery to formulation scientists. Lower bioavailability concern of conventional ocular formulation provokes the interest of researchers in the development of novel drug delivery system. Nanotechnology-based formulations have been extensively investigated and found propitious in improving bioavailability of drugs by overcoming ocular barriers prevailing in the eye. The advent of nanocrystals helped in combating the problem of poorly soluble drugs specifically for oral and parenteral drug delivery and led to development of various marketed products. Nanocrystal-based formulations explored for ocular drug delivery have been found successful in achieving increase in retention time, bioavailability, and permeability of drugs across the corneal and conjunctival epithelium. In this review, we have highlighted the ocular physiology and barriers in drug delivery. A comparative analysis of various nanotechnology-based ocular formulations is done with their pros and cons. Consideration is also given to various methods of preparation of nanocrystals with their patented technology. This article highlights the success achieved in conquering various challenges of ocular delivery by the use of nanocrystals while emphasizing on its advantages and application for ocular formulation. The perspectives of nanocrystals as an emerging flipside to explore the frontiers of ocular drug delivery are discussed.

I-Pu-Xe dating and the relative ages of the earth and moon

NASA Technical Reports Server (NTRS)

Swindle, T. D.; Caffee, M. W.; Hohenberg, C. M.; Taylor, S. R.

1986-01-01

The ages of the earth and moon as determined by various chronometric systems are discussed with primary emphasis placed on the development of an I-Pu-Xe chronometer. Data on excess fission xenon are reviewed with attention given to the strengths and weaknesses of the assumptions required for lunar I-Pu-Xe chronometry. Using I-Pu-Xe dating, it is estimated that the retention of excess fission xenon in lunar samples began no more than 63 + or - 42 m.y. after the time of primitive meteorite formation.

I-Xe dating of aqueous alteration in the CI chondrite Orgueil: I. Magnetite and ferromagnetic separates

NASA Astrophysics Data System (ADS)

Pravdivtseva, O.; Krot, A. N.; Hohenberg, C. M.

2018-04-01

The I-Xe system was studied in a ferromagnetic sample separated from the Orgueil CI carbonaceous chondrite with a hand-held magnet and in two magnetite samples, one chemically separated before and the other one after neutron irradiation. This work was done in order to investigate the effects of chemical separation by LiCl and NaOH on the I-Xe system in magnetite. Our test demonstrated that the chemical separation of magnetite before irradiation using either LiCl or NaOH, or both, does not contaminate the sample with iodine and thus cannot lead to erroneous I-Xe ages due to introduction of uncorrelated 128∗Xe. The I-Xe ages of two Orgueil magnetite samples are mutually consistent within experimental uncertainties and, when normalized to an absolute time scale with the reevaluated Shallowater aubrite standard, place the onset of aqueous alteration on the CI parent body at 4564.3 ± 0.3 Ma, 2.9 ± 0.3 Ma after formation of the CV Ca-AI-rich inclusions (CAIs). The I-Xe age of the ferromagnetic Orgueil separate is 3.4 Ma younger, corresponding to a closure of the I-Xe system at 4560.9 ± 0.2 Ma. These and previously published I-Xe data for Orgueil (Hohenberg et al., 2000) indicate that aqueous alteration on the CI parent body lasted for at least 5 Ma. Although the two magnetite samples gave indistinguishable I-Xe ages, their temperature release profiles differed. One of the two Orgueil magnetites released less radiogenic Xe than the other, 80% of it corresponding to the low-temperature peak of the release profile, compared to only 6% in case of the second Orgueil magnetite sample. This could be due to the difference in iodine trapping efficiencies for magnetite grains of different morphologies. Alternatively, the magnetite grains with the lower radiogenic Xe concentrations may have formed at a later stage of alteration when iodine in an aqueous solution was depleted.

ETV Report:Siemens Model H-4XE-HO Open Channel UV System

EPA Science Inventory

Verification testing of the Siemens Barrier Sunligt H-4XE-HO UV System was completed at the UV Validation and Research Center of New York (UV Center), located in Johnstown, NY. The H-4XE System utilizes 16 high-output, low-pressure lamps oriented horizontally and parallel to the...

Colloidal infrared reflective and transparent conductive aluminum-doped zinc oxide nanocrystals

DOEpatents

Buonsanti, Raffaella; Milliron, Delia J

2015-02-24

The present invention provides a method of preparing aluminum-doped zinc oxide (AZO) nanocrystals. In an exemplary embodiment, the method includes (1) injecting a precursor mixture of a zinc precursor, an aluminum precursor, an amine, and a fatty acid in a solution of a vicinal diol in a non-coordinating solvent, thereby resulting in a reaction mixture, (2) precipitating the nanocrystals from the reaction mixture, thereby resulting in a final precipitate, and (3) dissolving the final precipitate in an apolar solvent. The present invention also provides a dispersion. In an exemplary embodiment, the dispersion includes (1) nanocrystals that are well separated from each other, where the nanocrystals are coated with surfactants and (2) an apolar solvent where the nanocrystals are suspended in the apolar solvent. The present invention also provides a film. In an exemplary embodiment, the film includes (1) a substrate and (2) nanocrystals that are evenly distributed on the substrate.

Nanocrystal Additives for Advanced Lubricants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cooper, Gregory; Lohuis, James; Demas, Nicholaos

The innovations in engine and drivetrain lubricants are mainly driven by ever more stringent regulations, which demand better fuel economy, lower carbon emission, and less pollution. Many technologies are being developed for the next generations of vehicles to achieve these goals. Even if these technologies can be adopted, there still is a significant need for a “drop-in” lubricant solution for the existing ground vehicle fleet to reap immediate fuel savings at the same time reduce the pollution. Dramatic improvements were observed when Pixelligent’s proprietary, mono-dispersed, and highly scalable metal oxide nanocrystals were added to the base oils. The dispersions inmore » base and formulated oils are clear and without any change of appearance and viscosity. However, the benefits provided by the nanocrystals were limited to the base oils due to the interference of exiting additives in the fully formulated oils. Developing a prototype formulation including the nanocrystals that can demonstrate the same improvements observed in the base oils is a critical step toward the commercialization of these advanced nano-additives. A ‘bottom-up’ approach was adopted to develop a prototype lubricant formulation to avoid the complicated interactions with the multitude of additives, only minimal numbers of most essential additives are added, step by step, into the formulation, to ensure that they are compatible with the nanocrystals and do not compromise their tribological performance. Tribological performance are characterized to come up with the best formulations that can demonstrate the commercial potential of the nano-additives.« less

133Xe contamination found in internal bacteria filter of xenon ventilation system.

PubMed

Hackett, Michael T; Collins, Judith A; Wierzbinski, Rebecca S

2003-09-01

We report on (133)Xe contamination found in the reusable internal bacteria filter of our xenon ventilation system. Internal bacteria filters (n = 6) were evaluated after approximately 1 mo of normal use. The ventilation system was evacuated twice to eliminate (133)Xe in the system before removal of the filter. Upon removal, the filter was monitored using a survey meter with an energy-compensated probe and was imaged on a scintillation camera. The filter was monitored and imaged over several days and was stored in a fume hood. Estimated (133)Xe activity in each filter immediately after removal ranged from 132 to 2,035 kBq (3.6-55.0 micro Ci), based on imaging. Initial surface radiation levels ranged from 0.4 to 4.5 micro Sv/h (0.04-0.45 mrem/h). The (133)Xe activity did not readily leave the filter over time (i.e., time to reach half the counts of the initial decay-corrected image ranged from <6 to >72 h). The majority of the image counts (approximately 70%) were seen in 2 distinctive areas in the filter. They corresponded to sites where the manufacturer used polyurethane adhesive to attach the fiberglass filter medium to the filter housing. (133)Xe contamination within the reusable internal bacteria filter of our ventilation system was easily detected by a survey meter and imaging. Although initial activities and surface radiation levels were low, radiation safety practices would dictate that a (133)Xe-contaminated bacteria filter be stored preferably in a fume hood until it cannot be distinguished from background before autoclaving or disposal.

Optical properties of Si and Ge nanocrystals: Parameter-free calculations

NASA Astrophysics Data System (ADS)

Ramos, L. E.; Weissker, H.-Ch.; Furthmüller, J.; Bechstedt, F.

2005-12-01

The cover picture of the current issue refers to the Edi-tor's Choice article of Ramos et al. [1]. The paper gives an overview of the electronic and optical properties of silicon and germanium nanocrystals determined by state-of-the-art ab initio methods. Nanocrystals have promising applications in opto-electronic devices, since they can be used to confine electrons and holes and facilitate radiative recombination. Since meas-urements for single nanoparticles are difficult to make, ab initio theoretical investigations become important to understand the mechanisms of luminescence.The cover picture shows nanocrystals of four sizes with tetrahedral coordination whose dangling bonds at the surface are passivated with hydrogen. As often observed in experiments, the nanocrystals are not perfectly spherical, but contain facets. Apart from the size of the nanocrystals, which determines the quantum confinement, the way their dangling bonds are passivated is relevant for their electronic and optical properties. For instance, the passivation with hydroxyls reduces the quantum confine-ment. On the other hand, the oxidation of the silicon nanocrys-tals increases the quantum confinement and reduces the effect of single surface terminations on the gap. Due to the oscillator strengths of the lowest-energy optical transitions, Ge nanocrys-tals are in principle more suitable for opto-electronic applica-tions than Si nanocrystals.The first author, Luis E. Ramos, is a postdoc at the Institute of Solid-State Physics and Optics (IFTO), Friedrich-Schiller University Jena, Germany. He investigates electronic and optical properties of semiconductor nanocrystallites and is a member of the European Network of Excellence NANO-QUANTA and of the European Theoretical Spectroscopy Facility (ETSF).

Optical Properties of Nanocrystal Interfaces in Compressed MgO Nanopowders

PubMed Central

2011-01-01

The optical properties and charge trapping phenomena observed on oxide nanocrystal ensembles can be strongly influenced by the presence of nanocrystal interfaces. MgO powders represent a convenient system to study these effects due to the well-defined shape and controllable size distributions of MgO nanocrystals. The spectroscopic properties of nanocrystal interfaces are investigated by monitoring the dependence of absorption characteristics on the concentration of the interfaces in the nanopowders. The presence of interfaces is found to affect the absorption spectra of nanopowders more significantly than changing the size of the constituent nanocrystals and, thus, leading to the variation of the relative abundance of light-absorbing surface structures. We find a strong absorption band in the 4.0−5.5 eV energy range, which was previously attributed to surface features of individual nanocrystals, such as corners and edges. These findings are supported by complementary first-principles calculations. The possibility to directly address such interfaces by tuning the energy of excitation may provide new means for functionalization and chemical activation of nanostructures and can help improve performance and reliability for many nanopowder applications. PMID:21443262

Increased electronic coupling in silicon nanocrystal networks doped with F4-TCNQ.

PubMed

Carvalho, Alexandra; Oberg, Sven; Rayson, Mark J; Briddon, Patrick R

2013-02-01

The modification of the electronic structure of silicon nanocrystals using an organic dopant, 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4-TCNQ), is investigated using first-principles calculations. It is shown that physisorbed F4-TCNQ molecules have the effect of oxidizing the nanocrystal, attracting the charge density towards the F4-TCNQ-nanocrystal interface, and decreasing the excitation energy of the system. In periodic F4-TCNQ/nanocrystal superlattices, F4-TCNQ is suggested to enhance exciton separation, and in the presence of free holes, to serve as a bridge for electron/hole transfer between adjacent nanocrystals.

Synthesis of icosahedral gold nanocrystals: a thermal process strategy.

PubMed

Zhou, Min; Chen, Shenhao; Zhao, Shiyong

2006-03-16

We demonstrate a one-step thermal process route to the synthesis of icosahedral gold nanocrystals. By regulating the concentrations of poly(vinyl pyrrolidone) (PVP) and HAuCl4 or changing the temperature, we can readily access the shapes of icosahedral nanocrystals with good uniformity. These gold nanostructures, with unique geometrical shapes, might find use in areas that include photonics, optoelectronics, and optical sensing. We also observed that these gold nanocrystals have a strong tendency to be immobilized spontaneously on the glass substrate.

Lifetime of excitons localized in Si nanocrystals in amorphous silicon

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gusev, O. B.; Belolipetskiy, A. V., E-mail: alexey.belolipetskiy@mail.ioffe.ru; Yassievich, I. N.

2016-05-15

The introduction of nanocrystals plays an important role in improving the stability of the amorphous silicon films and increasing the carrier mobility. Here we report results of the study on the photoluminescence and its dynamics in the films of amorphous hydrogenated silicon containing less than 10% of silicon nanocrystals. The comparing of the obtained experimental results with the calculated probability of the resonant tunneling of the excitons localized in silicon nanocrystals is presented. Thus, it has been estimated that the short lifetime of excitons localized in Si nanocrystal is controlled by the resonant tunneling to the nearest tail state ofmore » the amorphous matrix.« less

Recent Progress in Photocatalysis Mediated by Colloidal II-VI Nanocrystals

PubMed Central

Wilker, Molly B; Schnitzenbaumer, Kyle J; Dukovic, Gordana

2012-01-01

The use of photoexcited electrons and holes in semiconductor nanocrystals as reduction and oxidation reagents is an intriguing way of harvesting photon energy to drive chemical reactions. This review focuses on recent research efforts to understand and control the photocatalytic processes mediated by colloidal II-VI nanocrystalline materials, such as cadmium and zinc chalcogenides. First, we highlight how nanocrystal properties govern the rates and efficiencies of charge-transfer processes relevant to photocatalysis. We then describe the use of nanocrystal catalyst heterostructures for fuel-forming reactions, most commonly H2 generation. Finally, we review the use of nanocrystal photocatalysis as a synthetic tool for metal–semiconductor nano-heterostructures. PMID:24115781

Interatomic potentials for HeAr, HeKr, and HeXe from multiproperty fits

DOE Office of Scientific and Technical Information (OSTI.GOV)

Danielson, L.J.; Keil, M.

1988-01-15

Crossed molecular beam measurements of differential cross sections (DCS) are reported for elastic scattering of He by Ar, Kr, and Xe at high resolution. Interatomic potentials are determined by simultaneously fitting the DCS's, as well as mixture viscosity and interaction second virial data. Bias due to systematic and potential model errors are examined and are used to estimate the accuracy of the potential energy curves obtained. Attractive well depths are 2.59, 2.67, and 2.64 meV +- 3% for HeAr, HeKr, and HeXe, respectively, agreeing with the best available HeAr potential and a previously proposed HeKr potential, but significantly deeper thanmore » previously reported potentials for HeXe. The HeXe attractive well is also considerably broader than previously reported. Attractive minimum positions are 3.48, 3.70, and 4.00 A ( +- 0.03 A) for HeAr, HeKr, and HeXe, respectively. Including the accurate diffusion data of Dunlop and co-workers (Physica A 95, 561 (1979)) and the absolute integral cross sections of Pirani and Vecchiocattivi (J. Chem. Phys. 66, 372 (1977) and revisions thereto) verify the error bounds for all three potentials.« less

Experimental ion mobility measurements in Xe-C2H6

NASA Astrophysics Data System (ADS)

Perdigoto, J. M. C.; Cortez, A. F. V.; Veenhof, R.; Neves, P. N. B.; Santos, F. P.; Borges, F. I. G. M.; Conde, C. A. N.

2017-10-01

In this paper we present the results of the ion mobility measurements made in gaseous mixtures of xenon (Xe) with ethane (C2H6) for pressures ranging from 6 to 10 Torr (8-10.6 mbar) and for low reduced electric fields in the 10 Td to 25 Td range (2.4-6.1 kVṡcm-1ṡ bar-1), at room temperature. The time of arrival spectra revealed two peaks throughout the entire range studied which were attributed to ion species with 3-carbons (C3H5+, C3H6+ C3H8+ and C3H9+) and with 4-carbons (C4H7+, C4H9+ and C4H10+). Besides these, and for Xe concentrations above 70%, a bump starts to appear at the right side of the main peak for reduced electric fields higher than 20 Td, which was attributed to the resonant charge transfer of C2H6+ to C2H6 that affects the mobility of its ion products (C3H8+ and C3H9+). The time of arrival spectra for Xe concentrations of 20%, 50%, 70% and 90% are presented, together with the reduced mobilities as a function of the Xe concentration calculated from the peaks observed for the low reduced electric fields and pressures studied.

Half-collision analysis of far-wing diffuse structure in Cs-Xe

NASA Technical Reports Server (NTRS)

Exton, R. J.; Hillard, M. E.; Lempert, W. R.

1987-01-01

Laser excitation in the far red wing of the second principal series doublet of Cs mixed with Xe revealed a diffuse structure associated with the 2P(3/2) component. The structure is thought to originate from a reflection type of spectrum between the weakly bound E 2Sigma(1/2) excited state and the X 2Sigma(1/2) repulsive ground state of CsXe.

Lung Morphometry with Hyperpolarized 129Xe: Theoretical Background

PubMed Central

Sukstanskii, A.L.; Yablonskiy, D.A.

2011-01-01

The 3He lung morphometry technique, based on MRI measurements of hyperpolarized 3He gas diffusion in lung airspaces, provides unique information on the lung microstructure at the alveolar level. In vivo 3D tomographic images of standard morphological parameters (airspace chord length, lung parenchyma surface-to-volume ratio, number of alveoli per unit volume) can be generated from a rather short (several seconds) MRI scan. The technique is based on a theory of gas diffusion in lung acinar airways and experimental measurements of diffusion attenuated MRI signal. The present work aims at developing the theoretical background of a similar technique based on hyperpolarized 129Xe gas. As the diffusion coefficient and gyromagnetic ratio of 129Xe gas are substantially different from those of 3He gas, the specific details of the theory and experimental measurements with 129Xe should be amended. We establish phenomenological relationships between acinar airway geometrical parameters and the diffusion attenuated MR signal for human and small animal lungs, both normal lungs and lungs with mild emphysema. Optimal diffusion times are shown to be about 5 ms for human and 1.3 ms for small animals. The expected uncertainties in measuring main morphometrical parameters of the lungs are estimated in the framework of Bayesian probability theory. PMID:21713985

Ligand Exchange Governs the Crystal Structures in Binary Nanocrystal Superlattices.

PubMed

Wei, Jingjing; Schaeffer, Nicolas; Pileni, Marie-Paule

2015-11-25

The surface chemistry in colloidal nanocrystals on the final crystalline structure of binary superlattices produced by self-assembly of two sets of nanocrystals is hereby demonstrated. By mixing nanocrystals having two different sizes and the same coating agent, oleylamine (OAM), the binary nanocrystal superlattices that are produced, such as NaCl, AlB2, NaZn13, and MgZn2, are well in agreement with the crystalline structures predicted by the hard-sphere model, their formation being purely driven by entropic forces. By opposition, when large and small nanocrystals are coated with two different ligands [OAM and dodecanethiol (DDT), respectively] while keeping all other experimental conditions unchanged, the final binary structures markedly change and various structures with lower packing densities, such as Cu3Au, CaB6, and quasicrystals, are observed. This effect of the nanocrystals' coating agents could also be extended to other binary systems, such as Ag-Au and CoFe2O4-Ag supracrystalline binary lattices. In order to understand this effect, a mechanism based on ligand exchange process is proposed. Ligand exchange mechanism is believed to affect the thermodynamics in the formation of binary systems composed of two sets of nanocrystals with different sizes and bearing two different coating agents. Hence, the formation of binary superlattices with lower packing densities may be favored kinetically because the required energetic penalty is smaller than that of a denser structure.

Atomic force microscopy nanomanipulation of silicon nanocrystals for nanodevice fabrication

NASA Astrophysics Data System (ADS)

Decossas, Sébastien; Mazen, Frédéric; Baron, Thierry; Brémond, Georges; Souifi, Abdelkader

2003-12-01

An atomic force microscopy (AFM) tip has been used to manipulate silicon nanocrystals deposited by low-pressure chemical vapour deposition on thermally oxidized p-type Si wafer. Three nanomanipulation methods are presented. The first one catches a nanocrystal with the AFM tip and deposits it elsewhere: the tip is used as an electrostatic 'nano-crane'. The second one simultaneously manipulates a set of nanocrystals in order to draw well-defined unidimensional lines: the tip is used as a 'nano-broom'. The third one manipulates individual nanocrystals with a precision of about 10 nm using both oscillating and contact AFM modes. Switching from strong interaction forces (chemical) to weak ones (van der Waals, electrostatic or capillarity) is the basis of these manipulation methods. We have applied the second method to connect two electrodes drawn by e-beam and lift-off with a 70 nm long silicon nanocrystal chain. Current versus voltage characterization of the nanofabricated device shows that the increase in nanocrystal density gives rise to conduction between the connected electrodes. Resonant tunnelling effects resulting from Si nanocrystal (nc-Si) multiple tunnel junctions have been observed at 300 K. We also show that offset charges directly influence the position of the resonant tunnelling peaks. Finally, the possibility of manipulating nc-Si with a diameter of around 5 nm is shown to be a promising way to fabricate single electron devices operating at room temperature and fully compatible with silicon technology.

Band gap and composition engineering on a nanocrystal (BCEN) in solution.

PubMed

Peng, Xiaogang

2010-11-16

Colloidal nanocrystals with "artificial" composition and electron band structure promise to expand the fields of nanomaterials and inorganic chemistry. Despite their promise as functional materials, the fundamental science associated with the synthesis, characterization, and properties of colloidal nanocrystals is still in its infancy and deserves systematic study. Furthermore, such studies are important for our basic understanding of crystallization, surface science, and solid state chemistry. "Band gap and composition engineering on a nanocrystal" (BCEN) refers to the synthesis of a colloidal nanocrystal with composition and/or electron energy band structure that are not found in natural bulk crystals. The BCEN nanostructure shown in the Figure includes a magnetic domain for the separation and recycling of the complex nanostructure, a photoactivated catalytic center, and an additional chemical catalytic center. A thin but porous film (such as a silicate) might be coated onto the nanocrystal, both to provide chemical stability and to isolate the reaction processes from the bulk solution. This example is a catalytic complex analogous to an enzyme that facilitates two sequential reactions in a microenvironment different from bulk solution. The synthesis of colloidal nanocrystals has advanced by a quantum leap in the past two decades. The field now seems ready to extend colloidal nanocrystal synthesis into the BCEN regime. Although BCEN is a very new branch of synthetic chemistry, this Account describes advances in related synthetic and characterization techniques that can serve as a useful starting point for this new area of investigation. To put these ideas into context, this Account compares this new field with organic synthesis, the most developed branch in synthetic chemistry. The structural and functional diversity of organic compounds results from extending design and synthesis beyond the construction of natural organic compounds. If this idea also holds true

Systems and methods of detecting force and stress using tetrapod nanocrystal

DOEpatents

Choi, Charina L.; Koski, Kristie J.; Sivasankar, Sanjeevi; Alivisatos, A. Paul

2013-08-20

Systems and methods of detecting force on the nanoscale including methods for detecting force using a tetrapod nanocrystal by exposing the tetrapod nanocrystal to light, which produces a luminescent response by the tetrapod nanocrystal. The method continues with detecting a difference in the luminescent response by the tetrapod nanocrystal relative to a base luminescent response that indicates a force between a first and second medium or stresses or strains experienced within a material. Such systems and methods find use with biological systems to measure forces in biological events or interactions.

Shape-Controlled Synthesis of Metal Nanocrystals: Simple Chemistry Meets Complex Physics?

PubMed Central

Xia, Younan; Xiong, Yujie; Lim, Byungkwon; Skrabalak, Sara E.

2009-01-01

Nanocrystals are fundamental to modern science and technology. Mastery over the shape of a nanocrystal enables control of its properties and enhancement of its usefulness for a given application. The aim of this article is to present a comprehensive review of current research activities that center on the shape-controlled synthesis of metal nanocrystals. We begin with a brief introduction to nucleation and growth within the context of metal nanocrystal synthesis, followed by a discussion of the possible shapes that a metal nanocrystal might take under different conditions. We then focus on a variety of experimental parameters that have been explored to manipulate the nucleation and growth of metal nanocrystals in solution-phase syntheses in an effort to generate specific shapes. We then elaborate on these approaches by selecting examples in which there is already reasonable understanding for the observed shape control or at least the protocols have proven to be reproducible and controllable. Toward the end of this article, we highlight a number of applications that have been enabled and/or enhanced by the shape-controlled synthesis of metal nanocrystals. We conclude this article with personal perspectives on the directions toward which future research in this field might take. PMID:19053095

Searches for double beta decay of Xe 134 with EXO-200

DOE PAGES

Albert, J. B.; Anton, G.; Badhrees, I.; ...

2017-11-03

Searches for double beta decay of 134Xe were performed with EXO-200, a single-phase liquid xenon detector designed to search for neutrinoless double beta decay of 136Xe. Using an exposure of 29.6 kg ∙ yr , the lower limits of Tmore » $$2νββ\\atop{1/2}$$ > 8.7 × 10 20 yr and T$$0νββ\\atop{1/2}$$ > 1.1 × 10 23 yr at 90% confidence level were derived, with corresponding half-life sensitivities of 1.2 × 10 21 yr and 1.9 × 10 23 yr . In conclusion, these limits exceed those in the literature for 134 Xe , improving by factors of nearly 10 5 and 2 for the two antineutrino and neutrinoless modes, respectively.« less

Metal Sulfide Nanocrystals inside Ferritin with Photovoltaic Applications

NASA Astrophysics Data System (ADS)

Hansen, Kameron; Peterson, J. Ryan; Olsen, Cameron; Hogg, Heather; Colton, John; Watt, Richard; Colton Team

Ferritin is a spherical protein shell used universally by organisms to store iron. Due to a number of ferritin's properties (a conductive shell, ability to be arranged in ordered arrays, and high stability), recent theoretical work has proposed that non-native semiconductor nanocrystals inside ferritin can be used for high-efficiency solar energy conversion. We present research on the synthesis of a variety of these nanocrystals (PbS, CuS, Mo2S, ZnS, and PbSe) inside ferritin's hollow interior and band gap energies of the resulting ferritin-nanocrystal constructs. We also report preliminary solar cell results for dye sensitized solar cells with PbS-ferritin as the dye.

Surface treatment of nanocrystal quantum dots after film deposition

DOEpatents

Sykora, Milan; Koposov, Alexey; Fuke, Nobuhiro

2015-02-03

Provided are methods of surface treatment of nanocrystal quantum dots after film deposition so as to exchange the native ligands of the quantum dots for exchange ligands that result in improvement in charge extraction from the nanocrystals.

Hierarchial Junction Solar Cells Based on Hyper-Branched Semiconductor Nanocrystals

DTIC Science & Technology

2009-06-30

Hyper-Branched Semiconductor Nanocrystals 4 2. Cu2S- CdS all-inorganic nanocrystal solar cells. We demonstrated the rational synthesis of... Hydrothermal Synthesis of Single Phase Pyrite FeS2 Nanocrystals. We demonstrated a single-source molecular precursor that can be used for the synthesis ... CdS Semiconductor Nanostructures,” Advanced Materials, (2008), 20(22), 4306. Y. Wu, C. Wadia, W. Ma, B. Sadtler, A. P. Alivisatos, “ Synthesis of

Synthesis, characterization and design of a nanocrystal based photovoltaic device

NASA Astrophysics Data System (ADS)

Erwin, Mary Margaret

Nanocomposites have shown promise as the active layer for photovoltaic energy conversion. Devices consisting of CdSe nanocrystals and semiconducting polymer, and devices consisting of C60 and semiconducting polymer have been recently investigated. This work will present the rational design, synthesis, fabrication and characterization of a nanocomposite photovoltaic device-containing Poly 3-hexylthiophene (P3HT), Cadmium Selenium (CdSe) nanocrystals, and C60. The use of these three components allows for a dedicated light harvester, CdSe nanocrystals, a dedicated hole transporter, P3HT, and a dedicated electron transporter, C60. Two primary premises were investigated in this work; first what effect the size of the nanocrystal would have on the efficiency of the devices and second would the addition of C 60 to a CdSe nanocrystal/semiconducting polymer device increase the efficiency of the devices. Three sizes of CdSe nanocrystals (30A, 45A, and 72A) were used in the photoactive layer. Five different composites were used for the photoactive layer ranging from 20% CdSe or C60 to 80% CdSe or C60 of each size of CdSe nanocrystal, while the percentage of P3HT was held constant at 20%. All of the composites were tested at 514 nm at 5 W/m2 and at the industry standard of AM 1.5 at 1000 W/m2 (1 sun). After all the results were analyzed, it was seen that with the addition of C60 only a small percentage of CdSe nanocrystals would be required to make an efficient device, thus making this device cost effective and with more research a viable new source of photovoltaic energy.

Synthesis and spectroscopic properties of silica-dye-semiconductor nanocrystal hybrid particles.

PubMed

Ren, Ting; Erker, Wolfgang; Basché, Thomas; Schärtl, Wolfgang

2010-12-07

We prepared silica-dye-nanocrystal hybrid particles and studied the energy transfer from semiconductor nanocrystals (= donor) to organic dye molecules (= acceptor). Multishell CdSe/CdS/ZnS semiconductor nanocrystals were adsorbed onto monodisperse Stöber silica particles with an outer silica shell of thickness 2-23 nm containing organic dye molecules (Texas Red). The thickness of this dye layer has a strong effect on the energy transfer efficiency, which is explained by the increase in the number of dye molecules homogeneously distributed within the silica shell, in combination with an enhanced surface adsorption of nanocrystals with increasing dye amount. Our conclusions were underlined by comparison of the experimental results with numerically calculated FRET efficiencies and by control experiments confirming attractive interaction between the nanocrystals and Texas Red freely dissolved in solution.

Emission efficiency limit of Si nanocrystals

PubMed Central

Limpens, Rens; Luxembourg, Stefan L.; Weeber, Arthur W.; Gregorkiewicz, Tom

2016-01-01

One of the important obstacles on the way to application of Si nanocrystals for development of practical devices is their typically low emissivity. In this study we explore the limits of external quantum yield of photoluminescence of solid-state dispersions of Si nanocrystals in SiO2. By making use of a low-temperature hydrogen passivation treatment we demonstrate a maximum emission quantum efficiency of approximately 35%. This is the highest value ever reported for this type of material. By cross-correlating PL lifetime with EQE values, we obtain a comprehensive understanding of the efficiency limiting processes induced by Pb-defects. We establish that the observed record efficiency corresponds to an interface density of Pb-centers of 1.3 × 1012 cm12, which is 2 orders of magnitude higher than for the best Si/SiO2 interface. This result implies that Si nanocrystals with up to 100% emission efficiency are feasible. PMID:26786062

Investigation of 124Xe nuclear structure with the 8Pi spectrometer at TRIUMF-ISAC

NASA Astrophysics Data System (ADS)

Radich, Allison; Garrett, P.; Jigmeddorj, B.; Michetti-Wilson, J.; Diaz Varela, A.; Hadinia, B.; Bianco, L.; Wong, J.; Chagnon-Lessard, S.; Dunlop, R.; Finlay, P.; Laffoley, A.; Leach, K. G.; Rand, E.; Sumithrarachchi, C.; Svennson, C. E.; Wood, J. L.; Yates, S. W.; Andreoiu, C.; Starosta, K.; Cross, D.; Garnsworthy, A. B.; Hackman, G.; Ball, G.; Triambak, S.

2013-10-01

The 124Xe nucleus has been thought to obey O(6) symmetry but a recent Coulomb excitation study has found that while O(5) may be preserved, O(6) appears to be badly broken. To further characterize the structure of this nucleus, a beta-decay experiment was performed at the TRIUMF-ISAC facility. A beam of radioactive 124Cs at a rate of 9.8 × 107 ions/s was implanted at the center of the 8Pi spectrometer where it underwent β + /EC decay into stable 124Xe. High-statistics gamma-gamma coincidence measurements have been analyzed to add to the level scheme of 124Xe, which has been extended considerably. The high statistics data set has revealed a new decay branch from a 124Cs high-spin isomer as well as several very-weak transitions between low-spin states in 124Xe. Branching ratios and B(E2) transition strengths have been calculated for the updated level scheme. The results will be important in determining collective properties and nuclear structure of the 124Xe.

Studies on cryogenic Xe capillary jet target for laser-produced plasma EUV-light source

NASA Astrophysics Data System (ADS)

Inoue, T.; Nica, P. E.; Kaku, K.; Shimoura, A.; Amano, S.; Miyamoto, S.; Mochizuki, T.

2006-03-01

In this paper, characterizations of a cryogenic Xe capillary jet target for a laser-produced plasma extreme ultraviolet (EUV) light source are reported. The capillary jet target is a candidate of fast-supplying targets for mitigating debris generation and target consumption in a vacuum chamber without reducing the EUV conversion efficiency. Xe capillary jets (jet velocity ~ 0.4 m/s) were generated in vacuum by using annular nozzles chilled to ~ 170 K at a Xe backing pressure of ~ 0.7 MPa. Forming mechanisms of the capillary jet targets were studied by using numerical calculations. Furthermore, laser-produced plasma EUV generation was performed by irradiating a Nd:YAG laser (1064 nm, ~ 0.5 J, 10 ns, 120 μmφ, ~ 4×10 11 W/cm2) on a Xe capillary jet target (outer / inner diameter = 100 / 70 μmφ). The angular distribution of EUV generation was approximately uniform around the Xe capillary jet target, and the peak kinetic energy of the fast-ions was evaluated to be ~ 2 keV.

Angular dependence of EWS time delay for photoionization of @Xe

NASA Astrophysics Data System (ADS)

Mandal, Ankur; Deshmukh, Pranawa; Kheifets, Anatoli; Dolmatov, Valeriy; Manson, Steven

2017-04-01

Interference between photoionization channels leads to angular dependence in photoionization time delay. Angular dependence is found to be a common effect for two-photon absorption experiments very recently. The effect of confinement on the time delay where each partial wave contributions to the ionization are studied. In this work we report angular dependence and confinement effects on Eisenbud-Wigner-Smith (EWS) time delay in atomic photoionization. Using and we computed the EWS time delay for free and confined Xe atom for photoionization from inner 4d3/2 and 4d5/2 and outer 5p1/2 and 5p3/2 subshells at various angles. The calculated EWS time delay is few tens to few hundreds of attoseconds (10-18 second). The photoionization time delay for @Xe follows that in the free Xe atom on which the confinement oscillations are built. The present work reveals the effect of confinement on the photoionization time delay at different angles between photoelectron ejection and the photon polarization.

Deep level transient spectroscopy (DLTS) on colloidal-synthesized nanocrystal solids.

PubMed

Bozyigit, Deniz; Jakob, Michael; Yarema, Olesya; Wood, Vanessa

2013-04-24

We demonstrate current-based, deep level transient spectroscopy (DLTS) on semiconductor nanocrystal solids to obtain quantitative information on deep-lying trap states, which play an important role in the electronic transport properties of these novel solids and impact optoelectronic device performance. Here, we apply this purely electrical measurement to an ethanedithiol-treated, PbS nanocrystal solid and find a deep trap with an activation energy of 0.40 eV and a density of NT = 1.7 × 10(17) cm(-3). We use these findings to draw and interpret band structure models to gain insight into charge transport in PbS nanocrystal solids and the operation of PbS nanocrystal-based solar cells.

Protein unfolding versus β-sheet separation in spider silk nanocrystals

NASA Astrophysics Data System (ADS)

Alam, Parvez

2014-03-01

In this communication a mechanism for spider silk strain hardening is proposed. Shear failure of β-sheet nanocrystals is the first failure mode that gives rise to the creation of smaller nanocrystals, which are of higher strength and stiffness. β-sheet unfolding requires more energy than nanocrystal separation in a shear mode of failure. As a result, unfolding occurs after the nanocrystals separate in shear. β-sheet unfolding yields a secondary strain hardening effect once the β-sheet conformation is geometrically stable and acts like a unidirectional fibre in a fibre reinforced composite. The mechanism suggested herein is based on molecular dynamics calculations of residual inter-β-sheet separation strengths against residual intra-β-sheet unfolding strengths.

Nuclear spin relaxation due to chemical shift anisotropy of gas-phase 129Xe.

PubMed

Hanni, Matti; Lantto, Perttu; Vaara, Juha

2011-08-14

Nuclear spin relaxation provides detailed dynamical information on molecular systems and materials. Here, first-principles modeling of the chemical shift anisotropy (CSA) relaxation time for the prototypic monoatomic (129)Xe gas is carried out, both complementing and predicting the results of NMR measurements. Our approach is based on molecular dynamics simulations combined with pre-parametrized ab initio binary nuclear shielding tensors, an "NMR force field". By using the Redfield relaxation formalism, the simulated CSA time correlation functions lead to spectral density functions that, for the first time, quantitatively determine the experimental spin-lattice relaxation times T(1). The quality requirements on both the Xe-Xe interaction potential and binary shielding tensor are investigated in the context of CSA T(1). Persistent dimers Xe(2) are found to be responsible for the CSA relaxation mechanism in the low-density limit of the gas, completely in line with the earlier experimental findings.

Nanocrystal assembly for bottom-up plasmonic materials

NASA Astrophysics Data System (ADS)

Tao, Andrea Rae

2007-12-01

Plasmonic materials are emerging as key platforms for applications that rely on the manipulation of light at small length scales. Materials that possess sub-wavelength metallic features support either localized or propagating surface plasmons that can induce huge local electromagnetic fields at the metal surface, facilitating a host of extraordinary optical phenomena. For many of the breakthrough photonic, spectroscopic, and optoelectronic applications of plasmonics, the bottom-up fabrication of these materials from low-dimensional structures has yet to be explored. Because colloidal metal nanostructures can be readily synthesized with controlled shapes and sizes, and because these structures also generate plasmon-mediated evanescent fields near their surfaces when irradiated with light, Ag nanocrystals and nanowires are ideal building blocks for rationally designed plasmonic materials. This dissertation addresses three major challenges: (1) the synthesis of Ag polyhedral nanocrystals and nanowires, (2) the bottom-up organization of these nanostructures into one-, two-, and three-dimensional assemblies, and (3) the application of these assemblies as spectroscopic sensing platforms. Faceted Ag colloids were synthesized in high yield and with remarkable monodispersity using the polyol process, where Ag+ is reduced in the presence of a polymer capping agent that serves to regulate nucleation and crystallographic growth direction. The resulting nanocrystals and nanowires are bound exclusively by {100} and {111} crystal planes, where nanowires possess pentagonal cross-sections and nanocrystals possess octahedral symmetry. Because allowed plasmon modes are explicitly dictated by geometric considerations, each shape exhibits a unique scattering spectrum in the optical wavelengths. These shaped colloidal building blocks were assembled into ordered groupings and superlattices to achieve controlled electromagnetic coupling between individual nanostructures. Of particular

Two-photon spectroscopy of autoionizing states of Xe² near threshold

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pratt, Stephen T.; Dehmer, Patricia M.; Dehmer, Joseph L.

1990-01-01

The two-photon ionization spectrum of Xe² in the region of the first ionization threshold is presented. Vibronic bands corresponding to at least four different autoionizing electronic states of Xe² are observed for the first time and are tentatively assigned. The observed appearance potential is significantly higher (by 415 cm-1) than the earlier single-photon ionization result (Ng, Trevor, Mahan and Lee, - J. Chem. Phys. 65 (1976) 4327).

General method for the synthesis of hierarchical nanocrystal-based mesoporous materials.

PubMed

Rauda, Iris E; Buonsanti, Raffaella; Saldarriaga-Lopez, Laura C; Benjauthrit, Kanokraj; Schelhas, Laura T; Stefik, Morgan; Augustyn, Veronica; Ko, Jesse; Dunn, Bruce; Wiesner, Ulrich; Milliron, Delia J; Tolbert, Sarah H

2012-07-24

Block copolymer templating of inorganic materials is a robust method for the production of nanoporous materials. The method is limited, however, by the fact that the molecular inorganic precursors commonly used generally form amorphous porous materials that often cannot be crystallized with retention of porosity. To overcome this issue, here we present a general method for the production of templated mesoporous materials from preformed nanocrystal building blocks. The work takes advantage of recent synthetic advances that allow organic ligands to be stripped off of the surface of nanocrystals to produce soluble, charge-stabilized colloids. Nanocrystals then undergo evaporation-induced co-assembly with amphiphilic diblock copolymers to form a nanostructured inorganic/organic composite. Thermal degradation of the polymer template results in nanocrystal-based mesoporous materials. Here, we show that this method can be applied to nanocrystals with a broad range of compositions and sizes, and that assembly of nanocrystals can be carried out using a broad family of polymer templates. The resultant materials show disordered but homogeneous mesoporosity that can be tuned through the choice of template. The materials also show significant microporosity, formed by the agglomerated nanocrystals, and this porosity can be tuned by the nanocrystal size. We demonstrate through careful selection of the synthetic components that specifically designed nanostructured materials can be constructed. Because of the combination of open and interconnected porosity, high surface area, and compositional tunability, these materials are likely to find uses in a broad range of applications. For example, enhanced charge storage kinetics in nanoporous Mn(3)O(4) is demonstrated here.

The aggregation and characteristics of radiation-induced defects in lithium fluoride nanocrystals

NASA Astrophysics Data System (ADS)

Voitovich, A. P.; Kalinov, V. S.; Korzhik, M. V.; Martynovich, E. F.; Runets, L. P.; Stupak, A. P.

2013-02-01

It has been established that diffusion activation energies for anion vacancies and centres ? in lithium fluoride nanocrystals are higher than those in bulk crystals. In nanocrystals, ? centres migrating in the range of the temperature close to room temperature is not observed and these centres remain stable. The ratio of centres ? and F 2 concentrations in nanocrystals is higher than in bulk crystals. A new type of colour centres, which is absent in bulk crystals, is discovered in nanocrystals.

Origins of Magnetite Nanocrystals in Martian Meteorite ALH84001

NASA Technical Reports Server (NTRS)

Thomas-Keprta, Kathie L.; Clemett, Simon J.; Mckay, David S.; Gibson, Everett K.; Wentworth, Susan J.

2009-01-01

The Martian meteorite ALH84001 preserves evidence of interaction with aqueous fluids while on Mars in the form of microscopic carbonate disks. These carbonate disks are believed to have precipitated 3.9 Ga ago at beginning of the Noachian epoch on Mars during which both the oldest extant Martian surfaces were formed, and perhaps the earliest global oceans. Intimately associated within and throughout these carbonate disks are nanocrystal magnetites (Fe3O4) with unusual chemical and physical properties, whose origins have become the source of considerable debate. One group of hypotheses argues that these magnetites are the product of partial thermal decomposition of the host carbonate. Alternatively, the origins of mag- netite and carbonate may be unrelated; that is, from the perspective of the carbonate the magnetite is allochthonous. For example, the magnetites might have already been present in the aqueous fluids from which the carbonates were believed to have been deposited. We have sought to resolve between these hypotheses through the detailed characterized of the compo- sitional and structural relationships of the carbonate disks and associated magnetites with the orthopyroxene matrix in which they are embedded. Extensive use of focused ion beam milling techniques has been utilized for sample preparation. We then compared our observations with those from experimental thermal decomposition studies of sideritic carbonates under a range of plausible geological heating scenarios. We conclude that the vast majority of the nanocrystal magnetites present in the car- bonate disks could not have formed by any of the currently proposed thermal decomposition scenarios. Instead, we find there is considerable evidence in support of an alternative allochthonous origin for the magnetite unrelated to any shock or thermal processing of the carbonates.

Process for forming shaped group III-V semiconductor nanocrystals, and product formed using process

DOEpatents

Alivisatos, A. Paul; Peng, Xiaogang; Manna, Liberato

2001-01-01

A process for the formation of shaped Group III-V semiconductor nanocrystals comprises contacting the semiconductor nanocrystal precursors with a liquid media comprising a binary mixture of phosphorus-containing organic surfactants capable of promoting the growth of either spherical semiconductor nanocrystals or rod-like semiconductor nanocrystals, whereby the shape of the semiconductor nanocrystals formed in said binary mixture of surfactants is controlled by adjusting the ratio of the surfactants in the binary mixture.

Process for forming shaped group II-VI semiconductor nanocrystals, and product formed using process

DOEpatents

Alivisatos, A. Paul; Peng, Xiaogang; Manna, Liberato

2001-01-01

A process for the formation of shaped Group II-VI semiconductor nanocrystals comprises contacting the semiconductor nanocrystal precursors with a liquid media comprising a binary mixture of phosphorus-containing organic surfactants capable of promoting the growth of either spherical semiconductor nanocrystals or rod-like semiconductor nanocrystals, whereby the shape of the semiconductor nanocrystals formed in said binary mixture of surfactants is controlled by adjusting the ratio of the surfactants in the binary mixture.

Syntheses and applications of manganese-doped II-VI semiconductor nanocrystals

NASA Astrophysics Data System (ADS)

Yang, Heesun

Syntheses, characterizations, and applications of two different Mn-doped semiconductor nanocrystals, ZnS:Mn and CdS:Mn/ZnS core/shell, were investigated. ZnS:Mn nanocrystals with sizes between 3 and 4 nm were synthesized via a competitive reaction chemistry. A direct current (dc) electroluminescent (EL) device having a hybrid organic/inorganic multilayer structure of an indium tin oxide (ITO) transparent conducting electrode, a (poly(3,4-ethylenedioxythiophene)/poly(styrenesulfonate) (PEDOT-PSS) and a poly(N-vinylcarbazole) (PVK) bilayer hole transport film, a ZnS:Mn nanocrystal layer, and Al dot contacts was demonstrated to emit blue (˜445 and ˜495 nm) from PVK and yellow (˜600 nm) light from Mn activator in ZnS. The EL emission spectrum was dependent upon both the voltage and Mn concentration, showing a decreasing nanocrystal to PVK emission ratio from 10 at 20 V to 4 at 28 V, and an increasing ratio from 1.3 at 0.40 mol % to 4.3 at 2.14 mol %. Mn-doped CdS core nanocrystals were produced ranging from 1.5 to 2.3 nm in diameter with a ZnS shell via a reverse micelle process. In contrast to CdS:Mn nanocrystals passivated by n-dodecanethiol, ZnS-passivated CdS:Mn (CdS:Mn/ZnS core/shell) nanocrystals were efficient and photostable. CdS:Mn/ZnS core/shell nanocrystals exhibited a quantum yield of ˜18%, and the photoluminescence (PL) intensity increased by 40% after 400 nm UV irradiation in air. X-ray photoelectron spectroscopy (XPS) data showed that UV irradiation of CdS:Mn/ZnS nanocrystals induces the photooxidation of the ZnS shell surface to ZnSO4. This photooxidation product is presumably responsible for the increased PL emission by serving as a passivating surface layer. Luminescent lifetime data from the core/shell nanocrystals could be fit with two exponential functions, with a time constant of ˜170 nsec for the defect-related centers and of ˜1 msec for the Mn centers. The CdS:Mn/ZnS nanocrystals with a core crystal diameter of 2.3 nm and a 0.4 nm thick Zn

CO2 controlled flocculation of microalgae using pH responsive cellulose nanocrystals

NASA Astrophysics Data System (ADS)

Eyley, Samuel; Vandamme, Dries; Lama, Sanjaya; van den Mooter, Guy; Muylaert, Koenraad; Thielemans, Wim

2015-08-01

Cellulose nanocrystals were grafted with imidazole functionalities up to DS 0.06 using a one-pot functionalization strategy. The resulting nanocrystals were shown to have a pH responsive surface charge which was found to be positive below pH 6 and negative above pH 7. These imidazolyl cellulose nanocrystals were tested for flocculation of Chlorella vulgaris using CO2 to induce flocculation. Up to 90% flocculation efficiency was achieved with 200 mg L-1 dose. Furthermore, the modified cellulose nanocrystals showed good compatibility with the microalgae during cultivation, giving potential for the production of reversible flocculation systems.Cellulose nanocrystals were grafted with imidazole functionalities up to DS 0.06 using a one-pot functionalization strategy. The resulting nanocrystals were shown to have a pH responsive surface charge which was found to be positive below pH 6 and negative above pH 7. These imidazolyl cellulose nanocrystals were tested for flocculation of Chlorella vulgaris using CO2 to induce flocculation. Up to 90% flocculation efficiency was achieved with 200 mg L-1 dose. Furthermore, the modified cellulose nanocrystals showed good compatibility with the microalgae during cultivation, giving potential for the production of reversible flocculation systems. Electronic supplementary information (ESI) available: Spectra for all products. See DOI: 10.1039/C5NR03853G

Synthesis and electron storage characteristics of isolated silver nanodots on/embedded in Al 2O 3 gate dielectric

NASA Astrophysics Data System (ADS)

Wang, Q.; Song, Z. T.; Liu, W. L.; Lin, C. L.; Wang, T. H.

2004-05-01

Monolayer-isolated silver (Ag) nanodots with the average diameter down to 7 nm are synthesized on Al 2O 3/Si substrate by vacuum electron-beam evaporation followed by annealing at 400 °C in N 2 ambient. Metal-insulator-silicon (MIS) structures with Ag nanodots embedded in Al 2O 3 gate dielectric are fabricated. Clear electron storage effect with the flatband voltage shift of 1.3 eV is observed through capacitance-conductance and conductance-voltage measurements. Our results demonstrate the feasibility of applying Ag nanodots for nanocrystal floating-gate memory devices.

Probing the formation of silicon nano-crystals (Si-ncs) using variable energy positron annihilation spectroscopy

NASA Astrophysics Data System (ADS)

Knights, A. P.; Bradley, J. D. B.; Hulko, O.; Stevanovic, D. V.; Edwards, C. J.; Kallis, A.; Coleman, P. G.; Crowe, I. F.; Halsall, M. P.; Gwilliam, R. M.

2011-01-01

We describe preliminary results from studies of the formation of silicon nano-crystals (Si-ncs) embedded in stoichiometric, thermally grown SiO2 using Variable Energy Positron Annihilation Spectroscopy (VEPAS). We show that the VEPAS technique is able to monitor the introduction of structural damage. In SiO2 through the high dose Si+ ion implantation required to introduce excess silicon as a precursor to Si-nc formation. VEPAS is also able to characterize the rate of the removal of this damage with high temperature annealing, showing strong correlation with photoluminescence. Finally, VEPAS is shown to be able to selectively probe the interface between Si-ncs and the host oxide. Introduction of hydrogen at these interfaces suppresses the trapping of positrons at the interfaces.

IR spectroscopic study of the displacement of an SF6 monolayer on graphite by Xe

NASA Astrophysics Data System (ADS)

Hess, G. B.; Xia, Yu

2017-09-01

We report a study of displacement by xenon of a monolayer of sulphur hexafluoride initially condensed on a graphite surface. Earlier work showed that, below 112 K, Xe displaces SF6 almost completely in a first-order transition. Working at higher temperatures, we show that this system has a simple eutectic-like phase diagram, at least for SF6 not too dilute. In our experiment, both adsorbates are in equilibrium with their respective vapors in a cold cell. In our infrared reflection-absorption spectroscopy measurements, the SF6 coverage on the surface is monitored by the frequency shift due to dynamic dipole coupling of the collective mode of the strong SF6 ν3 vibrational resonance. Simulations relate this frequency shift to the SF6 areal density. Below T ≈ 134 K, with increasing Xe pressure, a small amount Xe dissolves in the solid SF6 monolayer preceding its displacement by a solid predominantly Xe monolayer in a first-order transition. Above 134 K, there is a weaker first-order transition to a mixed liquid monolayer, followed by continuous increase in Xe concentration. If the initial SF6 monolayer is near its melting line, the melting transition on adding Xe appears to become continuous.

IR spectroscopic study of the displacement of an SF6 monolayer on graphite by Xe.

PubMed

Hess, G B; Xia, Yu

2017-09-07

We report a study of displacement by xenon of a monolayer of sulphur hexafluoride initially condensed on a graphite surface. Earlier work showed that, below 112 K, Xe displaces SF 6 almost completely in a first-order transition. Working at higher temperatures, we show that this system has a simple eutectic-like phase diagram, at least for SF 6 not too dilute. In our experiment, both adsorbates are in equilibrium with their respective vapors in a cold cell. In our infrared reflection-absorption spectroscopy measurements, the SF 6 coverage on the surface is monitored by the frequency shift due to dynamic dipole coupling of the collective mode of the strong SF 6 ν 3 vibrational resonance. Simulations relate this frequency shift to the SF 6 areal density. Below T ≈ 134 K, with increasing Xe pressure, a small amount Xe dissolves in the solid SF 6 monolayer preceding its displacement by a solid predominantly Xe monolayer in a first-order transition. Above 134 K, there is a weaker first-order transition to a mixed liquid monolayer, followed by continuous increase in Xe concentration. If the initial SF 6 monolayer is near its melting line, the melting transition on adding Xe appears to become continuous.

135Xe measurements with a two-element CZT-based radioxenon detector for nuclear explosion monitoring.

PubMed

Ranjbar, Lily; Farsoni, Abi T; Becker, Eric M

2017-04-01

Measurement of elevated concentrations of xenon radioisotopes ( 131m Xe, 133m Xe, 133 Xe and 135 Xe) in the atmosphere has been shown to be a very powerful method for verifying whether or not a detected explosion is nuclear in nature. These isotopes are among the few with enough mobility and with half-lives long enough to make their detection at long distances realistic. Existing radioxenon detection systems used by the Comprehensive Nuclear-Test-Ban Treaty Organization (CTBTO) suffer from problems such as complexity, need for high maintenance and memory effect. To study the response of CdZnTe (CZT) detectors to xenon radioisotopes and investigate whether it is capable of mitigating the aforementioned issues with the current radioxenon detection systems, a prototype detector utilizing two coplanar CZT detectors was built and tested at Oregon State University. The detection system measures xenon radioisotopes through beta-gamma coincidence technique by detecting coincidence events between the two detectors. In this paper, we introduce the detector design and report our measurement results with radioactive lab sources and 135 Xe produced in the OSU TRIGA reactor. Minimum Detectable Concentration (MDC) for 135 Xe was calculated to be 1.47 ± 0.05 mBq/m 3 . Copyright © 2017 Elsevier Ltd. All rights reserved.

Spindly cobalt ferrite nanocrystals: preparation, characterization and magnetic properties.

PubMed

Cao, Xuebo; Gu, Li

2005-02-01

In this paper we describe the preparation of homogeneously needle-shaped cobalt ferrite (CoFe(2)O(4)) nanocrystals on a large scale through the smooth decomposition of urea and the resulting co-precipitation of Co(2+) and Fe(3+) in oleic acid micelles. Furthermore, we found that other ferrite nanocrystals with a needle-like shape, such as zinc ferrite (ZnFe(2)O(4)) and nickel ferrite (NiFe(2)O(4)), can be prepared by the same process. Needle-shaped CoFe(2)O(4) nanocrystals dispersed in an aqueous solution containing oleic acid exhibit excellent stability and the formed colloid does not produce any precipitations after two months, which is of prime importance if these materials are applied in magnetic fluids. X-ray diffraction (XRD) measurements were used to characterize the phase and component of the co-precipitation products, and demonstrate that they are spinel ferrite with a cubic symmetry. Transmission electron microscopy (TEM) observation showed that all the nanocrystals present a needle-like shape with a 22 nm short axis and an aspect ratio of around 6. Varying the concentration of oleic acid did not bring about any obvious influence on the size distribution and shapes of CoFe(2)O(4). The magnetic properties of the needle-shaped CoFe(2)O(4) nanocrystals were evaluated by using a vibrating sample magnetometer (VSM), electron paramagnetic resonance (EPR), and a Mössbauer spectrometer, and the results all demonstrated that CoFe(2)O(4) nanocrystals were superparamagnetic at room temperature.

High-purity Cu nanocrystal synthesis by a dynamic decomposition method.

PubMed

Jian, Xian; Cao, Yu; Chen, Guozhang; Wang, Chao; Tang, Hui; Yin, Liangjun; Luan, Chunhong; Liang, Yinglin; Jiang, Jing; Wu, Sixin; Zeng, Qing; Wang, Fei; Zhang, Chengui

2014-12-01

Cu nanocrystals are applied extensively in several fields, particularly in the microelectron, sensor, and catalysis. The catalytic behavior of Cu nanocrystals depends mainly on the structure and particle size. In this work, formation of high-purity Cu nanocrystals is studied using a common chemical vapor deposition precursor of cupric tartrate. This process is investigated through a combined experimental and computational approach. The decomposition kinetics is researched via differential scanning calorimetry and thermogravimetric analysis using Flynn-Wall-Ozawa, Kissinger, and Starink methods. The growth was found to be influenced by the factors of reaction temperature, protective gas, and time. And microstructural and thermal characterizations were performed by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and differential scanning calorimetry. Decomposition of cupric tartrate at different temperatures was simulated by density functional theory calculations under the generalized gradient approximation. High crystalline Cu nanocrystals without floccules were obtained from thermal decomposition of cupric tartrate at 271°C for 8 h under Ar. This general approach paves a way to controllable synthesis of Cu nanocrystals with high purity.

High-purity Cu nanocrystal synthesis by a dynamic decomposition method

NASA Astrophysics Data System (ADS)

Jian, Xian; Cao, Yu; Chen, Guozhang; Wang, Chao; Tang, Hui; Yin, Liangjun; Luan, Chunhong; Liang, Yinglin; Jiang, Jing; Wu, Sixin; Zeng, Qing; Wang, Fei; Zhang, Chengui

2014-12-01

Cu nanocrystals are applied extensively in several fields, particularly in the microelectron, sensor, and catalysis. The catalytic behavior of Cu nanocrystals depends mainly on the structure and particle size. In this work, formation of high-purity Cu nanocrystals is studied using a common chemical vapor deposition precursor of cupric tartrate. This process is investigated through a combined experimental and computational approach. The decomposition kinetics is researched via differential scanning calorimetry and thermogravimetric analysis using Flynn-Wall-Ozawa, Kissinger, and Starink methods. The growth was found to be influenced by the factors of reaction temperature, protective gas, and time. And microstructural and thermal characterizations were performed by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and differential scanning calorimetry. Decomposition of cupric tartrate at different temperatures was simulated by density functional theory calculations under the generalized gradient approximation. High crystalline Cu nanocrystals without floccules were obtained from thermal decomposition of cupric tartrate at 271°C for 8 h under Ar. This general approach paves a way to controllable synthesis of Cu nanocrystals with high purity.

Probing the structure of the stable Xe isotopes with inelastic neutron scattering

NASA Astrophysics Data System (ADS)

Peters, Erin E.; Ross, Timothy J.; Crider, Benjamin P.; Yates, Steven W.

2018-05-01

The stable isotopes of xenon, which have attracted interest for a number of reasons, span a transitional region that evolves from γ-soft structures for the lighter mass isotopes to nearly spherical 136Xe with a closed neutron shell. The nature of this transition, which is gradual, is not well understood. To provide detailed spectroscopic information on the Xe isotopes, we have studied 130,132,134,136Xe at the University of Kentucky Accelerator Laboratory using inelastic neutron scattering and γ-ray detection. These measurements yielded γ-ray angular distributions, branching ratios, multipole mixing ratios, and level lifetimes (from the Doppler-shift attenuation method), which allowed the determination of reduced transition probabilities and provided insight into the structure of these nuclei.

Exciton-Delocalizing Ligands Can Speed Up Energy Migration in Nanocrystal Solids.

PubMed

Azzaro, Michael S; Dodin, Amro; Zhang, Diana Y; Willard, Adam P; Roberts, Sean T

2018-05-09

Researchers have long sought to use surface ligands to enhance energy migration in nanocrystal solids by decreasing the physical separation between nanocrystals and strengthening their electronic coupling. Exciton-delocalizing ligands, which possess frontier molecular orbitals that strongly mix with nanocrystal band-edge states, are well-suited for this role because they can facilitate carrier-wave function extension beyond the nanocrystal core, reducing barriers for energy transfer. This report details the use of the exciton-delocalizing ligand phenyldithiocarbamate (PDTC) to tune the transport rate and diffusion length of excitons in CdSe nanocrystal solids. A film composed of oleate-terminated CdSe nanocrystals is subjected to a solid-state ligand exchange to replace oleate with PDTC. Exciton migration in the films is subsequently investigated by femtosecond transient absorption. Our experiments indicate that the treatment of nanocrystal films with PDTC leads to rapid (∼400 fs) downhill energy migration (∼80 meV), while no such migration occurs in oleate-capped films. Kinetic Monte Carlo simulations allow us to extract both rates and length scales for exciton diffusion in PDTC-treated films. These simulations reproduce dynamics observed in transient absorption measurements over a range of temperatures and confirm excitons hop via a Miller-Abrahams mechanism. Importantly, our experiments and simulations show PDTC treatment increases the exciton hopping rate to 200 fs, an improvement of 5 orders of magnitude relative to oleate-capped films. This exciton hopping rate stands as one of the fastest determined for CdSe solids. The facile, room-temperature processing and improved transport properties offered by the solid-state exchange of exciton-delocalizing ligands show they offer promise for the construction of strongly coupled nanocrystal arrays.

Organo luminescent semiconductor nanocrystal probes for biological applications and process for making and using such probes

DOEpatents

Weiss, Shimon [Pinole, CA; Bruchez, Jr., Marcel; Alivisatos, Paul [Oakland, CA

2008-01-01

A semiconductor nanocrystal compound is described capable of linking to an affinity molecule. The compound comprises (1) a semiconductor nanocrystal capable of emitting electromagnetic radiation and/or absorbing energy, and/or scattering or diffracting electromagnetic radiation--when excited by an electromagnetic radiation source or a particle beam; and (2) an affinity molecule linked to the semiconductor nanocrystal. The semiconductor nanocrystal is linked to an affinity molecule to form a semiconductor nanocrystal probe capable of bonding with a detectable substance. Exposure of the semiconductor nanocrystal to excitation energy will excite the semiconductor nanocrystal causing the emission of electromagnetic radiation. Further described are processes for respectively: making the luminescent semiconductor nanocrystal compound; making the semiconductor nanocrystal probe; and using the probe to determine the presence of a detectable substance in a material.

A wearable multiplexed silicon nonvolatile memory array using nanocrystal charge confinement.

PubMed

Kim, Jaemin; Son, Donghee; Lee, Mincheol; Song, Changyeong; Song, Jun-Kyul; Koo, Ja Hoon; Lee, Dong Jun; Shim, Hyung Joon; Kim, Ji Hoon; Lee, Minbaek; Hyeon, Taeghwan; Kim, Dae-Hyeong

2016-01-01

Strategies for efficient charge confinement in nanocrystal floating gates to realize high-performance memory devices have been investigated intensively. However, few studies have reported nanoscale experimental validations of charge confinement in closely packed uniform nanocrystals and related device performance characterization. Furthermore, the system-level integration of the resulting devices with wearable silicon electronics has not yet been realized. We introduce a wearable, fully multiplexed silicon nonvolatile memory array with nanocrystal floating gates. The nanocrystal monolayer is assembled over a large area using the Langmuir-Blodgett method. Efficient particle-level charge confinement is verified with the modified atomic force microscopy technique. Uniform nanocrystal charge traps evidently improve the memory window margin and retention performance. Furthermore, the multiplexing of memory devices in conjunction with the amplification of sensor signals based on ultrathin silicon nanomembrane circuits in stretchable layouts enables wearable healthcare applications such as long-term data storage of monitored heart rates.

Comparison of air space measurement imaged by CT, small-animal CT, and hyperpolarized Xe MRI

NASA Astrophysics Data System (ADS)

Madani, Aniseh; White, Steven; Santyr, Giles; Cunningham, Ian

2005-04-01

Lung disease is the third leading cause of death in the western world. Lung air volume measurements are thought to be early indicators of lung disease and markers in pharmaceutical research. The purpose of this work is to develop a lung phantom for assessing and comparing the quantitative accuracy of hyperpolarized xenon 129 magnetic resonance imaging (HP 129Xe MRI), conventional computed tomography (HRCT), and highresolution small-animal CT (μCT) in measuring lung gas volumes. We developed a lung phantom consisting of solid cellulose acetate spheres (1, 2, 3, 4 and 5 mm diameter) uniformly packed in circulated air or HP 129Xe gas. Air volume is estimated based on simple thresholding algorithm. Truth is calculated from the sphere diameters and validated using μCT. While this phantom is not anthropomorphic, it enables us to directly measure air space volume and compare these imaging methods as a function of sphere diameter for the first time. HP 129Xe MRI requires partial volume analysis to distinguish regions with and without 129Xe gas and results are within %5 of truth but settling of the heavy 129Xe gas complicates this analysis. Conventional CT demonstrated partial-volume artifacts for the 1mm spheres. μCT gives the most accurate air-volume results. Conventional CT and HP 129Xe MRI give similar results although non-uniform densities of 129Xe require more sophisticated algorithms than simple thresholding. The threshold required to give the true air volume in both HRCT and μCT, varies with sphere diameters calling into question the validity of thresholding method.

Synthesis and applications of heterostructured semiconductor nanocrystals

NASA Astrophysics Data System (ADS)

Khon, Elena

Semiconductor nanocrystals (NCs) have been of great interest to researchers for several decades due to their unique optoelectronic properties. These nanoparticles are widely used for a variety of different applications. However, there are many unresolved issues that lower the efficiency and/or stability of devices which incorporate these NCs. Our research is dedicated to addressing these issues by identifying potential problems and resolving them, improving existing systems, generating new synthetic strategies, and/or building new devices. The general strategies for the synthesis of different nanocrystals were established in this work, one of which is the colloidal growth of gold domains onto CdS semiconductor nanocrystals. Control of shape and size was achieved simply by adjusting the temperature and the time of the reaction. Depending on the exact morphology of Au and CdS domains, fabricated nano-composites can undergo evaporation-induced self-assembly onto a substrate, which is very useful for building devices. CdS/Au heterostructures can assemble in two different ways: through end-to-end coupling of Au domains, resulting in the formation of one-dimensional chains; and via side-by-side packing of CdS nanorods, leading to the onset of two-dimensional superlattices. We investigated the nature of exciton-plasmon interactions in Au-tipped CdS nanorods using femtosecond transient absorption spectroscopy. The study demonstrated that the key optoelectronic properties of electrically coupled metal and semiconductor domains are significantly different from those observed in systems with weak inter-domain coupling. In particular, strongly-coupled nanocomposites promote mixing of electronic states at semiconductor-metal domain interfaces, which causes a significant suppression of both plasmon and exciton carrier excitations. Colloidal QDs are starting to replace organic molecules in many different applications, such as organic light emmiting diods (OLEDs), due to their

Structural and optical characterization of self-assembled Ge nanocrystal layers grown by plasma-enhanced chemical vapor deposition.

PubMed

Saeed, Saba; Buters, Frank; Dohnalova, Katerina; Wosinski, Lech; Gregorkiewicz, Tom

2014-10-10

We present a structural and optical study of solid-state dispersions of Ge nanocrystals prepared by plasma-enhanced chemical vapor deposition. Structural analysis shows the presence of nanocrystalline germanium inclusions embedded in an amorphous matrix of Si-rich SiO(2).Optical characterization reveals two prominent emission bands centered around 2.6 eV and 3.4 eV, and tunable by excitation energy. In addition, the lower energy band shows an excitation power-dependent blue shift of up to 0.3 eV. Decay dynamics of the observed emission contains fast (nanosecond) and slow (microseconds) components, indicating contributions of several relaxation channels. Based on these material characteristics, a possible microscopic origin of the individual emission bands is discussed.

The surface structure of silver-coated gold nanocrystals and its influence on shape control

DOE PAGES

Padmos, J. Daniel; Personick, Michelle L.; Tang, Qing; ...

2015-07-08

Understanding the surface structure of metal nanocrystals with specific facet indices is important due to its impact on controlling nanocrystal shape and functionality. However, this is particularly challenging for halide-adsorbed nanocrystals due to the difficulty in analysing interactions between metals and light halides (for example, chloride). Here we uncover the surface structures of chloride-adsorbed, silver-coated gold nanocrystals with {111}, {110}, {310} and {720} indexed facets by X-ray absorption spectroscopy and density functional theory modelling. The silver–chloride, silver–silver and silver–gold bonding structures are markedly different between the nanocrystal surfaces, and are sensitive to their formation mechanism and facet type. A uniquemore » approach of combining the density functional theory and experimental/simulated X-ray spectroscopy further verifies the surface structure models and identifies the previously indistinguishable valence state of silver atoms on the nanocrystal surfaces. Overall, this work elucidates the thus-far unknown chloride–metal nanocrystal surface structures and sheds light onto the halide-induced growth mechanism of anisotropic nanocrystals.« less

Relativistic, correlation, and polarization effects in two-photon photoionization of Xe

NASA Astrophysics Data System (ADS)

Lagutin, B. M.; Petrov, I. D.; Sukhorukov, V. L.; Demekhin, Ph. V.; Knie, A.; Ehresmann, A.

2017-06-01

Two-photon ionization of xenon was investigated theoretically for exciting-photon energies from 6.7 to 11.5 eV, which results in the ionization of Xe between 5 p1 /2 (13.43 eV) and 5 s (23.40 eV) thresholds. We describe the extension of a previously developed computational technique for the inclusion of relativistic effects to calculate energies of intermediate resonance state and cross sections for two-photon ionization. Reasonable consistency of cross sections calculated in length and velocity form was obtained only after considering many-electron correlations. Agreement between calculated and measured resonance energies is found when core polarization was additionally included in the calculations. The presently computed two-photon photoionization cross sections of Xe are compared with Ar cross sections in our previous work. Photoelectron angular distribution parameters calculated here indicate that intermediated resonances strongly influence photoelectron angular distribution of Xe.

Relaxation rates of low-field gas-phase ^129Xe storage cells

NASA Astrophysics Data System (ADS)

Limes, Mark; Saam, Brian

2010-10-01

A study of longitudinal nuclear relaxation rates T1 of ^129Xe and Xe-N2 mixtures in a magnetic field of 3.8 mT is presented. In this regime, intrinsic spin relaxation is dominated by the intramolecular spin-rotation interaction due to persistent xenon dimers, a mechanism that can be quelled by introducing large amounts of N2 into the storage cell. Extrinsic spin relaxation is dominated by the wall-relaxation rate, which is the primary quantity of interest for the various low-field storage cells and coatings that we have tested. Previous group work has shown that extremely long gas-phase relaxation times T1 can be obtained, but only at large magnetic fields and low xenon densities. The current work is motivated by the practical benefits of retaining hyperpolarized ^129Xe for extended periods of time in a small magnetic field.

Using Hyperpolarized 129Xe MRI to Quantify the Pulmonary Ventilation Distribution

PubMed Central

He, Mu; Driehuys, Bastiaan; Que, Loretta G.; Huang, Yuh-Chin T.

2017-01-01

Background Ventilation heterogeneity is impossible to detect with spirometry. Alternatively, pulmonary ventilation can be imaged 3-dimensionally using inhaled 129Xe MRI. To date such images have been quantified primarily based on ventilation defects. Here, we introduce a robust means to transform 129Xe MRI scans such that the underlying ventilation distribution and its heterogeneity can be quantified. Methods Quantitative 129Xe ventilation MRI was conducted in 12 younger (24.7±5.2 yrs), and 10 older (62.2±7.2 yrs) healthy individuals, as well as 9 younger (25.9±6.4 yrs) and 10 older (63.2±6.1 yrs) asthmatics. The younger healthy population was used to establish a reference ventilation distribution and thresholds for 6 intensity bins. These were used to display and quantify regions of ventilation defect (VDR), low ventilation (LVR) and high ventilation (HVR). Results The ventilation distribution in young subjects was roughly Gaussian with a mean and SD of 0.52±0.18, resulting in VDR=2.1±1.3%, LVR=15.6±5.4% and HVR=17.4±3.1%. Older healthy volunteers exhibited a significantly right-skewed distribution (0.46±0.20, p=0.034), resulting in significantly increased VDR (7.0±4.8%, p=0.008) and LVR (24.5±11.5%, p=0.025). In the asthmatics, VDR and LVR increased in the older population, and HVR was significantly reduced (13.5±4.6% vs 18.9±4.5%, p=0.009). Quantitative 129Xe MRI also revealed different ventilation distribution patterns in response to albuterol in two asthmatics with normal FEV1. Conclusions Quantitative 129Xe MRI provides a robust and objective means to display and quantify the pulmonary ventilation distribution, even in subjects who have airway function impairment not appreciated by spirometry. PMID:27617823

Optical properties of an indium doped CdSe nanocrystal: A density functional approach

DOE Office of Scientific and Technical Information (OSTI.GOV)

Salini, K.; Mathew, Vincent, E-mail: vincent@cukerala.ac.in; Mathew, Thomas

2016-05-06

We have studied the electronic and optical properties of a CdSe nanocrystal doped with n-type impurity atom. First principle calculations of the CdSe nanocrystal based on the density functional theory (DFT), as implemented in the Vienna Ab Initio Simulation Package (VASP) was used in the calculations. We have introduced a single Indium impurity atom into CdSe nanocrystal with 1.3 nm diameter. Nanocrystal surface dangling bonds are passivated with hydrogen atom. The band-structure, density of states and absorption spectra of the doped and undopted nanocrystals were discussed. Inclusion of the n-type impurity atom introduces an additional electron in conduction band, and significantlymore » alters the electronic and optical properties of undoped CdSe nanocrystal. Indium doped CdSe nannocrystal have potential applications in optoelectronic devices.« less

Single step synthesis of high-purity CoO nanocrystals.

PubMed

Yang, Huaming; Ouyang, Jing; Tang, Aidong

2007-07-19

Both octahedral and slice-shaped cubic cobalt monoxide (CoO) nanocrystals with narrow size distributions have been successfully synthesized by a simple solvothermal route. It was found that conditions of the solvothermal treatment showed obvious effects on the formation and purity of the as-synthesized CoO nanocrystals, only when cobalt acetate was used as the cobalt source and when temperature reached 190 degrees C could CoO be produced; also, freeze-drying was necessary for obtaining pure CoO. Size of the CoO nanocrystals varied from 30 to 130 nm. Morphology of the products could be controlled by simply changing the type of surfactant in solvent, and the octahedral CoO nanocrystals showed rounded turns. Purity of the products was detected by intensive X-ray photoelectron spectroscopy (XPS) investigation and Fourier transform infrared spectroscopy (FTIR) combined with differential scanning calorimetry/thermal gravity (DSC/TG). The results indicated an absence of unexpected trivalence cobalt series on surface of the samples, thanks to the protection of the surface by trace amount of carbonate ions, adsorbed hydroxylation, and surfactant with a maximum thickness of 2 nm, which were proved by high-resolution transmission electron microscopy (HRTEM). The as-synthesized CoO nanoparticles were added into positive electrode of Ni/MH batteries, and discharge/charge cycling tests were performed under different rates from 0.1C to 5.0C. The results indicated that the specific capacities of batteries with addition of 5% octahedral or slice CoO nanocrystals at 0.1C were 393.3 and 318.1 mAh/g, respectively, which were higher than that without CoO (269.2mAh/g). Specific capacity of battery with addition of 5% octahedral CoO nanocrystals was 40% higher than that without CoO at 5.0C. Octahedral CoO nanocrystals show better electrochemical activity than slice CoO and indicate interesting potential in the field of electrochemical application.

Using the DFT-D method to describe dispersion interactions in systems of weakly-bonded Xe-aromatic molecules

NASA Astrophysics Data System (ADS)

Andriichenko, N. N.; Ermilov, A. Yu.

2013-08-01

The optimum version of the DFT-D class of methods (BHHLYP-D2, 6-31G*) is chosen to describe binding in a Xe-phenol system with the aim of subsequent KM/MM calculations for complex Xe-containing protein systems. It is shown that the stability of the Xe-phenol system is due to weak dispersion interactions not described in conventional approaches using the density functional. The MP2 approach using the (aug)-cc-pVTZ basis and Stuttgart pseudopotential, which yield the best reproduction of the characteristics of a Xe2 xenon dimer, is chosen as the reference standard. It is noted that the 2010 DFT-D3 methods underestimate the binding energy by a factor of nearly three, while DFT methods without dispersion corrections do not reproduce the stability of Xe2 and Xe-phenol systems. It is found that in the best version of calculations, BHHLYP-D2, the binding energy in Xe-phenol complex is estimated to be 2.7 kcal/mol versus the 3.1 kcal/mol found using the comparative approach. It is concluded that BHHLYP-D2 adequately reproduces the difference between the two conformers of the Xe-phenol complex and trend toward an increase in binding energy in the series of aromatic amino acids (phenylalanine, tyrosine, and tryptophan). DFT-D can also indicate the existence of excess conformers that are missing in systems according to more precise descriptions (MP2/(aug)-cc-pVTZ).

Group IV nanocrystals with ion-exchangeable surface ligands and methods of making the same

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wheeler, Lance M.; Nichols, Asa W.; Chernomordik, Boris D.

Methods are described that include reacting a starting nanocrystal that includes a starting nanocrystal core and a covalently bound surface species to create an ion-exchangeable (IE) nanocrystal that includes a surface charge and a first ion-exchangeable (IE) surface ligand ionically bound to the surface charge, where the starting nanocrystal core includes a group IV element.

Nanostructured Drugs Embedded into a Polymeric Matrix: Vinpocetine/PVP Hybrids Investigated by Debye Function Analysis.

PubMed

Hasa, Dritan; Giacobbe, Carlotta; Perissutti, Beatrice; Voinovich, Dario; Grassi, Mario; Cervellino, Antonio; Masciocchi, Norberto; Guagliardi, Antonietta

2016-09-06

Microcrystalline vinpocetine, coground with cross-linked polyvinylpyrrolidone, affords hybrids containing nanosized drug nanocrystals, the size and size distributions of which depend on milling times and drug-to-polymer weight ratios. Using an innovative approach to microstructural characterization, we analyzed wide-angle X-ray total scattering data by the Debye function analysis and demonstrated the possibility to characterize pharmaceutical solid dispersions obtaining a reliable quantitative view of the physicochemical status of the drug dispersed in an amorphous carrier. The microstructural properties derived therefrom have been successfully employed in reconciling the enigmatic difference in behavior between in vitro and in vivo solubility tests performed on nanosized vinpocetine embedded in a polymeric matrix.

Semiconductor nanocrystal probes for biological applications and process for making and using such probes

DOEpatents

Weiss, Shimon; Bruchez, Marcel; Alivisatos, Paul

2014-01-28

A semiconductor nanocrystal compound and probe are described. The compound is capable of linking to one or more affinity molecules. The compound comprises (1) one or more semiconductor nanocrystals capable of, in response to exposure to a first energy, providing a second energy, and (2) one or more linking agents, having a first portion linked to the one or more semiconductor nanocrystals and a second portion capable of linking to one or more affinity molecules. One or more semiconductor nanocrystal compounds are linked to one or more affinity molecules to form a semiconductor nanocrystal probe capable of bonding with one or more detectable substances in a material being analyzed, and capable of, in response to exposure to a first energy, providing a second energy. Also described are processes for respectively: making the semiconductor nanocrystal compound; making the semiconductor nanocrystal probe; and treating materials with the probe.

Semiconductor nanocrystal probes for biological applications and process for making and using such probes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Weiss, Shimon; Bruchez, Marcel; Alivisatos, Paul A.

2016-12-27

A semiconductor nanocrystal compound and probe are described. The compound is capable of linking to one or more affinity molecules. The compound comprises (1) one or more semiconductor nanocrystals capable of, in response to exposure to a first energy, providing a second energy, and (2) one or more linking agents, having a first portion linked to the one or more semiconductor nanocrystals and a second portion capable of linking to one or more affinity molecules. One or more semiconductor nanocrystal compounds are linked to one or more affinity molecules to form a semiconductor nanocrystal probe capable of bonding with onemore » or more detectable substances in a material being analyzed, and capable of, in response to exposure to a first energy, providing a second energy. Also described are processes for respectively: making the semiconductor nanocrystal compound; making the semiconductor nanocrystal probe; and treating materials with the probe.« less

Cobalt ferrite nanocrystals: out-performing magnetotactic bacteria.

PubMed

Prozorov, Tanya; Palo, Pierre; Wang, Lijun; Nilsen-Hamilton, Marit; Jones, DeAnna; Orr, Daniel; Mallapragada, Surya K; Narasimhan, Balaji; Canfield, Paul C; Prozorov, Ruslan

2007-10-01

Magnetotactic bacteria produce exquisitely ordered chains of uniform magnetite (Fe(3)O(4)) nanocrystals, and the use of the bacterial mms6 protein allows for the shape-selective synthesis of Fe(3)O(4) nanocrystals. Cobalt ferrite (CoFe(2)O(4)) nanoparticles, on the other hand, are not known to occur in living organisms. Here we report on the use of the recombinant mms6 protein in a templated synthesis of CoFe(2)O(4) nanocrystals in vitro. We have covalently attached the full-length mms6 protein and a synthetic C-terminal domain of mms6 protein to self-assembling polymers in order to template hierarchical CoFe(2)O(4) nanostructures. This new synthesis pathway enables facile room-temperature shape-specific synthesis of complex magnetic crystalline nanomaterials with particle sizes in the range of 40-100 nm that are difficult to produce using conventional techniques.

A dual-colored bio-marker made of doped ZnO nanocrystals

NASA Astrophysics Data System (ADS)

Wu, Y. L.; Fu, S.; Tok, A. I. Y.; Zeng, X. T.; Lim, C. S.; Kwek, L. C.; Boey, F. C. Y.

2008-08-01

Bio-compatible ZnO nanocrystals doped with Co, Cu and Ni cations, surface capped with two types of aminosilanes and titania are synthesized by a soft chemical process. Due to the small particle size (2-5 nm), surface functional groups and the high photoluminescence emissions at the UV and blue-violet wavelength ranges, bio-imaging on human osteosarcoma (Mg-63) cells and histiocytic lymphoma U-937 monocyte cells showed blue emission at the nucleus and bright turquoise emission at the cytoplasm simultaneously. This is the first report on dual-color bio-images labeled by one semiconductor nanocrystal colloidal solution. Bright green emission was detected on mung bean seedlings labeled by all the synthesized ZnO nanocrystals. Cytotoxicity tests showed that the aminosilanes capped nanoparticles are non-toxic. Quantum yields of the nanocrystals varied from 79% to 95%. The results showed the potential of the pure ZnO and Co-doped ZnO nanocrystals for live imaging of both human cells and plant systems.

A wearable multiplexed silicon nonvolatile memory array using nanocrystal charge confinement

PubMed Central

Kim, Jaemin; Son, Donghee; Lee, Mincheol; Song, Changyeong; Song, Jun-Kyul; Koo, Ja Hoon; Lee, Dong Jun; Shim, Hyung Joon; Kim, Ji Hoon; Lee, Minbaek; Hyeon, Taeghwan; Kim, Dae-Hyeong

2016-01-01

Strategies for efficient charge confinement in nanocrystal floating gates to realize high-performance memory devices have been investigated intensively. However, few studies have reported nanoscale experimental validations of charge confinement in closely packed uniform nanocrystals and related device performance characterization. Furthermore, the system-level integration of the resulting devices with wearable silicon electronics has not yet been realized. We introduce a wearable, fully multiplexed silicon nonvolatile memory array with nanocrystal floating gates. The nanocrystal monolayer is assembled over a large area using the Langmuir-Blodgett method. Efficient particle-level charge confinement is verified with the modified atomic force microscopy technique. Uniform nanocrystal charge traps evidently improve the memory window margin and retention performance. Furthermore, the multiplexing of memory devices in conjunction with the amplification of sensor signals based on ultrathin silicon nanomembrane circuits in stretchable layouts enables wearable healthcare applications such as long-term data storage of monitored heart rates. PMID:26763827

Hypervalent surface interactions for colloidal stability and doping of silicon nanocrystals

PubMed Central

Wheeler, Lance M.; Neale, Nathan R.; Chen, Ting; Kortshagen, Uwe R.

2013-01-01

Colloidal semiconductor nanocrystals have attracted attention for cost-effective, solution-based deposition of quantum-confined thin films for optoelectronics. However, two significant challenges must be addressed before practical nanocrystal-based devices can be realized. The first is coping with the ligands that terminate the nanocrystal surfaces. Though ligands provide the colloidal stability needed to cast thin films from solution, these ligands dramatically hinder charge carrier transport in the resulting film. Second, after a conductive film is achieved, doping has proven difficult for further control of the optoelectronic properties of the film. Here we report the ability to confront both of these challenges by exploiting the ability of silicon to engage in hypervalent interactions with hard donor molecules. For the first time, we demonstrate the significant potential of applying the interaction to the nanocrystal surface. In this study, hypervalent interactions are shown to provide colloidal stability as well as doping of silicon nanocrystals. PMID:23893292

Structure refinement for tantalum nitrides nanocrystals with various morphologies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Lianyun; School of Science, Beijing Jiaotong University, 3 Shang Yuan Cun, Haidian District, Beijing 100044; Huang, Kai

2012-07-15

Graphical abstract: Tantalum nitrides nanocrystals with various phases and morphologies for the first time have been synthesized through homogenous sodium reduction under low temperature with the subsequent annealing process under high vacuum. Highlights: ► The spherical TaN, cuboidal TaN{sub 0.83} and TaN{sub 0.5} nanocrystals have been synthesized through homogenous sodium reduction under low temperature with the subsequent annealing process under high vacuum. ► The crystal structures of different tantalum nitrides were determined by Rietveld refinement on the X-ray diffraction data and the examinations of electron microcopies. ► The specific surface area of the tantalum nitrides powders was around 10 m{supmore » 2} g{sup −1}. ► Tantalum nitrides powders could be suitable for capacitor with high specific capacitance. -- Abstract: Tantalum nitrides (TaN{sub x}) nanocrystals with different phase and morphology have been synthesized through homogenous sodium reduction under low temperature with the subsequent annealing process under high vacuum. The crystal structures of tantalum nitrides were determined by Rietveld refinement based on the X-ray diffraction data. The morphologies of various tantalum nitrides nanocrystals in high quality were analyzed through the electron microcopies examinations. The spherical TaN nanoparticles, cuboidal TaN{sub 0.83} and TaN{sub 0.5} nanocrystals have been selectively prepared at different annealing temperatures. In addition, the specific surface areas of the tantalum nitrides nanocrystals measured by BET method were around 9.87–11.64 m{sup 2} g{sup −1}, indicating that such nano-sized tantalum nitrides could be suitable for capacitor with high specific capacitance.« less

Size-tunable phosphorescence in colloidal metastable gamma-Ga2O3 nanocrystals.

PubMed

Wang, Ting; Farvid, Shokouh S; Abulikemu, Mutalifu; Radovanovic, Pavle V

2010-07-14

We report a colloidal synthesis of gallium oxide (Ga(2)O(3)) nanocrystals having metastable cubic crystal structure (gamma phase) and uniform size distribution. Using the synthesized nanocrystal size series we demonstrate for the first time a size-tunable photoluminescence in Ga(2)O(3) from ultraviolet to blue, with the emission shifting to lower energies with increasing nanocrystal size. The observed photoluminescence is dominated by defect-based donor-acceptor pair recombination and has a lifetime of several milliseconds. Importantly, the decay of this phosphorescence is also size dependent. The phosphorescence energy and the decay rate increase with decreasing nanocrystal size, owing to a reduced donor-acceptor separation. These results allow for a rational and predictable tuning of the optical properties of this technologically important material and demonstrate the possibility of manipulating the localized defect interactions via nanocrystal size. Furthermore, the same defect states, particularly donors, are also implicated in electrical conductivity rendering monodispersed Ga(2)O(3) nanocrystals a promising material for multifunctional optoelectronic structures and devices.

Tuning the Magnetic Properties of Metal Oxide Nanocrystal Heterostructures by Cation Exchange

PubMed Central

2013-01-01

For three types of colloidal magnetic nanocrystals, we demonstrate that postsynthetic cation exchange enables tuning of the nanocrystal’s magnetic properties and achieving characteristics not obtainable by conventional synthetic routes. While the cation exchange procedure, performed in solution phase approach, was restricted so far to chalcogenide based semiconductor nanocrystals, here ferrite-based nanocrystals were subjected to a Fe2+ to Co2+ cation exchange procedure. This allows tracing of the compositional modifications by systematic and detailed magnetic characterization. In homogeneous magnetite nanocrystals and in gold/magnetite core shell nanocrystals the cation exchange increases the coercivity field, the remanence magnetization, as well as the superparamagnetic blocking temperature. For core/shell nanoheterostructures a selective doping of either the shell or predominantly of the core with Co2+ is demonstrated. By applying the cation exchange to FeO/CoFe2O4 core/shell nanocrystals the Neél temperature of the core material is increased and exchange-bias effects are enhanced so that vertical shifts of the hysteresis loops are obtained which are superior to those in any other system. PMID:23362940

Colloidal chemical synthesis and formation kinetics of uniformly sized nanocrystals of metals, oxides, and chalcogenides.

PubMed

Kwon, Soon Gu; Hyeon, Taeghwan

2008-12-01

Nanocrystals exhibit interesting electrical, optical, magnetic, and chemical properties not achieved by their bulk counterparts. Consequently, to fully exploit the potential of nanocrystals, the synthesis of nanocrystals must focus on producing materials with uniform size and shape. Top-down physical processes can produce large quantities of nanocrystals, but controlling the size is difficult with these methods. On the other hand, colloidal chemical synthetic methods can produce uniform nanocrystals with a controlled particle size. In this Account, we present our synthesis of uniform nanocrystals of various shapes and materials, and we discuss the kinetics of nanocrystal formation. We employed four different synthetic approaches including thermal decomposition, nonhydrolytic sol-gel reactions, thermal reduction, and use of reactive chalcogen reagents. We synthesized uniform oxide nanocrystals via heat-up methods. This method involved slowly heat-up reaction mixtures composed of metal precursors, surfactants, and solvents from room temperature to high temperature. We then held reaction mixtures at an aging temperature for a few minutes to a few hours. Kinetics studies revealed a three-step mechanism for the synthesis of nanocrystals through the heat-up method with size distribution control. First, as metal precursors thermally decompose, monomers accumulate. At the aging temperature, burst nucleation occurs rapidly; at the end of this second phase, nucleation stops, but continued diffusion-controlled growth leads to size focusing to produce uniform nanocrystals. We used nonhydrolytic sol-gel reactions to synthesize various transition metal oxide nanocrystals. We employed ester elimination reactions for the synthesis of ZnO and TiO(2) nanocrystals. Uniform Pd nanoparticles were synthesized via a thermal reduction reaction induced by heating up a mixture of Pd(acac)(2), tri-n-octylphosphine, and oleylamine to the aging temperature. Similarly, we synthesized

Controlled Chemical Doping of Semiconductor Nanocrystals Using Redox Buffers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Engel, Jesse H.; Surendranath, Yogesh; Alivisatos, Paul

Semiconductor nanocrystal solids are attractive materials for active layers in next-generation optoelectronic devices; however, their efficient implementation has been impeded by the lack of precise control over dopant concentrations. Herein we demonstrate a chemical strategy for the controlled doping of nanocrystal solids under equilibrium conditions. Exposing lead selenide nanocrystal thin films to solutions containing varying proportions of decamethylferrocene and decamethylferrocenium incrementally and reversibly increased the carrier concentration in the solid by 2 orders of magnitude from their native values. This application of redox buffers for controlled doping provides a new method for the precise control of the majority carrier concentrationmore » in porous semiconductor thin films.« less

Supramolecular Assembly of Single-Source Metal-Chalcogenide Nanocrystal Precursors.

PubMed

Smith, Stephanie C; Bryks, Whitney; Tao, Andrea R

2018-05-28

In this Feature Article, we discuss our recent work in the synthesis of novel supramolecular precursors for semiconductor nanocrystals. Metal chalcogenolates that adopt liquid crystalline phases are employed as single-source precursors that template the growth of shaped solid-state nanocrystals. Supramolecular assembly is programmed by both precursor chemical composition and molecular parameters such alkyl chain length, steric bulk, and the intercalation of halide ions. Here, we explore the various design principles that enable the rational synthesis of these single-source precursors, their liquid crystalline phases, and the various semiconductor nanocrystal products that can be generated by thermolysis, ranging from highly anisotropic two-dimensional nanosheets and nanodisks to spheres.

Cloning nanocrystal morphology with soft templates

NASA Astrophysics Data System (ADS)

Thapa, Dev Kumar; Pandey, Anshu

2016-08-01

In most template directed preparative methods, while the template decides the nanostructure morphology, the structure of the template itself is a non-general outcome of its peculiar chemistry. Here we demonstrate a template mediated synthesis that overcomes this deficiency. This synthesis involves overgrowth of silica template onto a sacrificial nanocrystal. Such templates are used to copy the morphologies of gold nanorods. After template overgrowth, gold is removed and silver is regrown in the template cavity to produce a single crystal silver nanorod. This technique allows for duplicating existing nanocrystals, while also providing a quantifiable breakdown of the structure - shape interdependence.

Optimizing the Ar-Xe infrared laser on the Naval Research Laboratory's Electra generator

DOE Office of Scientific and Technical Information (OSTI.GOV)

Apruzese, J. P.; Giuliani, J. L.; Wolford, M. F.

2008-07-01

The Ar-Xe infrared laser has been investigated in several series of experiments carried out on the Naval Research Laboratory's Electra generator. Our primary goals were to optimize the efficiency of the laser (within Electra's capabilities) and to gain understanding of the main physical processes underlying the laser's output as a function of controllable parameters such as Xe fraction, power deposition, and gas pressure. We find that the intrinsic efficiency maximizes at {approx}3% at a total pressure of 2.5 atm, Xe fraction of 1%, and electron beam power deposition density of 50-100 kW cm{sup -3}. We deployed an interferometer to measuremore » the electron density during lasing; the ionization fractions of 10{sup -5}-10{sup -4} that it detected well exceed previous theoretical estimates. Some trends in the data as a function of beam power and xenon fraction are not fully understood. The as-yet incomplete picture of Ar-Xe laser physics is likely traceable in large part to significant uncertainties still present in many important rates influencing the atomic and molecular kinetics.« less

Electron tomography and 3D molecular simulations of platinum nanocrystals

NASA Astrophysics Data System (ADS)

Florea, Ileana; Demortière, Arnaud; Petit, Christophe; Bulou, Hervé; Hirlimann, Charles; Ersen, Ovidiu

2012-07-01

This work reports on the morphology of individual platinum nanocrystals with sizes of about 5 nm. By using the electron tomography technique that gives 3D spatial selectivity, access to quantitative information in the real space was obtained. The morphology of individual nanoparticles was characterized using HAADF-STEM tomography and it was shown to be close to a truncated octahedron. Using molecular dynamics simulations, this geometrical shape was found to be the one minimizing the nanocrystal energy. Starting from the tomographic reconstruction, 3D crystallographic representations of the studied Pt nanocrystals were obtained at the nanometer scale, allowing the quantification of the relative amount of the crystallographic facets present on the particle surface.This work reports on the morphology of individual platinum nanocrystals with sizes of about 5 nm. By using the electron tomography technique that gives 3D spatial selectivity, access to quantitative information in the real space was obtained. The morphology of individual nanoparticles was characterized using HAADF-STEM tomography and it was shown to be close to a truncated octahedron. Using molecular dynamics simulations, this geometrical shape was found to be the one minimizing the nanocrystal energy. Starting from the tomographic reconstruction, 3D crystallographic representations of the studied Pt nanocrystals were obtained at the nanometer scale, allowing the quantification of the relative amount of the crystallographic facets present on the particle surface. Electronic supplementary information (ESI) available. See DOI: 10.1039/c2nr30990d

Precision Penning Trap Mass Spectrometry of S, Kr and Xe

NASA Astrophysics Data System (ADS)

Redshaw, Matthew

2005-04-01

Using a phase coherent technique to measure the cyclotron frequency of single ions in a Penning trap [1], we have performed mass measurements on ^32S and the two most abundant krypton and xenon isotopes ^84Kr, ^86Kr, ^ 129Xe and ^132Xe, to relative precisions of 0.1 ppb. This is a factor of ˜10-100 improvement in precision over current values [2]. [1] M.P. Bradley, J.V. Porto, S. Rainville, J.K. Thompson, and D.E. Pritchard, PRL 83, 4510 (1999). [2] G. Audi, A.H. Wapstra, and C. Thibault, Nucl Phys A729, 337 (2003).

XE991 and Linopirdine Are State-Dependent Inhibitors for Kv7/KCNQ Channels that Favor Activated Single Subunits.

PubMed

Greene, Derek L; Kang, Seungwoo; Hoshi, Naoto

2017-07-01

M-channel inhibitors, especially XE991, are being used increasingly in animal experiments; however, insufficient characterization of XE991 at times confounds the interpretation of results when using this compound. Here, we demonstrate that XE991 and linopirdine are state-dependent inhibitors that favor the activated-subunit of neuronal Kv7/KCNQ channels. We performed patch-clamp experiments on homomeric Kv7.2 or heteromeric Kv7.2/3 channels expressed in Chinese hamster ovary cells to characterize XE991 and linopirdine. Neither inhibitor was efficacious around the resting membrane potential of cells in physiologic conditions. Inhibition of Kv7.2 and Kv7.2/3 channels by XE991 was closely related with channel activation. When the voltage dependence of activation was left-shifted by retigabine or right-shifted by the mutation, Kv7.2(R214D), the shift in half-activation voltage proportionally coincided with the shift in the half-effective potential for XE991 inhibition. Inhibition kinetics during XE991 wash-in was facilitated at depolarized potentials. Ten-minute washout of XE991 resulted in ∼30% current recovery, most of which was attributed to surface transport of Kv7.2 channels. Linopirdine also exhibited similar inhibition characteristics, with the exception of near- complete current recovery after washout at depolarized potentials. Inhibition kinetics of both XE991 and linopirdine was not as sensitive to changes in voltage as would be predicted by open- channel inhibition. Instead, they were well explained by binding to a single activated subunit. The characteristics of XE991 and linopirdine should be taken into account when these M-channel inhibitors are used in experiments. Copyright © 2017 by The American Society for Pharmacology and Experimental Therapeutics.

Preparation and characterization of potato starch nanocrystal reinforced natural rubber nanocomposites.

PubMed

Rajisha, K R; Maria, H J; Pothan, L A; Ahmad, Zakiah; Thomas, S

2014-06-01

Potato starch nanocrystals were found to serve as an effective reinforcing agent for natural rubber (NR). Starch nanocrystals were obtained by the sulfuric acid hydrolysis of potato starch granules. After mixing the latex and the starch nanocrystals, the resulting aqueous suspension was cast into film by solvent evaporation method. The composite samples were successfully prepared by varying filler loadings, using a colloidal suspension of starch nanocrystals and NR latex. The morphology of the nanocomposite prepared was analyzed by field emission scanning electron microscopy (FESEM) and transmission electron microscopy (TEM). FESEM analysis revealed the size and shape of the crystal and their homogeneous dispersion in the composites. The crystallinity of the nanocomposites was studied using XRD analysis which indicated an overall increase in crystallinity with filler content. The mechanical properties of the nanocomposites such as stress-strain behavior, tensile strength, tensile modulus and elongation at break were measured according to ASTM standards. The tensile strength and modulus of the composites were found to improve tremendously with increasing nanocrystal content. This dramatic increase observed can be attributed to the formation of starch nanocrystal network. This network immobilizes the polymer chains leading to an increase in the modulus and other mechanical properties. Copyright © 2014 Elsevier B.V. All rights reserved.

Role of the inversion layer on the charge injection in silicon nanocrystal multilayered light emitting devices

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tondini, S.; Dipartimento di Fisica, Informatica e Matematica, Università di Modena e Reggio Emilia, Via Campi 213/a, 41125 Modena; Pucker, G.

2016-09-07

The role of the inversion layer on injection and recombination phenomena in light emitting diodes (LEDs) is here studied on a multilayer (ML) structure of silicon nanocrystals (Si-NCs) embedded in SiO{sub 2}. Two Si-NC LEDs, which are similar for the active material but different in the fabrication process, elucidate the role of the non-radiative recombination rates at the ML/substrate interface. By studying current- and capacitance-voltage characteristics as well as electroluminescence spectra and time-resolved electroluminescence under pulsed and alternating bias pumping scheme in both the devices, we are able to ascribe the different experimental results to an efficient or inefficient minoritymore » carrier (electron) supply by the p-type substrate in the metal oxide semiconductor LEDs.« less

Improvement of Polylactide Properties through Cellulose Nanocrystals Embedded in Poly(Vinyl Alcohol) Electrospun Nanofibers.

PubMed

López de Dicastillo, Carol; Garrido, Luan; Alvarado, Nancy; Romero, Julio; Palma, Juan Luis; Galotto, Maria Jose

2017-05-11

Electrospun nanofibers of poly (vinyl alcohol) (PV) were obtained to improve dispersion of cellulose nanocrystals (CNC) within hydrophobic biopolymeric matrices, such as poly(lactic acid) (PLA). Electrospun nanofibers (PV/CNC) n were successfully obtained with a final concentration of 23% ( w / w ) of CNC. Morphological, structural and thermal properties of developed CNC and electrospun nanofibers were characterized. X-ray diffraction and thermal analysis revealed that the crystallinity of PV was reduced by the electrospinning process, and the incorporation of CNC increased the thermal stability of biodegradable nanofibers. Interactions between CNC and PV polymer also enhanced the thermal stability of CNC and improved the dispersion of CNC within the PLA matrix. PLA materials with CNC lyophilized were also casted in order to compare the properties with materials based on CNC containing nanofibers. Nanofibers and CNC were incorporated into PLA at three concentrations: 0.5%, 1% and 3% (CNC respect to polymer weight) and nanocomposites were fully characterized. Overall, nanofibers containing CNC positively modified the physical properties of PLA materials, such as the crystallinity degree of PLA which was greatly enhanced. Specifically, materials with 1% nanofiber 1PLA(PV/CNC) n presented highest improvements related to mechanical and barrier properties; elongation at break was enhanced almost four times and the permeation of oxygen was reduced by approximately 30%.

Improvement of Polylactide Properties through Cellulose Nanocrystals Embedded in Poly(Vinyl Alcohol) Electrospun Nanofibers

PubMed Central

López de Dicastillo, Carol; Garrido, Luan; Alvarado, Nancy; Romero, Julio; Palma, Juan Luis; Galotto, Maria Jose

2017-01-01

Electrospun nanofibers of poly (vinyl alcohol) (PV) were obtained to improve dispersion of cellulose nanocrystals (CNC) within hydrophobic biopolymeric matrices, such as poly(lactic acid) (PLA). Electrospun nanofibers (PV/CNC)n were successfully obtained with a final concentration of 23% (w/w) of CNC. Morphological, structural and thermal properties of developed CNC and electrospun nanofibers were characterized. X-ray diffraction and thermal analysis revealed that the crystallinity of PV was reduced by the electrospinning process, and the incorporation of CNC increased the thermal stability of biodegradable nanofibers. Interactions between CNC and PV polymer also enhanced the thermal stability of CNC and improved the dispersion of CNC within the PLA matrix. PLA materials with CNC lyophilized were also casted in order to compare the properties with materials based on CNC containing nanofibers. Nanofibers and CNC were incorporated into PLA at three concentrations: 0.5%, 1% and 3% (CNC respect to polymer weight) and nanocomposites were fully characterized. Overall, nanofibers containing CNC positively modified the physical properties of PLA materials, such as the crystallinity degree of PLA which was greatly enhanced. Specifically, materials with 1% nanofiber 1PLA(PV/CNC)n presented highest improvements related to mechanical and barrier properties; elongation at break was enhanced almost four times and the permeation of oxygen was reduced by approximately 30%. PMID:28492470

Enhanced Luminescent Stability through Particle Interactions in Silicon Nanocrystal Aggregates

DOE Office of Scientific and Technical Information (OSTI.GOV)

Miller, Joseph B.; Dandu, Naveen; Velizhanin, Kirill A.

2015-10-27

Close-packed assemblies of ligand-passivated colloidal nanocrystals can exhibit enhanced photoluminescent stability, but the origin of this effect is unclear. Here, we use experiment, simulation, and ab initio computation to examine the influence of interparticle interactions on the photoluminescent stability of silicon nanocrystal aggregates. The time-dependent photoluminescence emitted by structures ranging in size from a single quantum dot to agglomerates of more than a thousand is compared with Monte Carlo simulations of noninteracting ensembles using measured single-particle blinking data as input. In contrast to the behavior typically exhibited by the metal chalcogenides, the measured photoluminescent stability shows an enhancement with respectmore » to the noninteracting scenario with increasing aggregate size. We model this behavior using time-dependent density functional theory calculations of energy transfer between neighboring nanocrystals as a function of nanocrystal size, separation, and the presence of charge and/or surface-passivation defects. Our results suggest that rapid exciton transfer from “bright” nanocrystals to surface trap states in nearest-neighbors can efficiently fill such traps and enhance the stability of emission by promoting the radiative recombination of slowly diffusing excited electrons.« less

Microstructure investigations of U3Si2 implanted by high-energy Xe ions at 600 °C

NASA Astrophysics Data System (ADS)

Miao, Yinbin; Harp, Jason; Mo, Kun; Kim, Yeon Soo; Zhu, Shaofei; Yacout, Abdellatif M.

2018-05-01

The microstructure investigations on a high-energy Xe-implanted U3Si2 pellet were performed. The promising accident tolerant fuel (ATF) candidate, U3Si2, was irradiated by 84 MeV Xe ions at 600 °C at Argonne Tandem Linac Accelerator System (ATLAS). The characterizations of the Xe implanted sample were conducted using advanced transmission electron microscopy (TEM) techniques. An oxidation layer was observed on the sample surface after irradiation under the ∼10-5 Pa vacuum. The study on the oxidation layer not only unveils the readily oxidation behavior of U3Si2 under high-temperature irradiation conditions, but also develops an understanding of its oxidation mechanism. Intragranular Xe bubbles with bimodal size distribution were observed within the Xe deposition region of the sample induced by 84 MeV Xe ion implantation. At the irradiation temperature of 600 °C, the gaseous swelling strain contributed by intragranular bubbles was found to be insignificant, indicating an acceptable fission gas behavior of U3Si2 as a light water reactor (LWR) fuel operating at such a temperature.

Crystallization Methods for Preparation of Nanocrystals for Drug Delivery System.

PubMed

Gao, Yuan; Wang, Jingkang; Wang, Yongli; Yin, Qiuxiang; Glennon, Brian; Zhong, Jian; Ouyang, Jinbo; Huang, Xin; Hao, Hongxun

2015-01-01

Low water solubility of drug products causes delivery problems such as low bioavailability. The reduced particle size and increased surface area of nanocrystals lead to the increasing of the dissolution rate. The formulation of drug nanocrystals is a robust approach and has been widely applied to drug delivery system (DDS) due to the significant development of nanoscience and nanotechnology. It can be used to improve drug efficacy, provide targeted delivery and minimize side-effects. Crystallization is the main and efficient unit operation to produce nanocrystals. Both traditional crystallization methods such as reactive crystallization, anti-solvent crystallization and new crystallization methods such as supercritical fluid crystallization, high-gravity controlled precipitation can be used to produce nanocrystals. The current mini-review outlines the main crystallization methods addressed in literature. The advantages and disadvantages of each method were summarized and compared.

Capping Ligand Vortices as "Atomic Orbitals" in Nanocrystal Self-Assembly.

PubMed

Waltmann, Curt; Horst, Nathan; Travesset, Alex

2017-11-28

We present a detailed analysis of the interaction between two nanocrystals capped with ligands consisting of hydrocarbon chains by united atom molecular dynamics simulations. We show that the bonding of two nanocrystals is characterized by ligand textures in the form of vortices. These results are generalized to nanocrystals of different types (differing core and ligand sizes) where the structure of the vortices depends on the softness asymmetry. We provide rigorous calculations for the binding free energy, show that these energies are independent of the chemical composition of the cores, and derive analytical formulas for the equilibrium separation. We discuss the implications of our results for the self-assembly of single-component and binary nanoparticle superlattices. Overall, our results show that the structure of the ligands completely determines the bonding of nanocrystals, fully supporting the predictions of the recently proposed Orbifold topological model.

Ligand exchange in quaternary alloyed nanocrystals--a spectroscopic study.

PubMed

Gabka, Grzegorz; Bujak, Piotr; Giedyk, Kamila; Kotwica, Kamil; Ostrowski, Andrzej; Malinowska, Karolina; Lisowski, Wojciech; Sobczak, Janusz W; Pron, Adam

2014-11-14

Exchange of initial, predominantly stearate ligands for pyridine in the first step and butylamine (BA) or 11-mercaptoundecanoic acid (MUA) in the second one was studied for alloyed quaternary Cu-In-Zn-S nanocrystals. The NMR results enabled us to demonstrate, for the first time, direct binding of the pyridine labile ligand to the nanocrystal surface as evidenced by paramagnetic shifts of the three signals attributed to its protons to 7.58, 7.95 and 8.75 ppm. XPS investigations indicated, in turn, a significant change in the composition of the nanocrystal surface upon the exchange of initial ligands for pyridine, which being enriched in indium in the 'as prepared' form became enriched in zinc after pyridine binding. This finding indicated that the first step of ligand exchange had to involve the removal of the surface layer enriched in indium with simultaneous exposure of a new, zinc-enriched layer. In the second ligand exchange step (replacement of pyridine with BA or MUA) the changes in the nanocrystal surface compositions were much less significant. The presence of zinc in the nanocrystal surface layer turned out necessary for effective binding of pyridine as shown by a comparative study of ligand exchange in Cu-In-Zn-S, Ag-In-Zn-S and CuInS2, carried out by complementary XPS and NMR investigations.

A Radiation-Tolerant, Low-Power Non-Volatile Memory Based on Silicon Nanocrystal Quantum Dots

NASA Technical Reports Server (NTRS)

Bell, L. D.; Boer, E. A.; Ostraat, M. L.; Brongersma, M. L.; Flagan, R. C.; Atwater, H. A.; deBlauwe, J.; Green, M. L.

2001-01-01

Nanocrystal nonvolatile floating-gate memories are a good candidate for space applications - initial results suggest they are fast, more reliable and consume less power than conventional floating gate memories. In the nanocrystal based NVM device, charge is not stored on a continuous polysilicon layer (so-called floating gate), but instead on a layer of discrete nanocrystals. Charge injection and storage in dense arrays of silicon nanocrystals in SiO2 is a critical aspect of the performance of potential nanocrystal flash memory structures. The ultimate goal for this class of devices is few- or single-electron storage in a small number of nanocrystal elements. In addition, the nanocrystal layer fabrication technique should be simple, 8-inch wafer compatible and well controlled in program/erase threshold voltage swing was seen during 100,000 program and erase cycles. Additional near-term goals for this project include extensive testing for radiation hardness and the development of artificial layered tunnel barrier heterostructures which have the potential for large speed enhancements for read/write of nanocrystal memory elements, compared with conventional flash devices. Additional information is contained in the original extended abstract.

Fundamental absorption edge of NiO nanocrystals

NASA Astrophysics Data System (ADS)

Sokolov, V. I.; Druzhinin, A. V.; Kim, G. A.; Gruzdev, N. B.; Yermakov, A. Ye.; Uimin, M. A.; Byzov, I. V.; Shchegoleva, N. N.; Vykhodets, V. B.; Kurennykh, T. E.

2013-12-01

NiO nanocrystals with the average size of 5, 10 and 25 nm were synthesized by gas-condensation method. The well-defined increase of the optical density D near the fundamental absorption edge of NiO nanocrystals in the range of 3.5-4.0 eV observed after the annealing in air is caused by the oxygen content growth. It is the direct experimental evidence of the fact that p-d charge transfer transitions form the fundamental absorption edge.

Surface states in the photoionization of high-quality CdSe core/shell nanocrystals.

PubMed

Li, Shu; Steigerwald, Michael L; Brus, Louis E

2009-05-26

We use electric force microscopy (EFM) to study single nanocrystal photoionization in two classes of high-quality nanocrystals whose exciton luminescence quantum yields approach unity in solution. The CdSe/CdS/ZnS core/shell nanocrystals do not photoionize, while the CdSe/CdS nanocrystals do show substantial photoionization. This verifies the theoretical prediction that the ZnS shell confines the excited electron within the nanocrystal. Despite the high luminescence quantum yield, photoionization varies substantially among the CdSe/CdS nanocrystals. We have studied the nanocrystal photoionization with both UV (396 nm) and green (532 nm) light, and we have found that the magnitude of the charge due to photoionization per absorbed photon is greater for UV excitation than for green excitation. A fraction of the photoionization occurs directly via a "hot electron" process, using trap states that are either on the particle surface, within the ligand sphere, or within the silicon oxide layer. This must occur without relaxation to the thermalized, lowest-energy, emitting exciton. We discuss the occurrence of hot carrier processes that are common to photoionization, luminescence blinking, and the fast transient optical absorption that is associated with multiple exciton generation MEG studies.

Synthesis and characterization of luminescent aluminium selenide nanocrystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Balitskii, O.A., E-mail: balitskii@electronics.wups.lviv.ua; Demchenko, P.Yu.; Mijowska, E.

Highlights: ► Synthesis procedure of size and sharp controlled Al{sub 2}Se{sub 3} nanocrystals is introduced. ► Obtained nanoparticles are highly crystalline of hexagonal wurtzite type. ► Colloidal Al{sub 2}Se{sub 3} nanocrystals are highly luminescent in the near UV spectral region. ► They can be implemented in light emitters/collectors, concurring with II–VI nanodots. -- Abstract: We propose the synthesis and characterization of colloidal aluminium selenide nanocrystals using trioctylphosphine as a solvent. The nanoparticles have several absorption bands in the spectral region 330–410 nm and are bright UV-blue luminescent, which is well demanded in light collecting and emitting devices, e.g. for tuningmore » their spectral characteristics to higher energy solar photons.« less

Effects of PEGylated paclitaxel nanocrystals on breast cancer and its lung metastasis

NASA Astrophysics Data System (ADS)

Zhang, Hua; Hu, Hongxiang; Zhang, Haoran; Dai, Wenbing; Wang, Xinglin; Wang, Xueqing; Zhang, Qiang

2015-06-01

As an attractive strategy developed rapidly in recent years, nanocrystals are used to deliver insoluble drugs. PEGylation may further prolong the circulation time of nanoparticles and improve the therapeutic outcome of drugs. In this study, paclitaxel (PTX) nanocrystals (PTX-NCs) and PEGylated PTX nanocrystals (PEG-PTX-NCs) were prepared using antisolvent precipitation augmented by probe sonication. The characteristics and antitumor efficacy of nanocrystals were investigated. The results indicated that the nanocrystals showed rod-like morphology, and the average particle size was 240 nm and 330 nm for PTX-NCs and PEG-PTX-NCs, respectively. The PEG molecules covered the surface of nanocrystals with an 11.54 nm fixed aqueous layer thickness (FALT), much higher than that of PTX-NCs (0.2 nm). PEG-PTX-NCs showed higher stability than PTX-NCs under both storage and physiological conditions. In breast cancer xenografted mice, PEG-PTX-NCs showed significantly better tumor inhibition compared to saline (p < 0.001) and PTX-NC groups (p < 0.05) after intravenous administration. In a model of lung tumor metastasis quantified by the luciferase activity, the PEG-PTX-NCs group showed higher anticancer efficacy not only than saline and PTX-NCs groups, but also than Taxol®, achieving an 82% reduction at the end of the experiment. These studies suggested the potential advantages of PEGylated PTX nanocrystals as alternative drug delivery systems for anticancer therapy.

Structural phase transitions in niobium oxide nanocrystals

NASA Astrophysics Data System (ADS)

Yuvakkumar, R.; Hong, Sun Ig

2015-09-01

Niobium oxide nanocrystals were successfully synthesized employing the green synthesis method. Phase formation, microstructure and compositional properties of 1, 4 and 7 days incubation treated samples after calcinations at 450 °C were examined using X-ray diffraction, Raman, photoluminescence (PL), infrared, X-ray photoelectron spectra and transmission electron microscopic characterizations. It was observed that phase formation of Nb2O5 nanocrystals was dependent upon the incubation period required to form stable metal oxides. The characteristic results clearly revealed that with increasing incubation and aging, the transformation of cubic, orthorhombic and monoclinic phases were observed. The uniform heating at room temperature (32 °C) and the ligation of niobium atoms due to higher phenolic constituents of utilized rambutan during aging processing plays a vital role in structural phase transitions in niobium oxide nanocrystals. The defects over a period of incubation and the intensities of the PL spectra changing over a period of aging were related to the amount of the defects induced by the phase transition.

Morphology evolution of single-crystalline hematite nanocrystals: magnetically recoverable nanocatalysts for enhanced facet-driven photoredox activity

NASA Astrophysics Data System (ADS)

Patra, Astam K.; Kundu, Sudipta K.; Bhaumik, Asim; Kim, Dukjoon

2015-12-01

We have developed a new green chemical approach for the shape-controlled synthesis of single-crystalline hematite nanocrystals in aqueous medium. FESEM, HRTEM and SAED techniques were used to determine the morphology and crystallographic orientations of each nanocrystal and its exposed facets. PXRD and HRTEM techniques revealed that the nanocrystals are single crystalline in nature; twins and stacking faults were not detected in these nanocrystals. The structural, vibrational, and electronic spectra of these nanocrystals were highly dependent on their shape. Different shaped hematite nanocrystals with distinct crystallographic planes have been synthesized under similar reaction conditions, which can be desired as a model for the purpose of properties comparison with the nanocrystals prepared under different reaction conditions. Here we investigated the photocatalytic performance of these different shaped-nanocrystals for methyl orange degradation in the presence of white light (λ > 420 nm). In this study, we found that the density of surface Fe3+ ions in particular facets was the key factor for the photocatalytic activity and was higher on the bitruncated-dodecahedron shape nanocrystals by coexposed {104}, {100} and {001} facets, attributing to higher catalytic activity. The catalytic activity of different exposed facet nanocrystals were as follows: {104} + {100} + {001} (bitruncated-dodecahedron) > {101} + {001} (bitruncated-octahedron) > {001} + {110} (nanorods) > {012} (nanocuboid) which provided the direct evidence of exposed facet-driven photocatalytic activity. The nanocrystals were easily recoverable using an external magnet and reused at least six times without significant loss of its catalytic activity.We have developed a new green chemical approach for the shape-controlled synthesis of single-crystalline hematite nanocrystals in aqueous medium. FESEM, HRTEM and SAED techniques were used to determine the morphology and crystallographic orientations of

Kinetic analysis of rare gas metastable production and optically pumped Xe lasers

NASA Astrophysics Data System (ADS)

Demyanov, A. V.; Kochetov, I. V.; Mikheyev, P. A.; Azyazov, V. N.; Heaven, M. C.

2018-01-01

Optically pumped all-rare-gas lasers use metastable rare gas atoms as the lasing species in mixtures with He or Ar buffer gas. The metastables are generated in a glow discharge, and we report model calculations for the optimal production of Ne*, Ar*, Kr* and Xe*. Discharge efficiency was estimated by solving the Boltzmann equation. Laser efficiency, gain and output power of the CW optically pumped Xe laser were assessed as functions of heavier rare gas content, pressure, optical pump intensity and the optical path length. It was found that, for efficient operation the heavier rare gas content has to be of the order of one percent or less, and the total pressure—in the range 0.3-1.5 atm. Output power and specific discharge power increase approximately linearly with pump intensity over the output range from 300-500 W cm-2. Ternary mixtures Xe:Ar:He were found to be the most promising. Total laser efficiency was found to be nearly the same for pumping the 2p8 or 2p9 state, reaching 61%-70% for a pump intensity of ~720 W cm-2 when the Xe fraction was in the range 0.001 ÷ 0.01 and Ar fraction—0.1 ÷ 0.5. However, when the 2p8 state was pumped, the maximum total efficiency occurred at larger pressures than for pumping of the 2p9 state. The discharge power density required to sustain a sufficient Xe* number density was in the range of tens of watts per cubic centimeter for 50% Ar in the mixture.

Synthesis and characterization of some metal oxide nanocrystals by microwave irradiation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rashad, M.; Gaber, A.; Abdelrahim, M. A.

2013-12-16

Copper oxide and cobalt oxide (CuO, Co3O4) nanocrystals (NCs) have been successfully prepared in a short time using microwave irradiation. The resulted powders of nanocrystals (NCs) were characterized by X-ray diffraction (XRD) and transmission electron microscopy (TEM). Thermogravimetric analysis (TGA) measurements are also studied. Fourier-transform infrared (FT-IR) and UV–visible absorption spectroscopy of both kind of nanoparticels are illustrated. Optical absorption analysis indicated the direct band gap for both kinds of nanocrystals.

Charge injection and discharging of Si nanocrystals and arrays by atomic force microscopy

NASA Technical Reports Server (NTRS)

Boer, E.; Ostraat, M.; Brongersma, M. L.; Flagan, R. C.; Atwater, H. A.

2000-01-01

Charge injection and storage in dense arrays of silicon nanocrystals in SiO(sub 2) is a critical aspect of the performance of potential nanocrystal flash memory structures. The ultimate goal for this class of devices is few-or single- electron storage in a small number of nanocrystal elements.

The interplay of shape and crystalline anisotropies in plasmonic semiconductor nanocrystals

DOE PAGES

Kim, Jongwook; Agrawal, Ankit; Krieg, Franziska; ...

2016-05-16

Doped semiconductor nanocrystals are an emerging class of materials hosting localized surface plasmon resonance (LSPR) over a wide optical range. Studies so far have focused on tuning LSPR frequency by controlling the dopant and carrier concentrations in diverse semiconductor materials. However, the influence of anisotropic nanocrystal shape and of intrinsic crystal structure on LSPR remain poorly explored. Here, we illustrate how these two factors collaborate to determine LSPR characteristics in hexagonal cesium-doped tungsten oxide nanocrystals. The effect of shape anisotropy is systematically analyzed via synthetic control of nanocrystal aspect ratio (AR), from disks to nanorods. We demonstrate the dominant influencemore » of crystalline anisotropy, which uniquely causes strong LSPR band-splitting into two distinct peaks with comparable intensities. Modeling typically used to rationalize particle shape effects is refined by taking into account the anisotropic dielectric function due to crystalline anisotropy, thus fully accounting for the AR-dependent evolution of multiband LSPR spectra. Furthermore, this new insight into LSPR of semiconductor nanocrystals provides a novel strategy for an exquisite tuning of LSPR line shape.« less

Structural diversity in binary superlattices self-assembled from polymer-grafted nanocrystals

DOE PAGES

Ye, Xingchen; Zhu, Chenhui; Ercius, Peter; ...

2015-12-02

Multicomponent nanocrystal superlattices represent an interesting class of material that derives emergent properties from mesoscale structure, yet their programmability can be limited by the alkyl-chain-based ligands decorating the surfaces of the constituent nanocrystals. Polymeric ligands offer distinct advantages, as they allow for more precise tuning of the effective size and ‘interaction softness’ through changes to the polymer’s molecular weight, chemical nature, architecture, persistence length and surrounding solvent. Here we show the formation of 10 different binary nanocrystal superlattices (BNSLs) with both two- and three-dimensional order through independent adjustment of the core size of spherical nanocrystals and the molecular weight ofmore » densely grafted polystyrene ligands. These polymer-brush-based ligands introduce new energetic contributions to the interparticle potential that stabilizes various BNSL phases across a range of length scales and interparticle spacings. In conclusion, our study opens the door for nanocrystals to become modular elements in the design of functional particle brush solids with controlled nanoscale interfaces and mesostructures.« less

Hyperpolarized (129) Xe imaging of the rat lung using spiral IDEAL.

PubMed

Doganay, Ozkan; Wade, Trevor; Hegarty, Elaine; McKenzie, Charles; Schulte, Rolf F; Santyr, Giles E

2016-08-01

To implement and optimize a single-shot spiral encoding strategy for rapid 2D IDEAL projection imaging of hyperpolarized (Hp) (129) Xe in the gas phase, and in the pulmonary tissue (PT) and red blood cells (RBCs) compartments of the rat lung, respectively. A theoretical and experimental point spread function analysis was used to optimize the spiral k-space read-out time in a phantom. Hp (129) Xe IDEAL images from five healthy rats were used to: (i) optimize flip angles by a Bloch equation analysis using measured kinetics of gas exchange and (ii) investigate the feasibility of the approach to characterize the exchange of Hp (129) Xe. A read-out time equal to approximately 1.8 × T2* was found to provide the best trade-off between spatial resolution and signal-to-noise ratio (SNR). Spiral IDEAL approaches that use the entire dissolved phase magnetization should give an SNR improvement of a factor of approximately three compared with Cartesian approaches with similar spatial resolution. The IDEAL strategy allowed imaging of gas, PT, and RBC compartments with sufficient SNR and temporal resolution to permit regional gas exchange measurements in healthy rats. Single-shot spiral IDEAL imaging of gas, PT and RBC compartments and gas exchange is feasible in rat lung using Hp (129) Xe. Magn Reson Med 76:566-576, 2016. © 2015 Wiley Periodicals, Inc. © 2015 Wiley Periodicals, Inc.

In situ bioinspired synthesis of silver chloride nanocrystals on silk fibroin fibers

NASA Astrophysics Data System (ADS)

Su, Huilan; Han, Jie; Dong, Qun; Xu, Jia; Chen, Ying; Gu, Yu; Song, Weiqiang; Zhang, Di

2011-02-01

Silver chloride (AgCl) nanocrystals were formed and grown on silk fibroin fibers (SFFs) by a room-temperature process. Practically, the degummed SFFs were immersed into silver nitrate solution and sodium chloride solution in turn. The amino acids on the SFF surface were negatively charged in alkaline impregnant, providing locations to immobilize silver ions and form silver chloride seeds. AgCl nanocrystals can further grow into cubic AgCl nanocrystals with an edge of about 100 nm. The morphologies of the AgCl nanocrystals were mostly influenced by the concentration of sodium chloride solution and the special configurations of the SFFs. The target AgCl/SFF nanocomposites constructed by AgCl nanocrystals and substrate SFFs could be used as photocatalysts in water splitting and antibacterial agents. This work provides an important example in the introduction of natural biofibers to the synthesis of functional hybrid nanocomposites by a green and mild technique.

Unravelling the surface chemistry of metal oxide nanocrystals, the role of acids and bases.

PubMed

De Roo, Jonathan; Van den Broeck, Freya; De Keukeleere, Katrien; Martins, José C; Van Driessche, Isabel; Hens, Zeger

2014-07-09

We synthesized HfO2 nanocrystals from HfCl4 using a surfactant-free solvothermal process in benzyl alcohol and found that the resulting nanocrystals could be transferred to nonpolar media using a mixture of carboxylic acids and amines. Using solution (1)H NMR, FTIR, and elemental analysis, we studied the details of the transfer reaction and the surface chemistry of the resulting sterically stabilized nanocrystals. As-synthesized nanocrystals are charge-stabilized by protons, with chloride acting as the counterion. Treatment with only carboxylic acids does not lead to any binding of ligands to the HfO2 surface. On the other hand, we find that the addition of amines provides the basic environment in which carboxylic acids can dissociate and replace chloride. This results in stable, aggregate-free dispersions of HfO2 nanocrystals, sterically stabilized by carboxylate ligands. Moreover, titrations with deuterated carboxylic acid show that the charge on the carboxylate ligands is balanced by coadsorbed protons. Hence, opposite from the X-type/nonstoichiometric nanocrystals picture prevailing in literature, one should look at HfO2/carboxylate nanocrystals as systems where carboxylic acids are dissociatively adsorbed to bind to the nanocrystals. Similar results were obtained with ZrO2 NCs. Since proton accommodation on the surface is most likely due to the high Brønsted basicity of oxygen, our model could be a more general picture for the surface chemistry of metal oxide nanocrystals with important consequences on the chemistry of ligand exchange reactions.

Infrared emitting and photoconducting colloidal silver chalcogenide nanocrystal quantum dots from a silylamide-promoted synthesis.

PubMed

Yarema, Maksym; Pichler, Stefan; Sytnyk, Mykhailo; Seyrkammer, Robert; Lechner, Rainer T; Fritz-Popovski, Gerhard; Jarzab, Dorota; Szendrei, Krisztina; Resel, Roland; Korovyanko, Oleksandra; Loi, Maria Antonietta; Paris, Oskar; Hesser, Günter; Heiss, Wolfgang

2011-05-24

Here, we present a hot injection synthesis of colloidal Ag chalcogenide nanocrystals (Ag(2)Se, Ag(2)Te, and Ag(2)S) that resulted in exceptionally small nanocrystal sizes in the range between 2 and 4 nm. Ag chalcogenide nanocrystals exhibit band gap energies within the near-infrared spectral region, making these materials promising as environmentally benign alternatives to established infrared active nanocrystals containing toxic metals such as Hg, Cd, and Pb. We present Ag(2)Se nanocrystals in detail, giving size-tunable luminescence with quantum yields above 1.7%. The luminescence, with a decay time on the order of 130 ns, was shown to improve due to the growth of a monolayer thick ZnSe shell. Photoconductivity with a quantum efficiency of 27% was achieved by blending the Ag(2)Se nanocrystals with a soluble fullerene derivative. The co-injection of lithium silylamide was found to be crucial to the synthesis of Ag chalcogenide nanocrystals, which drastically increased their nucleation rate even at relatively low growth temperatures. Because the same observation was made for the nucleation of Cd chalcogenide nanocrystals, we conclude that the addition of lithium silylamide might generally promote wet-chemical synthesis of metal chalcogenide nanocrystals, including in as-yet unexplored materials.

Apparatus for improving the working time of the XeBr laser

DOEpatents

Sander, R.K.; Balog, G.; Seegmiller, E.T.

1980-03-04

In XeBr lasers which make use of HBr as the source of bromine, it has been found that the working life of the laser is limited because of dissociation of the HBr in the lasing region to form H/sub 2/ and Br/sub 2/. Accordingly, apparatus is disclosed for substantially improving the working time of the XeBr laser wherein means are provided for recombining H/sub 2/ and Br/sub 2/ into HBr and for continuously circulating the gaseous working medium from the lasing region through the recombination region.

Photoelectron spectroscopy of color centers in negatively charged cesium iodide nanocrystals

NASA Astrophysics Data System (ADS)

Sarkas, Harry W.; Kidder, Linda H.; Bowen, Kit H.

1995-01-01

We present the photoelectron spectra of negatively charged cesium iodide nanocrystals recorded using 2.540 eV photons. The species examined were produced using an inert gas condensation cluster ion source, and they ranged in size from (CsI)-n=13 to nanocrystal anions comprised of 330 atoms. Nanocrystals showing two distinct types of photoemission behavior were observed. For (CsI)-n=13 and (CsI)-n=36-165, a plot of cluster anion photodetachment threshold energies vs n-1/3 gives a straight line extrapolating (at n-1/3=0, i.e., n=∞) to 2.2 eV, the photoelectric threshold energy for F centers in bulk cesium iodide. The linear extrapolation of the cluster anion data to the corresponding bulk property implies that the electron localization in these gas-phase nanocrystals is qualitatively similar to that of F centers in extended alkali halide crystals. These negatively charged cesium iodide nanocrystals are thus shown to support embryonic forms of F centers, which mature with increasing cluster size toward condensed phase impurity centers. Under an alternative set of source conditions, nanocrystals were produced which showed significantly lower photodetachment thresholds than the aforementioned F-center cluster anions. For these species, containing 83-131 atoms, a plot of their cluster anion photodetachment threshold energies versus n-1/3 gives a straight line which extrapolates to 1.4 eV. This value is in accord with the expected photoelectric threshold energy for F' centers in bulk cesium iodide, i.e., color centers with two excess electrons in a single defect site. These nanocrystals are interpreted to be the embryonic F'-center containing species, Cs(CsI)-n=41-65.

Stoichiometric control of lead chalcogenide nanocrystal solids to enhance their electronic and optoelectronic device performance.

PubMed

Oh, Soong Ju; Berry, Nathaniel E; Choi, Ji-Hyuk; Gaulding, E Ashley; Paik, Taejong; Hong, Sung-Hoon; Murray, Christopher B; Kagan, Cherie R

2013-03-26

We investigate the effects of stoichiometric imbalance on the electronic properties of lead chalcogenide nanocrystal films by introducing excess lead (Pb) or selenium (Se) through thermal evaporation. Hall-effect and capacitance-voltage measurements show that the carrier type, concentration, and Fermi level in nanocrystal solids may be precisely controlled through their stoichiometry. By manipulating only the stoichiometry of the nanocrystal solids, we engineer the characteristics of electronic and optoelectronic devices. Lead chalcogenide nanocrystal field-effect transistors (FETs) are fabricated at room temperature to form ambipolar, unipolar n-type, and unipolar p-type semiconducting channels as-prepared and with excess Pb and Se, respectively. Introducing excess Pb forms nanocrystal FETs with electron mobilities of 10 cm(2)/(V s), which is an order of magnitude higher than previously reported in lead chalcogenide nanocrystal devices. Adding excess Se to semiconductor nanocrystal solids in PbSe Schottky solar cells enhances the power conversion efficiency.

Nanocrystal-mediated charge screening effects in nanowire field-effect transistors

NASA Astrophysics Data System (ADS)

Yoon, C. J.; Yeom, D. H.; Jeong, D. Y.; Lee, M. G.; Moon, B. M.; Kim, S. S.; Choi, C. Y.; Koo, S. M.

2009-03-01

ZnO nanowire field-effect transistors having an omega-shaped floating gate (OSFG) have been successfully fabricated by directly coating CdTe nanocrystals (˜6±2.5 nm) at room temperature, and compared to simultaneously prepared control devices without nanocrystals. Herein, we demonstrate that channel punchthrough may occur when the depletion from the OSFG takes place due to the trapped charges in the nanocrystals. Electrical measurements on the OSFG nanowire devices showed static-induction transistorlike behavior in the drain output IDS-VDS characteristics and a hysteresis window as large as ˜3.1 V in the gate transfer IDS-VGS characteristics. This behavior is ascribed to the presence of the CdTe nanocrystals, and is indicative of the trapping and emission of electrons in the nanocrystals. The numerical simulations clearly show qualitatively the same characteristics as the experimental data and confirm the effect, showing that the change in the potential distribution across the channel, induced by both the wrapping-around gate and the drain, affects the transport characteristics of the device. The cross-sectional energy band and potential profile of the OSFG channel corresponding to the "programed (noncharged)" and "erased (charged)" operations for the device are also discussed on the basis of the numerical capacitance-voltage simulations.

Seeded Growth Route to Noble Calcium Carbonate Nanocrystal.

PubMed

Islam, Aminul; Teo, Siow Hwa; Rahman, M Aminur; Taufiq-Yap, Yun Hin

2015-01-01

A solution-phase route has been considered as the most promising route to synthesize noble nanostructures. A majority of their synthesis approaches of calcium carbonate (CaCO3) are based on either using fungi or the CO2 bubbling methods. Here, we approached the preparation of nano-precipitated calcium carbonate single crystal from salmacis sphaeroides in the presence of zwitterionic or cationic biosurfactants without external source of CO2. The calcium carbonate crystals were rhombohedron structure and regularly shaped with side dimension ranging from 33-41 nm. The high degree of morphological control of CaCO3 nanocrystals suggested that surfactants are capable of strongly interacting with the CaCO3 surface and control the nucleation and growth direction of calcium carbonate nanocrystals. Finally, the mechanism of formation of nanocrystals in light of proposed routes was also discussed.

Seeded Growth Route to Noble Calcium Carbonate Nanocrystal

PubMed Central

Islam, Aminul; Teo, Siow Hwa; Rahman, M. Aminur; Taufiq-Yap, Yun Hin

2015-01-01

A solution-phase route has been considered as the most promising route to synthesize noble nanostructures. A majority of their synthesis approaches of calcium carbonate (CaCO3) are based on either using fungi or the CO2 bubbling methods. Here, we approached the preparation of nano-precipitated calcium carbonate single crystal from salmacis sphaeroides in the presence of zwitterionic or cationic biosurfactants without external source of CO2. The calcium carbonate crystals were rhombohedron structure and regularly shaped with side dimension ranging from 33–41 nm. The high degree of morphological control of CaCO3 nanocrystals suggested that surfactants are capable of strongly interacting with the CaCO3 surface and control the nucleation and growth direction of calcium carbonate nanocrystals. Finally, the mechanism of formation of nanocrystals in light of proposed routes was also discussed. PMID:26700479

Adsorption of vitamin E on mesoporous titania nanocrystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shih, C.J., E-mail: cjshih@kmu.edu.tw; Lin, C.T.; Wu, S.M.

2010-07-15

Tri-block nonionic surfactant and titanium chloride were used as starting materials for the synthesis of mesoporous titania nanocrystallite powders. The main objective of the present study was to examine the synthesis of mesoporous titania nanocrystals and the adsorption of vitamin E on those nanocrystals using X-ray diffraction (XRD), transmission electron microscopy, and nitrogen adsorption and desorption isotherms. When the calcination temperature was increased to 300 {sup o}C, the reflection peaks in the XRD pattern indicated the presence of an anatase phase. The crystallinity of the nanocrystallites increased from 80% to 98.6% with increasing calcination temperature from 465 {sup o}C tomore » 500 {sup o}C. The N{sub 2} adsorption data and XRD data taken after vitamin E adsorption revealed that the vitamin E molecules were adsorbed in the mesopores of the titania nanocrystals.« less

Nondisruptive Dissolution of Hyperpolarized 129 Xe into Viscous Aqueous and Organic Liquid Crystalline Environments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Truxal, Ashley E.; Slack, Clancy C.; Gomes, Muller D.

2016-03-08

Studies of hyperpolarized xenon-129 in media such as liquid crystals and cell suspensions are in demand for applications ranging from biomedical imaging to materials engineering but have been hindered by the inability to bubble Xe through the desired media as a result of viscosity or perturbations caused by bubbles. This research reports on a device that can be reliably used to dissolve hp- 129 Xe into viscous aqueous and organic samples without bubbling. This method is robust, requires small sample volumes ( < 60 μL), is compatible with existing NMR hardware, and is made from readily available materials. Experiments showmore » that Xe can be introduced into viscous and aligned media without disrupting molecular order. We detected dissolved xenon in an aqueous liquid crystal that is disrupted by the shear forces of bubbling, and we observed liquid-crystal phase transitions in (MBBA). This tool allows an entirely new class of samples to be investigated by hyperpolarized-gas NMR spectroscopy. Blending into the crowd: A new device that facilitates the direct dissolution of hyperpolarized 129 Xe into viscous liquid-crystalline media is presented. 129 Xe and 2 H NMR spectra show the nondisruptive dissolution of xenon, the presence of ordered phases, and, in the case of the thermotropic liquid crystal N-(4-methoxybenzylidene)-4-butylaniline, a nematic-isotropic phase transition.« less

Inorganic Nanocrystals Functionalized Mesoporous Silica Nanoparticles: Fabrication and Enhanced Bio-applications

NASA Astrophysics Data System (ADS)

Zhao, Tiancong; Nguyen, Nam-Trung; Xie, Yang; Sun, Xiaofei; Li, Qin; Li, Xiaomin

2017-12-01

Mesoporous SiO2 nanoparticles (MSNs) are one of the most promising materials for bio-related applications due to advantages such as good biocompatibility, tunable mesopores and large pore volume. However, unlike the inorganic nanocrystals with abundant physical properties, MSNs alone lack functional features. Thus, they are not sufficiently suitable for bio-applications that require special functions. Consequently, MSNs are often functionalized by incorporating inorganic nanocrystals, which provide a wide range of intriguing properties. This review focuses on inorganic nanocrystals functionalized MSNs, both their fabrication and bio-applications. Some of the most utilized methods for coating mesoporous silica (mSiO2) on nanoparticles were summarized. Magnetic, fluorescence and photothermal inorganic nanocrystals functionalized MSNs were taken as examples to demonstrate the bio-applications. Furthermore, asymmetry of MSNs and their effects on functions were also highlighted.

Nanocrystal synthesis in microfluidic reactors: where next?

PubMed

Phillips, Thomas W; Lignos, Ioannis G; Maceiczyk, Richard M; deMello, Andrew J; deMello, John C

2014-09-07

The past decade has seen a steady rise in the use of microfluidic reactors for nanocrystal synthesis, with numerous studies reporting improved reaction control relative to conventional batch chemistry. However, flow synthesis procedures continue to lag behind batch methods in terms of chemical sophistication and the range of accessible materials, with most reports having involved simple one- or two-step chemical procedures directly adapted from proven batch protocols. Here we examine the current status of microscale methods for nanocrystal synthesis, and consider what role microreactors might ultimately play in laboratory-scale research and industrial production.

From Artificial Atoms to Nanocrystal Molecules: Preparation and Properties of More Complex Nanostructures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Choi, Charina L; Alivisatos, A Paul

2009-10-20

Quantum dots, which have found widespread use in fields such as biomedicine, photovoltaics, and electronics, are often called artificial atoms due to their size-dependent physical properties. Here this analogy is extended to consider artificial nanocrystal molecules, formed from well-defined groupings of plasmonically or electronically coupled single nanocrystals. Just as a hydrogen molecule has properties distinct from two uncoupled hydrogen atoms, a key feature of nanocrystal molecules is that they exhibit properties altered from those of the component nanoparticles due to coupling. The nature of the coupling between nanocrystal atoms and its response to vibrations and deformations of the nanocrystal moleculemore » bonds are of particular interest. We discuss synthetic approaches, predicted and observed physical properties, and prospects and challenges toward this new class of materials.« less

Nanocrystal waveguide (NOW) laser

DOEpatents

Simpson, John T.; Simpson, Marcus L.; Withrow, Stephen P.; White, Clark W.; Jaiswal, Supriya L.

2005-02-08

A solid state laser includes an optical waveguide and a laser cavity including at least one subwavelength mirror disposed in or on the optical waveguide. A plurality of photoluminescent nanocrystals are disposed in the laser cavity. The reflective subwavelength mirror can be a pair of subwavelength resonant gratings (SWG), a pair of photonic crystal structures (PC), or a distributed feedback structure. In the case of a pair of mirrors, a PC which is substantially transmissive at an operating wavelength of the laser can be disposed in the laser cavity between the subwavelength mirrors to improve the mode structure, coherence and overall efficiency of the laser. A method for forming a solid state laser includes the steps of providing an optical waveguide, creating a laser cavity in the optical waveguide by disposing at least one subwavelength mirror on or in the waveguide, and positioning a plurality of photoluminescent nanocrystals in the laser cavity.

The first narrow-band XeCl-excilamp application for complex psoriasis curing

NASA Astrophysics Data System (ADS)

Dmitruck, Vadim S.; Sosnin, Edward A.; Obgol'tz, Irina A.

2006-05-01

Clinical efficiency estimation of XeCl-excilamp application for psoriasis curing in comparison with other methods of phototherapy for has been carried out for the first time. Curing psoriasis by XeCl-excilamp assistance is shown to be an effective and present-date method. Such a phototherapy advantages suggested are the good tolerance, and absence of intact skin irradiation. The use of chemicals is no longer relevant, and the total doze of irradiation happens to be rather low.

Intrinsic behavior of face-centered-cubic supra-crystals of nanocrystals self-organized on mesoscopic scale

NASA Astrophysics Data System (ADS)

Pileni, M. P.

2005-12-01

We describe intrinsic behavior due to the high ordering of nanocrystals at the mesoscopic scale. The first example shows well-defined columns in the formation of cobalt nanocrystals when an applied magnetic field is applied during the evaporation process. Collective breathing properties between nanocrystals are demonstrated. In both cases, these features are observed when the nanocrystals are highly ordered in fcc supra-crystals.

Quantitative tunneling spectroscopy of nanocrystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

First, Phillip N; Whetten, Robert L; Schaaff, T Gregory

2007-05-25

The proposed goals of this collaborative work were to systematically characterize the electronic structure and dynamics of 3-dimensional metal and semiconducting nanocrystals using scanning tunneling microscopy/spectroscopy (STM/STS) and ballistic electron emission spectroscopy (BEES). This report describes progress in the spectroscopic work and in the development of methods for creating and characterizing gold nanocrystals. During the grant period, substantial effort also was devoted to the development of epitaxial graphene (EG), a very promising materials system with outstanding potential for nanometer-scale ballistic and coherent devices ("graphene" refers to one atomic layer of graphitic, sp2 -bonded carbon atoms [or more loosely, few layers]).more » Funding from this DOE grant was critical for the initial development of epitaxial graphene for nanoelectronics« less

Cryptophane Nanoscale Assemblies Expand 129Xe NMR Biosensing.

PubMed

Zemerov, Serge D; Roose, Benjamin W; Greenberg, Mara L; Wang, Yanfei; Dmochowski, Ivan J

2018-06-19

Cryptophane-based biosensors are promising agents for the ultrasensitive detection of biomedically relevant targets via 129 Xe NMR. Dynamic light scattering revealed that cryptophanes form water-soluble aggregates tens to hundreds of nanometers in size. Acridine orange fluorescence quenching assays allowed quantitation of the aggregation state, with critical concentrations ranging from 200 nM to 600 nM, depending on the cryptophane species in solution. The addition of excess carbonic anhydrase (CA) protein target to a benzenesulfonamide-functionalized cryptophane biosensor (C8B) led to C8B disaggregation and produced the expected 1:1 C8B-CA complex. C8B showed higher affinity at 298 K for the cytoplasmic isozyme CAII than the extracellular CAXII isozyme, which is a biomarker of cancer. Using hyper-CEST NMR, we explored the role of stoichiometry in detecting these two isozymes. Under CA-saturating conditions, we observed that isozyme CAII produces a larger 129 Xe NMR chemical shift change (δ = 5.9 ppm, relative to free biosensor) than CAXII (δ = 2.7 ppm), which indicates the strong potential for isozyme-specific detection. However, stoichiometry-dependent chemical shift data indicated that biosensor disaggregation contributes to the observed 129 Xe NMR chemical shift change that is normally assigned to biosensor-target binding. Finally, we determined that monomeric cryptophane solutions improve hyper-CEST saturation contrast, which enables ultrasensitive detection of biosensor-protein complexes. These insights into cryptophane-solution behavior support further development of xenon biosensors, but will require reinterpretation of the data previously obtained for many water-soluble cryptophanes.

Low-frequency (1/f) noise in nanocrystal field-effect transistors.

PubMed

Lai, Yuming; Li, Haipeng; Kim, David K; Diroll, Benjamin T; Murray, Christopher B; Kagan, Cherie R

2014-09-23

We investigate the origins and magnitude of low-frequency noise in high-mobility nanocrystal field-effect transistors and show the noise is of 1/f-type. Sub-band gap states, in particular, those introduced by nanocrystal surfaces, have a significant influence on the 1/f noise. By engineering the device geometry and passivating nanocrystal surfaces, we show that in the linear and saturation regimes the 1/f noise obeys Hooge's model of mobility fluctuations, consistent with transport of a high density of accumulated carriers in extended electronic states of the NC thin films. In the subthreshold regime, the Fermi energy moves deeper into the mobility gap and sub-band gap trap states give rise to a transition to noise dominated by carrier number fluctuations as described in McWhorter's model. CdSe nanocrystal field-effect transistors have a Hooge parameter of 3 × 10(-2), comparable to other solution-deposited, thin-film devices, promising high-performance, low-cost, low-noise integrated circuitry.

In situ microscopy of the self-assembly of branched nanocrystals in solution

DOE PAGES

Sutter, Eli; Tkachenko, Alexei V.; Sutter, Peter; ...

2016-04-04

Here, solution-phase self-assembly of nanocrystals into mesoscale structures is a promising strategy for constructing functional materials from nanoscale components. Liquid environments are key to self-assembly since they allow suspended nanocrystals to diffuse and interact freely, but they also complicate experiments. Real-time observations with single-particle resolution could have transformative impact on our understanding of nanocrystal self-assembly. Here we use real-time in situ imaging by liquid-cell electron microscopy to elucidate the nucleation and growth mechanism and properties of linear chains of octapod-shaped nanocrystals in their native solution environment. Statistical mechanics modelling based on these observations and using the measured chain-length distribution clarifiesmore » the relative importance of dipolar and entropic forces in the assembly process and gives direct access to the interparticle interaction. Our results suggest that monomer-resolved in situ imaging combined with modelling can provide unprecedented quantitative insight into the microscopic processes and interactions that govern nanocrystal self-assembly in solution.« less