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Sample records for 5f electron localization

  1. The degree of 5f electron localization in URu2Si2: electron energy-loss spectroscopy and spin-orbit sum rule analysis

    SciTech Connect

    Jeffries, J R; Moore, K T; Butch, N P; Maple, M B

    2010-05-19

    We examine the degree of 5f electron localization in URu{sub 2}Si{sub 2} using spin-orbit sum rule analysis of the U N{sub 4,5} (4d {yields} 5f) edge. When compared to {alpha}-U metal, US, USe, and UTe, which have increasing localization of the 5f states, we find that the 5f states of URu{sub 2}Si{sub 2} are more localized, although not entirely. Spin-orbit analysis shows that intermediate coupling is the correct angular momentum coupling mechanism for URu{sub 2}Si{sub 2} when the 5f electron count is between 2.6 and 2.8. These results have direct ramifications for theoretical assessment of the hidden order state of URu{sub 2}Si{sub 2}, where the degree of localization of the 5f electrons and their contribution to the Fermi surface are critical.

  2. Localized 5f electrons in superconducting PuCoIn₅: consequences for superconductivity in PuCoGa₅.

    PubMed

    Bauer, E D; Altarawneh, M M; Tobash, P H; Gofryk, K; Ayala-Valenzuela, O E; Mitchell, J N; McDonald, R D; Mielke, C H; Ronning, F; Griveau, J-C; Colineau, E; Eloirdi, R; Caciuffo, R; Scott, B L; Janka, O; Kauzlarich, S M; Thompson, J D

    2012-02-08

    The physical properties of the first In analog of the PuMGa(5) (M = Co, Rh) family of superconductors, PuCoIn(5), are reported. With its unit cell volume being 28% larger than that of PuCoGa(5), the characteristic spin-fluctuation energy scale of PuCoIn(5) is three to four times smaller than that of PuCoGa(5), which suggests that the Pu 5f electrons are in a more localized state relative to PuCoGa(5). This raises the possibility that the high superconducting transition temperature T(c) = 18.5 K of PuCoGa(5) stems from the proximity to a valence instability, while the superconductivity at T(c) = 2.5 K of PuCoIn(5) is mediated by antiferromagnetic spin fluctuations associated with a quantum critical point.

  3. Magnetic properties of actinide elements having the 5f/sup 6/ and 5f/sup 7/ electronic configurations

    SciTech Connect

    Nave, S.E.; Haire, R.G.; Huray, P.G.

    1983-09-01

    Magnetic susceptibility measurements have been made on multimicrogram quantities of /sup 243/AmF/sub 3/, /sup 248/CmF/sub 4/, /sup 248/CmO/sub 2/, and /sup 248/CmBaO/sub 3/ samples (nominally the 5f/sup 6/ electronic configuration) and on /sup 248/Cm/sub 2/O/sub 3/, /sup 248/CmF/sub 3/, /sup 249/BkF/sub 4/, and /sup 249/BkO/sub 2/ (nominally the 5f/sup 7/ electronic configuration) in the temperature range 4.2--300 K and in magnetic fields up to 1650 G. The experimentally determined effective magnetic moments and the Curie-Weiss constants for these compounds are presented. The deviation of the moments for the 5f/sup 6/ compounds from those expected from classic theory is discussed in terms of low-lying excited states, chemical composition, crystal-field perturbations, and realistic electronic structure.

  4. Electron correlation and relativity of the 5f electrons in the U-Zr alloy system

    NASA Astrophysics Data System (ADS)

    Söderlind, P.; Sadigh, B.; Lordi, V.; Landa, A.; Turchi, P. E. A.

    2014-01-01

    ] and VASP [4] codes. The Wien2K computations are set up with an APW + lo basis for the expansion of the wave functions within the muffin-tin spheres (with radius RMT = 2.5 a.u.) in partial waves with angular momenta up to l = 3, and an LAPW basis for all higher angular momenta up to l = 10. The plane-wave cutoff (Kmax) for the expansion of the wave functions in the interstitial region is chosen such that RMT × Kmax = 10. We apply the LSDA + U scheme proposed by Anisimov et al. [5] (Wien2K) and Dudarev et al. [6] (VASP) to the uranium f orbitals, which approximately corrects for their electron self interaction. An effective Ueff = U - J is chosen to be 2 eV (J = 0), which appears to be realistic for uranium systems [7]. The spin-orbit interaction is included using the second-variation method with scalar-relativistic orbitals as basis. This basis includes all Eigen states with energy less than 70 eV. For reason to improve the description of the relativistic orbitals, the p1/2 local orbitals are added to the basis set. For actinide metals, this technique for the spin-orbit coupling equals, with good approximation, that of the complete four-spinor Dirac formalism [8-10]. All calculations use a 12 × 12 × 12 Monkhorst-Pack k-point grid and a plane-wave cutoff of 23 Ry.In Table 1 we show our calculated equilibrium volumes (V) and bulk moduli (B) obtained with and without spin-orbit coupling (SOC) for bcc (γ) uranium metal using the Wien2K (VASP) codes. (The other component, Zr, is a light metal where relativistic effects are not important). The changes in V and B due to SOC are indeed quite small, consistent with results from previous studies [9,11], and within the scatter of the experimental data. The reason why the volume expands slightly is that the separation of the 5f5/2 and 5f7/2 states, due to spin-orbit coupling, weakens the cohesion of the bonding electrons. The separation is very small, as seen in Fig. 1[11] where we plot the total electronic density

  5. 5f band dispersion in the highly correlated electronic structure of uranium compounds

    NASA Astrophysics Data System (ADS)

    Moore, D. P.; Joyce, J. J.; Arko, A. J.; Morales, L.; Sarrao, J.

    2000-07-01

    Despite the fact that the 5f shell of the light actinides is less than half filled, the relatively short radial extent of 5f-electron wave functions yields at most minimal f-f overlap (the critical actinide-actinide spacing for which f-f overlap is no longer viable was first quantified by H. Hill and found to be 3.4 Å. The spacing for both USb2 and UAsSe is about 4.5. Å) and results in a myriad of phenomena collectively called correlated electron behavior. We present data from angle resolved photoemission studies of USb2 and UAsSe on correlated electron behavior.

  6. Effects of 5f-elements on electronic structures and spectroscopic properties of gold superatom model

    NASA Astrophysics Data System (ADS)

    Gao, Yang; Wang, Zhigang

    2016-08-01

    5f-elements encaged in a gold superatomic cluster are capable of giving rise to unique optical properties due to their hyperactive valence electrons and great radial components of 5f/6d orbitals. Herein, we review our first-principles studies on electronic structures and spectroscopic properties of a series of actinide-embedded gold superatomic clusters with different dimensions. The three-dimensional (3D) and two-dimensional (2D) superatom clusters possess the 18-electron configuration of 1S21P61D10 and 10-electron configuration of 1S21P41D4, respectively. Importantly, their electronic absorption spectra can also be effectively explained by the superatom orbitals. Specifically, the charge transfer (CT) transitions involved in surface-enhance Raman spectroscopy (SERS) spectra for 3D and 2D structures are both from the filled 1D orbitals, providing the enhancement factors of the order of ˜ 104 at 488 nm and ˜ 105 at 456 nm, respectively. This work implies that the superatomic orbital transitions involved in 5f-elements can not only lead to a remarkable spectroscopic performance, but also a new direction for optical design in the future. Project supported by the National Natural Science Foundation of China (Grant No. 11374004), the Science and Technology Development Program of Jilin Province, China (Grant No. 20150519021JH), the Fok Ying Tung Education Foundation, China (Grant No. 142001), and the Support from the High Performance Computing Center (HPCC) of Jilin University, China.

  7. Probing ultrafast dynamics of 5f electrons in crystalline UO2

    SciTech Connect

    An, Yong Q; Taylor, Antoinette J; Durakiewicz, Tomasz; Rodriguez, George

    2010-01-01

    The electronic structure and ultrafast dynamics of photoexcited carriers of Mott insulators attracts considerable attention in modern condensed matter physics. Cubic structured UO{sub 2} is a model system for understanding the physics of strongly correlated electrons in Mott insulators. Its 5f electrons may produce special electronic states and dynamics because of their complex nature. It shows an anti ferromagnetic transition at T{sub N} = 30.8 K. Several recent theoretical works have predicted the ground states and Mott characteristics of crystalline UO{sub 2}. It is believed that the band gap of UO{sub 2} is on the order of {approx} 2 eV and excitations across the gap are of the f-f character. We have performed ultrafast optical studies of carrier dynamics related to the Mott gap and its Hubbard bands with femtosecond pump-probe transient reflection measurements. From pump-probe reflectance measurements, we find the lifetimes of photoexcited 5f electrons in crystalline UO{sub 2}, {approx} 1.2 ns for midgap states and {approx} 2 {mu}s for upper Hubbard band states at low temperatures, and identify magnetic transitions.

  8. Electron Attachment and Detachment, and the Electron Affinities of C(5)F(5)N and C(5)HF(4)N

    DTIC Science & Technology

    2005-09-19

    detachment rate at 303 K was 520 ± 180 s-1. The attachment/detachment equilibrium yielded experimental electron affinities EA(CsF 5N) = 0.70-0.05 eV and EA...are in good agreement with the present experimental results. 15. SUBJECT TERMS Electron attachment Electron affinity Electron detachment Rate constant...attachment/detachment equilibrium yielded experimental electron affinities EA(C5F5 N)=0.70±0.05 eV and EA(2,3,5,6-C5HF 4N)=0.40±0.08 eV. Electronic

  9. Electron attachment and detachment, and the electron affinities of C5F5N and C5HF4N

    NASA Astrophysics Data System (ADS)

    Van Doren, Jane M.; Kerr, Donna M.; Miller, Thomas M.; Viggiano, A. A.

    2005-09-01

    Rate constants have been measured for electron attachment to C5F5N (297-433K) and to 2,3,5,6-C5HF4N (303K) using a flowing-afterglow Langmuir-probe apparatus (at a He gas pressure of 133Pa). In both cases only the parent anion was formed in the attachment process. The attachment rate constants measured at room temperature are 1.8±0.5×10-7 and 7±3×10-10cm-3s-1, respectively. Rate constants were also measured for thermal electron detachment from the parent anions of these molecules. For C5F5N- detachment is negligible at room temperature, but increases to 2530±890s-1 at 433K. For 2,3,5,6-C5HF4N-, the detachment rate at 303K was 520±180s-1. The attachment/detachment equilibrium yielded experimental electron affinities EA(C5F5N )=0.70±0.05eV and EA(2,3,5,6-C5HF4N )=0.40±0.08eV. Electronic structure calculations were carried out for these molecules and related C5HxF5-xN using density-functional theory and the G3(MP2)‖B3LYP compound method. The EAs are found to decrease by 0.25eV, on average, with each F substitution by H. The calculated EAs are in good agreement with the present experimental results.

  10. Electron attachment and detachment, and the electron affinities of C5F5N and C5HF4N.

    PubMed

    Van Doren, Jane M; Kerr, Donna M; Miller, Thomas M; Viggiano, A A

    2005-09-15

    Rate constants have been measured for electron attachment to C5F5N (297-433 K) and to 2, 3, 5, 6-C5HF4N (303 K) using a flowing-afterglow Langmuir-probe apparatus (at a He gas pressure of 133 Pa). In both cases only the parent anion was formed in the attachment process. The attachment rate constants measured at room temperature are 1.8 +/- 0.5 X 10(-7) and 7 +/- 3 X 10(-10) cm(-3) s(-1), respectively. Rate constants were also measured for thermal electron detachment from the parent anions of these molecules. For C5F5N- detachment is negligible at room temperature, but increases to 2530 +/- 890 s(-1) at 433 K. For 2, 3, 5, 6-C5HF4N-, the detachment rate at 303 K was 520 +/- 180 s(-1). The attachment/detachment equilibrium yielded experimental electron affinities EA(C5F5N)=0.70 +/- 0.05 eV and EA(2, 3, 5, 6-C5HF4N)=0.40 +/- 0.08 eV. Electronic structure calculations were carried out for these molecules and related C5HxF5-xN using density-functional theory and the G3(MP2)//B3LYP compound method. The EAs are found to decrease by 0.25 eV, on average, with each F substitution by H. The calculated EAs are in good agreement with the present experimental results.

  11. Response to letter "Electron correlation and relativity of the 5f electrons in the Usbnd Zr alloy system"

    NASA Astrophysics Data System (ADS)

    Xie, Wei; Marianetti, Chris A.; Morgan, Dane

    2016-08-01

    In the Letter [Söderlind et al., J. Nucl. Mater. 444, 356 (2014)], Söderlind et al. state their interpretation that 1) we view electron correlation to be strong and including spin-orbit coupling (SOC) to be necessary for U metal and Usbnd Zr alloy in our article [Xiong et al., J. Nucl. Mater. 443, 331 (2013)]. Further, they argue that 2) density functional theory (DFT) without adding the Hubbard U potential, especially when solved using all electron methods, already models U and Usbnd Zr accurately, and 3) adding the Hubbard U potential to DFT in DFT + U models U and Usbnd Zr worse than DFT according to volume, bulk modulus, and magnetic moments predicted from their calculations of the γU phase of elemental U metal. With respect to Söderlind et al.'s interpretation 1), we clarify that our opinions are that U and Usbnd Zr are not strongly, but weakly to moderately correlated and that including SOC is beneficial but not necessary for modeling most ground state properties of U and Usbnd Zr. With respect to Söderlind et al.'s argument 2) we demonstrate that previously neglected and very recent experimental data suggest that DFT in Söderlind's full-potential linear muffin-tin orbital calculations [Söderlind, Phys. Rev. B 66, 085113 (2002)] in fact models the bulk modulus and elastic constants of αU with errors considerably larger than other related elements, e.g., most transition metals. With respect to Söderlind et al.'s argument 3) we argue that they have inappropriately focused on just one phase (the BCC γU phase of U metal), neglecting the other phases which represent the majority of our evidence, and made overgeneralizations based on results at only one Ueff value of 2 eV. We therefore maintain our original conclusion that the accuracy of DFT for modeling U and Usbnd Zr has room for improvement and DFT + U can be of value for this purpose on at least some ground state properties.

  12. Role of the local structure in superconductivity of LaO0.5F0.5BiS2‑x Se x system

    NASA Astrophysics Data System (ADS)

    Paris, E.; Mizuguchi, Y.; Hacisalihoglu, M. Y.; Hiroi, T.; Joseph, B.; Aquilanti, G.; Miura, O.; Mizokawa, T.; Saini, N. L.

    2017-04-01

    We have studied the local structure of LaO0.5F0.5BiS2‑x Se x by Bi L1-edge extended x-ray absorption fine structure (EXAFS). We find a significant effect of Se substitution on the local atomic correlations with a gradual elongation of average in-plane Bi-S bondlength. The associated mean square relative displacement, measuring average local distortions in the BiS2 plane, hardly shows any change for small Se substitution, but decreases significantly for x≥slant 0.6 . The Se substitution appears to suppress the local distortions within the BiS2 plane that may optimize in-plane orbital hybridization and hence the superconductivity. The results suggest that the local structure of the BiS2-layer is one of the key ingredients to control the physical properties of the BiS2-based dichalcogenides.

  13. Gas-phase reactions of doubly charged actinide cations with alkanes and alkenes--probing the chemical activity of 5f electrons from Th to Cm.

    PubMed

    Marçalo, Joaquim; Santos, Marta; Gibson, John K

    2011-11-07

    Small alkanes (methane, ethane, propane, n-butane) and alkenes (ethene, propene, 1-butene) were used to probe the gas-phase reactivity of doubly charged actinide cations, An(2+) (An = Th, Pa, U, Np, Pu, Am, Cm), by means of Fourier transform ion cyclotron resonance mass spectrometry. Different combinations of doubly and singly charged ions were observed as reaction products, comprising species formed via metal-ion induced eliminations of small molecules, simple adducts and ions resulting from electron, hydride or methide transfer channels. Th(2+), Pa(2+), U(2+) and Np(2+) preferentially yielded doubly charged products of hydrocarbon activation, while Pu(2+), Am(2+) and Cm(2+) reacted mainly through transfer channels. Cm(2+) was also capable of forming doubly charged products with some of the hydrocarbons whereas Pu(2+) and Am(2+) were not, these latter two ions conversely being the only for which adduct formation was observed. The product distributions and the reaction efficiencies are discussed in relation to the electronic configurations of the metal ions, the energetics of the reactions and similar studies previously performed with doubly charged lanthanide and transition metal cations. The conditions for hydrocarbon activation to occur as related to the accessibility of electronic configurations with one or two 5f and/or 6d unpaired electrons are examined and the possible chemical activity of the 5f electrons in these early actinide ions, particularly Pa(2+), is considered.

  14. Localization of electrons and excitations

    NASA Astrophysics Data System (ADS)

    Larsson, Sven

    2006-07-01

    Electrons, electron holes, or excitations in finite or infinite 'multimer systems' may be localized or delocalized. In the theory of Hush, localization depends on the ratio Δ/ λ ( Δ/2 = coupling; λ = reorganization energy). The latter theory has been extended to the infinite system [S. Larsson, A. Klimkāns, Mol. Cryst. Liq. Cryst. 355 (2000) 217]. The metal/insulator transition often takes place abruptly as a function of Δ/ λ. It is argued that localization in a system with un-filled bands cannot be determined on the basis of Mott-Hubbard U alone, but depends on the number of accessible valence states, reorganization energy λ and coupling Δ (=2t). In fact U = 0 does not necessarily imply delocalization. The analysis here shows that there are many different situations for an insulator to metal transition. Charge transfer in doped NiO is characterized by Ni 2+ - Ni 3+ exchange while charge transfer in pure NiO is characterized by a disproportionation 2Ni 2+ → Ni + + Ni 3+. In spite of the great differences between these two cases, U has been applied without discrimination to both. The relevant localization parameters appear to be Δ and λ in the first case, with only two oxidation states, and U, Δ and λ in the second case with three oxidation states. The analysis is extended to insulator-metal transitions, giant magnetic resistance (GMR) and high Tc superconductivity (SC). λ and Δ can be determined quite accurately in quantum mechanical calculations involving only one and two monomers, respectively.

  15. Band structures of 4f and 5f materials studied by angle-resolved photoelectron spectroscopy

    NASA Astrophysics Data System (ADS)

    Fujimori, Shin-ichi

    2016-04-01

    Recent remarkable progress in angle-resolved photoelectron spectroscopy (ARPES) has enabled the direct observation of the band structures of 4f and 5f materials. In particular, ARPES with various light sources such as lasers (hν ∼ 7~\\text{eV} ) or high-energy synchrotron radiations (hν ≳ 400~\\text{eV} ) has shed light on the bulk band structures of strongly correlated materials with energy scales of a few millielectronvolts to several electronvolts. The purpose of this paper is to summarize the behaviors of 4f and 5f band structures of various rare-earth and actinide materials observed by modern ARPES techniques, and understand how they can be described using various theoretical frameworks. For 4f-electron materials, ARPES studies of \\text{Ce}M\\text{I}{{\\text{n}}5} (M=\\text{Rh} , \\text{Ir} , and \\text{Co} ) and \\text{YbR}{{\\text{h}}2}\\text{S}{{\\text{i}}2} with various incident photon energies are summarized. We demonstrate that their 4f electronic structures are essentially described within the framework of the periodic Anderson model, and that the band-structure calculation based on the local density approximation cannot explain their low-energy electronic structures. Meanwhile, electronic structures of 5f materials exhibit wide varieties ranging from itinerant to localized states. For itinerant \\text{U}~5f compounds such as \\text{UFeG}{{\\text{a}}5} , their electronic structures can be well-described by the band-structure calculation assuming that all \\text{U}~5f electrons are itinerant. In contrast, the band structures of localized \\text{U}~5f compounds such as \\text{UP}{{\\text{d}}3} and \\text{U}{{\\text{O}}2} are essentially explained by the localized model that treats \\text{U}~5f electrons as localized core states. In regards to heavy fermion \\text{U} -based compounds such as the hidden-order compound \\text{UR}{{\\text{u}}2}\\text{S}{{\\text{i}}2} , their electronic structures exhibit complex behaviors. Their overall band structures

  16. Band structures of 4f and 5f materials studied by angle-resolved photoelectron spectroscopy.

    PubMed

    Fujimori, Shin-ichi

    2016-04-20

    Recent remarkable progress in angle-resolved photoelectron spectroscopy (ARPES) has enabled the direct observation of the band structures of 4f and 5f materials. In particular, ARPES with various light sources such as lasers (hν ~ 7 eV) or high-energy synchrotron radiations (hν >/~ 400 eV) has shed light on the bulk band structures of strongly correlated materials with energy scales of a few millielectronvolts to several electronvolts. The purpose of this paper is to summarize the behaviors of 4f and 5f band structures of various rare-earth and actinide materials observed by modern ARPES techniques, and understand how they can be described using various theoretical frameworks. For 4f-electron materials, ARPES studies of CeMIn5(M = Rh, Ir, and Co) and YbRh2Si2 with various incident photon energies are summarized. We demonstrate that their 4f electronic structures are essentially described within the framework of the periodic Anderson model, and that the band-structure calculation based on the local density approximation cannot explain their low-energy electronic structures. Meanwhile, electronic structures of 5f materials exhibit wide varieties ranging from itinerant to localized states. For itinerant U5f compounds such as UFeGa5, their electronic structures can be well-described by the band-structure calculation assuming that all U5f electrons are itinerant. In contrast, the band structures of localized U5f compounds such as UPd3 and UO2 are essentially explained by the localized model that treats U5f electrons as localized core states. In regards to heavy fermion U-based compounds such as the hidden-order compound URu2Si2, their electronic structures exhibit complex behaviors. Their overall band structures are generally well-explained by the band-structure calculation, whereas the states in the vicinity of EF show some deviations due to electron correlation effects. Furthermore, the electronic structures of URu2Si2 in the paramagnetic and hidden-order phases are

  17. Investigations of electron attachment to the perfluorocarbon molecules c-C4F8, 2-C4F8, 1,3 C4F6, and c-C5F8

    NASA Astrophysics Data System (ADS)

    Feil, Stefan; Märk, Tilmann D.; Mauracher, Andreas; Scheier, Paul; Mayhew, Chris A.

    2008-11-01

    Non-dissociative and dissociative electron attachment to a series of gas-phase perfluorocarbons (PFCs), namely octafluorocyclobutane, c-C4F8, octafluorobut-2-ene (perfluoro-2-butene), 2-C4F8, hexafluorobuta-1,3-diene (1,3 perfluorobutadiene), 1,3 C4F6, and octafluorocyclopentene (perfluorocyclopentene), c-C5F8, of importance to technological plasmas, have been investigated using two different, but complimentary, instruments available in Innsbruck over the electron energy range 0-20 eV. Anion yields as a function of electron energy have been recorded, with the positions and intensities of the electron attachment resonances being determined. One of these instruments is a double focusing sector field mass spectrometer (VG-ZAB-2SEQ), which has been used for measurements requiring high sensitivity and for obtaining accurate relative anion yields. It has also been used to determine the electron detachment lifetimes of the parent anions under various accelerating voltages, and these results are also presented. The second instrument (CELIA) is a trochoidal electron monochromator coupled to a quadrupole mass filter with a pulse counting system for detecting product anionic species. This provides a much higher energy resolution than the VG-ZAB, which makes it a better instrument to investigate narrow energy resonances close to 0 eV. The results of anion yields, peak positions and the relative intensities presented in this paper are compared with previous data of electron attachment to the above PFCs, including investigations by Professor Eugen Illenberger.

  18. Local control approach to ultrafast electron transfer

    NASA Astrophysics Data System (ADS)

    Vindel-Zandbergen, Patricia; Meier, Christoph; Sola, Ignacio R.

    2016-10-01

    We study ultrafast electron transfer between separated nuclei using local control theory. By imposing electron ionization and electron transport through the continuum, different local control formulations are used to increase the yield of retrapping the electron at the desired nuclei. The control mechanism is based on impulsive de-excitation. Both symmetric and asymmetric nuclear arrangements are analyzed, as well as the role of the nuclear motion.

  19. How do electron localization functions describe π-electron delocalization?

    PubMed

    Steinmann, Stephan N; Mo, Yirong; Corminboeuf, Clemence

    2011-12-14

    Scalar fields provide an intuitive picture of chemical bonding. In particular, the electron localization function (ELF) has proven to be highly valuable in interpreting a broad range of bonding patterns. The discrimination between enhanced or reduced electron (de)localization within cyclic π-conjugated systems remains, however, challenging for ELF. In order to clearly distinguish between the local properties of ten highly and weakly π-(de)localized prototype systems, we compare the ELFs of both the canonical wave functions and electron-localized states (diabatic) with those of two closely related scalar fields: the electron localizability indicator (ELI-D) and the localized orbital locator (LOL). The simplest LOL function distinguishes enhanced from weak π-(de)localization in an insightful and reliable manner. LOL offers the finest contrast between annulenes with 4n/4n + 2 π electrons and their inorganic analogues as well as between hyperconjugated cyclopentadiene derivatives. LOL(π) also gives an appealing and intuitive picture of the π-bond. In contrast, the most popular ELF fails to capture subtle contrasting local electronic properties and suffers from the arbitrariness of the σ/π dissection. The orbital separation of the most recent ELI-D is clear-cut but the interpretations sometime less straightforward in the present context.

  20. Fermi energy 5f spectral weight variation in uranium alloys

    SciTech Connect

    Denlinger, J.D.; Clack, J.; Allen, J.W.

    1997-04-01

    Uranium materials display a wide range of thermal, electrical and magnetic properties, often exotic. For more than a decade there have been efforts to use photoemission spectroscopy to develop a systematic and unified understanding of the 5f electron states giving rise to this behavior. These efforts have been hampered by a paucity of systems where changes in transport properties are accompanied by substantial spectral changes, so as to allow an attempt to correlate the two kinds of properties within some model. The authors have made resonant photoemission measurements to extract the 5f spectral weight in three systems which show varying degrees of promise of permitting such an attempt, Y{sub 1{minus}x}U{sub x}Pd{sub 3}, U(Pd{sub x}Pt{sub 1{minus}x}){sub 3} and U(Pd{sub x}Cu{sub 1{minus}x}){sub 5}. They have also measured U 4f core level spectra. The 4f spectra can be modeled with some success by the impurity Anderson model (IAM), and the 5f spectra are currently being analyzed in that framework. The IAM characterizes the 5f-electrons of a single site by an f binding energy {epsilon}{sub f}, an f Coulomb interaction and a hybridization V to conduction electrons. Latent in the model are the phenomena of 5f mixed valence and the Kondo effect.

  1. Local orbitals in electron scattering calculations*

    NASA Astrophysics Data System (ADS)

    Winstead, Carl L.; McKoy, Vincent

    2016-05-01

    We examine the use of local orbitals to improve the scaling of calculations that incorporate target polarization in a description of low-energy electron-molecule scattering. After discussing the improved scaling that results, we consider the results of a test calculation that treats scattering from a two-molecule system using both local and delocalized orbitals. Initial results are promising. Contribution to the Topical Issue "Advances in Positron and Electron Scattering", edited by Paulo Limao-Vieira, Gustavo Garcia, E. Krishnakumar, James Sullivan, Hajime Tanuma and Zoran Petrovic.

  2. Excess Electron Localization in Solvated DNA Bases

    SciTech Connect

    Smyth, Maeve; Kohanoff, Jorge

    2011-06-10

    We present a first-principles molecular dynamics study of an excess electron in condensed phase models of solvated DNA bases. Calculations on increasingly large microsolvated clusters taken from liquid phase simulations show that adiabatic electron affinities increase systematically upon solvation, as for optimized gas-phase geometries. Dynamical simulations after vertical attachment indicate that the excess electron, which is initially found delocalized, localizes around the nucleobases within a 15 fs time scale. This transition requires small rearrangements in the geometry of the bases.

  3. Electron localization following attosecond molecular photoionization.

    PubMed

    Sansone, G; Kelkensberg, F; Pérez-Torres, J F; Morales, F; Kling, M F; Siu, W; Ghafur, O; Johnsson, P; Swoboda, M; Benedetti, E; Ferrari, F; Lépine, F; Sanz-Vicario, J L; Zherebtsov, S; Znakovskaya, I; L'huillier, A; Ivanov, M Yu; Nisoli, M; Martín, F; Vrakking, M J J

    2010-06-10

    For the past several decades, we have been able to directly probe the motion of atoms that is associated with chemical transformations and which occurs on the femtosecond (10(-15)-s) timescale. However, studying the inner workings of atoms and molecules on the electronic timescale has become possible only with the recent development of isolated attosecond (10(-18)-s) laser pulses. Such pulses have been used to investigate atomic photoexcitation and photoionization and electron dynamics in solids, and in molecules could help explore the prompt charge redistribution and localization that accompany photoexcitation processes. In recent work, the dissociative ionization of H(2) and D(2) was monitored on femtosecond timescales and controlled using few-cycle near-infrared laser pulses. Here we report a molecular attosecond pump-probe experiment based on that work: H(2) and D(2) are dissociatively ionized by a sequence comprising an isolated attosecond ultraviolet pulse and an intense few-cycle infrared pulse, and a localization of the electronic charge distribution within the molecule is measured that depends-with attosecond time resolution-on the delay between the pump and probe pulses. The localization occurs by means of two mechanisms, where the infrared laser influences the photoionization or the dissociation of the molecular ion. In the first case, charge localization arises from quantum mechanical interference involving autoionizing states and the laser-altered wavefunction of the departing electron. In the second case, charge localization arises owing to laser-driven population transfer between different electronic states of the molecular ion. These results establish attosecond pump-probe strategies as a powerful tool for investigating the complex molecular dynamics that result from the coupling between electronic and nuclear motions beyond the usual Born-Oppenheimer approximation.

  4. Impurities and electronic localization in graphene bilayers

    NASA Astrophysics Data System (ADS)

    Ojeda Collado, H. P.; Usaj, Gonzalo; Balseiro, C. A.

    2015-01-01

    We analyze the electronic properties of bilayer graphene with Bernal stacking and a low concentration of adatoms. Assuming that the host bilayer lies on top of a substrate, we consider the case where impurities are adsorbed only on the upper layer. We describe nonmagnetic impurities as a single orbital hybridized with carbon's pz states. The effect of impurity doping on the local density of states with and without a gated electric field perpendicular to the layers is analyzed. We look for Anderson localization in the different regimes and estimate the localization length. In the biased system, the field-induced gap is partially filled by strongly localized impurity states. Interestingly, the structure, distribution, and localization length of these states depend on the field polarization.

  5. Correlative photoactivated localization and scanning electron microscopy.

    PubMed

    Kopek, Benjamin G; Shtengel, Gleb; Grimm, Jonathan B; Clayton, David A; Hess, Harald F

    2013-01-01

    The ability to localize proteins precisely within subcellular space is crucial to understanding the functioning of biological systems. Recently, we described a protocol that correlates a precise map of fluorescent fusion proteins localized using three-dimensional super-resolution optical microscopy with the fine ultrastructural context of three-dimensional electron micrographs. While it achieved the difficult simultaneous objectives of high photoactivated fluorophore preservation and ultrastructure preservation, it required a super-resolution optical and specialized electron microscope that is not available to many researchers. We present here a faster and more practical protocol with the advantage of a simpler two-dimensional optical (Photoactivated Localization Microscopy (PALM)) and scanning electron microscope (SEM) system that retains the often mutually exclusive attributes of fluorophore preservation and ultrastructure preservation. As before, cryosections were prepared using the Tokuyasu protocol, but the staining protocol was modified to be amenable for use in a standard SEM without the need for focused ion beam ablation. We show the versatility of this technique by labeling different cellular compartments and structures including mitochondrial nucleoids, peroxisomes, and the nuclear lamina. We also demonstrate simultaneous two-color PALM imaging with correlated electron micrographs. Lastly, this technique can be used with small-molecule dyes as demonstrated with actin labeling using phalloidin conjugated to a caged dye. By retaining the dense protein labeling expected for super-resolution microscopy combined with ultrastructural preservation, simplifying the tools required for correlative microscopy, and expanding the number of useful labels we expect this method to be accessible and valuable to a wide variety of researchers.

  6. 5f Resonant photoemission from plutonium

    NASA Astrophysics Data System (ADS)

    Terry, J.; Schulze, R. K.; Farr, J. D.; Zocco, T.; Heinzelman, K.; Rotenberg, E.; Shuh, D. K.; Van der Laan, G.; Arena, D. A.; Tobin, J. G.

    2002-02-01

    Experimental resonant photoemission (ResPes) results for α-Pu and δ-Pu bulk samples are presented and compared to the results of an atomic model calculation. Both Pu samples exhibit limited agreement with the atomic model calculations. As expected, α-Pu appears to have more 5f valence band delocalization than δ-Pu. Evidence of an enhanced sensitivity to surface corruption, by using synchrotron radiation as the excitation, is presented.

  7. Rampant changes in 5f 5/2 and 5f 7/2 filling across the light and middle actinide metals

    SciTech Connect

    Moore, K; der Lann, G v; Wall, M; Schwartz, A; Haire, R

    2007-04-03

    We examine the branching ratio of the N{sub 4,5} (4d {yields} 5f ) spectra of Th, U, Np, Pu, Am, and Cm metal using electron energy-loss spectroscopy (EELS) in a transmission electron microscope (TEM), together with many-electron atomic spectral calculations and the spin-orbit sum rule. Our results show that: (1) The actinide metals Pu, Am, and Cm exhibit intermediate coupling. (2) The intermediate coupling values for the 5f states as calculated using a many-electron atomic model are correct for the actinides, this being proven by our new results for curium. (3) The EELS branching ratio is sensitive to the degree of 5f electron delocalization, which is illustrated by the transition from LS to intermediate coupling between U and Pu.

  8. Local electronic properties of organic semiconductor interfaces

    NASA Astrophysics Data System (ADS)

    Blumenfeld, Michael L.

    Understanding organic semiconductor interfaces is critical to developing organic photovoltaics (OPV). OPV interfaces are disordered due to weak intermolecular interactions, resulting in diverse charge transfer micro-environments. I present experimental data isolating high-order intermolecular interactions controlling interfacial energy level alignment and describe new instrumental capabilities providing access to the local electronic and kinetic landscape at organic semiconductor interfaces. Interface formation between vanadyl naphthalocyanine (VONc) and highly ordered pyrolytic graphite (HOPG) is investigated. Ultraviolet photoemission spectroscopy (UPS) shows that the VONc binding energy (BE) decouples from the work function, shifting in an opposite direction and contradicting the standard interface dipole model. This effect is quantitatively described using an electrostatic depolarization model and confirmed by simulations which show an inhomogeneous potential at the interface. New data and literature values suggest orthogonality between polarizability and molecular dipole in polar porphyrazines. Their potential for interface engineering is discussed. The electron-rich Au(111)/VONc interface is investigated. The organic layer induces a large interface dipole in Au(111) which can be fit to a depolarization model. Ionization potential and depolarization data suggest that the second VONc layer on Au(111) adopts a tilted geometry. Electrostatic differences between Au(111)/VONc and HOPG/VONc are discussed, demonstrating that interface dipole contributions are not interchangeable. The surface states of the Au(111)/VONc interface are characterized by angle resolved 2-photon photoemission to determine the magnitude of the perturbation. The measured free-electron-like effective mass and BE destabilization of the Shockley state is attributed to step edges caused by lifting the Au(111) (22x 3 ) reconstruction. The Shockley state is accessible primarily through resonance

  9. The Local Electronic Library: Science Fiction or the Real Future?

    ERIC Educational Resources Information Center

    Cuadra, Carlos A.

    1983-01-01

    Addresses the question of whether interest in downloading into local electronic libraries is a reflection of user needs or is being generated by those who have something to sell. Growth of online services, growth of local computer capacity, purposes of a local electronic library, and sources of data are highlighted. (EJS)

  10. Direct bulk-sensitive probe of 5f symmetry in URu2Si2

    NASA Astrophysics Data System (ADS)

    Sundermann, Martin; Haverkort, Maurits W.; Agrestini, Stefano; Al-Zein, Ali; Moretti Sala, Marco; Huang, Yingkai; Golden, Mark; de Visser, Anne; Thalmeier, Peter; Hao Tjeng, Liu; Severing, Andrea

    2016-12-01

    The second-order phase transition into a hidden order phase in URu2Si2 goes along with an order parameter that is still a mystery, despite 30 years of research. However, it is understood that the symmetry of the order parameter must be related to the symmetry of the low-lying local electronic f-states. Here, we present results of a spectroscopic technique, namely core-level nonresonant inelastic X-ray scattering (NIXS). This method allows for the measurement of local high-multipole excitations and is bulk-sensitive. The observed anisotropy of the scattering function unambiguously shows that the 5f ground-state wave function is composed mainly of the Γ1 with majority Jz = |4> + |-4> and/or Γ2 singlet states. The incomplete dichroism indicates the possibility that quantum states of other irreducible representation are mixed into the ground state.

  11. Direct bulk-sensitive probe of 5f symmetry in URu2Si2

    PubMed Central

    Sundermann, Martin; Haverkort, Maurits W.; Agrestini, Stefano; Al-Zein, Ali; Moretti Sala, Marco; Huang, Yingkai; Golden, Mark; de Visser, Anne; Thalmeier, Peter; Tjeng, Liu Hao; Severing, Andrea

    2016-01-01

    The second-order phase transition into a hidden order phase in URu2Si2 goes along with an order parameter that is still a mystery, despite 30 years of research. However, it is understood that the symmetry of the order parameter must be related to the symmetry of the low-lying local electronic f-states. Here, we present results of a spectroscopic technique, namely core-level nonresonant inelastic X-ray scattering (NIXS). This method allows for the measurement of local high-multipole excitations and is bulk-sensitive. The observed anisotropy of the scattering function unambiguously shows that the 5f ground-state wave function is composed mainly of the Γ1 with majority Jz = |4⟩ + |−4⟩ and/or Γ2 singlet states. The incomplete dichroism indicates the possibility that quantum states of other irreducible representation are mixed into the ground state. PMID:27872287

  12. The 5f2-->5f16d1 absorption spectrum of Cs2GeF6:U4+ crystals: A quantum chemical and experimental study.

    PubMed

    Ordejón, Belén; Karbowiak, Miroslaw; Seijo, Luis; Barandiarán, Zoila

    2006-08-21

    Single crystals of U(4+)-doped Cs2GeF6 with 1% U4+ concentration have been obtained by the modified Bridgman-Stockbarger method in spite of the large difference in ionic radii between Ge4+ and U4+ in octahedral coordination. Their UV absorption spectrum has been recorded at 7 K, between 190 and 350 nm; it consists of a first broad and intense band peaking at about 38,000 cm(-1) followed by a number of broad bands of lower intensity from 39,000 to 45,000 cm(-1). None of the bands observed shows appreciable fine vibronic structure, so that the energies of experimental electronic origins cannot be deduced and the assignment of the experimental spectrum using empirical methods based on crystal field theory cannot be attempted. Alternatively, the profile of the absorption spectrum has been obtained theoretically using the U-F bond lengths and totally symmetric vibrational frequencies of the ground 5f2 - 1A(1g) and 5f16d(t(2g))1 - iT(1u) excited states, their energy differences, and their corresponding electric dipole transition moments calculated using the relativistic ab initio model potential embedded cluster method. The calculations suggest that the observed bands are associated with the lowest five 5f2 - 1A(1g)-->5f16d(t(2g))1 - iT(1u) (i = 1-5) dipole allowed electronic origins and their vibrational progressions. In particular, the first broad and intense band peaking at about 38,000 cm(-1) can be safely assigned to the 0-0 and 0-1 members of the a(1g) progression of the 5f2 - 1A(1g)-->5f16d(t(2g))1 - 1T(1u) electronic origin. The electronic structure of all the states with main configurational character 5f16d(t(2g))1 has been calculated as well. The results show that the lowest crystal level of this manifold is 5f16d(t(2g))1 - 1E(u) and lies about 6200 cm(-1) above the 5f2 level closest in energy, which amounts to some 11 vibrational quanta. This large energy gap could result in low nonradiative decay and efficient UV emission, which suggest the interest of

  13. (39)K NMR and EPR study of multiferroic K(3)Fe(5)F(15).

    PubMed

    Blinc, R; Zalar, B; Cevc, P; Gregorovič, A; Zemva, B; Tavčar, G; Laguta, V; Scott, J F; Dalal, N

    2009-01-28

    (39)K NMR spectra and relaxation times of polycrystalline K(3)Fe(5)F(15) have been used as a microscopic detector of the local magnetic fields at the magnetic transition at T(N) = 123 K. The NMR lineshape widens abruptly upon crossing T(N) due to the onset of internal magnetic fields, while we find no significant lineshift. The paraelectric to ferroelectric transition at T(c) = 490 K and the magnetic transition at T(N) have also been studied using X-band EPR (electron paramagnetic resonance). An increase and subsequent decrease in the EPR susceptibilities is observed on approaching T(N) from above. There is also a significant increase in the linewidth. At the same time the g-factor first decreases and then increases with decreasing temperature. The local magnetic field is different at different K sites and is much smaller than the magnetic field around the Fe sites. This seems to be consistent with the behaviour of a weak ferrimagnet. The ferrimagnetism does not seem to be due to spin canting as the lattice is disordered, but may arise from thermal blocking of superparamagnetic percolation clusters. The ferroelectric transition at T(c) shows no electronic anomaly, demonstrating that we are dealing with a classical phonon anomaly as found in conventional oxides rather than an electronic transition.

  14. Total cross sections of electron scattering by C4H8O, C5H10O2, C6H5F, C6H5Cl, C6F5Cl, C6H4(CHO)F and C4H8O2 at 30-5000 eV

    NASA Astrophysics Data System (ADS)

    Shi, D. H.; Liu, Y. F.; Ma, H.; Yu, B. H.; Sun, J. F.; Zhu, Z. L.

    2008-08-01

    Total cross sections for electron scattering by large molecules C4H8O, C5H10O2, C6H5F, C6H5Cl, C6F5Cl, C6H4(CHO)F and C4H8O2 are calculated at the Hartree-Fork level using the modified additivity rule approach. The modified additivity rule approach, which was proposed by Shi et al. [Eur. Phys. J. D 45, 253 (2007); Nucl. Instrum. Meth. B 254, 205 (2007)], takes into consideration that the contributions of the geometric shielding effect vary with the energy of the incident electrons, the target’s molecular dimension and the atomic and electronic numbers of the molecule. The present calculations cover the collision energies ranging from 30 to 5000 eV. The quantitative total cross sections are compared with those obtained by experiments and other theories. Good agreement is obtained even at energies of several tens of eV. It shows that the modified additivity rule approach is applicable to calculate the total cross sections of electron scattering by so large molecules at intermediate and high energies, especially above 100 eV. The total cross sections for electron scattering by the C4H8O2 molecule are predicted although no experimental and theoretical data are available for comparison over the present energy region.

  15. Imaging of localized electronic states at a nonconducting surface by single-electron tunneling force microscopy.

    PubMed

    Bussmann, Ezra B; Zheng, Ning; Williams, Clayton C

    2006-11-01

    Localized electronic states near a nonconducting SiO(2) surface are imaged on a approximately 1 nm scale by single-electron tunneling between the states and a scanning probe tip. Each tunneling electron is detected by electrostatic force. The images represent the number of tunneling electrons at each spatial location. The spatial resolution of the single electron tunneling force microscope is determined by quantum mechanical tunneling, providing new atomic-scale access to electronic states in dielectric surfaces and nonconducting nanostructures.

  16. Electron localization of anions probed by nitrile vibrations

    DOE PAGES

    Mani, Tomoyasu; Grills, David C.; Newton, Marshall D.; ...

    2015-08-02

    Localization and delocalization of electrons is a key concept in chemistry, and is one of the important factors determining the efficiency of electron transport through organic conjugated molecules, which have potential to act as “molecular wires”. This, in turn, substantially influences the efficiencies of organic solar cells and other molecular electronic devices. It is also necessary to understand the electronic energy landscape and the dynamics of electrons through molecular chain that govern their transport capabilities in one-dimensional conjugated chains so that we can better define the design principles of conjugated molecules for their applications. We show that nitrile ν(C≡N) vibrationsmore » respond to the degree of electron localization in nitrile-substituted organic anions by utilizing time-resolved infrared (TRIR) detection combined with pulse radiolysis. Measurements of a series of aryl nitrile anions allow us to construct a semi-empirical calibration curve between the changes in the ν(C≡N) IR shifts and the changes in the electronic charges from the neutral to the anion states in the nitriles; more electron localization in the nitrile anion results in larger IR shifts. Furthermore, the IR linewidth in anions can report a structural change accompanying changes in the electronic density distribution. Probing the shift of the nitrile ν(C≡N) IR vibrational bands enables us to determine how the electron is localized in anions of nitrile-functionalized oligofluorenes, considered as organic mixed-valence compounds. We estimate the diabatic electron transfer distance, electronic coupling strengths, and energy barriers in these organic mixed-valence compounds. The analysis reveals a dynamic picture, showing that the electron is moving back and forth within the oligomers with a small activation energy of ≤ kBT, likely controlled by the movement of dihedral angles between monomer units. Thus, implications for the electron transport capability

  17. Electron localization of anions probed by nitrile vibrations

    SciTech Connect

    Mani, Tomoyasu; Grills, David C.; Newton, Marshall D.; Miller, John R.

    2015-08-02

    Localization and delocalization of electrons is a key concept in chemistry, and is one of the important factors determining the efficiency of electron transport through organic conjugated molecules, which have potential to act as “molecular wires”. This, in turn, substantially influences the efficiencies of organic solar cells and other molecular electronic devices. It is also necessary to understand the electronic energy landscape and the dynamics of electrons through molecular chain that govern their transport capabilities in one-dimensional conjugated chains so that we can better define the design principles of conjugated molecules for their applications. We show that nitrile ν(C≡N) vibrations respond to the degree of electron localization in nitrile-substituted organic anions by utilizing time-resolved infrared (TRIR) detection combined with pulse radiolysis. Measurements of a series of aryl nitrile anions allow us to construct a semi-empirical calibration curve between the changes in the ν(C≡N) IR shifts and the changes in the electronic charges from the neutral to the anion states in the nitriles; more electron localization in the nitrile anion results in larger IR shifts. Furthermore, the IR linewidth in anions can report a structural change accompanying changes in the electronic density distribution. Probing the shift of the nitrile ν(C≡N) IR vibrational bands enables us to determine how the electron is localized in anions of nitrile-functionalized oligofluorenes, considered as organic mixed-valence compounds. We estimate the diabatic electron transfer distance, electronic coupling strengths, and energy barriers in these organic mixed-valence compounds. The analysis reveals a dynamic picture, showing that the electron is moving back and forth within the oligomers with a small activation energy of ≤ kBT, likely controlled by the movement of dihedral angles between monomer units. Thus, implications for the electron transport

  18. Metastable and spin-polarized states in electron systems with localized electron-electron interaction

    NASA Astrophysics Data System (ADS)

    Sablikov, Vladimir A.; Shchamkhalova, Bagun S.

    2014-05-01

    We study the formation of spontaneous spin polarization in inhomogeneous electron systems with pair interaction localized in a small region that is not separated by a barrier from surrounding gas of non-interacting electrons. Such a system is interesting as a minimal model of a quantum point contact in which the electron-electron interaction is strong in a small constriction coupled to electron reservoirs without barriers. Based on the analysis of the grand potential within the self-consistent field approximation, we find that the formation of the polarized state strongly differs from the Bloch or Stoner transition in homogeneous interacting systems. The main difference is that a metastable state appears in the critical point in addition to the globally stable state, so that when the interaction parameter exceeds a critical value, two states coexist. One state has spin polarization and the other is unpolarized. Another feature is that the spin polarization increases continuously with the interaction parameter and has a square-root singularity in the critical point. We study the critical conditions and the grand potentials of the polarized and unpolarized states for one-dimensional and two-dimensional models in the case of extremely small size of the interaction region.

  19. POU5F1 isoforms show different expression patterns in human embryonic stem cells and preimplantation embryos.

    PubMed

    Cauffman, Greet; Liebaers, Inge; Van Steirteghem, André; Van de Velde, Hilde

    2006-12-01

    The contribution of the POU domain, class 5, transcription factor-1 (POU5F1) in maintaining totipotency in human embryonic stem cells (hESCs) has been repeatedly proven. In humans, two isoforms are encoded: POU5F1_iA and POU5F1_iB. So far, no discrimination has been made between the isoforms in POU5F1 studies, and it is unknown which isoform contributes to the undifferentiated phenotype. Using immunocytochemistry, expression of POU5F1_iA and POU5F1_iB was examined in hESCs and all stages of human preimplantation development to look for differences in expression, biological activity, and relation to totipotency. POU5F1_iA and POU5F1_iB displayed different temporal and spatial expression patterns. During human preimplantation development, a significant POU5F1_iA expression was seen in all nuclei of compacted embryos and blastocysts and a clear POU5F1_iB expression was detected from the four-cell stage onwards in the cytoplasm of all cells. The cytoplasmic localization might imply no or other biological functions beyond transcription activation for POU5F1_iB. The stemness properties of POU5F1 can be assigned to POU5F1_iA because hESCs expressed POU5F1_iA but not POU5F1_iB. However, POU5F1_iA is not the appropriate marker to identify totipotent cells, because POU5F1_iA was also expressed in the nontotipotent trophectoderm and was not expressed in zygotes and early cleavage stage embryos, which are assumed to be totipotent. The expression pattern of POU5F1_iA may suggest that POU5F1_iA alone cannot sustain totipotency and that coexpression with other stemness factors might be the key to totipotency.

  20. Localized electron heating by strong guide-field magnetic reconnection

    NASA Astrophysics Data System (ADS)

    Guo, Xuehan; Inomoto, Michiaki; Sugawara, Takumichi; Yamasaki, Kotaro; Ushiki, Tomohiko; Ono, Yasushi

    2015-10-01

    Localized electron heating of magnetic reconnection was studied under strong guide-field using two merging spherical tokamak plasmas in the University of Tokyo Spherical Tokamak experiment. Our new slide-type two-dimensional Thomson scattering system is documented for the first time the electron heating localized around the X-point. Shape of the high electron temperature area does not agree with that of energy dissipation term Et.jt . If we include a guide-field effect term Bt/(Bp+αBt) for Et.jt , the energy dissipation area becomes localized around the X-point, suggesting that the electrons are accelerated by the reconnection electric field parallel to the magnetic field and thermalized around the X-point.

  1. Weak localization and electron-electron interactions in few layer black phosphorus devices

    NASA Astrophysics Data System (ADS)

    Shi, Yanmeng; Gillgren, Nathaniel; Espiritu, Timothy; Tran, Son; Yang, Jiawei; Watanabe, Kenji; Taniguchi, Takahashi; Lau, Chun Ning

    2016-09-01

    Few layer phosphorene (FLP) devices are extensively studied due to their unique electronic properties and potential applications on nano-electronics. Here we present magnetotransport studies which reveal electron-electron interactions as the dominant scattering mechanism in hexagonal boron nitride-encapsulated FLP devices. From weak localization measurements, we estimate the electron dephasing length to be 30 to 100 nm at low temperatures, which exhibits a strong dependence on carrier density n and a power-law dependence on temperature (˜T -0.4). These results establish that the dominant scattering mechanism in FLP is electron-electron interactions.

  2. Non-locality, adiabaticity, thermodynamics and electron energy probability functions

    NASA Astrophysics Data System (ADS)

    Boswell, Roderick; Zhang, Yunchao; Charles, Christine; Takahashi, Kazunori

    2016-09-01

    Thermodynamic properties are revisited for electrons that are governed by nonlocal electron energy probability functions in a plasma of low collisionality. Measurements in a laboratory helicon double layer experiment have shown that the effective electron temperature and density show a polytropic correlation with an index of γe = 1 . 17 +/- 0 . 02 along the divergent magnetic field, implying a nearly isothermal plasma (γe = 1) with heat being brought into the system. However, the evolution of electrons along the divergent magnetic field is essentially an adiabatic process, which should have a γe = 5 / 3 . The reason for this apparent contradiction is that the nearly collisionless plasma is very far from local thermodynamic equilibrium and the electrons behave nonlocally. The corresponding effective electron enthalpy has a conservation relation with the potential energy, which verifies that there is no heat transferred into the system during the electron evolution. The electrons are shown in nonlocal momentum equilibrium under the electric field and the gradient of the effective electron pressure. The convective momentum of ions, which can be assumed as a cold species, is determined by the effective electron pressure and the effective electron enthalpy is shown to be the source for ion acceleration. For these nearly collisionless plasmas, the use of traditional thermodynamic concepts can lead to very erroneous conclusions regarding the thermal conductivity.

  3. Local representation of the electronic dielectric response function

    DOE PAGES

    Lu, Deyu; Ge, Xiaochuan

    2015-12-11

    We present a local representation of the electronic dielectric response function, based on a spatial partition of the dielectric response into contributions from each occupied Wannier orbital using a generalized density functional perturbation theory. This procedure is fully ab initio, and therefore allows us to rigorously define local metrics, such as “bond polarizability,” on Wannier centers. We show that the locality of the bare response function is determined by the locality of three quantities: Wannier functions of the occupied manifold, the density matrix, and the Hamiltonian matrix. Furthermore, in systems with a gap, the bare dielectric response is exponentially localized,more » which supports the physical picture of the dielectric response function as a collection of interacting local responses that can be captured by a tight-binding model.« less

  4. Local representation of the electronic dielectric response function

    SciTech Connect

    Lu, Deyu; Ge, Xiaochuan

    2015-12-11

    We present a local representation of the electronic dielectric response function, based on a spatial partition of the dielectric response into contributions from each occupied Wannier orbital using a generalized density functional perturbation theory. This procedure is fully ab initio, and therefore allows us to rigorously define local metrics, such as “bond polarizability,” on Wannier centers. We show that the locality of the bare response function is determined by the locality of three quantities: Wannier functions of the occupied manifold, the density matrix, and the Hamiltonian matrix. Furthermore, in systems with a gap, the bare dielectric response is exponentially localized, which supports the physical picture of the dielectric response function as a collection of interacting local responses that can be captured by a tight-binding model.

  5. Program For Local-Area-Network Electronic Mail

    NASA Technical Reports Server (NTRS)

    Weiner, Michael J.

    1989-01-01

    MailRoom is computer program for local-area network (LAN) electronic mail. Enables users of LAN to exchange electronically notes, letters, reminders, or any sort of communication via their computers. Links all users of LAN into communication circle in which messages created, sent, copied, printed, downloaded, uploaded, and deleted through series of menu-driven screens. Includes feature that enables users to determine whether messages sent have been read by receivers. Written in Microsoft QuickBasic.

  6. Studying localized corrosion using liquid cell transmission electron microscopy

    SciTech Connect

    Chee, See Wee; Pratt, Sarah H.; Hattar, Khalid; Duquette, David; Ross, Frances M.; Hull, Robert

    2014-11-07

    Using liquid cell transmission electron microscopy (LCTEM), localized corrosion of Cu and Al thin films immersed in aqueous NaCl solutions was studied. We demonstrate that potentiostatic control can be used to initiate pitting and that local compositional changes, due to focused ion beam implantation of Au+ ions, can modify the corrosion susceptibility of Al films. Likewise, a discussion on strategies to control the onset of pitting is also presented.

  7. Studying localized corrosion using liquid cell transmission electron microscopy

    DOE PAGES

    Chee, See Wee; Pratt, Sarah H.; Hattar, Khalid; ...

    2014-11-07

    Using liquid cell transmission electron microscopy (LCTEM), localized corrosion of Cu and Al thin films immersed in aqueous NaCl solutions was studied. We demonstrate that potentiostatic control can be used to initiate pitting and that local compositional changes, due to focused ion beam implantation of Au+ ions, can modify the corrosion susceptibility of Al films. Likewise, a discussion on strategies to control the onset of pitting is also presented.

  8. Electronic-structure calculation for metals by local optimization

    NASA Astrophysics Data System (ADS)

    Woodward, C.; Min, B. I.; Benedek, R.; Garner, J.

    1989-03-01

    Recent work by Car and Parrinello has generated considerable interest in the calculation of electronic structure by nonlinear optimization. The technique introduced by these authors, dynamical simulated annealing, is designed for problems that involve energy barriers. When local optimization suffices to determine the energy minimum, more direct methods are available. In this paper we apply the algorithm suggested by Williams and Soler to calculate the electronic structure of metals, using a plane-wave expansion for the electronic orbitals and an electron-ion pseudopotential of the Kleinman-Bylander form. Radial pseudopotentials were taken from the compilation of Bachelet, Hamann, and Schlüter. Calculations are performed to optimize the electronic structure (i) with fixed atomic configuration, or (ii) with the atomic volume being optimized simultaneously. It is found that the dual optimization (ii) converges in essentially the same number of steps as the static lattice optimization (i). Numerical results are presented for Li, K, Al, and simple-cubic P.

  9. Localized Electron Heating by Strong Guide-Field Magnetic Reconnection

    NASA Astrophysics Data System (ADS)

    Guo, Xuehan; Sugawara, Takumichi; Inomoto, Michiaki; Yamasaki, Kotaro; Ono, Yasushi; UTST Team

    2015-11-01

    Localized electron heating of magnetic reconnection was studied under strong guide-field (typically Bt 15Bp) using two merging spherical tokamak plasmas in Univ. Tokyo Spherical Tokamak (UTST) experiment. Our new slide-type two-dimensional Thomson scattering system documented for the first time the electron heating localized around the X-point. The region of high electron temperature, which is perpendicular to the magnetic field, was found to have a round shape with radius of 2 [cm]. Also, it was localized around the X-point and does not agree with that of energy dissipation term Et .jt . When we include a guide-field effect term Bt / (Bp + αBt) for Et .jt where α =√{ (vin2 +vout2) /v∥2 } , the energy dissipation area becomes localized around the X-point, suggesting that the electrons are accelerated by the reconnection electric field parallel to the magnetic field and thermalized around the X-point. This work was supported by JSPS A3 Foresight Program ``Innovative Tokamak Plasma Startup and Current Drive in Spherical Torus,'' a Grant-in-Aid from the Japan Society for the Promotion of Science (JSPS) Fellows 15J03758.

  10. Localized Electron States Near a Metal-SemiconductorNanocontact

    SciTech Connect

    Demchenko, Denis O.; Wang, Lin-Wang

    2007-04-25

    The electronic structure of nanowires in contact withmetallic electrodes of experimentally relevant sizes is calculated byincorporating the electrostatic polarization potential into the atomisticsingle particle Schrodinger equation. We show that the presence of anelectrode produces localized electron/hole states near the electrode, aphenomenon only exhibited in nanostructures and overlooked in the past.This phenomenon will have profound implications on electron transport insuch nanosystems. We calculate several electrode/nanowire geometries,with varying contact depths and nanowire radii. We demonstrate the changein the band gap of up to 0.5 eV in 3 nm diameter CdSe nanowires andcalculate the magnitude of the applied electric field necessary toovercome the localization.

  11. 5f{sup N} configurations and x-ray spectra of actinides

    SciTech Connect

    Kulagin, N.A.

    1995-04-01

    The electronic structure of 5f{sup N} configurations and the characteristic X-ray radiation energies for an entire actinium series are calculated using the Hartree-Fock-Pauli approximation, and the variations obtained are analyzed. The electrostatic and magnetic parameters of these ions, as well as energies of their K and L lines, exhibit essentially nonlinear dependence on the nuclear charge and number of electrons. This fact evidences that simplified models of atomic structure are inapplicable to heavy ions.

  12. Electronic spectrum and localization of electronic states in aperiodic quantum dot chains

    NASA Astrophysics Data System (ADS)

    Korotaev, P. Yu.; Vekilov, Yu. Kh.; Kaputkina, N. E.

    2014-02-01

    The electronic energy spectra of aperiodic Thue-Morse, Rudin-Shapiro, and double-periodic quantum dot chains are investigated in the tight-binding approximation. The dependence of the spectrum on all parameters of a "mixed" aperiodic chain model is studied: the electronic energy at quantum dots and the hopping integrals. The electronic degree of localization in the chains under consideration is determined by analyzing the inverse participation ratio. Its spectral distribution and the dependence of the band-averaged degree of localization on these model parameters have been calculated. It is shown that a transition of the system's sites to a resonant state in which the degree of electron localization decreases, while an overlap between the subbands occurs in the spectrum is possible when the parameters are varied.

  13. DNA Electronic Fingerprints by Local Spectroscopy on Graphene

    NASA Astrophysics Data System (ADS)

    Balatsky, Alexander

    2013-03-01

    Working and scalable alternatives to the conventional chemical methods of DNA sequencing that are based on electronic/ionic signatures would revolutionize the field of sequencing. The approach of a single molecule imaging and spectroscopy with unprecedented resolution, achieved by Scanning Tunneling Spectroscopy (STS) and nanopore electronics could enable this revolution. We use the data from our group and others in applying this local scanning tunneling microscopy and illustrate possibilities of electronic sequencing of freeze dried deposits on graphene. We will present two types of calculated fingerprints: first in Local Density of States (LDOS) of DNA nucleotide bases (A,C,G,T) deposited on graphene. Significant base-dependent features in the LDOS in an energy range within few eV of the Fermi level were found in our calculations. These features can serve as electronic fingerprints for the identification of individual bases in STS. In the second approach we present calculated base dependent electronic transverse conductance as DNA translocates through the graphene nanopore. Thus we argue that the fingerprints of DNA-graphene hybrid structures may provide an alternative route to DNA sequencing using STS. Work supported by US DOE, NORDITA.

  14. Correlated cryogenic photoactivated localization microscopy and cryo-electron tomography.

    PubMed

    Chang, Yi-Wei; Chen, Songye; Tocheva, Elitza I; Treuner-Lange, Anke; Löbach, Stephanie; Søgaard-Andersen, Lotte; Jensen, Grant J

    2014-07-01

    Cryo-electron tomography (CET) produces three-dimensional images of cells in a near-native state at macromolecular resolution, but identifying structures of interest can be challenging. Here we describe a correlated cryo-PALM (photoactivated localization microscopy)-CET method for localizing objects within cryo-tomograms to beyond the diffraction limit of the light microscope. Using cryo-PALM-CET, we identified multiple and new conformations of the dynamic type VI secretion system in the crowded interior of Myxococcus xanthus.

  15. Correlated cryogenic photoactivated localization microscopy and electron cryotomography

    PubMed Central

    Chang, Yi-Wei; Chen, Songye; Tocheva, Elitza I.; Treuner-Lange, Anke; Löbach, Stephanie; Søgaard-Andersen, Lotte; Jensen, Grant J.

    2014-01-01

    Electron cryotomography (ECT) produces three-dimensional images of cells in a near-native state at macromolecular resolution, but identifying structures of interest can be challenging. Here we describe a correlated "cryo-PALM"-ECT method for localizing objects within cryotomograms to beyond the diffraction limit of the light microscope, and use it to identify multiple and new conformations of the dynamic type VI secretion system in the crowded interior of Myxococcus xanthus. PMID:24813625

  16. Nano-fEM: protein localization using photo-activated localization microscopy and electron microscopy.

    PubMed

    Watanabe, Shigeki; Richards, Jackson; Hollopeter, Gunther; Hobson, Robert J; Davis, Wayne M; Jorgensen, Erik M

    2012-12-03

    Mapping the distribution of proteins is essential for understanding the function of proteins in a cell. Fluorescence microscopy is extensively used for protein localization, but subcellular context is often absent in fluorescence images. Immuno-electron microscopy, on the other hand, can localize proteins, but the technique is limited by a lack of compatible antibodies, poor preservation of morphology and because most antigens are not exposed to the specimen surface. Correlative approaches can acquire the fluorescence image from a whole cell first, either from immuno-fluorescence or genetically tagged proteins. The sample is then fixed and embedded for electron microscopy, and the images are correlated (1-3). However, the low-resolution fluorescence image and the lack of fiducial markers preclude the precise localization of proteins. Alternatively, fluorescence imaging can be done after preserving the specimen in plastic. In this approach, the block is sectioned, and fluorescence images and electron micrographs of the same section are correlated (4-7). However, the diffraction limit of light in the correlated image obscures the locations of individual molecules, and the fluorescence often extends beyond the boundary of the cell. Nano-resolution fluorescence electron microscopy (nano-fEM) is designed to localize proteins at nano-scale by imaging the same sections using photo-activated localization microscopy (PALM) and electron microscopy. PALM overcomes the diffraction limit by imaging individual fluorescent proteins and subsequently mapping the centroid of each fluorescent spot (8-10). We outline the nano-fEM technique in five steps. First, the sample is fixed and embedded using conditions that preserve the fluorescence of tagged proteins. Second, the resin blocks are sectioned into ultrathin segments (70-80 nm) that are mounted on a cover glass. Third, fluorescence is imaged in these sections using the Zeiss PALM microscope. Fourth, electron dense structures are

  17. The local electronic structure of alpha-Li3N.

    PubMed

    Fister, T T; Seidler, G T; Shirley, E L; Vila, F D; Rehr, J J; Nagle, K P; Linehan, J C; Cross, J O

    2008-07-28

    New theoretical and experimental investigations of the occupied and unoccupied local electronic densities of states (DOS) are reported for alpha-Li(3)N. Band-structure and density-functional theory calculations confirm the absence of covalent bonding character. However, real-space full-multiple-scattering (RSFMS) calculations of the occupied local DOS find less extreme nominal valences than have previously been proposed. Nonresonant inelastic x-ray scattering, RSFMS calculations, and calculations based on the Bethe-Salpeter equation are used to characterize the unoccupied electronic final states local to both the Li and N sites. There is a good agreement between experiment and theory. Throughout the Li 1s near-edge region, both experiment and theory find strong similarities in the s-and p-type components of the unoccupied local final DOS projected onto an orbital angular momentum basis (l-DOS). An unexpected, significant correspondence exists between the near-edge spectra for the Li 1s and N 1s initial states. We argue that both spectra are sampling essentially the same final DOS due to the combination of long core-hole lifetimes, long photoelectron lifetimes, and the fact that orbital angular momentum is the same for all relevant initial states. Such considerations may be generally applicable for low atomic number compounds.

  18. A mapping of the electron localization function for earth materials

    NASA Astrophysics Data System (ADS)

    Gibbs, G. V.; Cox, D. F.; Ross, N. L.; Crawford, T. D.; Burt, J. B.; Rosso, K. M.

    2005-06-01

    The electron localization function, ELF, generated for a number of geometry-optimized earth materials, provides a graphical representation of the spatial localization of the probability electron density distribution as embodied in domains ascribed to localized bond and lone pair electrons. The lone pair domains, displayed by the silica polymorphs quartz, coesite and cristobalite, are typically banana-shaped and oriented perpendicular to the plane of the SiOSi angle at ~0.60 Å from the O atom on the reflex side of the angle. With decreasing angle, the domains increase in magnitude, indicating an increase in the nucleophilic character of the O atom, rendering it more susceptible to potential electrophilic attack. The Laplacian isosurface maps of the experimental and theoretical electron density distribution for coesite substantiates the increase in the size of the domain with decreasing angle. Bond pair domains are displayed along each of the SiO bond vectors as discrete concave hemispherically-shaped domains at ~0.70 Å from the O atom. For more closed-shell ionic bonded interactions, the bond and lone pair domains are often coalesced, resulting in concave hemispherical toroidal-shaped domains with local maxima centered along the bond vectors. As the shared covalent character of the bonded interactions increases, the bond and lone pair domains are better developed as discrete domains. ELF isosurface maps generated for the earth materials tremolite, diopside, talc and dickite display banana-shaped lone pair domains associated with the bridging O atoms of SiOSi angles and concave hemispherical toroidal bond pair domains associated with the nonbridging ones. The lone pair domains in dickite and talc provide a basis for understanding the bonded interactions between the adjacent neutral layers. Maps were also generated for beryl, cordierite, quartz, low albite, forsterite, wadeite, åkermanite, pectolite, periclase, hurlbutite, thortveitite and vanthoffite. Strategies

  19. A Mapping of the Electron Localization Function for Earth Materials

    SciTech Connect

    Gibbs, Gerald V.; Cox, David F.; Ross, Nancy; Crawford, T Daniel; Burt, Jason; Rosso, Kevin M.

    2005-06-01

    The electron localization function, ELF, generated for a number of geometry-optimized earth materials, provides a graphical representation of the spatial localization of the probability electron density distribution as embodied in domains ascribed to localized bond and lone pair electrons. The lone pair domains, displayed by the silica polymorphs quartz, coesite and cristobalite, are typically banana-shaped and oriented perpendicular to the plane of the SiOSi angle at ~0.60 Å from the O atom on the reflex side of the angle. With decreasing angle, the domains increase in magnitude, indicating an increase in the nucleophilic character of the O atom, rendering it more susceptible to potential electrophilic attack. The Laplacian isosurface maps of the experimental and theoretical electron density distribution for coesite substantiates the increase in the size of the domain with decreasing angle. Bond pair domains are displayed along each of the SiO bond vectors as discrete concave hemispherically-shaped domains at ~0.70 Å from the O atom. For more closed-shell ionic bonded interactions, the bond and lone pair domains are often coalesced, resulting in concave hemispherical toroidal-shaped domains with local maxima centered along the bond vectors. As the shared covalent character of the bonded interactions increases, the bond and lone pair domains are better developed as discrete domains. ELF isosurface maps generated for the earth materials tremolite, diopside, talc and dickite display banana-shaped lone pair domains associated with the bridging O atoms of SiOSi angles and concave hemispherical toroidal bond pair domains associated with the nonbridging ones. The lone pair domains in dickite and talc provide a basis for understanding the bonded interactions between the adjacent neutral layers. Maps were also generated for beryl, cordierite, quartz, low albite, forsterite, wadeite, åkermanite, pectolite, periclase, hurlbutite, thortveitite and vanthoffite. Strategies

  20. ANALYSIS OF THE TANK 5F FINAL CHARATERIZATION SAMPLES-2011

    SciTech Connect

    Oji, L.; Diprete, D.; Coleman, C.; Hay, M.

    2012-01-20

    The Savannah River National Laboratory (SRNL) was requested by SRR to provide sample preparation and analysis of the Tank 5F final characterization samples to determine the residual tank inventory prior to grouting. Two types of samples were collected and delivered to SRNL: floor samples across the tank and subsurface samples from mounds near risers 1 and 5 of Tank 5F. These samples were taken from Tank 5F between January and March 2011. These samples from individual locations in the tank (nine floor samples and six mound Tank 5F samples) were each homogenized and combined in a given proportion into 3 distinct composite samples to mimic the average composition in the entire tank. These Tank 5F composite samples were analyzed for radiological, chemical and elemental components. Additional measurements performed on the Tank 5F composite samples include bulk density and water leaching of the solids to account for water soluble species. With analyses for certain challenging radionuclides as the exception, all composite Tank 5F samples were analyzed and reported in triplicate. The target detection limits for isotopes analyzed were based on customer desired detection limits as specified in the technical task request documents. SRNL developed new methodologies to meet these target detection limits and provide data for the extensive suite of components. While many of the target detection limits were met for the species characterized for Tank 5F, as specified in the technical task request, some were not met. In a few cases, the relatively high levels of radioactive species of the same element or a chemically similar element precluded the ability to measure some isotopes to low levels. The Technical Task Request allows that while the analyses of these isotopes is needed, meeting the detection limits for these isotopes is a lower priority than meeting detection limits for the other specified isotopes. The isotopes whose detection limits were not met in all cases included the

  1. ANALYSIS OF THE TANK 5F FINAL CHARACTERIZATION SAMPLES-2011

    SciTech Connect

    Oji, L.; Diprete, D.; Coleman, C.; Hay, M.

    2012-08-03

    The Savannah River National Laboratory (SRNL) was requested by SRR to provide sample preparation and analysis of the Tank 5F final characterization samples to determine the residual tank inventory prior to grouting. Two types of samples were collected and delivered to SRNL: floor samples across the tank and subsurface samples from mounds near risers 1 and 5 of Tank 5F. These samples were taken from Tank 5F between January and March 2011. These samples from individual locations in the tank (nine floor samples and six mound Tank 5F samples) were each homogenized and combined in a given proportion into 3 distinct composite samples to mimic the average composition in the entire tank. These Tank 5F composite samples were analyzed for radiological, chemical and elemental components. Additional measurements performed on the Tank 5F composite samples include bulk density and water leaching of the solids to account for water soluble species. With analyses for certain challenging radionuclides as the exception, all composite Tank 5F samples were analyzed and reported in triplicate. The target detection limits for isotopes analyzed were based on customer desired detection limits as specified in the technical task request documents. SRNL developed new methodologies to meet these target detection limits and provide data for the extensive suite of components. While many of the target detection limits were met for the species characterized for Tank 5F, as specified in the technical task request, some were not met. In a few cases, the relatively high levels of radioactive species of the same element or a chemically similar element precluded the ability to measure some isotopes to low levels. The Technical Task Request allows that while the analyses of these isotopes is needed, meeting the detection limits for these isotopes is a lower priority than meeting detection limits for the other specified isotopes. The isotopes whose detection limits were not met in all cases included the

  2. Analysis Of The Tank 5F Final Characterization Samples-2011

    SciTech Connect

    Oji, L. N.; Diprete, D.; Coleman, C. J.; Hay, M. S.

    2012-09-27

    The Savannah River National Laboratory (SRNL) was requested by SRR to provide sample preparation and analysis of the Tank 5F final characterization samples to determine the residual tank inventory prior to grouting. Two types of samples were collected and delivered to SRNL: floor samples across the tank and subsurface samples from mounds near risers 1 and 5 of Tank 5F. These samples were taken from Tank 5F between January and March 2011. These samples from individual locations in the tank (nine floor samples and six mound Tank 5F samples) were each homogenized and combined in a given proportion into 3 distinct composite samples to mimic the average composition in the entire tank. These Tank 5F composite samples were analyzed for radiological, chemical and elemental components. Additional measurements performed on the Tank 5F composite samples include bulk density and water leaching of the solids to account for water soluble species. With analyses for certain challenging radionuclides as the exception, all composite Tank 5F samples were analyzed and reported in triplicate. The target detection limits for isotopes analyzed were based on customer desired detection limits as specified in the technical task request documents. SRNL developed new methodologies to meet these target detection limits and provide data for the extensive suite of components. While many of the target detection limits were met for the species characterized for Tank 5F, as specified in the technical task request, some were not met. In a few cases, the relatively high levels of radioactive species of the same element or a chemically similar element precluded the ability to measure some isotopes to low levels. The Technical Task Request allows that while the analyses of these isotopes is needed, meeting the detection limits for these isotopes is a lower priority than meeting detection limits for the other specified isotopes. The isotopes whose detection limits were not met in all cases included the

  3. Plasmonic hot electron transport drives nano-localized chemistry

    PubMed Central

    Cortés, Emiliano; Xie, Wei; Cambiasso, Javier; Jermyn, Adam S.; Sundararaman, Ravishankar; Narang, Prineha; Schlücker, Sebastian; Maier, Stefan A.

    2017-01-01

    Nanoscale localization of electromagnetic fields near metallic nanostructures underpins the fundamentals and applications of plasmonics. The unavoidable energy loss from plasmon decay, initially seen as a detriment, has now expanded the scope of plasmonic applications to exploit the generated hot carriers. However, quantitative understanding of the spatial localization of these hot carriers, akin to electromagnetic near-field maps, has been elusive. Here we spatially map hot-electron-driven reduction chemistry with 15 nm resolution as a function of time and electromagnetic field polarization for different plasmonic nanostructures. We combine experiments employing a six-electron photo-recycling process that modify the terminal group of a self-assembled monolayer on plasmonic silver nanoantennas, with theoretical predictions from first-principles calculations of non-equilibrium hot-carrier transport in these systems. The resulting localization of reactive regions, determined by hot-carrier transport from high-field regions, paves the way for improving efficiency in hot-carrier extraction science and nanoscale regio-selective surface chemistry. PMID:28348402

  4. Plasmonic hot electron transport drives nano-localized chemistry.

    PubMed

    Cortés, Emiliano; Xie, Wei; Cambiasso, Javier; Jermyn, Adam S; Sundararaman, Ravishankar; Narang, Prineha; Schlücker, Sebastian; Maier, Stefan A

    2017-03-28

    Nanoscale localization of electromagnetic fields near metallic nanostructures underpins the fundamentals and applications of plasmonics. The unavoidable energy loss from plasmon decay, initially seen as a detriment, has now expanded the scope of plasmonic applications to exploit the generated hot carriers. However, quantitative understanding of the spatial localization of these hot carriers, akin to electromagnetic near-field maps, has been elusive. Here we spatially map hot-electron-driven reduction chemistry with 15 nm resolution as a function of time and electromagnetic field polarization for different plasmonic nanostructures. We combine experiments employing a six-electron photo-recycling process that modify the terminal group of a self-assembled monolayer on plasmonic silver nanoantennas, with theoretical predictions from first-principles calculations of non-equilibrium hot-carrier transport in these systems. The resulting localization of reactive regions, determined by hot-carrier transport from high-field regions, paves the way for improving efficiency in hot-carrier extraction science and nanoscale regio-selective surface chemistry.

  5. Site Sensitivity and local electronic symmetries in carboranes

    NASA Astrophysics Data System (ADS)

    Fister, T. T.; Seidler, G. T.; Vila, F. D.; Cross, J. O.; Linehan, J. C.

    2007-03-01

    Icosohedral carboranes containing ten boron and two carbon atoms are seeing renewed interest because of their potential use in new cancer and AIDS therapies. These molecules have flexible geometries which allow bonding to three types of carbon sites (e.g. ortho-, para-, and meta- configurations). Using a new multielement spectrometer, we present the first x-ray Raman scattering (XRS) study on each isomer with excited state spectra taken from the both the carbon and boron 1s states. The change in the electronic structure between the isomers is most pronounced in the carbon spectrum, where the position in the edge confirms prior density functional theory calculations. With the boron spectra, we used the unique momentum transfer dependence of XRS to extract the symmetry components of the density of unoccupied states, i.e. the l-DOS. These results give an improved picture of the local electronic properties of the carboranes.

  6. Symmetry breaking and hole localization in multiple core electron ionization.

    PubMed

    Carravetta, V; Ågren, H

    2013-08-08

    Motivated by recent opportunitites to study hollow molecules with multiple core holes offered by X-ray free electron lasers, we revisit the core-hole localization and symmetry breaking problem, now studying ionization of more than one core electron. It is shown, using a N2 molecule with one, two, three, and four core holes, for example, that in a multiconfigurational determination of the core ionization potentials employing a molecular point group with broken inversion symmetry, one particular configuration is sufficient to account for the symmetry breaking relaxation energy in an independent particle approximation in the case of one or three holes, whereas the choice of point group symmetry is unessential for two and four holes. The relaxation energy follows a quadratic dependence on the number of holes in both representations.

  7. Electronic structure and localized states in a model amorphous silicon

    NASA Astrophysics Data System (ADS)

    Allan, G.; Delerue, C.; Lannoo, M.

    1998-03-01

    The electronic structure of a model amorphous silicon (a-Si) represented by a supercell of 4096 silicon atoms [B.R. Djordjevic, M.F. Thorpe, and F. Wooten, Phys. Rev. B 52, 5685 (1995)] and of a model hydrogenated amorphous silicon (a-Si:H) that we have built from the a-Si model are calculated in the tight-binding approximation. The band edges near the gap are characterized by exponential tails of localized states induced mainly by the variations in bond angles. The spatial localization of the states is compared between a-Si and a-Si:H. Comparison with experiments suggests that the structural models give good descriptions of the amorphous materials.

  8. The local electron affinity for non-minimal basis sets.

    PubMed

    Clark, Timothy

    2010-07-01

    A technique known as intensity filtering is introduced to select valence-like virtual orbitals for calculating the local electron affinity, EA(L). Intensity filtering allows EA(L) to be calculated using semiempirical molecular orbital techniques that include polarisation functions. Without intensity filtering, such techniques yield spurious EA(L) values that are dominated by the polarisation functions. As intensity filtering should also be applicable for ab initio or density functional theory calculations with large basis sets, it also makes EA(L) available for these techniques.

  9. Local atomic order, electronic structure and electron transport properties of Cu-Zr metallic glasses

    NASA Astrophysics Data System (ADS)

    Antonowicz, J.; Pietnoczka, A.; Pekała, K.; Latuch, J.; Evangelakis, G. A.

    2014-05-01

    We studied atomic and electronic structures of binary Cu-Zr metallic glasses (MGs) using combined experimental and computational methods including X-ray absorption fine structure spectroscopy, electrical resistivity, thermoelectric power (TEP) measurements, molecular dynamics (MD) simulations, and ab-initio calculations. The results of MD simulations and extended X-ray absorption fine structure analysis indicate that atomic order of Cu-Zr MGs and can be described in terms of interpenetrating icosahedral-like clusters involving five-fold symmetry. MD configurations were used as an input for calculations of theoretical electronic density of states (DOS) functions which exhibits good agreement with the experimental X-ray absorption near-edge spectra. We found no indication of minimum of DOS at Fermi energy predicted by Mott's nearly free electron (NFE) model for glass-forming alloys. The theoretical DOS was subsequently used to test Mott's model describing the temperature variation of electrical resistivity and thermoelectric power of transition metal-based MGs. We demonstrate that the measured temperature variations of electrical resistivity and TEP remain in a contradiction with this model. On the other hand, the experimental temperature dependence of electrical resistivity can be explained by incipient localization of conduction electrons. It is shown that weak localization model works up to relatively high temperatures when localization is destroyed by phonons. Our results indicate that electron transport properties of Cu-Zr MGs are dominated by localization effects rather than by electronic structure. We suggest that NFE model fails to explain a relatively high glass-forming ability of binary Cu-Zr alloys.

  10. Local atomic order, electronic structure and electron transport properties of Cu-Zr metallic glasses

    SciTech Connect

    Antonowicz, J. Pietnoczka, A.; Pękała, K.; Latuch, J.; Evangelakis, G. A.

    2014-05-28

    We studied atomic and electronic structures of binary Cu-Zr metallic glasses (MGs) using combined experimental and computational methods including X-ray absorption fine structure spectroscopy, electrical resistivity, thermoelectric power (TEP) measurements, molecular dynamics (MD) simulations, and ab-initio calculations. The results of MD simulations and extended X-ray absorption fine structure analysis indicate that atomic order of Cu-Zr MGs and can be described in terms of interpenetrating icosahedral-like clusters involving five-fold symmetry. MD configurations were used as an input for calculations of theoretical electronic density of states (DOS) functions which exhibits good agreement with the experimental X-ray absorption near-edge spectra. We found no indication of minimum of DOS at Fermi energy predicted by Mott's nearly free electron (NFE) model for glass-forming alloys. The theoretical DOS was subsequently used to test Mott's model describing the temperature variation of electrical resistivity and thermoelectric power of transition metal-based MGs. We demonstrate that the measured temperature variations of electrical resistivity and TEP remain in a contradiction with this model. On the other hand, the experimental temperature dependence of electrical resistivity can be explained by incipient localization of conduction electrons. It is shown that weak localization model works up to relatively high temperatures when localization is destroyed by phonons. Our results indicate that electron transport properties of Cu-Zr MGs are dominated by localization effects rather than by electronic structure. We suggest that NFE model fails to explain a relatively high glass-forming ability of binary Cu-Zr alloys.

  11. Computation of Local and Global Properties of the Electron Localization Function Topology in Crystals.

    PubMed

    Contreras-García, J; Pendás, A Martín; Recio, J M; Silvi, B

    2009-01-13

    We present a novel computational procedure, general, automated, and robust, for the analysis of local and global properties of the electron localization function (ELF) in crystalline solids. Our algorithm successfully faces the two main shortcomings of the ELF analysis in crystals: (i) the automated identification and characterization of the ELF induced topology in periodic systems, which is impeded by the great number and concentration of critical points in crystalline cells, and (ii) the localization of the zero flux surfaces and subsequent integration of basins, whose difficulty is due to the diverse (in many occasions very flat or very steep) ELF profiles connecting the set of critical points. Application of the new code to representative crystals exhibiting different bonding patterns is carried out in order to show the performance of the algorithm and the conceptual possibilities offered by the complete characterization of the ELF topology in solids.

  12. Creating and Probing Graphene Electron Optics with Local Scanning Probes

    NASA Astrophysics Data System (ADS)

    Stroscio, Joseph

    Ballistic propagation and the light-like dispersion of graphene charge carriers make graphene an attractive platform for optics-inspired graphene electronics where gate tunable potentials can control electron refraction and transmission. In analogy to optical wave propagation in lenses, mirrors and metamaterials, gate potentials can be used to create a negative index of refraction for Veselago lensing and Fabry-Pérot interferometers. In circular geometries, gate potentials can induce whispering gallery modes (WGM), similar to optical and acoustic whispering galleries albeit on a much smaller length scale. Klein scattering of Dirac carriers plays a central role in determining the coherent propagation of electron waves in these resonators. In this talk, I examine the probing of electron resonators in graphene confined by linear and circular gate potentials with the scanning tunneling microscope (STM). The tip in the STM tunnel junction serves both as a tunable local gate potential, and as a probe of the graphene states through tunneling spectroscopy. A combination of a back gate potential, Vg, and tip potential, Vb, creates and controls a circular pn junction that confines the WGM graphene states. The resonances are observed in two separate channels in the tunneling spectroscopy experiment: first, by directly tunneling into the state at the bias energy eVb, and, second, by tunneling from the resonance at the Fermi level as the state is gated by the tip potential. The second channel produces a fan-like set of WGM peaks, reminiscent of the fringes seen in planar geometries by transport measurements. The WGM resonances split in a small applied magnetic field, with a large energy splitting approaching the WGM spacing at 0.5 T. These results agree well with recent theory on Klein scattering in graphene electron resonators. This work is done in collaboration with Y. Zhao, J. Wyrick, F.D. Natterer, J. F. Rodriquez-Nieva, C. Lewandoswski, K. Watanabe, T. Taniguchi, N. B

  13. An optimized locally adaptive non-local means denoising filter for cryo-electron microscopy data.

    PubMed

    Wei, Dai-Yu; Yin, Chang-Cheng

    2010-12-01

    Cryo-electron microscopy (cryo-EM) now plays an important role in structural analysis of macromolecular complexes, organelles and cells. However, the cryo-EM images obtained close to focus and under low dose conditions have a very high level of noise and a very low contrast, which hinders high-resolution structural analysis. Here, an optimized locally adaptive non-local (LANL) means filter, which can preserve signal details and simultaneously significantly suppress noise for cryo-EM data, is presented. This filter takes advantage of a wide range of pixels to estimate the denoised pixel values instead of the traditional filter that only uses pixels in the local neighborhood. The filter performed well on simulated data and showed promising results on raw cryo-EM images and tomograms. The predominant advantage of this optimized LANL-means filter is the structural signal and the background are clearly distinguishable. This locally adaptive non-local means filter may become a useful tool in the analysis of cryo-EM data, such as automatic particle picking, extracting structural features and segmentation of tomograms.

  14. Local Electronic And Dielectric Properties at Nanosized Interfaces

    SciTech Connect

    Bonnell, Dawn A.

    2015-02-23

    Final Report to the Department of Energy for period 6/1/2000 to 11/30/2014 for Grant # DE-FG02-00ER45813-A000 to the University of Pennsylvania Local Electronic And Dielectric Properties at Nanosized Interfaces PI: Dawn Bonnell The behavior of grain boundaries and interfaces has been a focus of fundamental research for decades because variations of structure and composition at interfaces dictate mechanical, electrical, optical and dielectric properties in solids. Similarly, the consequence of atomic and electronic structures of surfaces to chemical and physical interactions are critical due to their implications to catalysis and device fabrication. Increasing fundamental understanding of surfaces and interfaces has materially advanced technologies that directly bear on energy considerations. Currently, exciting developments in materials processing are enabling creative new electrical, optical and chemical device configurations. Controlled synthesis of nanoparticles, semiconducting nanowires and nanorods, optical quantum dots, etc. along with a range of strategies for assembling and patterning nanostructures portend the viability of new devices that have the potential to significantly impact the energy landscape. As devices become smaller the impact of interfaces and surfaces grows geometrically. As with other nanoscale phenomena, small interfaces do not exhibit the same properties as do large interfaces. The size dependence of interface properties had not been explored and understanding at the most fundamental level is necessary to the advancement of nanostructured devices. An equally important factor in the behavior of interfaces in devices is the ability to examine the interfaces under realistic conditions. For example, interfaces and boundaries dictate the behavior of oxide fuel cells which operate at extremely high temperatures in dynamic high pressure chemical environments. These conditions preclude the characterization of local properties during fuel cell

  15. How localized is ``local?'' Efficiency vs. accuracy of O(N) domain decomposition in local orbital based all-electron electronic structure theory

    NASA Astrophysics Data System (ADS)

    Havu, Vile; Blum, Volker; Scheffler, Matthias

    2007-03-01

    Numeric atom-centered local orbitals (NAO) are efficient basis sets for all-electron electronic structure theory. The locality of NAO's can be exploited to render (in principle) all operations of the self-consistency cycle O(N). This is straightforward for 3D integrals using domain decomposition into spatially close subsets of integration points, enabling critical computational savings that are effective from ˜tens of atoms (no significant overhead for smaller systems) and make large systems (100s of atoms) computationally feasible. Using a new all-electron NAO-based code,^1 we investigate the quantitative impact of exploiting this locality on two distinct classes of systems: Large light-element molecules [Alanine-based polypeptide chains (Ala)n], and compact transition metal clusters. Strict NAO locality is achieved by imposing a cutoff potential with an onset radius rc, and exploited by appropriately shaped integration domains (subsets of integration points). Conventional tight rc<= 3å have no measurable accuracy impact in (Ala)n, but introduce inaccuracies of 20-30 meV/atom in Cun. The domain shape impacts the computational effort by only 10-20 % for reasonable rc. ^1 V. Blum, R. Gehrke, P. Havu, V. Havu, M. Scheffler, The FHI Ab Initio Molecular Simulations (aims) Project, Fritz-Haber-Institut, Berlin (2006).

  16. Local electron-electron interaction strength in ferromagnetic nickel determined by spin-polarized positron annihilation.

    PubMed

    Ceeh, Hubert; Weber, Josef Andreas; Weber, Josef Andreass; Böni, Peter; Leitner, Michael; Benea, Diana; Chioncel, Liviu; Ebert, Hubert; Minár, Jan; Vollhardt, Dieter; Hugenschmidt, Christoph

    2016-02-16

    We employ a positron annihilation technique, the spin-polarized two-dimensional angular correlation of annihilation radiation (2D-ACAR), to measure the spin-difference spectra of ferromagnetic nickel. The experimental data are compared with the theoretical results obtained within a combination of the local spin density approximation (LSDA) and the many-body dynamical mean-field theory (DMFT). We find that the self-energy defining the electronic correlations in Ni leads to anisotropic contributions to the momentum distribution. By direct comparison of the theoretical and experimental results we determine the strength of the local electronic interaction U in ferromagnetic Ni as 2.0 ± 0.1 eV.

  17. Local electron-electron interaction strength in ferromagnetic nickel determined by spin-polarized positron annihilation

    PubMed Central

    Ceeh, Hubert; Weber, Josef Andreass; Böni, Peter; Leitner, Michael; Benea, Diana; Chioncel, Liviu; Ebert, Hubert; Minár, Jan; Vollhardt, Dieter; Hugenschmidt, Christoph

    2016-01-01

    We employ a positron annihilation technique, the spin-polarized two-dimensional angular correlation of annihilation radiation (2D-ACAR), to measure the spin-difference spectra of ferromagnetic nickel. The experimental data are compared with the theoretical results obtained within a combination of the local spin density approximation (LSDA) and the many-body dynamical mean-field theory (DMFT). We find that the self-energy defining the electronic correlations in Ni leads to anisotropic contributions to the momentum distribution. By direct comparison of the theoretical and experimental results we determine the strength of the local electronic interaction U in ferromagnetic Ni as 2.0 ± 0.1 eV. PMID:26879249

  18. Local electronic structures in electron-doped cuprates with coexisting orders

    NASA Astrophysics Data System (ADS)

    Liu, Bin; Hu, Xiao

    2010-12-01

    Motivated by the observation of a so-called non-monotonic gap in recent angle-resolved photoemission spectroscopy measurement, we study the local electronic structure near impurities in electron-doped cuprates by considering the influence of antiferromagnetic (AF) spin-density-wave (SDW) order. We find that the evolution of density of states (DOS) with AF SDW order clearly indicates the non-monotonic d-wave gap behavior. More interestingly, the local DOS for spin-up is much different from that for spin-down with increasing AF SDW order. As a result, the impurity induced resonance state near the Fermi energy exhibits a spin-polarized feature. These features can be detected by spin-polarized scanning tunneling microscopy experiments.

  19. Electron-electron interaction, weak localization and spin valve effect in vertical-transport graphene devices

    SciTech Connect

    Long, Mingsheng; Gong, Youpin; Wei, Xiangfei; Zhu, Chao; Xu, Jianbao; Liu, Ping; Guo, Yufen; Li, Weiwei; Liu, Liwei; Liu, Guangtong

    2014-04-14

    We fabricated a vertical structure device, in which graphene is sandwiched between two asymmetric ferromagnetic electrodes. The measurements of electron and spin transport were performed across the combined channels containing the vertical and horizontal components. The presence of electron-electron interaction (EEI) was found not only at low temperatures but also at moderate temperatures up to ∼120 K, and EEI dominates over weak localization (WL) with and without applying magnetic fields perpendicular to the sample plane. Moreover, spin valve effect was observed when magnetic filed is swept at the direction parallel to the sample surface. We attribute the EEI and WL surviving at a relatively high temperature to the effective suppress of phonon scattering in the vertical device structure. The findings open a way for studying quantum correlation at relatively high temperature.

  20. Electronic energy transfer: Localized operator partitioning of electronic energy in composite quantum systems

    NASA Astrophysics Data System (ADS)

    Khan, Yaser; Brumer, Paul

    2012-11-01

    A Hamiltonian based approach using spatially localized projection operators is introduced to give precise meaning to the chemically intuitive idea of the electronic energy on a quantum subsystem. This definition facilitates the study of electronic energy transfer in arbitrarily coupled quantum systems. In particular, the decomposition scheme can be applied to molecular components that are strongly interacting (with significant orbital overlap) as well as to isolated fragments. The result defines a consistent electronic energy at all internuclear distances, including the case of separated fragments, and reduces to the well-known Förster and Dexter results in their respective limits. Numerical calculations of coherent energy and charge transfer dynamics in simple model systems are presented and the effect of collisionally induced decoherence is examined.

  1. MAILROOM- A LOCAL AREA NETWORK ELECTRONIC MAIL PROGRAM

    NASA Technical Reports Server (NTRS)

    Weiner, M. J.

    1994-01-01

    The Mailroom program is a Local Area Network (LAN) electronic mail program. It allows LAN users to electronically exchange notes, letters, reminders, or any sort of communication via their computer. The Mailroom program links all LAN users into a communication circle where messages can be created, sent, copied, printed, downloaded, uploaded, and deleted through a series of menu-driven screens. Mailroom includes a feature which allows users to determine if a message they have sent has been read by the receiver. Each user must be separately installed and removed from Mailroom as they join or leave the network. Mailroom comes with a program that accomplishes this with minimum of effort on the part of the Network Administrator/Manager. There is also a program that allows the Network Administrator/Manager to install Mailroom on each user's workstation so that on execution of Mailroom the user's station may be identified and the configurations settings activated. It will create its own configuration and data/supporting files during the setup and installation process. The Mailroom program is written in Microsoft QuickBasic. It was developed to run on networked IBM XT/ATs or compatibles and requires that all participating workstations share a common drive. It has been implemented under DOS 3.2 and has a memory requirement of 71K. Mailroom was developed in 1988.

  2. Electron microscopic localization of cytoplasmic myosin with ferritin- labeled antibodies

    PubMed Central

    1981-01-01

    We localized myosin in vertebrate nonmuscle cells by electron microscopy using purified antibodies coupled with ferritin. Native and formaldehyde-fixed filaments of purified platelet myosin filaments each consisting of approximately 30 myosin molecules bound an equivalent number of ferritin-antimyosin conjugates. In preparations of crude platelet actomyosin, the ferritin-antimyosin bound exclusively to similar short, 10-15 nm wide filaments. In both cases, binding of the ferritin-antimyosin to the myosin filaments was blocked by preincubation with unlabeled antimyosin. With indirect fluorescent antibody staining at the light microscope level, we found that the ferritin-antimyosin and unlabeled antimyosin stained HeLa cells identically, with the antibodies concentrated in 0.5-microns spots along stress fibers. By electron microscopy, we found that the concentration of ferritin-antimyosin in the dense regions of stress fibers was five to six times that in the intervening less dense regions, 20 times that in the cytoplasmic matrix, and 100 times that in the nucleus. These concentration differences may account for the light microscope antibody staining pattern of spread interphase cells. Some, but certainly not all, of the ferritin-antimyosin was associated with 10-15-nm filaments. In mouse intestinal epithelial cells, ferritin- antimyosin was located almost exclusively in the terminal web. In isolated brush borders exposed to 5 mM MgCl2, ferritin-antimyosin was also concentrated in the terminal web associated with 10-15-nm filaments. PMID:7193682

  3. The local electronic structure of α-Li3N

    SciTech Connect

    Fister, Timothy T.; Siedler, Gerald T.; Shirley, E. L.; Vila, Fernando D.; Nagle, Kenneth P.; Rehr, John J.; Linehan, John C.; Cross, Julie O.

    2008-07-28

    We investigate the local electronic structure of α-Li3N by the combination of nonresonant inelastic x-ray scattering measurements and three independent ab initio theoretical treatments. Experimental determination of the local final density of states projected onto an orbital angular momentum basis (l-DOS) for Li 1s initial states finds strong similarities in the s- and p-DOS throughout the near-edge region, which we attribute to the 3-fold rotational symmetry about Li sites in the Li2N sheets of α-Li3N. We also find a significant correspondence between the near-edge spectra for the Li 1s and N 1s contributions to the NRIXS signal. This is unexpected, as such behavior is typically associated with covalent materials whereas α-Li3N is strongly ionic. We explain that such similarity in the DOS at different sites in either ionic or covalent systems may occur when the core-hole lifetimes are very long, so that the lifetime of the photoelectron is the dominant factor in cutting off high-order multiple scattering in the near-edge regime. This work was supported by the U.S. Department of Energy's Office of Basic Energy Sciences. The Pacific Northwest National Laboratory is operated by Battelle for DOE.

  4. Local electronic, sensing and optical properties of carbon nanotubes

    NASA Astrophysics Data System (ADS)

    Staii, Cristian

    The work presented in this thesis is focused on the electronic and optical properties of single wall carbon nanotubes (swCNs). In a first set of experiments we investigate the local electronic properties of swCNs using novel scanning probe microscopies. We use Scanning Gate Microscopy (SGM) to measure the energy of the resonant scattering centers in metallic swCNs, and to show the local nature of the memory effect observed in swCN field effect transistors (swCN-FETs). We also combine Impedance Spectroscopy and SGM to measure the high frequency properties of swCN-FETs. These experiments provide the first observations concerning the role of individual defects at high frequencies. The results are consistent with a simple parallel R-C circuit model for the swCN-FET. Furthermore, we present a quantitative model for the phase shifts observed in Scanning Conductance Microscopy (SCM) and demonstrate that this can be used to investigate the electronic properties of nanoscale samples without requiring electrical contacts. We provide a general method based on SCM that can be used to measure the dielectric constant of nanoscale objects. In a second set of experiments we demonstrate that swCN-FETs functionalized with single stranded DNA (ss-DNA) act as highly sensitive chemical sensors. The ss-DNA decorated swCN-FETs are sensitive to chemical species (odors) that do not cause a detectable response in non-functionalized swCN-FETs. Moreover, odor responses of these devices are different in sign and magnitude for different odors, and the odor response characteristics are dependent on the base sequence of the ss-DNA used to decorate the swCN. These results suggest that swCN-FET functionalized with ss-DNA and related molecules (RNA, aptamers, etc) are extremely promising candidates for sensing applications. Finally, we present photoluminescence measurements on individual swCNs, freely suspended across open apertures. These experiments show asymmetric peak line shapes, with line

  5. F-5F Shark Nose radome lightning test

    NASA Technical Reports Server (NTRS)

    Scott, G. W.

    1980-01-01

    A unique F-5F radome wtih a geometry similar to a Shark Nose profile was tested with a high voltage Marx generator, 1,200,000 volts in order to demonstrate the effectiveness of the lightning protection system with currents from 5,000 amperes or greater. An edge discontinuity configuration is a characteristic feature in the forward region of the radome and occasionally serves as an attachment point. The results of nineteen attachment tests at various aspect angles with an air gap of one meter indicated that no damage occurred to the dielectric material of the radom. The test proved the effectiveness of the lightning protection system.

  6. Oxalate Mass Balance During Chemical Cleaning in Tank 5F

    SciTech Connect

    Poirier, M.; Fink, S.

    2011-07-08

    The Savannah River Site (SRS) is preparing Tank 5F for closure. The first step in preparing the tank for closure is mechanical sludge removal. Following mechanical sludge removal, SRS performed chemical cleaning with oxalic acid to remove the sludge heel. Personnel are currently assessing the effectiveness of the chemical cleaning to determine whether the tank is ready for closure. SRS personnel collected liquid samples during chemical cleaning and submitted them to Savannah River National Laboratory (SRNL) for analysis. Following chemical cleaning, they collected a solid sample (also known as 'process sample') and submitted it to SRNL for analysis. The authors analyzed these samples to assess the effectiveness of the chemical cleaning process. Analysis of the anions showed the measured oxalate removed from Tank 5F to be approximately 50% of the amount added in the oxalic acid. To close the oxalate mass balance, the author collected solid samples, leached them with nitric acid, and measured the concentration of cations and anions in the leachate.

  7. Localized electrons on a lattice with incommensurate magnetic flux

    NASA Astrophysics Data System (ADS)

    Fishman, Shmuel; Shapir, Yonathan; Wang, Xiang-Rong

    1992-11-01

    The magnetic-field effects on lattice wave functions of Hofstadter electrons strongly localized at boundaries are studied analytically and numerically. The exponential decay of the wave function is modulated by a field-dependent amplitude J(t)=tprodt-1r=02 cos(παr), where α is the magnetic flux per plaquette (in units of a flux quantum) and t is the distance from the boundary (in units of the lattice spacing). The behavior of ||J(t)|| is found to depend sensitively on the value of α. While for rational values α=p/q the envelope of J(t) increases as 2t/q, the behavior for α irrational (q-->∞) is erratic with an aperiodic structure which drastically changes with α. For algebraic α it is found that J(t) increases as a power law tβ(α) while it grows faster (presumably as tβ(α)lnt) for transcendental α. This is very different from the growth rate J(t)~e√t that is typical for cosines with random phases. The theoretical analysis is extended to products of the type Jν(t)=tprodt-1r=02 cos(παrν) with ν>0. Different behavior of Jν(t) is found in various regimes of ν. It changes from periodic for small ν to randomlike for large ν.

  8. Localized SXR Emission During Electron Bernstein Wave Injection in MST

    NASA Astrophysics Data System (ADS)

    Anderson, Jay; Forest, Cary; Seltzman, Andrew

    2008-11-01

    The electron Bernstein wave has been suggested as a solution to the RFP confinement problem: sustained, off-axis current drive stabilizes the resistive tearing modes which govern thermal transport. A staged experiment to test the feasibility of EBW heating and current drive is underway on MST. Experiments (˜10^5 W) aimed at a demonstration of EBW heating have produced a localized increase in SXR emission. This measured emission is consistent with modeling in its location, energy spectrum and dependence on radial diffusion within the plasma. Preliminary analysis indicates that the emission is strongest in the region where ray tracing predicts maximum deposition of the injected power. The multi-chord SXR camera used is sensitive to 4-7 keV photons which is consistent with Fokker-Plank modeling of EBW injection. The enhanced SXR emission vanishes quickly when radial diffusion in the plasma is high (as indicated by m=0 magnetic activity); this is also consistent with Fokker-Plank modeling. An increase of boron emission (and presumably boron within the plasma) is also observed during EBW injection. This presents an alternative explanation to the enhanced SXR emission; recent efforts have been made to isolate the two effects.

  9. Electronically Tuned Local Oscillators for the NOEMA Interferometer

    NASA Astrophysics Data System (ADS)

    Mattiocco, Francois; Garnier, Olivier; Maier, Doris; Navarrini, Alessandro; Serres, Patrice

    2016-03-01

    We present an overview of the electronically tuned local oscillator (LO) system developed at the Institut de RadioAstronomie millimetrique (IRAM) for the superconductor-insulator-superconductor (SIS) receivers of the NOrthern Extended Millimeter Array interferometer (NOEMA). We modified the frequency bands and extended the bandwidths of the LO designs developed by the National Radio Astronomy Observatory (NRAO) for the Atacama Large Millimeter Array (ALMA) project to cover the four NOEMA LO frequency ranges 82-108.3 GHz (Band 1), 138.6-171.3 GHz (Band 2), 207.7-264.4 GHz (Band 3), and 283-365 GHz (Band 4). The NOEMA LO system employs commercially available MMICs and GaAs millimeter MMICs from NRAO which are micro-assembled into active multiplied chain (AMC) and power amplifier (PA) modules. We discuss the problem of the LO spurious harmonics and of the LO signal directly multiplied by the SIS mixers that add extra noise and lead to detections of unwanted spectral lines from higher order sidebands. A waveguide filter in the LO path is used to reduce the higher order harmonics level of the LO at the output of the final frequency multiplier, thus mitigating the undesired effects and improving the system noise temperature.

  10. ANALYSIS OF SAMPLES FROM TANK 5F CHEMICAL CLEANING

    SciTech Connect

    Poirier, M.; Fink, S.

    2011-03-07

    The Savannah River Site (SRS) is preparing Tank 5F for closure. The first step in preparing the tank for closure is mechanical sludge removal. Following mechanical sludge removal, SRS performed chemical cleaning with oxalic acid to remove the sludge heel. Personnel are currently assessing the effectiveness of the chemical cleaning. SRS personnel collected liquid samples during chemical cleaning and submitted them to Savannah River National Laboratory (SRNL) for analysis. Following chemical cleaning, they collected a solid sample (also known as 'process sample') and submitted it to SRNL for analysis. The authors analyzed these samples to assess the effectiveness of the chemical cleaning process. The conclusions from this work are: (1) With the exception of iron, the dissolution of sludge components from Tank 5F agreed with results from the actual waste demonstration performed in 2007. The fraction of iron removed from Tank 5F by chemical cleaning was significantly less than the fraction removed in the SRNL demonstrations. The likely cause of this difference is the high pH following the first oxalic acid strike. (2) Most of the sludge mass remaining in the tank is iron and nickel. (3) The remaining sludge contains approximately 26 kg of barium, 37 kg of chromium, and 37 kg of mercury. (4) Most of the radioactivity remaining in the residual material is beta emitters and {sup 90}Sr. (5) The chemical cleaning removed more than {approx} 90% of the uranium isotopes and {sup 137}Cs. (6) The chemical cleaning removed {approx} 70% of the neptunium, {approx} 83% of the {sup 90}Sr, and {approx} 21% of the {sup 60}Co. (7) The chemical cleaning removed less than 10% of the plutonium, americium, and curium isotopes. (8) The chemical cleaning removed more than 90% of the aluminium, calcium, and sodium from the tank. (9) The cleaning operations removed 61% of lithium, 88% of non-radioactive strontium, and 65% of zirconium. The {sup 90}Sr and non-radioactive strontium were measured

  11. Probing the population of the spin-orbit split levels in the actinide 5f states.

    PubMed

    Moore, K T; van der Laan, G; Tobin, J G; Chung, B W; Wall, M A; Schwartz, A J

    2006-03-01

    Spin-orbit interaction in the 5f states is believed to strongly influence exotic behaviors observed in actinide metals and compounds. Understanding these interactions and how they relate to the actinide series is of considerable importance. To address this issue, the branching ratio of the white-line peaks of the N4,5 edge for the light actinide metals, alpha-Th, alpha-U, and alpha-Pu were recorded using electron energy-loss spectroscopy (EELS) in a transmission electron microscope (TEM) and synchrotron-radiation-based X-ray absorption spectroscopy (XAS). Using the spin-orbit sum rule and the branching ratios from both experimental spectra and many-electron atomic spectral calculations, accurate values of the spin-orbit interaction, and thus the relative occupation of the j = 5/2 and 7/2 levels, are determined for the actinide 5f states. Results show that the spin-orbit sum rule works very well with both EELS and XAS spectra, needing little or no correction. This is important, since the high spatial resolution of a TEM can be used to overcome the problems of single-crystal growth often encountered with actinide metals, allowing acquisition of EELS spectra, and subsequent spin-orbit analysis, from nm-sized regions. The relative occupation numbers obtained by our method have been compared with recent theoretical results and they show a good agreement in their trend.

  12. Localized electron heating during magnetic reconnection in MAST

    NASA Astrophysics Data System (ADS)

    Yamada, T.; Tanabe, H.; Watanabe, T. G.; Hayashi, Y.; Imazawa, R.; Inomoto, M.; Ono, Y.; Gryaznevich, M.; Scannell, R.; Michael, C.; The MAST Team

    2016-10-01

    Significant increase in the plasma temperature above 1 keV was measured during the kilogauss magnetic field reconnection of two merging toroidal plasmas under the high-guide field and collision-less conditions. The electron temperature was observed to peak significantly at the X-point inside the current sheet, indicating Joule heating caused by the toroidal electric field along the X-line. This peaked temperature increases significantly with the guide field, in agreement with the electron mean-free path calculation. The slow electron heating in the downstream suggests energy conversion from ions to electrons through ion-electron collisions in the bulk plasma as the second electron heating mechanism in the bulk plasma. The electron density profile clearly reveals the electron density pile-up / fast shock structures in the downstream of reconnection, suggesting energy conversion from ion flow energy to ion thermal energy as well as significant ion heating by reconnection outflow.

  13. Site-selective electronic correlation in α-plutonium metal.

    PubMed

    Zhu, Jian-Xin; Albers, R C; Haule, K; Kotliar, G; Wills, J M

    2013-01-01

    An understanding of the phase diagram of elemental plutonium (Pu) must include both, the effects of the strong directional bonding and the high density of states of the Pu 5f electrons, as well as how that bonding weakens under the influence of strong electronic correlations. Here we present electronic-structure calculations of the full 16-atom per unit cell α-phase structure within the framework of density functional theory together with dynamical mean-field theory. Our calculations demonstrate that Pu atoms sitting on different sites within the α-Pu crystal structure have a strongly varying site dependence of the localization-delocalization correlation effects of their 5f electrons and a corresponding effect on the bonding and electronic properties of this complicated metal. In short, α-Pu has the capacity to simultaneously have multiple degrees of electron localization/delocalization of Pu 5f electrons within a pure single-element material.

  14. Pressure-induced changes in the electronic structure of americium metal

    SciTech Connect

    Soderlind, P; Moore, K T; Landa, A; Bradley, J A

    2011-02-25

    We have conducted electronic-structure calculations for Am metal under pressure to investigate the behavior of the 5f-electron states. Density-functional theory (DFT) does not reproduce the experimental photoemission spectra for the ground-state phase where the 5f electrons are localized, but the theory is expected to be correct when 5f delocalization occurs under pressure. The DFT prediction is that peak structures of the 5f valence band will merge closer to the Fermi level during compression indicating presence of itinerant 5f electrons. Existence of such 5f bands is argued to be a prerequisite for the phase transitions, particularly to the primitive orthorhombic AmIV phase, but does not agree with modern dynamical-mean-field theory (DMFT) results. Our DFT model further suggests insignificant changes of the 5f valence under pressure in agreement with recent resonant x-ray emission spectroscopy, but in contradiction to the DMFT predictions. The influence of pressure on the 5f valency in the actinides is discussed and is shown to depend in a non-trivial fashion on 5f band position and occupation relative to the spd valence bands.

  15. Multiconfigurational nature of 5f orbitals in uranium and plutonium and their intermetallic compounds

    NASA Astrophysics Data System (ADS)

    Booth, Corwin

    2013-03-01

    The structural, electronic, and magnetic properties of U and Pu elements and intermetallics remain poorly understood despite decades of effort, and currently represent an important scientific frontier toward understanding matter. The last decade has seen great progress both due to the discovery of superconductivity in PuCoGa5 and advances in theory that finally can explain fundamental ground state properties in elemental plutonium, such as the phonon dispersion curve, the non-magnetic ground state, and the volume difference between the α and δ phases. A new feature of the recent calculations is the presence not only of intermediate valence of the Pu 5f electrons, but of multiconfigurational ground states, where the different properties of the α and δ phases are primarily governed by the different relative weights of the 5f4, 5f5, and 5f6 electronic configurations. The usual method for measuring multiconfigurational states in the lanthanides is to measure the lanthanide LIII-edge x-ray absorption near-edge structure (XANES), a method that is severely limited for the actinides because the spectroscopic features are not well enough separated. Advances in resonant x-ray emission spectroscopy (RXES) have now allowed for spectra with sufficient resolution to resolve individual resonances associated with the various actinide valence states. Utilizing a new spectrometer at the Stanford Synchrotron Radiation Lightsource (SSRL), RXES data have been collected that show, for the first time, spectroscopic signatures of each of these configurations and their relative changes in various uranium and plutonium intermetallic compounds. In combination with conventional XANES spectra on related compounds, these data indicate such states may be ubiquitous in uranium and plutonium intermetallics, providing a new framework toward understanding properties ranging from heavy fermion behavior, superconductivity, and intermediate valence to mechanical and fundamental bonding behavior in

  16. Electronic dental anesthesia in a patient with suspected allergy to local anesthetics: report of case.

    PubMed

    Malamed, S F; Quinn, C L

    1988-01-01

    A 56-year-old patient with alleged allergy to local anesthetics required restorative dental treatment. Electronic dental anesthesia was used successfully, in lieu of injectable local anesthetics, to manage intraoperative pain associated with the restoration of vital mandibular teeth.

  17. CHARACTERIZATION AND ACTUAL WASTE TEST WITH TANK 5F SAMPLES

    SciTech Connect

    Hay, M. S.; Crapse, K. P.; Fink, S. D.; Pareizs, J. M.

    2007-08-30

    The initial phase of bulk waste removal operations was recently completed in Tank 5F. Video inspection of the tank indicates several mounds of sludge still remain in the tank. Additionally, a mound of white solids was observed under Riser 5. In support of chemical cleaning and heel removal programs, samples of the sludge and the mound of white solids were obtained from the tank for characterization and testing. A core sample of the sludge and Super Snapper sample of the white solids were characterized. A supernate dip sample from Tank 7F was also characterized. A portion of the sludge was used in two tank cleaning tests using oxalic acid at 50 C and 75 C. The filtered oxalic acid from the tank cleaning tests was subsequently neutralized by addition to a simulated Tank 7F supernate. Solids and liquid samples from the tank cleaning test and neutralization test were characterized. A separate report documents the results of the gas generation from the tank cleaning test using oxalic acid and Tank 5F sludge. The characterization results for the Tank 5F sludge sample (FTF-05-06-55) appear quite good with respect to the tight precision of the sample replicates, good results for the glass standards, and minimal contamination found in the blanks and glass standards. The aqua regia and sodium peroxide fusion data also show good agreement between the two dissolution methods. Iron dominates the sludge composition with other major contributors being uranium, manganese, nickel, sodium, aluminum, and silicon. The low sodium value for the sludge reflects the absence of supernate present in the sample due to the core sampler employed for obtaining the sample. The XRD and CSEM results for the Super Snapper salt sample (i.e., white solids) from Tank 5F (FTF-05-07-1) indicate the material contains hydrated sodium carbonate and bicarbonate salts along with some aluminum hydroxide. These compounds likely precipitated from the supernate in the tank. A solubility test showed the material

  18. Negative local resistance due to viscous electron backflow in graphene

    NASA Astrophysics Data System (ADS)

    Bandurin, Denis

    Theoretical and experimental studies of systems in which particles undergo frequent mutual collisions date back to more than two centuries ago. Transport in such systems is described by hydrodynamic theory that was found very successful in explaining the response of classical liquids and gases to external fields. It has been argued for a long time that collective behavior of charge carriers in solids can be also described by hydrodynamic approach. However, there has been almost no direct evidence to hydrodynamic electron transport so far. This is because the conditions at which the hydrodynamic effects become observable are very strict: the electron-electron scattering length should provide the shortest spatial scale in the problem. First of all, this requires ultra clean systems where the scattering at impurities is diminished. Second, the electron-phonon scattering rate should be smaller than that of electron-electron scattering. Due to weak electron-phonon coupling high mobility graphene devices offer an ideal system to study electron hydrodynamics. To amplify the hydrodynamic effects we employed a special measurement geometry. The idea is that in case of hydrodynamic electron flow, vortices emerge in the spatial electric current distribution near the current injection contact. That results in a development of a negative voltage drop at the nearby contacts. We were able to detect such negative signal over the range of temperatures when the electronic system is in a hydrodynamic regime. Finally, we performed a rheological study of electron liquid in graphene. The electron viscosity was found to be an order of magnitude larger than that of honey which is in good agreement with many-body calculation.

  19. Kinetics of vertical transport and localization of electrons in strained semiconductor supperlattices

    SciTech Connect

    Gerchikov, L. G. Mamaev, Yu. A.; Yashin, Yu. P.

    2015-08-15

    The kinetics of vertical electron transport in a semiconductor superlattice is considered taking into account partial localization of electrons. The time dependences of photoemission currents from samples based on a strained semiconductor superlattice calculated by numerically solving the kinetic equation are in good agreement with experimental data. Comparison of the theory with experiment makes it possible to determine the characteristic electron localization and thermoactivation times, the diffusion length, and losses of photoelectrons in the superlattice.

  20. The electron localization as the information content of the conditional pair density

    NASA Astrophysics Data System (ADS)

    Urbina, Andres S.; Torres, F. Javier; Rincon, Luis

    2016-06-01

    In the present work, the information gained by an electron for "knowing" about the position of another electron with the same spin is calculated using the Kullback-Leibler divergence (DKL) between the same-spin conditional pair probability density and the marginal probability. DKL is proposed as an electron localization measurement, based on the observation that regions of the space with high information gain can be associated with strong correlated localized electrons. Taking into consideration the scaling of DKL with the number of σ-spin electrons of a system (Nσ), the quantity χ = (Nσ - 1) DKLfcut is introduced as a general descriptor that allows the quantification of the electron localization in the space. fcut is defined such that it goes smoothly to zero for negligible densities. χ is computed for a selection of atomic and molecular systems in order to test its capability to determine the region in space where electrons are localized. As a general conclusion, χ is able to explain the electron structure of molecules on the basis of chemical grounds with a high degree of success and to produce a clear differentiation of the localization of electrons that can be traced to the fluctuation in the average number of electrons in these regions.

  1. Fast probe of local electronic states in nanostructures utilizing a single-lead quantum dot

    PubMed Central

    Otsuka, Tomohiro; Amaha, Shinichi; Nakajima, Takashi; Delbecq, Matthieu R.; Yoneda, Jun; Takeda, Kenta; Sugawara, Retsu; Allison, Giles; Ludwig, Arne; Wieck, Andreas D.; Tarucha, Seigo

    2015-01-01

    Transport measurements are powerful tools to probe electronic properties of solid-state materials. To access properties of local electronic states in nanostructures, such as local density of states, electronic distribution and so on, micro-probes utilizing artificial nanostructures have been invented to perform measurements in addition to those with conventional macroscopic electronic reservoirs. Here we demonstrate a new kind of micro-probe: a fast single-lead quantum dot probe, which utilizes a quantum dot coupled only to the target structure through a tunneling barrier and fast charge readout by RF reflectometry. The probe can directly access the local electronic states with wide bandwidth. The probe can also access more electronic states, not just those around the Fermi level, and the operations are robust against bias voltages and temperatures. PMID:26416582

  2. Using the electron localization function to correct for confinement physics in semi-local density functional theory

    SciTech Connect

    Hao, Feng Mattsson, Ann E.; Armiento, Rickard

    2014-05-14

    We have previously proposed that further improved functionals for density functional theory can be constructed based on the Armiento-Mattsson subsystem functional scheme if, in addition to the uniform electron gas and surface models used in the Armiento-Mattsson 2005 functional, a model for the strongly confined electron gas is also added. However, of central importance for this scheme is an index that identifies regions in space where the correction provided by the confined electron gas should be applied. The electron localization function (ELF) is a well-known indicator of strongly localized electrons. We use a model of a confined electron gas based on the harmonic oscillator to show that regions with high ELF directly coincide with regions where common exchange energy functionals have large errors. This suggests that the harmonic oscillator model together with an index based on the ELF provides the crucial ingredients for future improved semi-local functionals. For a practical illustration of how the proposed scheme is intended to work for a physical system we discuss monoclinic cupric oxide, CuO. A thorough discussion of this system leads us to promote the cell geometry of CuO as a useful benchmark for future semi-local functionals. Very high ELF values are found in a shell around the O ions, and take its maximum value along the Cu–O directions. An estimate of the exchange functional error from the effect of electron confinement in these regions suggests a magnitude and sign that could account for the error in cell geometry.

  3. Using the electron localization function to correct for confinement physics in semi-local density functional theory.

    PubMed

    Hao, Feng; Armiento, Rickard; Mattsson, Ann E

    2014-05-14

    We have previously proposed that further improved functionals for density functional theory can be constructed based on the Armiento-Mattsson subsystem functional scheme if, in addition to the uniform electron gas and surface models used in the Armiento-Mattsson 2005 functional, a model for the strongly confined electron gas is also added. However, of central importance for this scheme is an index that identifies regions in space where the correction provided by the confined electron gas should be applied. The electron localization function (ELF) is a well-known indicator of strongly localized electrons. We use a model of a confined electron gas based on the harmonic oscillator to show that regions with high ELF directly coincide with regions where common exchange energy functionals have large errors. This suggests that the harmonic oscillator model together with an index based on the ELF provides the crucial ingredients for future improved semi-local functionals. For a practical illustration of how the proposed scheme is intended to work for a physical system we discuss monoclinic cupric oxide, CuO. A thorough discussion of this system leads us to promote the cell geometry of CuO as a useful benchmark for future semi-local functionals. Very high ELF values are found in a shell around the O ions, and take its maximum value along the Cu-O directions. An estimate of the exchange functional error from the effect of electron confinement in these regions suggests a magnitude and sign that could account for the error in cell geometry.

  4. Electron localization in a mixed-valence diniobium benzene complex

    DOE PAGES

    Gianetti, Thomas L.; Nocton, Grégory; Minasian, Stefan G.; ...

    2014-11-11

    Reaction of the neutral diniobium benzene complex {[Nb(BDI)NtBu]2(μ-C6H6)} (BDI = N,N'-diisopropylbenzene-β-diketiminate) with Ag[B(C6F5)4] results in a single electron oxidation to produce a cationic diniobium arene complex, {[Nb(BDI)NtBu]2(μ-C6H6)}{B(C6F5)4}. Investigation of the solid state and solution phase structure using single-crystal X-ray diffraction, cyclic voltammetry, magnetic susceptibility, and multinuclear NMR spectroscopy indicates that the oxidation results in an asymmetric molecule with two chemically inequivalent Nb atoms. Further characterization using density functional theory (DFT) calculations, UV-visible, Nb L3,2-edge X-ray absorption near-edge structure (XANES), and EPR spectroscopies supports assignment of a diniobium complex, in which one Nb atom carries a single unpaired electron that ismore » not largely delocalized on the second Nb atom. During the oxidative transformation, one electron is removed from the δ-bonding HOMO, which causes a destabilization of the molecule and formation of an asymmetric product. Subsequent reactivity studies indicate that the oxidized product allows access to metal-based chemistry with substrates that did not exhibit reactivity with the starting neutral complex.« less

  5. Electron localization in a mixed-valence diniobium benzene complex

    SciTech Connect

    Gianetti, Thomas L.; Nocton, Grégory; Minasian, Stefan G.; Kaltsoyannis, Nikolas; Kilcoyne, A. L. David; Kozimor, Stosh A.; Shuh, David K.; Tyliszczak, Tolek; Bergman, Robert G.; Arnold, John

    2014-11-11

    Reaction of the neutral diniobium benzene complex {[Nb(BDI)NtBu]2(μ-C6H6)} (BDI = N,N'-diisopropylbenzene-β-diketiminate) with Ag[B(C6F5)4] results in a single electron oxidation to produce a cationic diniobium arene complex, {[Nb(BDI)NtBu]2(μ-C6H6)}{B(C6F5)4}. Investigation of the solid state and solution phase structure using single-crystal X-ray diffraction, cyclic voltammetry, magnetic susceptibility, and multinuclear NMR spectroscopy indicates that the oxidation results in an asymmetric molecule with two chemically inequivalent Nb atoms. Further characterization using density functional theory (DFT) calculations, UV-visible, Nb L3,2-edge X-ray absorption near-edge structure (XANES), and EPR spectroscopies supports assignment of a diniobium complex, in which one Nb atom carries a single unpaired electron that is not largely delocalized on the second Nb atom. During the oxidative transformation, one electron is removed from the δ-bonding HOMO, which causes a destabilization of the molecule and formation of an asymmetric product. Subsequent reactivity studies indicate that the oxidized product allows access to metal-based chemistry with substrates that did not exhibit reactivity with the starting neutral complex.

  6. Multiconfigurational nature of 5f orbitals in uranium and plutonium intermetallics

    PubMed Central

    Booth, C.H.; Jiang, Yu; Wang, D.L.; Mitchell, J.N.; Tobash, P.H.; Bauer, E.D.; Wall, M.A.; Allen, P.G.; Sokaras, D.; Nordlund, D.; Weng, T.-C.; Torrez, M.A.; Sarrao, J.L.

    2012-01-01

    Uranium and plutonium’s 5f electrons are tenuously poised between strongly bonding with ligand spd-states and residing close to the nucleus. The unusual properties of these elements and their compounds (e.g., the six different allotropes of elemental plutonium) are widely believed to depend on the related attributes of f-orbital occupancy and delocalization for which a quantitative measure is lacking. By employing resonant X-ray emission spectroscopy (RXES) and X-ray absorption near-edge structure (XANES) spectroscopy and making comparisons to specific heat measurements, we demonstrate the presence of multiconfigurational f-orbital states in the actinide elements U and Pu and in a wide range of uranium and plutonium intermetallic compounds. These results provide a robust experimental basis for a new framework toward understanding the strongly-correlated behavior of actinide materials. PMID:22706643

  7. Multiconfigurational nature of 5f orbitals in uranium and plutonium intermetallics.

    PubMed

    Booth, C H; Jiang, Yu; Wang, D L; Mitchell, J N; Tobash, P H; Bauer, E D; Wall, M A; Allen, P G; Sokaras, D; Nordlund, D; Weng, T-C; Torrez, M A; Sarrao, J L

    2012-06-26

    Uranium and plutonium's 5f electrons are tenuously poised between strongly bonding with ligand spd-states and residing close to the nucleus. The unusual properties of these elements and their compounds (e.g., the six different allotropes of elemental plutonium) are widely believed to depend on the related attributes of f-orbital occupancy and delocalization for which a quantitative measure is lacking. By employing resonant X-ray emission spectroscopy (RXES) and X-ray absorption near-edge structure (XANES) spectroscopy and making comparisons to specific heat measurements, we demonstrate the presence of multiconfigurational f-orbital states in the actinide elements U and Pu and in a wide range of uranium and plutonium intermetallic compounds. These results provide a robust experimental basis for a new framework toward understanding the strongly-correlated behavior of actinide materials.

  8. Circularly polarized luminescence of curium: a new characterization of the 5f actinide complexes.

    PubMed

    Law, Ga-Lai; Andolina, Christopher M; Xu, Jide; Luu, Vinh; Rutkowski, Philip X; Muller, Gilles; Shuh, David K; Gibson, John K; Raymond, Kenneth N

    2012-09-19

    A key distinction between the lanthanide (4f) and the actinide (5f) transition elements is the increased role of f-orbital covalent bonding in the latter. Circularly polarized luminescence (CPL) is an uncommon but powerful spectroscopy which probes the electronic structure of chiral, luminescent complexes or molecules. While there are many examples of CPL spectra for the lanthanides, this report is the first for an actinide. Two chiral, octadentate chelating ligands based on orthoamide phenol (IAM) were used to complex curium(III). While the radioactivity kept the amount of material limited to micromole amounts, spectra of the highly luminescent complexes showed significant emission peak shifts between the different complexes, consistent with ligand field effects previously observed in luminescence spectra.

  9. Electron density power spectrum in the local interstellar medium

    NASA Technical Reports Server (NTRS)

    Armstrong, J. W.; Rickett, B. J.; Spangler, S. R.

    1995-01-01

    Interstellar scintillation (ISS), fluctuations in the amplitude and phase of radio waves caused by scattering in the interstellar medium, is important as a diagnostic of interstellar plasma turbulence. ISS is also of interest because it is noise for other radio astronomical observations. The unifying concern is the power spectrum of the interstellar electron density. Here we use ISS observations through the nearby (less than or approximately =1 kpc) (ISM) to estimate the spectrum. From measurements of angular broadening of pulsars and extragalactic sources, decorrelation bandwidth of pulsars, refractive steering of features in pulsar dynamic spectra, dispersion measured fluctuations of pulsars, and refractive scintillation index measurements, we construct a composite structure function that is approximately power law over 2 x 10(exp 6) m less than scale less than 10(exp 13) m. The data are consistent with the structure function having a logarithmic slope versus baseline less than 2; thus there is a meaningful connection between scales in the radiowave fluctuation field and the scales in the electron density field causing the scattering. The data give an upper limit to the inner scale, l(sub o) less than or approximately 10(exp 8) m and are consistent with much smaller values. We construct a composite electron density spectrum that is approximately power law over at least the approximately = 5 decade wavenumber range 10(exp -13)/m less than wavenumber less than 10(exp -8)/m and that may extend to higher wavenumbers. The average spectral index of electron density over this wavenumber range is approximately = 3.7, very close to the value expected for a Kolmogorov process. The outer scale size, L(sub o), must be greater than or approximately = 10(exp 13) m (determined from dispersion measure fluctuations). When the ISS data are combined with measurements of differential Faraday rotation angle, and gradients in the average electron density, constraints can be put on the

  10. The imprint of Gould's belt on the local cosmic ray electron spectrum

    NASA Astrophysics Data System (ADS)

    Pohl, M.; Perrot, C.; Grenier, I.

    2001-08-01

    In a recent paper Pohl and Esposito (1998) demonstrated that if the sources of cosmic-rays are discrete, as are Supernova Remnants (SNR), then the spectra of cosmic-ray electrons largely vary with location and time and the locally measured electron spectrum may not be representative of the electron spectra elsewhere in the Galaxy, which could be substantially harder than the local one. They have shown that the observed excess of γ-ray emission above 1 GeV can in fact be partially explained as a correspondingly hard inverse Compton component, provided the bulk of cosmic-ray electrons is produced in SNR. As part of a program to model the Galactic γ-ray foreground we have continued the earlier studies by investigating the impact of the star forming region Gould's Belt on the local electron spectrum. If the electron sources in Gould's Belt were continous, the local electron spectrum would be slightly hardened. If the electron sources are discrete, which is the more probable case, the variation in the local electron spectrum found by Pohl & Esposito persists. 1 The local cosmic-ray electron spectrum The recent detections of non-thermal X-ray synchrotron radiation from the supernova remnants SN1006 (Koyama et al., 1995), RX J1713.7-3946 (Koyama et al., 1997), IC443 (Keohane et al., 1997; Slane et al., 1999), Cas A (Allen et al., 1997), and RCW86 (Borkowski et al., 2001) and the subsequent detections of SN1006 (Tanimori et al., 1998), RX J1713.7-3946 (Muraishi et al., 2000), and Cas A (Aharonian et al., 2001) at TeV energies support the hypothesis that at least Galactic cosmic-ray electrons are accelerated predominantly in SNR. The Galactic distribution and spectrum of cosmic-ray electrons are intimately linked to the distribution and nature of their sources. Supernovae and hence their remnants are tran-

  11. Studies of local electron heat transport on TFTR

    SciTech Connect

    Fredrickson, E.D.; Chang, Z.Y.; Janos, A.; McGuire, K.M.; Scott, S.; Taylor, G.

    1993-08-16

    The anomalously fast relaxation of the perturbations to the electron temperature profile caused by a sawtooth crash has been studied extensively on TFTR. We will show that on a short timescale the heat pulse is not simply diffusive as has been generally assumed, but that modeling of the heat pulse requires a transient enhancement in {chi}{sub e} following the sawtooth crash. It will be shown that the time-dependent enhancement in {chi}{sub e} predicted by non-linear thermal transport models, i.e., incremental {chi} models or the Rebut-Lallia-Watkins transport model, is much smaller than that required to explain the anomalies in the heat pulse propagation.

  12. A Transport Model for Non-Local Heating of Electrons in ICP Reactors

    NASA Technical Reports Server (NTRS)

    Chang, C. H.; Bose, Deepak; Arnold, James O. (Technical Monitor)

    1998-01-01

    A new model has been developed for non-local heating of electrons in ICP reactors, based on a hydrodynamic approach. The model has been derived using the electron momentum conservation in azimuthal direction with electromagnetic and frictional forces respectively as driving force and damper of harmonic oscillatory motion of electrons. The resulting transport equations include the convection of azimuthal electron momentum in radial and axial directions, thereby accounting for the non-local effects. The azimuthal velocity of electrons and the resulting electrical current are coupled to the Maxwell's relations, thus forming a self-consistent model for non-local heating. This model is being implemented along with a set of Navier-Stokes equations for plasma dynamics and gas flow to simulate low-pressure (few mTorr's) ICP discharges. Characteristics of nitrogen plasma in a TCP 300mm etch reactor is being studied. The results will be compared against the available Langmuir probe measurements.

  13. Electron localization function in full-potential representation for crystalline materials.

    PubMed

    Ormeci, A; Rosner, H; Wagner, F R; Kohout, M; Grin, Yu

    2006-01-26

    The electron localization function (ELF) is implemented in the first-principles, all-electron, full-potential local orbital method. This full-potential implementation increases the accuracy with which the ELF can be computed for crystalline materials. Some representative results obtained are presented and compared with the results of other methods. Although for crystal structures with directed bonding only minor differences are found, in simple elemental metals, there are differences in the valence region, which give rise to different ELF topologies.

  14. Quantum transport through disordered 1D wires: Conductance via localized and delocalized electrons

    SciTech Connect

    Gopar, Víctor A.

    2014-01-14

    Coherent electronic transport through disordered systems, like quantum wires, is a topic of fundamental and practical interest. In particular, the exponential localization of electron wave functions-Anderson localization-due to the presence of disorder has been widely studied. In fact, Anderson localization, is not an phenomenon exclusive to electrons but it has been observed in microwave and acoustic experiments, photonic materials, cold atoms, etc. Nowadays, many properties of electronic transport of quantum wires have been successfully described within a scaling approach to Anderson localization. On the other hand, anomalous localization or delocalization is, in relation to the Anderson problem, a less studied phenomenon. Although one can find signatures of anomalous localization in very different systems in nature. In the problem of electronic transport, a source of delocalization may come from symmetries present in the system and particular disorder configurations, like the so-called Lévy-type disorder. We have developed a theoretical model to describe the statistical properties of transport when electron wave functions are delocalized. In particular, we show that only two physical parameters determine the complete conductance distribution.

  15. Dynamic modulation of electronic properties of graphene by localized carbon doping using focused electron beam induced deposition.

    PubMed

    Kim, S; Russell, M; Henry, M; Kim, S S; Naik, R R; Voevodin, A A; Jang, S S; Tsukruk, V V; Fedorov, A G

    2015-09-28

    We report on the first demonstration of controllable carbon doping of graphene to engineer local electronic properties of a graphene conduction channel using focused electron beam induced deposition (FEBID). Electrical measurements indicate that an "n-p-n" junction on graphene conduction channel is formed by partial carbon deposition near the source and drain metal contacts by low energy (<50 eV) secondary electrons due to inelastic collisions of long range backscattered primary electrons generated from a low dose of high energy (25 keV) electron beam (1 × 10(18) e(-) per cm(2)). Detailed AFM imaging provides direct evidence of the new mechanism responsible for dynamic evolution of the locally varying graphene doping. The FEBID carbon atoms, which are physisorbed and weakly bound to graphene, diffuse towards the middle of graphene conduction channel due to their surface chemical potential gradient, resulting in negative shift of Dirac voltage. Increasing a primary electron dose to 1 × 10(19) e(-) per cm(2) results in a significant increase of carbon deposition, such that it covers the entire graphene conduction channel at high surface density, leading to n-doping of graphene channel. Collectively, these findings establish a unique capability of FEBID technique to dynamically modulate the doping state of graphene, thus enabling a new route to resist-free, "direct-write" functional patterning of graphene-based electronic devices with potential for on-demand re-configurability.

  16. On the Stability of Parainfluenza Virus 5 F Proteins

    PubMed Central

    Poor, Taylor A.; Song, Albert S.; Welch, Brett D.; Kors, Christopher A.; Jardetzky, Theodore S.

    2015-01-01

    The crystal structure of the F protein (prefusion form) of the paramyxovirus parainfluenza virus 5 (PIV5) WR isolate was determined. We investigated the basis by which point mutations affect fusion in PIV5 isolates W3A and WR, which differ by two residues in the F ectodomain. The P22 stabilizing site acts through a local conformational change and a hydrophobic pocket interaction, whereas the S443 destabilizing site appears sensitive to both conformational effects and amino acid charge/polarity changes. PMID:25589638

  17. Study of local atomic order in amorphous materials in a computerized transmission electron microscope.

    PubMed

    Balossier, G; Garg, R K; Bonhomme, P; Thomas, X

    1989-03-01

    Experimental results obtained by electron diffraction (ED) and extended electron energy loss fine structure (EXELFS) techniques to study the local atomic order in amorphous materials such as carbon, silicon, and its oxides are described. Potential applications of ED and EXELFS techniques and their limitations are also discussed.

  18. Electronic Resources in a Next-Generation Catalog: The Case of WorldCat Local

    ERIC Educational Resources Information Center

    Shadle, Steve

    2009-01-01

    In April 2007, the University of Washington Libraries debuted WorldCat Local (WCL), a localized version of the WorldCat database that interoperates with a library's integrated library system and fulfillment services to provide a single-search interface for a library's physical and electronic content. This brief will describe how WCL incorporates a…

  19. Interlibrary Service Requests for Locally and Electronically Available Items: Patterns of Use, Users, and Canceled Requests

    ERIC Educational Resources Information Center

    Page, Jessica R.; Kuehn, Jennifer

    2009-01-01

    As the use of the Ohio State University Libraries interlibrary services has increased, there have been more requests to borrow items that are already available to patrons locally, often in electronic format. Patterns relating to why patrons could not find locally available materials were identified in the record of canceled interlibrary requests…

  20. Quantum-classical simulation of electron localization in negatively charged methanol clusters.

    PubMed

    Mones, Letif; Rossky, Peter J; Turi, László

    2011-08-28

    A series of quantum molecular dynamics simulations have been performed to investigate the energetic, structural, dynamic, and spectroscopic properties of methanol cluster anions, [(CH(3)OH)(n)](-), (n = 50-500). Consistent with the inference from photo-electron imaging experiments, we find two main localization modes of the excess electron in equilibrated methanol clusters at ∼200 K. The two different localization patterns have strikingly different physical properties, consistent with experimental observations, and are manifest in comparable cluster sizes to those observed. Smaller clusters (n ≤ 128) tend to localize the electron in very weakly bound, diffuse electronic states on the surface of the cluster, while in larger ones the electron is stabilized in solvent cavities, in compact interior-bound states. The interior states exhibit properties that largely resemble and smoothly extrapolate to those simulated for a solvated electron in bulk methanol. The surface electronic states of methanol cluster anions are significantly more weakly bound than the surface states of the anionic water clusters. The key source of the difference is the lack of stabilizing free hydroxyl groups on a relaxed methanol cluster surface. We also provide a mechanistic picture that illustrates the essential role of the interactions of the excess electron with the hydroxyl groups in the dynamic process of the transition of the electron from surface-bound states to interior-bound states.

  1. Local spin torque induced by electron electric dipole moment in the YbF molecule

    SciTech Connect

    Fukuda, Masahiro; Senami, Masato; Ogiso, Yoji; Tachibana, Akitomo

    2014-10-06

    In this study, we show the modification of the equation of motion of the electronic spin, which is derived by the quantum electron spin vorticity principle, by the effect of the electron electric dipole moment (EDM). To investigate the new contribution to spin torque by EDM, using first principle calculations, we visualize distributions of the local spin angular momentum density and local spin torque density of the YbF molecule on which the static electric field and magnetic field are applied at t = 0.

  2. Localized conductive patterning via focused electron beam reduction of graphene oxide

    SciTech Connect

    Kim, Songkil; Henry, Mathias; Kulkarni, Dhaval D.; Zackowski, Paul; Jang, Seung Soon; Tsukruk, Vladimir V.; Fedorov, Andrei G.

    2015-03-30

    We report on a method for “direct-write” conductive patterning via reduction of graphene oxide (GO) sheets using focused electron beam induced deposition (FEBID) of carbon. FEBID treatment of the intrinsically dielectric graphene oxide between two metal terminals opens up the conduction channel, thus enabling a unique capability for nanoscale conductive domain patterning in GO. An increase in FEBID electron dose results in a significant increase of the domain electrical conductivity with improving linearity of drain-source current vs. voltage dependence, indicative of a change of graphene oxide electronic properties from insulating to semiconducting. Density functional theory calculations suggest a possible mechanism underlying this experimentally observed phenomenon, as localized reduction of graphene oxide layers via interactions with highly reactive intermediates of electron-beam-assisted dissociation of surface-adsorbed hydrocarbon molecules. These findings establish an unusual route for using FEBID as nanoscale lithography and patterning technique for engineering carbon-based nanomaterials and devices with locally tailored electronic properties.

  3. Local treatment of electron excitations in the EOM-CCSD method

    NASA Astrophysics Data System (ADS)

    Korona, Tatiana; Werner, Hans-Joachim

    2003-02-01

    The Equation-of-Motion coupled cluster method restricted to single and double excitations (EOM-CCSD) and singlet excited states is formulated in a basis of nonorthogonal local orbitals. In the calculation of excited states only electron promotions from localized molecular orbitals into subspaces (excitation domains) of the local basis are allowed, which strongly reduces the number of EOM-CCSD amplitudes to be optimized. Furthermore, double excitations are neglected unless the excitation domains of the corresponding localized occupied orbitals are close to each other. Unlike in the local methods for the ground state, the excitation domains cannot be simply restricted to the atomic orbitals that are spatially close to the localized occupied orbitals. In the present paper the choice of the excitation domains is based on the analysis of wave functions computed by more approximate (and cheaper) methods like, e.g., configuration-interaction singles. The effect of various local approximations is investigated in detail, and it is found that a balanced description of the local configuration spaces describing the ground and excited states is essential to obtain accurate results. Using a single set of parameters for a given basis set, test calculations with the local EOM-CCSD method were performed for 14 molecules and 49 electronically excited states. The excitation energies computed by the local EOM-CCSD method reproduce the conventional EOM-CCSD excitation energies with an average error of 0.06 eV.

  4. Pharmacology of Indole and Indazole Synthetic Cannabinoid Designer Drugs AB-FUBINACA, ADB-FUBINACA, AB-PINACA, ADB-PINACA, 5F-AB-PINACA, 5F-ADB-PINACA, ADBICA, and 5F-ADBICA.

    PubMed

    Banister, Samuel D; Moir, Michael; Stuart, Jordyn; Kevin, Richard C; Wood, Katie E; Longworth, Mitchell; Wilkinson, Shane M; Beinat, Corinne; Buchanan, Alexandra S; Glass, Michelle; Connor, Mark; McGregor, Iain S; Kassiou, Michael

    2015-09-16

    Synthetic cannabinoid (SC) designer drugs based on indole and indazole scaffolds and featuring l-valinamide or l-tert-leucinamide side chains are encountered with increasing frequency by forensic researchers and law enforcement agencies and are associated with serious adverse health effects. However, many of these novel SCs are unprecedented in the scientific literature at the time of their discovery, and little is known of their pharmacology. Here, we report the synthesis and pharmacological characterization of AB-FUBINACA, ADB-FUBINACA, AB-PINACA, ADB-PINACA, 5F-AB-PINACA, 5F-ADB-PINACA, ADBICA, 5F-ADBICA, and several analogues. All synthesized SCs acted as high potency agonists of CB1 (EC50 = 0.24-21 nM) and CB2 (EC50 = 0.88-15 nM) receptors in a fluorometric assay of membrane potential, with 5F-ADB-PINACA showing the greatest potency at CB1 receptors. The cannabimimetic activities of AB-FUBINACA and AB-PINACA in vivo were evaluated in rats using biotelemetry. AB-FUBINACA and AB-PINACA dose-dependently induced hypothermia and bradycardia at doses of 0.3-3 mg/kg, and hypothermia was reversed by pretreatment with a CB1 (but not CB2) antagonist, indicating that these SCs are cannabimimetic in vivo, consistent with anecdotal reports of psychoactivity in humans.

  5. Spin noise of localized electrons: Interplay of hopping and hyperfine interaction

    NASA Astrophysics Data System (ADS)

    Glazov, M. M.

    2015-05-01

    The theory of spin fluctuations is developed for an ensemble of localized electrons, taking into account both the hyperfine interaction of electron and nuclear spins and electron hopping between the sites. The analytical expression for the spin noise spectrum is derived for an arbitrary relation between the electron spin precession frequency in a field of nuclear fluctuations and the hopping rate. An increase in the hopping rate results in a drastic change in the spin noise spectrum. The effect of an external magnetic field is briefly addressed.

  6. Assessment of delocalized and localized molecular orbitals through electron momentum spectroscopy

    NASA Astrophysics Data System (ADS)

    Liu, Yuan; Cheung, Ling-Fung; Ning, Chuan-Gang

    2014-06-01

    Recently, there was a hot controversy about the concept of localized orbitals, which was triggered by Grushow's work titled “Is it time to retire the hybrid atomic orbital?” [J. Chem. Educ. 88, 860 (2011)]. To clarify the issue, we assess the delocalized and localized molecular orbitals from an experimental view using electron momentum spectroscopy. The delocalized and localized molecular orbitals based on various theoretical models for CH4, NH3, and H2O are compared with the experimental momentum distributions. Our results show that the delocalized molecular orbitals rather than the localized ones can give a direct interpretation of the experimental (e, 2e) results.

  7. Inhibitory effect of 5F on development of lung cancer in A/J mice

    PubMed Central

    Ye, Hua; Yang, Xiaoqing; Wu, Kefeng; Li, Li; Lv, Yingnian; Liu, Yi; Zheng, Xuebao

    2015-01-01

    The purpose of the study is to investigate the effect of ent-11α-hydroxy-15-oxo-kaur-16-en-19-oic-acid (5F) on the model of induced A/J mice lung cancer in A/J mice. The expressions of tumor-related molecules including P65 and Bcl-2 at protein level were examined using the immunohistochemical method (IHC). Side effects of 5F were also monitored. The results indicated that 5F significantly suppressed the development of B[a]P and NNK-induced lung cancer in vivo by facilitating cell apoptosis with minimal side effects. Compared to the expressions of P65 and Bcl-2 in model group, the levels were strongly attenuated both in blank and 5F injection groups. Moreover, P65 and Bcl-2 levels varied among different groups receiving 5F treatment. The expressions of P65 and Bcl-2 were much lower in groups receiving high-concentration 5F treatment than those with low-concentration 5F injection. Findings revealed that 5F inhibited the pathogenesis of lung cancer through accelerating apoptosis in a dose-dependent manner. PMID:26097604

  8. Localized electronic states at grain boundaries on the surface of graphene and graphite

    NASA Astrophysics Data System (ADS)

    Luican-Mayer, Adina; Barrios-Vargas, Jose E.; Toft Falkenberg, Jesper; Autès, Gabriel; Cummings, Aron W.; Soriano, David; Li, Guohong; Brandbyge, Mads; Yazyev, Oleg V.; Roche, Stephan; Andrei, Eva Y.

    2016-09-01

    Recent advances in large-scale synthesis of graphene and other 2D materials have underscored the importance of local defects such as dislocations and grain boundaries (GBs), and especially their tendency to alter the electronic properties of the material. Understanding how the polycrystalline morphology affects the electronic properties is crucial for the development of applications such as flexible electronics, energy harvesting devices or sensors. We here report on atomic scale characterization of several GBs and on the structural-dependence of the localized electronic states in their vicinity. Using low temperature scanning tunneling microscopy and spectroscopy, together with tight binding and ab initio numerical simulations we explore GBs on the surface of graphite and elucidate the interconnection between the local density of states and their atomic structure. We show that the electronic fingerprints of these GBs consist of pronounced resonances which, depending on the relative orientation of the adjacent crystallites, appear either on the electron side of the spectrum or as an electron-hole symmetric doublet close to the charge neutrality point. These two types of spectral features will impact very differently the transport properties allowing, in the asymmetric case to introduce transport anisotropy which could be utilized to design novel growth and fabrication strategies to control device performance.

  9. Local intelligent electronic device (IED) rendering templates over limited bandwidth communication link to manage remote IED

    DOEpatents

    Bradetich, Ryan; Dearien, Jason A; Grussling, Barry Jakob; Remaley, Gavin

    2013-11-05

    The present disclosure provides systems and methods for remote device management. According to various embodiments, a local intelligent electronic device (IED) may be in communication with a remote IED via a limited bandwidth communication link, such as a serial link. The limited bandwidth communication link may not support traditional remote management interfaces. According to one embodiment, a local IED may present an operator with a management interface for a remote IED by rendering locally stored templates. The local IED may render the locally stored templates using sparse data obtained from the remote IED. According to various embodiments, the management interface may be a web client interface and/or an HTML interface. The bandwidth required to present a remote management interface may be significantly reduced by rendering locally stored templates rather than requesting an entire management interface from the remote IED. According to various embodiments, an IED may comprise an encryption transceiver.

  10. Interfacial valence electron localization and the corrosion resistance of Al-SiC nanocomposite

    PubMed Central

    Mosleh-Shirazi, Sareh; Hua, Guomin; Akhlaghi, Farshad; Yan, Xianguo; Li, Dongyang

    2015-01-01

    Microstructural inhomogeneity generally deteriorates the corrosion resistance of materials due to the galvanic effect and interfacial issues. However, the situation may change for nanostructured materials. This article reports our studies on the corrosion behavior of SiC nanoparticle-reinforced Al6061 matrix composite. It was observed that the corrosion resistance of Al6061 increased when SiC nanoparticles were added. Overall electron work function (EWF) of the Al-SiC nanocomposite increased, along with an increase in the corrosion potential. The electron localization function of the Al-SiC nanocomposite was calculated and the results revealed that valence electrons were localized in the region of SiC-Al interface, resulting in an increase in the overall work function and thus building a higher barrier to hinder electrons in the nano-composite to participate in corrosion reactions. PMID:26667968

  11. Evidence of local power deposition and electron heating by a standing electromagnetic wave in electron-cyclotron-resonance plasma.

    PubMed

    Durocher-Jean, A; Stafford, L; Dap, S; Makasheva, K; Clergereaux, R

    2014-09-01

    Microwave plasmas excited at electron-cyclotron resonance were studied in the 0.5-15 mTorr pressure range. In contrast with low-limit pressure conditions where the plasma emission highlights a fairly homogeneous spatial structure, a periodic spatial modulation (period ∼6.2 cm) appeared as pressure increased. This feature is ascribed to a local power deposition (related to the electron density) due to the presence of a standing electromagnetic wave created by the feed electromagnetic field (2.45 GHz) in the cavity formed by the reactor walls. Analysis of the electron energy probability function by Langmuir probe and optical emission spectroscopy further revealed the presence of a high-energy tail that showed strong periodic spatial modulation at higher pressure. The spatial evolution of the electron density and of the characteristic temperature of these high-energy electrons coincides with the nodes (maximum) and antinodes (minimum) of the standing wave. These spatially-modulated power deposition and electron heating mechanisms are then discussed.

  12. Wavelength dependence of electron localization in the laser-driven dissociation of H2(+).

    PubMed

    Liu, Kunlong; Hong, Weiyi; Zhang, Qingbin; Lu, Peixiang

    2011-12-19

    We theoretically investigate the laser wavelength dependence of asymmetric dissociation of H2(+). It is found that the electron localization in molecular dissociation is significantly manipulated by varying the wavelength of the driving field. Through creating a strong nuclear vibration in the laser-molecular interaction, our simulations demonstrate that the few-cycle mid-infrared pulse can effectively localize the electron at one of the dissociating nuclei with weak ionization. Moreover, we show that the observed phase-shift of the dissociation asymmetry is attributed to the different population transfers by the remaining fields after the internuclear distances reach the one-photon coupling point.

  13. Crossed Andreev Reflection and Spin-Resolved Non-local Electron Transport

    NASA Astrophysics Data System (ADS)

    Kalenkov, Mikhail S.; Zaikin, Andrei D.

    The phenomenon of crossed Andreev reflection (CAR) is known to play a key role in non-local electron transport across three-terminal normal-superconducting-normal (NSN) devices. Here, we review our general theory of non-local charge transport in three-terminal disordered ferromagnet-superconductor-ferromagnet (FSF) structures. We demonstrate that CAR is highly sensitive to electron spins and yields a rich variety of properties of non-local conductance, which we describe non-perturbatively at arbitrary voltages, temperature, degree of disorder, spin-dependent interface transmissions and their polarizations. We demonstrate that magnetic effects have different implications: While strong exchange field suppresses disorder-induced electron interference in ferromagnetic electrodes, spin-sensitive electron scattering at SF interfaces can drive the total non-local conductance negative at sufficiently low energies. At higher energies, magnetic effects become less important and the non-local resistance behaves similarly to the non-magnetic case. Our results can be applied to multi-terminal hybrid structures with normal, ferromagnetic and half-metallic electrodes and can be directly tested in future experiments.

  14. The role of localized inductive electric fields in electron injections around dipolarizing flux bundles

    NASA Astrophysics Data System (ADS)

    Gabrielse, Christine; Harris, Camilla; Angelopoulos, Vassilis; Artemyev, Anton; Runov, Andrei

    2016-10-01

    We study energetic electron injections by using an analytical model that self-consistently describes electric and magnetic field perturbations of a transient, localized dipolarizing flux bundle (DFB). This simple model reproduces most injection signatures at multiple locations simultaneously, reaffirming earlier findings that an earthward-traveling DFB can both transport and accelerate electrons to suprathermal energies, and can thus be considered an important driver of short-lived ( < 10 min) injections. We find that energetic electron drift paths are greatly influenced by the sharp magnetic field gradients around a localized DFB. Because a DFB is so localized (only a few RE wide across the tail), there are strong duskward magnetic field gradients on the DFB's dawn flank and strong dawnward magnetic field gradients on its dusk flank. Electrons on the DFB's dawnside therefore ∇B drift farther earthward from the reconnection site, whereas electrons on its duskside can potentially evacuate the inner magnetosphere by ∇B drifting tailward. This results in flux decrease at the front's duskside. As a result, the source of electrons observed during injection depends sensitively on the spacecraft location relative to the DFB and on the DFB's properties. We similarly find that the process of electron energization depends on how the electrons interact with the DFB. The initial injection signature is from electrons that interact with the front and gain the majority of their energy from the increasing magnetic field (∂B/∂t), whereas populations that arrive later gain most of their energy from ∇B drifting across the flow channel and against the DFB's electric fields.

  15. Validation of local hybrid functionals for TDDFT calculations of electronic excitation energies

    NASA Astrophysics Data System (ADS)

    Maier, Toni M.; Bahmann, Hilke; Arbuznikov, Alexei V.; Kaupp, Martin

    2016-02-01

    The first systematic evaluation of local hybrid functionals for the calculation of electronic excitation energies within linear-response time-dependent density functional theory (TDDFT) is reported. Using our recent efficient semi-numerical TDDFT implementation [T. M. Maier et al., J. Chem. Theory Comput. 11, 4226 (2015)], four simple, thermochemically optimized one-parameter local hybrid functionals based on local spin-density exchange are evaluated against a database of singlet and triplet valence excitations of organic molecules, and against a mixed database including also Rydberg, intramolecular charge-transfer (CT) and core excitations. The four local hybrids exhibit comparable performance to standard global or range-separated hybrid functionals for common singlet valence excitations, but several local hybrids outperform all other functionals tested for the triplet excitations of the first test set, as well as for relative energies of excited states. Evaluation for the combined second test set shows that local hybrids can also provide excellent Rydberg and core excitations, in the latter case rivaling specialized functionals optimized specifically for such excitations. This good performance of local hybrids for different excitation types could be traced to relatively large exact-exchange (EXX) admixtures in a spatial region intermediate between valence and asymptotics, as well as close to the nucleus, and lower EXX admixtures in the valence region. In contrast, the tested local hybrids cannot compete with the best range-separated hybrids for intra- and intermolecular CT excitation energies. Possible directions for improvement in the latter category are discussed. As the used efficient TDDFT implementation requires essentially the same computational effort for global and local hybrids, applications of local hybrid functionals to excited-state problems appear promising in a wide range of fields. Influences of current-density dependence of local kinetic

  16. Quasi-relativistic SCF X. cap alpha. study of octahedral 5f/sup 1/ complexes

    SciTech Connect

    Thornton, G.; Roesch, N.; Edelstein, N.

    1980-05-01

    Quasi-relativistic SCF X..cap alpha.. calculations have been carried out for the octahedral 5f/sup 1/ complexes Pa/sup IV/X/sub 6//sup 2 -/, U/sup V/X/sub 6//sup -/(X = F, Cl, Br, I), and Np/sup VI/F/sub 6/. The 5f ..-->.. 5f excitation energies calculated by using the transition-state method agree well with the available absorption spectra. Ionic effects appear to dominate the trends observed in the f-orbital ligand field splitting.

  17. Quantification of nanoscale density fluctuations using electron microscopy: Light-localization properties of biological cells

    SciTech Connect

    Pradhan, Prabhakar; Damania, Dhwanil; Turzhitsky, Vladimir; Subramanian, Hariharan; Backman, Vadim; Joshi, Hrushikesh M.; Dravid, Vinayak P.; Roy, Hemant K.; Taflove, Allen

    2010-12-13

    We report a study of the nanoscale mass-density fluctuations of heterogeneous optical dielectric media, including nanomaterials and biological cells, by quantifying their nanoscale light-localization properties. Transmission electron microscope images of the media are used to construct corresponding effective disordered optical lattices. Light-localization properties are studied by the statistical analysis of the inverse participation ratio (IPR) of the localized eigenfunctions of these optical lattices at the nanoscale. We validated IPR analysis using nanomaterials as models of disordered systems fabricated from dielectric nanoparticles. As an example, we then applied such analysis to distinguish between cells with different degrees of aggressive malignancy.

  18. Electron localization due to side-attached molecules on graphene nanoribbons

    NASA Astrophysics Data System (ADS)

    Nunez, C. D.; Orellana, P. A.; Rosales, L.

    2016-10-01

    In this work, we have studied the electron localization due to a random distribution of side-attached linear organic molecules on graphene nanoribbons. By using the Green's function formalism within a tight binding Hamiltonian approximation and considering an Anderson-like disorder, we have calculated the conductance of the systems and the corresponding localization lengths. Our results show that the localization length strongly depends on the molecular concentration and on the length of the molecules, effects that are robust for different ribbon widths. These results suggest possible applications in molecular detectors or sensors based on graphene nanoribbons.

  19. Characterizing the Locality of Diabatic States for Electronic Excitation Transfer by Decomposing the Diabatic Coupling

    SciTech Connect

    Vura-Weis, Josh; Newton, M. D.; Wasielewski, Michael R; Subotnik, J.E.

    2010-12-09

    A common strategy to calculate electronic coupling matrix elements for charge or energy transfer is to take the adiabatic states generated by electronic structure computations and rotate them to form localized diabatic states. In this paper, we show that, for intermolecular transfer of singlet electronic excitation, usually we cannot fully localize the electronic excitations in this way. Instead, we calculate putative initial and final states with small excitation tails caused by weak interactions with high energy excited states in the electronic manifold. These tails do not lead to substantial changes in the total diabatic coupling between states, but they do lead to a different partitioning of the total coupling between Coulomb (Förster), exchange (Dexter), and one-electron components. The tails may be reduced by using a multistate diabatic model or eliminated entirely by truncation (denoted as “chopping”). Without more information, we are unable to conclude with certainty whether the observed diabatic tails are a physical reality or a computational artifact. This research suggests that decomposition of the diabatic coupling between chromophores into Coulomb, exchange, and one-electron components may depend strongly on the number of states considered, and such results should be treated with caution.

  20. Generation of off-axially localized tail electrons in helical antenna produce cylindrical plasma

    NASA Astrophysics Data System (ADS)

    Yadav, Sonu; Ghosh, Soumen; Bose, Sayak; Chattopadhyay, P. K.; Ghosh, J.; Bora, D.

    2016-09-01

    Off-axially localized tail electrons are observed in helical antenna produce cylindrical radio frequency (RF) plasma. Although, tail electrons are commonly observed in capacitive and inductive plasmas, localization of their population only at the off-axis of a cylindrical RF system is very unique. Moreover, we are reporting the generation of tail electrons even in absence of double layer in expanding helical antenna produce plasma. It is also shown that the confinements of these tail electrons are restricted only at the off-axis at Argon fill pressure bellow 1x10-3mbar. Experimental results will be presented to show that the tail electrons which generate off-axially in the source chamber are also found at the expansion chamber. External axial diverging magnetic field lines are bringing them from narrow source to large expansion chamber. To understand the underline mechanism of these tail electrons generation, role of (a) RF electric fields via changing RF source power and (b) their off-axial confinement with rising magnetic fields are discussed. Quantitative discussion on self-consistent model for collisionless RF power coupling with edge electrons will also be presented.

  1. Evidence of locally enhanced target heating due to instabilities of counter-streaming fast electron beams

    NASA Astrophysics Data System (ADS)

    Koester, Petra; Booth, Nicola; Cecchetti, Carlo A.; Chen, Hui; Evans, Roger G.; Gregori, Gianluca; Labate, Luca; Levato, Tadzio; Li, Bin; Makita, Mikako; Mithen, James; Murphy, Christopher D.; Notley, Margaret; Pattathil, Rajeev; Riley, David; Woolsey, Nigel; Gizzi, Leonida A.

    2015-02-01

    The high-current fast electron beams generated in high-intensity laser-solid interactions require the onset of a balancing return current in order to propagate in the target material. Such a system of counter-streaming electron currents is unstable to a variety of instabilities such as the current-filamentation instability and the two-stream instability. An experimental study aimed at investigating the role of instabilities in a system of symmetrical counter-propagating fast electron beams is presented here for the first time. The fast electron beams are generated by double-sided laser-irradiation of a layered target foil at laser intensities above 1019 W/cm2. High-resolution X-ray spectroscopy of the emission from the central Ti layer shows that locally enhanced energy deposition is indeed achieved in the case of counter-propagating fast electron beams.

  2. Evidence of locally enhanced target heating due to instabilities of counter-streaming fast electron beams

    SciTech Connect

    Koester, Petra; Cecchetti, Carlo A.; Booth, Nicola; Woolsey, Nigel; Chen, Hui; Evans, Roger G.; Gregori, Gianluca; Li, Bin; Mithen, James; Murphy, Christopher D.; Labate, Luca; Gizzi, Leonida A.; Levato, Tadzio; Makita, Mikako; Riley, David; Notley, Margaret; Pattathil, Rajeev

    2015-02-15

    The high-current fast electron beams generated in high-intensity laser-solid interactions require the onset of a balancing return current in order to propagate in the target material. Such a system of counter-streaming electron currents is unstable to a variety of instabilities such as the current-filamentation instability and the two-stream instability. An experimental study aimed at investigating the role of instabilities in a system of symmetrical counter-propagating fast electron beams is presented here for the first time. The fast electron beams are generated by double-sided laser-irradiation of a layered target foil at laser intensities above 10{sup 19 }W/cm{sup 2}. High-resolution X-ray spectroscopy of the emission from the central Ti layer shows that locally enhanced energy deposition is indeed achieved in the case of counter-propagating fast electron beams.

  3. The direction of the electron motion of H2 + in the dissociation localization

    NASA Astrophysics Data System (ADS)

    Jia, Z. M.; Zeng, Z. N.; Li, R. X.; Xu, Z. Z.

    2016-11-01

    A terahertz laser pulse is used to steer the electron motion after {{{{H}}}2}+ is irradiated by an ultrashort ultraviolet laser pulse. The numerical simulation demonstrates that the ionized electron is pulled out along the polarization direction of the electric field, in contrast, the electrons in the dissociative state move in the opposite direction to that of the electric force. Referring to the coupled dynamic equations for the 1s{σ }g and 2p{σ }u states and the analytical solution of the electron localization of the two lowest states of a double-well Coulomb potential model in an external static electric field, one can easily disclose the underlying mechanism for such an electron motion steering.

  4. Effect of structural distortion and polarization in localization of electronic excitations in organic semiconductor materials

    NASA Astrophysics Data System (ADS)

    Nayyar, Iffat; Batista, Enrique; Tretiak, Sergei; Saxena, Avadh; Smith, Darryl; Martin, Richard

    2012-02-01

    Organic polymers find varied applications in optoelectronic devices such as solar cells, light emitting diodes and lasers. Detailed understanding of charge carrier transport by polarons and excitonic energy transfer producing singlet and triplet excitations is critical to improve their efficiency. We benchmarked the ability of current functional models to describe the spatial extent of self-trapped neutral and charged excitations for MEH-PPV owing to its superior luminescence and experimental evidence. Now we are interested in distinguishing between two distinct origins leading to localization; spatial localization of the wavefunction by itself on the undistorted geometry and localization of the wavefunction assured by distortion of the structure during its relaxation. We suggest localization is produced by electronic rearrangements and character of the functional. We also observe that different functionals place the highest occupied and lowest virtual orbitals at different positions in the energy band diagram based on their ability to predict the extent of localization of these states.

  5. Perpendicular Localization of Electron Holes by Spatially Inhomogeneous Flows During Magnetic Reconnection*

    NASA Astrophysics Data System (ADS)

    Newman, D. L.; Goldman, M. V.

    2008-12-01

    Bipolar fields signaling the presence of electron phase space holes have been observed in situ by satellites near regions of magnetic reconnection in Earth's magnetopause and magnetotail. In order to identify possible origins for such holes, a recent numerical study [1] employed 1D and 2D electrostatic Vlasov simulations initialized with electron and ion distributions taken from 2D electromagnetic Particle in Cell (PIC) simulations of magnetic reconnection. Both electron-electron instabilities along the X-line and electron-ion (i.e., Buneman) instabilities along the separatrix were found to be viable sources of electron holes. However, long-lived coherent Buneman-driven holes only formed when the destabilizing current was restricted to a narrow channel perpendicular to the local magnetic field vector B. In this presentation we extend the 2D Vlasov study of electron holes driven by unstable distributions to include both e-e and e-i instabilities localized in the direction perpendicular to B. Emphasis will be placed on how the ion/electron mass and temperature ratios (mi/me and Ti/Te) and the magnetization ratios (Ωe/ωe and Ωi/ωi) influence the properties of the resulting electron holes, including their spatial size and aspect ratio. Distributions from recent implicit PIC reconnection simulations [2] will be used to guide the initialization of the Vlasov simulations. *Research supported by NASA, NSF, and DOE. [1] M. V. Goldman, D. L. Newman, and P. L. Pritchett, "Vlasov Simulations of Electron Holes Driven by Particle Distributions from PIC Reconnection Simulations with a Guide Field," submitted to Geophys.~Res.~Lett. (2008). [2] A. Divin, G. Lapenta, D. L. Newman and M. V. Goldman, "Implicit PIC Simulations of Guide Field Magnetic Reconnection," this meeting.

  6. A semi-classical model of attosecond electron localization in dissociative ionization of hydrogen.

    PubMed

    Kelkensberg, Freek; Sansone, Giuseppe; Ivanov, Misha Y; Vrakking, Marc

    2011-05-21

    In the development of attosecond molecular science, a series of experiments have recently been performed where ionic fragment asymmetries in the dissociative ionization of H(2) into H(+) + H and that of D(2) into D(+) + D were used to uncover electron localization processes that occur on the attosecond and few-femtosecond timescale. Electron localization was observed both in strong-field dissociative ionization using carrier envelope phase-stable few-cycle laser pulses [Kling et al., Science, 2006, 312, 246] and in a two-color extreme ultra-violet + infrared attosecond pump-probe experiment [Sansone et al., Nature, 2010, 465, 763]. Here we show that the observed electron localization can be well understood using a semi-classical model that describes the dynamics in terms of quasi-static states that take the interaction of the molecule with the laser field instantaneously into account. The electron localization is shown to be determined by the passage of the dissociating molecule through a regime where the laser-molecule interaction is neither diabatic nor adiabatic.

  7. Sustainable Development and African Local Government: Can Electronic Training Help Build Capacities?

    ERIC Educational Resources Information Center

    Johnson, Hazel; Thomas, Alan

    2007-01-01

    A recent study carried out by European and African organizations into the potential for electronic distance training (EDT) on sustainability in African local governments concluded that EDT was both "useful and feasible". This article reflects on some of the theoretical and practical implications of that study. It focuses on the…

  8. Ultrafast electronic response of graphene to a strong and localized electric field

    NASA Astrophysics Data System (ADS)

    Gruber, Elisabeth; Wilhelm, Richard A.; Pétuya, Rémi; Smejkal, Valerie; Kozubek, Roland; Hierzenberger, Anke; Bayer, Bernhard C.; Aldazabal, Iñigo; Kazansky, Andrey K.; Libisch, Florian; Krasheninnikov, Arkady V.; Schleberger, Marika; Facsko, Stefan; Borisov, Andrei G.; Arnau, Andrés; Aumayr, Friedrich

    2016-12-01

    The way conduction electrons respond to ultrafast external perturbations in low dimensional materials is at the core of the design of future devices for (opto)electronics, photodetection and spintronics. Highly charged ions provide a tool for probing the electronic response of solids to extremely strong electric fields localized down to nanometre-sized areas. With ion transmission times in the order of femtoseconds, we can directly probe the local electronic dynamics of an ultrathin foil on this timescale. Here we report on the ability of freestanding single layer graphene to provide tens of electrons for charge neutralization of a slow highly charged ion within a few femtoseconds. With values higher than 1012 A cm-2, the resulting local current density in graphene exceeds previously measured breakdown currents by three orders of magnitude. Surprisingly, the passing ion does not tear nanometre-sized holes into the single layer graphene. We use time-dependent density functional theory to gain insight into the multielectron dynamics.

  9. Ultrafast electronic response of graphene to a strong and localized electric field

    PubMed Central

    Gruber, Elisabeth; Wilhelm, Richard A.; Pétuya, Rémi; Smejkal, Valerie; Kozubek, Roland; Hierzenberger, Anke; Bayer, Bernhard C.; Aldazabal, Iñigo; Kazansky, Andrey K.; Libisch, Florian; Krasheninnikov, Arkady V.; Schleberger, Marika; Facsko, Stefan; Borisov, Andrei G.; Arnau, Andrés; Aumayr, Friedrich

    2016-01-01

    The way conduction electrons respond to ultrafast external perturbations in low dimensional materials is at the core of the design of future devices for (opto)electronics, photodetection and spintronics. Highly charged ions provide a tool for probing the electronic response of solids to extremely strong electric fields localized down to nanometre-sized areas. With ion transmission times in the order of femtoseconds, we can directly probe the local electronic dynamics of an ultrathin foil on this timescale. Here we report on the ability of freestanding single layer graphene to provide tens of electrons for charge neutralization of a slow highly charged ion within a few femtoseconds. With values higher than 1012 A cm−2, the resulting local current density in graphene exceeds previously measured breakdown currents by three orders of magnitude. Surprisingly, the passing ion does not tear nanometre-sized holes into the single layer graphene. We use time-dependent density functional theory to gain insight into the multielectron dynamics. PMID:28000666

  10. Investigation of S3-2 satellite data for local time variation of energetic electron precipitation

    NASA Technical Reports Server (NTRS)

    Robbe, S.; Sheldon, W. R.; Benbrook, J. R.; Bering, E. A.; Vampola, A. L.

    1994-01-01

    Data on precipitating electrons from the S3-2 satellite were investigated for local time variation at four L = 4 stations in the southern hemisphere. The equatorial pitch angles of electrons mirroring at 100 km, assumed to be the edge of the bounce loss cone, are calculated for L = 4 using the International Geomagnetic Reference Field for the epoch of the S3-2 data, along with the variation in mirror altitude per degree of equatorial pitch angle. The largest obstacle to the investigation was uneven sampling in terms of local time for all of the stations. However, this situation was improved upon by the use of S3-2 measurements at the conjugate locations of the four stations which provided additional data on electrons in the southern hemisphere bounce loss cone. Evidence for an effect of the dawn-to-dusk geoelectric field was found at two of the stations, Halley Bay and Siple, in the form of a minimum in electron precipitation at dusk. However, the present study does not completely resolve the question of local time modulation of electron precipitation at L = 4 in the southern hemisphere. Furthermore, while the average precipitation was lowest at the Kerguelen site, as would be expected on the basis of drift loss cone (DLC) theories, the intensity at that site exceeds the level that is expected on the basis of these DLC theories.

  11. Launch mission summary: Intelsat 5 (F3) Atlas/Centaur-55

    NASA Technical Reports Server (NTRS)

    1981-01-01

    Intelsat 5 (F3) spacecraft, launch vehicle, and mission are described. Information relative to launch windows, flight plan, radar and telemetry coverage, selected trajectory information, and a brief sequence of flight events is provided.

  12. Localized operator partitioning method for electronic excitation energies in the time-dependent density functional formalism.

    PubMed

    Nagesh, Jayashree; Frisch, Michael J; Brumer, Paul; Izmaylov, Artur F

    2016-12-28

    We extend the localized operator partitioning method (LOPM) [J. Nagesh, A. F. Izmaylov, and P. Brumer, J. Chem. Phys. 142, 084114 (2015)] to the time-dependent density functional theory framework to partition molecular electronic energies of excited states in a rigorous manner. A molecular fragment is defined as a collection of atoms using Becke's atomic partitioning. A numerically efficient scheme for evaluating the fragment excitation energy is derived employing a resolution of the identity to preserve standard one- and two-electron integrals in the final expressions. The utility of this partitioning approach is demonstrated by examining several excited states of two bichromophoric compounds: 9-((1- naphthyl)- methyl)- anthracene and 4-((2- naphthyl)- methyl)- benzaldehyde. The LOPM is found to provide nontrivial insights into the nature of electronic energy localization that is not accessible using a simple density difference analysis.

  13. First-Principles-Based Method for Electron Localization: Application to Monolayer Hexagonal Boron Nitride.

    PubMed

    Ekuma, C E; Dobrosavljević, V; Gunlycke, D

    2017-03-10

    We present a first-principles-based many-body typical medium dynamical cluster approximation and density function theory method for characterizing electron localization in disordered structures. This method applied to monolayer hexagonal boron nitride shows that the presence of boron vacancies could turn this wide-gap insulator into a correlated metal. Depending on the strength of the electron interactions, these calculations suggest that conduction could be obtained at a boron vacancy concentration as low as 1.0%. We also explore the distribution of the local density of states, a fingerprint of spatial variations, which allows localized and delocalized states to be distinguished. The presented method enables the study of disorder-driven insulator-metal transitions not only in h-BN but also in other physical materials.

  14. First-Principles-Based Method for Electron Localization: Application to Monolayer Hexagonal Boron Nitride

    NASA Astrophysics Data System (ADS)

    Ekuma, C. E.; Dobrosavljević, V.; Gunlycke, D.

    2017-03-01

    We present a first-principles-based many-body typical medium dynamical cluster approximation and density function theory method for characterizing electron localization in disordered structures. This method applied to monolayer hexagonal boron nitride shows that the presence of boron vacancies could turn this wide-gap insulator into a correlated metal. Depending on the strength of the electron interactions, these calculations suggest that conduction could be obtained at a boron vacancy concentration as low as 1.0%. We also explore the distribution of the local density of states, a fingerprint of spatial variations, which allows localized and delocalized states to be distinguished. The presented method enables the study of disorder-driven insulator-metal transitions not only in h -BN but also in other physical materials.

  15. New approach to Tolman's electronic parameter based on local vibrational modes.

    PubMed

    Kalescky, Robert; Kraka, Elfi; Cremer, Dieter

    2014-01-06

    Tolman's electronic parameter (TEP) derived from the A1-symmetrical CO stretching frequency of nickel-phosphine-tricarbonyl complexes, R3PNi(CO)3, is brought to a new, improved level by replacing normal with local vibrational frequencies. CO normal vibrational frequencies are always flawed by mode-mode coupling especially with metal-carbon stretching modes, which leads to coupling frequencies as large as 100 cm(-1) and can become even larger when the transition metal and the number of ligands is changed. Local TEP (LTEP) values, being based on local CO stretching force constants rather than normal mode frequencies, no longer suffer from mode coupling and mass effects. For 42 nickel complexes of the type LNi(CO)3, it is shown that LTEP values provide a different ordering of ligand electronic effects as previously suggested by TEP and CEP values. The general applicability of the LTEP concept is demonstrated.

  16. Distinct local electronic structure and magnetism for Mn in amorphous Si and Ge

    SciTech Connect

    Zeng, Li; Cao, J. X.; Helgren, E.; Karel, J.; Arenholz, E.; Ouyang, Lu; Smith, David J.; Wu, R. Q.; Hellman, F.

    2010-06-01

    Transition metals such as Mn generally have large local moments in covalent semiconductors due to their partially filled d shells. However, Mn magnetization in group-IV semiconductors is more complicated than often recognized. Here we report a striking crossover from a quenched Mn moment (<0.1 {mu}{sub B}) in amorphous Si (a-Si) to a large distinct local Mn moment ({ge}3{mu}{sub B}) in amorphous Ge (a-Ge) over a wide range of Mn concentrations (0.005-0.20). Corresponding differences are observed in d-shell electronic structure and the sign of the Hall effect. Density-functional-theory calculations show distinct local structures, consistent with different atomic density measured for a-Si and a-Ge, respectively, and the Mn coordination number N{sub c} is found to be the key factor. Despite the amorphous structure, Mn in a-Si is in a relatively well-defined high coordination interstitial type site with broadened d bands, low moment, and electron (n-type) carriers, while Mn in a-Ge is in a low coordination substitutional type site with large local moment and holes (p-type) carriers. Moreover, the correlation between N{sub c} and the magnitude of the local moment is essentially independent of the matrix; the local Mn moments approach zero when N{sub c} > 7 for both a-Si and a-Ge.

  17. Local electron heating in the Io plasma torus associated with Io: the HISAKI observation

    NASA Astrophysics Data System (ADS)

    Tsuchiya, F.; Yoshioka, K.; Kimura, T.; Murakami, G.; Kagitani, M.; Yamazaki, A.; Kasaba, Y.; Sakanoi, T.; Yoshikawa, I.; Nozawa, H.

    2014-12-01

    Io-correlated brightness change in Io plasma torus (IPT) has been discovered by Voyager and show an evidence of local electron heating around Io. However, the amount of observation data is still limited to investigate its detail properties. In addition, the clear Io-correlated change has not been detected by EUVE and Cassini observations. Cause of the Io-correlated effect is still open issue. The HISAKI satellite was launched on Sep. 14, 2013 and started observation of IPT and Jovian aurora for more than two months since the end of Dec. 2013. EUV spectrograph onboard the HISAKI satellite covers wavelength range from 55 to 145 nm, a wide slit which had a field of view of 400 x 140 arc-second was chosen to measure radial distribution and time variation of IPT. Observation of IPT with HISAKI showed clear Io-correlated brightness change since the Voyager observation. The amplitude of the periodic variation associated with Io's orbital period was found. It also showed long-term variation during the HISAKI's observation period. Through the observation period, the amplitude was larger in the short wavelength than in long wavelength. The wavelength dependence suggests significant electron heating and/or hot electron production. The Io phase dependence shows that bright region is located just downstream of Io. These are evidence of local electron heating around/downstream of Io and consistent with the Voyager result. The brightness also depends on system-III longitude and has local maximum around 120 and 300 degrees. Based on an empirical model of IPT, electron density at Io also shows maxima around the same longitudes. This suggests that the electron heating process is related with plasma density at Io. Candidate mechanisms which are responsible for the electron heating will be discussed.

  18. Electronic structure of delta-Pu and PuCoGa[sub 3] from photoemission and the mixed level model

    SciTech Connect

    Joyce, J. J.; Wills, J. M.; Durakiewicz, T.; Butterfield, M. T.; Guziewicz, E.; Sarrao, John L.,; Arko, A. J.; Moore, D. P.; Morales, L. A.; Eriksson, O.

    2004-01-01

    The electronic structure of {delta}-phase Pu metal and the Pu-based superconductor PuCoGa{sub 5} is explored using photoelectron spectroscopy and a novel theoretical scheme. Excellent agreement between calculation and experiment defines a path forward for understanding electronic structure aspects of Pu-based materials. The photoemission results show two separate regions of 5f electron spectral intensity, one at the Fermi energy and another centered 1.2 eV below the Fermi level. A comparison is made between the photoemission data and five computational schemes for {delta}-Pu. The results for {delta}-Pu and PuCoGa{sub 5} indicate 5f electron behavior on the threshold between localized and itinerant and a broader framework for understanding the fundamental electronic properties of the Pu 5f levels in general within two configurations, one localized and one itinerant.

  19. Effect of non-local electron conduction in compression of solid ball target for fast ignition

    NASA Astrophysics Data System (ADS)

    Nagatomo, Hideo; Asahina, Takashi; Nicolai, Philippe; Sunahara, Atsushi; Johzaki, Tomoyuki

    2016-10-01

    In the first phase of the fast ignition scheme, fuel target is compressed by the implosion laser, where only achievement of high dense fuel is required because the increment of the temperature to ignite the fuel is given by heating lasers. The ideal compression method for solid target is isentropic compression with tailored pulse shape. However, it requires the high laser intensity >1015 W/cm2 which cause the hot electrons. Numerical simulation for these conditions non-local electron transport model is necessary. Recently, we have installed SNB model to a 2-D radiation hydrodynamic simulation code. In this presentation, effect of hot electron in isentropic compression and optimum method are discussed, which may be also significant for shock ignition scheme. Also effect of external magnetic field to the hot electron will be considered. This study was supported by JSPS KAKENHI Grant No. 26400532.

  20. Sum rules and static local-field corrections of electron liquids in two and three dimensions

    NASA Technical Reports Server (NTRS)

    Iwamoto, N.

    1984-01-01

    The dielectric functions of electron liquids which take into account short-range electron-electron correlations via the static local-field corrections are examined in the light of the frequency-moment sum rules. The formation is given for degenerate as well as classical electron liquids in arbitrary (d) spatial dimensions, which is suitable for comparison between the two- and three-dimensional cases. By using the virial equations of state it is shown that such dielectric functions cannot satisfy the compressibility sum rule and the third-frequency-moment sum rule simultaneously. In the degenerate case, the plasmon, single-pair, and multipair contributions to the sum rules are analyzed, and the reason for this incompatibility is discussed.

  1. Role of electronic localization in the phosphorescence of iridium sensitizing dyes.

    PubMed

    Himmetoglu, Burak; Marchenko, Alex; Dabo, Ismaïla; Cococcioni, Matteo

    2012-10-21

    In this work we present a systematic study of three representative iridium dyes, namely, Ir(ppy)(3), FIrpic, and PQIr, which are commonly used as sensitizers in organic optoelectronic devices. We show that electronic correlations play a crucial role in determining the excited-state energies in these systems, due to localization of electrons on Ir d orbitals. Electronic localization is captured by employing hybrid functionals within time-dependent density-functional theory and with Hubbard-model corrections within the Δ-SCF approach. The performance of both methods are studied comparatively and shown to be in good agreement with experiment. The Hubbard-corrected functionals provide further insight into the localization of electrons and on the charge-transfer character of excited-states. The gained insight allows us to comment on envisioned functionalization strategies to improve the performance of these systems. Complementary discussions on the Δ-SCF method are also presented in order to fill some of the gaps in the literature.

  2. Aromaticity of rings-in-molecules (RIMs) from electron localization-delocalization matrices (LDMs)

    NASA Astrophysics Data System (ADS)

    Sumar, Ismat; Cook, Ronald; Ayers, Paul W.; Matta, Chérif F.

    2016-01-01

    A new and powerful molecular descriptor termed the LDM (localization-delocalization matrix) has recently been proposed as a molecular fingerprinting tool and has been shown to yield robust quantitative-structure-to-activity/property-relationships (QSAR/QSPR). An LDM lists the average number of electrons localized within an atom in a molecule along its diagonal while the off-diagonal elements are the pair-wise average number of electrons shared between every pair of atoms in the molecule, bonded or not. Hence, the LDM is a representation of a fuzzy molecular graph that accounts for the whereabouts of all electron(s) in the molecule and can be expected to encode for several facets of its chemistry at once. We show that the LDM captures the aromatic character of a ring-in-a-molecule by comparing the aromaticity ranking based on the LDMs and their eigenvalues of 6-membered carbon rings within (polycyclic) benzenoid hydrocarbons with the ranking based on four well-established local aromaticity measures (harmonic oscillator model of aromaticity, acromatic fluctuation index, para delocalization index, and nucleus independent chemical shift(0)). This paper is dedicated to the memory of Professor Paul von Ragué Schleyer (1930-2014).

  3. High-energy localized eigenstates of an electronic resonator in a magnetic field

    NASA Astrophysics Data System (ADS)

    Zalipaev, V. V.; Kusmartsev, F. V.; Popov, M. M.

    2008-02-01

    We present a semiclassical analysis of the high-energy eigenstates of an electron inside a closed resonator. An asymptotic method of the construction of the energy spectrum and eigenfunctions, localized in the small neighborhood of a periodic orbit, is developed in the presence of a homogeneous magnetic field and arbitrary scalar potential. The isolated periodic orbit is confined between two interfaces which could be planar, concave or even convex. Such a system represents a quantum electronic resonator, an analog of the well-known high-frequency optical or acoustic resonator with eigenmodes called 'bouncing ball vibrations'. The first step in the asymptotic analysis involves constructing a solitary localized asymptotic solution to the Schrödinger equation (electronic Gaussian beam—wavepackage). Then, the stability of a closed continuous family of periodic trajectories confined between two reflecting surfaces of the resonator boundary was studied. The asymptotics of the eigenfunctions were constructed as a superposition of two electronic Gaussian beams propagating in opposite directions between two reflecting points of the periodic orbits. The asymptotics of the energy spectrum are obtained by the generalized Bohr-Sommerfeld quantization condition derived as a requirement for the eigenfunction asymptotics to be periodic. For one class of periodic orbits, localized eigenstates were computed numerically by the finite element method using FEMLAB and proved to be in a very good agreement with those computed semiclassically.

  4. Effect of oxygen deficiency on electronic properties and local structure of amorphous tantalum oxide thin films

    SciTech Connect

    Denny, Yus Rama; Firmansyah, Teguh; Oh, Suhk Kun; Kang, Hee Jae; Yang, Dong-Seok; Heo, Sung; Chung, JaeGwan; Lee, Jae Cheol

    2016-10-15

    Highlights: • The effect of oxygen flow rate on electronic properties and local structure of tantalum oxide thin films was studied. • The oxygen deficiency induced the nonstoichiometric state a-TaOx. • A small peak at 1.97 eV above the valence band side appeared on nonstoichiometric Ta{sub 2}O{sub 5} thin films. • The oxygen flow rate can change the local electronic structure of tantalum oxide thin films. - Abstract: The dependence of electronic properties and local structure of tantalum oxide thin film on oxygen deficiency have been investigated by means of X-ray photoelectron spectroscopy (XPS), Reflection Electron Energy Loss Spectroscopy (REELS), and X-ray absorption spectroscopy (XAS). The XPS results showed that the oxygen flow rate change results in the appearance of features in the Ta 4f at the binding energies of 23.2 eV, 24.4 eV, 25.8, and 27.3 eV whose peaks are attributed to Ta{sup 1+}, Ta{sup 2+}, Ta{sup 3+}/Ta{sup 4+}, and Ta{sup 5+}, respectively. The presence of nonstoichiometric state from tantalum oxide (TaOx) thin films could be generated by the oxygen vacancies. In addition, XAS spectra manifested both the increase of coordination number of the first Ta-O shell and a considerable reduction of the Ta-O bond distance with the decrease of oxygen deficiency.

  5. Interaction of electrons with optical phonons localized in a quantum well

    SciTech Connect

    Pozela, J. Pozela, K.; Juciene, V.; Suziedelis, A.; Shkolnik, A. S.; Mikhrin, S. S.; Mikhrin, V. S.

    2009-12-15

    The scattering rate of electrons in a quantum well by localized polar optical and interface phonons is considered. The dependence of the force of the electron-phonon interaction on the frequency of optical phonons in materials of the heterostructure forming the electron and phonon quantum wells is determined. It is shown that, by varying the composition of semiconductors forming the quantum well and its barriers, it is possible to vary the scattering rates of electrons by a factor of several times. The scattering rates of electrons by polar optical phonons are calculated depending on the fractions In{sub x} and In{sub y} in the composition of semiconductors forming the In{sub x}Al{sub 1-x}As/In{sub y}Ga{sub 1-y}As quantum wells. Dependences of the mobility and saturated drift velocity of electrons in high electric fields and quantum wells In{sub y}Ga{sub 1-y}As on the composition of the In{sub x}Al{sub 1-x}As barriers introduced into quantum wells are determined experimentally. The electron mobility increases, while the saturated drift velocity decreases as the fraction of In{sub x} in the composition of barriers is increased.

  6. An efficient implementation of the localized operator partitioning method for electronic energy transfer

    SciTech Connect

    Nagesh, Jayashree; Brumer, Paul; Izmaylov, Artur F.

    2015-02-28

    The localized operator partitioning method [Y. Khan and P. Brumer, J. Chem. Phys. 137, 194112 (2012)] rigorously defines the electronic energy on any subsystem within a molecule and gives a precise meaning to the subsystem ground and excited electronic energies, which is crucial for investigating electronic energy transfer from first principles. However, an efficient implementation of this approach has been hindered by complicated one- and two-electron integrals arising in its formulation. Using a resolution of the identity in the definition of partitioning, we reformulate the method in a computationally efficient manner that involves standard one- and two-electron integrals. We apply the developed algorithm to the 9 − ((1 − naphthyl) − methyl) − anthracene (A1N) molecule by partitioning A1N into anthracenyl and CH{sub 2} − naphthyl groups as subsystems and examine their electronic energies and populations for several excited states using configuration interaction singles method. The implemented approach shows a wide variety of different behaviors amongst the excited electronic states.

  7. Copper plasmonics and catalysis: role of electron-phonon interactions in dephasing localized surface plasmons.

    PubMed

    Sun, Qi-C; Ding, Yuchen; Goodman, Samuel M; Funke, Hans H; Nagpal, Prashant

    2014-11-07

    Copper metal can provide an important alternative for the development of efficient, low-cost and low-loss plasmonic nanoparticles, and selective nanocatalysts. However, poor chemical stability and lack of insight into photophysics and plasmon decay mechanisms has impeded study. Here, we use smooth conformal ALD coating on copper nanoparticles to prevent surface oxidation, and study dephasing time for localized surface plasmons on different sized copper nanoparticles. Using dephasing time as a figure of merit, we elucidate the role of electron-electron, electron-phonon, impurity, surface and grain boundary scattering on the decay of localized surface plasmon waves. Using our quantitative analysis and different temperature dependent measurements, we show that electron-phonon interactions dominate over other scattering mechanisms in dephasing plasmon waves. While interband transitions in copper metal contributes substantially to plasmon losses, tuning surface plasmon modes to infrared frequencies leads to a five-fold enhancement in the quality factor. These findings demonstrate that conformal ALD coatings can improve the chemical stability for copper nanoparticles, even at high temperatures (>300 °C) in ambient atmosphere, and nanoscaled copper is a good alternative material for many potential applications in nanophotonics, plasmonics, catalysis and nanoscale electronics.

  8. Delocalized and localized states of eg electrons in half-doped manganites.

    PubMed

    Winkler, E L; Tovar, M; Causa, M T

    2013-07-24

    We have studied the magnetic behaviour of half-doped manganite Y0.5Ca0.5MnO3 in an extended range of temperatures by means of magnetic susceptibility, χ(T), and electron spin resonance (ESR) experiments. At high temperature the system crystallizes in an orthorhombic structure. The resistivity value, ρ ≃ 0.05 Ω cm at 500 K, indicates a metallic behaviour, while the Curie-Weiss dependence of χ(T) and the thermal evolution of the ESR parameters are very well described by a model that considers a system conformed by localized Mn(4+) cores, [Formula: see text], and itinerant, eg, electrons. The strong coupling between t2g and eg electrons results in an enhanced Curie constant and an FM Curie-Weiss temperature that overcomes the AFM interactions between the [Formula: see text] cores. A transition to a more distorted phase is observed at T ≈ 500 K and signatures of localization of the eg electrons appear in the χ(T) behaviour below 300 K. A new Curie-Weiss regime is observed, where the Curie-constant value is consistent with dimer formation. Based on mean-field calculations, the dimer formation is predicted as a function of the interaction strength between the t2g and eg electrons.

  9. Electron affinities for rare gases and some actinides from local-spin-density-functional theory

    SciTech Connect

    Guo, Y.; Wrinn, M.C.; Whitehead, M.A. )

    1989-12-01

    The negative ions of the rare gases (He, Ne, Ar, Kr, Xe, and Rn) and some actinides (Pu, Am, Bk, Cf, and Es) have been calculated self-consistently by the generalized exchange local-spin-density-functional theory with self-interaction correction and correlation. The electron affinities were obtained as the differences between the statistical total energies of the negative ions and neutral atoms; the electron affinities were positive around several millirydbergs. Consequently, the negative ions are predicted stable for the rare gases and actinides.

  10. Second Line of Defense: Electronic Maintenance Reports, Local Maintenance Provider User Guide, Rev. 3

    SciTech Connect

    Leigh, Richard J.

    2012-09-01

    The Electronic Maintenance Report forms allow Local Maintenance Providers (LMP) and other program staff to enter maintenance information into a simple and secure system. This document describes the features and information required to complete the Maintenance Report forms. It is expected that all Corrective Maintenance Reports from LMPs will be submitted electronically into the SLD Portal. As an exception (e.g., when access to the SLD Portal is unavailable), Maintenance Reports can be submitted via a secure Adobe PDF form available through the Sustainability Manager assigned to each country.

  11. Dissociative electron attachment to the H2O molecule II: nucleardynamics on coupled electronic surfaces within the local complexpotential model

    SciTech Connect

    Haxton, Daniel J.; Rescigno, Thomas N.; McCurdy, C. William

    2006-12-21

    We report the results of a first-principles study of dissociative electron attachment (DEA) to H{sub 2}O. The cross sections were obtained from nuclear dynamics calculations carried out in full dimensionality within the local complex potential model by using the multi-configuration time-dependent Hartree method. The calculations employ our previously obtained global, complex-valued, potential energy surfaces for the three ({sup 2}B{sub 1}, {sup 2}A{sub 1}, and {sup 2}B{sub 2}) electronic Feshbach resonances involved in this process. These three metastable states of H{sub 2}O{sup -} undergo several degeneracies, and we incorporate both the Renner-Teller coupling between the {sup 2}B{sub 1} and {sup 2}A{sub 1} states, as well as the conical intersection between the {sup 2}A{sub 1} and {sup 2}B{sub 2} states, into our treatment. The nuclear dynamics are inherently multi-dimensional and involve branching between different final product arrangements as well as extensive excitation of the diatomic fragment. Our results successfully mirror the qualitative features of the major fragment channels observed, but are less successful in reproducing the available results for some of the minor channels. We comment on the applicability of the local complex potential model to such a complicated resonant system.

  12. Localize.pytom: a modern webserver for cryo-electron tomography

    PubMed Central

    Hrabe, Thomas

    2015-01-01

    Localize.pytom, available through http://localize.pytom.org is a webserver for the localize module in the PyTom package. It is a free website and open to all users and there is no login requirement. The server accepts tomograms as they are imaged and reconstructed by Cryo-Electron Tomography (CET) and returns densities and coordinates of candidate-macromolecules in the tomogram. Localization of macromolecules in cryo-electron tomograms is one of the key procedures to unravel structural features of imaged macromolecules. Positions of localized molecules are further used for structural analysis by single particle procedures such as fine alignment, averaging and classification. Accurate localization can be furthermore used to generate molecular atlases of whole cells. Localization uses a cross-correlation-based score and requires a reference volume as input. A reference can either be a previously detected macromolecular structure or extrapolated on the server from a specific PDB chain. Users have the option to use either coarse or fine angular sampling strategies based on uniformly distributed rotations and to accurately compensate for the CET common ‘Missing Wedge’ artefact during sampling. After completion, all candidate macromolecules cut out from the tomogram are available for download. Their coordinates are stored and available in XML format, which can be easily integrated into successive analysis steps in other software. A pre-computed average of the first one hundred macromolecules is also available for immediate download, and the user has the option to further analyse the average, based on the detected score distribution in a novel web-density viewer. PMID:25934806

  13. Local temperature measurements on nanoscale materials using a movable nanothermocouple assembled in a transmission electron microscope

    NASA Astrophysics Data System (ADS)

    Kawamoto, Naoyuki; Wang, Ming-Sheng; Wei, Xianlong; Tang, Dai-Ming; Murakami, Yasukazu; Shindo, Daisuke; Mitome, Masanori; Golberg, Dmitri

    2011-12-01

    A nanoscale thermocouple consisting of merged Cu and Cu-Ni tips is developed for local temperature measurements on advanced nanomaterials by using a probing technique in a high-resolution transmission electron microscope (TEM) equipped with a double probe scanning tunneling microcopy (STM) unit. The fabricated nanothermocouple works as the so-called T-type thermocouple and displays a quick response and high spatial and thermal resolutions. A generated thermoelectromotive force which reflects rapid temperature changes controlled by electron beam intensity alternations on a metal nanoelectrode proves the technique's usefulness for high-precision local temperature measurements. The developed method demonstrates the effectiveness while also measuring temperature changes in Joule heated multi-walled carbon nanotubes (CNTs) and in a modeled electrical conductive composite nanosystem.

  14. Exploiting the spatial locality of electron correlation within the parametric two-electron reduced-density-matrix method

    NASA Astrophysics Data System (ADS)

    DePrince, A. Eugene; Mazziotti, David A.

    2010-01-01

    The parametric variational two-electron reduced-density-matrix (2-RDM) method is applied to computing electronic correlation energies of medium-to-large molecular systems by exploiting the spatial locality of electron correlation within the framework of the cluster-in-molecule (CIM) approximation [S. Li et al., J. Comput. Chem. 23, 238 (2002); J. Chem. Phys. 125, 074109 (2006)]. The 2-RDMs of individual molecular fragments within a molecule are determined, and selected portions of these 2-RDMs are recombined to yield an accurate approximation to the correlation energy of the entire molecule. In addition to extending CIM to the parametric 2-RDM method, we (i) suggest a more systematic selection of atomic-orbital domains than that presented in previous CIM studies and (ii) generalize the CIM method for open-shell quantum systems. The resulting method is tested with a series of polyacetylene molecules, water clusters, and diazobenzene derivatives in minimal and nonminimal basis sets. Calculations show that the computational cost of the method scales linearly with system size. We also compute hydrogen-abstraction energies for a series of hydroxyurea derivatives. Abstraction of hydrogen from hydroxyurea is thought to be a key step in its treatment of sickle cell anemia; the design of hydroxyurea derivatives that oxidize more rapidly is one approach to devising more effective treatments.

  15. EPW: A program for calculating the electron-phonon coupling using maximally localized Wannier functions

    NASA Astrophysics Data System (ADS)

    Noffsinger, Jesse; Giustino, Feliciano; Malone, Brad D.; Park, Cheol-Hwan; Louie, Steven G.; Cohen, Marvin L.

    2010-12-01

    EPW ( Electron- Phonon coupling using Wannier functions) is a program written in Fortran90 for calculating the electron-phonon coupling in periodic systems using density-functional perturbation theory and maximally localized Wannier functions. EPW can calculate electron-phonon interaction self-energies, electron-phonon spectral functions, and total as well as mode-resolved electron-phonon coupling strengths. The calculation of the electron-phonon coupling requires a very accurate sampling of electron-phonon scattering processes throughout the Brillouin zone, hence reliable calculations can be prohibitively time-consuming. EPW combines the Kohn-Sham electronic eigenstates and the vibrational eigenmodes provided by the Quantum ESPRESSO package (see Giannozzi et al., 2009 [1]) with the maximally localized Wannier functions provided by the wannier90 package (see Mostofi et al., 2008 [2]) in order to generate electron-phonon matrix elements on arbitrarily dense Brillouin zone grids using a generalized Fourier interpolation. This feature of EPW leads to fast and accurate calculations of the electron-phonon coupling, and enables the study of the electron-phonon coupling in large and complex systems. Program summaryProgram title: EPW Catalogue identifier: AEHA_v1_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AEHA_v1_0.html Program obtainable from: CPC Program Library, Queen's University, Belfast, N. Ireland Licensing provisions: GNU Public License No. of lines in distributed program, including test data, etc.: 304 443 No. of bytes in distributed program, including test data, etc.: 1 487 466 Distribution format: tar.gz Programming language: Fortran 90 Computer: Any architecture with a Fortran 90 compiler Operating system: Any environment with a Fortran 90 compiler Has the code been vectorized or parallelized?: Yes, optimized for 1 to 64 processors RAM: Heavily system dependent, as small as a few MB Supplementary material: A copy of the "EPW/examples" directory

  16. Anomalous organic magnetoresistance from competing carrier-spin-dependent interactions with localized electronic and nuclear spins

    NASA Astrophysics Data System (ADS)

    Flatté, Michael E.

    Transport of carriers through disordered electronic energy landscapes occurs via hopping or tunneling through various sites, and can enhance the effects of carrier spin dynamics on the transport. When incoherent hopping preserves the spin orientation of carriers, the magnetic-field-dependent correlations between pairs of spins influence the charge conductivity of the material. Examples of these phenomena have been identified in hopping transport in organic semiconductors and colloidal quantum dots, as well as tunneling through oxide barriers in complex oxide devices, among other materials. The resulting room-temperature magnetic field effects on the conductivity or electroluminescence require external fields of only a few milliTesla. These magnetic field effects can be dramatically modified by changes in the local spin environment. Recent theoretical and experimental work has identified a regime for low-field magnetoresistance in organic semiconductors in which the spin-relaxing effects of localized nuclear spins and electronic spins interfere1. The regime is studied experimentally by the controlled addition of localized electronic spins, through the addition of a stable free radical (galvinoxyl) to a material (MEH-PPV) that exhibits substantial room-temperature magnetoresistance (20 initially suppressed by the doping, as the localized electronic spin mixes one of the two spins whose correlation controls the transport. At intermediate doping, when one spin is fully decohered but the other is not, there is a regime where the magnetoresistance is insensitive to the doping level. For much greater doping concentrations the magnetoresistance is fully suppressed as both spins that control the charge conductivity of the material are mixed. The behavior is described within a theoretical model describing the effect of carrier spin dynamics on the current. Generalizations to amorphous and other disordered crystalline semiconductors will also be described. This work was

  17. EPW: Electron-phonon coupling, transport and superconducting properties using maximally localized Wannier functions

    NASA Astrophysics Data System (ADS)

    Poncé, S.; Margine, E. R.; Verdi, C.; Giustino, F.

    2016-12-01

    The EPW (Electron-Phonon coupling using Wannier functions) software is a Fortran90 code that uses density-functional perturbation theory and maximally localized Wannier functions for computing electron-phonon couplings and related properties in solids accurately and efficiently. The EPW v4 program can be used to compute electron and phonon self-energies, linewidths, electron-phonon scattering rates, electron-phonon coupling strengths, transport spectral functions, electronic velocities, resistivity, anisotropic superconducting gaps and spectral functions within the Migdal-Eliashberg theory. The code now supports spin-orbit coupling, time-reversal symmetry in non-centrosymmetric crystals, polar materials, and k and q-point parallelization. Considerable effort was dedicated to optimization and parallelization, achieving almost a ten times speedup with respect to previous releases. A computer test farm was implemented to ensure stability and portability of the code on the most popular compilers and architectures. Since April 2016, version 4 of the EPW code is fully integrated in and distributed with the Quantum ESPRESSO package, and can be downloaded through QE-forge at http://qe-forge.org/gf/project/q-e.

  18. Relationship between edge localized mode severity and electron transport in the National Spherical Torus Experiment

    SciTech Connect

    Tritz, K.; Stutman, D.; Delgado-Aparicio, L.; Finkenthal, M.; Kaye, S.; Bell, R.; LeBlanc, B.; Mazzucato, E.; Park, H.; Smith, D. R.; Maingi, R.; Sabbagh, S.; Domier, C. W.; Luhmann, N. C. Jr.; Lee, W.

    2008-05-15

    In the National Spherical Torus Experiment [J. Menard et al., Nucl. Fusion 47, S645 (2007)], 'giant' edge localized modes (ELMs) can occur resulting in a loss of plasma stored energy of up to 30%. These events are distinct from type I ELMs, whose energy loss is typically 4-10%, and they are accompanied by a cold pulse that causes a global decrease in the electron temperature profile. Estimates of the electron thermal transport during the cold pulses show a large enhancement over the underlying cross-field thermal diffusivity, {chi}{sub e}, of up to several tens of m{sup 2}/s. Following the ELM, short-wavelength fluctuations increase in the plasma edge and core, corresponding to an increase in the electron temperature gradient from the propagating cold pulse. Fast electron temperature measurements indicate that the normalized electron temperature scale length, R/L{sub Te}, reaches the threshold value for instability predicted by a fit to linear stability calculations. This is observed on time scales that match the growth of the high-k fluctuations in the plasma core, indicating that the enhanced {chi}{sub e} and energy loss from the 'giant' ELM appears to be related to critical gradient physics and the destabilization of electron temperature gradient modes.

  19. Relationship between edge localized mode severity and electron transport in the National Spherical Torus Experiment

    SciTech Connect

    Tritz, K.; Kaye, S.; Maingi, R.; Sabbagh, S. A.; Stutman, D.; Bell, R. E.; Delgado-Aparicio, L.; Domier, C. W.; Finkenthal, M.; LeBlanc, B; Lee, W.; Luhmann, N. C.; Mazzucato, E.; Park, H.; Smith, D. R.

    2008-01-01

    n the National Spherical Torus Experiment [J. Menard , Nucl. Fusion 47, S645 (2007)], "giant" edge localized modes (ELMs) can occur resulting in a loss of plasma stored energy of up to 30%. These events are distinct from type I ELMs, whose energy loss is typically 4-10%, and they are accompanied by a cold pulse that causes a global decrease in the electron temperature profile. Estimates of the electron thermal transport during the cold pulses show a large enhancement over the underlying cross-field thermal diffusivity, chi(e), of up to several tens of m(2)/s. Following the ELM, short-wavelength fluctuations increase in the plasma edge and core, corresponding to an increase in the electron temperature gradient from the propagating cold pulse. Fast electron temperature measurements indicate that the normalized electron temperature scale length, R/L-Te, reaches the threshold value for instability predicted by a fit to linear stability calculations. This is observed on time scales that match the growth of the high-k fluctuations in the plasma core, indicating that the enhanced chi(e) and energy loss from the "giant" ELM appears to be related to critical gradient physics and the destabilization of electron temperature gradient modes. (C) 2008 American Institute of Physics.

  20. Relationship between edge localized mode severity and electron transport in the National Spherical Torus Experimenta)

    NASA Astrophysics Data System (ADS)

    Tritz, K.; Kaye, S.; Maingi, R.; Sabbagh, S.; Stutman, D.; Bell, R.; Delgado-Aparicio, L.; Domier, C. W.; Finkenthal, M.; LeBlanc, B.; Lee, W.; Luhmann, N. C.; Mazzucato, E.; Park, H.; Smith, D. R.

    2008-05-01

    In the National Spherical Torus Experiment [J. Menard et al., Nucl. Fusion 47, S645 (2007)], "giant" edge localized modes (ELMs) can occur resulting in a loss of plasma stored energy of up to 30%. These events are distinct from type I ELMs, whose energy loss is typically 4-10%, and they are accompanied by a cold pulse that causes a global decrease in the electron temperature profile. Estimates of the electron thermal transport during the cold pulses show a large enhancement over the underlying cross-field thermal diffusivity, χe, of up to several tens of m2/s. Following the ELM, short-wavelength fluctuations increase in the plasma edge and core, corresponding to an increase in the electron temperature gradient from the propagating cold pulse. Fast electron temperature measurements indicate that the normalized electron temperature scale length, R /LTe, reaches the threshold value for instability predicted by a fit to linear stability calculations. This is observed on time scales that match the growth of the high-k fluctuations in the plasma core, indicating that the enhanced χe and energy loss from the "giant" ELM appears to be related to critical gradient physics and the destabilization of electron temperature gradient modes.

  1. Time-dependent behavior of a localized electron at a heterojunction boundary of graphene

    SciTech Connect

    Jang, Min S.; Kim, Hyungjun; Atwater, Harry A.; Goddard, William A.

    2010-01-01

    We develop a finite-difference time-domain(FDTD) method for simulating the dynamics of graphene electrons, denoted GraFDTD. We then use GraFDTD to study the temporal behavior of a single localized electron wave packet, showing that it exhibits optical-like dynamics including the Goos–Hänchen effect [F. Goos and H. Hänchen, Ann. Phys.436, 333 (1947)] at a heterojunction, but the behavior is quantitatively different than for electromagnetic waves. This suggests issues that must be addressed in designing graphene-based electronic devices analogous to optical devices. GraFDTD should be useful for studying such complex time-dependent behavior of a quasiparticle in graphene.

  2. Electron states in amorphous semiconductor : localized to extended transition and transport

    NASA Astrophysics Data System (ADS)

    Dong, Jianjun; Drabold, David A.

    1996-11-01

    We study the electron states in a large (4096 atoms) and realistic model of amorphous diamond (B. Djordjevic, M. Thorpe and F. Wooten, Phys. Rev. B, 52) 5685, (1995) . We compute the full electronic density of states with the linear scaling Maximum Entropy method footnote D. A. Drabold and O. F. Sankey, Phys. Rev. Lett., 52 3631, (1993) . Approximately exponential band tails are observed at both valence- and conduction-bandfootnote J. Dong and D.A. Drabold, ( to appear ) Phys. Rev. B, 54 , (1996) . We also explicitly compute more than 700 electron states in the vincity of band-gap using a modified Lanczos approach. Within finite-size limitations, the localized to extended transition is illustrated for this model. The zero temperature dc conductivity is estimated from the Kubo formula.

  3. Local conditions for the Pauli potential in order to yield self-consistent electron densities exhibiting proper atomic shell structure

    SciTech Connect

    Finzel, Kati

    2016-01-21

    The local conditions for the Pauli potential that are necessary in order to yield self-consistent electron densities from orbital-free calculations are investigated for approximations that are expressed with the help of a local position variable. It is shown that those local conditions also apply when the Pauli potential is given in terms of the electron density. An explicit formula for the Ne atom is given, preserving the local conditions during the iterative procedure. The resulting orbital-free electron density exhibits proper shell structure behavior and is in close agreement with the Kohn-Sham electron density. This study demonstrates that it is possible to obtain self-consistent orbital-free electron densities with proper atomic shell structure from simple one-point approximations for the Pauli potential at local density level.

  4. Local atomic and electronic structure of boron chemical doping in monolayer graphene.

    PubMed

    Zhao, Liuyan; Levendorf, Mark; Goncher, Scott; Schiros, Theanne; Pálová, Lucia; Zabet-Khosousi, Amir; Rim, Kwang Taeg; Gutiérrez, Christopher; Nordlund, Dennis; Jaye, Cherno; Hybertsen, Mark; Reichman, David; Flynn, George W; Park, Jiwoong; Pasupathy, Abhay N

    2013-10-09

    We use scanning tunneling microscopy and X-ray spectroscopy to characterize the atomic and electronic structure of boron-doped and nitrogen-doped graphene created by chemical vapor deposition on copper substrates. Microscopic measurements show that boron, like nitrogen, incorporates into the carbon lattice primarily in the graphitic form and contributes ~0.5 carriers into the graphene sheet per dopant. Density functional theory calculations indicate that boron dopants interact strongly with the underlying copper substrate while nitrogen dopants do not. The local bonding differences between graphitic boron and nitrogen dopants lead to large scale differences in dopant distribution. The distribution of dopants is observed to be completely random in the case of boron, while nitrogen displays strong sublattice clustering. Structurally, nitrogen-doped graphene is relatively defect-free while boron-doped graphene films show a large number of Stone-Wales defects. These defects create local electronic resonances and cause electronic scattering, but do not electronically dope the graphene film.

  5. Femtosecond X-ray absorption study of electron localization in photoexcited anatase TiO2

    PubMed Central

    Santomauro, F. G.; Lübcke, A.; Rittmann, J.; Baldini, E.; Ferrer, A.; Silatani, M.; Zimmermann, P.; Grübel, S.; Johnson, J. A.; Mariager, S. O.; Beaud, P.; Grolimund, D.; Borca, C.; Ingold, G.; Johnson, S.L.; Chergui, M.

    2015-01-01

    Transition metal oxides are among the most promising solar materials, whose properties rely on the generation, transport and trapping of charge carriers (electrons and holes). Identifying the latter’s dynamics at room temperature requires tools that combine elemental and structural sensitivity, with the atomic scale resolution of time (femtoseconds, fs). Here, we use fs Ti K-edge X-ray absorption spectroscopy (XAS) upon 3.49 eV (355 nm) excitation of aqueous colloidal anatase titanium dioxide nanoparticles to probe the trapping dynamics of photogenerated electrons. We find that their localization at Titanium atoms occurs in <300 fs, forming Ti3+ centres, in or near the unit cell where the electron is created. We conclude that electron localization is due to its trapping at pentacoordinated sites, mostly present in the surface shell region. The present demonstration of fs hard X-ray absorption capabilities opens the way to a detailed description of the charge carrier dynamics in transition metal oxides. PMID:26437873

  6. Femtosecond X-ray absorption study of electron localization in photoexcited anatase TiO2.

    PubMed

    Santomauro, F G; Lübcke, A; Rittmann, J; Baldini, E; Ferrer, A; Silatani, M; Zimmermann, P; Grübel, S; Johnson, J A; Mariager, S O; Beaud, P; Grolimund, D; Borca, C; Ingold, G; Johnson, S L; Chergui, M

    2015-10-06

    Transition metal oxides are among the most promising solar materials, whose properties rely on the generation, transport and trapping of charge carriers (electrons and holes). Identifying the latter's dynamics at room temperature requires tools that combine elemental and structural sensitivity, with the atomic scale resolution of time (femtoseconds, fs). Here, we use fs Ti K-edge X-ray absorption spectroscopy (XAS) upon 3.49 eV (355 nm) excitation of aqueous colloidal anatase titanium dioxide nanoparticles to probe the trapping dynamics of photogenerated electrons. We find that their localization at Titanium atoms occurs in <300 fs, forming Ti(3+) centres, in or near the unit cell where the electron is created. We conclude that electron localization is due to its trapping at pentacoordinated sites, mostly present in the surface shell region. The present demonstration of fs hard X-ray absorption capabilities opens the way to a detailed description of the charge carrier dynamics in transition metal oxides.

  7. Local Electronic Characterization of Conjugated Polymer Films using Conducting-Probe Atomic Force Microscopy

    NASA Astrophysics Data System (ADS)

    O'Brien, G.; Quinn, A. J.; Redmond, G.

    2004-03-01

    Correlation of local electronic properties with film morphology is a key challenge to be addressed in order to understand (and therefore control) charge injection, transport and recombination in organic electronic devices. We present a flexible method, Conducting-Probe Atomic Force Microscopy (CP-AFM), which can be used as a local probe of both film morphology and spectroscopy. MEH-PPV layers with thickness values comparable to films used in organic electronic devices (60 nm) are spun onto gold substrates under inert conditions. Tip-height vs bias voltage (z-V) sweeps taken at constant tunnel current (50 pA) show clear charge injection thresholds at both positive and negative bias (E_+,E_-). Statistical analysis of measured single-particle gap energies, E_gsp=E_+-E_-, reveals a distribution across the surface with peaks corresponding to (extracted) exciton binding energies of 100 meV and 400 meV respectively. Analysis of measured E_gsp values for films prepared under ambient conditions show a large density of mid-gap states confirming that the preparation route is critical for organic electronic devices.

  8. Localization of fluorescently labeled structures in frozen-hydrated samples using integrated light electron microscopy.

    PubMed

    Faas, F G A; Bárcena, M; Agronskaia, A V; Gerritsen, H C; Moscicka, K B; Diebolder, C A; van Driel, L F; Limpens, R W A L; Bos, E; Ravelli, R B G; Koning, R I; Koster, A J

    2013-03-01

    Correlative light and electron microscopy is an increasingly popular technique to study complex biological systems at various levels of resolution. Fluorescence microscopy can be employed to scan large areas to localize regions of interest which are then analyzed by electron microscopy to obtain morphological and structural information from a selected field of view at nm-scale resolution. Previously, an integrated approach to room temperature correlative microscopy was described. Combined use of light and electron microscopy within one instrument greatly simplifies sample handling, avoids cumbersome experimental overheads, simplifies navigation between the two modalities, and improves the success rate of image correlation. Here, an integrated approach for correlative microscopy under cryogenic conditions is presented. Its advantages over the room temperature approach include safeguarding the native hydrated state of the biological specimen, preservation of the fluorescence signal without risk of quenching due to heavy atom stains, and reduced photo bleaching. The potential of cryo integrated light and electron microscopy is demonstrated for the detection of viable bacteria, the study of in vitro polymerized microtubules, the localization of mitochondria in mouse embryonic fibroblasts, and for a search into virus-induced intracellular membrane modifications within mammalian cells.

  9. Non-Landau damping of magnetic excitations in systems with localized and itinerant electrons.

    PubMed

    Chubukov, Andrey V; Betouras, Joseph J; Efremov, Dmitry V

    2014-01-24

    We discuss the form of the damping of magnetic excitations in a metal near a ferromagnetic instability. The paramagnon theory predicts that the damping term should have the form γ(q,Ω)∝Ω/Γ(q), with Γ(q)∝q (the Landau damping). However, the experiments on uranium metallic compounds UGe2 and UCoGe showed that Γ(q) is essentially independent of q. A nonzero γ(q=0,Ω) is impossible in systems with one type of carrier (either localized or itinerant) because it would violate the spin conservation. It has been conjectured recently that a near-constant Γ(q) in UGe2 and UCoGe may be due to the presence of both localized and itinerant electrons in these materials, with ferromagnetism involving predominantly localized spins. We present the microscopic analysis of the damping of near-critical localized excitations due to interaction with itinerant carriers. We show explicitly how the presence of two types of electrons breaks the cancellation between the contributions to Γ(0) from the self-energy and vertex correction insertions into the spin polarization bubble. We compare our theory with the available experimental data.

  10. Localized reconstruction of subunits from electron cryomicroscopy images of macromolecular complexes

    PubMed Central

    Ilca, Serban L.; Kotecha, Abhay; Sun, Xiaoyu; Poranen, Minna M.; Stuart, David I.; Huiskonen, Juha T.

    2015-01-01

    Electron cryomicroscopy can yield near-atomic resolution structures of highly ordered macromolecular complexes. Often however some subunits bind in a flexible manner, have different symmetry from the rest of the complex, or are present in sub-stoichiometric amounts, limiting the attainable resolution. Here we report a general method for the localized three-dimensional reconstruction of such subunits. After determining the particle orientations, local areas corresponding to the subunits can be extracted and treated as single particles. We demonstrate the method using three examples including a flexible assembly and complexes harbouring subunits with either partial occupancy or mismatched symmetry. Most notably, the method allows accurate fitting of the monomeric RNA-dependent RNA polymerase bound at the threefold axis of symmetry inside a viral capsid, revealing for the first time its exact orientation and interactions with the capsid proteins. Localized reconstruction is expected to provide novel biological insights in a range of challenging biological systems. PMID:26534841

  11. Electron-microscopic cytochemical localization of diamine and polyamine oxidases in pea and maize tissues

    NASA Technical Reports Server (NTRS)

    Slocum, R. D.; Furey MJ, 3. d.

    1991-01-01

    An electron-microscopic cytochemical method was used to localize diamine oxidase (DAO) in pea and polyamine oxidase (PAO) in maize (Zea mays L.). The method, based on the precipitation of amine-oxidase-generated H2O2 by CeCl3, was shown to be specific for DAO and PAO and permitted their localization in plant tissues with a high degree of resolution. Both enzymes are localized exclusively in the cell wall. Both DAO- and PAO-activity staining is most intense in the middle lamellar region of the wall and in cells exhibiting highly lignified walls. The oxidases could provide H2O2 for peroxidase-mediated cross-linking reactions in the cell wall and may, in this capacity, play a role in the regulation of plant growth.

  12. Characteristics of Local Health Departments Associated with Implementation of Electronic Health Records and Other Informatics Systems

    PubMed Central

    Leider, Jonathon P.; Castrucci, Brian C.; Williams, Karmen S.; Luo, Huabin

    2016-01-01

    Objective Assessing local health departments' (LHDs') informatics capacities is important, especially within the context of broader, systems-level health reform. We assessed a nationally representative sample of LHDs' adoption of information systems and the factors associated with adoption and implementation by examining electronic health records, health information exchange, immunization registry, electronic disease reporting system, and electronic laboratory reporting. Methods We used data from the National Association of County and City Health Officials' 2013 National Profile of LHDs. We performed descriptive statistics and multinomial logistic regression for the five implementation-oriented outcome variables of interest, with three levels of implementation (implemented, plan to implement, and no activity). Independent variables included infrastructural and financial capacity and other characteristics associated with informatics capacity. Results Of 505 LHDs that responded to the survey, 69 (13.5%) had implemented health information exchanges, 122 (22.2%) had implemented electronic health records, 245 (47.5%) had implemented electronic laboratory reporting, 368 (73.0%) had implemented an electronic disease reporting system, and 416 (83.8%) had implemented an immunization registry. LHD characteristics associated with health informatics adoption included provision of greater number of clinical services, greater per capita public health expenditures, health information systems specialists on staff, larger population size, decentralized governance system, one or more local boards of health, metropolitan jurisdiction, and top executive with more years in the job. Conclusion Many LHDs lack health informatics capacity, particularly in smaller, rural jurisdictions. Cross-jurisdictional sharing, investment in public health informatics infrastructure, and additional training may help address these shortfalls. PMID:26957662

  13. The roles of 4f- and 5f-orbitals in bonding: A magnetochemical, crystal field, density functional theory, and multi-reference wavefunction study

    SciTech Connect

    Lukens, Wayne W.; Speldrich, Manfred; Yang, Ping; Duignan, T. J.; Autschbach, J.; Kogerler, P.

    2016-05-31

    The electronic structures of 4f3/5f3 Cp"3M and Cp"3M·alkylisocyanide complexes, where Cp" is 1,3-bis-(trimethylsilyl)cyclopentadienyl, are explored with a focus on the splitting of the f-orbitals, which provides information about the strengths of the metal–ligand interactions. While the f-orbital splitting in many lanthanide complexes has been reported in detail, experimental determination of the f-orbital splitting in actinide complexes remains rare in systems other than halide and oxide compounds, since the experimental approach, crystal field analysis, is generally significantly more difficult for actinide complexes than for lanthanide complexes. In this study, a set of analogous neodymium(III) and uranium(III) tris-cyclopentadienyl complexes and their isocyanide adducts was characterized by electron paramagnetic resonance (EPR) spectroscopy and magnetic susceptibility. The crystal field model was parameterized by combined fitting of EPR and susceptibility data, yielding an accurate description of f-orbital splitting. The isocyanide derivatives were also studied using density functional theory, resulting in f-orbital splitting that is consistent with crystal field fitting, and by multi-reference wavefunction calculations that support the electronic structure analysis derived from the crystal-field calculations. The results highlight that the 5f-orbitals, but not the 4f-orbitals, are significantly involved in bonding to the isocyanide ligands. The main interaction between isocyanide ligand and the metal center is a σ-bond, with additional 5f to π* donation for the uranium complexes. As a result, while interaction with the isocyanide π*-orbitals lowers the energies of the 5fxz2 and 5fyz2-orbitals, spin–orbit coupling greatly reduces the population of 5fxz2 and 5fyz2 in the ground state.

  14. Localization of electronic states in finite ladder models: Participation ratio and localization length as measures of the wave-function extension

    NASA Astrophysics Data System (ADS)

    Carrillo-Nuñez, H.; Schulz, Peter A.

    2008-12-01

    In this work we discuss and compare different definitions for localization of electronic states in low-dimensional systems. We choose a heuristic model for DNA-like molecules as a system prototype in order to establish ranges of equivalence for the localization length obtained from both the conductance and participation ratios. The results suggest also criteria to infer the extension of wave function in mesoscopic systems within the diffusive transport regime as complementary information to the localization length.

  15. The effects of local correlations on the electronic structure of FeSe

    NASA Astrophysics Data System (ADS)

    Watson, Matthew; Kim, Timur; Haghighirad, Amir; Coldea, Amalia

    FeSe is structurally the simplest of Fe-based superconductors, but its complex and unique properties pose important theoretical questions. One important aspect of the physics of FeSe is the understanding of the strength and effects of electronic correlations. In order to explore this, we have performed angle-resolved photo-emission spectroscopy (ARPES) measurements on high quality bulk single crystals of FeSe over a wide range of binding energies, in different scattering geometries and with varying incident photon energies, analysing the quasiparticle renormalisations, scattering rates and degree of coherence. We find that FeSe exhibits moderately strong, orbital-dependent correlation effects which are understood to arise primarily due to local electron-electron interactions on the Fe sites. We conclude that electronic correlations constitute a key ingredient in understanding the electronic structure of FeSe. Part of this work was supported by EPSRC, UK (EP/I004475/1, EP/I017836/1). We thank Diamond Light Source for access to Beamline I05.

  16. Simulation of NMR data reveals that proteins' local structures are stabilized by electronic polarization.

    PubMed

    Tong, Yan; Ji, Chang G; Mei, Ye; Zhang, John Z H

    2009-06-24

    Molecular dynamics simulations of NMR backbone relaxation order parameters have been carried out to investigate the polarization effect on the protein's local structure and dynamics for five benchmark proteins (bovine pancreatic trypsin inhibitor, immunoglobulin-binding domain (B1) of streptococcal protein G, bovine apo-calbindin D9K, human interleukin-4 R88Q mutant, and hen egg white lysozyme). In order to isolate the polarization effect from other interaction effects, our study employed both the standard AMBER force field (AMBER03) and polarized protein-specific charges (PPCs) in the MD simulations. The simulated order parameters, employing both the standard nonpolarizable and polarized force fields, are directly compared with experimental data. Our results show that residue-specific order parameters at some specific loop and turn regions are significantly underestimated by the MD simulations using the standard AMBER force field, indicating hyperflexibility of these local structures. Detailed analysis of the structures and dynamic motions of individual residues reveals that the hyperflexibility of these local structures is largely related to the breaking or weakening of relevant hydrogen bonds. In contrast, the agreement with the experimental results is significantly improved and more stable local structures are observed in the MD simulations using the polarized force field. The comparison between theory and experiment provides convincing evidence that intraprotein hydrogen bonds in these regions are stabilized by electronic polarization, which is critical to the dynamical stability of these local structures in proteins.

  17. Electron Localization and Superconductivity in Two-Dimensional Metal Film Systems

    NASA Astrophysics Data System (ADS)

    Burns, Michael Joseph

    The low temperature electrical transport properties of very thin polycrystalline palladium and palladium-gold films grown on glass or fused quartz, and also the properties of epitaxially grown silver films on germanium (001), have been investigated. These, and other two dimensional electronic systems, display a nonmetallic conductivity which has been attributed to electron localization and/or electron-electron interaction effects. According to the various theories, some of the transport properties should display different behaviors, thus allowing one to distinguish between the two effects. Measurements of Pd and Pd-Au film resistivities as a function of temperature, electric and magnetic field, plus the thermopower, were performed on films ranging from 18 to 30 Angstroms in thickness, having resistivities from 600 to 500000 ohms/square at 10(DEGREES)K. The magnetotransport properties imply the presence of strong spin-orbit coupling, although the temperature dependence of the resistivity of these films does not. All 'metallic' samples (resistivities less than 30000 ohms/square) have a material specific thermopower which tends to zero as the temperature goes to zero. Samples whose resistivities increase above 30000 ohms/square have thermopowers which diverge as the temperature approaches zero. Thus the density of states for the electronic transport is zero at the Fermi energy (i.e. an energy gap opens in the density of states at 30000 ohms/square) for high -resistivity films. The very thin (2.5 monolayer) silver films epitaxially grown on Ge (001) consist of a monolayer coverage plus isolated three dimensional islands. Below 70(DEGREES)K the conductivity is dominated by the metal film and displays the temperature and electric and magnetic field dependencies characteristic of metallic weak localization in two dimensions. Below about 2(DEGREES)K, the resistance drops rapidly in a manner resembling an incomplete superconducting transition. The resistance is restored by

  18. Photo-electron momentum distribution and electron localization studies from laser-induced atomic and molecular dissociations

    NASA Astrophysics Data System (ADS)

    Ray, Dipanwita

    The broad objective of ultrafast strong-field studies is to be able to measure and control atomic and molecular dynamics on a femtosecond timescale. This thesis work has two major themes: (1) Study of high-energy photoelectron distributions from atomic targets. (2) Electron localization control in atomic and molecular reactions using shaped laser pulses. The first section focuses on the study of photoelectron diffraction patterns of simple atomic targets to understand the target structure. We measure the full vector momentum spectra of high energy photoelectrons from atomic targets (Xe, Ar and Kr) generated by intense laser pulses. The target dependence of the angular distribution of the highest energy photoelectrons as predicted by Quantitative Rescattering Theory (QRS) is explored. More recent developments show target structure information can be retrieved from photoelectrons over a range of energies, from 4Up up to 10Up, independent of the peak intensity at which the photoelectron spectra have been measured. Controlling the fragmentation pathways by manipulating the pulse shape is another major theme of ultrafast science today. In the second section we study the asymmetry of electron (and ion) emission from atoms (and molecules) by interaction with asymmetric pulses formed by the superposition of two colors (800 & 400 nm). Xe electron momentum spectra obtained as a function of the two-color phase exhibit a pronounced asymmetry. Using QRS theory we can analyze this asymmetric yield of the high energy photoelectrons to determine accurately the laser peak intensity and the absolute phase of the two-color electric field. This can be used as a standard pulse calibration method for all two-color studies. Experiments showing strong left-right asymmetry in D+ ion yield from D2 molecules using two-color pulses is also investigated. The asymmetry effect is found to be very ion-energy dependent.

  19. Theory of electronic polarization and localization in insulators with applications to solid hydrogen

    NASA Astrophysics Data System (ADS)

    Souza, Ivo Nuno Saldanha Do Rosario E.

    A theory is formulated, and practical expressions are derived, for the full quantum-mechanical distribution of the intrinsic macroscopic polarization of an insulator in terms of the ground state wave function. The formalism applies to an insulating system of N electrons obeying twisted boundary conditions over a finite volume. The central quantity is a cumulant generating function which yields, upon successive differentiation, all the cumulants and moments of the probability distribution of an appropriately defined center of mass X/N of the electrons ( X=SN i=1xi ). The first moment is the average polarization, where we recover the well-known Berry phase expression. The second cumulant gives the mean-square fluctuation of the polarization, which defines an electronic localization length squared x2m along each direction m:x2m= X2m -Xm 2/N . It can be expressed in terms of a metric, which measures the infinitesimal distance between quantum states in a Hilbert space parametrized by the twisted boundary conditions. The fluctuation-dissipation relation is used to show that in the thermodynamic limit x2m diverges when the system becomes metallic and is a finite, measurable quantity in the insulating state, related to the optical gap by x2m≤ℎ2 /2meEg . In noninteracting systems x2m is related to the spread of the Wannier functions, and this picture is generalized to correlated insulators by defining the many-body analog of Wannier functions. In the limit of large N the maximally-localized many-body Wannier functions become localized in disconnected regions of the high-dimensional configuration space of the N electrons, establishing a direct connection with Kohn's theory of the insulating state. By recasting the generating function in terms of these functions, it is shown that macroscopic polarization results from the localized character of an insulating wave function in configuration space. The Berry phase theory is used to compute the Born effective charges in

  20. Anderson localization of electrons in single crystals: LixFe7Se8

    PubMed Central

    Ying, Tianping; Gu, Yueqiang; Chen, Xiao; Wang, Xinbo; Jin, Shifeng; Zhao, Linlin; Zhang, Wei; Chen, Xiaolong

    2016-01-01

    Anderson (disorder-induced) localization, proposed more than half a century ago, has inspired numerous efforts to explore the absence of wave diffusions in disordered media. However, the proposed disorder-induced metal-insulator transition (MIT), associated with the nonpropagative electron waves, has hardly been observed in three-dimensional (3D) crystalline materials, let alone single crystals. We report the observation of an MIT in centimeter-size single crystals of LixFe7Se8 induced by lattice disorder. Both specific heat and infrared reflectance measurements reveal the presence of considerable electronic states in the vicinity of the Fermi level when the MIT occurs, suggesting that the transition is not due to Coulomb repulsion mechanism. The 3D variable range hopping regime evidenced by electrical transport measurements at low temperatures indicates the localized nature of the electronic states on the Fermi level. Quantitative analyses of carrier concentration, carrier mobility, and simulated density of states (DOS) fully support that LixFe7Se8 is an Anderson insulator. On the basis of these results, we provide a unified DOS picture to explain all the experimental results, and a schematic diagram for finding other potential Anderson insulators. This material will thus serve as a rich playground for both theoretical and experimental investigations on MITs and disorder-induced phenomena. PMID:26989781

  1. Nucleophilic Aromatic Substitution Reactions Described by the Local Electron Attachment Energy.

    PubMed

    Stenlid, Joakim H; Brinck, Tore

    2017-03-17

    A local multiorbital electrophilicity descriptor, the local electron attachment energy [E(r)], is used to study the nucleophilic aromatic substitution reactions of SNAr and VNS (vicarious nucleophilic substitution). E(r) considers all virtual orbitals below the free electron limit and is determined on the molecular isodensity contour of 0.004 atomic units. Good (R(2) = 0.83) to excellent (R(2) = 0.98) correlations are found between descriptor values and experimental reactivity data for six series of electron deficient arenes. These include homo- and heteroarenes, rings of five to six atoms, and a variety of fluorine, bromine, and hydride leaving groups. The solvent, temperature, and nucleophile are in addition varied across the series. The surface E(r) [ES(r)] is shown to provide reactivity predictions better than those of transition-state calculations for a concerted SNAr reaction with a bromine nucleofug, gives correlations substantially stronger than those of LUMO energies, and is overall more reliable than the molecular electrostatic potential. With the use of ES(r), one can identify the various electrophilic sites within a molecule and correctly predict isomeric distributions. Since the calculations of ES(r) are computationally inexpensive, the descriptor offers fast but accurate reactivity predictions for the important nucleophilic aromatic substitution class of reactions. Applications in, e.g., drug discovery, synthesis, and toxicology studies are envisaged.

  2. Correlative infrared-electron nanoscopy reveals the local structure-conductivity relationship in zinc oxide nanowires

    NASA Astrophysics Data System (ADS)

    Stiegler, J. M.; Tena-Zaera, R.; Idigoras, O.; Chuvilin, A.; Hillenbrand, R.

    2012-10-01

    High-resolution characterization methods play a key role in the development, analysis and optimization of nanoscale materials and devices. Because of the various material properties, only a combination of different characterization techniques provides a comprehensive understanding of complex functional materials. Here we introduce correlative infrared-electron nanoscopy, a novel method yielding transmission electron microscope and infrared near-field images of one and the same nanostructure. While transmission electron microscopy provides structural information up to the atomic level, infrared near-field imaging yields nanoscale maps of chemical composition and conductivity. We demonstrate the method's potential by studying the relation between conductivity and crystal structure in ZnO nanowire cross-sections. The combination of infrared conductivity maps and the local crystal structure reveals a radial free-carrier gradient, which inversely correlates to the density of extended crystalline defects. Our method opens new avenues for studying the local interplay between structure, conductivity and chemical composition in widely different material systems.

  3. Immuno- and correlative light microscopy-electron tomography methods for 3D protein localization in yeast.

    PubMed

    Mari, Muriel; Geerts, Willie J C; Reggiori, Fulvio

    2014-10-01

    Compartmentalization of eukaryotic cells is created and maintained through membrane rearrangements that include membrane transport and organelle biogenesis. Three-dimensional reconstructions with nanoscale resolution in combination with protein localization are essential for an accurate molecular dissection of these processes. The yeast Saccharomyces cerevisiae is a key model system for identifying genes and characterizing pathways essential for the organization of cellular ultrastructures. Electron microscopy studies of yeast, however, have been hampered by the presence of a cell wall that obstructs penetration of resins and cryoprotectants, and by the protein dense cytoplasm, which obscures the membrane details. Here we present an immuno-electron tomography (IET) method, which allows the determination of protein distribution patterns on reconstructed organelles from yeast. In addition, we extend this IET approach into a correlative light microscopy-electron tomography procedure where structures positive for a specific protein localized through a fluorescent signal are resolved in 3D. These new investigative tools for yeast will help to advance our understanding of the endomembrane system organization in eukaryotic cells.

  4. Electron localization in ultrathin films of three-dimensional topological insulators

    NASA Astrophysics Data System (ADS)

    Liao, Jian; Shi, Gang; Liu, Nan; Li, Yongqing

    2016-11-01

    The recent discovery of three-dimensional (3D) topological insulators (TIs) has provided a fertile ground for obtaining further insights into electron localization in condensed matter systems. In the past few years, a tremendous amount of research effort has been devoted to investigate electron transport properties of 3D TIs and their low dimensional structures in a wide range of disorder strength, covering transport regimes from weak antilocalization to strong localization. The knowledge gained from these studies not only offers sensitive means to probe the surface states of 3D TIs but also forms a basis for exploring novel topological phases. In this article, we briefly review the main experimental progress in the study of the localization in 3D TIs, with a focus on the latest results on ultrathin TI films. Some new transport data will also be presented in order to complement those reported previously in the literature. Project supported by the National Basic Research Program of China (Grant Nos. 2012CB921703 and 2015CB921102), the National Natural Science Foundation of China (Grant Nos. 61425015, 11374337, and 91121003), and the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No. XDB070202).

  5. Local Electron Attachment Energy and Its Use for Predicting Nucleophilic Reactions and Halogen Bonding.

    PubMed

    Brinck, Tore; Carlqvist, Peter; Stenlid, Joakim H

    2016-12-22

    A new local property, the local electron attachment energy [E(r)], is introduced and is demonstrated to be a useful guide to predict intermolecular interactions and chemical reactivity. The E(r) is analogous to the average local ionization energy but indicates susceptibility toward interactions with nucleophiles rather than electrophiles. The functional form E(r) is motivated based on Janak's theorem and the piecewise linear energy dependence of electron addition to atomic and molecular systems. Within the generalized Kohn-Sham method (GKS-DFT), only the virtual orbitals with negative eigenvalues contribute to E(r). In the present study, E(r) has been computed from orbitals obtained from GKS-DFT computations with a hybrid exchange-correlation functional. It is shown that E(r) computed on a molecular isodensity surface, ES(r), reflects the regioselectivity and relative reactivity for nucleophilic aromatic substitution, nucleophilic addition to activated double bonds, and formation of halogen bonds. Good to excellent correlations between experimental or theoretical measures of interaction strengths and minima in ES(r) (ES,min) are demonstrated.

  6. Local imaging of high mobility two-dimensional electron systems with virtual scanning tunneling microscopy

    SciTech Connect

    Pelliccione, M.; Bartel, J.; Goldhaber-Gordon, D.; Sciambi, A.; Pfeiffer, L. N.; West, K. W.

    2014-11-03

    Correlated electron states in high mobility two-dimensional electron systems (2DESs), including charge density waves and microemulsion phases intermediate between a Fermi liquid and Wigner crystal, are predicted to exhibit complex local charge order. Existing experimental studies, however, have mainly probed these systems at micron to millimeter scales rather than directly mapping spatial organization. Scanning probes should be well-suited to study the spatial structure of these states, but high mobility 2DESs are found at buried semiconductor interfaces, beyond the reach of conventional scanning tunneling microscopy. Scanning techniques based on electrostatic coupling to the 2DES deliver important insights, but generally with resolution limited by the depth of the 2DES. In this letter, we present our progress in developing a technique called “virtual scanning tunneling microscopy” that allows local tunneling into a high mobility 2DES. Using a specially designed bilayer GaAs/AlGaAs heterostructure where the tunnel coupling between two separate 2DESs is tunable via electrostatic gating, combined with a scanning gate, we show that the local tunneling can be controlled with sub-250 nm resolution.

  7. Sac2/INPP5F is an inositol 4-phosphatase that functions in the endocytic pathway.

    PubMed

    Nakatsu, Fubito; Messa, Mirko; Nández, Ramiro; Czapla, Heather; Zou, Yixiao; Strittmatter, Stephen M; De Camilli, Pietro

    2015-04-13

    The recruitment of inositol phosphatases to endocytic membranes mediates dephosphorylation of PI(4,5)P2, a phosphoinositide concentrated in the plasma membrane, and prevents its accumulation on endosomes. The importance of the conversion of PI(4,5)P2 to PtdIns during endocytosis is demonstrated by the presence of both a 5-phosphatase and a 4-phosphatase (Sac domain) module in the synaptojanins, endocytic PI(4,5)P2 phosphatases conserved from yeast to humans and the only PI(4,5)P2 phosphatases in yeast. OCRL, another 5-phosphatase that couples endocytosis to PI(4,5)P2 dephosphorylation, lacks a Sac domain. Here we show that Sac2/INPP5F is a PI4P phosphatase that colocalizes with OCRL on endocytic membranes, including vesicles formed by clathrin-mediated endocytosis, macropinosomes, and Rab5 endosomes. An OCRL-Sac2/INPP5F interaction could be demonstrated by coimmunoprecipitation and was potentiated by Rab5, whose activity is required to recruit Sac2/INPP5F to endosomes. Sac2/INPP5F and OCRL may cooperate in the sequential dephosphorylation of PI(4,5)P2 at the 5 and 4 position of inositol in a partnership that mimics that of the two phosphatase modules of synaptojanin.

  8. 48 CFR 47.303-5 - F.o.b. origin, with differentials.

    Code of Federal Regulations, 2010 CFR

    2010-10-01

    ... 48 Federal Acquisition Regulations System 1 2010-10-01 2010-10-01 false F.o.b. origin, with... CONTRACT MANAGEMENT TRANSPORTATION Transportation in Supply Contracts 47.303-5 F.o.b. origin, with differentials. (a) Explanation of delivery term. F.o.b. origin, with differentials means— (1) Free of expense...

  9. 48 CFR 47.303-5 - F.o.b. origin, with differentials.

    Code of Federal Regulations, 2011 CFR

    2011-10-01

    ... 48 Federal Acquisition Regulations System 1 2011-10-01 2011-10-01 false F.o.b. origin, with... CONTRACT MANAGEMENT TRANSPORTATION Transportation in Supply Contracts 47.303-5 F.o.b. origin, with differentials. (a) Explanation of delivery term. F.o.b. origin, with differentials means— (1) Free of expense...

  10. 26 CFR 5f.103-2 - Public approval of industrial development bonds.

    Code of Federal Regulations, 2011 CFR

    2011-04-01

    ... 26 Internal Revenue 14 2011-04-01 2010-04-01 true Public approval of industrial development bonds... RESPONSIBILITY ACT OF 1982 § 5f.103-2 Public approval of industrial development bonds. (a) General rule. An industrial development bond (within the meaning of § 1.103-7(b)(1) issued after December 31, 1982, shall...

  11. 26 CFR 5f.103-2 - Public approval of industrial development bonds.

    Code of Federal Regulations, 2010 CFR

    2010-04-01

    ... 26 Internal Revenue 14 2010-04-01 2010-04-01 false Public approval of industrial development bonds... RESPONSIBILITY ACT OF 1982 § 5f.103-2 Public approval of industrial development bonds. (a) General rule. An industrial development bond (within the meaning of § 1.103-7(b)(1) issued after December 31, 1982, shall...

  12. Ab initio electronic structure, magnetism, and magnetocrystalline anisotropy of UGa2

    NASA Astrophysics Data System (ADS)

    Diviš, Martin; Richter, Manuel; Eschrig, Helmut; Steinbeck, Lutz

    1996-04-01

    Ab initio electronic structure calculations for the intermetallic compound UGa2 were performed using an optimized linear combination of atomic orbitals method based on the local spin density approximation. Three separate calculations were done treating the uranium 5f states as band states and as localized states with occupation two and three, respectively. In the itinerant approach, spin and orbital moments, magnetocrystalline anisotropy, and the Sommerfeld constant were calculated and found to deviate significantly from the related experimental data. In the localized approach, crystal field parameters were obtained for the 5f states, which have been treated by self-interaction corrected local-density theory. This approach with 5f2 occupation is shown to provide reasonable results for the anisotropy of the susceptibility, for the field dependence of the magnetic moments, and for the Sommerfeld constant.

  13. The effects of local chemistry on the growth and electronic properties of carbon nanotubes

    NASA Astrophysics Data System (ADS)

    Simmons, Jason M.

    Though carbon nanotubes have been actively studied for fifteen years, their interaction with their local environment is still an active area of research. Since every atom in a single-walled nanotube is a surface atom, changes in the local chemistry can have large effects on nanotube properties. This feature has been exploited in a number of attempts at using nanotubes for various sensor applications, but it is important for every application, from transistors to composites. Nanotubes will always feel their environment; and environmental effects must be understood in order to control them. In the course of this thesis research, I have investigated local chemical effects on the growth and properties of single-walled carbon nanotubes. During the catalytic growth of carbon nanotubes, the transition metal catalyst must remain active. Interactions with the substrate, particularly silicon, can lead to non-catalytic compounds that prevent nanotube growth. By controlling the thickness of the silicon dioxide diffusion barrier, high yield nanotube growth from iron catalysts can be achieved on ultra-thin (>4 nm) oxides. Once the nanotube is placed into an electronic device, local chemistry can again affect the nanotube properties. Using ozone oxidation as a model for covalent functionalization, I show that the disruption of the conjugated pi band in the nanotube lattice leads to drastic reductions in the conductivity. Though there are a large number of other potential causes for the conductivity reduction; the use of several experimental techniques, from electrical transport to optical and electron spectroscopies, enables each of them to be excluded as the dominant processes. The conductivity in a nanotube transistor can also be controlled by the local chemistry. This is demonstrated by functionalizing nanotube transistors with an organic chromophore. Photoisomerization of the chromophore changes the molecular dipole moments and causes a change in the local electrostatic

  14. Sawtooth stabilization by localized electron cyclotron heating in a tokamak plasma

    SciTech Connect

    Hanada, K.; Tanaka, H.; Iida, M.; Minami, T.; Maekawa, T.; Terumichi, Y.; Tanaka, S. . Dept. of Physics); Ide, S. . Naka Fusion Research Establishment); Nakamura, M. ); Yamada, M.; Manickam, J.; White, R.B. . Plasma Physics Lab.)

    1990-11-01

    Sawtooth oscillations (STO) in the ohmically heated WT-3 tokamak are strongly modified or suppressed by localized electron cyclotron resonance heating (ECH) near the q = 1 surface, where q refers to the safety factor. The effect of ECH is much stronger when it is applied on the high field side (the inner side of the tokamak) as compared to the low field side (outer side). Complete suppression of the STO is achieved for the duration of the ECH when it is applied on the high field side, in a low density plasma, provided the ECH power exceeds a thresholds value. The STO stabilization is attributed to a modification of the current density profile by hot electrons generated by ECH, which reduces the shear in the q = region. 14 refs., 5 figs.

  15. Spin coherence and dephasing of localized electrons in monolayer MoS2

    SciTech Connect

    Yang, Luyi; Chen, Weibing; McCreary, Kathleen M.; Jonker, Berend T.; Lou, Jun; Crooker, Scott A.

    2015-11-10

    Here, we report a systematic study of coherent spin precession and spin dephasing in electron-doped monolayer MoS2. Using time-resolved Kerr rotation spectroscopy and applied in-plane magnetic fields, a nanosecond time scale Larmor spin precession signal commensurate with g-factor |g0| ≃ 1.86 is observed in several different MoS2 samples grown by chemical vapor deposition. The dephasing rate of this oscillatory signal increases linearly with magnetic field, suggesting that the coherence arises from a subensemble of localized electron spins having an inhomogeneously broadened distribution of g-factors, g0 + Δg. In contrast to g0, Δg is sample-dependent and ranges from 0.042 to 0.115.

  16. Spin coherence and dephasing of localized electrons in monolayer MoS2

    DOE PAGES

    Yang, Luyi; Chen, Weibing; McCreary, Kathleen M.; ...

    2015-11-10

    Here, we report a systematic study of coherent spin precession and spin dephasing in electron-doped monolayer MoS2. Using time-resolved Kerr rotation spectroscopy and applied in-plane magnetic fields, a nanosecond time scale Larmor spin precession signal commensurate with g-factor |g0| ≃ 1.86 is observed in several different MoS2 samples grown by chemical vapor deposition. The dephasing rate of this oscillatory signal increases linearly with magnetic field, suggesting that the coherence arises from a subensemble of localized electron spins having an inhomogeneously broadened distribution of g-factors, g0 + Δg. In contrast to g0, Δg is sample-dependent and ranges from 0.042 to 0.115.

  17. Local crystal structure analysis with 10-pm accuracy using scanning transmission electron microscopy.

    PubMed

    Saito, Mitsuhiro; Kimoto, Koji; Nagai, Takuro; Fukushima, Shun; Akahoshi, Daisuke; Kuwahara, Hideki; Matsui, Yoshio; Ishizuka, Kazuo

    2009-06-01

    We demonstrate local crystal structure analysis based on annular dark-field (ADF) imaging in scanning transmission electron microscopy (STEM). Using a stabilized STEM instrument and customized software, we first realize high accuracy of elemental discrimination and atom-position determination with a 10-pm-order accuracy, which can reveal major cation displacements associated with a variety of material properties, e.g. ferroelectricity and colossal magnetoresistivity. A-site ordered/disordered perovskite manganites Tb(0.5)Ba(0.5)MnO(3) are analysed; A-site ordering and a Mn-site displacement of 12 pm are detected in each specific atomic column. This method can be applied to practical and advanced materials, e.g. strongly correlated electron materials.

  18. Fluctuating local moments, itinerant electrons, and the magnetocaloric effect: Compositional hypersensitivity of FeRh

    NASA Astrophysics Data System (ADS)

    Staunton, J. B.; Banerjee, R.; Dias, M. dos Santos; Deak, A.; Szunyogh, L.

    2014-02-01

    We describe an ab initio disordered local moment theory for materials with quenched static compositional disorder traversing first-order magnetic phase transitions. It accounts quantitatively for metamagnetic changes and the magnetocaloric effect. For perfect stoichiometric B2-ordered FeRh, we calculate the transition temperature of the ferromagnetic-antiferromagnetic transition to be Tt= 495 K and a maximum isothermal entropy change in 2 T of |ΔS|=21.1 J K-1 kg-1. A large (40%) component of |ΔS| is electronic. The transition results from a fine balance of competing electronic effects which is disturbed by small compositional changes; e.g., swapping just 2% Fe of "defects" onto the Rh sublattice makes Tt drop by 290 K. This hypersensitivity explains the narrow compositional range of the transition and impurity doping effects.

  19. Calculation of smooth potential energy surfaces using local electron correlation methods

    NASA Astrophysics Data System (ADS)

    Mata, Ricardo A.; Werner, Hans-Joachim

    2006-11-01

    The geometry dependence of excitation domains in local correlation methods can lead to noncontinuous potential energy surfaces. We propose a simple domain merging procedure which eliminates this problem in many situations. The method is applied to heterolytic bond dissociations of ketene and propadienone, to SN2 reactions of Cl- with alkylchlorides, and in a quantum mechanical/molecular mechanical study of the chorismate mutase enzyme. It is demonstrated that smooth potentials are obtained in all cases. Furthermore, basis set superposition error effects are reduced in local calculations, and it is found that this leads to better basis set convergence when computing barrier heights or weak interactions. When the electronic structure strongly changes between reactants or products and the transition state, the domain merging procedure leads to a balanced description of all structures and accurate barrier heights.

  20. Calculation of smooth potential energy surfaces using local electron correlation methods

    SciTech Connect

    Mata, Ricardo A.; Werner, Hans-Joachim

    2006-11-14

    The geometry dependence of excitation domains in local correlation methods can lead to noncontinuous potential energy surfaces. We propose a simple domain merging procedure which eliminates this problem in many situations. The method is applied to heterolytic bond dissociations of ketene and propadienone, to SN2 reactions of Cl{sup -} with alkylchlorides, and in a quantum mechanical/molecular mechanical study of the chorismate mutase enzyme. It is demonstrated that smooth potentials are obtained in all cases. Furthermore, basis set superposition error effects are reduced in local calculations, and it is found that this leads to better basis set convergence when computing barrier heights or weak interactions. When the electronic structure strongly changes between reactants or products and the transition state, the domain merging procedure leads to a balanced description of all structures and accurate barrier heights.

  1. Localized bulk electron heating with ICRF mode conversion in the JET tokamak

    NASA Astrophysics Data System (ADS)

    Mantsinen, M. J.; Mayoral, M.-L.; Van Eester, D.; Alper, B.; Barnsley, R.; Beaumont, P.; Bucalossi, J.; Coffey, I.; Conroy, S.; de Baar, M.; de Vries, P.; Erents, K.; Figueiredo, A.; Gondhalekar, A.; Gowers, C.; Hellsten, T.; Joffrin, E.; Kiptily, V.; Lamalle, P. U.; Lawson, K.; Lyssoivan, A.; Mailloux, J.; Mantica, P.; Meo, F.; Milani, F.; Monakhov, I.; Murari, A.; Nguyen, F.; Noterdaeme, J.-M.; Ongena, J.; Petrov, Yu.; Rachlew, E.; Riccardo, V.; Righi, E.; Rimini, F.; Stamp, M.; Tuccillo, A. A.; Zastrow, K.-D.; Zerbini, M.; EFDA contributors, JET

    2004-01-01

    Ion cyclotron resonance frequencies (ICRF) mode conversion has been developed for localized on-axis and off-axis bulk electron heating on the JET tokamak. The fast magnetosonic waves launched from the low-field side ICRF antennas are mode-converted to short-wavelength waves on the high-field side of the 3He ion cyclotron resonance layer in D and 4He plasmas and subsequently damped on the bulk electrons. The resulting electron power deposition, measured using ICRF power modulation, is narrow with a typical full-width at half-maximum of ap30 cm (i.e. about 30% of the minor radius) and the total deposited power to electrons comprises at least up to 80% of the applied ICRF power. The ICRF mode conversion power deposition has been kept constant using 3He bleed throughout the ICRF phase with a typical duration of 4-6 s, i.e. 15-40 energy confinement times. Using waves propagating in the counter-current direction minimizes competing ion damping in the presence of co-injected deuterium beam ions.

  2. Analysis of local strain in aluminum interconnects by convergent beam electron diffraction

    NASA Astrophysics Data System (ADS)

    Krämer, Stephan; Mayer, Joachim

    1999-11-01

    Energy filtered convergent beam electron diffraction (CBED) was used to investigate localized strain in aluminum interconnects. An analysis of the higher order Laue zone (HOLZ) line positions in CBED patterns makes it possible to measure the lattice strain with high accuracy (˜104) and high spatial resolution (10 to 100 nm). The strain development in a single grain was measured during thermal cycling between -170 °C and +100 °C. The grain showed reversible, elastic behavior over the whole temperature range building up large strains at low temperatures. By comparing with finite element simulations, a detailed understanding of the tri-axial strain state could be achieved.

  3. Local electronic effects and irradiation resistance in high-entropy alloys

    DOE PAGES

    Egami, Takeshi; Stocks, George Malcolm; Nicholson, Don; ...

    2015-01-01

    High-entropy alloys are multicomponent solid solutions in which various elements with different chemistries and sizes occupy the same crystallographic lattice sites. Thus, none of the atoms perfectly fit the lattice site, giving rise to considerable local lattice distortions and atomic-level stresses. These characteristics can be beneficial for performance under both radiation and in a high-temperature environment, making them attractive candidates as nuclear materials. We discuss electronic origin of the atomic-level stresses based upon first-principles calculations using a density functional theory approach.

  4. Inelastic electron tunneling spectroscopy of local “spin accumulation” devices

    SciTech Connect

    Tinkey, Holly N.; Li, Pengke; Appelbaum, Ian

    2014-06-09

    We investigate the origin of purported “spin accumulation” signals observed in local “three-terminal” (3T) measurements of ferromagnet/insulator/n-Si tunnel junctions using inelastic electron tunneling spectroscopy (IETS). Voltage bias and magnetic field dependences of the IET spectra were found to account for the dominant contribution to 3T magnetoresistance, thus indicating that it arises from inelastic tunneling through impurities and defects at junction interfaces and within the barrier, rather than from spin accumulation due to pure elastic tunneling into bulk Si as has been previously assumed.

  5. Improved non-local electron thermal transport model for two-dimensional radiation hydrodynamics simulations

    SciTech Connect

    Cao, Duc; Moses, Gregory; Delettrez, Jacques

    2015-08-15

    An implicit, non-local thermal conduction algorithm based on the algorithm developed by Schurtz, Nicolai, and Busquet (SNB) [Schurtz et al., Phys. Plasmas 7, 4238 (2000)] for non-local electron transport is presented and has been implemented in the radiation-hydrodynamics code DRACO. To study the model's effect on DRACO's predictive capability, simulations of shot 60 303 from OMEGA are completed using the iSNB model, and the computed shock speed vs. time is compared to experiment. Temperature outputs from the iSNB model are compared with the non-local transport model of Goncharov et al. [Phys. Plasmas 13, 012702 (2006)]. Effects on adiabat are also examined in a polar drive surrogate simulation. Results show that the iSNB model is not only capable of flux-limitation but also preheat prediction while remaining numerically robust and sacrificing little computational speed. Additionally, the results provide strong incentive to further modify key parameters within the SNB theory, namely, the newly introduced non-local mean free path. This research was supported by the Laboratory for Laser Energetics of the University of Rochester.

  6. TiO2 nanotube arrays for photocatalysis: Effects of crystallinity, local order, and electronic structure

    DOE PAGES

    Liu, Jing; Hosseinpour, Pegah M.; Luo, Si; ...

    2014-11-19

    To furnish insight into correlations of electronic and local structure and photoactivity, arrays of short and long TiO₂ nanotubes were synthesized by electrochemical anodization of Ti foil, followed by thermal treatment in O₂ (oxidizing), Ar (inert), and H₂ (reducing) environments. The physical and electronic structures of these nanotubes were probed with x-ray diffraction, scanning electron microscopy, and synchrotron-based x-ray absorption spectroscopy, and correlated with their photocatalytic properties. The photocatalytic activity of the nanotubes was evaluated by monitoring the degradation of methyl orange under UV-VIS light irradiation. Results show that upon annealing at 350 °C all as-anodized amorphous TiO₂ nanotube samplesmore » partially transform to the anatase structure, with variations in the degree of crystallinity and in the concentration of local defects near the nanotubes' surface (~5 nm) depending on the annealing conditions. Degradation of methyl orange was not detectable for the as-anodized TiO₂ nanotubes regardless of their length. The annealed long nanotubes demonstrated detectable catalytic activity, which was more significant with the H₂-annealed nanotubes than with the Ar- and O₂-annealed nanotube samples. This enhanced photocatalytic response of the H₂-annealed long nanotubes relative to the other samples is positively correlated with the presence of a larger concentration of lattice defects (such as Ti3+ and anticipated oxygen vacancies) and a slightly lower degree of crystallinity near the nanotube surface. These physical and electronic structural attributes impact the efficacy of visible light absorption; moreover, the increased concentration of surface defects is postulated to promote the generation of hydroxyl radicals and thus accelerate the photodegradation of the methyl orange. The information obtained from this study provides unique insight into the role of the near-surface electronic and defect structure

  7. Probing the band structure and local electronic properties of low-dimensional semiconductor structures

    NASA Astrophysics Data System (ADS)

    Walrath, Jenna Cherie

    Low-dimensional semiconductor structures are important for a wide variety of applications, and recent advances in nanoscale fabrication are paving the way for increasingly precise nano-engineering of a wide range of materials. It is therefore essential that the physics of materials at the nanoscale are thoroughly understood to unleash the full potential of nanotechnology, requiring the development of increasingly sophisticated instrumentation and modeling. Of particular interest is the relationship between the local density of states (LDOS) of low-dimensional structures and the band structure and local electronic properties. This dissertation presents the investigation of the band structure, LDOS, and local electronic properties of nanostructures ranging from zero-dimensional (0D) quantum dots (QDs) to two-dimensional (2D) thin films, synthesizing computational and experimental approaches including Poisson-Schrodinger band structure calculations, scanning tunneling microscopy (STM), scanning tunneling spectroscopy (STS), and scanning thermoelectric microscopy (SThEM). A method is presented for quantifying the local Seebeck coefficient (S) with SThEM, using a quasi-3D conversion matrix approach to directly convert temperature gradient-induced voltages S. For a GaAs p-n junction, the resulting S-profile is consistent with that computed using the free carrier concentration profile. This combined computational-experimental approach is expected to enable nanoscale measurements of S across a wide variety of heterostructure interfaces. The local carrier concentration, n, is profiled across epitaxial InAs/GaAs QDs, where SThEM is used to profile the temperature gradient-induced voltage, which is converted to a profile of the local S and finally to an n profile. The S profile is converted to a conduction band-edge profile and compared with Poisson-Schrodinger band-edge simulations. The combined computational-experimental approach suggests a reduced n in the QD center in

  8. Local ionospheric electron density reconstruction from simultaneous ground-based GNSS and ionosonde measurements

    NASA Astrophysics Data System (ADS)

    Stankov, S. M.; Warnant, R.; Stegen, K.

    2009-04-01

    The purpose of the LIEDR (Local Ionospheric Electron Density Reconstruction) system is to acquire and process data from simultaneous ground-based GNSS TEC and digital ionosonde measurements, and subsequently to deduce the vertical electron density distribution in the local ionosphere. LIEDR is primarily designed to operate in real time for service applications, and, if sufficient data from solar and geomagnetic observations are available, to provide short-term forecast as well. For research applications and further development of the system, a post-processing mode of operation is also envisaged. In essence, the reconstruction procedure consists in the following. The high-precision ionosonde measurements are used for directly obtaining the bottom part of the electron density profile. The ionospheric profiler for the lower side (i.e. below the density peak height, hmF2) is based on the Epstein layer functions using the known values of the critical frequencies, foF2 and foE, and the propagation factor, M3000F2. The corresponding bottom-side part of the total electron content is calculated from this profile and is then subtracted from the GPS TEC value in order to obtain the unknown portion of the TEC in the upper side (i.e. above the hmF2). Ionosonde data, together with the simultaneously-measured TEC and empirically obtained O+/H+ ion transition level values, are all required for the determination of the topside electron density scale height. The topside electron density is considered as a sum of the constituent oxygen and hydrogen ion densities with unknown vertical scale heights. The latter are calculated by solving a system of transcendental equations that arise from the incorporation of a suitable ionospheric profiler (Chapman, Epstein, or Exponential) into formulae describing ionospheric conditions (plasma quasi-neutrality, ion transition level). Once the topside scale heights are determined, the construction of the vertical electron density distribution in the

  9. Local electron heating in the Io plasma torus associated with Io from HISAKI satellite observation

    NASA Astrophysics Data System (ADS)

    Tsuchiya, Fuminori; Kagitani, Masato; Yoshioka, Kazuo; Kimura, Tomoki; Murakami, Go; Yamazaki, Atsushi; Nozawa, Hiromasa; Kasaba, Yasumasa; Sakanoi, Takeshi; Uemizu, Kazunori; Yoshikawa, Ichiro

    2015-12-01

    Io-correlated brightness change in the Io plasma torus (IPT) was discovered by the Voyager spacecraft, showing evidence of local electron heating around Io. However, its detailed properties and the cause of electron heating are still open issues. The extreme ultraviolet spectrograph on board the HISAKI satellite continuously observed the IPT from the end of December 2013 to the middle of January 2014. The variation in the IPT brightness showed that clear periodicity associated with Io's orbital period (42 h) and that the bright region was located downstream of Io. The amplitude of the periodic variation was larger at short wavelengths than at long wavelengths. From spectral analyses, we found that Io-correlated brightening is caused by the increase in the hot electron population in the region downstream of Io. We also found that the brightness depends on the system III longitude and found primary and secondary peaks in the longitude ranges of 100-130° and 250-340°, respectively. Io's orbit crosses the center of the IPT around these longitudes. This longitude dependence suggests that the electron heating process is related to the plasma density around Io. The total radiated power from the IPT in January 2014 was estimated to be 1.4 TW in the wavelength range from 60 to 145 nm. The Io-correlated component produced 10% of this total radiated power. The interaction between Io and the IPT continuously produces a large amount of energy around Io, and 140 GW of that energy is immediately converted to hot electron production in the IPT.

  10. Dipole anisotropy in cosmic electrons and positrons: inspection on local sources

    NASA Astrophysics Data System (ADS)

    Manconi, S.; Di Mauro, M.; Donato, F.

    2017-01-01

    The cosmic electrons and positrons have been measured with unprecedented statistics up to several hundreds GeV, thus permitting to explore the role that close single sources can have in shaping the flux at different energies. In the present analysis, we consider electrons and positrons in cosmic rays to be produced by spallations of hadron fluxes with the interstellar medium, by a smooth Supernova Remnant (SNR) population, by all the ATNF catalog pulsars, and by few discrete, local SNRs. We test several source models on the e++e‑ and e+ AMS-02 flux data. For the configurations compatible with the data, we compute the dipole anisotropy in e++e‑, e+, e+/e‑ from single sources. Our study includes a dedicated analysis to the Vela SNR. We show that Fermi-LAT present data on dipole anisotropy of e++e‑ start to explore some of the models for the Vela SNR selected by AMS-02 flux data. We also investigate how the observed anisotropy could result from a combination of local sources. Our analysis shows that the search of anisotropy in the lepton fluxes up to TeV energies can be an interesting tool for the inspection of properties of close SNRs, complementary to the high precision flux data.

  11. Electron Temperature Evolution During Local Helicity Injection on the Pegasus Toroidal Experiment

    NASA Astrophysics Data System (ADS)

    Schlossberg, D. J.; Barr, J. L.; Bodner, G. M.; Bongard, M. W.; Fonck, R. J.; Perry, J. M.; Reusch, J. A.; Rodriguez Sanchez, C.

    2016-10-01

    Understanding the electron temperature (Te) evolution during local helicity injection (LHI) is critical for scaling up this non-solenoidal startup technique to MA-class devices. The first comprehensive Te measurements during LHI reveal centrally-peaked profiles with Te > 100 eV for plasma current Ip > 120 kA, toroidal field 0.15 T, and electron density ne 1019 m-3. Te rises and is sustained from just after magnetic relaxation through the plasma decoupling from edge-localized injectors. Results are presented for two injector edge locations: outboard midplane and inboard divertor. Outboard midplane injection couples LHI with inductive drive from poloidal field ramps and radial compression during inward plasma growth. Comparisons of Te at different LHI-to-inductive drive ratios show some profile flattening for higher LHI drive fraction. The latter, constant-shape discharges were necessarily lower performance, with Ip 50 kA and reduced Te , max. Inboard divertor injection achieves higher Ip using minimal inductive drive and thus isolates effects of LHI drive on Te. Initial results in this configuration show Te rising rapidly at the injector location as the discharge grows, settling to a roughly flat profile 100 eV. Thus far, both scenarios provide relatively stable discharges with moderate ne and high-Te, suitable for coupling to auxiliary current drive. Detailed studies of confinement dynamics and discharge optimization are planned for the near future. Work supported by US DOE Grant DE-FG02-96ER54375.

  12. Electronic structure and local magnetism of 3d-5d impurity substituted CeFe2

    NASA Astrophysics Data System (ADS)

    Das, Rakesh; Das, G. P.; Srivastava, S. K.

    2016-04-01

    We present here a systematic first-principles study of electronic structure and local magnetic properties of Ce[Fe0.75M0.25]2 compounds, where M is a 3d, 4d or 5d transition or post-transition element, using the generalized gradient approximation of the density functional theory. The d-f band hybridizations existing in CeFe2 get modified by the impurity M in an orderly manner across a period for each impurity series: the hybridization is strongest for the Mn group impurity in the period and gets diminished on either side of it. The weakening of the d-f hybridization strength is also associated with a relative localization of the Ce 4f states with respect to the delocalized 4f states in CeFe2. The above effects are most prominent for 3d impurity series, while for 4d and 5d impurities, the hybridizations and relocalizations are relatively weak due primarily to the relatively extended nature of 4d and 5d wavefunctions. The Ce local moment is found to decrease from the CeFe2 value in proportion to the strength of relocalization, thus following almost the same orderly trend as obeyed by the d-f hybridization. Further, depending on the way the spin-up and spin-down densities of states of an impurity shift relative to the Fermi energy, the impurity local moments are highest for Mn or Fe group, reduce on either side, become zero for Ni to Ga, and are small but negative for V and Ti. The Ce hyperfine field is found to follow the M local moment in a linear fashion, and vice-versa.

  13. Spectral properties and localization of an electron in a two-dimensional system with point scatterers in a magnetic field

    NASA Astrophysics Data System (ADS)

    Gredeskul, S. A.; Zusman, M.; Avishai, Y.; Azbel', M. Ya.

    1997-09-01

    Electron spectral properties and localization in a two-dimensional system with point potentials subject to a perpendicular magnetic field are studied. A brief review of the known results concerning electron dynamics in such systems is presented. For a set of periodic point potentials, exact dispersion laws and energy-flux diagram (Hofstadter-type butterfly) are obtained. It is shown that, in the case of one-dimensional disorder, the electron localization in a strong magnetic field is described by the random Harper equation. Energy-flux diagram for the localization length is presented and the fractal structure of the localization length is demonstrated. Near the Landau levels an exact formula for the localization length as a function of energy and disorder is obtained. The corresponding critical exponent is equal to unity which is reminiscent of one-dimensional characteristics.

  14. Electron transfer mechanism and the locality of the system-bath interaction: a comparison of local, semilocal, and pure dephasing models.

    PubMed

    Weiss, Emily A; Katz, Gil; Goldsmith, Randall H; Wasielewski, Michael R; Ratner, Mark A; Kosloff, Ronnie; Nitzan, Abraham

    2006-02-21

    We simulate the effects of two types of dephasing processes, a nonlocal dephasing of system eigenstates and a dephasing of semilocal eigenstates, on the rate and mechanism of electron transfer (eT) through a series of donor-bridge-acceptor systems, D-B(N)-A, where N is the number of identical bridge units. Our analytical and numerical results show that pure dephasing, defined as the perturbation of system eigenstates through the system-bath interaction, does not disrupt coherent eT because it induces no localization; electron transfer may proceed through superexchange in a system undergoing only pure dephasing. A more physically reasonable description may be obtained via a system-bath interaction that reflects the perturbation of more local electronic structure by local nuclear distortions and dipole interactions. The degree of locality of this interaction is guided by the structure of the system Hamiltonian and by the nature of the measurement performed on the system (i.e., the nature of the environment). We compare our result from this "semilocal" model with an even more local phenomenological dephasing model. We calculate electron transfer rate by obtaining nonequilibrium steady-state solutions for the elements of a reduced density matrix; a semigroup formalism is used to write down the dissipative part of the equation of motion.

  15. Electronic viscosity in a quantum well: A test for the local-density approximation

    NASA Astrophysics Data System (ADS)

    D'Agosta, Roberto; di Ventra, Massimiliano; Vignale, Giovanni

    2007-07-01

    In the local-density approximation (LDA) for electronic time-dependent current-density-functional theory, many-body effects are described in terms of the viscoelastic constants of the homogeneous three-dimensional electron gas. In this paper, we critically examine the applicability of the three-dimensional LDA to the calculation of the viscous damping of one-dimensional collective oscillations of angular frequency ω in a quasi-two-dimensional quantum well. We calculate the effective viscosity ζ(ω) from perturbation theory in the screened Coulomb interaction and compare it with the commonly used three-dimensional LDA viscosity Y(ω) . Significant differences are found. At low frequency, Y(ω) is dominated by a shear term, which is absent in ζ(ω) . At high frequency, ζ(ω) and Y(ω) exhibit different power-law behaviors ( ω-3 and ω-5/2 , respectively), reflecting different spectral densities of electron-hole excitations in two and three dimensions. These findings demonstrate the need for better approximations for the exchange-correlation stress tensor in specific systems where the use of the three-dimensional functionals may lead to unphysical results.

  16. Local lattice strain measurements in semiconductor devices by using convergent-beam electron diffraction

    NASA Astrophysics Data System (ADS)

    Toda, Akio; Ikarashi, Nobuyuki; Ono, Haruhiko

    2000-03-01

    We examined the lattice strain distribution around local oxidation of silicon (LOCOS) in a semiconductor device by using highly accurate (1.8×10 -4 standard deviation) convergent-beam electron diffraction (CBED) at a nanometer-scale spatial resolution (10 nm in diameter). The nanometer-scale measurement was done by reducing the elastic relaxation using a thick (about 600 nm) sample and by removing the inelastically scattered electrons by means of an electron energy filter. A highly accurate measurement was achieved through the analysis of higher-order Laue zone (HOLZ) patterns using the least-squares fitting of HOLZ line intersection distances between the observations and calculations. Our examination showed that the LOCOS structure gave singularities in strain distributions at the field edge. That is, compressive strain exists in both the vertical and horizontal directions of the substrate, and the shear strain increased there. Most notably, two-dimensional measurements revealed that the singularity of the normal strain in the horizontal direction of the substrate generated at the field edge propagated into the substrate.

  17. Basis set limit and systematic errors in local-orbital based all-electron DFT

    NASA Astrophysics Data System (ADS)

    Blum, Volker; Behler, Jörg; Gehrke, Ralf; Reuter, Karsten; Scheffler, Matthias

    2006-03-01

    With the advent of efficient integration schemes,^1,2 numeric atom-centered orbitals (NAO's) are an attractive basis choice in practical density functional theory (DFT) calculations of nanostructured systems (surfaces, clusters, molecules). Though all-electron, the efficiency of practical implementations promises to be on par with the best plane-wave pseudopotential codes, while having a noticeably higher accuracy if required: Minimal-sized effective tight-binding like calculations and chemically accurate all-electron calculations are both possible within the same framework; non-periodic and periodic systems can be treated on equal footing; and the localized nature of the basis allows in principle for O(N)-like scaling. However, converging an observable with respect to the basis set is less straightforward than with competing systematic basis choices (e.g., plane waves). We here investigate the basis set limit of optimized NAO basis sets in all-electron calculations, using as examples small molecules and clusters (N2, Cu2, Cu4, Cu10). meV-level total energy convergence is possible using <=50 basis functions per atom in all cases. We also find a clear correlation between the errors which arise from underconverged basis sets, and the system geometry (interatomic distance). ^1 B. Delley, J. Chem. Phys. 92, 508 (1990), ^2 J.M. Soler et al., J. Phys.: Condens. Matter 14, 2745 (2002).

  18. Density and localized states' impact on amorphous carbon electron transport mechanisms

    NASA Astrophysics Data System (ADS)

    Caicedo-Dávila, S.; Lopez-Acevedo, O.; Velasco-Medina, J.; Avila, A.

    2016-12-01

    This work discusses the electron transport mechanisms that we obtained as a function of the density of amorphous carbon (a-C) ultra-thin films. We calculated the density of states (total and projected), degree of electronic states' localization, and transmission function using the density functional theory and nonequilibrium Green's functions method. We generated 25 sample a-C structures using ab-initio molecular dynamics within the isothermal-isobaric ensemble. We identified three transport regimes as a function of the density, varying from semimetallic in low-density samples ( ≤2.4 g/cm3) to thermally activated in high-density ( ≥2.9 g/cm3) tetrahedral a-C. The middle-range densities (2.4 g/cm3 ≤ρ≤ 2.9 g/cm3) are characterized by resonant tunneling and hopping transport. Our findings offer a different perspective from the tight-binding model proposed by Katkov and Bhattacharyya [J. Appl. Phys. 113, 183712 (2013)], and agree with experimental observations in low-dimensional carbon systems [see S. Bhattacharyya, Appl. Phys. Lett. 91, 21 (2007)]. Identifying transport regimes is crucial to the process of understanding and applying a-C thin film in electronic devices and electrode coating in biosensors.

  19. Local electronic structure and nanolevel hierarchical organization of bone tissue: theory and NEXAFS study

    NASA Astrophysics Data System (ADS)

    Pavlychev, A. A.; Avrunin, A. S.; Vinogradov, A. S.; Filatova, E. O.; Doctorov, A. A.; Krivosenko, Yu S.; Samoilenko, D. O.; Svirskiy, G. I.; Konashuk, A. S.; Rostov, D. A.

    2016-12-01

    Theoretical and experimental investigations of native bone are carried out to understand relationships between its hierarchical organization and local electronic and atomic structure of the mineralized phase. The 3D superlattice model of a coplanar assembly of the hydroxyapatite (HAP) nanocrystallites separated by the hydrated nanolayers is introduced to account the interplay of short-, long- and super-range order parameters in bone tissue. The model is applied to (i) predict and rationalize the HAP-to-bone spectral changes in the electronic structure and (ii) describe the mechanisms ensuring the link of the hierarchical organization with the electronic structure of the mineralized phase in bone. To check the predictions the near-edge x-ray absorption fine structure (NEXAFS) at the Ca 2p, P 2p and O 1s thresholds is measured for native bone and compared with NEXAFS for reference compounds. The NEXAFS analysis has demonstrated the essential hierarchy induced HAP-to-bone red shifts of the Ca and P 2p-to-valence transitions. The lowest O 1s excitation line at 532.2 eV in bone is assigned with superposition of core transitions in the hydroxide OH-(H2O) m anions, Ca2+(H2O) n cations, the carboxyl groups inside the collagen and [PO4]2- and [PO4]- anions with unsaturated P-O bonds.

  20. Self-localized states for electron transfer in nonlocal continuum deformable media

    NASA Astrophysics Data System (ADS)

    Cisneros-Ake, Luis A.

    2016-08-01

    We consider the problem of electron transport in a deformable continuum medium subjected to an external harmonic substrate potential. We then consider the quasi-stationary state of the full problem to find a Gross-Pitaevskii type equation with a nonlocal external potential, which is solved by variational and numerical means (considered as the exact solution) to find the parameter conditions for the existence of self-localized solutions. The variational approach predicts a threshold on the on-site or nonlocality parameter where localized solutions cease to exist from the Non-Linear Schrödinger soliton limit. A numerical continuation of stationary state solutions in the corresponding discrete system is used to confirm the prediction of the turning value in the on-site term. We finally study the full stationary state and make use of an approximation, proposed by Briedis et al. [17], for the nonlocal term, corresponding to strong nonlocalities, to find analytic expressions for self-localized states in terms of the series solutions of a nonlinear modified Bessel equation.

  1. Establishing local and regional DRLs by means of electronic radiographical X-ray examination records.

    PubMed

    Charnock, P; Moores, B M; Wilde, R

    2013-11-01

    The objective of the paper is to demonstrate that patient dose audits may be undertaken at the local and regional levels by employing electronic examination records contained in Radiology Information Systems (RISs) that have been collected, analysed and managed by modern IT systems. The resulting mean and third quartile values obtained may then be used to establish local and regional dose reference levels (DRLs) as part of an optimisation strategy. The method involved the collection of roughly 1.3 million radiographical examination records stored in hospital RIS over a 3-y period from 10 hospital sites in the north of England. These were analysed according to the process employed in the national patient dose (NPD) audits undertaken every 5 y in the UK. Data processing and analysis methods are described that are suitable for handling very large data sets quickly and efficiently. Because RIS data involve manual data entry it may be susceptible to data entry errors. Therefore, a comparison of results obtained from both RIS and DICOM generated data was first of all undertaken in order to 'calibrate' the RIS-based method and demonstrate its accuracy. The results obtained from this comparison indicate that the RIS-based examination records provide patient dose distributions with an equivalent statistical accuracy compared with those employing DICOM data and, therefore, may be employed in patient dose audits in order to establish both local and regional DRLs for use in patient dose management and optimisation strategies.

  2. Subcellular Localization of the Sigma-1 Receptor in Retinal Neurons — an Electron Microscopy Study

    PubMed Central

    Mavlyutov, Timur A.; Epstein, Miles; Guo, Lian-Wang

    2015-01-01

    The Sigma-1 receptor (S1R) is known to play a protective role in the central nervous system including the retina. A major barrier for understanding the underlying mechanism is an ambiguity of S1R subcellular localizations. We thus conducted the first electron microscopy (EM) study of S1R subcellular distribution in the mouse retina. Immuno-EM imaging showed previously under-appreciated S1R presence in photoreceptor cells. Unlike in other cell types in previous reports, in photoreceptor cells S1R was found in the nuclear envelope but not localized in the endoplasmic reticulum (ER), raising a possibility of S1R-mediated modulatory mechanisms different than conventionally thought. While in bipolar cells S1R was detected only in the nuclear envelope, in ganglion cells S1R was identified predominantly in the nuclear envelope and found in the ER as well. A predominant localization of S1R in the nuclear envelope in all three retinal neurons implicates a potential role of S1R in modulating nuclear activities. Moreover, its absence in the plasma membrane and presence in the subsurface ER cisternae that are juxtaposed to the plasma membrane in ganglion cells may lend mechanistic insights generally important for frequently reported S1R modulations of ion channels in neurons. PMID:26033680

  3. Nqrs Data for C10H5F6IO4 (Subst. No. 1206)

    NASA Astrophysics Data System (ADS)

    Chihara, H.; Nakamura, N.

    This document is part of Subvolume A `Substances Containing Ag … C10H15' of Volume 48 `Nuclear Quadrupole Resonance Spectroscopy Data' of Landolt-Börnstein - Group III `Condensed Matter'. It contains an extract of Section `3.2 Data tables' of the Chapter `3 Nuclear quadrupole resonance data' providing the NQRS data for C10H5F6IO4 (Subst. No. 1206)

  4. Pou5f3.2-induced proliferative state of embryonic cells during gastrulation of Xenopus laevis embryo.

    PubMed

    Nishitani, Eriko; Li, Chong; Lee, Jaehoon; Hotta, Hiroyo; Katayama, Yuta; Yamaguchi, Masahiro; Kinoshita, Tsutomu

    2015-12-01

    POU class V (POU-V) transcription factors play the important role in maintenance of pluripotency and cell differentiation. Pou5f3.2 (Oct25), one of Xenopus POU-V transcription factors, shows the zygotic expression prior to gastrulation. In order to know the molecular mechanism of pou5f3.2 expression at gastrula stage, we examined a responsiveness of pou5f3.2 to Nodal signaling. Animal cap assay demonstrated that Xnr2 activates the gene expression of pou5f3.2. In comparative analysis of the 5'-flanking region of pou5f3.2 between Xenopus laevis and X. tropicalis, two conserved regions were detected within the flanking region. Reporter analyses showed that one of the conserved regions contained an enhancer region, which had several Smad2/3 and FoxH1 binding motifs. ChIP assay demonstrated that Smad2 binds to the enhancer region. These results suggest that Nodal signaling induces zygotic expression of pou5f3.2 at gastrula stage. To understand a role of pou5f3.2 in gastrula embryos, morpholino oligo DNA of pou5f3.2 was injected into the lateral side of one blastomere at the 2-cell stage. The morphant embryos showed diminution of Xbra1 expression and gastrulation defect in the injection side, suggesting the essential role of pou5f3.2 at the gastrula stage. Xbra1 expression and gastrulation were also inhibited by injecting with the synthesized RNAs of pou5f3.2. Furthermore, in the pou5f3.2-injected embryo, gene expression of p27Xic1 was drastically suppressed, and the number of dividing cells increased in the injection side. These results suggest that one role of pou5f3.2 is to keep the embryonic cells in undifferentiated and proliferative state during gastrulation.

  5. Spin response to localized pumps: Exciton polaritons versus electrons and holes

    NASA Astrophysics Data System (ADS)

    Sacksteder, Vincent; Pervishko, A. A.; Shelykh, I. A.

    2016-02-01

    Polariton polarization can be described in terms of a pseudospin which can be oriented along the x ,y , or z axis, similarly to electron and hole spin. Unlike electrons and holes where time-reversal symmetry requires that the spin-orbit interaction be odd in the momentum, the analog of the spin-orbit interaction for polaritons, the so-called TE-TM splitting, is even in the momentum. We calculate and compare spin transport of polariton, electron, and hole systems, in the diffusive regime of many scatterings. After dimensional rescaling diffusive systems with spatially uniform particle densities have identical dynamics, regardless of the particle type. Differences between the three particles appear in spatially nonuniform systems, with pumps at a specific localized point. We consider both oscillating pumps and transient (delta function) pumps. In such systems each particle type produces distinctive spin patterns. The particles can be distinguished by their differing spatial multipole character, their response and resonances in a perpendicular magnetic field, and their relative magnitude which is largest for electrons and weakest for holes. These patterns are manifested both in response to unpolarized pumps which produce in-plane and perpendicular spin signals, and to polarized pumps where the spin precesses from in-plane to out-of-plane and vice versa. These results will be useful for designing systems with large spin polarization signals, for identifying the dominant spin-orbit interaction and measuring subdominant terms in experimental devices, and for measuring the scattering time and the spin-orbit coupling's magnitude.

  6. Electron Temperature and Density in Local Helicity Injection and High betat Plasmas

    NASA Astrophysics Data System (ADS)

    Schlossberg, David J.

    Tokamak startup in a spherical torus (ST) and an ST-based fusion nuclear science facility can greatly benefit from using non-inductive methods. The Pegasus Toroidal Experiment has developed a non-inductive startup technique using local helicity injection (LHI). Electron temperature, T e(r), and density, ne( r), profiles during LHI are unknown. These profiles are critical for understanding both the physics of the injection and relaxation mechanisms, as well as for extrapolating this technique to larger devices. A new Thomson scattering system has been designed, installed, and used to characterize Te(r, t) and ne(r, t) during LHI. The diagnostic leverages new technology in image intensified CCD cameras, high-efficiency diffraction gratings, and reliable Nd:YAG lasers. Custom systems for stray light mitigation, fast shuttering, and precision timing have been developed and implemented. The overall system provides a low-maintenance, economic, and effective means to explore novel physics regimes in Pegasus. Electron temperature and density profiles during LHI have been measured for the first time. Results indicate Te(r) peaked in the core of plasmas, and sustained while plasmas are coupled to injection drive. Electron densities also peak near the core of the tokamak, up to local values of n e ˜ 1.5 x 1019 m -3. A comparison of Te( r, t) has been made between discharges with dominant drive voltage from induction versus helicity injection. In both cases Te ( r, t) profiles remain peaked, with values for Te ,max > 150 eV in dominantly helicity-driven plasmas using high-field side LHI. Sustained values of betat ˜ 100% have been demonstrated in a tokamak for the first time. Plasmas are created and driven entirely non-solenoidally, and exhibit MHD stability. Measured temperature and density profiles are used to constrain magnetic equilibrium reconstructions, which calculate 80% < betat < 100% throughout a toroidal field ramp-down. For a continued decrease in the toroidal

  7. Curly arrows meet electron density transfers in chemical reaction mechanisms: from electron localization function (ELF) analysis to valence-shell electron-pair repulsion (VSEPR) inspired interpretation.

    PubMed

    Andrés, Juan; Berski, Sławomir; Silvi, Bernard

    2016-07-07

    Probing the electron density transfers during a chemical reaction can provide important insights, making possible to understand and control chemical reactions. This aim has required extensions of the relationships between the traditional chemical concepts and the quantum mechanical ones. The present work examines the detailed chemical insights that have been generated through 100 years of work worldwide on G. N. Lewis's ground breaking paper on The Atom and the Molecule (Lewis, G. N. The Atom and the Molecule, J. Am. Chem. Soc. 1916, 38, 762-785), with a focus on how the determination of reaction mechanisms can be reached applying the bonding evolution theory (BET), emphasizing how curly arrows meet electron density transfers in chemical reaction mechanisms and how the Lewis structure can be recovered. BET that combines the topological analysis of the electron localization function (ELF) and Thom's catastrophe theory (CT) provides a powerful tool providing insight into molecular mechanisms of chemical rearrangements. In agreement with physical laws and quantum theoretical insights, BET can be considered as an appropriate tool to tackle chemical reactivity with a wide range of possible applications. Likewise, the present approach retrieves the classical curly arrows used to describe the rearrangements of chemical bonds for a given reaction mechanism, providing detailed physical grounds for this type of representation. The ideas underlying the valence-shell-electron pair-repulsion (VSEPR) model applied to non-equilibrium geometries provide simple chemical explanations of density transfers. For a given geometry around a central atom, the arrangement of the electronic domain may comply or not with the VSEPR rules according with the valence shell population of the considered atom. A deformation yields arrangements which are either VSEPR defective (at least a domain is missing to match the VSEPR arrangement corresponding to the geometry of the ligands), VSEPR compliant

  8. Localized heating of electrons in ionization zones: Going beyond the Penning-Thornton paradigm in magnetron sputtering

    SciTech Connect

    Anders, Andre

    2014-12-07

    The fundamental question of how energy is supplied to a magnetron discharge is commonly answered by the Penning-Thornton paradigm invoking secondary electrons. Huo et al. (Plasma Sources Sci. Technol. 22, 045005, (2013)) used a global discharge model to show that electron heating in the electric field of the magnetic presheath is dominant. In this contribution, this concept is applied locally taking into account the electric potential structure of ionization zones. Images of ionization zones can and should be interpreted as diagrams of the localization of electric potential and related electron energy, where certain collisions promote or dampen their formation.

  9. CONDENSED MATTER: ELECTRONIC STRUCTURE, ELECTRICAL, MAGNETIC, AND OPTICAL PROPERTIES Electronic Transport Calculations Using Maximally-Localized Wannier Functions

    NASA Astrophysics Data System (ADS)

    Wang, Neng-Ping

    2011-01-01

    I present a method to calculate the ballistic transport properties of atomic-scale structures under bias. The electronic structure of the system is calculated using the Kohn-Sham scheme of density functional theory (DFT). The DFT eigenvectors are then transformed into a set of maximally localized Wannier functions (MLWFs) [N. Marzari and D. Vanderbilt, Phys. Rev. B 56 (1997) 12847]. The MLWFs are used as a minimal basis set to obtain the Hamitonian matrices of the scattering region and the adjacent leads, which are needed for transport calculation using the nonequilibrium Green's function formalism. The coupling of the scattering region to the semi-infinite leads is described by the self-energies of the leads. Using the nonequilibrium Green's function method, one calculates self-consistently the charge distribution of the system under bias and evaluates the transmission and current through the system. To solve the Poisson equation within the scheme of MLWFs I introduce a computationally efficient method. The method is applied to a molecular hydrogen contact in two transition metal monatomic wires (Cu and Pt). It is found that for Pt the I-V characteristics is approximately linear dependence, however, for Cu the I-V characteristics manifests a linear dependence at low bias voltages and exhibits apparent nonlinearity at higher bias voltages. I have also calculated the transmission in the zero bias voltage limit for a single CO molecule adsorbed on Cu and Pt monatomic wires. While a chemical scissor effect occurs for the Cu monatomic wire with an adsorbed CO molecule, it is absent for the Pt monatomic wire due to the contribution of d-orbitals at the Fermi energy.

  10. Local increases in auroral electron precipitation which were not accompanied by a corresponding increase in the electric potential of the auroral electron acceleration region

    NASA Astrophysics Data System (ADS)

    Calvert, W.; Hardy, D. A.

    The Oedipus C rocket that was launched from Poker Flats, Alaska in November 1995 has detected significant local increases in the observed auroral electron precipitation flux during an auroral substorm which were not accompanied by a corresponding increase in the electric potential of the auroral electron acceleration region. The energy of the electrons which contributed to these increases in flux were also found to extend well below the electric potential energy of these electrons at the top of the acceleration region, thereby requiring a related loss in energy inside the acceleration region. This loss in energy must therefore be attributed to a wave instability which extracts energy from the electrons which are scattered into the loss cone inside the electron acceleration region to cause the discrete aurora during a substorm.

  11. Localization of Somatic Antigen on Gram-Negative Bacteria by Electron Microscopy

    PubMed Central

    Shands, J. W.

    1965-01-01

    Shands, J. W. (University of Florida, Gainesville). Localization of somatic antigen on gram-negative bacteria by electron microscopy. J. Bacteriol. 90:266–270. 1965.—Antisera specific for the somatic antigens of Salmonella typhimurium and Escherichia coli O113 were prepared, and globulins isolated from these antisera were labeled with ferritin. Micrographs of labeled, sectioned bacteria show that somatic antigen is located in considerable quantities on the surface of the bacteria, and, furthermore, that it can extend up to 150 mμ beyond the confines of the cell wall. The arrangement of the ferritin on the bacteria suggests that the antigenic sites are located on fibrillar structures. Images PMID:16562028

  12. Local spectroscopy of moiré-induced electronic structure in gate-tunable twisted bilayer graphene

    NASA Astrophysics Data System (ADS)

    Wong, Dillon; Wang, Yang; Jung, Jeil; Pezzini, Sergio; DaSilva, Ashley M.; Tsai, Hsin-Zon; Jung, Han Sae; Khajeh, Ramin; Kim, Youngkyou; Lee, Juwon; Kahn, Salman; Tollabimazraehno, Sajjad; Rasool, Haider; Watanabe, Kenji; Taniguchi, Takashi; Zettl, Alex; Adam, Shaffique; MacDonald, Allan H.; Crommie, Michael F.

    2015-10-01

    Twisted bilayer graphene (tBLG) forms a quasicrystal whose structural and electronic properties depend on the angle of rotation between its layers. Here, we present a scanning tunneling microscopy study of gate-tunable tBLG devices supported by atomically smooth and chemically inert hexagonal boron nitride (BN). The high quality of these tBLG devices allows identification of coexisting moiré patterns and moiré super-superlattices produced by graphene-graphene and graphene-BN interlayer interactions. Furthermore, we examine additional tBLG spectroscopic features in the local density of states beyond the first van Hove singularity. Our experimental data are explained by a theory of moiré bands that incorporates ab initio calculations and confirms the strongly nonperturbative character of tBLG interlayer coupling in the small twist-angle regime.

  13. Local interlayer tunneling between two-dimensional electron systems in the ballistic regime

    NASA Astrophysics Data System (ADS)

    Luna, Katherine; Kim, Eun-Ah; Oreto, Paul; Kivelson, Steven A.; Goldhaber-Gordon, David

    2010-12-01

    We study a theoretical model of virtual scanning tunneling microscopy (VSTM) [A. Sciambi, M. Pelliccione, M. Lilly, S. Bank, A. Gossard, L. Pfeiffer, K. West, and D. Goldhaber-Gordon, arXiv:1008.0668 (unpublished); A. Sciambi, M. Pelliccione, S. R. Bank, A. C. Gossard, and D. Goldhaber-Gordon, Appl. Phys. Lett. 97, 132103 (2010)10.1063/1.3492440]: a proposed application of interlayer tunneling in a bilayer system to locally probe a two-dimensional electron system (2DES) in a semiconductor heterostructure. We consider tunneling for the case where transport in the 2DESs is ballistic and show that the zero-bias anomaly is suppressed by extremely efficient screening. Since such an anomaly would complicate the interpretation of data from VSTM, this result is encouraging for efforts to implement such a microscopy technique.

  14. Tetramine dichloro-palladium subcellular localization in the kidney: electron microprobe study.

    PubMed

    Berry, J P

    1987-01-01

    Palladium salt has been used for some time in experimental therapy protocols; with this in mind, we carried out a study of the effect of tetramine dichloro-palladium (soluble salt) upon kidney cells. Using an electron microprobe, we were able to detect the presence of palladium associated with sulfur and iron in the lysosomes of the proximal tubule cells. Our results were compared with those obtained using Cis-diaminedichloro-platinum (Cis-DDP), an anti-cancer drug used in the treatment of diverse tumors. The mechanism of intralysosomal concentration of palladium as a non soluble salt associated with sulfur appeared to be related to local sulfatase activity. Finally, iron concentration appeared to be related to the inhibition process of erythropoiesis.

  15. Sawtooth stabilization by localized electron cyclotron heating in the WT-3 tokamak

    SciTech Connect

    Hanada, K.; Maehara, T.; Makino, K.; Kishigami, Y.; Kishino, T.; Minami, T.; Tanaka, H.; Iida, M.; Nakamura, M.; Maekawa, T.; Terumichi, Y.; Tanaka, S. )

    1992-11-01

    The effect on sawtooth oscillations (STO) by localized electron-cyclotron-resonance heating (ECH) on the WT-3 tokamak ({ital Plasma} {ital Physics} {ital and} {ital Controlled} {ital Nuclear} {ital Fusion} {ital Research}, 1988 (International Atomic Energy Agency, Vienna, 1989), Vol. 1, p. 563) is studied. STO are strongly modified or stabilized by ECH near the {ital q}=1 surface, where {ital q} refers to the safety factor. The effect of ECH is much stronger when it is applied on the high-field side as compared to the low-field side. Further, even when ECH is applied outside the {ital q}=1 surface, the amplitude of STO decreases and STO stabilizes. In the very high {ital q}{sub {ital L}} discharge, the excitation of STO can be obtained by applying ECH.

  16. The impact of pedestal turbulence and electron inertia on edge-localized-mode crashes

    SciTech Connect

    Xi, P. W.; Xu, X. Q.; Diamond, P. H.

    2014-05-15

    We demonstrate that the occurrence of Edge-Localized-Modes (ELM) crashes does not depend only on the linear peeling-ballooning threshold, but also relies on nonlinear processes. Wave-wave interaction constrains the growth time of a mode, thus inducing a shift in the criterion for triggering an ELM crash. An ELM crash requires the P-B growth rate to exceed a critical value γ>γ{sub c}, where γ{sub c} is set by 1/τ{sup ¯}{sub c}, and τ{sup ¯}{sub c} is the averaged mode phase coherence time. For 0<γ<γ{sub c}, P-B turbulence develops but drives enhanced turbulent transport. We also show that electron inertia dramatically changes the instability threshold when density is low. However, P-B turbulence alone cannot generate enough current transport to allow fast reconnection during an ELM crash.

  17. New compact and efficient local oscillator optic system for the KSTAR electron cyclotron emission imaging system

    NASA Astrophysics Data System (ADS)

    Nam, Y. B.; Lee, D. J.; Lee, J.; Kim, C.; Yun, G. S.; Lee, W.; Park, H. K.

    2016-11-01

    Electron cyclotron emission imaging (ECEI) diagnostic on Korean Superconducting Tokamak Advanced Research utilizes quasi-optical heterodyne-detection method to measure 2D (vertical and radial) Te fluctuations from two toroidally separated poloidal cross section of the plasma. A cylindrical lens local oscillator (LO) optics with optical path length (OPL) 2-2.5 m has been used in the current ECEI system to couple the LO source to the 24 vertically aligned array of ECE detectors. For efficient and compact LO optics employing the Powell lens is proposed so that the OPL of the LO source is significantly reduced from ˜2.0 m to 0.4 m with new optics. The coupling efficiency of the LO source is expected to be improved especially at the edge channels. Results from the optical simulation together with the laboratory test of the prototype optics will be discussed in this paper.

  18. A statistical characterization of local mid-latitude total electron content

    SciTech Connect

    Gail, W.B.; Prag, A.B.; Coco, D.S.; Coker, C.

    1993-09-01

    The integrated line-of-slight electron density within the ionosphere, known as the total electron content (TEC), is commonly used to quantify ionospheric propagation effects. In order to extrapolate single-point measurements of TEC to other locations and times, some characterization of the TEC spatiotemporal variation must be available. Using a four-channel receiver tracking coded signals from the NAVSTAR Global Positioning System satellites, estimates of both the mean variation and correlation coefficient have been made for the approximately 1200-km or 1-hour local time radius ionospheric region within view of a mid-latitude station. Results were obtained for morning and midday over a 4-week period near the autumnal equinox in 1989. The derived mean variation was found to be well characterized by linear functions of the local time and latitude separation between the ground site and the ionospheric penetration point of the signal. The correlation coefficient during midday was found to decrease linearly with latitude, longitude, and time separation, with values of about 0.91 for a 1000-km separation and 0.98 for a 1-hour separation. During morning hours the longitude and time coefficients were similar to the midday values, but the latitude coefficient was found to have a nonlinear dependence, with values as small as 0.70. The combined results suggest that the decorrelation is due primarily to longer term TEC fluctuation, such as day-to-day variation in the TEC spatial dependence, rather than to transient effects such as traveling ionospheric disturbances. The analysis provides a spatiotemporal characterization of TEC that can be used to extrapolate TEC values from single-point measurements. 13 refs., 8 figs.

  19. Localized Hartree product treatment of multiple protons in the nuclear-electronic orbital framework

    NASA Astrophysics Data System (ADS)

    Auer, Benjamin; Hammes-Schiffer, Sharon

    2010-02-01

    An approximation for treating multiple quantum nuclei within the nuclear-electronic orbital (NEO) framework for molecular systems is presented. In the approximation to NEO-Hartree-Fock, the nuclear wave function is represented by a Hartree product rather than a Slater determinant, corresponding to the neglect of the nuclear exchange interactions. In the approximation to NEO-density functional theory, the nuclear exchange-correlation functional is chosen to be the diagonal nuclear exchange interaction terms, thereby eliminating the nuclear self-interaction terms. To further enhance the simplicity and computational efficiency, the nuclear molecular orbitals or Kohn-Sham orbitals are expanded in terms of localized nuclear basis sets. These approximations are valid because of the inherent localization of the nuclear orbitals and the numerical insignificance of the nuclear exchange interactions in molecular systems. Moreover, these approximations lead to substantial computational savings due to the reduction in both the number of integrals that must be calculated and the size of the matrices that must be diagonalized. These nuclear Hartree product approximation (HPA) methods scale linearly with the number of quantum protons and are highly parallelizable. Applications to a water hexamer, glycine dimer, and 32-water cluster, where all hydrogen nuclei are treated quantum mechanically, illustrate the accuracy and computational efficiency of the nuclear HPA methods. These strategies will facilitate the implementation of explicitly correlated NEO methods for molecular systems with multiple quantum protons.

  20. Localized Tail States and Electron Mobility in Amorphous ZnON Thin Film Transistors

    PubMed Central

    Lee, Sungsik; Nathan, Arokia; Ye, Yan; Guo, Yuzheng; Robertson, John

    2015-01-01

    The density of localized tail states in amorphous ZnON (a-ZnON) thin film transistors (TFTs) is deduced from the measured current-voltage characteristics. The extracted values of tail state density at the conduction band minima (Ntc) and its characteristic energy (kTt) are about 2 × 1020 cm−3eV−1 and 29 meV, respectively, suggesting trap-limited conduction prevails at room temperature. Based on trap-limited conduction theory where these tail state parameters are considered, electron mobility is accurately retrieved using a self-consistent extraction method along with the scaling factor ‘1/(α + 1)’ associated with trapping events at the localized tail states. Additionally, it is found that defects, e.g. oxygen and/or nitrogen vacancies, can be ionized under illumination with hv ≫ Eg, leading to very mild persistent photoconductivity (PPC) in a-ZnON TFTs. PMID:26304606

  1. Suppression of stimulated Raman scattering due to localization of electron plasma wave in laser beam filaments

    SciTech Connect

    Sharma, Prerana; Sharma, R. P.

    2009-03-15

    The filamentation of the high power laser beam by taking off-axial contribution is investigated when ponderomotive nonlinearity is taken into account. The splitted profile of the laser beam is obtained due to uneven focusing of the off-axial rays. It is observed that the weak electron plasma wave (EPW) propagating in the z direction is nonlinearly coupled in the modified filamentary regions of the laser beam. The semianalytical solution of the nonlinear coupled EPW equation in the presence of laser beam filaments has been found and it is observed that the nonlinear coupling between these two waves leads to localization of the EPW. Stimulated Raman scattering (SRS) of this EPW is studied and backreflectivity has been calculated. Further, the localization of EPW affects the eigenfrequency and damping of plasma wave. As a result of this, mismatch and modified enhanced Landau damping lead to the disruption of SRS process and a substantial reduction in the backreflectivity. For the typical laser beam and plasma parameters with wavelength ({lambda}=1064 nm), power flux ({approx_equal}10{sup 16} W cm{sup -2}), and plasma density (n/n{sub cr})=0.2; the backreflectivity was found to be suppressed by a factor of around 20%.

  2. Suppression of stimulated Raman scattering due to localization of electron plasma wave in laser beam filaments

    NASA Astrophysics Data System (ADS)

    Sharma, Prerana; Sharma, R. P.

    2009-03-01

    The filamentation of the high power laser beam by taking off-axial contribution is investigated when ponderomotive nonlinearity is taken into account. The splitted profile of the laser beam is obtained due to uneven focusing of the off-axial rays. It is observed that the weak electron plasma wave (EPW) propagating in the z direction is nonlinearly coupled in the modified filamentary regions of the laser beam. The semianalytical solution of the nonlinear coupled EPW equation in the presence of laser beam filaments has been found and it is observed that the nonlinear coupling between these two waves leads to localization of the EPW. Stimulated Raman scattering (SRS) of this EPW is studied and backreflectivity has been calculated. Further, the localization of EPW affects the eigenfrequency and damping of plasma wave. As a result of this, mismatch and modified enhanced Landau damping lead to the disruption of SRS process and a substantial reduction in the backreflectivity. For the typical laser beam and plasma parameters with wavelength (λ =1064 nm), power flux (≈1016 W cm-2), and plasma density (n /ncr)=0.2; the backreflectivity was found to be suppressed by a factor of around 20%.

  3. Suppression of stimulated Raman scattering due to localization of electron plasma wave in laser beam filaments

    NASA Astrophysics Data System (ADS)

    Sharma, Prerana; Sharma, Rampal

    2009-11-01

    The filamentation of the high power laser beam by taking off-axial contribution is investigated when ponderomotive nonlinearity is taken into account. The splitted profile of the laser beam is obtained due to uneven focusing of the off-axial rays. It is observed that the weak electron plasma wave (EPW) propagating in the z direction is nonlinearly coupled in the modified filamentary regions of the laser beam. The semi-analytical solution of the nonlinear coupled EPW equation in the presence of laser beam filaments has been found and it is observed that the nonlinear coupling between these two waves leads to localization of the EPW. Stimulated Raman scattering (SRS) of this EPW is studied and back reflectivity has been calculated. Further, the localization of EPW affects the eigen frequency and damping of plasma wave. As a result of this, mismatch and modified enhanced Landau damping lead to the disruption of SRS process and a substantial reduction in the back reflectivity. For the typical laser beam and plasma parameters with wavelength (λ=1064nm), power flux ( 10^16 W cm-2), and plasma density (n/ncr) = 0.2; the back reflectivity was found to be suppressed by a factor of around 20%.

  4. Local instability driving extreme events in a pair of coupled chaotic electronic circuits

    NASA Astrophysics Data System (ADS)

    de Oliveira, Gilson F.; Di Lorenzo, Orlando; de Silans, Thierry Passerat; Chevrollier, Martine; Oriá, Marcos; Cavalcante, Hugo L. D. de Souza

    2016-06-01

    For a long time, extreme events happening in complex systems, such as financial markets, earthquakes, and neurological networks, were thought to follow power-law size distributions. More recently, evidence suggests that in many systems the largest and rarest events differ from the other ones. They are dragon kings, outliers that make the distribution deviate from a power law in the tail. Understanding the processes of formation of extreme events and what circumstances lead to dragon kings or to a power-law distribution is an open question and it is a very important one to assess whether extreme events will occur too often in a specific system. In the particular system studied in this paper, we show that the rate of occurrence of dragon kings is controlled by the value of a parameter. The system under study here is composed of two nearly identical chaotic oscillators which fail to remain in a permanently synchronized state when coupled. We analyze the statistics of the desynchronization events in this specific example of two coupled chaotic electronic circuits and find that modifying a parameter associated to the local instability responsible for the loss of synchronization reduces the occurrence of dragon kings, while preserving the power-law distribution of small- to intermediate-size events with the same scaling exponent. Our results support the hypothesis that the dragon kings are caused by local instabilities in the phase space.

  5. Combined Modality Therapy Including Intraoperative Electron Irradiation for Locally Recurrent Colorectal Cancer

    SciTech Connect

    Haddock, Michael G.; Miller, Robert C.; Nelson, Heidi; Pemberton, John H.; Dozois, Eric J.; Alberts, Steven R.; Gunderson, Leonard L.

    2011-01-01

    Purpose: To evaluate survival, relapse patterns, and prognostic factors in patients with colorectal cancer relapse treated with curative-intent therapy, including intraoperative electron radiation therapy (IOERT). Methods and Materials: From April 1981 through January 2008, 607 patients with recurrent colorectal cancer received IOERT as a component of treatment. IOERT was preceded or followed by external radiation (median dose, 45.5 Gy) in 583 patients (96%). Resection was classified as R0 in 227 (37%), R1 in 224 (37%), and R2 in 156 (26%). The median IOERT dose was 15 Gy (range, 7.5-30 Gy). Results: Median overall survival was 36 months. Five- and 10-year survival rates were 30% and 16%, respectively. Survival estimates at 5 years were 46%, 27%, and 16% for R0, R1, and R2 resection, respectively. Multivariate analysis revealed that R0 resection, no prior chemotherapy, and more recent treatment (in the second half of the series) were associated with improved survival. The 3-year cumulative incidence of central, local, and distant relapse was 12%, 23%, and 49%, respectively. Central and local relapse were more common in previously irradiated patients and in those with subtotal resection. Toxicity Grade 3 or higher partially attributable to IOERT was observed in 66 patients (11%). Neuropathy was observed in 94 patients (15%) and was more common with IOERT doses exceeding 12.5 Gy. Conclusions: Long-term survival and disease control was achievable in patients with locally recurrent colorectal cancer. Continued evaluation of curative-intent, combined-modality therapy that includes IOERT is warranted in this high-risk population.

  6. Electron beam induced local crystallization of HfO2 nanopores for biosensing applications

    NASA Astrophysics Data System (ADS)

    Shim, Jiwook; Rivera, Jose A.; Bashir, Rashid

    2013-10-01

    We report the development of single, locally crystallized nanopores in HfO2 membranes for biosensing applications. HfO2 is chosen for its isoelectric point of 7.0, mechanical and chemical stability in solution, and for its potential as a high-k material for nanopore ionic field effect transistor applications. The HfO2 membrane is deposited on a graphene layer suspended over a 300 nm FIB hole, where graphene is used as the mechanical support. Exposure of the membrane to a focused electron beam causes crystallization in the vicinity of the nanopore during pore formation. We investigate the effects of crystallization on the electrical and surface properties of HfO2 films. Our surface analysis of HfO2 reveals improved hydrophilicity of crystallized HfO2, a notable advantage over the hydrophobicity of as-deposited HfO2. We also demonstrate detection of dsDNA translocation through HfO2 nanopores under various applied bias levels. In addition, our device architecture also presents a promising first step toward the realization of high-k HfO2 nanopore transistors.We report the development of single, locally crystallized nanopores in HfO2 membranes for biosensing applications. HfO2 is chosen for its isoelectric point of 7.0, mechanical and chemical stability in solution, and for its potential as a high-k material for nanopore ionic field effect transistor applications. The HfO2 membrane is deposited on a graphene layer suspended over a 300 nm FIB hole, where graphene is used as the mechanical support. Exposure of the membrane to a focused electron beam causes crystallization in the vicinity of the nanopore during pore formation. We investigate the effects of crystallization on the electrical and surface properties of HfO2 films. Our surface analysis of HfO2 reveals improved hydrophilicity of crystallized HfO2, a notable advantage over the hydrophobicity of as-deposited HfO2. We also demonstrate detection of dsDNA translocation through HfO2 nanopores under various applied

  7. Electric Field Tuned Crossover from Classical to Weakly Localized Quantum Transport in Electron Doped SrTiO3

    SciTech Connect

    Ngai, J.H.; Segal, Y.; Su, D.; Zhu, Y.; Walker, F.J.; Ismail-Beigi, S.; Le Hur, K.; Ahn, C.H.

    2010-06-21

    Electron gases created by modulating the charge density near interfaces and surfaces of insulating SrTiO{sub 3} offer a wide range of tunable behavior. Here, we utilize the nonlinear dielectric response of SrTiO{sub 3} to electrostatically manipulate the spatial confinement of an electron gas relative to an interface, where scattering is enhanced. Magnetotransport measurements reveal that the electron gas can be tuned from weakly localized to classical transport regimes. This crossover in transport demonstrates that elastic scattering can be electrostatically controlled, providing another degree of tunability for electron gases in SrTiO{sub 3}.

  8. A soft X-ray spectroscopic perspective of electron localization and transport in tungsten doped bismuth vanadate single crystals.

    PubMed

    Jovic, Vedran; Rettie, Alexander J E; Singh, Vijay R; Zhou, Jianshi; Lamoureux, Bethany; Buddie Mullins, C; Bluhm, Hendrik; Laverock, Jude; Smith, Kevin E

    2016-11-23

    Doped BiVO4 is a promising photoelectrochemical water splitting anode, whose activity is hampered by poor charge transport. Here we use a set of X-ray spectroscopic methods to probe the origin and nature of localized electron states in W:BiVO4. Furthermore, using the polarized nature of the X-rays, we probe variations in the electronic structure along the crystal axes. In this manner, we reveal aspects of the electronic structure related to electron localization and observations consistent with conductivity anisotropy between the ab-plane and c-axis. We verify that tungsten substitutes as W(6+) for V(5+) in BiVO4. This is shown to result in the presence of inter-band gap states related to electrons at V(4+) sites of e symmetry. The energetic position of the states in the band gap suggest that they are highly localized and may act as recombination centres. Polarization dependent X-ray absorption spectra reveal anisotropy in the electronic structure between the ab-plane and c-axis. Results show the superior hybridization between V 3d and O 2p states, higher V wavefunction overlap and broader conduction bands in the ab-plane than in the c-axis. These insights into the electronic structure are discussed in the context of existing experimental and theoretical reports regarding charge transport in BiVO4.

  9. Electronic fluxes during Diels-Alder reactions involving 1,2-benzoquinones: mechanistic insights from the analysis of electron localization function and catastrophe theory.

    PubMed

    González-Navarrete, Patricio; Domingo, Luis R; Andrés, Juan; Berski, Slawomir; Silvi, Bernard

    2012-11-15

    By means of the joint use of electron localization function (ELF) and Thom's catastrophe theory, a theoretical analysis of the energy profile for the hetero-Diels-Alder reaction of 4-methoxy-1,2-benzoquinone 1 and methoxyethylene 2 has been carried out. The 12 different structural stability domains obtained by the bonding evolution theory have been identified as well as the bifurcation catastrophes (fold and cusp) responsible for the changes in the topology of the system. This analysis permits finding a relationship between the ELF topology and the evolution of the bond breaking/forming processes and electron pair rearrangements through the reaction progress in terms of the different ways of pairing up the electrons. The reaction mechanism corresponds to an asynchronous electronic flux; first, the O1-C5 bond is formed by the nucleophilic attack of the C5 carbon of the electron rich ethylene 2 on the most electrophilically activated carbonyl O1 oxygen of 1, and once the σ bond has been completed, the formation process of the second O4C6 bond takes place. In addition, the values of the local electrophilicity and local nucleophilcity indices in the framework of conceptual density functional theory accounts for the asychronicity of the process as well as for the observed regioselectivity.

  10. Local Dynamic Stability Assessment of Motion Impaired Elderly Using Electronic Textile Pants.

    PubMed

    Liu, Jian; Lockhart, Thurmon E; Jones, Mark; Martin, Tom

    2008-10-01

    A clear association has been demonstrated between gait stability and falls in the elderly. Integration of wearable computing and human dynamic stability measures into home automation systems may help differentiate fall-prone individuals in a residential environment. The objective of the current study was to evaluate the capability of a pair of electronic textile (e-textile) pants system to assess local dynamic stability and to differentiate motion-impaired elderly from their healthy counterparts. A pair of e-textile pants comprised of numerous e-TAGs at locations corresponding to lower extremity joints was developed to collect acceleration, angular velocity and piezoelectric data. Four motion-impaired elderly together with nine healthy individuals (both young and old) participated in treadmill walking with a motion capture system simultaneously collecting kinematic data. Local dynamic stability, characterized by maximum Lyapunov exponent, was computed based on vertical acceleration and angular velocity at lower extremity joints for the measurements from both e-textile and motion capture systems. Results indicated that the motion-impaired elderly had significantly higher maximum Lyapunov exponents (computed from vertical acceleration data) than healthy individuals at the right ankle and hip joints. In addition, maximum Lyapunov exponents assessed by the motion capture system were found to be significantly higher than those assessed by the e-textile system. Despite the difference between these measurement techniques, attaching accelerometers at the ankle and hip joints was shown to be an effective sensor configuration. It was concluded that the e-textile pants system, via dynamic stability assessment, has the potential to identify motion-impaired elderly.

  11. Rapid precipitation of radiation belt electrons induced by EMIC rising tone emissions localized in longitude inside and outside the plasmapause

    NASA Astrophysics Data System (ADS)

    Kubota, Yuko; Omura, Yoshiharu

    2017-01-01

    By performing test particle simulations of relativistic electrons scattered by electromagnetic ion cyclotron (EMIC) rising tone emissions, we find a nonlinear scattering process named SLPA (Scattering at Low Pitch Angle) totally different from the nonlinear wave trapping. The nonlinear wave trapping, occurring for high pitch angles away from the loss cone, scatters some of resonant electrons to lower pitch angles, and a fraction of the electrons is further transported into the loss cone by SLPA after being released from the wave trapping. SLPA as well as the nonlinear wave trapping can work in any cases with proton band or helium band and inside or outside the plasmapause. We clarify that the combined scattering process causes significant depletion of the outer radiation belt. In the time evolution of an electron distribution observed locally in longitude, we find echoes of the electron depletion by the localized EMIC emissions. Monitoring fluxes of electrons being lost into the atmosphere in the wave generation region, we also find that efficient relativistic electron precipitation in several seconds. The characteristics of the precipitating electron flux as a function of kinetic energy vary significantly depending on the wave frequency range and the plasma density.

  12. Probability Density Functions of Floating Potential Fluctuations Due to Local Electron Flux Intermittency in a Linear ECR Plasma

    NASA Astrophysics Data System (ADS)

    Yoshimura, Shinji; Terasaka, Kenichiro; Tanaka, Eiki; Aramaki, Mitsutoshi; Tanaka, Masayoshi Y.

    An intermittent behavior of local electron flux in a laboratory ECR plasma is statistically analyzed by means of probability density functions (PDFs). The PDF constructed from a time series of the floating potential signal on a Langmuir probe has a fat tail in the negative value side, which reflects the intermittency of the local electron flux. The PDF of the waiting time, which is defined by the time interval between two successive events, is found to exhibit an exponential distribution, suggesting that the phenomenon is characterized by a stationary Poisson process. The underlying Poisson process is also confirmed by the number of events in given time intervals that is Poisson distributed.

  13. The roles of 4f- and 5f-orbitals in bonding: A magnetochemical, crystal field, density functional theory, and multi-reference wavefunction study

    DOE PAGES

    Lukens, Wayne W.; Speldrich, Manfred; Yang, Ping; ...

    2016-05-31

    The electronic structures of 4f3/5f3 Cp"3M and Cp"3M·alkylisocyanide complexes, where Cp" is 1,3-bis-(trimethylsilyl)cyclopentadienyl, are explored with a focus on the splitting of the f-orbitals, which provides information about the strengths of the metal–ligand interactions. While the f-orbital splitting in many lanthanide complexes has been reported in detail, experimental determination of the f-orbital splitting in actinide complexes remains rare in systems other than halide and oxide compounds, since the experimental approach, crystal field analysis, is generally significantly more difficult for actinide complexes than for lanthanide complexes. In this study, a set of analogous neodymium(III) and uranium(III) tris-cyclopentadienyl complexes and their isocyanidemore » adducts was characterized by electron paramagnetic resonance (EPR) spectroscopy and magnetic susceptibility. The crystal field model was parameterized by combined fitting of EPR and susceptibility data, yielding an accurate description of f-orbital splitting. The isocyanide derivatives were also studied using density functional theory, resulting in f-orbital splitting that is consistent with crystal field fitting, and by multi-reference wavefunction calculations that support the electronic structure analysis derived from the crystal-field calculations. The results highlight that the 5f-orbitals, but not the 4f-orbitals, are significantly involved in bonding to the isocyanide ligands. The main interaction between isocyanide ligand and the metal center is a σ-bond, with additional 5f to π* donation for the uranium complexes. As a result, while interaction with the isocyanide π*-orbitals lowers the energies of the 5fxz2 and 5fyz2-orbitals, spin–orbit coupling greatly reduces the population of 5fxz2 and 5fyz2 in the ground state.« less

  14. Bulk and Local Electron Transport and Optical Properties of Aluminum-doped Zinc Oxide

    NASA Astrophysics Data System (ADS)

    Likovich, Edward Michael

    ZnO is a promising transparent conducting oxide (TCO) because its components are naturally abundant and inexpensive; and ZnO can be synthesized by several methods as thin films and nanostructures. Doping ZnO with Al (to form what is called AZO) significantly increases electrical conductivity while retaining high optical transparency, making AZO ideal for use as transparent electrodes in optoelectronic devices. However, the electrical conductivity of AZO has not exceeded that of indium tin oxide (ITO), the most widely-utilized TCO. A systematic study of bulk and local electrical and optical properties of AZO is needed to improve conductivity while maintaining transparency. To this end, we conducted bulk magnetotransport measurements on AZO, which indicated that its electron mobility was significantly lower than that of single-crystal ZnO, primarily due to electron scattering at AZO grain boundaries. To further understand this detrimental effect, we directly probed these grain boundaries with a scanning tunneling microscope. These measurements are the first investigation of a broad spectrum of grain boundary traps in AZO, which include shallow states near the conduction band edge that may limit electron mobility, and deeper states that may deplete carriers. Because optical properties can affect transparency in devices, we characterized AZO through a combination of photoluminescence and scanning tunneling microscope cathodoluminescence (STM-CL). STM-CL, which probes only the surface, shows a dramatic narrowing of emission lines compared to bulk photoluminescence. We attribute this to different charge states of oxygen vacancies preferentially located near the surface. This observed difference is especially of interest in understanding transport across interfaces. Finally, we present one application of AZO: a monolayer quantum dot (QD) light-emitting device with AZO electrodes that uses atomic layer deposited insulating oxide to fill the interstices among QDs. This

  15. Strain localization parameters of AlCu4MgSi processed by high-energy electron beams

    SciTech Connect

    Lunev, A. G. Nadezhkin, M. V.; Konovalov, S. V.; Teresov, A. D.

    2015-10-27

    The influence of the electron beam surface treatment of AlCu4MgSi on the strain localization parameters and on the critical strain value of the Portevin–Le Chatelier effect has been considered. The strain localization parameters were measured using speckle imaging of the specimens subjected to the constant strain rate uniaxial tension at a room temperature. Impact of the surface treatment on the Portevin–Le Chatelier effect has been investigated.

  16. Quantitative imaging reveals real-time Pou5f3–Nanog complexes driving dorsoventral mesendoderm patterning in zebrafish

    PubMed Central

    Perez-Camps, Mireia; Tian, Jing; Chng, Serene C; Sem, Kai Pin; Sudhaharan, Thankiah; Teh, Cathleen; Wachsmuth, Malte; Korzh, Vladimir; Ahmed, Sohail; Reversade, Bruno

    2016-01-01

    Formation of the three embryonic germ layers is a fundamental developmental process that initiates differentiation. How the zebrafish pluripotency factor Pou5f3 (homologous to mammalian Oct4) drives lineage commitment is unclear. Here, we introduce fluorescence lifetime imaging microscopy and fluorescence correlation spectroscopy to assess the formation of Pou5f3 complexes with other transcription factors in real-time in gastrulating zebrafish embryos. We show, at single-cell resolution in vivo, that Pou5f3 complexes with Nanog to pattern mesendoderm differentiation at the blastula stage. Later, during gastrulation, Sox32 restricts Pou5f3–Nanog complexes to the ventrolateral mesendoderm by binding Pou5f3 or Nanog in prospective dorsal endoderm. In the ventrolateral endoderm, the Elabela / Aplnr pathway limits Sox32 levels, allowing the formation of Pou5f3–Nanog complexes and the activation of downstream BMP signaling. This quantitative model shows that a balance in the spatiotemporal distribution of Pou5f3–Nanog complexes, modulated by Sox32, regulates mesendoderm specification along the dorsoventral axis. DOI: http://dx.doi.org/10.7554/eLife.11475.001 PMID:27684073

  17. Local electronic structure and ferromagnetic interaction in La(Co,Ni)O3

    NASA Astrophysics Data System (ADS)

    Huang, Meng-Jie; Nagel, Peter; Fuchs, Dirk; von Loehneysen, Hilbert; Merz, Michael; Schuppler, Stefan

    Perovskite-related transition-metal oxides exhibit a wide range of properties from insulating to superconducting as well as many peculiar magnetic phases, and cobaltites, in particular, have been known for their proximity to spin-state transitions. How this changes with partial substitution by Ni is the topic of the present study. The local electronic structure and the ferromagnetic interaction in La(Co1-xNix) O3 has been studied by x-ray absorption (XAS) and x-ray magnetic circular dichroism (XMCD). XAS clearly indicates a mixed-valence state for both Co and Ni, with both valences changing systematically with Ni content, x. While the gradual spin-state transition of Co3+ from low-spin (LS) to high-spin (HS) is preserved for low x it is suppressed in the high Ni-content samples. Regarding the spin configuration of Ni we find it stabilized in a ``mixed'' spin state, unlike the purely LS state of Ni in LaNiO3. XMCD identifies the element-specific contributions to the magnetic moment and interactions. In particular, we find that it must be the coexistence of the HS state in both Co3+ and Ni3 + that induces t2 g-based ferromagnetic interaction via the double-exchange mechanism.

  18. Graphene Tunable Transparency to Tunneling Electrons: A Direct Tool To Measure the Local Coupling.

    PubMed

    González-Herrero, Héctor; Pou, Pablo; Lobo-Checa, Jorge; Fernández-Torre, Delia; Craes, Fabian; Martínez-Galera, Antonio J; Ugeda, Miguel M; Corso, Martina; Ortega, J Enrique; Gómez-Rodríguez, José M; Pérez, Rubén; Brihuega, Iván

    2016-05-24

    The local interaction between graphene and a host substrate strongly determines the actual properties of the graphene layer. Here we show that scanning tunneling microscopy (STM) can selectively help to visualize either the graphene layer or the substrate underneath, or even both at the same time, providing a comprehensive picture of this coupling with atomic precision and high energy resolution. We demonstrate this for graphene on Cu(111). Our spectroscopic data show that, in the vicinity of the Fermi level, graphene π bands are well preserved presenting a small n-doping induced by Cu(111) surface state electrons. Such results are corroborated by Angle-Resolved Photoemission Spectra (ARPES) and Density Functional Theory with van der Waals (DFT + vdW) calculations. Graphene tunable transparency also allows the investigation of the interaction between the substrate and foreign species (such as atomic H or C vacancies) on the graphene layer. Our calculations explain graphene tunable transparency in terms of the rather different decay lengths of the graphene Dirac π states and the metal surface state, suggesting that it should apply to a good number of graphene/substrate systems.

  19. Edge states and local electronic structure around an adsorbed impurity in a topological superconductor

    NASA Astrophysics Data System (ADS)

    Tai, Yuan-Yen; Choi, Hongchul; Ahmed, Towfiq; Ting, C. S.; Zhu, Jian-Xin

    2015-11-01

    Recently, topological superconducting states have attracted much interest. In this paper, we consider a topological superconductor with Z2 topological mirror order [Y.-Y. Tai et al., Phys. Rev. B 91, 041111(R) (2015), 10.1103/PhysRevB.91.041111] and s±-wave superconducting pairing symmetry, within a two-orbital model originally designed for iron-based superconductivity [Y.-Y. Tai et al., Europhys. Lett. 103, 67001 (2013), 10.1209/0295-5075/103/67001]. We predict the existence of gapless edge states. We also study the local electronic structure around an adsorbed interstitial magnetic impurity in the system, and find the existence of low-energy in-gap bound states even with a weak spin polarization on the impurity. We also discuss the relevance of our results to a recent scanning tunneling microscopy experiment on a Fe(Te,Se) compound with an adsorbed Fe impurity [J.-X. Yin et al., Nat. Phys. 11, 543 (2015), 10.1038/nphys3371], for which our density functional calculations show the Fe impurity is spin polarized.

  20. Local sample thickness determination via scanning transmission electron microscopy defocus series.

    PubMed

    Beyer, A; Straubinger, R; Belz, J; Volz, K

    2016-05-01

    The usable aperture sizes in (scanning) transmission electron microscopy ((S)TEM) have significantly increased in the past decade due to the introduction of aberration correction. In parallel with the consequent increase of convergence angle the depth of focus has decreased severely and optical sectioning in the STEM became feasible. Here we apply STEM defocus series to derive the local sample thickness of a TEM sample. To this end experimental as well as simulated defocus series of thin Si foils were acquired. The systematic blurring of high resolution high angle annular dark field images is quantified by evaluating the standard deviation of the image intensity for each image of a defocus series. The derived dependencies exhibit a pronounced maximum at the optimum defocus and drop to a background value for higher or lower values. The full width half maximum (FWHM) of the curve is equal to the sample thickness above a minimum thickness given by the size of the used aperture and the chromatic aberration of the microscope. The thicknesses obtained from experimental defocus series applying the proposed method are in good agreement with the values derived from other established methods. The key advantages of this method compared to others are its high spatial resolution and that it does not involve any time consuming simulations.

  1. Platypus Pou5f1 reveals the first steps in the evolution of trophectoderm differentiation and pluripotency in mammals.

    PubMed

    Niwa, Hitoshi; Sekita, Yoko; Tsend-Ayush, Enkhjargal; Grützner, Frank

    2008-01-01

    Uterine nourishment of embryos by the placenta is a key feature of mammals. Although a variety of placenta types exist, they are all derived from the trophectoderm (TE) cell layer of the developing embryo. Egg-laying mammals (platypus and echidnas) are distinguished by a very short intrauterine embryo development, in which a simple placenta forms from TE-like cells. The Pou5f1 gene encodes a class V POU family transcription factor Oct3/4. In mice, Oct3/4 together with the highly conserved caudal-related homeobox transcription factor Cdx2, determines TE fate in pre-implantation development. In contrast to Cdx2, Pou5f1 has only been identified in eutherian mammals and marsupials, whereas, in other vertebrates, pou2 is considered to be the Pou5f1 ortholog. Here, we show that platypus and opossum genomes contain a Pou5f1 and pou2 homolog, pou2-related, indicating that these two genes are paralogues and arose by gene duplication in early mammalian evolution. In a complementation assay, we found that platypus or human Pou5f1, but not opossum or zebrafish pou2, restores self-renewal in Pou5f1-null mouse ES cells, showing that platypus possess a fully functional Pou5f1 gene. Interestingly, we discovered that parts of one of the conserved regions (CR4) is missing from the platypus Pou5f1 promoter, suggesting that the autoregulation and reciprocal inhibition between Pou5f1 and Cdx2 evolved after the divergence of monotremes and may be linked to the development of more elaborate placental types in marsupial and eutherian mammals.

  2. Characterizing the Locality of Diabatic States forElectronic Excitation Transfer By Decomposing theDiabatic Coupling

    SciTech Connect

    Newton, M.D.; Vura-Weis, J.; Wasielewski, M.R.; Subotnik, J.E.

    2010-10-19

    A common strategy to calculate electronic coupling matrix elements for charge or energy transfer is to take the adiabatic states generated by electronic structure computations and rotate them to form localized diabatic states. In this paper, we show that, for intermolecular transfer of singlet electronic excitation, usually we cannot fully localize the electronic excitations in this way. Instead, we calculate putative initial and final states with small excitation tails caused by weak interactions with high energy excited states in the electronic manifold. These tails do not lead to substantial changes in the total diabatic coupling between states, but they do lead to a different partitioning of the total coupling between Coulomb (Forster), exchange (Dexter), and one-electron components. The tails may be reduced by using a multistate diabatic model or eliminated entirely by truncation (denoted as 'chopping'). Without more information, we are unable to conclude with certainty whether the observed diabatic tails are a physical reality or a computational artifact. This research suggests that decomposition of the diabatic coupling between chromophores into Coulomb, exchange, and one-electron components may depend strongly on the number of states considered, and such results should be treated with caution.

  3. Hyperglycemia induces apoptosis and p53 mobilization to mitochondria in RINm5F cells.

    PubMed

    Ortega-Camarillo, C; Guzmán-Grenfell, A M; García-Macedo, R; Rosales-Torres, A M; Avalos-Rodríguez, A; Durán-Reyes, G; Medina-Navarro, R; Cruz, M; Díaz-Flores, M; Kumate, J

    2006-01-01

    The mechanisms related to hyperglycemia-induced pancreatic beta-cell apoptosis are poorly defined. Rat insulin-producing cells (RINm5F) cultured in high glucose concentrations (30 mM) showed increased apoptosis and protein p53 translocation to mitochondria. In addition, hyperglycemia induced both the disruption of mitochondrial membrane potential (Delta psi (m)), and an increase in reactive oxygen species (ROS), as shown by fluorescence changes of JC-1 and dichlorodihydrofluorescein-diacetate (DCDHF-DA), respectively. The increased intracellular ROS by high glucose exposure was blunted by mitochondrial-function and NADPH-oxidase inhibitors. We postulate that the concomitant mobilization of p53 protein to the mitochondria and the subsequent changes on the Delta psi (m), lead to an important pancreatic beta-cell apoptosis mechanism induced by oxidative stress caused by hyperglycemia.

  4. Acute intoxication caused by synthetic cannabinoids 5F-ADB and MMB-2201: A case series.

    PubMed

    Barceló, Bernardino; Pichini, Simona; López-Corominas, Victoria; Gomila, Isabel; Yates, Christopher; Busardò, Francesco Paolo; Pellegrini, Manuela

    2017-04-01

    Synthetic cannabinoids are relatively new substances of abuse. Recently, abuse of synthetic cannabinoids has been increasingly reported in the lay press and medical literature. When new compounds are introduced, their use is initially not restricted by prohibition therefore their consumption cannot be verified by standard drug tests. The use of these compounds among adolescents and young adults is constantly growing, making it important for emergency services to be familiar with the signs and symptoms of intoxication present. Overdose and chronic use of these substances can cause adverse effects including altered mental status, tachycardia, and loss of consciousness. Here, we report five cases of acute intoxication by synthetic cannabinoids 5F-ADB and MMB-2201 with analytical confirmation.

  5. Self-Assembly of Hexanuclear Clusters of 4f and 5f Elements with Cation Specificity

    SciTech Connect

    Diwu, J.; Good, Justin J.; DiStefano, Victoria H.; Albrecht-Schmitt, Thomas E.

    2011-02-10

    Six hexanuclear clusters of 4f and 5f elements were synthesized by room-temperature slow concentration experiments. Cerium(IV), thorium(IV), and plutonium(IV) each form two different hexanuclear clusters, among which the cerium and plutonium clusters are isotypic, whereas the thorium clusters show more diversity. The change in ionic radii of approximately 0.08 Å between these different metal ions tunes the cavity size so that NH{sub 4}{sup +} (1.48 Å) has the right dimensions to assemble the cerium and plutonium clusters, whereas Cs{sup +} (1.69 Å) is necessary to assemble the thorium clusters. If these cations are not used in the reactions, only amorphous material is obtained.

  6. Structure of the parainfluenza virus 5 F protein in its metastable, prefusion conformation

    SciTech Connect

    Yin, Hsien-Sheng; Wen, Xiaolin; Paterson, Reay G.; Lamb, Robert A.; Jardetzky, Theodore S.

    2010-03-08

    Enveloped viruses have evolved complex glycoprotein machinery that drives the fusion of viral and cellular membranes, permitting entry of the viral genome into the cell. For the paramyxoviruses, the fusion (F) protein catalyses this membrane merger and entry step, and it has been postulated that the F protein undergoes complex refolding during this process. Here we report the crystal structure of the parainfluenza virus 5 F protein in its prefusion conformation, stabilized by the addition of a carboxy-terminal trimerization domain. The structure of the F protein shows that there are profound conformational differences between the pre- and postfusion states, involving transformations in secondary and tertiary structure. The positions and structural transitions of key parts of the fusion machinery, including the hydrophobic fusion peptide and two helical heptad repeat regions, clarify the mechanism of membrane fusion mediated by the F protein.

  7. Propagation of localized structures in relativistic magnetized electron-positron plasmas using particle-in-cell simulations

    SciTech Connect

    López, Rodrigo A.; Muñoz, Víctor; Viñas, Adolfo F.; Valdivia, Juan A.

    2015-09-15

    We use a particle-in-cell simulation to study the propagation of localized structures in a magnetized electron-positron plasma with relativistic finite temperature. We use as initial condition for the simulation an envelope soliton solution of the nonlinear Schrödinger equation, derived from the relativistic two fluid equations in the strongly magnetized limit. This envelope soliton turns out not to be a stable solution for the simulation and splits in two localized structures propagating in opposite directions. However, these two localized structures exhibit a soliton-like behavior, as they keep their profile after they collide with each other due to the periodic boundary conditions. We also observe the formation of localized structures in the evolution of a spatially uniform circularly polarized Alfvén wave. In both cases, the localized structures propagate with an amplitude independent velocity.

  8. Dimensional crossover of electron weak localization in ZnO/TiOx stacked layers grown by atomic layer deposition

    NASA Astrophysics Data System (ADS)

    Saha, D.; Misra, P.; Bhartiya, S.; Gupta, M.; Joshi, M. P.; Kukreja, L. M.

    2016-01-01

    We report on the dimensional crossover of electron weak localization in ZnO/TiOx stacked layers having well-defined and spatially-localized Ti dopant profiles along film thickness. These films were grown by in situ incorporation of sub-monolayer TiOx on the growing ZnO film surface and subsequent overgrowth of thin conducting ZnO spacer layer using atomic layer deposition. Film thickness was varied in the range of ˜6-65 nm by vertically stacking different numbers (n = 1-7) of ZnO/TiOx layers of nearly identical dopant-profiles. The evolution of zero-field sheet resistance (R⊙) versus temperature with decreasing film thickness showed a metal to insulator transition. On the metallic side of the metal-insulator transition, R⊙(T) and magnetoresistance data were found to be well corroborated with the theoretical framework of electron weak localization in the diffusive transport regime. The temperature dependence of both R⊙ and inelastic scattering length provided strong evidence for a smooth crossover from 2D to 3D weak localization behaviour. Results of this study provide deeper insight into the electron transport in low-dimensional n-type ZnO/TiOx stacked layers which have potential applications in the field of transparent oxide electronics.

  9. Quantum Monte Carlo study of the itinerant-localized model of strongly correlated electrons: Spin-spin correlation functions

    NASA Astrophysics Data System (ADS)

    Ivantsov, Ilya; Ferraz, Alvaro; Kochetov, Evgenii

    2016-12-01

    We perform quantum Monte Carlo simulations of the itinerant-localized periodic Kondo-Heisenberg model for the underdoped cuprates to calculate the associated spin correlation functions. The strong electron correlations are shown to play a key role in the abrupt destruction of the quasi-long-range antiferromagnetic order in the lightly doped regime.

  10. A 1.5 THz hot-electron bolometer mixer operated by a planar diode based local oscillator

    NASA Technical Reports Server (NTRS)

    Tong, C. Y. E.; Meledin, D.; Blundell, R.; Erickson, N.; Mehdi, I.; Goltsman, G.

    2003-01-01

    We have developed a 1.5 THz superconducting NbN Hot-Electron Bolometer mixer. It is oprated by an all-solid-state Local Oscillator comprising of a cascade of 4 planar doublers following an MMIC based W-band power amplifier.

  11. Strong impact of lattice vibrations on electronic and magnetic properties of paramagnetic Fe revealed by disordered local moments molecular dynamics

    NASA Astrophysics Data System (ADS)

    Alling, B.; Körmann, F.; Grabowski, B.; Glensk, A.; Abrikosov, I. A.; Neugebauer, J.

    2016-06-01

    We study the impact of lattice vibrations on magnetic and electronic properties of paramagnetic bcc and fcc iron at finite temperature, employing the disordered local moments molecular dynamics (DLM-MD) method. Vibrations strongly affect the distribution of local magnetic moments at finite temperature, which in turn correlates with the local atomic volumes. Without the explicit consideration of atomic vibrations, the mean local magnetic moment and mean field derived magnetic entropy of paramagnetic bcc Fe are larger compared to paramagnetic fcc Fe, which would indicate that the magnetic contribution stabilizes the bcc phase at high temperatures. In the present study we show that this assumption is not valid when the coupling between vibrations and magnetism is taken into account. At the γ -δ transition temperature (1662 K), the lattice distortions cause very similar magnetic moments of both bcc and fcc structures and hence magnetic entropy contributions. This finding can be traced back to the electronic densities of states, which also become increasingly similar between bcc and fcc Fe with increasing temperature. Given the sensitive interplay of the different physical excitation mechanisms, our results illustrate the need for an explicit consideration of vibrational disorder and its impact on electronic and magnetic properties to understand paramagnetic Fe. Furthermore, they suggest that at the γ -δ transition temperature electronic and magnetic contributions to the Gibbs free energy are extremely similar in bcc and fcc Fe.

  12. Electron localization of {{{\\rm{H}}}_{3}}^{+} and {{\\rm{HeH}}}^{2+} in an ultrashort ultraviolet laser field

    NASA Astrophysics Data System (ADS)

    Jia, Z. M.; Tang, W. T.; Zeng, Z. N.; Li, R. X.; Xu, Z. Z.

    2017-02-01

    Electron localization in the dissociation of the molecular ions {{{{H}}}3}+ and HeH2+ in an intense ultrashort ultraviolet laser pulse is studied with the Schrödinger equation. Two different dissociation channels, {{{{H}}}3}+ + nγ → H2 + p and {{{{H}}}3}+ + nγ → {{{{H}}}2}++ H, and HeH2+ + nγ → He+ + p and HeH2+ + nγ → α + H, for {{{{H}}}3}+ and HeH2+, are investigated, respectively. The numerical and analytical results both show that, for a molecular ion with an asymmetric double-well Coulomb potential, most electrons of the 1s{σ }g state are localized at the potential well with lower energies. For electrons of the 2p{σ }u state, most are localized at the potential well with higher energies when in a single ultraviolet laser pulse. Therefore, for {{{{H}}}3}+, most electrons of the dissociation state are stabilized at the potential well with higher energies (H+), for the lowest dissociation state is the 2p{σ }u state. Most of the electrons of the dissociation state of HeH2+ are captured by the potential well with lower energies (He2+), because the lowest dissociation state is the 1s{σ }g state and the 2p{σ }u state is bounded.

  13. Electron-beam-induced deposition and post-treatment processes to locally generate clean titanium oxide nanostructures on Si(100).

    PubMed

    Schirmer, M; Walz, M-M; Vollnhals, F; Lukasczyk, T; Sandmann, A; Chen, C; Steinrück, H-P; Marbach, H

    2011-02-25

    We have investigated the lithographic generation of TiO(x) nanostructures on Si(100) via electron-beam-induced deposition (EBID) of titanium tetraisopropoxide (TTIP) in ultra-high vacuum (UHV) by scanning electron microscopy (SEM) and local Auger electron spectroscopy (AES). In addition, the fabricated nanostructures were also characterized ex situ via atomic force microscopy (AFM) under ambient conditions. In EBID, a highly focused electron beam is used to locally decompose precursor molecules and thereby to generate a deposit. A drawback of this nanofabrication technique is the unintended deposition of material in the vicinity of the impact position of the primary electron beam due to so-called proximity effects. Herein, we present a post-treatment procedure to deplete the unintended deposits by moderate sputtering after the deposition process. Moreover, we were able to observe the formation of pure titanium oxide nanocrystals (<100 nm) in situ upon heating the sample in a well-defined oxygen atmosphere. While the nanocrystal growth for the as-deposited structures also occurs in the surroundings of the irradiated area due to proximity effects, it is limited to the pre-defined regions, if the sample was sputtered before heating the sample under oxygen atmosphere. The described two-step post-treatment procedure after EBID presents a new pathway for the fabrication of clean localized nanostructures.

  14. Electron-beam-induced deposition and post-treatment processes to locally generate clean titanium oxide nanostructures on Si(100)

    NASA Astrophysics Data System (ADS)

    Schirmer, M.; Walz, M.-M.; Vollnhals, F.; Lukasczyk, T.; Sandmann, A.; Chen, C.; Steinrück, H.-P.; Marbach, H.

    2011-02-01

    We have investigated the lithographic generation of TiOx nanostructures on Si(100) via electron-beam-induced deposition (EBID) of titanium tetraisopropoxide (TTIP) in ultra-high vacuum (UHV) by scanning electron microscopy (SEM) and local Auger electron spectroscopy (AES). In addition, the fabricated nanostructures were also characterized ex situ via atomic force microscopy (AFM) under ambient conditions. In EBID, a highly focused electron beam is used to locally decompose precursor molecules and thereby to generate a deposit. A drawback of this nanofabrication technique is the unintended deposition of material in the vicinity of the impact position of the primary electron beam due to so-called proximity effects. Herein, we present a post-treatment procedure to deplete the unintended deposits by moderate sputtering after the deposition process. Moreover, we were able to observe the formation of pure titanium oxide nanocrystals (<100 nm) in situ upon heating the sample in a well-defined oxygen atmosphere. While the nanocrystal growth for the as-deposited structures also occurs in the surroundings of the irradiated area due to proximity effects, it is limited to the pre-defined regions, if the sample was sputtered before heating the sample under oxygen atmosphere. The described two-step post-treatment procedure after EBID presents a new pathway for the fabrication of clean localized nanostructures.

  15. Local atomic and electronic structure in LaMnO{sub 3} across the orbital ordering transition

    SciTech Connect

    Souza, Raquel A.; Souza-Neto, Narcizo M.; Ramos, Aline Y.; Tolentino, Helio C.N.; Granado, Eduardo

    2004-12-01

    The local atomic disorder and electronic structure in the environment of manganese atoms in LaMnO{sub 3} has been studied by x-ray absorption spectroscopy over a temperature range (300-870 K) covering the orbital ordering transition ({approx}710 K). The Mn-O distance splitting into short and long bonds (1.95 and 2.15 A) is kept across the transition temperature, so that the MnO{sub 6} octahedra remain locally Jahn-Teller distorted. Discontinuities in the Mn local structure are identified in the extended x-ray fine structure spectra at this temperature, associated with a reduction of the disorder in the superexchange angle and to the removal of the anisotropy in the radial disorder within the coordination shell. Subtle changes in the electronic local structure also take place at the Mn site at the transition temperature. The near-edge spectra show a small drop of the Mn 4p hole count and a small enhancement in the pre-edge structures at the transition temperature. These features are associated with an increase of the covalence of the Mn-O bonds. Our results shed light on the local electronic and structural phenomena in a model of order-disorder transition, where the cooperative distortion is overcome by the thermal disorder.

  16. Molecular dipole static polarisabilities and hyperpolarisabilities of conjugated oligomer chains calculated with the local π-electron coupled cluster theory

    NASA Astrophysics Data System (ADS)

    Ivanov, Vladimir V.; Zakharov, Anton B.; Adamowicz, Ludwik

    2013-12-01

    A new semi-empirical π-electron local coupled cluster theory has been developed to calculate static dipole polarisabilities and hyperpolarisabilities of extended π-conjugated systems. The key idea of the approach is the use of the ethylene molecular orbitals as the orbital basis set for π-conjugated compounds (the method is termed the Covalent Unbonded Molecules of Ethylene method, cue). Test calculations of some small model organic conjugated compounds demonstrate high accuracy of the version of the cue local coupled cluster theory developed in this work in comparison with the π-electron full configuration interaction (FCI) method. Calculations of different conjugated carbon-based oligomer chains (polyenes, polyynes, polyacenes, polybenzocyclobutadiene, etc.) demonstrate fast convergence (per π-electron) of the polarisability and hyperpolarisability values in the calculations when more classes of orbital excitations are included in the coupled cluster single and double (CCSD) excitation operator. The results show qualitatively correct dependence on the system size.

  17. Characterization of the local crystallinity via reflectance of very slow electrons

    SciTech Connect

    Pokorna, Z.; Mikmekova, S.; Muellerova, I.; Frank, L.

    2012-06-25

    The reflectance of very slow electrons from solids and its electron energy dependence are shown as characteristic for the crystal system and its spatial orientation so they can serve, e.g., to fingerprinting the orientation of grains in polycrystals. Measurements on single crystals and polycrystals are validated via electron backscatter diffraction analyses. Sensitivity of the method to fine details of crystallinity is demonstrated.

  18. Long-term results of intraoperative electron beam radiation therapy for nonmetastatic locally advanced pancreatic cancer

    PubMed Central

    Chen, Yingtai; Che, Xu; Zhang, Jianwei; Huang, Huang; Zhao, Dongbing; Tian, Yantao; Li, Yexiong; Feng, Qinfu; Zhang, Zhihui; Jiang, Qinglong; Zhang, Shuisheng; Tang, Xiaolong; Huang, Xianghui; Chu, Yunmian; Zhang, Jianghu; Sun, Yuemin; Zhang, Yawei; Wang, Chengfeng

    2016-01-01

    Abstract To assess prognostic benefits of intraoperative electron beam radiation therapy (IOERT) in patients with nonmetastatic locally advanced pancreatic cancer (LAPC) and evaluate optimal adjuvant treatment after IOERT. A retrospective cohort study using prospectively collected data was conducted at the Cancer Hospital of the Chinese Academy of Medical Sciences, China National Cancer Center. Two hundred forty-seven consecutive patients with nonmetastatic LAPC who underwent IOERT between January 2008 and May 2015 were identified and included in the study. Overall survival (OS) was calculated from the day of IOERT. Prognostic factors were examined using Cox proportional hazards models. The 1-, 2-, and 3-year actuarial survival rates were 40%, 14%, and 7.2%, respectively, with a median OS of 9.0 months. On multivariate analysis, an IOERT applicator diameter < 6 cm (hazards ratio [HR], 0.67; 95% confidence interval [CI], 0.47–0.97), no intraoperative interstitial sustained-release 5-fluorouracil chemotherapy (HR, 0.46; 95% CI, 0.32–0.66), and receipt of postoperative chemoradiotherapy followed by chemotherapy (HR, 0.11; 95% CI, 0.04–0.25) were significantly associated with improved OS. Pain relief after IOERT was achieved in 111 of the 117 patients, with complete remission in 74 and partial remission in 37. Postoperative complications rate and mortality were 14.0% and 0.4%, respectively. Nonmetastatic LAPC patients with smaller size tumors could achieve positive long-term survival outcomes with a treatment strategy incorporating IOERT and postoperative adjuvant treatment. Chemoradiotherapy followed by chemotherapy might be a recommended adjuvant treatment strategy for well-selected cases. Intraoperative interstitial sustained-release 5-fluorouracil chemotherapy should not be recommended for patients with nonmetastatic LAPC. PMID:27661028

  19. Safe and Simplified Salvage Technique for Exposed Implantable Cardiac Electronic Devices under Local Anesthesia

    PubMed Central

    Jung, Chang Young; Kim, Sung-Eun

    2017-01-01

    Background Skin erosion is a dire complication of implantable cardiac pacemakers and defibrillators. Classical treatments involve removal of the entire generator and lead systems, however, these may result in fatal complications. In this study, we present our experience with a simplified salvage technique for exposed implantable cardiac electronic devices (ICEDs) without removing the implanted device, in an attempt to reduce the risks and complication rates associated with this condition. Methods The records of 10 patients who experienced direct ICED exposure between January 2012 and December 2015 were retrospectively reviewed. The following surgical procedure was performed in all patients: removal of skin erosion and capsule, creation of a new pocket at least 1.0–1.5 cm inferior to its original position, migration of the ICED to the new pocket, and insertion of closed-suction drainage. Patients with gross local sepsis or septicemia were excluded from this study. Results Seven patients had cardiac pacemakers and the other 3 had implantable cardiac defibrillators. The time from primary ICED placement to exposure ranged from 0.3 to 151 months (mean, 29 months. Postoperative follow-up in this series ranged from 8 to 31 months (mean follow-up, 22 months). Among the 10 patients, none presented with any signs of overt infection or cutaneous lesions, except 1 patient with hematoma on postoperative day 5. The hematoma was successfully treated by surgical removal and repositioning of the closed-suction drainage. Conclusions Based on our experience, salvage of exposed ICEDs is possible without removing the device in selected patients. PMID:28194346

  20. Station Based Polynomial Modeling of the local ionospheric Vertical Total Electron Content (VTEC) using Particle Filter

    NASA Astrophysics Data System (ADS)

    Erdogan, Eren; Onur Karslioglu, Mahmut; Durmaz, Murat; Aghakarimi, Armin

    2014-05-01

    parameters, Ionospheric VTEC map covering the predefined region has been produced by interpolation. VTEC values at a grid node of the map have been computed based on the four closest ground stations by means of inverse distance squared weighted average. The GPS data which is acquired from ground based stations have been made available from the International GNSS Service (IGS) and the Reference Frame Sub-commission for Europe (EUREF). Raw GPS observations have been preprocessed to detect cycle slips and to form geometry-free linear combinations of observables for each continuous arc. Then the obtained pseudoranges have been smoothed with the carrier to code leveling method. Finally, the performance of the particle filter to investigate the local characteristics of the ionospheric Vertical Total Electron Content (VTEC) has been evaluated and the result has been compared with the result of a standard Kalman filter. Keywords: ionosphere, GPS , Particle filer, VTEC modeling

  1. A Theoretical Study of NO2 Complexes with Aluminium and Gallium Based on Topological Analysis of Electron Density and Electron Localization Function

    SciTech Connect

    Panek, Jaroslaw; Latajaka, Zdzislaw

    2000-12-26

    Results of DFT and MP4 calculations on AlNO2 and GaNO2 molecules are presented. One Cs and two C2v structures (two minima and one TS) are found and their energies and vibrational frequencies are reported and discussed. The minima are close in energy and lie ca. 70 kcal mol-1 below reactants (M+NO2). More insight is obtained via topological analysis of electron density and electron localization function (ELF). It is shown that the molecules are bound mainly via electrostatic interactions, and there is a significant charge transfer from metal atom to the NO2 moiety. Detailed analysis of the ELF shows that the loss of stability of gallium complexes with respect to aluminium structures is best explained by (antibonding) influence of gallium semi-cored electrons.

  2. Nonlinear simulations of peeling-ballooning modes with anomalous electron viscosity and their role in edge localized mode crashes

    SciTech Connect

    Xu, X. Q.; Dudson, B.; Snyder, P. B.; Umansky, M. V.; Wilson, H.

    2010-10-22

    A minimum set of equations based on the peeling-ballooning (P-B) model with nonideal physics effects (diamagnetic drift, E×B drift, resistivity, and anomalous electron viscosity) is found to simulate pedestal collapse when using the new BOUT++ simulation code, developed in part from the original fluid edge code BOUT. Nonlinear simulations of P-B modes demonstrate that the P-B modes trigger magnetic reconnection, which leads to the pedestal collapse. With the addition of a model of the anomalous electron viscosity under the assumption that the electron viscosity is comparable to the anomalous electron thermal diffusivity, it is found from simulations using a realistic high-Lundquist number that the pedestal collapse is limited to the edge region and the edge localized mode (ELM) size is about 5–10% of the pedestal stored energy. Furthermore, this is consistent with many observations of large ELMs.

  3. Nonlinear simulations of peeling-ballooning modes with anomalous electron viscosity and their role in edge localized mode crashes

    DOE PAGES

    Xu, X. Q.; Dudson, B.; Snyder, P. B.; ...

    2010-10-22

    A minimum set of equations based on the peeling-ballooning (P-B) model with nonideal physics effects (diamagnetic drift, E×B drift, resistivity, and anomalous electron viscosity) is found to simulate pedestal collapse when using the new BOUT++ simulation code, developed in part from the original fluid edge code BOUT. Nonlinear simulations of P-B modes demonstrate that the P-B modes trigger magnetic reconnection, which leads to the pedestal collapse. With the addition of a model of the anomalous electron viscosity under the assumption that the electron viscosity is comparable to the anomalous electron thermal diffusivity, it is found from simulations using a realisticmore » high-Lundquist number that the pedestal collapse is limited to the edge region and the edge localized mode (ELM) size is about 5–10% of the pedestal stored energy. Furthermore, this is consistent with many observations of large ELMs.« less

  4. Local electron tomography using angular variations of surface tangents: Stomo version 2

    NASA Astrophysics Data System (ADS)

    Petersen, T. C.; Ringer, S. P.

    2012-03-01

    . Program summaryProgram title: STOMO version 2 Catalogue identifier: AEFS_v2_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AEFS_v2_0.html Program obtainable from: CPC Program Library, Queen's University, Belfast, N. Ireland Licensing provisions: Standard CPC licence, http://cpc.cs.qub.ac.uk/licence/licence.html No. of lines in distributed program, including test data, etc.: 2854 No. of bytes in distributed program, including test data, etc.: 23 559 Distribution format: tar.gz Programming language: C/C++ Computer: PC Operating system: Windows XP RAM: Scales as the product of experimental image dimensions multiplied by the number of points chosen by the user in polynomial fitting. Typical runs require between 50 Mb and 100 Mb of RAM. Supplementary material: Sample output files, for the test run provided, are available. Classification: 7.4, 14 Catalogue identifier of previous version: AEFS_v1_0 Journal reference of previous version: Comput. Phys. Comm. 181 (2010) 676 Does the new version supersede the previous version?: Yes Nature of problem: A local electron tomography algorithm of specimens for which conventional back projection may fail and or data for which there is a limited angular range (which would otherwise cause significant 'missing-wedge' artefacts). The algorithm does not solve the tomography back projection problem but rather locally reconstructs the 3D morphology of surfaces defined by varied scattering densities. Solution method: Local reconstruction is effected using image-analysis edge and ridge detection computations on experimental tilt series to measure smooth angular variations of surface tangent-line intersections, which generate point clouds decorating the embedded and or external scattering surfaces of a specimen. Reasons for new version: The new version was coded to cater for rectangular images in experimental tilt-series, ensure smoother image rotations, provide ridge detection (suitable for sensing phase-contrast Fresnel fringes and other

  5. Aryl Hydrocarbon Receptor Ligand 5F 203 Induces Oxidative Stress That Triggers DNA Damage in Human Breast Cancer Cells

    PubMed Central

    McLean, Lancelot S.; Watkins, Cheri N.; Campbell, Petreena; Zylstra, Dain; Rowland, Leah; Amis, Louisa H.; Scott, Lia; Babb, Crystal E.; Livingston, W. Joel; Darwanto, Agus; Davis, Willie L.; Senthil, Maheswari; Sowers, Lawrence C.; Brantley, Eileen

    2015-01-01

    Breast tumors often show profound sensitivity to exogenous oxidative stress. Investigational agent 2-(4-amino-3-methylphenyl)-5-fluorobenzothiazole (5F 203) induces aryl hydrocarbon receptor (AhR)-mediated DNA damage in certain breast cancer cells. Since AhR agonists often elevate intracellular oxidative stress, we hypothesize that 5F 203 increases reactive oxygen species (ROS) to induce DNA damage, which thwarts breast cancer cell growth. We found that 5F 203 induced single-strand break formation. 5F 203 enhanced oxidative DNA damage that was specific to breast cancer cells sensitive to its cytotoxic actions, as it did not increase oxidative DNA damage or ROS formation in nontumorigenic MCF-10A breast epithelial cells. In contrast, AhR agonist and procarcinogen benzo[a]pyrene and its metabolite, 1,6-benzo[a]pyrene quinone, induced oxidative DNA damage and ROS formation, respectively, in MCF-10A cells. In sensitive breast cancer cells, 5F 203 activated ROS-responsive kinases: c-Jun-N-terminal kinase (JNK) and p38 mitogen activated protein kinase (p38). AhR antagonists (alpha-naphthoflavone, CH223191) or antioxidants (N-acetyl-l-cysteine, EUK-134) attenuated 5F 203-mediated JNK and p38 activation, depending on the cell type. Pharmacological inhibition of AhR, JNK, or p38 attenuated 5F 203-mediated increases in intracellular ROS, apoptosis, and single-strand break formation. 5F 203 induced the expression of cytoglobin, an oxidative stress-responsive gene and a putative tumor suppressor, which was diminished with AhR, JNK, or p38 inhibition. Additionally, 5F 203-mediated increases in ROS production and cytoglobin were suppressed in AHR100 cells (AhR ligand-unresponsive MCF-7 breast cancer cells). Our data demonstrate 5F 203 induces ROS-mediated DNA damage at least in part via AhR, JNK, or p38 activation and modulates the expression of oxidative stress-responsive genes such as cytoglobin to confer its anticancer action. PMID:25781201

  6. Filamentation of laser beam and suppression of stimulated Raman scattering due to localization of electron plasma wave

    NASA Astrophysics Data System (ADS)

    Purohit, Gunjan; Sharma, Prerana; Sharma, R. P.

    2012-02-01

    This paper presents the effect of laser beam filamentation on the localization of electron plasma wave (EPW) and stimulated Raman scattering (SRS) in unmagnetized plasma when relativistic and ponderomotive nonlinearities are operative. The splitted profile of the laser beam is obtained due to uneven focusing of the off-axial rays. The semi-analytical solution of the nonlinearly coupled EPW equation in the presence of laser beam filaments has been found. It is observed that due to this nonlinear coupling between these two waves, localization of EPW takes place. Stimulated Raman scattering of this EPW is studied and back reflectivity has been calculated. Further, the localization of EPW affects the eigenfrequency and damping of plasma wave. The new enhanced damping of the plasma wave has been calculated and it is found that the SRS process gets suppressed due to the localization of plasma wave in laser beam filamentary structures.

  7. A practical approach to temperature effects in dissociative electron attachment cross sections using local complex potential theory

    NASA Astrophysics Data System (ADS)

    Sugioka, Yuji; Takayanagi, Toshiyuki

    2012-09-01

    We propose a practical computational scheme to obtain temperature dependence of dissociative electron attachment cross sections to polyatomic molecules within a local complex potential theory formalism. First we perform quantum path-integral molecular dynamics simulations on the potential energy surface for the neutral molecule in order to sample initial nuclear configurations as well as momenta. Classical trajectories are subsequently integrated on the potential energy surface for the anionic state and survival probabilities are simultaneously calculated along the obtained trajectories. We have applied this simple scheme to dissociative electron attachment processes to H2O and CF3Cl, for which several previous studies are available from both the experimental and theoretical sides.

  8. Electron Microscopy Localization and Characterization of Functionalized Composite Organic-Inorganic SERS Nanoparticles on Leukemia Cells

    PubMed Central

    Koh, Ai Leen; Shachaf, Catherine M.; Elchuri, Sailaja; Nolan, Garry P.; Sinclair, Robert

    2008-01-01

    We demonstrate the use of electron microscopy as a powerful characterization tool to identify and locate antibody-conjugated composite organic-inorganic (COINs) surface enhanced Raman scattering (SERS) nanoparticles on cells. U937 leukemia cells labeled with antibody CD54-conjugated COINs were characterized in their native, hydrated state using wet Scanning Electron Microscopy (SEM) and in their dehydrated state using high-resolution SEM. In both cases, the backscattered electron detector (BSE) was used to detect and identify the silver constituents in COINs due to its high sensitivity to atomic number variations within a specimen. The imaging and analytical capabilities in the SEM were further complemented by higher resolution Transmission Electron Microscope (TEM) images and Scanning Auger Electron Spectroscopy (AES) data to give reliable and high-resolution information about nanoparticles and their binding to cell surface antigens. PMID:18995965

  9. Local versus global electronic properties of chalcopyrite alloys: X-ray absorption spectroscopy and ab initio calculations

    SciTech Connect

    Sarmiento-Pérez, Rafael; Botti, Silvana; Schnohr, Claudia S.; Lauermann, Iver; Rubio, Angel; Johnson, Benjamin

    2014-09-07

    Element-specific unoccupied electronic states of Cu(In, Ga)S{sub 2} were studied as a function of the In/Ga ratio by combining X-ray absorption spectroscopy with density functional theory calculations. The S absorption edge shifts with changing In/Ga ratio as expected from the variation of the band gap. In contrast, the cation edge positions are largely independent of composition despite the changing band gap. This unexpected behavior is well reproduced by our calculations and originates from the dependence of the electronic states on the local atomic environment. The changing band gap arises from a changing spatial average of these localized states with changing alloy composition.

  10. Influence of cell physiological state on gene delivery to T lymphocytes by chimeric adenovirus Ad5F35

    PubMed Central

    Zhang, Wen-feng; Shao, Hong-wei; Wu, Feng-lin; Xie, Xin; Li, Zhu-Ming; Bo, Hua-Ben; Shen, Han; Wang, Teng; Huang, Shu-lin

    2016-01-01

    Adoptive transfer of genetically-modified T cells is a promising approach for treatment of both human malignancies and viral infections. Due to its ability to efficiently infect lymphocytes, the chimeric adenovirus Ad5F35 is potentially useful as an immunotherapeutic for the genetic modification of T cells. In previous studies, it was found that the infection efficiency of Ad5F35 was significantly increased without enhanced expression of the viral receptor after T cell stimulation; however, little is known about the underlying mechanism. Nonetheless, cell physiology has long been thought to affect viral infection. Therefore, we aimed to uncover the physiologic changes responsible for the increased infection efficiency of Ad5F35 following T cell stimulation. Given the complexity of intracellular transport we analyzed viral binding, entry, and escape using a Jurkat T cell model and found that both cell membrane fluidity and endosomal escape of Ad5F35 were altered under different physiological states. This, in turn, resulted in differences in the amount of virus entering cells and reaching the cytoplasm. These results provide additional insight into the molecular mechanisms underlying Ad5F35 infection of T cells and consequently, will help further the clinical application of genetically-modified T cells for immunotherapy. PMID:26972139

  11. Crossover from itinerant-electron to localized-electron behavior in Sr(1-x)Ca(x)CrO3 perovskite solid solution.

    PubMed

    Long, Youwen; Yang, Liuxiang; Lv, Yuxi; Liu, Qingqing; Jin, Changqing; Zhou, Jianshi; Goodenough, John B

    2011-09-07

    Polycrystalline samples of the perovskite family Sr(1-x)Ca(x)CrO(3) have been prepared at high pressure and temperature in steps of 1/6 over the range 0 ≤ x ≤ 1. Rietveld analysis shows a series of structural phase transitions from cubic to tetragonal to orthorhombic with increasing x. The cubic samples have no long-range magnetic order; the other samples become antiferromagnetically ordered below a T(N) that increases with x. At ambient pressure, the electric transport properties of the cubic and tetragonal phases are semiconducting with a small (meV range) activation energy that increases with x; the orthorhombic phase exhibits variable-range hopping rather than the small-polaron behavior typically found for mixed-valent, localized-electron configurations. Above a pressure P=P(C), a smooth insulator-metal transition is found at a T(IM) that decreases with increasing P for a fixed x; P(C) increases with x. These phenomena are rationalized qualitatively with a π(∗)-band model having a width W(π) that approaches crossover from itinerant-electron to localized-electron behavior as W(π) decreases with increasing x. The smaller size of the Ca(2+) ion induces the structural changes and the greater acidity of the Ca(2+) ion is primarily responsible for narrowing W(π) as x increases.

  12. Localized electron transfer rates and microelectrode-based enrichment of microbial communities within a phototrophic microbial mat

    PubMed Central

    Babauta, Jerome T.; Atci, Erhan; Ha, Phuc T.; Lindemann, Stephen R.; Ewing, Timothy; Call, Douglas R.; Fredrickson, James K.; Beyenal, Haluk

    2014-01-01

    Phototrophic microbial mats frequently exhibit sharp, light-dependent redox gradients that regulate microbial respiration on specific electron acceptors as a function of depth. In this work, a benthic phototrophic microbial mat from Hot Lake, a hypersaline, epsomitic lake located near Oroville in north-central Washington, was used to develop a microscale electrochemical method to study local electron transfer processes within the mat. To characterize the physicochemical variables influencing electron transfer, we initially quantified redox potential, pH, and dissolved oxygen gradients by depth in the mat under photic and aphotic conditions. We further demonstrated that power output of a mat fuel cell was light-dependent. To study local electron transfer processes, we deployed a microscale electrode (microelectrode) with tip size ~20 μm. To enrich a subset of microorganisms capable of interacting with the microelectrode, we anodically polarized the microelectrode at depth in the mat. Subsequently, to characterize the microelectrode-associated community and compare it to the neighboring mat community, we performed amplicon sequencing of the V1–V3 region of the 16S gene. Differences in Bray-Curtis beta diversity, illustrated by large changes in relative abundance at the phylum level, suggested successful enrichment of specific mat community members on the microelectrode surface. The microelectrode-associated community exhibited substantially reduced alpha diversity and elevated relative abundances of Prosthecochloris, Loktanella, Catellibacterium, other unclassified members of Rhodobacteraceae, Thiomicrospira, and Limnobacter, compared with the community at an equivalent depth in the mat. Our results suggest that local electron transfer to an anodically polarized microelectrode selected for a specific microbial population, with substantially more abundance and diversity of sulfur-oxidizing phylotypes compared with the neighboring mat community. PMID:24478768

  13. TiO2 nanotube arrays for photocatalysis: Effects of crystallinity, local order, and electronic structure

    SciTech Connect

    Liu, Jing; Hosseinpour, Pegah M.; Luo, Si; Heiman, Don; Menon, Latika; Arena, Dario A.; Lewis, Laura H.

    2014-11-19

    To furnish insight into correlations of electronic and local structure and photoactivity, arrays of short and long TiO₂ nanotubes were synthesized by electrochemical anodization of Ti foil, followed by thermal treatment in O₂ (oxidizing), Ar (inert), and H₂ (reducing) environments. The physical and electronic structures of these nanotubes were probed with x-ray diffraction, scanning electron microscopy, and synchrotron-based x-ray absorption spectroscopy, and correlated with their photocatalytic properties. The photocatalytic activity of the nanotubes was evaluated by monitoring the degradation of methyl orange under UV-VIS light irradiation. Results show that upon annealing at 350 °C all as-anodized amorphous TiO₂ nanotube samples partially transform to the anatase structure, with variations in the degree of crystallinity and in the concentration of local defects near the nanotubes' surface (~5 nm) depending on the annealing conditions. Degradation of methyl orange was not detectable for the as-anodized TiO₂ nanotubes regardless of their length. The annealed long nanotubes demonstrated detectable catalytic activity, which was more significant with the H₂-annealed nanotubes than with the Ar- and O₂-annealed nanotube samples. This enhanced photocatalytic response of the H₂-annealed long nanotubes relative to the other samples is positively correlated with the presence of a larger concentration of lattice defects (such as Ti3+ and anticipated oxygen vacancies) and a slightly lower degree of crystallinity near the nanotube surface. These physical and electronic structural attributes impact the efficacy of visible light absorption; moreover, the increased concentration of surface defects is postulated to promote the generation of hydroxyl radicals and thus accelerate the photodegradation of the methyl orange. The information obtained from this study provides unique insight into the role of the near-surface electronic and defect structure

  14. Localized electron transfer rates and microelectrode-based enrichment of microbial communities within a phototrophic microbial mat

    SciTech Connect

    Babauta, Jerome T.; Atci, Erhan; Ha, Phuc T.; Lindemann, Stephen R.; Ewing, Timothy; Call, Douglas R.; Fredrickson, James K.; Beyenal, Haluk

    2014-01-01

    Phototrophic microbial mats frequently exhibit sharp, light-dependent redox gradients that regulate microbial respiration on specific electron acceptors as a function of depth. In this work, a benthic phototrophic microbial mat from Hot Lake, a hypersaline, epsomitic lake located near Oroville in north-central Washington, was used to develop a microscale electrochemical method to study local electron transfer processes within the mat. To characterize the physicochemical variables influencing electron transfer, we initially quantified redox potential, pH, and dissolved oxygen gradients by depth in the mat under photic and aphotic conditions. We further demonstrated that power output of a mat fuel cell was light-dependent. To study local electron transfer processes, we deployed a microscale electrode (microelectrode) with tip size ~20 μm. To enrich a subset of microorganisms capable of interacting with the microelectrode, we anodically polarized the microelectrode at depth in the mat. Subsequently, to characterize the microelectrode- associated community and compare it to the neighboring mat community, we performed amplicon sequencing of the V1-V3 region of the 16S gene. Differences in Bray-Curtis beta diversity, illustrated by large changes in relative abundance at the phylum level, suggested successful enrichment of specific mat community members on the microelectrode surface. The microelectrode-associated community exhibited substantially reduced alpha diversity and elevated relative abundances of Prosthecochloris, Loktanella, Catellibacterium, other unclassified members of Rhodobacteraceae, Thiomicrospira, and Limnobacter, compared with the community at an equivalent depth in the mat. Our results suggest that local electron transfer to an anodically polarized microelectrode selected for a specific microbial population, with substantially more abundance and diversity of sulfur-oxidizing phylotypes compared with the neighboring mat community.

  15. The effect of electron measurements both inside and outside the heliosphere on the modelling of local interstellar spectra

    NASA Astrophysics Data System (ADS)

    Bisschoff, Driaan; Potgieter, Marius

    2016-07-01

    A local interstellar spectrum (LIS) for electrons can be calculated with Galactic propagation models to benefit both Galactic and heliospheric propagation studies by considering the improved measurements for cosmic rays (CRs) made over the last few years, such as by Voyager 1 and PAMELA. Cosmic ray measurements made by Voyager 1 outside the dominant influence of solar modulation uniquely allows the direct comparison of modelled Galactic spectra to experimental data. Recent improved analysis of the PAMELA electron spectra gives measurements for the exceptional solar minimum of 2009 which clearly depict ideal minimum modulation conditions for CRs in the heliosphere. Utilizing the GALPROP code, a LIS for electrons is computed to directly reproduce the electron spectra observed by Voyager 1. Using this LIS as input to a comprehensive solar modulation model enables the comparison with the PAMELA electron spectra. To accomplish reproducing the electron measurements of both CR experiments, we established a LIS with by varying the source spectrum and diffusion parameters in the GALPROP code. Inclusion of reacceleration in Galactic space improves the LIS to also match the lower energy PAMELA values after been modulated through a full 3D solar modulation model.

  16. Localized electron states and phase separation at the LaAlO3/SrTiO3 interface

    NASA Astrophysics Data System (ADS)

    Satpathy, S.; Shanavas, K. V.

    2012-02-01

    Even though the 2D electron gas at the polar interfaces of LAO/STO has been studied extensively, an explanation for the observed magnetic centers or the coexistence of magnetism and superconductivity is still lacking. Earlier density-functional calculations have indicated the presence of multi-bands and two types of electrons at the interface [1]. Here we propose that a combination of lattice disorder, octahedral rotations, and Jahn-Teller distortion can lead to some of these electrons to be localized near the interface and form lattice polarons. Evidence for this is presented from detailed density-functional calculations, which indicate that the energy gain associated with JT distortion and impurity or disorder induced local potentials can offset the kinetic energy cost of localization. Our model studies [2] also show the possible existence of a phase separation, thereby providing a natural explanation for the coexistence of magnetism and superconductivity [3].[4pt] [1] Z. S. Popovi'c, S. Satpathy and R. M. Martin Phys. Rev. Lett., 101, 256801 (2008)[0pt] [2] B. R. K. Nanda and S. Satpathy Phys. Rev B, 83, 195114 (2011)[0pt] [3] L. Li et. al. Nature Physics, 7, 762 (2011); J. A. Bert et. al. ibid, 767 (2011);

  17. Magnetic, optical, and electron transport properties of n -type CeO2: Small polarons versus Anderson localization

    NASA Astrophysics Data System (ADS)

    Kolodiazhnyi, Taras; Charoonsuk, Thitirat; Seo, Yu-Seong; Chang, Suyong; Vittayakorn, Naratip; Hwang, Jungseek

    2017-01-01

    We report magnetic susceptibility, electrical conductivity and optical absorption of Ce1 -xMxO2 where M = Nb,Ta and 0 ≤x ≤0.03 . The dc conductivity follows a simple thermally activated Arrhenius-type behavior in the T =70 -700 K range with a change in slope at T*≈155 K. The high-temperature activation energy shows gradual increase from ≈170 to 220 meV as the dopant concentration increases. The activation energy of the low-temperature conductivity shows a broad minimum of ≈77 meV at x ≈0.01 . Electron transport and localization mechanisms are analyzed in the framework of the Holstein small polaron, Anderson localization, and Jahn-Teller distortion models. The fit to the small polaron mobility is dramatically improved when, instead of the longitudinal phonons, the transverse optical phonons are considered in the phonon-assisted electron transport. This serves as an indirect evidence of a strong 4 f1 orbital interaction with the oxygen ligands, similar to the case of PrO2. Based on comparison of the experimental data to the models, it is proposed that the defect-induced random electric fields make the dominant contribution to the electron localization in donor-doped ceria.

  18. Development of a Method for Local Electron Temperature and Density Measurements in the Divertor of the JET Tokamak

    NASA Technical Reports Server (NTRS)

    Jupen, C.; Meigs, A.; Bhatia, A. K.; Brezinsek, S.; OMullane, M.

    2004-01-01

    Plasma volume recombination in the divertor, a process in which charged particles recombine to neutral atoms, contributes to plasma detachment and hence cooling at the divertor target region. Detachment has been observed at JET and other tokamaks and is known to occur at low electron temperatures (T(sub e)<1 eV) and at high electron density (n(sub e)>10(exp 20)/m(exp 3)). The ability to measure such low temperatures is therefore of interest for modelling the divertor. In present work we report development of a new spectroscopic technique for investigation of local electron density (n(sub e)) and temperature (T,) in the outer divertor at JET.

  19. Highly Charged Ions from Laser-Cluster Interactions: Local-Field-Enhanced Impact Ionization and Frustrated Electron-Ion Recombination

    SciTech Connect

    Fennel, Thomas; Ramunno, Lora; Brabec, Thomas

    2007-12-07

    Our molecular dynamics analysis of Xe{sub 147-5083} clusters identifies two mechanisms that contribute to the yet unexplained observation of extremely highly charged ions in intense laser cluster experiments. First, electron impact ionization is enhanced by the local cluster electric field, increasing the highest charge states by up to 40%; a corresponding theoretical method is developed. Second, electron-ion recombination after the laser pulse is frustrated by acceleration electric fields typically used in ion detectors. This increases the highest charge states by up to 90%, as compared to the usual assumption of total recombination of all cluster-bound electrons. Both effects together augment the highest charge states by up to 120%, in reasonable agreement with experiments.

  20. Highly charged ions from laser-cluster interactions: local-field-enhanced impact ionization and frustrated electron-ion recombination.

    PubMed

    Fennel, Thomas; Ramunno, Lora; Brabec, Thomas

    2007-12-07

    Our molecular dynamics analysis of Xe_{147-5083} clusters identifies two mechanisms that contribute to the yet unexplained observation of extremely highly charged ions in intense laser cluster experiments. First, electron impact ionization is enhanced by the local cluster electric field, increasing the highest charge states by up to 40%; a corresponding theoretical method is developed. Second, electron-ion recombination after the laser pulse is frustrated by acceleration electric fields typically used in ion detectors. This increases the highest charge states by up to 90%, as compared to the usual assumption of total recombination of all cluster-bound electrons. Both effects together augment the highest charge states by up to 120%, in reasonable agreement with experiments.

  1. Ultrafast Studies on Electron Transfer in the Betaines: Evidence for Local Heating

    DTIC Science & Technology

    1992-05-18

    should limit the rate. 12-14 In inverted regime reactions, intrarnolecular vibrational modes can a&elerate the reaction by reducing the effective...is the reverse ET or ground state recovery. This electron transfer occurs in the inverted regime. Therefore, we expect that intramolecular vibrational ... modes will be important in ET dynamics. We have used ultrafast pump probe spectroscopy to investigate the ET kinetics of the lowest electronic

  2. Electron distribution function behavior during localized transverse ion acceleration events in the topside auroral zone

    NASA Technical Reports Server (NTRS)

    Lynch, K. A.; Arnoldy, R. L.; Kintner, P. M.; Vago, J. L.

    1994-01-01

    The Topaz3 auroral sounding rocket made the following observations concerning the transfer of precipitating auroral electron energy to transverse ion acceleration in the topside auroral zone. During the course of the flight, the precipitating electron beam was modified to varying degrees by interaction with VLF hiss, at times changing the beam into a field-aligned plateau. The electron distribution functions throughout the flight are classified according to the extent of this modification, and correspondences with ion acceleration events are sought. The hiss power during most of this rocket flight apparently exceeded the threshold for collapse into solitary structures. At the times of plateaued electron distributions, the collapse of these structures was limited by Landau damping through the ambient ions, resulting in a velocity-dependent acceleration of both protons and oxygen. This initial acceleration is sufficient to supply the number flux of upflowing ions observed at satellite altitudes. The bursty ion acceleration was anticorrelated, on 1-s or smaller timescales, with dispersive bursts of precipitating field-aligned electrons, although on longer timescales the bursty ions and the bursty electrons are correlated.

  3. Non-rigid registration and non-local principle component analysis to improve electron microscopy spectrum images

    NASA Astrophysics Data System (ADS)

    Yankovich, Andrew B.; Zhang, Chenyu; Oh, Albert; Slater, Thomas J. A.; Azough, Feridoon; Freer, Robert; Haigh, Sarah J.; Willett, Rebecca; Voyles, Paul M.

    2016-09-01

    Image registration and non-local Poisson principal component analysis (PCA) denoising improve the quality of characteristic x-ray (EDS) spectrum imaging of Ca-stabilized Nd2/3TiO3 acquired at atomic resolution in a scanning transmission electron microscope. Image registration based on the simultaneously acquired high angle annular dark field image significantly outperforms acquisition with a long pixel dwell time or drift correction using a reference image. Non-local Poisson PCA denoising reduces noise more strongly than conventional weighted PCA while preserving atomic structure more faithfully. The reliability of and optimal internal parameters for non-local Poisson PCA denoising of EDS spectrum images is assessed using tests on phantom data.

  4. Histone methylation is a critical regulator of the abnormal expression of POU5F1 and RASSF1A in testis cancer cell lines.

    PubMed

    Lambrot, R; Kimmins, S

    2011-04-01

    DNA and histone methylation are epigenetic modifications functioning in transcriptional control and have been implicated in the deregulation of gene expression in cancer. As a first step to determine if histone methylation could be involved in testis cancer pathogenesis, we performed immunofluorescent localization of histone H3 methylation at lysine 4 (H3-K4; gene activating) and lysine 9 (H3-K9; gene silencing) in healthy testis tissue and in samples of non-seminoma germ-cell tumours. In healthy testis, the distribution of histone H3 methylation was dependent on the developmental stage of spermatogenic cells and in non-seminoma, histone H3-K4 and K9 methylation was detected in all histological subtypes. This suggested that histone H3-K4 and K9 methylation could be associated with abnormal gene expression in non-seminoma. To determine the gene-specific function of histone H3 methylation, we proceeded to define the epigenetic status of key genes implicated in the pathogenesis of non-seminoma, namely the proto-oncogene POU5F1, which is overexpressed in testis cancer, and the tumour suppressor RASSF1A, which is aberrantly silenced. Cell lines representative of non-seminoma were treated with the chromatin-modifying drug, 5-aza-2'-deoxycytidine (5-aza-dC). Chromatin immunoprecipitation and real-time polymerase chain reaction analyses revealed that treatment with 5-aza-dC restored RASSF1A expression through a loss of gene silencing H3-K9 methylation and by retention of gene activating H3-K4 tri-methylation in the promoter region. In contrast, the expression of POU5F1 was reduced by 5-aza-dC and was associated with a loss of gene activating H3-K4 di-methylation in the promoter region. Analysis of DNA methylation revealed a slight reduction in DNA hypermethylation at the RASSF1A promoter, whereas the POU5F1 promoter remained mostly unmethylated and unaffected. Our results indicate that the effects of 5-aza-dC on histone methylation profiles are gene-specific and that

  5. Autoradiographic distribution of /sup 14/C-labeled 3H-imidazo(4,5-f)quinoline-2-amines in mice

    SciTech Connect

    Bergman, K.

    1985-03-01

    The highly mutagenic heterocyclic amines, 2-amino-3-methylimidazo(4,5-f)quinoline (IQ) and 2-amino-3,4-dimethylimidazo(4,5-f)quinoline (MeIQ), are formed during heating of protein-rich foods. In order to gain information about the distribution and fate of IQ and MeIQ in vivo, a whole-body autoradiographic study of i.v.-injected /sup 14/C-labeled IQ and MeIQ has been performed in male NMRI, pregnant NMRI, and female C3H mice. IQ and MeIQ showed similar distribution patterns. At short survival times, the autoradiograms were characterized by an accumulation of radioactivity in metabolic and excretory organs (liver, kidney, bile, urine, gastric and intestinal contents, salivary glands, nasal mucosa, and Harder's gland), as well as in lymphomyeloid tissues (bone marrow, thymus, spleen and lymph nodes) and in endocrine and reproductive tissues (adrenal medulla, pancreatic islets, thyroid, hypophysis, testis, epididymis, seminal vesicles, ampulla, and prostate). The liver and kidney cortex were identified as sites of retention of nonextractable radioactivity. IQ and MeIQ showed a strong affinity for melanin. IQ and MeIQ passed the placenta, but no radioactivity was retained in fetal tissues. The results pinpoint the liver as a site of IQ- and MeIQ-mediated toxicity. Future studies of IQ and MeIQ may be guided by and clarify the role of other tissue localizations in the toxicity of IQ and MeIQ.

  6. Superconductivity in a new layered bismuth oxyselenide: LaO(0.5)F(0.5)BiSe₂.

    PubMed

    Krzton-Maziopa, A; Guguchia, Z; Pomjakushina, E; Pomjakushin, V; Khasanov, R; Luetkens, H; Biswas, P K; Amato, A; Keller, H; Conder, K

    2014-05-28

    We report superconductivity at T(c) ≈ 2.6 K in a new layered bismuth oxyselenide LaO(0.5)F(0.5)BiSe2 with the ZrCuSiAs-type structure composed of alternating superconducting BiSe2 and blocking LaO layers. The superconducting properties of LaO(0.5)F(0.5)BiSe2 were investigated by means of dc magnetization, resistivity and muon-spin rotation experiments, revealing the appearance of bulk superconductivity with a rather large superconducting volume fraction of ≈ 70% at 1.8 K.

  7. Novel method of simultaneous multiple immunogold localization on resin sections in high resolution scanning electron microscopy.

    PubMed

    Nebesarova, Jana; Wandrol, Petr; Vancova, Marie

    2016-01-01

    We present a new method of multiple immunolabeling that is suitable for a broad spectrum of biomedical applications. The general concept is to label both sides of the ultrathin section with the thickness of 70-80 nm with different antibodies conjugated to gold nanoparticles and to distinguish the labeled side by advanced imaging methods with high resolution scanning electron microscopy, such as by correlating images acquired at different energies of primary electrons using different signals. From the Clinical Editor: The use of transmission electron microscopy has become an indispensible tool in the detection of cellular proteins. In this short but interesting article, the authors described their new method of labeling and the identification of four different proteins simultaneously, which represents another advance in imaging technique.

  8. Localization of electrons in dome-shaped GeSi/Si islands

    SciTech Connect

    Yakimov, A. I.; Kirienko, V. V.; Bloshkin, A. A.; Armbrister, V. A.; Kuchinskaya, P. A.; Dvurechenskii, A. V.

    2015-01-19

    We report on intraband photocurrent spectroscopy of dome-shaped GeSi islands embedded in a Si matrix with n{sup +}-type bottom and top Si layers. An in-plane polarized photoresponse in the 85–160 meV energy region has been observed and ascribed to the optical excitation of electrons from states confined in the strained Si near the dome apexes to the continuum states of unstrained Si. The electron confinement is caused by a modification of the conduction band alignment induced by inhomogeneous tensile strain in Si around the buried GeSi quantum dots. Sensitivity of the device to the normal incidence radiation proves a zero-dimensional nature of confined electronic wave functions.

  9. New Electron Temperature Measurements During Local Helicity Injection and H-mode Plasmas at the Pegasus Toroidal Experiment

    NASA Astrophysics Data System (ADS)

    Schlossberg, D. J.; Bodner, G. M.; Fonck, R. J.; Reusch, J. A.; Winz, G. R.

    2015-11-01

    Extrapolation of non-solenoidal startup via local helicity injection (LHI) to larger devices depends critically on confinement during the injection process. To begin quantifying confinement regimes, the Thomson scattering diagnostic on the Pegasus ST was upgraded to include 12 radial positions and high temperature (0.1 electron distributions, with central Te = 150 eV. In the low-density LHI startup plasmas shot-to-shot averaging of data improves background measurements and increases signal-to-noise ratio. Initial core measurements during the drive phase of LHI suggest average Te of several hundred eV for plasmas with ne ~ 3x1018 m-3 and Ip ~ 0.15 MA. Experiments are underway to verify these unexpectedly high electron temperatures. If verified, these temperatures may reflect the dominance of high-energy electrons via fueling with LHI current streams with average energy ~1 keV. Further investigations will explore the dependence of the inferred electron distribution on fueling source, density, and electron injection potential. The upgraded Thomson scattering diagnostic will also be applied to Ohmic H-mode plasmas in Pegasus. Work supported by US DOE grant DE-FG02-96ER54375.

  10. Materials Data on KNb4O5F (SG:123) by Materials Project

    SciTech Connect

    Kristin Persson

    2016-02-05

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  11. Materials Data on S2O5F2 (SG:114) by Materials Project

    SciTech Connect

    Kristin Persson

    2016-02-04

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  12. Materials Data on Pr2SbO5F (SG:4) by Materials Project

    SciTech Connect

    Kristin Persson

    2016-02-04

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  13. Materials Data on LiV2O5F (SG:18) by Materials Project

    DOE Data Explorer

    Kristin Persson

    2014-07-09

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  14. Materials Data on SrLa5F17 (SG:1) by Materials Project

    SciTech Connect

    Kristin Persson

    2014-07-09

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  15. Materials Data on Mn3O5F (SG:12) by Materials Project

    SciTech Connect

    Kristin Persson

    2016-04-22

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  16. Materials Data on V3O5F (SG:10) by Materials Project

    DOE Data Explorer

    Kristin Persson

    2016-04-22

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  17. Materials Data on Ba2Cu5F14 (SG:15) by Materials Project

    SciTech Connect

    Kristin Persson

    2016-02-10

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  18. Materials Data on V3O5F (SG:7) by Materials Project

    SciTech Connect

    Kristin Persson

    2016-04-22

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  19. Materials Data on Mn6O5F7 (SG:7) by Materials Project

    SciTech Connect

    Kristin Persson

    2016-04-22

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  20. Materials Data on Fe4O5F3 (SG:7) by Materials Project

    SciTech Connect

    Kristin Persson

    2016-04-22

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  1. Materials Data on CaPH4O5F (SG:2) by Materials Project

    SciTech Connect

    Kristin Persson

    2016-02-04

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  2. Materials Data on Sn2H2SO5F2 (SG:14) by Materials Project

    SciTech Connect

    Kristin Persson

    2016-03-28

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  3. Electronic and optical properties of free standing Pt nanowires using localized basis sets

    NASA Astrophysics Data System (ADS)

    Kumar, Arun; Kumar, Ashok; Ahluwalia, P. K.

    2012-06-01

    In this paper we have investigated structural, electronic and optical properties of free standing ultrathin NWs of Pt with different topologies using ab-initio SIESTA code. Dimer and ladder chains have found smallest and largest cohesive energy respectively. Electronic band structure and DOS calculations finds more bands and states respectively around Fermi level in ladder topology of Pt chains. It is found that linear and dimer chains act as a good reflector as compared to ladder and zig-zag topologies of Pt chains. Plasmonic frequency of zig-zag and ladder chains are found largest and smallest respectively.

  4. Dissociative electron attachment to the H2O molecule. II. Nuclear dynamics on coupled electronic surfaces within the local complex potential model

    NASA Astrophysics Data System (ADS)

    Haxton, Daniel J.; Rescigno, T. N.; McCurdy, C. W.

    2007-01-01

    We report the results of a first-principles study of dissociative electron attachment to H2O . The cross sections were obtained from nuclear dynamics calculations carried out in full dimensionality within the local complex potential model by using the multiconfiguration time-dependent Hartree method. The calculations employ our previously obtained global, complex-valued, potential-energy surfaces for the three ( B12 , A12 , and B22 ) electronic Feshbach resonances involved in this process. These three metastable states of H2O- undergo several degeneracies, and we incorporate both the Renner-Teller coupling between the B12 and A12 states as well as the conical intersection between the A12 and B22 states into our treatment. The nuclear dynamics are inherently multidimensional and involve branching between different final product arrangements as well as extensive excitation of the diatomic fragment. Our results successfully mirror the qualitative features of the major fragment channels observed, but are less successful in reproducing the available results for some of the minor channels. We comment on the applicability of the local complex potential model to such a complicated resonant system.

  5. Second Line of Defense Help Desk: Electronic Maintenance Reports - Local Maintenance Provider User Guide Rev. 1

    SciTech Connect

    Leigh, Richard J.

    2011-12-14

    The Electronic Maintenance Report forms present a uniform dataset for analysis of Sustainability metrics. These forms collect readily minable data while allowing the attachment of site-specific checklists or other supporting files for review by the Sustainability Manager and Program Management.

  6. Path Integrals for Electronic Densities, Reactivity Indices, and Localization Functions in Quantum Systems

    PubMed Central

    Putz, Mihai V.

    2009-01-01

    The density matrix theory, the ancestor of density functional theory, provides the immediate framework for Path Integral (PI) development, allowing the canonical density be extended for the many-electronic systems through the density functional closure relationship. Yet, the use of path integral formalism for electronic density prescription presents several advantages: assures the inner quantum mechanical description of the system by parameterized paths; averages the quantum fluctuations; behaves as the propagator for time-space evolution of quantum information; resembles Schrödinger equation; allows quantum statistical description of the system through partition function computing. In this framework, four levels of path integral formalism were presented: the Feynman quantum mechanical, the semiclassical, the Feynman-Kleinert effective classical, and the Fokker-Planck non-equilibrium ones. In each case the density matrix or/and the canonical density were rigorously defined and presented. The practical specializations for quantum free and harmonic motions, for statistical high and low temperature limits, the smearing justification for the Bohr’s quantum stability postulate with the paradigmatic Hydrogen atomic excursion, along the quantum chemical calculation of semiclassical electronegativity and hardness, of chemical action and Mulliken electronegativity, as well as by the Markovian generalizations of Becke-Edgecombe electronic focalization functions – all advocate for the reliability of assuming PI formalism of quantum mechanics as a versatile one, suited for analytically and/or computationally modeling of a variety of fundamental physical and chemical reactivity concepts characterizing the (density driving) many-electronic systems. PMID:20087467

  7. Bringing Up Gopher: Access to Local & Remote Electronic Resources for University Library Users.

    ERIC Educational Resources Information Center

    Brown, Melvin Marlo; And Others

    Some of the administrative and organizational issues in creating a gopher, specifically a library gopher for university libraries, are discussed. In 1993 the Electronic Collections Task Force of the New Mexico State University library administration began to develop a library-based gopher system that would enable users to have unlimited access to…

  8. Path integrals for electronic densities, reactivity indices, and localization functions in quantum systems.

    PubMed

    Putz, Mihai V

    2009-11-10

    The density matrix theory, the ancestor of density functional theory, provides the immediate framework for Path Integral (PI) development, allowing the canonical density be extended for the many-electronic systems through the density functional closure relationship. Yet, the use of path integral formalism for electronic density prescription presents several advantages: assures the inner quantum mechanical description of the system by parameterized paths; averages the quantum fluctuations; behaves as the propagator for time-space evolution of quantum information; resembles Schrödinger equation; allows quantum statistical description of the system through partition function computing. In this framework, four levels of path integral formalism were presented: the Feynman quantum mechanical, the semiclassical, the Feynman-Kleinert effective classical, and the Fokker-Planck non-equilibrium ones. In each case the density matrix or/and the canonical density were rigorously defined and presented. The practical specializations for quantum free and harmonic motions, for statistical high and low temperature limits, the smearing justification for the Bohr's quantum stability postulate with the paradigmatic Hydrogen atomic excursion, along the quantum chemical calculation of semiclassical electronegativity and hardness, of chemical action and Mulliken electronegativity, as well as by the Markovian generalizations of Becke-Edgecombe electronic focalization functions - all advocate for the reliability of assuming PI formalism of quantum mechanics as a versatile one, suited for analytically and/or computationally modeling of a variety of fundamental physical and chemical reactivity concepts characterizing the (density driving) many-electronic systems.

  9. Performance of a local electron density trigger to select extensive air showers at sea level

    NASA Technical Reports Server (NTRS)

    Abbas, T.; Madani, J.; Ashton, F.

    1985-01-01

    Time coincident voltage pulses in the two closely space (1.6m) plastic scintillators were recorded. Most of the recorded events are expeted to be due to electrons in cosmic ray showers whose core fall at some distance from the detectors. This result is confirmed from a measurement of the frequency distribution of the recorded density ratios of the two scintillators.

  10. Electronic localization and bad-metallicity in pure and electron-doped troilite: A local-density-approximation plus dynamical-mean-field-theory study of FeS for lithium-ion batteries

    NASA Astrophysics Data System (ADS)

    Craco, L.; Faria, J. L. B.

    2016-02-01

    Iron sulfides are promising candidates for the next generation of rechargeable lithium-ion battery materials. Motivated thereby, we present a detailed study of correlation- and doping-induced electronic reconstruction in troilite. Based on local-density-approximation plus dynamical-mean-field-theory, we stress the importance of multi-orbital Coulomb interactions in concert with first-principles band structure calculations for a consistent understanding of intrinsic Mott-Hubbard insulating state in FeS. We explore the anomalous nature of electron doping-induced insulator-bad metal transition, showing that it is driven by orbital-selective dynamical spectral weight transfer. Our results are relevant for understanding charge dynamics upon electrochemical lithiation of iron monosulfides electrode materials for lithium-ion batteries.

  11. Self-generated local heating induced nanojoining for room temperature pressureless flexible electronic packaging.

    PubMed

    Peng, Peng; Hu, Anming; Gerlich, Adrian P; Liu, Yangai; Zhou, Y Norman

    2015-03-19

    Metallic bonding at an interface is determined by the application of heat and/or pressure. The means by which these are applied are the most critical for joining nanoscale structures. The present study considers the feasibility of room-temperature pressureless joining of copper wires using water-based silver nanowire paste. A novel mechanism of self-generated local heating within the silver nanowire paste and copper substrate system promotes the joining of silver-to-silver and silver-to-copper without any external energy input. The localized heat energy was delivered in-situ to the interfaces to promote atomic diffusion and metallic bond formation with the bulk component temperature stays near room-temperature. This local heating effect has been detected experimentally and confirmed by calculation. The joints formed at room-temperature without pressure achieve a tensile strength of 5.7 MPa and exhibit ultra-low resistivity in the range of 101.3 nOhm · m. The good conductivity of the joint is attributed to the removal of organic compounds in the paste and metallic bonding of silver-to-copper and silver-to-silver. The water-based silver nanowire paste filler material is successfully applied to various flexible substrates for room temperature bonding. The use of chemically generated local heating may become a potential method for energy in-situ delivery at micro/nanoscale.

  12. Self-generated Local Heating Induced Nanojoining for Room Temperature Pressureless Flexible Electronic Packaging

    PubMed Central

    Peng, Peng; Hu, Anming; Gerlich, Adrian P.; Liu, Yangai; Zhou, Y. Norman

    2015-01-01

    Metallic bonding at an interface is determined by the application of heat and/or pressure. The means by which these are applied are the most critical for joining nanoscale structures. The present study considers the feasibility of room-temperature pressureless joining of copper wires using water-based silver nanowire paste. A novel mechanism of self-generated local heating within the silver nanowire paste and copper substrate system promotes the joining of silver-to-silver and silver-to-copper without any external energy input. The localized heat energy was delivered in-situ to the interfaces to promote atomic diffusion and metallic bond formation with the bulk component temperature stays near room-temperature. This local heating effect has been detected experimentally and confirmed by calculation. The joints formed at room-temperature without pressure achieve a tensile strength of 5.7 MPa and exhibit ultra-low resistivity in the range of 101.3 nOhm·m. The good conductivity of the joint is attributed to the removal of organic compounds in the paste and metallic bonding of silver-to-copper and silver-to-silver. The water-based silver nanowire paste filler material is successfully applied to various flexible substrates for room temperature bonding. The use of chemically generated local heating may become a potential method for energy in-situ delivery at micro/nanoscale. PMID:25788019

  13. Virtual Staff Meetings: Electronic Tutor Training with a Local E-Mail Listserv Discussion Group.

    ERIC Educational Resources Information Center

    Strenski, Ellen; And Others

    1995-01-01

    Analyzes dynamics of an online discussion group of graduate students who teach introductory composition and literature classes at the University of California at Irvine: advantages of a listserv over a distributed mailing list; benefits of a local listserv over a national listserv; resistance to a listserv; and various "nuts and bolts"…

  14. Local Electronic and Chemical Structure of Oligo-acetylene Derivatives Formed Through Radical Cyclizations at a Surface

    PubMed Central

    2014-01-01

    Semiconducting π-conjugated polymers have attracted significant interest for applications in light-emitting diodes, field-effect transistors, photovoltaics, and nonlinear optoelectronic devices. Central to the success of these functional organic materials is the facile tunability of their electrical, optical, and magnetic properties along with easy processability and the outstanding mechanical properties associated with polymeric structures. In this work we characterize the chemical and electronic structure of individual chains of oligo-(E)-1,1′-bi(indenylidene), a polyacetylene derivative that we have obtained through cooperative C1–C5 thermal enediyne cyclizations on Au(111) surfaces followed by a step-growth polymerization of the (E)-1,1′-bi(indenylidene) diradical intermediates. We have determined the combined structural and electronic properties of this class of oligomers by characterizing the atomically precise chemical structure of individual monomer building blocks and oligomer chains (via noncontact atomic force microscopy (nc-AFM)), as well as by imaging their localized and extended molecular orbitals (via scanning tunneling microscopy and spectroscopy (STM/STS)). Our combined structural and electronic measurements reveal that the energy associated with extended π-conjugated states in these oligomers is significantly lower than the energy of the corresponding localized monomer orbitals, consistent with theoretical predictions. PMID:24387223

  15. Local unitary transformation method toward practical electron correlation calculations with scalar relativistic effect in large-scale molecules.

    PubMed

    Seino, Junji; Nakai, Hiromi

    2013-07-21

    In order to perform practical electron correlation calculations, the local unitary transformation (LUT) scheme at the spin-free infinite-order Douglas-Kroll-Hess (IODKH) level [J. Seino and H. Nakai, J. Chem. Phys. 136, 244102 (2012); and ibid. 137, 144101 (2012)], which is based on the locality of relativistic effects, has been combined with the linear-scaling divide-and-conquer (DC)-based Hartree-Fock (HF) and electron correlation methods, such as the second-order Mo̸ller-Plesset (MP2) and the coupled cluster theories with single and double excitations (CCSD). Numerical applications in hydrogen halide molecules, (HX)n (X = F, Cl, Br, and I), coinage metal chain systems, Mn (M = Cu and Ag), and platinum-terminated polyynediyl chain, trans,trans-{(p-CH3C6H4)3P}2(C6H5)Pt(C≡C)4Pt(C6H5){(p-CH3C6H4)3P}2, clarified that the present methods, namely DC-HF, MP2, and CCSD with the LUT-IODKH Hamiltonian, reproduce the results obtained using conventional methods with small computational costs. The combination of both LUT and DC techniques could be the first approach that achieves overall quasi-linear-scaling with a small prefactor for relativistic electron correlation calculations.

  16. Microencapsulation of inorganic nanocrystals into PLGA microsphere vaccines enables their intracellular localization in dendritic cells by electron and fluorescence microscopy.

    PubMed

    Schliehe, Christopher; Schliehe, Constanze; Thiry, Marc; Tromsdorf, Ulrich I; Hentschel, Joachim; Weller, Horst; Groettrup, Marcus

    2011-05-10

    Biodegradable poly-(D,L-lactide-co-glycolide) microspheres (PLGA-MS) are approved as a drug delivery system in humans and represent a promising antigen delivery device for immunotherapy against cancer. Immune responses following PLGA-MS vaccination require cross-presentation of encapsulated antigen by professional antigen presenting cells (APCs). While the potential of PLGA-MS as vaccine formulations is well established, the intracellular pathway of cross-presentation following phagocytosis of PLGA-MS is still under debate. A part of the controversy stems from the difficulty in unambiguously identifying PLGA-MS within cells. Here we show a novel strategy for the efficient encapsulation of inorganic nanocrystals (NCs) into PLGA-MS as a tool to study their intracellular localization. We microencapsulated NCs as an electron dense marker to study the intracellular localization of PLGA-MS by transmission electron microscopy (TEM) and as fluorescent labels for confocal laser scanning microscopy. Using this method, we found PLGA-MS to be rapidly taken up by dendritic cells and macrophages. Co-localization with the lysosomal marker LAMP1 showed a lysosomal storage of PLGA-MS for over two days after uptake, long after the initiation of cross-presentation had occurred. Our data argue against an escape of PLGA-MS from the endosome as has previously been suggested as a mechanism to facilitate cross-presentation of PLGA-MS encapsulated antigen.

  17. Potentially Functional Polymorphisms in POU5F1 Gene Are Associated with the Risk of Lung Cancer in Han Chinese.

    PubMed

    Niu, Rui; Wang, Yuzhuo; Zhu, Meng; Wen, Yifan; Sun, Jie; Shen, Wei; Cheng, Yang; Zhang, Jiahui; Jin, Guangfu; Ma, Hongxia; Hu, Zhibin; Shen, Hongbing; Dai, Juncheng

    2015-01-01

    POU5F1 is a key regulator of self-renewal and differentiation in embryonic stem cells and may be associated with initiation, promotion, and progression in cancer. We hypothesized that functional polymorphisms in POU5F1 may play an important role in modifying the lung cancer risk. To test this hypothesis, we conducted a case-control study to explore the association between 17 potentially functional SNPs in POU5F1 gene and the lung cancer risk in 1,341 incident lung cancer cases and 1,982 healthy controls in a Chinese population. We found that variant alleles of rs887468 and rs3130457 were significantly associated with increased risk of lung cancer after multiple comparison (OR = 1.29, 95% CI: 1.11-1.51, P fdr = 0.017 for rs887468; OR = 1.29, 95% CI: 1.10-1.51, P fdr = 0.034 for rs3130457, resp.). In addition, we detected a significant interaction between rs887468 genotypes and smoking status on lung cancer risk (P = 0.017). Combined analysis of these 2 SNPs showed a significant allele-dosage association between the number of risk alleles and increased risk of lung cancer (P trend < 0.001). These findings indicate that potentially functional polymorphisms in POU5F1 gene may contribute to lung cancer susceptibility in a Chinese population.

  18. 26 CFR 5f.103-1 - Obligations issued after December 31, 1982, required to be in registered form.

    Code of Federal Regulations, 2014 CFR

    2014-04-01

    ... 103 (a) or any other provision of law, exclusive of any treaty obligation of the United States, unless... 26 Internal Revenue 14 2014-04-01 2013-04-01 true Obligations issued after December 31, 1982... EQUITY AND FISCAL RESPONSIBILITY ACT OF 1982 § 5f.103-1 Obligations issued after December 31,...

  19. 49 CFR Appendix A to Part 591 - Section 591.5(f) Bond for the Entry of a Single Vehicle

    Code of Federal Regulations, 2012 CFR

    2012-10-01

    ... 49 Transportation 7 2012-10-01 2012-10-01 false Section 591.5(f) Bond for the Entry of a Single Vehicle A Appendix A to Part 591 Transportation Other Regulations Relating to Transportation (Continued... VEHICLES AND EQUIPMENT SUBJECT TO FEDERAL SAFETY, BUMPER AND THEFT PREVENTION STANDARDS Pt. 591, App....

  20. Potentially Functional Polymorphisms in POU5F1 Gene Are Associated with the Risk of Lung Cancer in Han Chinese

    PubMed Central

    Niu, Rui; Wang, Yuzhuo; Zhu, Meng; Wen, Yifan; Sun, Jie; Shen, Wei; Cheng, Yang; Zhang, Jiahui; Jin, Guangfu; Ma, Hongxia; Hu, Zhibin; Shen, Hongbing; Dai, Juncheng

    2015-01-01

    POU5F1 is a key regulator of self-renewal and differentiation in embryonic stem cells and may be associated with initiation, promotion, and progression in cancer. We hypothesized that functional polymorphisms in POU5F1 may play an important role in modifying the lung cancer risk. To test this hypothesis, we conducted a case-control study to explore the association between 17 potentially functional SNPs in POU5F1 gene and the lung cancer risk in 1,341 incident lung cancer cases and 1,982 healthy controls in a Chinese population. We found that variant alleles of rs887468 and rs3130457 were significantly associated with increased risk of lung cancer after multiple comparison (OR = 1.29, 95% CI: 1.11–1.51, Pfdr = 0.017 for rs887468; OR = 1.29, 95% CI: 1.10–1.51, Pfdr = 0.034 for rs3130457, resp.). In addition, we detected a significant interaction between rs887468 genotypes and smoking status on lung cancer risk (P = 0.017). Combined analysis of these 2 SNPs showed a significant allele-dosage association between the number of risk alleles and increased risk of lung cancer (Ptrend < 0.001). These findings indicate that potentially functional polymorphisms in POU5F1 gene may contribute to lung cancer susceptibility in a Chinese population. PMID:26824036

  1. A theory of local and global processes which affect solar wind electrons. I - The origin of typical 1 AU velocity distribution functions - Steady state theory

    NASA Technical Reports Server (NTRS)

    Scudder, J. D.; Olbert, S.

    1979-01-01

    A kinetic theory for the velocity distribution of solar wind electrons which illustrates the global and local properties of the solar wind expansion is proposed. By means of the Boltzmann equation with the Krook collision operator accounting for Coulomb collisions, it is found that Coulomb collisions determine the population and shape of the electron distribution function in both the thermal and suprathermal energy regimes. For suprathermal electrons, the cumulative effects of Coulomb interactions are shown to take place on the scale of the heliosphere itself, whereas the Coulomb interactions of thermal electrons occur on a local scale near the point of observation (1 AU). The bifurcation of the electron distribution between thermal and suprathermal electrons is localized to the deep solar corona (1 to 10 solar radii).

  2. Tailoring the local structure and electronic property of AuPd nanoparticles by selecting capping molecules

    NASA Astrophysics Data System (ADS)

    Liu, Feng; Zhang, Peng

    2010-01-01

    Nine AuPd nanoparticle samples selectively capped with tetraoctylphosphonium bromide, primary amine and tertiary amine molecules were studied with the Au L3-edge x-ray absorption spectroscopy (XAS). The AuPd mixing patterns were analyzed by comparing the XAS results with the theoretical coordination numbers of 24 AuPd model clusters of varied size, Au concentration, and bimetal mixing pattern. It was found that the use of amines, particularly tertiary amine, produced a more homogeneous AuPd mixing pattern and the Au d-electron density was fine-tunable by tailoring the density of Au-Pd bonds. Mechanisms for the tailored structural and electronic properties of these nanoparticles were proposed.

  3. Dynamic Localization of Electronic Excitation in Photosynthetic Complexes Revealed with Chiral Two-Dimensional Spectroscopy

    PubMed Central

    Fidler, Andrew F.; Singh, Ved P.; Long, Phillip D.; Dahlberg, Peter D.; Engel, Gregory S.

    2014-01-01

    Time-resolved ultrafast optical probes of chiral dynamics provide a new window allowing us to explore how interactions with such structured environments drive electronic dynamics. Incorporating optical activity into time-resolved spectroscopies has proven challenging due to the small signal and large achiral background. Here, we demonstrate that two-dimensional electronic spectroscopy can be adapted to detect chiral signals and that these signals reveal how excitations delocalize and contract following excitation. We dynamically probe the evolution of chiral electronic structure in the light harvesting complex 2 of purple bacteria following photoexcitation by creating a chiral two-dimensional mapping. The dynamics of the chiral two-dimensional signal directly reports on changes in the degree of delocalization of the excitonic state following photoexcitation. The mechanism of energy transfer in this system may enhance transfer probability due to the coherent coupling among chromophores while suppressing fluorescence that arises from populating delocalized states. This generally applicable spectroscopy will provide an incisive tool to probe ultrafast transient molecular fluctuations that are obscured in non-chiral experiments. PMID:24504144

  4. Saturation of SRS-LDI with Non-local Growth of SRS Driven Electron Plasma Wave

    NASA Astrophysics Data System (ADS)

    Salcedo, A.; Bers, A.; Ram, A. K.

    2000-10-01

    Experimental observations have shown the coupling of SRS and Langmuir decay interaction (LDI), in ICF experiments where the SRS backscattering is dependent on the damping of ion acoustic waves.(Juan P. Fernandez, et al., Phys. Rev. Lett.) 77, 2702 (1996); R. K. Kirkwood, et al., Phys. Rev. Lett. 77, 13, (1996). A model 3-wave interaction equations for LDI with a growing EPW (driven by SRS) and its non-local Landau damping, gives a simple description of the effect of LDI on the saturation of SRS and its dependence on IAW damping. ( A. Salcedo, A. Bers, A. K. Ram, in Proc. 1st IFSA), Bordeaux, France (1999), pp. 343-348. We present results on the extension of this model to include the non-local growth of the SRS driven EPW, and a comparison with simulations of the full five-wave interaction equations for SRS coupled to LDI. (J. A. Heikkinen, J. Karttunen, Phys. Fluids) 29 (4), (1986).

  5. Electron acceleration at localized wave structures in the solar corona (German Title: Elektronenbeschleunigung an lokalen Wellenstrukturen in der Sonnenkorona)

    NASA Astrophysics Data System (ADS)

    Miteva, Rositsa Stoycheva

    2007-07-01

    Our dynamic Sun manifests its activity by different phenomena: from the 11-year cyclic sunspot pattern to the unpredictable and violent explosions in the case of solar flares. During flares, a huge amount of the stored magnetic energy is suddenly released and a substantial part of this energy is carried by the energetic electrons, considered to be the source of the nonthermal radio and X-ray radiation. One of the most important and still open question in solar physics is how the electrons are accelerated up to high energies within (the observed in the radio emission) short time scales. Because the acceleration site is extremely small in spatial extent as well (compared to the solar radius), the electron acceleration is regarded as a local process. The search for localized wave structures in the solar corona that are able to accelerate electrons together with the theoretical and numerical description of the conditions and requirements for this process, is the aim of the dissertation. Two models of electron acceleration in the solar corona are proposed in the dissertation: I. Electron acceleration due to the solar jet interaction with the background coronal plasma (the jet--plasma interaction) A jet is formed when the newly reconnected and highly curved magnetic field lines are relaxed by shooting plasma away from the reconnection site. Such jets, as observed in soft X-rays with the Yohkoh satellite, are spatially and temporally associated with beams of nonthermal electrons (in terms of the so-called type III metric radio bursts) propagating through the corona. A model that attempts to give an explanation for such observational facts is developed here. Initially, the interaction of such jets with the background plasma leads to an (ion-acoustic) instability associated with growing of electrostatic fluctuations in time for certain range of the jet initial velocity. During this process, any test electron that happen to feel this electrostatic wave field is drawn to co

  6. Finite-temperature electron correlations in the framework of a dynamic local-field correction

    SciTech Connect

    Schweng, H.K.; Boehm, H.M. )

    1993-07-15

    The quantum-mechanical version of the Singwi-Tosi-Land-Sjoelander (STLS) approximation is applied to finite temperatures. This approximation has two main advantages. First, it includes a dynamic local-field correction and second, it gives positive values for the pair-distribution function in the short-range region at zero temperature. This is even valid for rather low densities. After a description of the numerical difficulties arising with the use of a dynamic approximation, the results for the static-structure factor and the pair-distribution function are discussed thoroughly. Detailed work is performed on the static part of the local-field correction, with special emphasis put on the investigation of its structure. A peak is found at a wave vector [ital q][approx]2.8 (in units of the Fermi wave vector) for small temperatures, which tends towards higher values of [ital q] with increasing temperature. This peak causes an attractive particle-hole interaction in a certain [ital q] region and thus gives rise to the appearance of a charge-density wave. A parametric description is given for the static local-field correction in order to simplify further applications. Furthermore, the exchange-and-correlation free energy is considered. The results are compared with the STLS results and with the modified convolution approach.

  7. Probing the symmetry of the potential of localized surface plasmon resonances with phase-shaped electron beams.

    PubMed

    Guzzinati, Giulio; Béché, Armand; Lourenço-Martins, Hugo; Martin, Jérôme; Kociak, Mathieu; Verbeeck, Jo

    2017-04-12

    Plasmonics, the science and technology of the interaction of light with metallic objects, is fundamentally changing the way we can detect, generate and manipulate light. Although the field is progressing swiftly, thanks to the availability of nanoscale manufacturing and analysis methods, fundamental properties such as the plasmonic excitations' symmetries cannot be accessed directly, leading to a partial, sometimes incorrect, understanding of their properties. Here we overcome this limitation by deliberately shaping the wave function of an electron beam to match a plasmonic excitations' symmetry in a modified transmission electron microscope. We show experimentally and theoretically that this offers selective detection of specific plasmon modes within metallic nanoparticles, while excluding modes with other symmetries. This method resembles the widespread use of polarized light for the selective excitation of plasmon modes with the advantage of locally probing the response of individual plasmonic objects and a far wider range of symmetry selection criteria.

  8. Nature of localized states in two-dimensional electron systems in the quantum Hall regime: Acoustic studies

    NASA Astrophysics Data System (ADS)

    Drichko, I. L.; Smirnov, I. Yu.; Suslov, A. V.; Galperin, Y. M.; Pfeiffer, L. N.; West, K. W.

    2017-01-01

    We review our work on high-frequency conductance in two-dimensional high-mobility electronic systems in wide n-AlGaAs/GaAs/AlGaAs quantum wells. Using simultaneous measurements of the attenuation and velocity of a surface acoustic wave we obtained both real and imaginary components of the complex high-frequency conductance. Based on the experimental results and their analysis we conclude that close to the filling factor ν = 1/5, as well as in the interval 0.18 > ν > 0.125, a Wigner crystal pinned by disorder is formed. Both the melting temperature and the correlation length of the pinning-induced domains in the Wigner crystal were found. In close vicinities of ν = 1 and 2, transitions from single-electron localization to a Wigner crystal were observed.

  9. Tissue and cellular localization of tannins in Tunisian dates (Phoenix dactylifera L.) by light and transmission electron microscopy.

    PubMed

    Hammouda, Hédi; Alvarado, Camille; Bouchet, Brigitte; Kalthoum-Chérif, Jamila; Trabelsi-Ayadi, Malika; Guyot, Sylvain

    2014-07-16

    A histological approach including light microscopy and transmission electron microscopy (TEM) was used to provide accurate information on the localization of condensed tannins in the edible tissues and in the stone of date fruits (Phoenix dactylifera L.). Light microscopy was carried out on fresh tissues after staining by 4-dimethylaminocinnamaldehyde (DMACA) for a specific detection of condensed tannins. Thus, whether under light microscopy or transmission electron microscopy (TEM), results showed that tannins are not located in the epidermis but more deeply in the mesocarp in the vacuole of very large cells. Regarding the stones, tannins are found in a specific cell layer located at 50 μm from the sclereid cells of the testa.

  10. Dynamics of electronic excitations relaxation in hydrophilic colloidal CdS quantum dots in gelatin with involvement of localized states

    NASA Astrophysics Data System (ADS)

    Smirnov, M. S.; Buganov, O. V.; Shabunya-Klyachkovskaya, E. V.; Tikhomirov, S. A.; Ovchinnikov, O. V.; Vitukhnovsky, A. G.; Perepelitsa, A. S.; Matsukovich, A. S.; Katsaba, A. V.

    2016-10-01

    Dynamics of the 1Se-1S3/2 exciton in colloidal CdS quantum dots with diameter of 3.1 ÷ 4.5 nm in gelatin with involvement of localized states was studied by means of femtosecond photoinduced absorption spectroscopy (pump-probe), thermally stimulated luminescence (TSL) observed under permanently excited luminescence. It was found that the bleaching band occurs in the energy region of exciton ground state under excitation by femtosecond laser pulses. The complex dynamics of bleaching recovery is caused by the capture of electron on localized states, found using TSL. The stochastic model describing the dynamics of bleaching recovery is discussed. It is shown that the low efficiency of exciton luminescence is caused by the rapid capture of holes by luminescence centers.

  11. Bayesian deconvolution of scanning electron microscopy images using point-spread function estimation and non-local regularization.

    PubMed

    Roels, Joris; Aelterman, Jan; De Vylder, Jonas; Hiep Luong; Saeys, Yvan; Philips, Wilfried

    2016-08-01

    Microscopy is one of the most essential imaging techniques in life sciences. High-quality images are required in order to solve (potentially life-saving) biomedical research problems. Many microscopy techniques do not achieve sufficient resolution for these purposes, being limited by physical diffraction and hardware deficiencies. Electron microscopy addresses optical diffraction by measuring emitted or transmitted electrons instead of photons, yielding nanometer resolution. Despite pushing back the diffraction limit, blur should still be taken into account because of practical hardware imperfections and remaining electron diffraction. Deconvolution algorithms can remove some of the blur in post-processing but they depend on knowledge of the point-spread function (PSF) and should accurately regularize noise. Any errors in the estimated PSF or noise model will reduce their effectiveness. This paper proposes a new procedure to estimate the lateral component of the point spread function of a 3D scanning electron microscope more accurately. We also propose a Bayesian maximum a posteriori deconvolution algorithm with a non-local image prior which employs this PSF estimate and previously developed noise statistics. We demonstrate visual quality improvements and show that applying our method improves the quality of subsequent segmentation steps.

  12. Modeling biophysical and biological properties from the characteristics of the molecular electron density, electron localization and delocalization matrices, and the electrostatic potential.

    PubMed

    Matta, Chérif F

    2014-06-15

    The electron density and the electrostatic potential are fundamentally related to the molecular hamiltonian, and hence are the ultimate source of all properties in the ground- and excited-states. The advantages of using molecular descriptors derived from these fundamental scalar fields, both accessible from theory and from experiment, in the formulation of quantitative structure-to-activity and structure-to-property relationships, collectively abbreviated as QSAR, are discussed. A few such descriptors encode for a wide variety of properties including, for example, electronic transition energies, pK(a)'s, rates of ester hydrolysis, NMR chemical shifts, DNA dimers binding energies, π-stacking energies, toxicological indices, cytotoxicities, hepatotoxicities, carcinogenicities, partial molar volumes, partition coefficients (log P), hydrogen bond donor capacities, enzyme-substrate complementarities, bioisosterism, and regularities in the genetic code. Electronic fingerprinting from the topological analysis of the electron density is shown to be comparable and possibly superior to Hammett constants and can be used in conjunction with traditional bulk and liposolubility descriptors to accurately predict biological activities. A new class of descriptors obtained from the quantum theory of atoms in molecules' (QTAIM) localization and delocalization indices and bond properties, cast in matrix format, is shown to quantify transferability and molecular similarity meaningfully. Properties such as "interacting quantum atoms (IQA)" energies which are expressible into an interaction matrix of two body terms (and diagonal one body "self" terms, as IQA energies) can be used in the same manner. The proposed QSAR-type studies based on similarity distances derived from such matrix representatives of molecular structure necessitate extensive investigation before their utility is unequivocally established.

  13. Modeling Biophysical and Biological Properties From the Characteristics of the Molecular Electron Density, Electron Localization and Delocalization Matrices, and the Electrostatic Potential

    PubMed Central

    Matta*, Chérif F

    2014-01-01

    The electron density and the electrostatic potential are fundamentally related to the molecular hamiltonian, and hence are the ultimate source of all properties in the ground- and excited-states. The advantages of using molecular descriptors derived from these fundamental scalar fields, both accessible from theory and from experiment, in the formulation of quantitative structure-to-activity and structure-to-property relationships, collectively abbreviated as QSAR, are discussed. A few such descriptors encode for a wide variety of properties including, for example, electronic transition energies, pKa's, rates of ester hydrolysis, NMR chemical shifts, DNA dimers binding energies, π-stacking energies, toxicological indices, cytotoxicities, hepatotoxicities, carcinogenicities, partial molar volumes, partition coefficients (log P), hydrogen bond donor capacities, enzyme–substrate complementarities, bioisosterism, and regularities in the genetic code. Electronic fingerprinting from the topological analysis of the electron density is shown to be comparable and possibly superior to Hammett constants and can be used in conjunction with traditional bulk and liposolubility descriptors to accurately predict biological activities. A new class of descriptors obtained from the quantum theory of atoms in molecules' (QTAIM) localization and delocalization indices and bond properties, cast in matrix format, is shown to quantify transferability and molecular similarity meaningfully. Properties such as “interacting quantum atoms (IQA)” energies which are expressible into an interaction matrix of two body terms (and diagonal one body “self” terms, as IQA energies) can be used in the same manner. The proposed QSAR-type studies based on similarity distances derived from such matrix representatives of molecular structure necessitate extensive investigation before their utility is unequivocally established. © 2014 The Author and the Journal of Computational Chemistry Published

  14. Largely defocused probe scanning transmission electron microscopy for imaging local modulation of strain field in a hetero interface

    SciTech Connect

    Kim, Suhyun Jung, Younheum; Kim, Joong Jung; Lee, Sunyoung; Lee, Haebum; Oshima, Yoshifumi

    2014-10-13

    We present an innovative method for characterizing the strain field in three dimensions in a hetero interface. Largely defocused probe scanning transmission electron microscopy (LDP-STEM) was employed for imaging the inhomogeneous strain field in a germanium (Ge) layer deposited on a silicon (Si) substrate. In the LDP-STEM image, Ge-atomic columns that are relaxed or strained to the Si substrate in the Si/Ge hetero interface were observed to be distinguishable, allowing for the qualitative characterization of the coherency of the crystal growth. Our results revealed that the strain field is locally modulated along the in-plane direction in the Si/Ge hetero interface.

  15. Properties of Welded Joints from Alloy Zr - 2.5 % Nb after Electron-Beam Local Thermocycling

    NASA Astrophysics Data System (ADS)

    Semenov, A. N.; Plyshevskii, M. I.; Melyukov, V. V.; Korepanov, A. G.; Rassoshkina, N. S.; Uvarov, A. A.

    2014-03-01

    Modes of electron-beam local thermocycling treatment of welded joints of ∅ 88 × 4 mm pipes from alloy É125 (Zr - 2.5 % Nb) are tested. The structure of the welds is studied. The characteristics of mechanical properties are determined under tension and static and dynamic bending. The corrosion resistance is determined in long-term tests in an autoclave with water at 285 °C and in fast tests in an autoclave at 360 °C for 336 h in accordance with the International Standard.

  16. Toroidal mode number estimation of the edge-localized modes using the KSTAR 3-D electron cyclotron emission imaging system

    SciTech Connect

    Lee, J.; Yun, G. S. Lee, J. E.; Kim, M.; Choi, M. J.; Lee, W.; Park, H. K.; Domier, C. W.; Luhmann, N. C.; Sabbagh, S. A.; Park, Y. S.; Lee, S. G.; Bak, J. G.

    2014-06-15

    A new and more accurate technique is presented for determining the toroidal mode number n of edge-localized modes (ELMs) using two independent electron cyclotron emission imaging (ECEI) systems in the Korea Superconducting Tokamak Advanced Research (KSTAR) device. The technique involves the measurement of the poloidal spacing between adjacent ELM filaments, and of the pitch angle α{sub *} of filaments at the plasma outboard midplane. Equilibrium reconstruction verifies that α{sub *} is nearly constant and thus well-defined at the midplane edge. Estimates of n obtained using two ECEI systems agree well with n measured by the conventional technique employing an array of Mirnov coils.

  17. Toroidal mode number estimation of the edge-localized modes using the KSTAR 3-D electron cyclotron emission imaging system

    NASA Astrophysics Data System (ADS)

    Lee, J.; Yun, G. S.; Lee, J. E.; Kim, M.; Choi, M. J.; Lee, W.; Park, H. K.; Domier, C. W.; Luhmann, N. C.; Sabbagh, S. A.; Park, Y. S.; Lee, S. G.; Bak, J. G.

    2014-06-01

    A new and more accurate technique is presented for determining the toroidal mode number n of edge-localized modes (ELMs) using two independent electron cyclotron emission imaging (ECEI) systems in the Korea Superconducting Tokamak Advanced Research (KSTAR) device. The technique involves the measurement of the poloidal spacing between adjacent ELM filaments, and of the pitch angle α* of filaments at the plasma outboard midplane. Equilibrium reconstruction verifies that α* is nearly constant and thus well-defined at the midplane edge. Estimates of n obtained using two ECEI systems agree well with n measured by the conventional technique employing an array of Mirnov coils.

  18. Toroidal mode number estimation of the edge-localized modes using the KSTAR 3-D electron cyclotron emission imaging system.

    PubMed

    Lee, J; Yun, G S; Lee, J E; Kim, M; Choi, M J; Lee, W; Park, H K; Domier, C W; Luhmann, N C; Sabbagh, S A; Park, Y S; Lee, S G; Bak, J G

    2014-06-01

    A new and more accurate technique is presented for determining the toroidal mode number n of edge-localized modes (ELMs) using two independent electron cyclotron emission imaging (ECEI) systems in the Korea Superconducting Tokamak Advanced Research (KSTAR) device. The technique involves the measurement of the poloidal spacing between adjacent ELM filaments, and of the pitch angle α* of filaments at the plasma outboard midplane. Equilibrium reconstruction verifies that α* is nearly constant and thus well-defined at the midplane edge. Estimates of n obtained using two ECEI systems agree well with n measured by the conventional technique employing an array of Mirnov coils.

  19. Probing the structural and dynamical properties of liquid water with models including non-local electron correlation

    SciTech Connect

    Del Ben, Mauro Hutter, Jürg; VandeVondele, Joost

    2015-08-07

    Water is a ubiquitous liquid that displays a wide range of anomalous properties and has a delicate structure that challenges experiment and simulation alike. The various intermolecular interactions that play an important role, such as repulsion, polarization, hydrogen bonding, and van der Waals interactions, are often difficult to reproduce faithfully in atomistic models. Here, electronic structure theories including all these interactions at equal footing, which requires the inclusion of non-local electron correlation, are used to describe structure and dynamics of bulk liquid water. Isobaric-isothermal (NpT) ensemble simulations based on the Random Phase Approximation (RPA) yield excellent density (0.994 g/ml) and fair radial distribution functions, while various other density functional approximations produce scattered results (0.8-1.2 g/ml). Molecular dynamics simulation in the microcanonical (NVE) ensemble based on Møller-Plesset perturbation theory (MP2) yields dynamical properties in the condensed phase, namely, the infrared spectrum and diffusion constant. At the MP2 and RPA levels of theory, ice is correctly predicted to float on water, resolving one of the anomalies as resulting from a delicate balance between van der Waals and hydrogen bonding interactions. For several properties, obtaining quantitative agreement with experiment requires correction for nuclear quantum effects (NQEs), highlighting their importance, for structure, dynamics, and electronic properties. A computed NQE shift of 0.6 eV for the band gap and absorption spectrum illustrates the latter. Giving access to both structure and dynamics of condensed phase systems, non-local electron correlation will increasingly be used to study systems where weak interactions are of paramount importance.

  20. TiO{sub 2} nanotube arrays for photocatalysis: Effects of crystallinity, local order, and electronic structure

    SciTech Connect

    Liu, Jing; Hosseinpour, Pegah M.; Lewis, Laura H.; Luo, Si; Heiman, Don; Menon, Latika; Arena, Dario A.

    2015-03-15

    To furnish insight into correlations of electronic and local structure and photoactivity, arrays of short and long TiO{sub 2} nanotubes were synthesized by electrochemical anodization of Ti foil, followed by thermal treatment in O{sub 2} (oxidizing), Ar (inert), and H{sub 2} (reducing) environments. The physical and electronic structures of these nanotubes were probed with x-ray diffraction, scanning electron microscopy, and synchrotron-based x-ray absorption spectroscopy, and correlated with their photocatalytic properties. The photocatalytic activity of the nanotubes was evaluated by monitoring the degradation of methyl orange under UV-VIS light irradiation. Results show that upon annealing at 350 °C all as-anodized amorphous TiO{sub 2} nanotube samples partially transform to the anatase structure, with variations in the degree of crystallinity and in the concentration of local defects near the nanotubes' surface (∼5 nm) depending on the annealing conditions. Degradation of methyl orange was not detectable for the as-anodized TiO{sub 2} nanotubes regardless of their length. However, the annealed long nanotubes demonstrated detectable catalytic activity, which was more significant with the H{sub 2}-annealed nanotubes than with the Ar- and O{sub 2}-annealed nanotube samples. This enhanced photocatalytic response of the H{sub 2}-annealed long nanotubes relative to the other samples is positively correlated with the presence of a larger concentration of lattice defects (such as Ti{sup 3+} and anticipated oxygen vacancies) and a slightly lower degree of crystallinity near the nanotube surface. These physical and electronic structural attributes impact the efficacy of visible light absorption; moreover, the increased concentration of surface defects is postulated to promote the generation of hydroxyl radicals and thus accelerate the photodegradation of the methyl orange. The information obtained from this study provides unique insight into the role of the near

  1. Local environment effects in the magnetic properties and electronic structure of disordered FePt

    NASA Astrophysics Data System (ADS)

    Khan, Saleem Ayaz; Minár, Ján; Ebert, Hubert; Blaha, Peter; Šipr, Ondřej

    2017-01-01

    Local aspects of magnetism of disordered FePt are investigated by ab initio fully relativistic full-potential calculations, employing the supercell approach and the coherent potential approximation (CPA). The focus is on trends of the spin and orbital magnetic moments with chemical composition and with bond lengths around the Fe and Pt atoms. A small but distinct difference between average magnetic moments obtained when using the supercells and when relying on the CPA is identified and linked to the neglect of the Madelung potential in the CPA.

  2. Photoemission electron microscopy of localized surface plasmons in silver nanostructures at telecommunication wavelengths

    SciTech Connect

    Mårsell, Erik; Larsen, Esben W.; Arnold, Cord L.; Xu, Hongxing; Mauritsson, Johan; Mikkelsen, Anders

    2015-02-28

    We image the field enhancement at Ag nanostructures using femtosecond laser pulses with a center wavelength of 1.55 μm. Imaging is based on non-linear photoemission observed in a photoemission electron microscope (PEEM). The images are directly compared to ultra violet PEEM and scanning electron microscopy (SEM) imaging of the same structures. Further, we have carried out atomic scale scanning tunneling microscopy on the same type of Ag nanostructures and on the Au substrate. Measuring the photoelectron spectrum from individual Ag particles shows a larger contribution from higher order photoemission processes above the work function threshold than would be predicted by a fully perturbative model, consistent with recent results using shorter wavelengths. Investigating a wide selection of both Ag nanoparticles and nanowires, field enhancement is observed from 30% of the Ag nanoparticles and from none of the nanowires. No laser-induced damage is observed of the nanostructures neither during the PEEM experiments nor in subsequent SEM analysis. By direct comparison of SEM and PEEM images of the same nanostructures, we can conclude that the field enhancement is independent of the average nanostructure size and shape. Instead, we propose that the variations in observed field enhancement could originate from the wedge interface between the substrate and particles electrically connected to the substrate.

  3. Development of Local Oscillator Integrated Antenna Array for Electron Cyclotron Emission Imaging Diagnostics

    NASA Astrophysics Data System (ADS)

    Kuwahara, Daisuke; Ito, Naoki; Nagayama, Yoshio; Tsuchiya, Hayato; Yoshikawa, Masayuki; Kohagura, Junko; Yoshinaga, Tomokazu; Yamaguchi, Soichiro; Kogi, Yuichiro; Mase, Atsushi

    2016-10-01

    Microwave imaging systems include difficulties in terms of multi-channelization and cost. Our group solved these problems by developing a Horn-antenna Mixer Array (HMA), a 50 - 110 GHz 1-D heterodyne-type antenna array, which can be easily stacked as a 2-D receiving array. However, the HMA still evidenced problems owing to the requirement for local oscillation (LO) optics and an expensive high-power LO source. To solve this problem, we have developed an upgraded HMA, named the Local Integrated Antenna array (LIA), in which each channel has an internal LO supply using a frequency multiplier integrated circuit. Therefore, the proposed antenna array eliminates the need for both the LO optics and the high-power LO source. However, the LIA still has problems, that the instabilities of the sensitivity and poor channel isolation. This paper describes the principle of the LIA, and solutions of above-mentioned problems. This work is performed with the support and under the auspices of the NIFS Collaborative Research Program (NIFS15KOAP029 and NIFS16KUGM115).

  4. Resolving local voltage variations in opto-electronic devices with Kelvin probe force microscopy

    NASA Astrophysics Data System (ADS)

    Tennyson, Elizabeth; Garrett, Joseph; Munday, Jeremy; Leite, Marina

    We employ illuminated Kelvin probe force microscopy (KPFM) to spatially resolve the open-circuit voltage (Voc) of optoelectronic devices with nanoscale spatial resolution, >5 orders of magnitude better than previous methods. In illuminated-KPFM, we measure the difference in work function between the sample surface and the probe, termed the contact potential difference (CPD). By grounding the bottom contact of the solar cell to the AFM probe, the difference between the illuminated and the dark signals is proportional to quasi-Fermi level splitting and, therefore, the Voc. We apply our scanning probe technique to a variety of solar cell materials, including polycrystalline CIGS, where we resolve local variations in Voc >150 mV. We use heterodyne-KPFM (where we map 1 μm2 in 16 seconds) to probe hybrid perovskites solar cells, and quantify in real-time the voltage changes upon material relaxation after illumination. This metrology yields new insights into the local electrical properties of solar cells, and can be expanded to any optoelectronic device.

  5. Localized holes and delocalized electrons in photoexcited inorganic perovskites: Watching each atomic actor by picosecond X-ray absorption spectroscopy.

    PubMed

    Santomauro, Fabio G; Grilj, Jakob; Mewes, Lars; Nedelcu, Georgian; Yakunin, Sergii; Rossi, Thomas; Capano, Gloria; Al Haddad, André; Budarz, James; Kinschel, Dominik; Ferreira, Dario S; Rossi, Giacomo; Gutierrez Tovar, Mario; Grolimund, Daniel; Samson, Valerie; Nachtegaal, Maarten; Smolentsev, Grigory; Kovalenko, Maksym V; Chergui, Majed

    2017-07-01

    We report on an element-selective study of the fate of charge carriers in photoexcited inorganic CsPbBr3 and CsPb(ClBr)3 perovskite nanocrystals in toluene solutions using time-resolved X-ray absorption spectroscopy with 80 ps time resolution. Probing the Br K-edge, the Pb L3-edge, and the Cs L2-edge, we find that holes in the valence band are localized at Br atoms, forming small polarons, while electrons appear as delocalized in the conduction band. No signature of either electronic or structural changes is observed at the Cs L2-edge. The results at the Br and Pb edges suggest the existence of a weakly localized exciton, while the absence of signatures at the Cs edge indicates that the Cs(+) cation plays no role in the charge transport, at least beyond 80 ps. This first, time-resolved element-specific study of perovskites helps understand the rather modest charge carrier mobilities in these materials.

  6. Localized holes and delocalized electrons in photoexcited inorganic perovskites: Watching each atomic actor by picosecond X-ray absorption spectroscopy

    PubMed Central

    Santomauro, Fabio G.; Grilj, Jakob; Mewes, Lars; Nedelcu, Georgian; Yakunin, Sergii; Rossi, Thomas; Capano, Gloria; Al Haddad, André; Budarz, James; Kinschel, Dominik; Ferreira, Dario S.; Rossi, Giacomo; Gutierrez Tovar, Mario; Grolimund, Daniel; Samson, Valerie; Nachtegaal, Maarten; Smolentsev, Grigory; Kovalenko, Maksym V.; Chergui, Majed

    2016-01-01

    We report on an element-selective study of the fate of charge carriers in photoexcited inorganic CsPbBr3 and CsPb(ClBr)3 perovskite nanocrystals in toluene solutions using time-resolved X-ray absorption spectroscopy with 80 ps time resolution. Probing the Br K-edge, the Pb L3-edge, and the Cs L2-edge, we find that holes in the valence band are localized at Br atoms, forming small polarons, while electrons appear as delocalized in the conduction band. No signature of either electronic or structural changes is observed at the Cs L2-edge. The results at the Br and Pb edges suggest the existence of a weakly localized exciton, while the absence of signatures at the Cs edge indicates that the Cs+ cation plays no role in the charge transport, at least beyond 80 ps. This first, time-resolved element-specific study of perovskites helps understand the rather modest charge carrier mobilities in these materials. PMID:28083541

  7. The accuracy of timed maximum local anaesthetic dose calculations with an electronic calculator, nomogram, and pen and paper.

    PubMed

    Walker, J D; Williams, N; Williams, D J

    2017-02-24

    Forty anaesthetists calculated maximum permissible doses of eight local anaesthetic formulations for simulated patients three times with three methods: an electronic calculator; nomogram; and pen and paper. Correct dose calculations with the nomogram (85/120) were more frequent than with the calculator (71/120) or pen and paper (57/120), Bayes Factor 4 and 287, p = 0.01 and p = 0.0003, respectively. The rates of calculations at least 120% the recommended dose with each method were different, Bayes Factor 7.9, p = 0.0007: 14/120 with the calculator; 5/120 with the nomogram; 13/120 with pen and paper. The median (IQR [range]) speed of calculation with pen and paper, 38.0 (25.0-56.3 [5-142]) s, was slower than with the calculator, 24.5 (17.8-37.5 [6-204]) s, p = 0.0001, or nomogram, 23.0 (18.0-29.0 [4-100]) s, p = 1 × 10(-7) . Local anaesthetic dose calculations with the nomogram were more accurate than with an electronic calculator or pen and paper and were faster than with pen and paper.

  8. Nonlinear response of magnetic islands to localized electron cyclotron current injection

    SciTech Connect

    Borgogno, D.; Comisso, L.; Grasso, D.; Lazzaro, E.

    2014-06-15

    The magnetic island evolution under the action of a current generated externally by electron cyclotron wave beams is studied using a reduced resistive magnetohydrodynamics plasma model. The use of a two-dimensional reconnection model shows novel features of the actual nonlinear evolution as compared to the zero-dimensional model of the generalized Rutherford equation. When the radio frequency control is applied to a small magnetic island, the complete annihilation of the island width is followed by a spatial phase shift of the island, referred as “flip” instability. On the other hand, a current-drive injection in a large nonlinear island can be accompanied by the occurrence of a Kelvin-Helmholtz instability. These effects need to be taken into account in designing tearing mode control systems based on radio frequency current-drive.

  9. A theory of local and global processes which affect solar wind electrons. 1: The origin of typical 1 AU velocity distribution functions: Steady state theory

    NASA Technical Reports Server (NTRS)

    Scudder, J. D.

    1978-01-01

    A detailed first principle kinetic theory for electrons which is neither a classical fluid treatment nor an exospheric calculation is presented. This theory illustrates the global and local properties of the solar wind expansion that shape the observed features of the electron distribution function, such as its bifurcation, its skewness and the differential temperatures of the thermal and suprathermal subpopulations. Coulomb collisions are substantial mediators of the interplanetary electron velocity distribution function and they place a zone for a bifurcation of the electron distribution function deep in the corona. The local cause and effect precept which permeates the physics of denser media is modified for electrons in the solar wind. The local form of transport laws and equations of state which apply to collision dominated plasmas are replaced with global relations that explicitly depend on the relative position of the observer to the boundaries of the system.

  10. Self-consistent GW: All-electron implementation with localized basis functions

    NASA Astrophysics Data System (ADS)

    Caruso, Fabio; Rinke, Patrick; Ren, Xinguo; Rubio, Angel; Scheffler, Matthias

    2013-08-01

    This paper describes an all-electron implementation of the self-consistent GW (sc-GW) approach—i.e., based on the solution of the Dyson equation—in an all-electron numeric atom-centered orbital basis set. We cast Hedin's equations into a matrix form that is suitable for numerical calculations by means of (i) the resolution-of-identity technique to handle four-center integrals and (ii) a basis representation for the imaginary-frequency dependence of dynamical operators. In contrast to perturbative G0W0, sc-GW provides a consistent framework for ground- and excited-state properties and facilitates an unbiased assessment of the GW approximation. For excited states, we benchmark sc-GW for five molecules relevant for organic photovoltaic applications: thiophene, benzothiazole, 1,2,5-thiadiazole, naphthalene, and tetrathiafulvalene. At self-consistency, the quasiparticle energies are found to be in good agreement with experiment and, on average, more accurate than G0W0 based on Hartree-Fock or density-functional theory with the Perdew-Burke-Ernzerhof exchange-correlation functional. Based on the Galitskii-Migdal total energy, structural properties are investigated for a set of diatomic molecules. For binding energies, bond lengths, and vibrational frequencies sc-GW and G0W0 achieve a comparable performance, which is, however, not as good as that of exact-exchange plus correlation in the random-phase approximation and its advancement to renormalized second-order perturbation theory. Finally, the improved description of dipole moments for a small set of diatomic molecules demonstrates the quality of the sc-GW ground-state density.

  11. Electronic, structural and transport properties of (almost) rare-earth-like actinide hydrides

    SciTech Connect

    Ward, J.W.; Cort, B.; Goldstone, J.A.; Lawson, A.C.; Cox, L.E. ); Haire, R.G. )

    1990-01-01

    By the virtue of broad-band, hybridized 5f-electron behavior, the hydride systems for Pa and U exhibit unique properties and structures, the actinide metal atoms existing in different states. A sudden change at Np to more rare-earth-like behavior implies a major change in electronic structure. There are both many parallels but also enigmas for the Np + H and Pu + H systems. Electrical resistivities are large and complex with temperature. Low-temperature structural transitions as studied by neutron diffraction help elucidate some of these effects. Phonon spectra are quite rare-earth-like, and XPS data imply a metal atom with mostly d-screened core levels. Then it is at americium, where fully localized and corelike 5f electrons are found, that we look finally for true rare-earth-like behavior, which should include a large drop in electrical resistivity. 33 refs., 7 figs., 1 tab.

  12. Local structural evidence for strong electronic correlations in spinel LiRh2O4

    NASA Astrophysics Data System (ADS)

    Knox, K. R.; Abeykoon, A. M. M.; Zheng, H.; Yin, W.-G.; Tsvelik, A. M.; Mitchell, J. F.; Billinge, S. J. L.; Bozin, E. S.

    2013-11-01

    The local structure of the spinel LiRh2O4 has been studied using atomic-pair distribution function analysis of powder x-ray diffraction data. This measurement is sensitive to the presence of short Rh-Rh bonds that form due to dimerization of Rh4+ ions on the pyrochlore sublattice, independent of the existence of long-range order. We show that structural dimers exist in the low-temperature phase, as previously supposed, with a bond shortening of Δr˜0.15 Å. The dimers persist up to 350 K, well above the insulator-metal transition, with Δr decreasing in magnitude on warming. Such behavior is inconsistent with the Fermi-surface nesting-driven Peierls transition model. Instead, we argue that LiRh2O4 should properly be described as a strongly correlated system.

  13. Localization of LHCP II in the Golgi of synchronized Euglena cells by immuno-electron microscopy

    SciTech Connect

    Osafune, Tetsuaki ); Schiff, J.A. ); Hase, E. )

    1990-05-01

    We have previously localized LHCP II apoprotein in the Golgi thylakoids of Euglena gracilis (bacillaris Z strain) using specific antibody protein A-gold, during plastid development induction of LHCP II synthesis by increased light intensity. Using light/dark synchronized cells we now show that thylakoids are always immunoreactive. There is no reaction in the Golgi at 0 h. (beginning of light period), but immunoreaction appears in the Golgi soon thereafter, rises to a peak at 8 h. declines again to zero by 16 h. (2 h. into the dark period). The peak in immunoreaction in the Golgi immediately precedes the peak in {sup 14}C-labeling of cellular LHCP, supporting our suggestion that processing in the Golgi precedes deposition of LHCP II apoprotein in the thylakoids. Synchronized mutant Gr{sub 1} which lacks LHCP apoprotein fails to show immunoreaction in the Golgi or thylakoids at any stage.

  14. Local Health Departments' Partners and Challenges in Electronic Exchange of Health Information

    PubMed Central

    Vest, Joshua R.; Lovelace, Kay; McCullough, J. Mac

    2016-01-01

    Background: Unprecedented amounts of data are produced by the health care and other sectors, presenting opportunities for local health departments (LHDs) to access these data. LHDs will need to participate in health information exchange (HIE) with a number of partners in order to benefit from these data resources. LHDs' participation in HIEs with specific partners has not been studied. Objectives: To describe the level of and challenges in LHD participation in HIE with other partners, and variation by LHD population size and governance type. Data and Methods: This research uses data from the 2015 Informatics Capacity and Needs Assessment Survey, with a target population of all LHDs in the United States. A representative sample of 650 LHDs was drawn using a stratified random sampling design. A total of 324 completed responses were received with a 50% response rate. Survey data were cleaned, and bivariate comparisons were conducted using χ2 and Somer's D. Results: Substantial variation existed in LHDs' participation in HIE by type of exchange partner. Although 71% participated in HIE with the state departments of health, only 12% with jail/correctional health, 14% with health or county-based purchasing plans, and 15% with home health agencies. Compared with large LHDs (jurisdiction populations of ≥500 000), smaller LHDs were more likely to participate in HIE with state departments of health, but less likely with other exchange partners. The challenges to HIE participation were technological, and organizational/interorganizational in nature and variation existed by LHDs' population size and governance structure with respect to state authority. Conclusions: Local public health agencies more commonly participate in HIE with some partners, but may need to improve HIE with many others. National strategies targeting an increase in HIE of LHDs may use our findings to focus those initiatives. PMID:27684617

  15. Electron spin polarization transfer to the charge-separated state from locally excited triplet configuration: theory and its application to characterization of geometry and electronic coupling in the electron donor-acceptor system.

    PubMed

    Kobori, Yasuhiro; Fuki, Masaaki; Murai, Hisao

    2010-11-18

    We present a theoretical model of analysis of the time-resolved electron paramagnetic resonance (TREPR) spectrum of the charge-separated (CS) state generated by the photoinduced electron transfer (ET) reaction via the locally excited triplet state in an electron donor-acceptor (D-A) system with a fixed molecular orientation. We show, by the stochastic-Liouville equation, that chemically induced dynamic electron polarization (CIDEP) of the triplet mechanism is explained by lack of transfer of quantum coherence terms in the primary triplet spin state, resulting in net emissive or absorptive electron spin polarization (ESP) which is dependent on anisotropy of the singlet-triplet intersystem crossing in the precursor excited state. This disappearance of the coherence is clearly shown to occur when the photoinduced ET rate is smaller than the angular frequency of the Zeeman splitting: the transferred coherence terms are averaged to be zero due to effective quantum oscillations during the time that the chemical reaction proceeds. The above theory has been applied to elucidate the molecular geometries and spin-spin exchange interactions (2J) of the CS states for both folded and extended conformers by computer simulations of TREPR spectra of the zinc porphyrin-fullerene dyad (ZnP-C(60)) bridged by diphenyldisilane. On the extended conformation, the electronic coupling is estimated from the 2J value. It has been revealed that the coupling term is smaller than the reported electronic interactions of the porphyrin-C(60) systems bridged by diphenylamide spacers. The difference in the electronic couplings has been explained by the difference in the LUMO levels of the bridge moieties that mediate the superexchange coupling for the long-range ET reaction.

  16. Local unitary transformation method toward practical electron correlation calculations with scalar relativistic effect in large-scale molecules

    SciTech Connect

    Seino, Junji; Nakai, Hiromi

    2013-07-21

    In order to perform practical electron correlation calculations, the local unitary transformation (LUT) scheme at the spin-free infinite-order Douglas–Kroll–Hess (IODKH) level [J. Seino and H. Nakai, J. Chem. Phys.136, 244102 (2012); J. Seino and H. Nakai, J. Chem. Phys.137, 144101 (2012)], which is based on the locality of relativistic effects, has been combined with the linear-scaling divide-and-conquer (DC)-based Hartree–Fock (HF) and electron correlation methods, such as the second-order Møller–Plesset (MP2) and the coupled cluster theories with single and double excitations (CCSD). Numerical applications in hydrogen halide molecules, (HX){sub n} (X = F, Cl, Br, and I), coinage metal chain systems, M{sub n} (M = Cu and Ag), and platinum-terminated polyynediyl chain, trans,trans-((p-CH{sub 3}C{sub 6}H{sub 4}){sub 3}P){sub 2}(C{sub 6}H{sub 5})Pt(C≡C){sub 4}Pt(C{sub 6}H{sub 5})((p-CH{sub 3}C{sub 6}H{sub 4}){sub 3}P){sub 2}, clarified that the present methods, namely DC-HF, MP2, and CCSD with the LUT-IODKH Hamiltonian, reproduce the results obtained using conventional methods with small computational costs. The combination of both LUT and DC techniques could be the first approach that achieves overall quasi-linear-scaling with a small prefactor for relativistic electron correlation calculations.

  17. Planar metal plasmon waveguides: frequency-dependent dispersion, propagation, localization, and loss beyond the free electron model

    NASA Astrophysics Data System (ADS)

    Dionne, J. A.; Sweatlock, L. A.; Atwater, H. A.; Polman, A.

    2005-08-01

    A numerical analysis of surface plasmon dispersion, propagation, and localization on smooth lossy films is presented. Particular attention is given to determining wavelength-dependent behavior of thin Ag slab waveguides embedded in a symmetric SiO2 environment. Rather than considering Ag as a damped free electron gas, the metal is defined by the experimentally determined optical constants of Johnson and Christy and Palik. As in free electron gas models, analytic dispersion results indicate a splitting of plasmon modes—corresponding to symmetric and antisymmetric field distributions—as film thickness is decreased below 50nm . However, unlike free electron gas models, the surface plasmon wave vector remains finite at resonance with the antisymmetric-field plasmon converging to a pure photon mode for very thin films. In addition, allowed excitation modes are found to exist between the bound and radiative branches of the dispersion curve. The propagation characteristics of all modes are determined, and for thin films (depending upon electric field symmetry), propagation distances range from microns to centimeters in the near infrared. Propagation distances are correlated with both the field decay (skin depth) and energy density distribution in the metal and surrounding dielectric. While the energy density of most long-range surface plasmons exhibits a broad spatial extent with limited confinement in the waveguide, it is found that high-field confinement does not necessarily limit propagation. In fact, enhanced propagation is observed for silver films at ultraviolet wavelengths despite strong field localization in the metal. The surface plasmon characteristics described in this paper provide a numerical springboard for engineering nanoscale metal plasmon waveguides, and the results may provide a new avenue for integrated optoelectronic applications.

  18. Olefin epoxidation by molybdenum peroxo compound: molecular mechanism characterized by the electron localization function and catastrophe theory.

    PubMed

    Berski, Slawomir; Sensato, Fabrício R; Polo, Victor; Andrés, Juan; Safont, V S

    2011-02-03

    The oxygen atom transfer reaction from the Mimoun-type complex MoO(η(2)-O(2))(2)OPH(3) to ethylene C(2)H(4) affording oxirane C(2)H(4)O has been investigated within the framework of the Bonding Evolution Theory in which the corresponding molecular mechanism is characterized by the topological analysis of the electron localization function (ELF) and Thom's catastrophe theory (CT). Topological analysis of ELF and electron density analysis reveals that all Mo-O bonds in MoO(η(2)-O(2))(2)OPH(3) and MoO(2)(η(2)-O(2))OPH(3) belong to closed-shell type interactions though negative values of total energy densities E(e)(r(BCP)) imply some covalent contribution. The peroxo O(i)-O(j) bonds are characterized as charge-shift or protocovalent species in which pairs of monosynaptic basins V(3)(O(i)), V(3)(O(j)) with a small electron population of ~0.25e each, are localized between core basins C(O(i)), C(O(j)). The oxygen transfer reaction from molybdenum diperoxo complex MoO(η(2)-O(2))(2)OPH(3) to C(2)H(4) system can be described by the following consecutive chemical events: (a) protocovalent peroxo O(2)-O(1) bond breaking, (b) reduction of the double C(1)=C(2) bond to single C(1)-C(2) bond in ethylene, (c) displacement of oxygen O(1) with two nonbonding basins, V(i=1,2)(O(1)), (d) increase of a number of the nonbonding basins to three (V(i=1,2,4)(O(1))); (e) reorganization and reduction in the number of nonbonding basis to two basins (V(i=1,4)(O(1))) resembling the ELF-topology of the nonbonding electron density in oxirane, (e) formation of the first O(1)-C(2) bond in oxirane, (f) C(2)-O(1)-C(2) ring closure, (g) formation of singular nonbonding basin V(O(2)) in new Mo=O(2) bond. The oxygen atom is transferred as an anionic moiety carrying a rather small electronic charge ranging from 0.5 to 0.7e.

  19. Improved beta (local beta >1) and density in electron cyclotron resonance heating on the RT-1 magnetosphere plasma

    NASA Astrophysics Data System (ADS)

    Nishiura, M.; Yoshida, Z.; Saitoh, H.; Yano, Y.; Kawazura, Y.; Nogami, T.; Yamasaki, M.; Mushiake, T.; Kashyap, A.

    2015-05-01

    This study reports the recent progress in improved plasma parameters of the RT-1 device. Increased input power and the optimized polarization of electron cyclotron resonance heating (ECRH) with an 8.2 GHz klystron produce a significant increase in electron beta, which is evaluated by an equilibrium analysis of the Grad-Shafranov equation. The peak value of the local electron beta βe is found to exceed 1. In the high-beta and high-density regime, the density limit is observed for H, D and He plasmas. The line-averaged density is close to the cutoff density for 8.2 GHz ECRH. When the filling gas pressure is increased, the density limit still exists even in the low-beta region. This result indicates that the density limit is caused by the cutoff density rather than the beta limit. From the analysis of interferometer data, we found that inward diffusion causes a peaked density profile beyond the cutoff density.

  20. Electronic resonance and local field effects on the nonlinear optical activity of H-aggregate-forming stilbazolium amphiphiles

    SciTech Connect

    Xu, Z.; Lu, W.; Bohn, P.W.

    1995-05-04

    Stilbazolium dyes, which form H-aggregates upon condensation at the air-water interface, typically display nonlinear optical (NLO) activity far below what would be predicted on the basis of their large intrinsic molecular hyperpolarizability, {beta}. Three separate hypothesis have been put forward to explain this observation: structural inversion to produce a centrosymmetric head-to-tail structure, local field effects, which act to reduce the effective magnitude of the nonlinear driving field, and changes in electronic structure, which shift the electronic resonance frequencies for the aggregates. Investigation of the linear and nonlinear spectroscopy of the dye 4-(4-dihexadecylaminostyryl)-N-methylpyridinium iodide were performed on a series of samples in which the aggregation state of the structure was changed systematically, but without changing the composition of the film. These experiments show that, for this particular dye, changes in electronic structure upon aggregation comprise the most important factor in determining the reduction in second harmonic generation (SHG) efficiency of the aggregate. 23 refs., 4 figs.

  1. Forging Fast Ion Conducting Nanochannels with Swift Heavy Ions: The Correlated Role of Local Electronic and Atomic Structure

    DOE PAGES

    Sachan, Ritesh; Cooper, Valentino R.; Liu, Bin; ...

    2016-12-19

    Atomically disordered oxides have attracted significant attention in recent years due to the possibility of enhanced ionic conductivity. However, the correlation between atomic disorder, corresponding electronic structure, and the resulting oxygen diffusivity is not well understood. The disordered variants of the ordered pyrochlore structure in gadolinium titanate (Gd2Ti2O7) are seen as a particularly interesting prospect due to intrinsic presence of a vacant oxygen site in the unit atomic structure, which could provide a channel for fast oxygen conduction. In this paper, we provide insights into the subangstrom scale on the disordering-induced variations in the local atomic environment and its effectmore » on the electronic structure in high-energy ion irradiation-induced disordered nanochannels, which can be utilized as pathways for fast oxygen ion transport. With the help of an atomic plane-by-plane-resolved analyses, the work shows how the presence of various types of TiOx polyhedral that exist in the amorphous and disordered crystalline phase modify the electronic structures relative to the ordered pyrochlore phase in Gd2Ti2O7. Finally, the correlated molecular dynamics simulations on the disordered structures show a remarkable enhancement in oxygen diffusivity as compared with ordered pyrochlore lattice and make that a suitable candidate for applications requiring fast oxygen conduction.« less

  2. Forging Fast Ion Conducting Nanochannels with Swift Heavy Ions: The Correlated Role of Local Electronic and Atomic Structure

    SciTech Connect

    Sachan, Ritesh; Cooper, Valentino R.; Liu, Bin; Aidhy, Dilpuneet S.; Voas, Brian K.; Lang, Maik; Ou, Xin; Trautmann, Christina; Zhang, Yanwen; Chisholm, Matthew F.; Weber, William J.

    2016-12-19

    Atomically disordered oxides have attracted significant attention in recent years due to the possibility of enhanced ionic conductivity. However, the correlation between atomic disorder, corresponding electronic structure, and the resulting oxygen diffusivity is not well understood. The disordered variants of the ordered pyrochlore structure in gadolinium titanate (Gd2Ti2O7) are seen as a particularly interesting prospect due to intrinsic presence of a vacant oxygen site in the unit atomic structure, which could provide a channel for fast oxygen conduction. In this paper, we provide insights into the subangstrom scale on the disordering-induced variations in the local atomic environment and its effect on the electronic structure in high-energy ion irradiation-induced disordered nanochannels, which can be utilized as pathways for fast oxygen ion transport. With the help of an atomic plane-by-plane-resolved analyses, the work shows how the presence of various types of TiOx polyhedral that exist in the amorphous and disordered crystalline phase modify the electronic structures relative to the ordered pyrochlore phase in Gd2Ti2O7. Finally, the correlated molecular dynamics simulations on the disordered structures show a remarkable enhancement in oxygen diffusivity as compared with ordered pyrochlore lattice and make that a suitable candidate for applications requiring fast oxygen conduction.

  3. Localization-delocalization transition of electrons at the percolation threshold of semiconductor GaAs1–xNx alloys: The appearance of a mobility edge

    DOE PAGES

    Alberi, K.; Fluegel, B.; Beaton, D. A.; ...

    2012-07-09

    Electrons in semiconductor alloys have generally been described in terms of Bloch states that evolve from constructive interference of electron waves scattering from perfectly periodic potentials, despite the loss of structural periodicity that occurs on alloying. Using the semiconductor alloy GaAs₁₋xNx as a prototype, we demonstrate a localized to delocalized transition of the electronic states at a percolation threshold, the emergence of a mobility edge, and the onset of an abrupt perturbation to the host GaAs electronic structure, shedding light on the evolution of electronic structure in these abnormal alloys.

  4. Evaluation of regulatory genetic variants in POU5F1 and risk of congenital heart disease in Han Chinese

    NASA Astrophysics Data System (ADS)

    Lin, Yuan; Ding, Chenyue; Zhang, Kai; Ni, Bixian; da, Min; Hu, Liang; Hu, Yuanli; Xu, Jing; Wang, Xiaowei; Chen, Yijiang; Mo, Xuming; Cui, Yugui; Shen, Hongbing; Sha, Jiahao; Liu, Jiayin; Hu, Zhibin

    2015-10-01

    OCT4 is a transcription factor of the POU family, which plays a key role in embryonic development and stem cell pluripotency. Previous studies have shown that Oct4 is required for cardiomyocyte differentiation in mice and its depletion could result in cardiac morphogenesis in embryo. However, whether the genetic variations in OCT4 coding gene, POU5F1, confer the predisposition to congenital heart disease (CHD) is unclear. This study sought to investigate the associations between low-frequency (defined here as having minor allele frequency (MAF) between 0.1%-5%) and rare (MAF below 0.1%) variants with potential function in POU5F1 and risk of CHD. We conducted association analysis in a two-stage case-control study with a total of 2,720 CHD cases and 3,331 controls in Chinese. The low-frequency variant rs3130933 was observed to be associated with a significantly increased risk of CHD [additive model: adjusted odds ratio (OR) = 2.15, adjusted P = 3.37 × 10-6]. Furthermore, luciferase activity assay showed that the variant A allele led to significantly lower expression levels as compared to the G allele. These findings indicate for the first time that low-frequency functional variant in POU5F1 may contribute to the risk of congenital heart malformations.

  5. Asymptotic Near Nucleus Structure of the Electron-Interaction Potential in Local Effective Potential Theories

    NASA Astrophysics Data System (ADS)

    Sahni, Viraht; Qian, Zhixin

    2007-03-01

    In previous work, it has been shown that for spherically symmetric or sphericalized systems, the asymptotic near nucleus structure of the electron-interaction potential is vee(r) = vee(0) + βr + γr^2. In this paper we prove via time-independent Quantal Density Functional Theory[1](Q-DFT): (i) correlations due to the Pauli exclusion principle and Coulomb repulsion do not contribute to the linear structure;(ii) these Pauli and Coulomb correlations contribute quadratically; (iii) the linear structure is solely due to Correlation-Kinetic effects, the coefficient β being determined analytically. By application of adiabatic coupling constant perturbation theory via QDFT we further prove: (iv) the Kohn-Sham (KS-DFT) `exchange' potential vx(r) approaches the nucleus linearly, this structure being due solely to lowest- order Correlation-Kinetic effects: (v) the KS-DFT `correlation' potential vc(r) also approaches the nucleus linearly, being solely due to higher-order Correlation-Kinetic contributions. The above conclusions are equally valid for system of arbitrary symmetry, provided spherical averages of the properties are employed. 1 Quantal Density Functional Theory, V. Sahni (Springer-Verlag 2004)

  6. Non-local Lateral electron heat transport from one or more hot spots.

    NASA Astrophysics Data System (ADS)

    Matte, Jean-Pierre; Alouani-Bibi, Fathallah

    2000-10-01

    Fokker-Planck simulations of collisional absorption and transport in long scale length, preformed, underdense plasmas heated by intense and narrow laser hot spots, as in certain recent LANL experiments [1], are presented. The temperature profiles compared with those obtained from flux limited or delocalized heat flow models. For the former, the temperature peaks can be matched only if a very low flux limiter is used, and even then, the scale length of the temperature profile is always overestimated. The electron distribution function will be characterized, and compared to the "DLM" shape, exp(-(v/u)^m), [2] and the best fit for m will be compared to older formulas for uniform plasmas [2]. Hydrodynamic effects are also addressed with simulations which include ion motion; both with and without the ponderomotive force. The enhancement of sound velocity due to the "DLM" shape [3] inside the hot spot will be quantified. [1] J.A. Cobble et al., Phys. Plasmas, 7, 323 (2000) [2] J.P. Matte et al., Plasma Phys. and Contr. Fusion, 30, 1665, (1988) [3] B. B. Afeyan et al., PRL 81, 2322 (1998).

  7. Localization of single-chain interruptions in bacteriophage T5 DNA I. Electron microscopic studies.

    PubMed Central

    Scheible, P P; Rhoades, E A; Rhoades, M

    1977-01-01

    Bacteriophage T5 DNA was examined in an electron microscope after limited digestion with exonuclease III from Escherichia coli. The effect of the exonuclease treatment was to convert each naturally occurring single-chain interruption in T5 DNA into a short segment of single-stranded DNA. The locations of these segments were determined for T5st(+) DNA, T5st(0) DNA, and fragments of T5st(0) DNA generated by EcoRI restriction endonuclease. The results indicate that single-chain interruptions occurr in a variable, but nonrandom, manner in T5 DNA. T5st(+) DNA has four principal interruptions located at sites approximately 7.9, 18.5, 32.6, and 64.8% from one end of the molecule. Interruptions occur at these sites in 80 to 90% of the population. A large number of additional sites, located primarily at the ends of the DNA, contain interruptions at lower frequencies. The average number of interruptions per genome, as determined by this method, is 8. A similar distribution of breaks occurs in T5st(0) DNA, except that the 32.6% site is missing. At least one of the principal interruptions is reproducibly located within an interval of 0.2% of the entire DNA. Images PMID:330881

  8. IMPORTANCE OF FULL COULOMB INTERACTIONS FOR UNDERSTANDING THE ELECTRONIC STRUCTURE OF DELTA-Pu

    SciTech Connect

    Gorelov, E; Kolorenc, J; Wehling, T; Hafermann, H; Lichtenstein, A I; Shick, A B; Rubtsov, A N; Katsnelson, M I; Landa, A; McMahan, A K

    2010-04-01

    The solid-state properties of most elements are now well understood on the basis of quantum physics - with few exceptions, notably the element number 94, plutonium. Plutonium has six crystalline phases at ambient pressure, some of which are separated by unusual phase transitions with large discontinuities in volume, exhibit negative thermal expansion coefficients, or form exotic low-symmetry structures. The main challenge to explain these anomalous properties is that the characteristic ingredient of actinides, the 5f electronic states, are in the cross-over regime between the localized and delocalized (itinerant) behaviour in Pu. The early part of the actinide series with the 5f states being itinerant, i.e. part of the metallic bond, culminates with Pu; starting with Am (Z = 95), the 5f states are localized, nonbonding, and resemble the 4f states in lanthanides. Both itinerant and localized regimes are well covered by existing theories, but they cannot be simply interpolated due to the importance of dynamical electron-electron correlations. Here we present accurate quantum Monte Carlo calculations achieving previously inaccessible resolution. Obtained results demonstrate that interplay of the full Coulomb interaction vertex with spin-orbital coupling is crucial for understanding the experimentally observed spectral properties of plutonium near the Fermi level.

  9. Local electronic structure of aqueous zinc acetate: oxygen K-edge X-ray absorption and emission spectroscopy on micro-jets.

    PubMed

    Golnak, Ronny; Atak, Kaan; Suljoti, Edlira; Hodeck, Kai F; Lange, Kathrin M; Soldatov, Mikhail A; Engel, Nicholas; Aziz, Emad F

    2013-06-07

    Oxygen K-edge X-ray absorption, emission, and resonant inelastic X-ray scattering spectra were measured to site selectively gain insights into the electronic structure of aqueous zinc acetate solution. The character of the acetate ion and the influence of zinc and water on its local electronic structure are discussed.

  10. Multiphoton-generated localized electron plasma for membrane permeability modification in single cells

    NASA Astrophysics Data System (ADS)

    Merritt, T.; Leblanc, M.; McMillan, J.; Westwood, J.; Khodaparast, G. A.

    2014-03-01

    Successful incorporation of a specific macromolecule into a single cell would be ideal for characterizing trafficking dynamics through plasmodesmata or for studying intracellular localizations. Here, we demonstrate NIR femtosecond laser-mediated infiltration of a membrane impermeable dextran-conjugated dye into living cells of Arabidopsis thaliana seedling stems. Based on the reactions of fluorescing vacuoles of transgenic cells and artificial cell walls comprised of nanocellulose, laser intensity and exposure time were adjusted to avoid deleterious effects. Using these plant-tailored laser parameters, cells were injected with the fluorophores and long-term dye retention was observed, all while preserving vital cell functions. This method is ideal for studies concerning cell-to-cell interactions and potentially paves the way for introducing transgenes to specific cells. This work was supported by NSF award IOS-0843372 to JHW, with additional support from and U.S. Department of Agriculture Hatch Project no. 135997, and by the Institute of Critical Technology and Applied Sciences (ICTAS) at Virginia Tech.

  11. Photophysical properties of ESIPT inspired fluorescent 2-(2-hydroxyphenyl)-6-methylimidazo[4,5-f]isoindole-5,7(1H,6H)-dione and its derivative: Experimental and DFT based approach

    NASA Astrophysics Data System (ADS)

    Deshmukh, Mininath S.; Sekar, Nagaiyan

    2015-01-01

    The excited-state intramolecular proton transfer chromophores 2-(2-hydroxyphenyl)-6-methylimidazo[4,5-f]isoindole-5,7(1H,6H)-dione and 2-(4-(diethylamino)-2-hydroxyphenyl)-6-methylimidazo[4,5-f]isoindole-5,7(1H,6H)-dione are synthesized from 4,5-diamino-N-methylphthalimide. The photophysical behavior of the synthesized chromophores was studied using UV-visible and fluorescence spectroscopy in the polar and non-polar solvents. The synthesized o-hydroxyphenyl benzimidazole derivatives are fluorescent and very sensitive to the solvent polarity. These dyes are thermally stable up to 317 °C. Density Functional Theory computations have been used to understand the structural, molecular, electronic and photophysical properties of the chromophores. The experimental absorption and emission wavelengths are in good agreement with the computed vertical excitation and theoretical emission obtained by Density Functional Theory and Time Dependant Density Functional Theory.

  12. A theoretical study of the local electronic structure of two adjacent CuOplanes in YBa 2Cu 3O 7

    NASA Astrophysics Data System (ADS)

    Suter, H. U.; Stoll, E. P.; Hüsser, P.; Schafroth, S.; Meier, P. F.

    1997-08-01

    To reveal the local electronic structure of the two adjacent CuOplanes in YBa 2Cu 3O 7, ab initio studies on a small cluster (Cu 2Y 4O 8) were performed. Electron correlation was investigated with both density functional theory and Møller-Plesset theory. The ionisation energies, electron affinities adn the singlet-triplet differences are discussed with respect to model Hamiltonians of high-T c compounds.

  13. Analysis of electron correlation effects and contributions of NMR J-couplings from occupied localized molecular orbitals.

    PubMed

    Zarycz, Natalia; Aucar, Gustavo A

    2012-02-02

    NMR J-coupling calculations at the second-order of polarization propagator approach, SOPPA, are among the most reliable. They include a high percentage of the total electron correlation effects in saturated and unsaturated molecular systems. Furthermore, J-couplings are quite sensitive to the whole electronic molecular framework. We present in this article the first study of all three response mechanisms, Fermi contact, FC, spin-dipolar, SD and paramagnetic spin-orbital, PSO, for J-couplings with occupied localized molecular orbitals at the SOPPA level of approach. Even though SOPPA results are not invariant under unitary transformations, the difference between results obtained with canonical and localized molecular orbitals, LMOs, are small enough to permit its application with confidence. The following small-size saturated and unsaturated compounds were analyzed: CH(4), CH(3)F, C(2)H(6), NH(3), C(2)H(4), CH(2)NH, H(2)C═CHF, and FHC═CHF. The local character of the FC mechanism that appears in J-couplings of these molecular models is shown through the analysis of contributions from LMOs. The importance of including the electron correlation on the engaged bonding orbitals for one-bond couplings is emphasized. Almost all electron correlation effects are included in such orbitals. Interesting findings were the large contributions by s-type LMOs to the C-H and C-C J-couplings; they are responsible for the variation of (1)J(C-C) when going from ethane to ethene and to 1,2-difluoroethene. The previously proposed hyperconjugative transfer mechanism has been tested. Among other tests we found the difference anti-syn of one-bond (1)J(C-H) in imine as due to both the corresponding σ(C-H) and the lone-pair, LP, contribution. Geminal and vicinal J-couplings were also analyzed. Our findings are in accord with a previous work by Pople and Bothner-by, who considered results taken from calculations or empirical data. For all geminal couplings the pattern of J-couplings, like

  14. Magnetism, f-electron localization and superconductivity in 122-type heavy-fermion metals.

    PubMed

    Steglich, F; Arndt, J; Stockert, O; Friedemann, S; Brando, M; Klingner, C; Krellner, C; Geibel, C; Wirth, S; Kirchner, S; Si, Q

    2012-07-25

    Both CeCu2Si2 and YbRh2Si2 crystallize in the tetragonal ThCr2Si2 crystal structure. Recent neutron-scattering results on normal-state CeCu2Si2 reveal a slowing down of the quasielastic response which complies with the scaling expected for a quantum critical point (QCP) of itinerant, i.e., three-dimensional spin-density-wave (SDW), type. This interpretation is in full agreement with the non-Fermi-liquid behavior observed in transport and thermodynamic measurements. The momentum dependence of the magnetic excitation spectrum reveals two branches of an overdamped dispersive mode whose coupling to the heavy charge carriers is strongly retarded. These overdamped spin fluctuations are considered to be the driving force for superconductivity in CeCu2Si2 (Tc = 600 mK). The weak antiferromagnet YbRh2Si2 (TN = 70 mK) exhibits a magnetic-field-induced QCP at BN = 0.06 T (B⊥c). There is no indication of superconductivity down to T = 10 mK. The magnetic QCP appears to concur with a breakdown of the Kondo effect. Doping-induced variations of the average unit-cell volume result in a detachment of the magnetic and electronic instabilities. A comparison of the properties of these isostructural compounds suggests that 3D SDW QCPs are favorable for unconventional superconductivity. The question whether a Kondo-breakdown QCP may also give rise to superconductivity, however, remains to be clarified.

  15. Density Fitting and Cholesky Decomposition of the Two-Electron Integrals in Local Multireference Configuration Interaction Theory.

    PubMed

    Krisiloff, David B; Krauter, Caroline M; Ricci, Francis J; Carter, Emily A

    2015-11-10

    To treat large molecules with accurate ab initio quantum chemistry, reduced scaling correlated wave function methods are now commonly employed. Optimization of these wave functions in practice requires some approximation of the two-electron integrals. Both Cholesky decomposition (CD) and density fitting (DF) are widely used approaches to approximate these integrals. Here, we compare CD and DF for use in local multireference singles and doubles configuration interaction (LMRSDCI). DF-LMRSDCI provides less accurate total energies than CD-LMRSDCI, but both methods are accurate for energy differences. However, DF-LMRSDCI is significantly less computationally expensive than CD-LMRSDCI on the molecules tested, suggesting that DF-LMRSDCI is an efficient, often sufficiently accurate alternative to our previously reported CD-LMRSDCI method.

  16. Biomarkers of sensitivity to potent and selective antitumor 2-(4-amino-3-methylphenyl)-5-fluorobenzothiazole (5F203) in ovarian cancer.

    PubMed

    Callero, Mariana A; Luzzani, Gabriela A; De Dios, Diana O; Bradshaw, Tracey D; Perez, Andrea I Loaiza

    2013-10-01

    2-(4-Amino-3-methylphenyl)-5-fluorobenzothiazole (5F203, NSC 703786) lysylamide belongs to a novel mechanistic class of antitumor agents. It elicits activity against ovarian, breast, kidney and colorectal cancer models. In sensitive breast cancer cells, 5F203 activates aryl hydrocarbon receptor (AhR) signaling. Herein, we evaluate the role of AhR in 5F203 activity in two ovarian cancer cell lines: IGROV-1 (sensitive to 5F203), SKOV-3 (resistant to this agent). In addition, cancer cells have been isolated from ascites fluid of ovarian cancer patients; sensitivity to 5F203 and concurrent AhR signal transduction has been examined in ascites-isolated ovarian cancer patients' cells. 5F203 induced enhanced CYP1A1 expression, AhR translocation and ROS formation in IGROV-1 cells and ascites-isolated ovarian cancer cells that were sensitive to 5F203. In IGROV-1 cells 5F203-induced ROS formation was accompanied by JNK, ERK and P38MAPK phosphorylation, DNA damage and cell cycle arrest prior to apoptosis. In contrast, 5F203 failed to induce CYP1A1 expression, AhR translocation or oxidative stress in 5F203-resistant SKOV-3 cells, or in ovarian cancer ascites cells inherently resistant to this agent. We propose that AhR may represent a new molecular target in the treatment of ovarian tumors and 5F203 may exemplify a potential novel treatment. Furthermore, putative biomarkers of sensitivity to this agent have been identified.

  17. A Novel Pre-Processing Technique for Original Feature Matrix of Electronic Nose Based on Supervised Locality Preserving Projections

    PubMed Central

    Jia, Pengfei; Huang, Tailai; Wang, Li; Duan, Shukai; Yan, Jia; Wang, Lidan

    2016-01-01

    An electronic nose (E-nose) consisting of 14 metal oxide gas sensors and one electronic chemical gas sensor has been constructed to identify four different classes of wound infection. However, the classification results of the E-nose are not ideal if the original feature matrix containing the maximum steady-state response value of sensors is processed by the classifier directly, so a novel pre-processing technique based on supervised locality preserving projections (SLPP) is proposed in this paper to process the original feature matrix before it is put into the classifier to improve the performance of the E-nose. SLPP is good at finding and keeping the nonlinear structure of data; furthermore, it can provide an explicit mapping expression which is unreachable by the traditional manifold learning methods. Additionally, some effective optimization methods are found by us to optimize the parameters of SLPP and the classifier. Experimental results prove that the classification accuracy of support vector machine (SVM combined with the data pre-processed by SLPP outperforms other considered methods. All results make it clear that SLPP has a better performance in processing the original feature matrix of the E-nose. PMID:27376295

  18. Photoexcitation of electron wave packets in quantum spin Hall edge states: Effects of chiral anomaly from a localized electric pulse

    NASA Astrophysics Data System (ADS)

    Dolcini, Fabrizio; Iotti, Rita Claudia; Montorsi, Arianna; Rossi, Fausto

    2016-10-01

    We show that, when a spatially localized electric pulse is applied at the edge of a quantum spin Hall system, electron wave packets of the helical states can be photoexcited by purely intrabranch electrical transitions, without invoking the bulk states or the magnetic Zeeman coupling. In particular, as long as the electric pulse remains applied, the photoexcited densities lose their character of right and left movers, whereas after the ending of the pulse they propagate in opposite directions without dispersion, i.e., maintaining their space profile unaltered. Notably we find that, while the momentum distribution of the photoexcited wave packets depends on the temperature T and the chemical potential μ of the initial equilibrium state and displays a nonlinear behavior on the amplitude of the applied pulse, in the mesoscopic regime the space profile of the wave packets is independent of T and μ . Instead, it depends purely on the applied electric pulse, in a linear manner, as a signature of the chiral anomaly characterizing massless Dirac electrons. We also discuss how the photoexcited wave packets can be tailored with the electric pulse parameters, for both low and finite frequencies.

  19. Interplay of electron correlations and localization in disordered β-tantalum films: Evidence from dc transport and spectroscopic ellipsometry study

    SciTech Connect

    Kovaleva, N. N.; Chvostova, D.; Dejneka, A.; Bagdinov, A. V.; Petrova, M. G.; Demikhov, E. I.; Pudonin, F. A.

    2015-02-02

    We report the dc transport (5 K ≲ T ≲ 380 K) and spectroscopic ellipsometry (0.8 eV ≤ hν ≤ 8.5 eV, T ≃ 300 K) study of β-Ta films prepared by rf sputtering deposition as a function of their thickness in the range 2.5 nm ≲ d ≲ 200 nm. The dc transport of the β-Ta films with a thickness d ≳ 25 nm is characterized by negative temperature coefficient of resistivity (TCR) caused by localization effects peculiar of highly disordered metals. Their dielectric function spectra display non-metallic-like behavior due to the presence of the pronounced band at 2 eV. We found that with increasing TCR absolute value, specifying elevated degree disorder, the optical spectral weight (SW) of free charge carriers decreases. The associated SW is recovered in the range of Mott-Hubbard transitions, indicating the mechanism of localization enhancement by electronic correlations in disordered metals.

  20. Interplay of electron correlations and localization in disordered β-tantalum films: Evidence from dc transport and spectroscopic ellipsometry study

    NASA Astrophysics Data System (ADS)

    Kovaleva, N. N.; Chvostova, D.; Bagdinov, A. V.; Petrova, M. G.; Demikhov, E. I.; Pudonin, F. A.; Dejneka, A.

    2015-02-01

    We report the dc transport (5 K ≲ T ≲ 380 K) and spectroscopic ellipsometry (0.8 eV ≤ hν ≤ 8.5 eV, T ≃ 300 K) study of β-Ta films prepared by rf sputtering deposition as a function of their thickness in the range 2.5 nm ≲ d ≲ 200 nm. The dc transport of the β-Ta films with a thickness d ≳ 25 nm is characterized by negative temperature coefficient of resistivity (TCR) caused by localization effects peculiar of highly disordered metals. Their dielectric function spectra display non-metallic-like behavior due to the presence of the pronounced band at 2 eV. We found that with increasing TCR absolute value, specifying elevated degree disorder, the optical spectral weight (SW) of free charge carriers decreases. The associated SW is recovered in the range of Mott-Hubbard transitions, indicating the mechanism of localization enhancement by electronic correlations in disordered metals.

  1. Identification of local phase of nanoscale BaTiO₃ powders by high-resolution electron energy loss spectroscopy.

    PubMed

    Moon, Sun-Min; Wang, Xiaohui; Cho, Nam-Hee

    2013-08-01

    The electron energy loss spectroscopy (EELS) technique was applied to investigate the local variation in the phase of barium titanate (BaTiO₃) ceramics. It was found that the fine structure of the titanium L₂,₃ edge and their satellite peaks were sensitively varied with the tetragonal-cubic phase transition. The peak splitting of Ti-L₃ edge of tetragonal-phased BaTiO₃ ceramics was widened because of the increased crystal field effect compared with that of cubic-phased BaTiO₃. In case of nanoscale BaTiO₃ powders, the L₃ edge splitting of the core region was found to be smaller than that of the shell region. The energy gap between peaks t₂g and eg varied from 2.36 to 1.94 eV with changing the probe position from 1 to 20 nm from the surface. These results suggest that the EELS technique can be used to identify the local phase of sintered BaTiO₃ ceramics.

  2. Localization of EB1, IFT polypeptides, and kinesin-2 in Chlamydomonas flagellar axonemes via immunogold scanning electron microscopy.

    PubMed

    Sloboda, Roger D; Howard, Louisa

    2007-06-01

    Intraflagellar transport (IFT) refers to the bi-directional movement of particles and associated cargo along the axonemes of eukaryotic flagella and cilia. To provide a new perspective on the morphology of IFT particles, their association with the axoneme, and their composition, we have used immunogold localization coupled to detection via scanning electron microscopy. Here we co-localize in the Chlamydomonas flagellar axoneme polypeptides labeled with specific antibodies. Chlamydomonas EB1 localizes to the distal tip of the axoneme, as expected from previous immunofluorescent data (Pedersen et al. Curr Biol2003;13(22):1969-1974), thus demonstrating the utility of this approach. Using antibodies to IFT-related polypeptides, particles can be identified associated with the axoneme that fall into one of two classes: The first class is composed of IFT particles labeled with polyclonal antibodies to kinesin-2 and monoclonal antibodies to either IFT139 (an IFT complex A polypeptide) or IFT172 (a complex B polypeptide). The second class is comprised of particles that label with antibodies to IFT139 alone; thus, discrete particles are present associated with the axoneme that are composed only of complex A polypeptides. When IFT particles were purified by sucrose gradient ultracentrifugation, they appeared as more or less spherical aggregates of varying dimensions labeled with antibodies to IFT139 and to the motor protein kinesin-2. By contrast, isolated IFT particles that were labeled with IFT172 antibodies were not labeled with kinesin-2 antibodies. The data are discussed in terms of the total polypeptide composition of an IFT particle and the interaction of the particles with the motors that power IFT.

  3. The contribution of Fermi gamma-ray pulsars to the local flux of cosmic-ray electrons and positrons

    SciTech Connect

    Gendelev, Leo; Profumo, Stefano; Dormody, Michael E-mail: profumo@scipp.ucsc.edu

    2010-02-01

    We analyze the contribution of gamma-ray pulsars from the first Fermi-Large Area Telescope (LAT) catalogue to the local flux of cosmic-ray electrons and positrons (e{sup +}e{sup −}). We present new distance estimates for all Fermi gamma-ray pulsars, based on the measured gamma-ray flux and pulse shape. We then estimate the contribution of gamma-ray pulsars to the local e{sup +}e{sup −} flux, in the context of a simple model for the pulsar e{sup +}e{sup −} emission. We find that 10 of the Fermi pulsars potentially contribute significantly to the measured e{sup +}e{sup −} flux in the energy range between 100 GeV and 1 TeV. Of the 10 pulsars, 2 are old EGRET gamma-ray pulsars, 2 pulsars were discovered with radio ephemerides, and 6 were discovered with the Fermi pulsar blind-search campaign. We argue that known radio pulsars fall in regions of parameter space where the e{sup +}e{sup −} contribution is predicted to be typically much smaller than from those regions where Fermi-LAT pulsars exist. However, comparing the Fermi gamma-ray flux sensitivity to the regions of pulsar parameter space where a significant e{sup +}e{sup −} contribution is predicted, we find that a few known radio pulsars that have not yet been detected by Fermi can also significantly contribute to the local e{sup +}e{sup −} flux if a) they are closer than 2 kpc, and if b) they have a characteristic age on the order of one mega-year.

  4. Efficient and accurate local approximations to coupled-electron pair approaches: An attempt to revive the pair natural orbital method

    NASA Astrophysics Data System (ADS)

    Neese, Frank; Wennmohs, Frank; Hansen, Andreas

    2009-03-01

    Coupled-electron pair approximations (CEPAs) and coupled-pair functionals (CPFs) have been popular in the 1970s and 1980s and have yielded excellent results for small molecules. Recently, interest in CEPA and CPF methods has been renewed. It has been shown that these methods lead to competitive thermochemical, kinetic, and structural predictions. They greatly surpass second order Møller-Plesset and popular density functional theory based approaches in accuracy and are intermediate in quality between CCSD and CCSD(T) in extended benchmark studies. In this work an efficient production level implementation of the closed shell CEPA and CPF methods is reported that can be applied to medium sized molecules in the range of 50-100 atoms and up to about 2000 basis functions. The internal space is spanned by localized internal orbitals. The external space is greatly compressed through the method of pair natural orbitals (PNOs) that was also introduced by the pioneers of the CEPA approaches. Our implementation also makes extended use of density fitting (or resolution of the identity) techniques in order to speed up the laborious integral transformations. The method is called local pair natural orbital CEPA (LPNO-CEPA) (LPNO-CPF). The implementation is centered around the concepts of electron pairs and matrix operations. Altogether three cutoff parameters are introduced that control the size of the significant pair list, the average number of PNOs per electron pair, and the number of contributing basis functions per PNO. With the conservatively chosen default values of these thresholds, the method recovers about 99.8% of the canonical correlation energy. This translates to absolute deviations from the canonical result of only a few kcal mol-1. Extended numerical test calculations demonstrate that LPNO-CEPA (LPNO-CPF) has essentially the same accuracy as parent CEPA (CPF) methods for thermochemistry, kinetics, weak interactions, and potential energy surfaces but is up to 500

  5. Profile of Ventana ALK (D5F3) companion diagnostic assay for non-small-cell lung carcinomas.

    PubMed

    Conde, Esther; Hernandez, Susana; Prieto, Mario; Martinez, Rebeca; Lopez-Rios, Fernando

    2016-06-01

    The development of several ALK inhibitors means that the importance of accurately identifying ALK-positive lung cancer has never been greater. Therefore, it is crucial that ALK testing assays become more standardized. The aim of this review is to comment on the recently FDA-approved VENTANA ALK (D5F3) Companion Diagnostic (CDx) Assay. This kit provides high sensitivity and specificity for the detection of ALK rearrangements and seamless integration into the laboratory workflow, with a fully automated analytical phase and fast interpretation. The use of controls increases the sensitivity and specificity and a dichotomous scoring approach enhances reproducibility.

  6. Extended electron energy loss fine structure simulation of the local boron environment in sodium aluminoborosilicate glasses containing gadolinium

    SciTech Connect

    Qian, Morris; Li, Hong; Li, Liyu ); Strachan, Denis M. )

    2003-10-15

    Gadolinium can be dissolved in sodium-alumino-borosilicate glasses up to 47 wt% in a baseline borosilicate glass (mol%) 20 B2O3, 5 Al2O3, 60 SiO2,and 20 Na2O. Understanding of Gd dissolution in borosilicate melts is important in glass formulation optimization. Electron energy loss fine structure (ELFS) spectroscopy is chosen, which provides well resolved local atomic structure information for both amorphous and crystalline materials with high sensitivity to low Z elements such as Al, B, Na, O, and Si where the x-ray absorption fine structure (XAFS) technique faces experimental difficulty. In this study, we report our results of boron K-edge ELFS study. Two borosilicate glass samples with 30 and 47 mass% Gd2O3, B20Gd30 and B20Gd47were chosen for B K-edge ELFS study. EEL spectra were acquired on a Philips 430 TEM equipped with Gatan PEELS system 666 and EL/P 2.1 software with Custom function AcqLong. The ELFS data analysis was performed using UWELFS, UWXAFS and FEFF software. From our Gd solubility study, the local structure of Gd in the borate environment possibly resembles double chain structure found in crystalline Gd(BO2)3 as proposed by Chakraborty et al. The B/Gd ratio's in both glasses are smaller then 3, which means the excess Gd atoms in the Si-sites would be 17 and 60 mol% of the total Gd atoms, respectively according to the model, yet the local environment of borate sites saturated with Gd should be remained. To verity above hypothesis, the double chain structure model was applied to fit boron K-edge. The model was shown to well fit experimental boron K-edge EELS spectra for both glasses with some degree of distance distortion which is understandable in amorphous structure. Therefore, it is very likely that Gd stabilized in borate sites has a local structure resembling the double chain Gd(BO2)3 structure as proposed by our solubility study and literature.

  7. Pou5f1-dependent EGF expression controls E-cad endocytosis, cell adhesion, and zebrafish epiboly movements

    PubMed Central

    Song, Sungmin; Eckerle, Stephanie; Onichtchouk, Daria; Marrs, James A.; Nitschke, Roland; Driever, Wolfgang

    2013-01-01

    Summary Initiation of motile cell behavior in embryonic development occurs during late blastula stages when gastrulation begins. At this stage, the strong adhesion of blastomeres has to be modulated to enable dynamic behavior, similar to epithelial-to-mesenchymal transitions. We show that in zebrafish MZspg embryos mutant for the stem cell transcription factor Pou5f1/Oct4, which are severely delayed in the epiboly gastrulation movement, all blastomeres are defective in E-cad endosomal trafficking and E-cad accumulates at the plasma membrane. We find that Pou5f1-dependent control of EGF expression regulates endosomal E-cad trafficking. EGFR may act via modulation of p120 activity. Loss of E-cad dynamics reduces cohesion of cells in reaggregation assays. Quantitative analysis of cell behavior indicates that dynamic E-cad endosomal trafficking is required for epiboly cell movements. We hypothesize that dynamic control of E-cad trafficking is essential to effectively generate new adhesion sites when cells move relative to each other. PMID:23484854

  8. Self-assembly of a 3d-5f trinuclear single-molecule magnet from a pentavalent uranyl complex.

    PubMed

    Chatelain, Lucile; Walsh, James P S; Pécaut, Jacques; Tuna, Floriana; Mazzanti, Marinella

    2014-12-01

    Mixed-metal uranium compounds are very attractive candidates in the design of single-molecule magnets (SMMs), but only one 3d-5f hetero-polymetallic SMM containing a uranium center is known. Herein, we report two trimeric heterodimetallic 3d-5f complexes self-assembled by cation-cation interactions between a uranyl(V) complex and a TPA-capped M(II)  complex (M=Mn (1), Cd (2); TPA=tris(2-pyridylmethyl)amine). The metal centers were strategically chosen to promote the formation of discrete molecules rather than extended chains. Compound 1, which contains an almost linear {MnOUOMn} core, exhibits SMM behavior with a relaxation barrier of 81±0.5 K-the highest reported for a mono-uranium system-arising from intramolecular Mn-U exchange interactions combined with the high Ising anisotropy of the uranyl(V) moiety. Compound 1 also exhibits an open magnetic hysteresis loop at temperatures less than 3 K, with a significant coercive field of 1.9 T at 1.8 K.

  9. Extended electron energy loss fine structure simulation of the local boron environment in sodium aluminoborosilicate glasses containing gadolinium

    SciTech Connect

    Qian, Morris; Li, Hong; Li, Liyu ); Strachan, Denis M. )

    2003-12-01

    Phase separation in sodium-aluminoborosilicate glasses was systematically studied as a function of Gd2O3 concentration with transmission electron microscopy (TEM), energy dispersive x-ray spectroscopy (EDS), and electron energy loss spectroscopy (EELS) methods. Gadolinium-induced phase separation in the three systems can be consistently explained by proposing that Gd cations partition to the borate-rich environments and subsequent agglomeration of the Gd-borate moieties, or short-range ordered structural groups, in the glass. Agglomeration of the Gd-borate rich environments is further discussed within the context of excess metal oxides,[Na2O]ex or[Al2O3]ex=|Na2O - Al2O3|, and excess B2O3,[B2O3]ex, available for incorporating Gd cations. Results showed that agglomeration of the Gd-borate rich environments occurred at a much lower Gd2O3 concentration in the glass without[Na2O]ex or[Al2O3]ex and at a significantly higher Gd2O3 concentration in the glass with either[Na2O]ex or[Al2O3]ex. Assuming 1BO4 : 1Gd : 2BO3 (based on literature-reported Gd-metaborate structure) as a local Gd-borate environment in glass, we introduced the saturation index of boron, SI[B]= Gd2O3/(1/3[B2O3]ex), to examine the glass susceptibility to Gd-induced phase separation for all three alkali-aluminoborosilicate systems. While our results have provided some insight to the glass structure, they also provide insight to the mechanism by which the metal oxide is dissolved into the melt. This appears to occur predominantly through boron complexation of the metal oxide.

  10. Electron microscopic localization of calelectrin, a Mr 36 000 calcium-regulated protein, at the cholinergic electromotor synapse of Torpedo.

    PubMed

    Fiedler, W; Walker, J H

    1985-07-01

    Calelectrin is a calcium-binding protein of Mr 36 000 which has previously been shown to be associated with membranes of the cholinergic synapse in a calcium-dependent manner. We report here that calelectrin was solubilized from the electric organ of Torpedo marmorata in the absence of calcium together with proteins of Mr 54 000 and Mr 15 000. In cholinergic nerve endings isolated from the electric organ only calelectrin was solubilized in a calcium-dependent manner. A specific antiserum to calelectrin was used to localize the antigen by immunofluorescence microscopy on sections of electric organ and showed that calelectrin is distributed throughout the postsynaptic cell. Calelectrin was also detected in axons and in the cell bodies of the cholinergic neurones where it was concentrated in discrete patches throughout the cells. Electric organ tissue was processed to localize calelectrin with the electron microscope using an immunoperoxidase method. The most intense staining was observed on the cytoplasmic face of the acetylcholine receptor-containing postsynaptic membrane and also associated with the intracellular filaments of the electrocyte. The intensity of staining associated with these structures could be greatly reduced by preincubating the tissue with calcium chelators. In nerve terminals calelectrin was associated with synaptic vesicles in a polarized fashion. Calelectrin was also found on the cytoplasmic face of the synaptosomal plasma membrane and associated with neurofilaments. No extracellular staining was ever observed. Our results strongly support our original hypothesis that calelectrin is a calcium-regulated component of intracellular structure associated both with membranes and filaments.

  11. The effect of the electronic structure, phase transition, and localized dynamics of atoms in the formation of tiny particles of gold

    NASA Astrophysics Data System (ADS)

    Ali, Mubarak; Lin, I.-Nan

    2017-01-01

    In addition to self-governing properties, tiny-sized particles of metallic colloids are the building blocks of large-sized particles; thus, their study has been the subject of a large number of publications. In the present work, it has been discussed that geometry structure of tiny particle made through atom-to-atom amalgamation depends on attained dynamics of gold atoms along with protruded orientations. The localized process conditions direct two-dimensional structure of a tiny particle at atomically flat air-solution interface while heating locally dynamically approached atoms, thus, negate the role of van der Waals interactions. At electronphoton-solution interface, impinging electrons stretch or deform atoms of tiny particles depending on the mechanism of impingement. In addition, to strike regular grid of electrons ejected on split of atoms not executing excitations and de-excitations of their electrons, atoms of tiny particles also deform or stretch while occupying various sites depending on the process of synergy. Under suitable impinging electron streams, those tiny particles in monolayer two-dimensional structure electron states of their atoms are diffused in the direction of transferred energy, thus, coincide to the next adjacent atoms in each one-dimensional array dealing the same sort of behavior. Instantaneously, photons of adequate energy propagate on the surfaces of such electronic structures and modify those into smooth elements, thus, disregard the phenomenon of localized surface plasmons. This study highlights the fundamental process of formation of tiny particles where the role of localized dynamics of atoms and their electronic structure along with interaction to light are discussed. Such a tool of processing materials, in nonequilibrium pulse-based process, opens a number of possibilities to develop engineered materials with specific chemical, optical, and electronic properties.

  12. Involvement of 5f-orbitals in the bonding and reactivity of organoactinide compounds: thorium(IV) and uranium(IV) bis (hydrazonato) complexes

    SciTech Connect

    Cantat, Thibault; Graves, Christopher R; Morris, David E; Kiplinger, Jaqueline L

    2008-01-01

    Migratory insertion of diphenyldiazomethane into both metal-carbon bonds of the bis(alkyl) and bis(aryl) complexes (C5Me5)2AnR2 yields the first f-element bis(hydrazonato) complexes (C5Me5)2An[2-(N,N')-R-N-NCPh2]2 [An = Th, R = CH3 (18), PhCH2 (15), Ph (16); An = U, R = CH3 (17), PhCH2 (14)], which have been characterized by a combination of spectroscopy, electrochemistry, and X-ray crystallography. The two hydrazonato ligands adopt an 2-coordination mode leading to 20-electron (for Th) and 22-electron (for U) complexes that have no transition-metal analogues. In fact, reaction of (C5H5)2Zr(CH3)2 or (C5Me5)2Hf(CH3)2 with diphenyldiazomethane is limited to the formation of the corresponding mono(hydrazonato) complex (C5R5)2M[2-(N,N')-CH3-N-NCPh2](CH3) (M = Zr, R = H or M = Hf, R = CH3). The difference in the reactivities of the group 4 metal complexes and the actinides was used as a unique platform for investigating in depth the role of 5f orbitals on the reactivity and bonding in actinide organometallic complexes. The electronic structure of the (C5H5)2M[2-(N,N')-CH3-N-NCH2]2 (M = Zr, Th, U) model complexes was studied using density functional theory (DFT) calculations and compared to experimental structural, electrochemical, and spectroscopic results. Whereas transition-metal bis(cyclopentadienyl) complexes are known to stabilize three ligands in the metallocene girdle to form saturated (C5H5)2ML3 species, in a bis(hydrazonato) system, a fourth ligand is coordinated to the metal center to give (C5H5)2ML4. DFT calculations have shown that 5f orbitals in the actinide complexes play a crucial role in stabilizing this fourth ligand by stabilizing both the s and p electrons of the two 2-coordinated hydrazonato ligands. In contrast, the stabilization of the hydrazonato ligands was found to be significantly less effective for the putative bis(hydrazonato) zirconium(IV) complex, yielding a higher energy structure. However, the difference in the reactivities of the group 4

  13. Evidence for the involvement of 5f orbitals in the bonding and reactivity of organometallic actinide compounds: thorium(IV) and uranium(IV) bis(hydrazonato) complexes.

    PubMed

    Cantat, Thibault; Graves, Christopher R; Jantunen, Kimberly C; Burns, Carol J; Scott, Brian L; Schelter, Eric J; Morris, David E; Hay, P Jeffrey; Kiplinger, Jaqueline L

    2008-12-24

    Migratory insertion of diphenyldiazomethane into both metal-carbon bonds of the bis(alkyl) and bis(aryl) complexes (C(5)Me(5))(2)AnR(2) yields the first f-element bis(hydrazonato) complexes (C(5)Me(5))(2)An[eta(2)-(N,N')-R-N-N=CPh(2)](2) [An = Th, R = CH(3) (18), PhCH(2) (15), Ph (16); An = U, R = CH(3) (17), PhCH(2) (14)], which have been characterized by a combination of spectroscopy, electrochemistry, and X-ray crystallography. The two hydrazonato ligands adopt an eta(2)-coordination mode leading to 20-electron (for Th) and 22-electron (for U) complexes that have no transition-metal analogues. In fact, reaction of (C(5)H(5))(2)Zr(CH(3))(2) or (C(5)Me(5))(2)Hf(CH(3))(2) with diphenyldiazomethane is limited to the formation of the corresponding mono(hydrazonato) complex (C(5)R(5))(2)M[eta(2)-(N,N')-CH(3)-N-N=CPh(2)](CH(3)) (M = Zr, R = H or M = Hf, R = CH(3)). The difference in the reactivities of the group 4 metal complexes and the actinides was used as a unique platform for investigating in depth the role of 5f orbitals on the reactivity and bonding in actinide organometallic complexes. The electronic structure of the (C(5)H(5))(2)M[eta(2)-(N,N')-CH(3)-N-N=CH(2)](2) (M = Zr, Th, U) model complexes was studied using density functional theory (DFT) calculations and compared to experimental structural, electrochemical, and spectroscopic results. Whereas transition-metal bis(cyclopentadienyl) complexes are known to stabilize three ligands in the metallocene girdle to form saturated (C(5)H(5))(2)ML(3) species, in a bis(hydrazonato) system, a fourth ligand is coordinated to the metal center to give (C(5)H(5))(2)ML(4). DFT calculations have shown that 5f orbitals in the actinide complexes play a crucial role in stabilizing this fourth ligand by stabilizing both the sigma and pi electrons of the two eta(2)-coordinated hydrazonato ligands. In contrast, the stabilization of the hydrazonato ligands was found to be significantly less effective for the putative bis

  14. Effect of isopropyl alcohol on the surface localization and recombination of conduction-band electrons in Degussa P25 TiO sub 2. A pulse-radiolysis time-resolved microwave conductivity study. [Accelerated electrons

    SciTech Connect

    Warman, J.M.; Hass, M.P. de ); Pichat, P. ); Serpone, N. Concordia Univ., Montreal, Quebec )

    1991-10-31

    Conduction-band electrons, formed by pulse radiolysis of Degussa P25 TiO{sub 2} particles, have been monitored by time-resolved microwave conductivity and found to undergo equilibrium localization and eventual recombination at the particle surface. In the presence of isopropyl alcohol recombination is retarded due to surface hole scavenging. The particle bulk can then be pumped with mobile electrons, which survive for seconds.

  15. Laser-induced fluorescence studies of excited Sr reactions: II. Sr(3P1)+CH3F, C2H5F, C2H4F2

    NASA Astrophysics Data System (ADS)

    Teule, J. M.; Janssen, M. H. M.; Bulthuis, J.; Stolte, S.

    1999-06-01

    The vibrational and rotational energy distributions of ground state SrF(X 2Σ) formed in the reactions of electronically excited Sr(3P1) with methylfluoride, ethylfluoride, and 1,1-difluoroethane have been studied by laser-induced fluorescence. Although the reactions of ground state Sr with these reactants are exothermic, no SrF products are observed for those reactions in this study. The fraction of available energy disposed into the sum of rotational and vibrational energy of the SrF(X 2Σ) product is approximately the same for all three reactions, i.e., 40%. The reaction of Sr(3P1) with CH3F results in very low vibrational excitation in the SrF reaction product. The product vibration increases in going to C2H5F and C2H4F2. It is concluded that the alkyl group influences the energy disposal mechanism in these reactions, and some suggestions are given for a partial explanation of the observations.

  16. Intracellular viral localization in murine coxsackievirus-B3 myocarditis. Ultrastructural study by electron microscopic in situ hybridization.

    PubMed Central

    Ukimura, A.; Deguchi, H.; Kitaura, Y.; Fujioka, S.; Hirasawa, M.; Kawamura, K.; Hirai, K.

    1997-01-01

    Group B Coxsackieviruses are a common cause of myocarditis. To detect the viral genome and its localization in the myocardium, we examined C3H/He mice with Coxsackievirus B3 (CVB3) myocarditis on days 5, 8, and 14 after inoculation by the reverse transcriptase polymerase chain reaction and by in situ hybridization. Sense and antisense CVB3 RNA were detected in the myocardium of all mice up to day 14 by reverse transcriptase polymerase chain reaction. Light microscopic in situ hybridization with a cDNA probe for CVB3 showed clusters of positive signals in the areas of myocardial necrosis and cell infiltration. With electron microscopic in situ hybridization, CVB3 RNA was detected in the cytoplasm of cardiocytes, between the myofibrils, near the mitochondria, and in tubular or vesicular structures. Viral RNA was also detected in necrotic debris, in the cytoplasm of macrophages, and in the cytoplasm of interstitial fibroblasts. These findings suggest that CVB3 RNA is replicated in the cytoplasm of cardiocytes, transferred into tubular or vesicular structures, released into the interstitium, and phagocytosed by macrophages. Some positive signals were also detected in the cytoplasm of cardiocytes showing close contact with infiltrating lymphocytes, suggesting that the lymphocytes recognized virus-infected cardiocytes and caused cell-mediated immune cardiocyte damage. Images Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Figure 8 Figure 9 Figure 10 Figure 11 Figure 12 PMID:9176398

  17. Probing local and electronic structure in Warm Dense Matter: single pulse synchrotron x-ray absorption spectroscopy on shocked Fe

    PubMed Central

    Torchio, Raffaella; Occelli, Florent; Mathon, Olivier; Sollier, Arnaud; Lescoute, Emilien; Videau, Laurent; Vinci, Tommaso; Benuzzi-Mounaix, Alessandra; Headspith, Jon; Helsby, William; Bland, Simon; Eakins, Daniel; Chapman, David; Pascarelli, Sakura; Loubeyre, Paul

    2016-01-01

    Understanding Warm Dense Matter (WDM), the state of planetary interiors, is a new frontier in scientific research. There exists very little experimental data probing WDM states at the atomic level to test current models and those performed up to now are limited in quality. Here, we report a proof-of-principle experiment that makes microscopic investigations of materials under dynamic compression easily accessible to users and with data quality close to that achievable at ambient. Using a single 100 ps synchrotron x-ray pulse, we have measured, by K-edge absorption spectroscopy, ns-lived equilibrium states of WDM Fe. Structural and electronic changes in Fe are clearly observed for the first time at such extreme conditions. The amplitude of the EXAFS oscillations persists up to 500 GPa and 17000 K, suggesting an enduring local order. Moreover, a discrepancy exists with respect to theoretical calculations in the value of the energy shift of the absorption onset and so this comparison should help to refine the approximations used in models. PMID:27246145

  18. pH, redox potential and local biofilm potential microenvironments within Geobacter sulfurreducens biofilms and their roles in electron transfer.

    PubMed

    Babauta, Jerome T; Nguyen, Hung Duc; Harrington, Timothy D; Renslow, Ryan; Beyenal, Haluk

    2012-10-01

    The limitation of pH inside electrode-respiring biofilms is a well-known concept. However, little is known about how pH and redox potential are affected by increasing current inside biofilms respiring on electrodes. Quantifying the variations in pH and redox potential with increasing current is needed to determine how electron transfer is tied to proton transfer within the biofilm. In this research, we quantified pH and redox potential variations in electrode-respiring Geobacter sulfurreducens biofilms as a function of respiration rates, measured as current. We also characterized pH and redox potential at the counter electrode. We concluded that (1) pH continued to decrease in the biofilm through different growth phases, showing that the pH is not always a limiting factor in a biofilm and (2) decreasing pH and increasing redox potential at the biofilm electrode were associated only with the biofilm, demonstrating that G. sulfurreducens biofilms respire in a unique internal environment. Redox potential inside the biofilm was also compared to the local biofilm potential measured by a graphite microelectrode, where the tip of the microelectrode was allowed to acclimatize inside the biofilm.

  19. pH, Redox Potential and Local Biofilm Potential Microenvironments Within Geobacter sulfurreducens Biofilms and Their Roles in Electron Transfer

    PubMed Central

    Babauta, Jerome T.; Nguyen, Hung Duc; Harrington, Timothy D.; Renslow, Ryan; Beyenal, Haluk

    2012-01-01

    The limitation of pH inside electrode-respiring biofilms is a well-known concept. However, little is known about how pH and redox potential are affected by increasing current inside biofilms respiring on electrodes. Quantifying the variations in pH and redox potential with increasing current is needed to determine how electron transfer is tied to proton transfer within the biofilm. In this research, we quantified pH and redox potential variations in electrode-respiring Geobacter sulfurreducens biofilms as a function of respiration rates, measured as current. We also characterized pH and redox potential at the counter electrode. We concluded that (1) pH continued to decrease in the biofilm through different growth phases, showing that the pH is not always a limiting factor in a biofilm and (2) decreasing pH and increasing redox potential at the biofilm electrode were associated only with the biofilm, demonstrating that G. sulfurreducens biofilms respire in a unique internal environment. Redox potential inside the biofilm was also compared to the local biofilm potential measured by a graphite microelectrode, where the tip of the micro-electrode was allowed to acclimatize inside the biofilm. PMID:22549331

  20. Spectral butterfly and electronic localization in rippled-graphene nanoribbons: Mapping onto effective one-dimensional chains

    NASA Astrophysics Data System (ADS)

    Roman-Taboada, Pedro; Naumis, Gerardo G.

    2015-07-01

    We report an exact map into one-dimensional effective chains of the tight-binding Hamiltonian for electrons in armchair and zigzag graphene nanoribbons with any uniaxial ripple. This mapping is used for studying the effect of uniaxial periodic ripples, taking into account the relative orientation changes between π orbitals. Such effects are important for short-wavelength ripples, while for long-wave ones, the system behaves nearly as strained graphene. The spectrum has a complex nature, akin to the Hofstadter butterfly with a rich localization behavior. Gaps at the Fermi level and dispersionless bands were observed, as well. The complex features of the spectrum arise as a consequence of the quasiperiodic or periodic nature of the effective one-dimensional system. Some features of these systems can be understood by considering weakly coupled dimers. The eigenenergies of such dimers are highly degenerate, and the net effect of the ripple can be seen as a perturbation potential that splits the energy spectrum. Several particular cases were analytically solved to understand this feature.

  1. Scanning tunneling microscopy and spectroscopy of the electronic local density of states of graphite surfaces near monoatomic step edges

    NASA Astrophysics Data System (ADS)

    Niimi, Y.; Matsui, T.; Kambara, H.; Tagami, K.; Tsukada, M.; Fukuyama, Hiroshi

    2006-02-01

    We measured the electronic local density of states (LDOS) of graphite surfaces near monoatomic step edges, which consist of either the zigzag or armchair edge, with the scanning tunneling microscopy (STM) and spectroscopy (STS) techniques. The STM data reveal that the (3×3)R30° and honeycomb superstructures coexist over a length scale of 3-4nm from both the edges. By comparing with density-functional derived nonorthogonal tight-binding calculations, we show that the coexistence is due to a slight admixing of the two types of edges at the graphite surfaces. In the STS measurements, a clear peak in the LDOS at negative bias voltages from -100 to -20mV was observed near the zigzag edges, while such a peak was not observed near the armchair edges. We concluded that this peak corresponds to the graphite “edge state” theoretically predicted by Fujita [J. Phys. Soc. Jpn. 65, 1920 (1996)] with a tight-binding model for graphene ribbons. The existence of the edge state only at the zigzag type edge was also confirmed by our first-principles calculations with different edge terminations.

  2. Probing local and electronic structure in Warm Dense Matter: single pulse synchrotron x-ray absorption spectroscopy on shocked Fe

    NASA Astrophysics Data System (ADS)

    Torchio, Raffaella; Occelli, Florent; Mathon, Olivier; Sollier, Arnaud; Lescoute, Emilien; Videau, Laurent; Vinci, Tommaso; Benuzzi-Mounaix, Alessandra; Headspith, Jon; Helsby, William; Bland, Simon; Eakins, Daniel; Chapman, David; Pascarelli, Sakura; Loubeyre, Paul

    2016-06-01

    Understanding Warm Dense Matter (WDM), the state of planetary interiors, is a new frontier in scientific research. There exists very little experimental data probing WDM states at the atomic level to test current models and those performed up to now are limited in quality. Here, we report a proof-of-principle experiment that makes microscopic investigations of materials under dynamic compression easily accessible to users and with data quality close to that achievable at ambient. Using a single 100 ps synchrotron x-ray pulse, we have measured, by K-edge absorption spectroscopy, ns-lived equilibrium states of WDM Fe. Structural and electronic changes in Fe are clearly observed for the first time at such extreme conditions. The amplitude of the EXAFS oscillations persists up to 500 GPa and 17000 K, suggesting an enduring local order. Moreover, a discrepancy exists with respect to theoretical calculations in the value of the energy shift of the absorption onset and so this comparison should help to refine the approximations used in models.

  3. A triphenylamine-grafted imidazo[4,5-f][1,10]phenanthroline ruthenium(II) complex: acid-base and photoelectric properties.

    PubMed

    Fan, Su-Hua; Zhang, An-Guo; Ju, Chuan-Chuan; Gao, Li-Hua; Wang, Ke-Zhi

    2010-04-19

    A new heteroleptic ruthenium(II) complex of [Ru(Hipdpa)(Hdcbpy)(NCS)(2)](-).0.5H(+).0.5[N(C(4)H(9))(4)](+) Ru(Hipdpa) {where Hdcbpy = monodeprotonated 4,4'-dicarboxy-2,2'-bipyridine and Hipdpa = 4-(1H-imidazo[4,5-f][1,10]phenanthrolin-2-yl)-N,N-diphenylaniline} was synthesized and characterized by elementary analysis, standard spectroscopy techniques, and cyclic voltammetry. The ground- and excited-state acid-base properties of Ru(Hipdpa) were studied by means of UV-vis absorption spectrophotometric and spectrofluorimetric titrations in 4:1(v/v) Britton-Robinson/dimethylformamide buffer solution. The four-step separate protonation/deprotonation processes were found in the ground states, and one of which taking place near the physiological pH range. The two observable excited-state protonation/deprotonation processes were found for the Ru(Hipdpa), constituting pH-induced "off-on-off" emission switches. The performance of the complexes as photosensitizers in nanocrystalline TiO(2)-based liquid solar cells containing an electrolyte solution (0.05 M I(2), 0.5 M LiI, and 0.5 M 4-tert-butylpyridine in 50% acetonitrile and 50% propylene carbonate) was investigated and found to achieve a much improved device performance (a short-circuit photocurrent density of 18.7 mA cm(-2), an open-circuit voltage of 630 mV, and an overall conversion efficiency of 6.85%) compared to a triphenylamine-free parent complex [Ru(Hpip)(Hdcbpy)(NCS)(2)](-).[N(C(4)H(9))(4)](+)-based device {Hpip = 2-phenyl-1H-imidazo[4,5-f][1,10]phenanthroline} and a comparable performance to that of cis-bis(isothiocyanato)bis(2,2'-bipyridine-4,4'-dicarboxylic acid)ruthenium(II) (N3) under identical experimental conditions. A density functional theory calculation of the molecular structures and electronic properties of the complexes was also carried out in an effort to understand their effectiveness in TiO(2)-based solar cells.

  4. The relations among Shannon information entropy, quantum discord, concurrence and localization properties of one-dimensional single-electron wave functions

    NASA Astrophysics Data System (ADS)

    Gong, Longyan; Zheng, Yongcui; Wang, Haihong; Cheng, Weiwen; Zhao, Shengmei

    2014-09-01

    Shannon information entropy (SE), concurrence (CC), quantum discord (QD) and localization properties for various one-dimensional one-electron wave functions are intensively studied, respectively. They include Gaussian functions, power-law functions, and functions in the Anderson model and the Harper ones. For all these wave functions, we find that SE, CC and QD increase as the localization length of a wave function increases, respectively. There are linear or quadratic relationships between two of them. Therefore, we can confirm for the analyzed models that SE, CC and QD are statistically equivalent quantities to reflect the localization properties of wave functions though they are different measures of quantum information.

  5. [application of the analytical transmission electron microscopy techniques for detection, identification and visualization of localization of nanoparticles of titanium and cerium oxides in mammalian cells].

    PubMed

    Shebanova, A S; Bogdanov, A G; Ismagulova, T T; Feofanov, A V; Semenyuk, P I; Muronets, V I; Erokhina, M V; Onishchenko, G E; Kirpichnikov, M P; Shaitan, K V

    2014-01-01

    This work represents the results of the study on applicability of the modern methods of analytical transmission electron microscopy for detection, identification and visualization of localization of nanoparticles of titanium and cerium oxides in A549 cell, human lung adenocarcinoma cell line. A comparative analysis of images of the nanoparticles in the cells obtained in the bright field mode of transmission electron microscopy, under dark-field scanning transmission electron microscopy and high-angle annular dark field scanning transmission electron was performed. For identification of nanoparticles in the cells the analytical techniques, energy-dispersive X-ray spectroscopy and electron energy loss spectroscopy, were compared when used in the mode of obtaining energy spectrum from different particles and element mapping. It was shown that the method for electron tomography is applicable to confirm that nanoparticles are localized in the sample but not coated by contamination. The possibilities and fields of utilizing different techniques for analytical transmission electron microscopy for detection, visualization and identification of nanoparticles in the biological samples are discussed.

  6. Dimensional crossover of electron weak localization in ZnO/TiO{sub x} stacked layers grown by atomic layer deposition

    SciTech Connect

    Saha, D. E-mail: pmisra@rrcat.gov.in; Misra, P. E-mail: pmisra@rrcat.gov.in; Joshi, M. P.; Kukreja, L. M.; Bhartiya, S.; Gupta, M.

    2016-01-25

    We report on the dimensional crossover of electron weak localization in ZnO/TiO{sub x} stacked layers having well-defined and spatially-localized Ti dopant profiles along film thickness. These films were grown by in situ incorporation of sub-monolayer TiO{sub x} on the growing ZnO film surface and subsequent overgrowth of thin conducting ZnO spacer layer using atomic layer deposition. Film thickness was varied in the range of ∼6–65 nm by vertically stacking different numbers (n = 1–7) of ZnO/TiO{sub x} layers of nearly identical dopant-profiles. The evolution of zero-field sheet resistance (R{sub ◻}) versus temperature with decreasing film thickness showed a metal to insulator transition. On the metallic side of the metal-insulator transition, R{sub ◻}(T) and magnetoresistance data were found to be well corroborated with the theoretical framework of electron weak localization in the diffusive transport regime. The temperature dependence of both R{sub ◻} and inelastic scattering length provided strong evidence for a smooth crossover from 2D to 3D weak localization behaviour. Results of this study provide deeper insight into the electron transport in low-dimensional n-type ZnO/TiO{sub x} stacked layers which have potential applications in the field of transparent oxide electronics.

  7. New Theoretical Developments in Exploring Electronically Excited States: Including Localized Configuration Interaction Singles and Application to Large Helium Clusters

    NASA Astrophysics Data System (ADS)

    Closser, Kristina Danielle

    This thesis presents new developments in excited state electronic structure theory. Contrasted with the ground state, the electronically excited states of atoms and molecules often are unstable and have short lifetimes, exhibit a greater diversity of character and are generally less well understood. The very unusual excited states of helium clusters motivated much of this work. These clusters consist of large numbers of atoms (experimentally 103--109 atoms) and bands of nearly degenerate excited states. For an isolated atom the lowest energy excitation energies are from 1s → 2s and 1s → 2 p transitions, and in clusters describing the lowest energy band minimally requires four states per atom. In the ground state the clusters are weakly bound by van der Waals interactions, however in the excited state they can form well-defined covalent bonds. The computational cost of quantum chemical calculations rapidly becomes prohibitive as the size of the systems increase. Standard excited-state methods such as configuration interaction singles (CIS) and time-dependent density functional theory (TD-DFT) can be used with ≈100 atoms, and are optimized to treat only a few states. Thus, one of our primary aims is to develop a method which can treat these large systems with large numbers of nearly degenerate excited states. Additionally, excited states are generally formed far from their equilibrium structures. Vertical excitations from the ground state induce dynamics in the excited states. Thus, another focus of this work is to explore the results of these forces and the fate of the excited states. Very little was known about helium cluster excited states when this work began, thus we first investigated the excitations in small helium clusters consisting of 7 or 25 atoms using CIS. The character of these excited states was determined using attachment/detachment density analysis and we found that in the n = 2 manifold the excitations could generally be interpreted as

  8. Localization and chemical forms of cadmium in plant samples by combining analytical electron microscopy and X-ray spectromicroscopy

    NASA Astrophysics Data System (ADS)

    Isaure, Marie-Pierre; Fayard, Barbara; Sarret, Géraldine; Pairis, Sébastien; Bourguignon, Jacques

    2006-12-01

    Cadmium (Cd) is a metal of high toxicity for plants. Resolving its distribution and speciation in plants is essential for understanding the mechanisms involved in Cd tolerance, trafficking and accumulation. The model plant Arabidopsis thaliana was exposed to cadmium under controlled conditions. Elemental distributions in the roots and in the leaves were determined using scanning electron microscopy coupled with energy dispersive X-ray microanalysis (SEM-EDX), and synchrotron-based micro X-ray fluorescence (μ-XRF), which offers a better sensitivity. The chemical form(s) of cadmium was investigated using Cd L III-edge (3538 eV) micro X-ray absorption near edge structure (μ-XANES) spectroscopy. Plant μ-XANES spectra were fitted by linear combination of Cd reference spectra. Biological sample preparation and conditioning is a critical point because of possible artifacts. In this work we compared freeze-dried samples analyzed at ambient temperature and frozen hydrated samples analyzed at -170 °C. Our results suggest that in the roots Cd is localized in vascular bundles, and coordinated to S ligands. In the leaves, trichomes (epidermal hairs) represent the main compartment of Cd accumulation. In these specialized cells, μ-XANES results show that the majority of Cd is bound to O/N ligands likely provided by the cell wall, and a minor fraction could be bound to S-containing ligands. No significant difference in Cd speciation was observed between freeze-dried and frozen hydrated samples. This work illustrates the interest and the sensitivity of Cd L III-edge XANES spectroscopy, which is applied here for the first time to plant samples. Combining μ-XRF and Cd L III-edge μ-XANES spectroscopy offers promising tools to study Cd storage and trafficking mechanisms in plants and other biological samples.

  9. Diurnal evolution of the F region electron density local time gradient at low and middle latitudes resolved by the Swarm constellation

    NASA Astrophysics Data System (ADS)

    Xiong, Chao; Zhou, Yun-Liang; Lühr, Hermann; Ma, Shu-Ying

    2016-09-01

    In this study we have provided new insights into the local time gradient of F region electron density (ΔNe) derived from the lower pair of Swarm satellites flying side by side. Our result shows that the electron density (Ne) increase starts just at sunrise, around 06:00 LT, simultaneously at low and middle latitudes due to the increased photoionization. At equatorial latitudes the increase in electron density gets even steeper after 07:00 LT, and the steepest increase of electron density (about 3 · 1010 m-3 within 6 min) occurs around 09:00 LT. We suggest that the upward vertical plasma drift in connection with the buildup of the equatorial fountain effect plays a major role. We also found that the local time variations of the equatorial ionization anomaly (EIA) crest electron density during daytime are similar to the respective evolutions at the equator, but about 1-2 h delayed. We relate this delay to the response time between the equatorial electric field and the buildup of the plasma fountain. At equinox months a fast decrease of the F region electron density is seen at the EIA trough region during the prereversal enhancement, while an increase is found meanwhile at crest regions. Afterward, a fast decrease of the EIA crest electron density occurs between 19:00 and 23:00 LT, with seasonal dependence. The local time gradient between Swarm A and C shows also prominent longitudinal wave-4 pattern around August months, and the phase of DE3 in ΔNe is found to be delayed by 6 h compared to that in Ne.

  10. Evolutionary Conservation of pou5f3 Genomic Organization and Its Dynamic Distribution during Embryogenesis and in Adult Gonads in Japanese Flounder Paralichthys olivaceus

    PubMed Central

    Gao, Jinning; Wang, Xubo; Zhang, Quanqi

    2017-01-01

    Octamer-binding transcription factor 4 (Oct4) is a member of POU (Pit-Oct-Unc) transcription factor family Class V that plays a crucial role in maintaining the pluripotency and self-renewal of stem cells. Though it has been deeply investigated in mammals, its lower vertebrate homologue, especially in the marine fish, is poorly studied. In this study, we isolated the full-length sequence of Paralichthys olivaceus pou5f3 (Popou5f3), and we found that it is homologous to mammalian Oct4. We identified two transcript variants with different lengths of 3′-untranslated regions (UTRs) generated by alternative polyadenylation (APA). Quantitative real-time RT-PCR (qRT-PCR), in situ hybridization (ISH) and immunohistochemistry (IHC) were implemented to characterize the spatial and temporal expression pattern of Popou5f3 during early development and in adult tissues. Our results show that Popou5f3 is maternally inherited, abundantly expressed at the blastula and early gastrula stages, then greatly diminishes at the end of gastrulation. It is hardly detectable from the heart-beating stage onward. We found that Popou5f3 expression is restricted to the adult gonads, and continuously expresses during oogenesis while its dynamics are downregulated during spermatogenesis. Additionally, numerous cis-regulatory elements (CRE) on both sides of the flanking regions show potential roles in regulating the expression of Popou5f3. Taken together, these findings could further our understanding of the functions and evolution of pou5f3 in lower vertebrates, and also provides fundamental information for stem cell tracing and genetic manipulation in Paralichthys olivaceus. PMID:28124980

  11. Expression analysis of Cdx2 and Pou5f1 in a marsupial, the stripe-faced dunnart, during early development.

    PubMed

    Familari, Mary; Au, Phil Chi Khang; de Iongh, Robb U; Cruz, Yolanda; Selwood, Lynne

    2016-02-01

    The first lineage allocation during mouse development forms the trophectoderm and inner cell mass, in which Cdx2 and Pou5f1 display reciprocal expression. Yet Cdx2 is not required for trophectoderm specification in other mammals, such as the human, cow, pig, or in two marsupials, the tammar and opossum. The role of Cdx2 and Pou5f1 in the first lineage allocation of Sminthopsis macroura, the stripe-faced dunnart, is unknown. In this study, expression of Cdx2 and Pou5f1 during oogenesis, development from cleavage to blastocyst stages, and in the allocation of the first three lineages was analyzed for this dunnart. Cdx2 mRNA was present in late antral-stage oocytes, but not present again until Day 5.5. Pou5f1 mRNA was present from primary follicles to zygotes, and then expression resumed starting at the early unilaminar blastocyst stage. All cleavage stages and the pluriblast and trophoblast cells co-expressed CDX2 and POU5F1 proteins, which persisted until early stages of hypoblast formation. Hypoblast cells also show co-localisation of POU5F1 and CDX2 once they were allocated, and this persisted during their division and migration. Our studies suggest that CDX2, and possibly POU5F1, are maternal proteins, and that the first lineage to differentiate is the trophoblast, which differentiates to trophectoderm after shell loss one day before implantation. In the stripe-faced dunnart, cleavage cells, as well as trophoblast and pluriblast cells, are polarized, suggesting the continued presence of CDX2 in both lineages until late blastocyst stages may play a role in the formation and maintenance of polarity.

  12. Laser induced local structural and property modifications in semiconductors for electronic and photonic superstructures - Silicon carbide to graphene conversion

    NASA Astrophysics Data System (ADS)

    Yue, Naili

    Graphene is a single atomic layer two-dimensional (2D) hexagonal crystal of carbon atoms with sp2-bonding. Because of its various special or unique properties, graphene has attracted huge attention and considerable interest in recent years. This PhD research work focuses on the development of a novel approach to fabricating graphene micro- and nano-structures using a 532 nm Nd:YAG laser, a technique based on local conversion of 3C-SiC thin film into graphene. Different from other reported laser-induced graphene on single crystalline 4H- or 6H- SiC, this study focus on 3C-SiC polycrystal film grown using MBE. Because the SiC thin film is grown on silicon wafer, this approach may potentially lead to various new technologies that are compatible with those of Si microelectronics for fabricating graphene-based electronic, optoelectronic, and photonic devices. The growth conditions for depositing 3C-SiC using MBE on Si wafers with three orientations, (100), (110), and (111), were evaluated and explored. The surface morphology and crystalline structure of 3C-SiC epilayer were investigated with SEM, AFM, XRD, μ-Raman, and TEM. The laser modification process to convert 3C-SiC into graphene layers has been developed and optimized by studying the quality dependence of the graphene layers on incident power, irradiation time, and surface morphology of the SiC film. The laser and power density used in this study which focused on thin film SiC was compared with those used in other related research works which focused on bulk SiC. The laser-induced graphene was characterized with μ-Raman, SEM/EDS, TEM, AFM, and, I-V curve tracer. Selective deposition of 3C-SiC thin film on patterned Si substrate with SiO2 as deposition mask has been demonstrated, which may allow the realization of graphene nanostructures (e.g., dots and ribbons) smaller than the diffraction limit spot size of the laser beam, down to the order of 100 nm. The electrical conductance of directly written graphene

  13. Atomic-scale observation of a graded polar discontinuity and a localized two-dimensional electron density at an insulating oxide interface

    NASA Astrophysics Data System (ADS)

    Chang, C.-P.; Lin, J. G.; Jeng, H. T.; Cheng, S.-L.; Pong, W. F.; Shao, Y. C.; Chin, Y. Y.; Lin, H.-J.; Chen, C. W.; Yang, J.-R.; Chen, C. H.; Chu, M.-W.

    2013-02-01

    Using atomically resolved electron energy-loss spectroscopy, the atomic-plane-by-atomic-plane, unit-cell-by-unit-cell stoichiometry, and charge characteristics of the oxide interface (Nd0.35Sr0.65)MnO3/SrTiO3, with a primitive polar discontinuity of (Nd0.35Sr0.65O)0.35+-(TiO2)0, were thoroughly investigated. (Nd0.35Sr0.65)MnO3 is a strongly correlated insulator and the interface was characterized to be insulating. The cell-specific stoichiometric evaluation unveiled an extensive interdiffusion across the interface. The plane-specific charge characterization revealed that the interdiffusion grades the primitive polar discontinuity. Despite the graded polar discontinuity, a charge transfer inversely into (Nd0.35Sr0.65)MnO3 was firmly resolved with a length scale of ˜2 nm and a charge density on the order of ˜1013/cm2 and is effectively mediated by an asymmetric Ti interdiffusion. The intricate electronic correlations of the interfacial (Nd0.35Sr0.65)MnO3 unit cells and the interdiffusion-induced chemical disorder tend to render the charges localized, resulting in a localized two-dimensional electron density and thus the insulating interface, in distinct contrast to the conventional understanding of a vanishing charge density for an insulating interface and the metallic two-dimensional electron gas found at other classical polar-discontinuous interface systems. A potential strain manipulation on the electronic localization of the electron density was also proposed.

  14. Electronic transitions, crystal field effects and phonons in UO 2

    NASA Astrophysics Data System (ADS)

    Schoenes, J.

    1980-08-01

    An extensive optical study of the 5f magnetic semiconductor UO 2 is presented. The experimental data include near normal incidence reflectivity measurements from 0.0025 to 13 eV, absorption and Faraday rotation measurements as function of temperature and of magnetic fields up to 100 kOe and photoemission results. From the data in the fundamental absorption region an energy level scheme is derived. This level scheme differs markedly from an earlier model but it is quantitatively supported by a calculation using the thermochemical Haber-Born process and also by cluster calculations. The localized nature of the 5f electrons is demonstrated. The absorption edge at 2 eV shows an abrupt shift to lower energies at the first order phase transition of UO 2 to the antiferromagnetic state. This shift is shown to be larger than expected from the lattice contraction indicating a magnetic order induced contribution to the total red shift. Below the absorption edge, intra-5f transitions and multiphonon excitations are reported, showing striking order induced effects at and below TN = 30.8 K. New results are presented for ε st, ε opt, ω TO and ω LO which fulfill the Lyddane-Sachs-Teller relation.

  15. Effect of magnetic field on energy spectrum and localization of electron in CdS/HgS/CdS/HgS/CdS multilayered spherical nanostructure

    NASA Astrophysics Data System (ADS)

    Holovatsky, V. A.; Bernik, I. B.; Yakhnevych, M. Ya.

    2017-03-01

    The theoretical investigation of magnetic field effect on energy spectrum and localization of the electron and oscillator strengths of intraband quantum transitions in the nanostructure CdS/HgS/CdS/HgS/CdS is performed. The calculations are made in the framework of effective mass approximation and rectangular potential barriers model using the method of the expansion of quasi-particle wave functions over the complete basis of functions obtained as the exact solutions of the Schrodinger equation for the electron in the nanostructure without the magnetic field. It is shown that the magnetic field violates the spherical symmetry of the system and takes off the degeneration of energy spectrum with respect to the magnetic quantum number. The energy of the electron in the states with m≥0 increases when magnetic field enhances; for the states with m<0 these dependences are non-monotonous (decreasing at first and then increasing). Moreover, the ground state of electron is formed alternately by the states with m=0, -1, -2, …. Magnetic field influences on the distribution of quasi-particle density. It is shown that the electron significantly changes its localization in the nanostructure with two potential wells tunneling through the potential barrier under the effect of magnetic field, changing the oscillator strengths of intraband quantum transitions.

  16. Electronic Structures of Uranium Compounds Studied by Soft X-ray Photoelectron Spectroscopy

    NASA Astrophysics Data System (ADS)

    Fujimori, Shin-ichi; Takeda, Yukiharu; Okane, Tetsuo; Saitoh, Yuji; Fujimori, Atsushi; Yamagami, Hiroshi; Haga, Yoshinori; Yamamoto, Etsuji; Ōnuki, Yoshichika

    2016-06-01

    The electronic structures of uranium-based compounds have been studied by photoelectron spectroscopy with soft X-ray synchrotron radiation. Angle-resolved photoelectron spectroscopy with soft X-rays has made it possible to directly observe their bulk band structures and Fermi surfaces. It has been shown that the band structures and Fermi surfaces of itinerant compounds such as UB2, UN, and UFeGa5 are quantitatively described by a band-structure calculation treating all U 5f electrons as itinerant. Furthermore, the overall electronic structures of heavy-fermion compounds such as UPd2Al3, UNi2Al3, and URu2Si2 are also explained by a band-structure calculation, although some disagreements exist, which might originate from the electron correlation effect. This suggests that the itinerant description of U 5f states is an appropriate starting point for the description of their electronic structures. The situation is similar for ferromagnetic superconductors such as UGe2, URhGe, UCoGe, and UIr, although the complications from their low-symmetry crystal structures make it more difficult to describe their detailed electronic structures. The local electronic structures of the uranium site have been probed by core-level photoelectron spectroscopy with soft X-rays. The comparisons of core-level spectra of heavy-fermion compounds with typical itinerant and localized compounds suggest that the local electronic structures of most itinerant and heavy-fermion compounds are close to the U 5f3 configuration except for UPd2Al3 and UPt3. The core-level spectrum of UPd2Al3 has similarities to those of both itinerant and localized compounds, suggesting that it is located at the boundary between the itinerant and localized states. Moreover, the spectrum of UPt3 is very close to that of the localized compound UPd3, suggesting that it is nearly localized, although there are narrow quasi-particle bands in the vicinity of EF.

  17. Alternative Chemical Cleaning Methods for High Level Waste Tanks: Actual Waste Testing with SRS Tank 5F Sludge

    SciTech Connect

    King, William D.; Hay, Michael S.

    2016-08-30

    Solubility testing with actual High Level Waste tank sludge has been conducted in order to evaluate several alternative chemical cleaning technologies for the dissolution of sludge residuals remaining in the tanks after the exhaustion of mechanical cleaning and sludge sluicing efforts. Tests were conducted with archived Savannah River Site (SRS) radioactive sludge solids that had been retrieved from Tank 5F in order to determine the effectiveness of an optimized, dilute oxalic/nitric acid cleaning reagent toward dissolving the bulk non-radioactive waste components. Solubility tests were performed by direct sludge contact with the oxalic/nitric acid reagent and with sludge that had been pretreated and acidified with dilute nitric acid. For comparison purposes, separate samples were also contacted with pure, concentrated oxalic acid following current baseline tank chemical cleaning methods. One goal of testing with the optimized reagent was to compare the total amounts of oxalic acid and water required for sludge dissolution using the baseline and optimized cleaning methods. A second objective was to compare the two methods with regard to the dissolution of actinide species known to be drivers for SRS tank closure Performance Assessments (PA). Additionally, solubility tests were conducted with Tank 5 sludge using acidic and caustic permanganate-based methods focused on the “targeted” dissolution of actinide species.

  18. Stabilization of Tetravalent 4f (Ce), 5d (Hf), or 5f (Th, U) Clusters by the [α-SiW9O34](10-) Polyoxometalate.

    PubMed

    Duval, Sylvain; Béghin, Sébastien; Falaise, Clément; Trivelli, Xavier; Rabu, Pierre; Loiseau, Thierry

    2015-09-08

    The reaction of Na10[α-SiW9O34] with tetravalent metallic cations such as 4f ((NH4)2Ce(NO3)6), 5d (HfCl4), or 5f (UCl4 and Th(NO3)4) in a pH 4.7 sodium acetate buffer solution leads to the formation of four sandwich-type polyoxometalates [Ce4(μ(3)-O)2(SiW9O34)2(CH3COO)2](10-) (1), [U4(μ(3)-O)2(SiW9O34)2(CH3COO)2](10-) (2), [Th3(μ(3)-O)(μ(2)-OH)3(SiW9O34)2](13-) (3), and [Hf3(μ(2)-OH)3(SiW9O34)2](11-) (4). All four compounds consist of a polynuclear cluster fragment stabilized by two [α-SiW9O34](10-) polyanions. Compounds 1 and 2 are isostructural with a tetranuclear core (Ce4, U4), while compound 3 presents a trinuclear Th3 core bearing a μ(3)-O-centered bridge. It is an unprecedented configuration in the case of the thorium(IV) cluster. Compound 4 also possesses a trinuclear Hf3 core but with the absence of the μ(3)-O bridge. The molecules have been characterized by single-crystal X-ray diffraction, (183)W and (29)Si nuclear magnetic resonance (NMR) spectroscopy, infrared (IR) spectroscopy, thermogravimetric analysis (TGA), and scanning electron microscopy/energy-dispersive X-ray (SEM/EDX) analysis.

  19. Formation and microstructural properties of locally distributed ZnSiO3 nanoparticles embedded in a SiO2 layer by using a focused electron beam.

    PubMed

    Shin, J W; No, Y S; Kim, T W; Choi, W K

    2008-10-01

    Locally distributed crystalline ZnSiO3 nanoparticles embedded in a SiO2 layer inserted between the ZnO thin film and the Si substrate were formed using transmission electron microscopy (TEM) with a focused electron beam irradiation process. High-resolution TEM (HRTEM) images and energy dispersive X-ray spectroscopy (EDS) profiles showed that ZnSiO3 nanocrystals with a size of approximately 6 nm were formed in the SiO2 layer. The formation mechanisms of the ZnSiO3 nanocrystals in the SiO2 layer are described on the basis of the HRTEM images and the EDS profiles.

  20. Evidence for New Excess Electron Localization Sites in Na{sub {ital n}}F{sub {ital n}{minus}1 } Alkali-Halide Clusters

    SciTech Connect

    Durand, G.; Spiegelmann, F.; Labastie, P.; LHermite, J.; Poncharal, P.

    1997-07-01

    This Letter examines new types of localization sites for an excess electron in finite alkali-halide clusters resulting from defects on cuboidal structures, namely {open_quotes}edge states,{close_quotes} R center, and other surface defects. We present theoretical calculations on Na{sub n}F {sub n{minus}1} clusters with one excess electron. Comparisons with experimental results are presented for different cluster sizes (n=17 , 23, 28, and 29). Structures with edge or surface defects are relevant for n=23 , 28, and 29. {copyright} {ital 1997} {ital The American Physical Society}

  1. Combination of the human anti-CD30 antibody 5F11 with cytostatic drugs enhances its antitumor activity against Hodgkin and anaplastic large cell lymphoma cell lines.

    PubMed

    Heuck, Friederike; Ellermann, Julia; Borchmann, Peter; Rothe, Achim; Hansen, Hinrich; Engert, Andreas; von Strandmann, Elke Pogge

    2004-01-01

    Due to its selective overexpression on the malignant cells of Hodgkin's lymphoma (HL) and large cell anaplastic lymphoma (ALCL), CD30 is an excellent target for immunotherapy of these diseases. The fully human monoclonal anti-CD30-antibody 5F11 has been shown to be effective against CD30-expressing cell lines both in vitro and in vivo. In addition, 5F11 shows promising antitumor activity in phase 1/2 clinical trials. To extend these promising results, the authors evaluated combinations of 5F11 with conventional cytostatic drugs against a variety of lymphoma cell lines in vitro. Most combinations tested showed at least additive cytotoxic effects on the HL-derived cell lines L428, L540, and L1236 and the ALCL-derived cell line Karpas 299 as measured by proliferation assays (XTT) and the induction of apoptosis (annexin-V FACS analysis). The most impressive results were detected with the combination of 5F11 and gemcitabine or etoposide. The data suggest that the combination of the human antibody 5F11 with conventional chemotherapy might be beneficial in the combined chemo-immunotherapy of CD30-positive lymphomas.

  2. Aloe-Emodin Protects RIN-5F (Pancreatic β-cell) Cell from Glucotoxicity via Regulation of Pro-Inflammatory Cytokine and Downregulation of Bax and Caspase 3.

    PubMed

    Alshatwi, Ali A; Subash-Babu, P

    2016-01-01

    To determine the protective effect of aloe-emodin (AE) from high glucose induced toxicity in RIN-5F (pancreatic β-cell) cell and restoration of its function was analyzed. RIN-5F cells have been cultured in high glucose (25 mM glucose) condition, with and without AE treatment. RIN-5F cells cultured in high glucose decreased cell viability and increased ROS levels after 48 hr compared with standard medium (5.5 mM glucose). Glucotoxicity was confirmed by significantly increased ROS production, increased pro-inflammatory (IFN-γ, IL-1β,) & decreased anti-inflammatory (IL-6&IL-10) cytokine levels, increased DNA fragmentation. In addition, we found increased Bax, caspase 3, Fadd, and Fas and significantly reduced Bcl-2 expression after 48 hr. RIN-5F treated with both high glucose and AE (20 μM) decreased ROS generation and prevent RIN-5F cell from glucotoxicity. In addition, AE treated cells cultured in high glucose were transferred to standard medium, normal responsiveness to glucose was restored within 8hr and normal basal insulin release within 24 hr was achieved when compared to high glucose.

  3. Aloe-Emodin Protects RIN-5F (Pancreatic β-cell) Cell from Glucotoxicity via Regulation of Pro-Inflammatory Cytokine and Downregulation of Bax and Caspase 3

    PubMed Central

    Alshatwi, Ali A; Subash-Babu, P.

    2016-01-01

    To determine the protective effect of aloe-emodin (AE) from high glucose induced toxicity in RIN-5F (pancreatic β-cell) cell and restoration of its function was analyzed. RIN-5F cells have been cultured in high glucose (25 mM glucose) condition, with and without AE treatment. RIN-5F cells cultured in high glucose decreased cell viability and increased ROS levels after 48 hr compared with standard medium (5.5 mM glucose). Glucotoxicity was confirmed by significantly increased ROS production, increased pro-inflammatory (IFN-γ, IL-1β,) & decreased anti-inflammatory (IL-6&IL-10) cytokine levels, increased DNA fragmentation. In addition, we found increased Bax, caspase 3, Fadd, and Fas and significantly reduced Bcl-2 expression after 48 hr. RIN-5F treated with both high glucose and AE (20 μM) decreased ROS generation and prevent RIN-5F cell from glucotoxicity. In addition, AE treated cells cultured in high glucose were transferred to standard medium, normal responsiveness to glucose was restored within 8hr and normal basal insulin release within 24 hr was achieved when compared to high glucose. PMID:26759701

  4. Localized surface plasmon induced enhancement of electron-hole generation with silver metal island at n-Al:ZnO/p-Cu{sub 2}O heterojunction

    SciTech Connect

    Kaur, Gurpreet Yadav, K. L.; Mitra, Anirban

    2015-08-03

    Localized surface plasmon induced generation of electron-hole pairs with inclusion of metal islands of noble metal like Ag can enhance the photocurrent. A heterostructure of n-Al:ZnO/p-Cu{sub 2}O with inclusion of Ag metalislands at the junction has been fabricated. I-V characteristic curve of these heterostructures shows a significant enhancement of photocurrent under the illumination (1.5 AMU). This enhancement of photocurrent is attributed to the supply of hot electrons generated in silver metal nanoislands. It has also been shown that inclusion of metal islands increases the absorption of solar spectrum in visible region at 500 nm. Enhancement of photocurrent may also be due to the direct resonance energy transfer from Localized Surface Plasmons of metal islands to Cu{sub 2}O.

  5. Temperature dependent evolution of the electronic and local atomic structure in the cubic colossal magnetoresistive manganite La1-xSrxMnO3

    SciTech Connect

    Arenholz, Elke; Mannella, N.; Booth, C.H.; Rosenhahn, A.; Sell, B.C.; Nambu, A.; Marchesini, S.; Mun, B. S.; Yang, S.-H.; Watanabe, M.; Ibrahim, K.; Arenholz, E.; Young, A.; Guo, J.; Tomioka, Y.; Fadley, C.S.

    2007-12-06

    We have studied the temperature-dependent evolution of the electronic and local atomic structure in the cubic colossal magnetoresistive manganite La{sub 1-x}Sr{sub x}MnO{sub 3} (x= 0.3-0.4) with core and valence level photoemission (PE), x-ray absorption spectroscopy (XAS), x-ray emission spectroscopy (XES), resonant inelastic x-ray scattering (RIXS), extended x-ray absorption fine structure (EXAFS) spectroscopy and magnetometry. As the temperature is varied across the Curie temperature T{sub c}, our PE experiments reveal a dramatic change of the electronic structure involving an increase in the Mn spin moment from {approx} 3 {micro}B to {approx} 4 {micro}B, and a modification of the local chemical environment of the other constituent atoms indicative of electron localization on the Mn atom. These effects are reversible and exhibit a slow-timescale {approx}200 K-wide hysteresis centered at T{sub c}. Based upon the probing depths accessed in our PE measurements, these effects seem to survive for at least 35-50 {angstrom} inward from the surface, while other consistent signatures for this modification of the electronic structure are revealed by more bulk sensitive spectroscopies like XAS and XES/RIXS. We interpret these effects as spectroscopic fingerprints for polaron formation, consistent with the presence of local Jahn-Teller distortions of the MnO{sub 6} octahedra around the Mn atom, as revealed by the EXAFS data. Magnetic susceptibility measurements in addition show typical signatures of ferro-magnetic clusters formation well above the Curie temperature.

  6. The local skin dose conversion coefficients of electrons, protons and alpha particles calculated using the Geant4 code.

    PubMed

    Zhang, Bintuan; Dang, Bingrong; Wang, Zhuanzi; Wei, Wei; Li, Wenjian

    2013-10-01

    The skin tissue-equivalent slab reported in the International Commission on Radiological Protection (ICRP) Publication 116 to calculate the localised skin dose conversion coefficients (LSDCCs) was adopted into the Monte Carlo transport code Geant4. The Geant4 code was then utilised for computation of LSDCCs due to a circular parallel beam of monoenergetic electrons, protons and alpha particles <10 MeV. The computed LSDCCs for both electrons and alpha particles are found to be in good agreement with the results using the MCNPX code of ICRP 116 data. The present work thus validates the LSDCC values for both electrons and alpha particles using the Geant4 code.

  7. Local structures of electrons with energies of hundreds of keV in the inner belt and the slot region observed from the Vernov satellite

    NASA Astrophysics Data System (ADS)

    Kovtyukh, A. S.; Myagkova, I. N.; Bogomolov, A. V.; Bogomolov, V. V.; Panasyuk, M. I.; Svertilov, S. I.

    2016-11-01

    The structure and dynamics of electron fluxes of subrelativistic energies in the range 235-300 keV at L < 4 during December 3-8, 2014, are analyzed according to the RELEC instrument onboard the Vernov satellite. Sharp changes in the parameters of the solar wind and the IMF were detected on December 6, but they did not lead to a magnetic storm. However, after the event of December 6, subrelativistic electron fluxes in the inner belt and the slot region were enhanced and structured. The dynamics of electron fluxes in the local transient bursts at L 1.5-1.7 is considered in detail. It is shown that these bursts are associated with the development of the cyclotron instability in the tops of magnetic flux tubes near the inner belt maximum. The electron anisotropic index is estimated in these bursts. It is shown that in the beginning these bursts are anisotropic and that they become isotropic as the decay proceeds. The most likely chain of physical mechanisms that could lead to variations in electron fluxes of the inner belt described in this paper is presented. For the first time, the topological effects in stationary distributions of the electrons of the inner belt observed at low altitudes in the South Atlantic Anomaly region are explained.

  8. Dynamical properties and instability of local fluorite BaF(2) structure around doped Mn(2+) ions-EPR and electron spin echo studies.

    PubMed

    Lijewski, S; Hoffmann, S K; Goslar, J; Wencka, M; Ulanov, V A

    2008-09-24

    The electron paramagnetic resonance (EPR) and electron spin echo (ESE) were measured at the X-band for Mn(2+) in a BaF(2) crystal in the temperature range 4.2-300 K. In addition to the cubic symmetry centre, two other lower concentration tetragonal centres were identified. Temperature variations and computer simulation of the EPR spectrum confirm that the cubic symmetry of the MnF(8) centre is deformed to two T(d) tetrahedra of different dimensions at around 45 K. Electron spin relaxation was measured in the temperature range 4.2-35 K, where the ESE signal was detectable. For higher temperature the Mn(2+) dynamics produces homogeneously broadened EPR lines. At the lowest temperatures the spin-lattice relaxation is governed by ordinary phonon processes with 1/T(1)∼T(5). The efficiency of these processes rapidly decreases and at about 11 K a local mode of energy 17 cm(-1) becomes the relaxation mechanism. Phase relaxation observed as ESE signal dephasing indicates that after the local deformation jumps (tunnelling with frequency 4 × 10(8) s(-1)) between the two tetrahedral configurations appear, with the energy barrier being the local mode energy. This motion is directly visible as a resonance-type enhancement of the ESE dephasing rate 1/T(M) around 11 K. Only the cubic centre displays the above dynamics.

  9. Hyperglycemia promotes p53-Mdm2 interaction but reduces p53 ubiquitination in RINm5F cells.

    PubMed

    Barzalobre-Gerónimo, R; Raúl, Barzalobre-Gerónimo; Flores-López, L A; Antonio, Flores-López Luis; Baiza-Gutman, L A; Arturo, Baiza-Gutman Luis; Cruz, M; Miguel, Cruz; García-Macedo, R; Rebeca, García-Macedo; Ávalos-Rodríguez, A; Alejandro, Ávalos-Rodríguez; Contreras-Ramos, A; Alejandra, Contreras-Ramos; Díaz-Flores, A; Margarita, Díaz-Flores; Ortega-Camarillo, C; Clara, Ortega-Camarillo

    2015-07-01

    The apoptosis of β cells induced by hyperglycemia has been associated with p53 mobilization to mitochondria and p53 phosphorylation. Murine double minute 2 (Mdm2) induces the degradation of p53 and thereby protects cells from apoptosis. We studied the effect of glucose at high concentration on the ability of Mdm2 to ubiquitinate p53 and promote its degradation. RINm5F cells were grown in RPMI-1640 medium with 5 or 30 mM glucose for varying periods of time. After this treatment, the expression of Mdm2 was measured using real-time PCR. The phosphorylation of Mdm2 at Ser166, p53 at Ser15, and the kinases Akt and ATM were measured by Western blotting. The formation of the p53-Mdm2 complex and p53 ubiquitination was assessed by p53 immunoprecipitation and immunofluorescence. Our results showed that high glucose reduced Mdm2 mRNA expression and protein concentration and increased Mdm2 and Akt phosphorylation, albeit with slower kinetics for Akt. It also promoted p53-Mdm2 complex formation, whereas p53 ubiquitination was suppressed. Furthermore, phosphorylation of both p53 Ser15 and ATM was increased in the presence of 30 mM glucose. These data indicate that high concentration glucose decrease the mRNA expression and cytosolic concentration of Mdm2. However, although the increase in glucose promoted the phosphorylation of Mdm2, it also decreased p53 ubiquitination, thus avoiding p53 degradation. In hyperglycemic conditions, such as diabetes mellitus, the reduction of pancreatic β cells mass is favored by stabilization of p53 in association with low p53 ubiquitination and reduced expression of Mdm2.

  10. Superconductivity phase diagram of Se-substituted CeO0.5F0.5Bi(S1-xSex)2

    NASA Astrophysics Data System (ADS)

    Mizuguchi, Yoshikazu; Hiroi, Takafumi; Miura, Osuke

    2016-02-01

    We investigated the effects of Se substitution on the lattice constants and superconducting properties of CeO0.5F0.5Bi(S1-xSex)2. With increasing Se concentration, the a lattice constant increased, while the c lattice constant did not show any significant increase between x = 0.1 and x = 0.5. Bulk superconductivity was observed in samples with x = 0.2-0.4, and the superconducting transition temperature was the highest at x = 0.3. The obtained superconductivity phase diagram was compared to those of LaO0.5F0.5Bi(S1-xSex)2 and NdO0.5F0.5Bi(S1-xSex)2.

  11. Detection of local chemical states of lithium and their spatial mapping by scanning transmission electron microscopy, electron energy-loss spectroscopy and hyperspectral image analysis.

    PubMed

    Muto, Shunsuke; Tatsumi, Kazuyoshi

    2017-02-08

    Advancements in the field of renewable energy resources have led to a growing demand for the analysis of light elements at the nanometer scale. Detection of lithium is one of the key issues to be resolved for providing guiding principles for the synthesis of cathode active materials, and degradation analysis after repeated use of those materials. We have reviewed the different techniques currently used for the characterization of light elements such as high-resolution transmission electron microscopy, scanning transmission electron microscopy (STEM) and electron energy-loss spectroscopy (EELS). In the present study, we have introduced a methodology to detect lithium in solid materials, particularly for cathode active materials used in lithium-ion battery. The chemical states of lithium were isolated and analyzed from the overlapping multiple spectral profiles, using a suite of STEM, EELS and hyperspectral image analysis. The method was successfully applied in the chemical state analyses of hetero-phases near the surface and grain boundary regions of the active material particles formed by chemical reactions between the electrolyte and the active materials.

  12. CONDENSED MATTER: ELECTRONIC STRUCTURE, ELECTRICAL, MAGNETIC, AND OPTICAL PROPERTIES: Localized electronic states in gaps on hole-net structures of silicon

    NASA Astrophysics Data System (ADS)

    Huang, Wei-Qi; Lü, Quan; Zhang, Rong-Tao; Wang, Xiao-Yun; Yu, Shi-Qiang

    2009-11-01

    Hole-net structure silicon is fabricated by laser irradiation and annealing, on which a photoluminescence (PL) band in a the region of 650-750 nm is pinned and its intensity increases obviously after oxidation. It is found that the PL intensity changes with both laser irradiation time and annealing time. Calculations show that some localized states appear in the band gap of the smaller nanocrystal when Si = O bonds or Si-O-Si bonds are passivated on the surface. It is discovered that the density and the number of Si = O bonds or Si-O-Si bonds related to both the irradiation time and the annealing time obviously affect the generation of the localized gap states of hole-net silicon, by which the production of stimulated emission through controlling oxidation time can be explained.

  13. Nano-focused Bremstrahlung Isochromat Spectroscopy (nBIS) Determination of the Unoccupied Electronic Structure of Pu

    SciTech Connect

    Tobin, J G; Butterfield, M; Teslich, N; Bliss, A; Chung, B; Gross, J; McMahan, A; Schwartz, A

    2006-12-20

    While chemically toxic and highly radioactive, Pu may be the most scientifically interesting element in the periodic table. It's properties include the following: six different phases, close to each other in energy and sensitive to variations of temperature, pressure and chemistry; the face-centered-cubic phase (delta) is the least dense; Pu expands when it solidifies from the melt; and it is clearly the nexus of the actinide binary phase diagrams of the actinides. In a sense, it is the boundary between the light (ostensibly delocalized 5f electrons) and heavy (ostensibly localized or correlated 5f electrons) actinide elements, but this is an over-simplification. The localized atomic 5f states are naturally correlated, but important regimes of correlated electron states are conceivable as extended states on the delocalized side of the possible Mott transition between conductive and insulating behavior. The proximity to this crossover may be the driving force behind all these exotic properties. Pu remains of immense scientific and technological importance and the advancement to a firm, scientific understanding of the electronic structure of Pu and its compounds, mixtures, alloys and solutions is a crucial issue. Moreover, while there are a number of ongoing experimental efforts directed at determining the occupied (valence band, below the Fermi Energy) electronic structure of Pu, there is essential no experimental data on the unoccupied (conduction band, above the Fermi Energy) electronic structure of Pu. Our objective is to determine the conduction band (unoccupied) electronic structure of Pu and other actinides (and possibly rare earths as well), in a phase specific fashion and emphasizing bulk contributions. This is world-class science directed at issue that is central to LLNL and DOE: Pu structure property relationships.

  14. Latitudinal variation of the specific local time of postmidnight enhancement peaks in F layer electron density at low latitudes: A case study

    NASA Astrophysics Data System (ADS)

    Jiang, Chunhua; Deng, Chi; Yang, Guobin; Liu, Jing; Zhu, Peng; Yokoyama, Tatsuhiro; Song, Huan; Lan, Ting; Zhou, Chen; Wu, Xiongbin; Zhang, Yuannong; Zhao, Zhengyu; Komolmis, Tharadol; Supnithi, Pornchai; Yatini, Clara Y.

    2016-04-01

    Ionospheric nighttime enhancements are manifested in an increase of the electron density at nighttime. This paper studies the latitudinal variation of the specific local time of postmidnight enhancement peaks using ionosondes distributed at low latitudes. To obtain the parameters of the ionosphere, we manually extracted ionograms recorded by ionosondes. Cases show that there are significant latitudinal variations in the observed local time of the postmidnight enhancement peaks. Results show that the lower the geomagnetic latitude, the earlier the enhancement peak occurred in the geomagnetic northern hemisphere. Additionally, the enhancement peaks occurred earlier in the geomagnetic southern hemisphere than that in the geomagnetic northern hemisphere for these present cases. We suggest that the combined effect of the geomagnetic inclination and transequatorial meridional wind might be the main driving force for latitudinal variation of the local time of the occurrence.

  15. Impact of local strain on Ti-L₂,₃ electron energy-loss near-edge structures of BaTiO₃: a first-principles multiplet study.

    PubMed

    Ootsuki, Shirou; Ikeno, Hidekazu; Umeda, Yuji; Yonezawa, Yu; Moriwake, Hiroki; Kuwabara, Akihide; Kido, Osamu; Ueda, Satoko; Tanaka, Isao; Fujikawa, Yoshinori; Mizoguchi, Teruyasu

    2014-06-01

    Identification of local strains is crucial because the local strains largely influence the ferroelectric property of BaTiO₃. The effects of local strains induced by external pressures on the Ti-L₂,₃ electron energy-loss near-edge structure (ELNES) of BaTiO₃ were theoretically investigated using first-principles multiplet calculations. We revealed that the effects appear in the position of the spectral threshold, namely the spectrum shifts to lower and higher energy sides by the tensile and compressive pressures, respectively. We concluded that conventional ELNES observations can identify only large strains induced by -10 GPa, and 0.1 eV energy resolution is required to identify ±2% of strains.

  16. Temperature dependent behavior of localized and delocalized electrons in nitrogen-doped 6H SiC crystals as studied by electron spin resonance

    SciTech Connect

    Savchenko, D.; Kalabukhova, E.; Shanina, B.; Kiselov, V.; Cichoň, S.; Honolka, J.; Mokhov, E.

    2016-01-28

    We have studied the temperature behavior of the electron spin resonance (ESR) spectra of nitrogen (N) donors in n-type 6H SiC crystals grown by Lely and sublimation sandwich methods (SSM) with donor concentration of 10{sup 17 }cm{sup −3} at T = 60–150 K. A broad signal in the ESR spectrum was observed at T ≥ 80 K with Lorentzian lineshape and g{sub ||} = 2.0043(3), g{sub ⊥} = 2.0030(3), which was previously assigned in the literature to the N donors in the 1s(E) excited state. Based on the analysis of the ESR lineshape, linewidth and g-tensor we attribute this signal to the conduction electrons (CE). The emergence of the CE ESR signal at T > 80 K was explained by the ionization of electrons from the 1s(A{sub 1}) ground and 1s(E) excited states of N donors to the conduction band while the observed reduction of the hyperfine (hf) splitting for the N{sub k1,k2} donors with the temperature increase is attributed to the motional narrowing effect of the hf splitting. The temperature dependence of CE ESR linewidth is described by an exponential law (Orbach process) with the activation energy corresponding to the energy separation between 1s(A{sub 1}) and 1s(E) energy levels for N residing at quasi-cubic sites (N{sub k1,k2}). The theoretical analysis of the temperature dependence of microwave conductivity measured by the contact-free method shows that due to the different position of the Fermi level in two samples the ionization of free electrons occurs from the energy levels of N{sub k1,k2} donors in Lely grown samples and from the energy level of N{sub h} residing at hexagonal position in 6H SiC grown by SSM.

  17. Materials Data on Pr4Se3(O5F3)2 (SG:15) by Materials Project

    SciTech Connect

    Kristin Persson

    2016-05-18

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  18. Materials Data on ReH12C4O5F (SG:2) by Materials Project

    SciTech Connect

    Kristin Persson

    2016-02-11

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  19. Materials Data on Na15S5Cl(O5F)4 (SG:157) by Materials Project

    SciTech Connect

    Kristin Persson

    2014-07-09

    Computed materials data using density functional theory calculations. These calculations determine the electronic structure of bulk materials by solving approximations to the Schrodinger equation. For more information, see https://materialsproject.org/docs/calculations

  20. A Transition from Localized to Strongly Correlated Electron Behavior and Mixed Valence Driven by Physical or Chemical Pressure in ACo2As2 (A = Eu and Ca).

    PubMed

    Tan, Xiaoyan; Fabbris, Gilberto; Haskel, Daniel; Yaroslavtsev, Alexander A; Cao, Huibo; Thompson, Corey M; Kovnir, Kirill; Menushenkov, Alexey P; Chernikov, Roman V; Garlea, V Ovidiu; Shatruk, Michael

    2016-03-02

    We demonstrate that the action of physical pressure, chemical compression, or aliovalent substitution in ACo2As2 (A = Eu and Ca) has a general consequence of causing these antiferromagnetic materials to become ferromagnets. In all cases, the mixed valence triggered at the electropositive A site results in the increase of the Co 3d density of states at the Fermi level. Remarkably, the dramatic alteration of magnetic behavior results from the very minor (<0.15 electron) change in the population of the 3d orbitals. The mixed valence state of Eu observed in the high-pressure (HP) form of EuCo2As2 exhibits a remarkable stability, achieving the average oxidation state of +2.25 at 12.6 GPa. In the case of CaCo2As2, substituting even 10% of Eu or La into the Ca site causes ferromagnetic ordering of Co moments. Similar to HP-EuCo2As2, the itinerant 3d ferromagnetism emerges from electronic doping into the Co layer because of chemical compression of Eu sites in Ca0.9Eu0.1Co1.91As2 or direct electron doping in Ca0.85La0.15Co1.89As2. The results reported herein demonstrate the general possibility of amplifying minor localized electronic effects to achieve major changes in material's properties via involvement of strongly correlated electrons.

  1. A Transition from Localized to Strongly Correlated Electron Behavior and Mixed Valence Driven by Physical or Chemical Pressure in ACo2As2 (A = Eu and Ca)

    DOE PAGES

    Tan, Xiaoyan; Fabbris, Gilberto; Haskel, Daniel; ...

    2016-02-03

    In this paper, we demonstrate that the action of physical pressure, chemical compression, or aliovalent substitution in ACo2As2 (A = Eu and Ca) has a general consequence of causing these antiferromagnetic materials to become ferromagnets. In all cases, the mixed valence triggered at the electropositive A site results in the increase of the Co 3d density of states at the Fermi level. Remarkably, the dramatic alteration of magnetic behavior results from the very minor (<0.15 electron) change in the population of the 3d orbitals. The mixed valence state of Eu observed in the high-pressure (HP) form of EuCo2As2 exhibits amore » remarkable stability, achieving the average oxidation state of +2.25 at 12.6 GPa. In the case of CaCo2As2, substituting even 10% of Eu or La into the Ca site causes ferromagnetic ordering of Co moments. Similar to HP-EuCo2As2, the itinerant 3d ferromagnetism emerges from electronic doping into the Co layer because of chemical compression of Eu sites in Ca0.9Eu0.1Co1.91As2 or direct electron doping in Ca0.85La0.15Co1.89As2. Finally, the results reported herein demonstrate the general possibility of amplifying minor localized electronic effects to achieve major changes in material’s properties via involvement of strongly correlated electrons.« less

  2. [Electron microscopic and cytochemical research on the function of the glial cells in a focus of local cortical destruction].

    PubMed

    Kleshchinov, V N; Koĭdan, E I; Kolomeets, N S

    1986-08-01

    The activity of DNA-RNA-protein synthesizing system of some glial cells was studied using electron cytochemical method for determination of chromatin state and RNA-particles. A dependence of functional state of satellite glial cells (oligodendroglia and astroglia) on the tinctorial neuron state (hyper- and hypochromic scale) was shown. The functional state of interfascicular oligodendroglial cells has been characterized.

  3. sall1 and sall4 repress pou5f3 family expression to allow neural patterning, differentiation, and morphogenesis in Xenopus laevis.

    PubMed

    Exner, Cameron R T; Kim, Albert Y; Mardjuki, Sarah M; Harland, Richard M

    2017-03-18

    The embryonic precursor of the vertebrate central nervous system, the neural plate, is patterned along the anterior-posterior axis and shaped by morphogenetic movements early in development. We previously identified the genes sall1 and sall4, known regulators of pluripotency in other contexts, as transcriptional targets of developmental signaling pathways that regulate neural development. Here, we demonstrate that these two genes are required for induction of posterior neural fates, the cell shape changes that contribute to neural tube closure, and later neurogenesis. Upon sall1 or sall4 knockdown, defects are associated with the failure of the neural plate to differentiate. Consistent with this, sall-deficient neural tissue exhibits an aberrant upregulation of pou5f3 family genes, the Xenopus homologs of the mammalian stem cell maintenance factor Pou5f1 (Oct4). Furthermore, overexpression of pou5f3 genes in Xenopus causes defects in neural patterning, morphogenesis, and differentiation that phenocopy those observed in sall1 and sall4 morphants. In all, this work shows that both sall1 and sall4 act to repress pou5f3 family gene expression in the neural plate, thereby allowing vertebrate neural development to proceed.

  4. Local electronic states of Fe4N films revealed by x-ray absorption spectroscopy and x-ray magnetic circular dichroism

    NASA Astrophysics Data System (ADS)

    Ito, Keita; Toko, Kaoru; Takeda, Yukiharu; Saitoh, Yuji; Oguchi, Tamio; Suemasu, Takashi; Kimura, Akio

    2015-05-01

    We performed x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) measurements at Fe L2,3 and N K-edges for Fe4N epitaxial films grown by molecular beam epitaxy. In order to clarify the element specific local electronic structure of Fe4N, we compared experimentally obtained XAS and XMCD spectra with those simulated by a combination of a first-principles calculation and Fermi's golden rule. We revealed that the shoulders observed at Fe L2,3-edges in the XAS and XMCD spectra were due to the electric dipole transition from the Fe 2p core-level to the hybridization state generated by σ* anti-bonding between the orbitals of N 2p at the body-centered site and Fe 3d on the face-centered (II) sites. Thus, the observed shoulders were attributed to the local electronic structure of Fe atoms at II sites. As to the N K-edge, the line shape of the obtained spectra was explained by the dipole transition from the N 1s core-level to the hybridization state formed by π* and σ* anti-bondings between the Fe 3d and N 2p orbitals. This hybridization plays an important role in featuring the electronic structures and physical properties of Fe4N.

  5. Non-inductive current built-up by local electron cyclotron heating and current drive with a 28 GHz focused beam on QUEST

    NASA Astrophysics Data System (ADS)

    Onchi, Takumi; Idei, Hiroshi; Hasegawa, Makoto; Ohwada, Hiroaki; Zushi, Hideki; Hanada, Kazuaki; Kariya, Tsuyoshi; Mishra, Kishore; Shikama, Taichi; Quest Team

    2016-10-01

    The plasma current can be driven solely by injecting electron cyclotron waves (ECWs) in spherical tokamak (ST) configuration. A system of 28 GHz gyrotron (maximum power: 270 kW) is renewed and reinstalled on QUEST. A focused ECW beam, whose diameter is about 5 cm at the second harmonic resonance, is injected for local ECW heating and current drive. The local power density at resonance exceeds 75 MW/m2 at an injection power of 150 kW. The incident ECW polarization can be adjusted employing the phase shifter consisting of two corrugated plates. During 1.25 second pulse of ECH, plasma current is built up to Ip = 70 kA fully non-inductively with a core electron density of ne > 1018 m-3. The closed flux in such ST plasma is determined at the inboard limiter on the center stack. Energetic electrons are also responsible for the pressure and equilibrium. This work is supported by JSPS KAKENHI (15H04231, 15K17800), NIFS Collaboration Research program (NIFS13KUTR085, NIFS11KUTR069, NIFS16KUTR114).

  6. Photo-induced reactions from efficient molecular dynamics with electronic transitions using the FIREBALL local-orbital density functional theory formalism

    NASA Astrophysics Data System (ADS)

    Zobač, Vladimír; Lewis, James P.; Abad, Enrique; Mendieta-Moreno, Jesús I.; Hapala, Prokop; Jelínek, Pavel; Ortega, José

    2015-05-01

    The computational simulation of photo-induced processes in large molecular systems is a very challenging problem. Firstly, to properly simulate photo-induced reactions the potential energy surfaces corresponding to excited states must be appropriately accessed; secondly, understanding the mechanisms of these processes requires the exploration of complex configurational spaces and the localization of conical intersections; finally, photo-induced reactions are probability events, that require the simulation of hundreds of trajectories to obtain the statistical information for the analysis of the reaction profiles. Here, we present a detailed description of our implementation of a molecular dynamics with electronic transitions algorithm within the local-orbital density functional theory code FIREBALL, suitable for the computational study of these problems. As an example of the application of this approach, we also report results on the [2 + 2] cycloaddition of ethylene with maleic anhydride and on the [2 + 2] photo-induced polymerization reaction of two C60 molecules. We identify different deactivation channels of the initial electron excitation, depending on the time of the electronic transition from LUMO to HOMO, and the character of the HOMO after the transition.

  7. An insight into crystal, electronic, and local structures of lithium iron silicate (Li2FeSiO4) materials upon lithium extraction

    NASA Astrophysics Data System (ADS)

    Kamon-in, O.; Klysubun, W.; Limphirat, W.; Srilomsak, S.; Meethong, N.

    2013-05-01

    Recently, orthosilicate, Li2MSiO4 (where M=transition metal) materials have been attracting considerable attention for potential use as a new generation cathode for Li-ion batteries due to their safety, low toxicity, and low cost characteristics. In addition, the presence of two Li+ ions in the molecule offers a multiple electron-charge transfer (M2+/M3+ and M3+/M4+ redox couples), thus allowing a high achievable capacity of more than 320 mA h/g per M unit. Good electrochemical properties of Li2FeSiO4 have been reported through several approaches such as downsizing of the particles, carbon-coating, etc. However, in addition to electrochemical performance, fundamental understanding regarding crystal, electronic and local structure changes during charge/discharge processes is also important and needs more rigorous investigation. In this work, lithium iron silicates (Li2FeSiO4/C) in space group of Pnma: a=10.6671(3) Å, b=6.2689(2) Å, and c=5.0042(2) Å have been prepared by solid-state reaction. The synthesized as well as chemical delithiated samples have been characterized by XRD, HRTEM, AAS and XAS techniques. We will show the results focusing on Fe K-edge XANES, EXAFS, HRTEM and XRD of the Li2-xFeSiO4 samples and discuss how the crystal, electronic, and local structure changes upon Li+ de-intercalation.

  8. Photo-induced reactions from efficient molecular dynamics with electronic transitions using the FIREBALL local-orbital density functional theory formalism.

    PubMed

    Zobač, Vladimír; Lewis, James P; Abad, Enrique; Mendieta-Moreno, Jesús I; Hapala, Prokop; Jelínek, Pavel; Ortega, José

    2015-05-08

    The computational simulation of photo-induced processes in large molecular systems is a very challenging problem. Firstly, to properly simulate photo-induced reactions the potential energy surfaces corresponding to excited states must be appropriately accessed; secondly, understanding the mechanisms of these processes requires the exploration of complex configurational spaces and the localization of conical intersections; finally, photo-induced reactions are probability events, that require the simulation of hundreds of trajectories to obtain the statistical information for the analysis of the reaction profiles. Here, we present a detailed description of our implementation of a molecular dynamics with electronic transitions algorithm within the local-orbital density functional theory code FIREBALL, suitable for the computational study of these problems. As an example of the application of this approach, we also report results on the [2 + 2] cycloaddition of ethylene with maleic anhydride and on the [2 + 2] photo-induced polymerization reaction of two C60 molecules. We identify different deactivation channels of the initial electron excitation, depending on the time of the electronic transition from LUMO to HOMO, and the character of the HOMO after the transition.

  9. Local electronic states of Fe{sub 4}N films revealed by x-ray absorption spectroscopy and x-ray magnetic circular dichroism

    SciTech Connect

    Ito, Keita; Toko, Kaoru; Suemasu, Takashi; Takeda, Yukiharu; Saitoh, Yuji; Oguchi, Tamio; Kimura, Akio

    2015-05-21

    We performed x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) measurements at Fe L{sub 2,3} and N K-edges for Fe{sub 4}N epitaxial films grown by molecular beam epitaxy. In order to clarify the element specific local electronic structure of Fe{sub 4}N, we compared experimentally obtained XAS and XMCD spectra with those simulated by a combination of a first-principles calculation and Fermi's golden rule. We revealed that the shoulders observed at Fe L{sub 2,3}-edges in the XAS and XMCD spectra were due to the electric dipole transition from the Fe 2p core-level to the hybridization state generated by σ* anti-bonding between the orbitals of N 2p at the body-centered site and Fe 3d on the face-centered (II) sites. Thus, the observed shoulders were attributed to the local electronic structure of Fe atoms at II sites. As to the N K-edge, the line shape of the obtained spectra was explained by the dipole transition from the N 1s core-level to the hybridization state formed by π* and σ* anti-bondings between the Fe 3d and N 2p orbitals. This hybridization plays an important role in featuring the electronic structures and physical properties of Fe{sub 4}N.

  10. Vigorous thermal excitations in a double-tetrahedral chain of localized Ising spins and mobile electrons mimic a temperature-driven first-order phase transition

    NASA Astrophysics Data System (ADS)

    Gálisová, Lucia; Strečka, Jozef

    2015-02-01

    A hybrid spin-electron system defined on a one-dimensional double-tetrahedral chain, in which the localized Ising spin regularly alternates with two mobile electrons delocalized over a triangular plaquette, is exactly solved with the help of generalized decoration-iteration transformation. It is shown that a macroscopic degeneracy of ferromagnetic and ferrimagnetic ground states arising from chiral degrees of freedom of the mobile electrons cannot be lifted by a magnetic field in contrast to a macroscopic degeneracy of the frustrated ground state, which appears due to a kinetically driven frustration of the localized Ising spins. An anomalous behavior of all basic thermodynamic quantities can be observed on account of massive thermal excitations, which mimic a temperature-driven first-order phase transition from the nondegenerate frustrated state to the highly degenerate ferrimagnetic state at nonzero magnetic fields. A substantial difference in the respective degeneracies is responsible for an immense low-temperature peak of the specific heat and very abrupt (almost discontinuous) thermal variations of the entropy and sublattice magnetizations.

  11. Role of defects in BiFeO₃ multiferroic films and their local electronic structure by x-ray absorption spectroscopy

    SciTech Connect

    Ravalia, Ashish; Vagadia, Megha; Solanki, P. S.; Shah, N. A.; Kuberkar, D. G.; Gautam, S.; Chae, K. H.; Asokan, K.

    2014-10-21

    Present study reports the role of defects in the electrical transport in BiFeO₃ (BFO) multiferroic films and its local electronic structure investigated by near-edge X-ray absorption fine structure. Defects created by high energy 200 MeV Ag⁺¹⁵ ion irradiation with a fluence of ∼5 × 10¹¹ ions/cm² results in the increase in structural strain and reduction in the mobility of charge carriers and enhancement in resistive (I-V) and polarization (P-E) switching behaviour. At higher fluence of ∼5 × 10¹² ions/cm², there is a release in the structural strain due to local annealing effect, resulting in an increase in the mobility of charge carriers, which are released from oxygen vacancies and hence suppression in resistive and polarization switching. Near-edge X-ray absorption fine structure studies at Fe L₃,₂- and O K-edges show a significant change in the spectral features suggesting the modifications in the local electronic structure responsible for changes in the intrinsic magnetic moment and electrical transport properties of BFO.

  12. Experimental Bench-marking of Pu Electronic Structure

    SciTech Connect

    Lawrence Livermore National Laboratory

    2007-07-31

    Our plan is to do Ce (as a Pu surrogate) this year and be ready to do Pu next year. The Fano (Spin-resolved Photoelectron Spectroscopy) measurements are essential to testing electron correlation in the occupied 5f states. BIS (Bremstrahlung Isochromat Spectroscopy or high energy Inverse Photoelectron Spectroscopy) experiments are crucial to a quantitative determination of the 5f unoccupied density of states (5f-UDOS). The 5f UDOS is the key to differentiation between a myriad of models of 5f electronic structure. During this time, we will work to converge to a solution for the Pu safety issues, with the plan to implement these in the next FY. Acceleration of this schedule and implementation of the safety plan in this FY will require a very significant increase in funding. Ultimately, results from the Pu experiments will be fed into calculations performed by P. Soderlind, A. Landa, and others.

  13. Use of 2,3,5-F3Y-β2 and 3-NH2Y-α2 to study PCET in E. coli Ribonucleotide Reductase

    PubMed Central

    Seyedsayamdost, Mohammad R.; Yee, Cyril S.; Stubbe, JoAnne

    2011-01-01

    E. coli ribonucleotide reductase is an α2β2 complex that catalyzes the conversion of nucleoside 5′-diphosphates (NDPs) to deoxynucleotides (dNDPs). The active site for NDP reduction resides in α2, and the essential diferric-tyrosyl radical (Y122•) cofactor that initiates radical transfer to the active site cysteine in α2 (C439), 35 Å removed, is in β2. The oxidation is proposed to involve a hopping mechanism through aromatic amino acids (Y122→W48→Y356 in β2 to Y731→Y730→C439 in α2) and reversible proton coupled electron transfer (PCET). Recently 2,3,5-F3Y (F3Y) was site-specifically incorporated in place of Y356 in β2, and 3-NH2Y (NH2Y) in place of Y731 and Y730 in α2. A pH rate profile with F3Y356-β2 suggested that as the pH is elevated, the rate-determining step of RNR can be altered from a conformational change to PCET and that the altered driving force for F3Y oxidation, by residues adjacent to it in the pathway, is responsible for this change. Studies with NH2Y731(730)-α2/β2/CDP/ATP resulted in detection of NH2Y radical (NH2Y•) intermediates capable of dNDP formation. In this study, the reaction of F3Y356-β2/α2/CDP/ATP has been examined by stopped flow (SF) absorption and rapid freeze quench EPR spectroscopy and has failed to reveal any radical intermediates. F3Y356-β2/CDP/ATP has also been examined with NH2Y731-α2 (or NH2Y730-α2) by stopped-flow kinetics from pH 6.5–9.2 and revealed rate constants for NH2Y• formation that support a change in rate limiting step at elevated pH. The results together with kinetic simulations provide a guide for future studies to detect radical intermediates in the pathway. PMID:21182280

  14. Microwave fixation and localization of calcium in synaptic terminals using x-ray microanalysis and electron energy loss spectroscopy imaging.

    PubMed

    Mizuhira, V; Hasegawa, H

    1997-01-01

    The distribution of calcium ions is demonstrated in synaptic terminals by means of a two-step chemical precipitation of calcium ions in the rat brain. K-oxalate/K-antimonate chemical replacement with simultaneous computerized microwave irradiation was used. This precipitate in nerve cell structures was investigated by computerized electron probe x-ray microanalysis (EDX) and electron energy loss spectroscopic (EELS) imaging. The values obtained by EDX agreed with those of the standard sample and theoretical values of Ca-antimonate. Typical EELS spectra of Ca:L, O:K, and Sb:M were obtained from nerve terminals in the same tissue block as that used for EDX analysis. Excellent net Ca:L and Sb:M EELS digital images were obtained after their background images were subtracted. Calcium ions were distributed in the nerve terminals, synaptic vesicles, mitochondria, and synaptic membranes.

  15. Electronic structure and magnetic properties of dilute U impurities in metals

    NASA Astrophysics Data System (ADS)

    Mohanta, S. K.; Cottenier, S.; Mishra, S. N.

    2016-05-01

    The electronic structure and magnetic moment of dilute U impurity in metallic hosts have been calculated from first principles. The calculations have been performed within local density approximation of the density functional theory using Augmented plane wave+local orbital (APW+lo) technique, taking account of spin-orbit coupling and Coulomb correlation through LDA+U approach. We present here our results for the local density of states, magnetic moment and hyperfine field calculated for an isolated U impurity embedded in hosts with sp-, d- and f-type conduction electrons. The results of our systematic study provide a comprehensive insight on the pressure dependence of 5f local magnetism in metallic systems. The unpolarized local density of states (LDOS), analyzed within the frame work of Stoner model suggest the occurrence of local moment for U in sp-elements, noble metals and f-block hosts like La, Ce, Lu and Th. In contrast, U is predicted to be nonmagnetic in most transition metal hosts except in Sc, Ti, Y, Zr, and Hf consistent with the results obtained from spin polarized calculation. The spin and orbital magnetic moments of U computed within the frame of LDA+U formalism show a scaling behavior with lattice compression. We have also computed the spin and orbital hyperfine fields and a detail analysis has been carried out. The host dependent trends for the magnetic moment, hyperfine field and