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Sample records for 5f electronic states

  1. 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.

  2. 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.

  3. 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.

  4. 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.

  5. 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-of-states

  6. 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.

  7. 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.

  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. 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.

  12. 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.

  13. 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

  14. 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.

  15. 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.

  16. 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.

  17. Energy up-conversion and trapping: Dynamics of 5f states of Bk sup 4+ in CeF sub 4

    SciTech Connect

    Liu, G.K.; Beitz, J.V.

    1991-01-01

    Energy transfer mechanisms of excited 5f states of Bk{sup 4+} (0.05 atom %) in CeF{sub 4} containing circa 0.95 atom % Cf{sup 4+} have been investigated at 4 K. The observed anti-Stokes fluorescence arises from both up-conversion and two-photon excitation. Nonexponential decays of Stokes fluorescence are ascribed to both excitation-excitation annihilation and site-dependent trapping processes and, therefore, are not describable by the Inokuti-Hirayama or exciton annihilation models. Based on the Forster-Dexter energy transfer theory, a new model is developed to fit the observed fluorescence decay data. 16 refs., 3 figs.

  18. Photophysical Dynamics and Relaxation Pathways of Ligand-to-Metal Charge-Transfer States in the 5f(1) [Np(VI)O2Cl4](2-) Anion.

    PubMed

    Barker, Beau J; Berg, John M; Kozimor, Stosh A; Wozniak, Nicholas R; Wilkerson, Marianne P

    2017-03-30

    Although several publications report on the electronic structure of the neptunyl ion, experimental measurements to detail the photophysical dynamics of this open-shell actinyl system are limited in number. Time-resolved photoluminescence has been a useful experimental approach for understanding photophysical dynamics and relaxation pathways of a variety of other molecular and ionic systems, including gaseous plutonium hexafluoride and solid-state uranyl compounds. Here, we investigate time-resolved photoluminescence emission of the 5f(1) neptunyl tetrachloride ([Np(VI)O2Cl4](2-)) dianion following visible excitation. Photoemission of the lowest energy neptunyl ligand-to-metal charge-transfer (LMCT) transitions to both the ground and first electronically excited states is observed. Analyses of the decay lifetimes of the excited states suggest different relaxation pathways as a function of excitation energy. Vibronic progressions associated with the Np-oxo symmetric stretching mode are measured in emission spectra, and the energies from these progressions are compared with energies of vibronic progressions associated with the excitation spectra of [Np(VI)O2Cl4](2-). This study expands our understanding of this open-shell actinyl system beyond identification of excited states, allowing characterization of photophysical properties and evidence for the electronic character of the ground state, and suggests that this approach may be applicable to more complex actinide systems.

  19. 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.

  20. Electronic states of WH

    NASA Astrophysics Data System (ADS)

    Ma, Zhongxin; Balasubramanian, K.

    1991-07-01

    Spectroscopic constants and potential energy curves of 15 electronic states of WH are obtained using the complete-active-space multi-configuration self-consistent field (CAS MCSCF) followed by full second-order configuration-interaction (SOCI) calculations. The spin-orbit effects are introduced using the relativistic-configuration-interaction (RCI) method. Our computations confirm the assignment of the observed emission spectrum at 6800 Å but yield different vibrational frequencies for the two observed states.

  1. 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

  2. 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.

  3. 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

  4. 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

  5. Excited state reaction dynamics of Ti(a{sup 5}F{sub J}) + O{sub 2} → TiO(A{sup 3}Φ, B{sup 3}Π, C{sup 3}Δ) + O studied by a crossed-beam velocity map imaging technique

    SciTech Connect

    Honma, Kenji Tanaka, Yuhki

    2015-04-21

    Oxidation reactions of the gas-phase titanium atom in its excited state with oxygen molecule, Ti(a{sup 5}F{sub J}) + O{sub 2} → TiO(A{sup 3}Φ, B{sup 3}Π, C{sup 3}Δ) + O, were studied by a crossed-beam velocity map imaging technique at 14.3 kJ/mol of collision energy. Metastable excited Ti, Ti(a{sup 5}F{sub J}), was generated by an optical pumping method and the reaction products were detected by single photon-ionization followed by a time-of-flight mass analysis and a two dimensional detection. Three wavelengths were selected to ionize electronically excited TiO{sup ∗}, TiO(A{sup 3}Φ, B{sup 3}Π, C{sup 3}Δ). Time sliced images were measured, and angular and speed distributions of TiO{sup ∗} were determined. In all three ionization wavelengths, the angular distributions showed a forward-backward symmetry with low intensity at the sideway direction. The speed distributions were represented by the distributions based on the statistical energy partition into products. These results suggested that the reaction of Ti(a{sup 5}F{sub J}) to form TiO(B) and TiO(C) proceeds via a long-lived intermediate and confirmed that the mechanism proposed by the previous chemiluminescence study.

  6. Single electron states in polyethylene

    SciTech Connect

    Wang, Y.; MacKernan, D.; Cubero, D. E-mail: n.quirke@imperial.ac.uk; Coker, D. F.; Quirke, N. E-mail: n.quirke@imperial.ac.uk

    2014-04-21

    We report computer simulations of an excess electron in various structural motifs of polyethylene at room temperature, including lamellar and interfacial regions between amorphous and lamellae, as well as nanometre-sized voids. Electronic properties such as density of states, mobility edges, and mobilities are computed on the different phases using a block Lanczos algorithm. Our results suggest that the electronic density of states for a heterogeneous material can be approximated by summing the single phase density of states weighted by their corresponding volume fractions. Additionally, a quantitative connection between the localized states of the excess electron and the local atomic structure is presented.

  7. Tamm states in electron plasma

    NASA Astrophysics Data System (ADS)

    2013-11-01

    Researchers have fabricated a voltage-tunable plasmonic crystal in a two-dimensional electron gas that operates at terahertz frequencies. Nature Photonics spoke to Eric Shaner, Greg Dyer and Greg Aizin about the observation of Tamm states at the crystal's edge.

  8. Electronic structure and magnetic state of transuranium metals under pressure.

    PubMed

    Lukoyanov, A V; Shorikov, A O; Bystrushkin, V B; Dyachenko, A A; Kabirova, L R; Tsiovkin, Yu Yu; Povzner, A A; Dremov, V V; Korotin, M A; Anisimov, V I

    2010-12-15

    The electronic structures of bcc Np, fcc Pu, Am, and Cm pure metals under pressure have been investigated employing the LDA + U method with spin-orbit coupling (LDA + U + SO). The magnetic state of the actinide ions was analyzed in both LS and jj coupling schemes to reveal the applicability of corresponding coupling bases. It was demonstrated that whereas Pu and Am are well described within the jj coupling scheme, Np and Cm can be described appropriately neither in a {mσ}, nor in a {jmj} basis, due to intermediate coupling scheme realization in these metals that requires some finer treatment. The LDA + U + SO results for the considered transuranium metals reveal band broadening and gradual 5f electron delocalization under pressure.

  9. 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.

  10. 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

  11. 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.

  12. 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

  13. Correlated Diskoid-like Electronic States

    PubMed Central

    Baskin, Artem; Sadeghpour, Hossein R.; Král, Petr

    2014-01-01

    We study highly excited diskoid-like electronic states formed in the vicinity of charged and strongly polarizable diskotic nanostructures, such as circular graphene flakes. First, we study the nature of such extended states in a simple two-electron model. The two electrons are attached to a point-like nucleus with a charge 2+, where the material electron is forced to move within a 2D disk area centered at the nucleus, while the extended electron is free to move in 3D. Pronounced and complex correlations are revealed in the diskoid-like states. We also develop semiclassical one-electron models of such diskotic systems and explain how the one-electron and many-electron solutions are related. PMID:25081595

  14. Electronic states of GeCl +

    NASA Astrophysics Data System (ADS)

    Dai, Dingguo; Xu, Hua; Balasubramanian, K.

    1995-11-01

    Twenty-eight electronic states of GeCl + are studied using the complete active space self-consistent field (CASSCF) followed by first- and second-order configuration interaction (FOCI, SOCI) methods. Spectroscopic constants of electronic states exhibiting minima are computed.

  15. 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

  16. 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.

  17. Manipulation of electronic states and photonic states in nanosilicon

    NASA Astrophysics Data System (ADS)

    Huang, Wei-Qi; Huang, Zhong-Mei; Miao, Xin-Jian; Qin, Chao-Jian; Lv, Quan

    2014-04-01

    On different size hierarchy, period symmetry provides energy band structure, and symmetry breaking produces localized states in gap, for example nanostructures open electronic band gap by confining electrons, but defects in symmetry system produce localized electronic states in gap. The experimental results demonstrate that controlling localized states in gap by changing passivation environment can manipulate emission wavelength, such as stimulated emission at 700 nm due to oxygen passivation and enhanced electroluminescence near 1600 nm due to ytterbium passivation on nanosilicon. In same way, modulating filling fraction and period parameters in photonic crystal enlarges width of photonic band gap (PBG) by confining photons. Symmetry breaking due to defects is effective in manipulating photonic states. New applications for selecting modes in nanolaser and for building single photon source in quantum information are explored by manipulating and coupling between electronic states and photonic states.

  18. State electronic disease surveillance systems --- United States, 2007 and 2010.

    PubMed

    2011-10-21

    The National Electronic Disease Surveillance System (NEDSS) is a web-based infrastructure for public health surveillance data exchange between CDC and the 50 states. In 2007, the Council of State and Territorial Epidemiologists (CSTE) conducted an assessment to evaluate states' electronic disease surveillance capacity. In 2010, CSTE conducted a follow-up assessment to evaluate the operational status and progress of integration, interoperability, and capacity of state electronic disease surveillance systems. This report summarizes the results of that assessment, which indicated a 17.5% increase from 40 states in 2007 to 47 states in 2010 with fully operational general communicable disease (GCD) electronic surveillance systems, a 211.5% increase from 13 to 39 states in the number of systems that were interoperable, a 22.4% increase from 23 to 34 states in the number with integrated systems, and a 20.0% increase to 42 states with the capacity to receive electronic laboratory reports (ELRs). New Centers for Medicare and Medicaid Services rules for meaningful use of health information technology encourage data exchange between electronic health record systems and public health agencies, including submission of ELRs. To meet national goals for health information exchange to improve population health, variation in disease surveillance systems should decrease, and functionality should increase.

  19. Electronic Information Services, Louisiana State University Libraries.

    ERIC Educational Resources Information Center

    Bolner, Smittie; And Others

    Reports prepared by the Louisiana State University (LSU) Libraries Task Force on Electronic Services examine the present level of automated services at the LSU libraries and make recommendations for both long- and short-term plans to handle information in electronic format. The reports, each of which is followed by a list of recommendations, focus…

  20. 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.

  1. 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.

  2. Unoccupied electronic states of Ru(0001)

    NASA Astrophysics Data System (ADS)

    del Campo, Valeria; Correa, Julián-David; Correa-Puerta, Jonathan; Kroeger, Daniel; Häberle, Patricio

    2016-11-01

    This report presents a combined theoretical and experimental description of the unoccupied electronic states of Ru(0001), along the Γ̅M̅ high symmetry direction of the Brillouin zone. A direct comparison between angle-resolved inverse photoemission spectroscopy and ab initio calculations of the 3-dimensional (3D) electronic structure of Ru(0001) have been used to determine the energy dispersion and the identification of different states and surface resonances. Both, measurements and calculations, complement previous reports regarding the electronic structure of Ru.

  3. Intense steady state electron beam generator

    DOEpatents

    Hershcovitch, Ady; Kovarik, Vincent J.; Prelec, Krsto

    1990-01-01

    An intense, steady state, low emittance electron beam generator is formed by operating a hollow cathode discharge plasma source at critical levels in combination with an extraction electrode and a target electrode that are operable to extract a beam of fast primary electrons from the plasma source through a negatively biased grid that is critically operated to repel bulk electrons toward the plasma source while allowing the fast primary electrons to move toward the target in the desired beam that can be successfully transported for relatively large distances, such as one or more meters away from the plasma source.

  4. Proteins as solid-state electronic conductors.

    PubMed

    Ron, Izhar; Pecht, Israel; Sheves, Mordechai; Cahen, David

    2010-07-20

    Protein structures can facilitate long-range electron transfer in solution. But a fundamental question remains: can these structures also serve as solid-state electronic conductors? Answering this question requires methods for studying conductivity of the "dry" protein (which only contains tightly bound structured water molecules) sandwiched between two electronic conductors in a solid-state type configuration. If successful, such systems could serve as the basis for future, bioinspired electronic device technology. In this Account, we survey, analyze, and compare macroscopic and nanoscopic (scanning probe) solid-state conductivities of proteins, noting the inherent constraints of each of these, and provide the first status report on this research area. This analysis shows convincing evidence that "dry" proteins pass orders of magnitude higher currents than saturated molecules with comparable thickness and that proteins with known electrical activity show electronic conductivity, nearly comparable to that of conjugated molecules ("wires"). These findings suggest that the structural features of proteins must have elements that facilitate electronic conductivity, even if they do not have a known electron transfer function. As a result, proteins could serve not only as sensing, polar,or photoactive elements in devices (such as field-effect transistor configurations) but also as electronic conductors. Current knowledge of peptide synthesis and protein modification paves the way toward a greater understanding of how changes in a protein's structure affect its conductivity. Such an approach could minimize the need for biochemical cascades in systems such as enzyme-based circuits, which transduce the protein's response to electronic current. In addition, as precision and sensitivity of solid-state measurements increase, and as knowledge of the structure and function of "dry" proteins grows, electronic conductivity may become an additional approach to study electron

  5. TCEQ State of Texas Environmental Electronic Reporting System (STEERS)

    EPA Pesticide Factsheets

    TCEQ's State of Texas Environmental Electronic Reporting System (STEERS) is an existing electronic document receiving system for collecting numerous reports required under the state's EPA-authorized programs.

  6. Electronics: State of the Art No. 2.

    ERIC Educational Resources Information Center

    Gosling, W.

    1979-01-01

    Reviewed is a brief history of electronics technology, from the early beginnings of vacuum devices to development of solid state devices, silicon fabrication in the use of transistors, and integrated circuits. Educational needs at the university or polytechnic level are discussed. (CS)

  7. Electronic ground state of Ni2+

    NASA Astrophysics Data System (ADS)

    Zamudio-Bayer, V.; Lindblad, R.; Bülow, C.; Leistner, G.; Terasaki, A.; v. Issendorff, B.; Lau, J. T.

    2016-11-01

    The 9/2 4Φ ground state of the Ni2+ diatomic molecular cation is determined experimentally from temperature and magnetic-field-dependent x-ray magnetic circular dichroism spectroscopy in a cryogenic ion trap, where an electronic and rotational temperature of 7.4 ±0.2 K was reached by buffer gas cooling of the molecular ion. The contribution of the spin dipole operator to the x-ray magnetic circular dichroism spin sum rule amounts to 7 Tz =0.17 ± 0.06 μB per atom, approximately 11% of the spin magnetic moment. We find that, in general, homonuclear diatomic molecular cations of 3d transition metals seem to adopt maximum spin magnetic moments in their electronic ground states.

  8. Electronic States in Capped Carbon Nanotubes

    NASA Astrophysics Data System (ADS)

    Yaguchi, Tatsuya; Ando, Tsuneya

    2001-05-01

    Scattering of an electron wave at various caps closing an armchair nanotube is studied. The reflection coefficients can be understood as an effective shift in boundary position and phase shift at the boundary. The phase shift is approximately given by π for states with parity + and 0 for states with parity -, respectively. The effective position is approximated by (1/4)P, where P is the height of an equilateral triangle having a base line determined by neighboring five-membered rings located at the boundary between the tube and the cap. The electronic structure of a finite-length armchair nanotube closed by a cap can be calculated with the use of the phase shifts.

  9. MHD Equation of State with Relativistic Electrons

    NASA Astrophysics Data System (ADS)

    Gong, Zhigang; Däppen, Werner; Zejda, Ladislav

    2001-01-01

    The Mihalas-Däppen-Hummer (MHD) equation of state does not include the effect of relativistic partially degenerate electrons, although nonrelativistic partial degeneracy is taken into account. The discovery of a relativistic correction in helioseismology forces us to perform an appropriate upgrade of the MHD equation of state. We have adopted the method of J. M. Aparicio to evaluate the relativistic Fermi-Dirac functions. Our calculations confirm the validity of the approximation used, which works well for the weakly relativistic electrons under solar-center conditions. However, our results will also provide reliable thermodynamic quantities in the stronger relativistic regime as found in more massive stars. Since a particular feature of the original MHD papers was an explicit list of the adopted free energy and its first- and second-order analytical derivatives, we give the corresponding relativistic quantities in the Appendix.

  10. 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.

  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. Recoherence by squeezed states in electron interferometry

    SciTech Connect

    Hsiang, J.-T.; Ford, L. H.

    2008-09-15

    Coherent electrons coupled to the quantized electromagnetic field undergo decoherence which can be viewed as due either to fluctuations of the Aharonov-Bohm phase or to photon emission. When the electromagnetic field is in a squeezed vacuum state, it is possible for this decoherence to be reduced, leading to the phenomenon of recoherence. This recoherence effect requires electrons which are emitted at selected times during the cycle of the excited mode of the electromagnetic field. We show that there are bounds on the degree of recoherence which are analogous to quantum inequality restriction on negative energy densities in quantum field theory. We make some estimates of the degree of recoherence, and show that although small, it is in principle observable.

  13. 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.

  14. 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.

  15. 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

  16. 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

  17. 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

  18. Electron correlations in solid state physics

    SciTech Connect

    Freericks, J.K.

    1991-04-01

    Exactly solvable models of electron correlations in solid state physics are presented. These models include the spinless Falicov- Kimball model, the t-t{prime}-J model, and the Hubbard model. The spinless Falicov-Kimball model is analyzed in one-dimension. Perturbation theory and numerical techniques are employed to determine the phase diagram at zero temperature. A fractal structure is found where the ground-state changes (discontinuously) at each rational electron filling. The t-t{prime}-J model (strongly interacting limit of a Hubbard model) is studied on eight-site small clusters in the simple-cubic, body-centered-cubic, face-centered-cubic, and square lattices. Symmetry is used to simplify the problem and determine the exact many-body wavefunctions. Ground states are found that exhibit magnetic order or heavy-fermionic character. Attempts to extrapolate to the thermodynamic limit are also made. The Hubbard model is examined on an eight-site square-lattice cluster in the presence of and in the absence of a magnetic field'' that couples only to orbital motion. A new magnetic phase is discovered for the ordinary Hubbard model at half-filling. In the magnetic field'' case, it is found that the strongly frustrated Heisenberg model may be studied from adiabatic continuation of a tight-binding model (from weak to strong coupling) at one point. The full symmetries of the Hamiltonian are utilized to make the exact diagonalization feasibile. Finally, the presence of hidden'' extra symmetry for finite size clusters with periodic boundary conditions is analyzed for a variety of clusters. Moderately sized systems allow nonrigid transformations that map a lattice onto itself preserving its neighbor structure; similar operations are not present in smaller or larger systems. The additional symmetry requires particular representations of the space group to stick together explaining many puzzling degeneracies found in exact diagonalization studies.

  19. Enhanced negative ion formation via electron attachment to electronically-excited states

    SciTech Connect

    Pinnaduwage, L.A. |

    1995-12-31

    Recent basic studies on electron attachment to laser-excited molecules show that electron attachment to electronically-excited states can have orders of magnitude larger cross sections compared to the respective ground electronic states. Even though systematic studies have not been conducted, there are indications that electronically-excited states may play a significant role in negative ion formation in gas discharges. The high-lying Rydberg states could be of particular significance since, (i) their production efficiencies are high, and (ii) they have comparatively long lifetimes. Such states could be populated in discharge sources via direct electron impact or via excitation transfer from metastable states of inert gases.

  20. On the Electronically Excited States of Uracil

    SciTech Connect

    Epifanovsky, Evgeny; Kowalski, Karol; Fan, Peng-Dong; Valiev, Marat; Matsika, Spiridoula; Krylov, Anna

    2008-10-09

    Vertical excitation energies in uracil in the gas phase and in water solution are investigated by the equation-of-motion coupled-cluster and multi-reference configuration interaction methods. Basis set effects are found to be important for converged results. The analysis of electronic wave functions reveals that the lowest singlet states are predominantly of a singly excited character and are therefore well described by single-reference equation-of-motion methods augmented by a perturbative triples correction to account for dynamical correlation. Our best estimates for the vertical excitation energies for the lowest singlet n and are 5.0±0.1 eV and 5.3±0.1 eV, respectively. The solvent effects for these states are estimated to be +0.5 eV and ±0.1 eV, respectively. We attribute the difference between the computed vertical excitations and the maximum of the experimental absorption to strong vibronic interaction between the lowest A00 and A0 states leading to intensity borrowing by the forbidden transition.

  1. Electronically shielded solid state charged particle detector

    DOEpatents

    Balmer, David K.; Haverty, Thomas W.; Nordin, Carl W.; Tyree, William H.

    1996-08-20

    An electronically shielded solid state charged particle detector system having enhanced radio frequency interference immunity includes a detector housing with a detector entrance opening for receiving the charged particles. A charged particle detector having an active surface is disposed within the housing. The active surface faces toward the detector entrance opening for providing electrical signals representative of the received charged particles when the received charged particles are applied to the active surface. A conductive layer is disposed upon the active surface. In a preferred embodiment, a nonconductive layer is disposed between the conductive layer and the active surface. The conductive layer is electrically coupled to the detector housing to provide a substantially continuous conductive electrical shield surrounding the active surface. The inner surface of the detector housing is supplemented with a radio frequency absorbing material such as ferrite.

  2. Electronically shielded solid state charged particle detector

    DOEpatents

    Balmer, D.K.; Haverty, T.W.; Nordin, C.W.; Tyree, W.H.

    1996-08-20

    An electronically shielded solid state charged particle detector system having enhanced radio frequency interference immunity includes a detector housing with a detector entrance opening for receiving the charged particles. A charged particle detector having an active surface is disposed within the housing. The active surface faces toward the detector entrance opening for providing electrical signals representative of the received charged particles when the received charged particles are applied to the active surface. A conductive layer is disposed upon the active surface. In a preferred embodiment, a nonconductive layer is disposed between the conductive layer and the active surface. The conductive layer is electrically coupled to the detector housing to provide a substantially continuous conductive electrical shield surrounding the active surface. The inner surface of the detector housing is supplemented with a radio frequency absorbing material such as ferrite. 1 fig.

  3. Electronically shielded solid state charged particle detector

    SciTech Connect

    Balmer, D.K.; Haverty, T.W.; Nordin, C.W.; Tyree, W.H.

    1995-12-31

    An electronically shielded solid state charged particle detector system having enhanced radio frequency interference immunity includes a detector housing with a detector entrance opening for receiving the charged particles. A charged particle detector having an active surface is disposed within the housing. The active surface faces toward the detector entrance opening for providing electrical signals representative of the received charged particles when the received charged particles are applied to the active surface. A conductive layer is disposed upon the active surface. In a preferred embodiment, a nonconductive layer is disposed between the conductive layer and the active surface. The conductive layer is electrically coupled to the detector housing to provide a substantially continuous conductive electrical shield surrounding the active surface. The inner surface of the detector housing is supplemented with a radio frequency absorbing material such as ferrite.

  4. Electronic states of coupled graphene nanoribbons

    NASA Astrophysics Data System (ADS)

    Hashimoto, Futo; Mori, Nobuya; Kubo, Osamu; Katayama, Mitsuhiro

    2017-04-01

    Electronic states of laterally coupled graphene nanoribbons (GNRs) have been calculated within a nearest-neighbor tight-binding approximation with varying inter-GNR coupling strength γ from γ = 0 to t (intra-GNR transfer integral). For a coupled zigzag-edge GNR array, both almost flat bands and anisotropic Dirac cones appear near the Fermi level. For a coupled armchair-edge GNR array with a ribbon width N = 3n or 3n + 1, the system is semiconducting with a finite bandgap at γ = 0, which decreases as γ increases. For N = 3n, it becomes metallic with a zero bandgap only at γ = t. On the other hand, for N = 3n + 1, it becomes metallic when γ ≥ t/2. At γ = t/2, a peculiar energy dispersion emerges; the energy dispersion is parabolic perpendicular to the GNR axis and linear parallel to the GNR axis. When N = 3n + 2, the system is always metallic regardless of γ.

  5. Electronic excited states of CO/sub 2/: An electron impact investigation

    SciTech Connect

    McDiarmid, R.; Doering, J.P.

    1984-01-15

    The electronic excited states of CO/sub 2/ were restudied by variable incident energy, variable angle electron impact spectroscopy. In this study, valence states of mixed configurations were distinguished from pure Rydberg states. Our results are incompatible with the theoretical description of CO/sub 2/, in which only two valence singlet states are located.

  6. Importance of electronic state of two-dimensional electron gas for electron injection process in nano-electronic devices

    NASA Astrophysics Data System (ADS)

    Muraguchi, M.; Endoh, T.; Takada, Y.; Sakurai, Y.; Nomura, S.; Shiraishi, K.; Ikeda, M.; Makihara, K.; Miyazaki, S.; Shigeta, Y.

    2010-09-01

    We report the unexpected temperature dependence of electron tunneling from the two-dimensional electron gas (2DEG) to the Si-dot in a Si-dots floating gate metal-oxide-semiconductor (MOS) capacitor. We indicate that this temperature dependence of the electron tunneling cannot be explained by the conventional one-dimensional tunneling model, and show that it is necessary for a new model which includes the geometrical factor of the system. To extract a mechanism of the electron injection process from the 2DEG to the nano-structure, we have employed the numerical simulation, which includes both the geometrical condition of the system and the experimental setup. We suggest in our new tunneling model that the main contribution to the electron tunneling is induced by the wave-packet-like state of the electron below the Si-dots. We successfully show that the temperature dependence of the electron injection voltage in the Si-dots floating gate MOS capacitor fits our model. This indicates that the spatial distribution of electron density in the two-dimensional electron gas would play a crucial role in the electron tunneling.

  7. Minimal parametrization of an n -electron state

    NASA Astrophysics Data System (ADS)

    Kutzelnigg, Werner; Mukherjee, Debashis

    2005-02-01

    The Hamiltonian H for an n -electron system in a finite one-electron basis of dimension m is characterized by d=O(m4) matrix elements. The eigenstates of this Hamiltonian—i.e., the full-CI states Ψ —depend, however, on the usually much larger set of N=O(mn) parameters. One can, nevertheless, write a full-CI state as Ψ=eSΦ with Φ a reference function and S an operator familiar from traditional coupled cluster (TCC) theory. The “exact” operator S can be expressed (though in an implicit and rather complicated way) in terms of d parameters. An alternative ansatz Ψ=eTΦ with T depending in a very simple way on d parameters only (namely, with T having the same structure in Fock space as H ) has been studied by Nooijen and by Nakatsuji and been called coupled-cluster with generalized single and double excitations (CCGSD). Nooijen has conjectured that the full-CI equations can be fulfilled with this ansatz. This paper is devoted to a comprehensive analysis of the Nooijen conjecture (NC). Several features make this analysis difficult and even intriguing. (a) One deals with coupled nonlinear systems of equations, for which theorems concerning the existence of their solution are hardly available. (b) There are different possible interpretations of the NC, especially as far as the choice of the reference function Φ is concerned. (c) There are solutions of the CCGSD equations, for which some elements of T becomes negative infinite, and eT becomes a projection operator. Such solutions are undesired but difficult to eliminate. We show by direct comparison of the exact wave operator with that of CCGSD theory, for a closed-shell state with Φ a single Slater determinant, using a perturbation expansion, that CCGSD cannot be exact. This required a reformulation of the CCGSD operator eT to an equivalent exponential form eR , with R similar to the S of TCC theory, but with constraints on the cluster amplitudes, such that these depend on d parameters only. The CCGSD ansatz

  8. An incompressible state of a photo-excited electron gas

    PubMed Central

    Chepelianskii, Alexei D.; Watanabe, Masamitsu; Nasyedkin, Kostyantyn; Kono, Kimitoshi; Konstantinov, Denis

    2015-01-01

    Two-dimensional electrons in a magnetic field can form new states of matter characterized by topological properties and strong electronic correlations as displayed in the integer and fractional quantum Hall states. In these states, the electron liquid displays several spectacular characteristics, which manifest themselves in transport experiments with the quantization of the Hall resistance and a vanishing longitudinal conductivity or in thermodynamic equilibrium when the electron fluid becomes incompressible. Several experiments have reported that dissipationless transport can be achieved even at weak, non-quantizing magnetic fields when the electrons absorb photons at specific energies related to their cyclotron frequency. Here we perform compressibility measurements on electrons on liquid helium demonstrating the formation of an incompressible electronic state under these resonant excitation conditions. This new state provides a striking example of irradiation-induced self-organization in a quantum system. PMID:26007282

  9. 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.

  10. 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.

  11. 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

  12. Electron states in semiconductor quantum dots

    SciTech Connect

    Dhayal, Suman S.; Ramaniah, Lavanya M.; Ruda, Harry E.; Nair, Selvakumar V.

    2014-11-28

    In this work, the electronic structures of quantum dots (QDs) of nine direct band gap semiconductor materials belonging to the group II-VI and III-V families are investigated, within the empirical tight-binding framework, in the effective bond orbital model. This methodology is shown to accurately describe these systems, yielding, at the same time, qualitative insights into their electronic properties. Various features of the bulk band structure such as band-gaps, band curvature, and band widths around symmetry points affect the quantum confinement of electrons and holes. These effects are identified and quantified. A comparison with experimental data yields good agreement with the calculations. These theoretical results would help quantify the optical response of QDs of these materials and provide useful input for applications.

  13. 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

  14. Electron and electron-hole quasiparticle states in a driven quantum contact

    NASA Astrophysics Data System (ADS)

    Vanević, Mihajlo; Gabelli, Julien; Belzig, Wolfgang; Reulet, Bertrand

    2016-01-01

    We study the many-body electronic state created by a time-dependent drive of a mesoscopic contact. The many-body state is expressed manifestly in terms of single-electron and electron-hole quasiparticle excitations with the amplitudes and probabilities of creation which depend on the details of the applied voltage. We experimentally probe the time dependence of the constituent electronic states by using an analog of the optical Hong-Ou-Mandel correlation experiment where electrons emitted from the terminals with a relative time delay collide at the contact. The electron wave packet overlap is directly related to the current noise power in the contact. We have confirmed the time dependence of the electronic states predicted theoretically by measurements of the current noise power in a tunnel junction under harmonic excitation.

  15. 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.

  16. Microscopic theory of the insulating electronic ground states of the actinide dioxides AnO2 (An = U, Np, Pu, Am, and Cm)

    NASA Astrophysics Data System (ADS)

    Suzuki, M.-T.; Magnani, N.; Oppeneer, P. M.

    2013-11-01

    The electronic states of the actinide dioxides AnO2 (with An = U, Np, Pu, Am, and Cm) are investigated employing first-principles calculations within the framework of the local density approximation +U (LDA+U) approach, implemented in a full-potential linearized augmented plane-wave scheme. A systematic analysis of the An-5f states is performed which provides intuitive connections between the electronic structures and the local crystalline fields of the f states in the AnO2 series. Particularly the mechanisms leading to the experimentally observed insulating ground states are investigated. These are found to be caused by the strong spin-orbit and Coulomb interactions of the 5f orbitals; however, as a result of the different configurations, this mechanism works in distinctly different ways for each of the AnO2 compounds. In agreement with experimental observations, the nonmagnetic states of plutonium and curium dioxide are computed to be insulating, whereas those of uranium, neptunium, and americium dioxides require additional symmetry breaking to reproduce the insulator ground states, a condition which is met with magnetic phase transitions. We show that the occupancy of the An-f orbitals is closely connected to each of the appearing insulating mechanisms. We furthermore investigate the detailed constitution of the noncollinear multipolar moments for transverse 3q magnetic ordered states in UO2 and longitudinal 3q high-rank multipolar ordered states in NpO2 and AmO2.

  17. 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.

  18. On the electron wavepacket dynamics of photoionizing states

    NASA Astrophysics Data System (ADS)

    Takatsuka, Kazuo

    2014-06-01

    To study electron wavepacket dynamics of photoionizing states in polyatomic molecules, we discuss two crucial issues to be overcome in the theory of molecular electronic wavepacket dynamics in an intense laser field (Takatsuka and Yonehara 2011 Phys. Chem. Chem. Phys. 13 4987). One is about the description of the ionization process from electronically excited states composed of many multiply excited configuration-state functions. The other is how to reconstruct the electronic states remaining in the molecular site while electrons are flowing out of the molecular bounds. These are both critical to extend the realm of the theories of electron dynamics based on the so-called expansion (algebraic) method in terms of basis functions. To calculate the photoionization amplitude and thereby to estimate the time-dependent amount of electron loss from a molecule, we extract the electron flux (probability current density) from the electron wavepackets without use of scattering theory. This is justified by the success of the recent works by Bandrauk’s group for attosecond photoionization dynamics from the hydrogen molecule ion, who performed numerical integration of the relevant Schrödinger equation (Yuan et al 2013 J. Chem. Phys. 138 134316). A key feature in the present study, on the other hand, is to calculate the electron flux in terms of complex-valued NOs, which arise from the complex electronic wavepackets. Through the change of these NOs, we reconstruct the involved electronic configurations during the flow of electrons out of molecular regions. These repopulated electronic wavefunctions are (non-adiabatically) evolved in time under laser fields.

  19. 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

  20. Two state electron model for geminate recombination of electron-ion pairs in liquid isooctane

    NASA Astrophysics Data System (ADS)

    Lukin, L. V.; Yakovlev, B. S.

    2011-04-01

    Recombination kinetics of geminate electron-ion pairs is considered in the framework of the two state model for electron transport in liquid hydrocarbons. It is shown that the model well reproduces recent experimental data on the subpicosecond geminate recombination obtained in liquid isooctane. The life time of electrons in a localized state in isooctane is estimated to lie in the range between 0.14 ps and 0.57 ps at room temperature.

  1. Timekeeping with electron spin states in diamond

    NASA Astrophysics Data System (ADS)

    Hodges, J. S.; Yao, N. Y.; Maclaurin, D.; Rastogi, C.; Lukin, M. D.; Englund, D.

    2013-03-01

    Frequency standards based on atomic states, such as Rb or Cs vapors, or single-trapped ions, are the most precise measures of time. Here we propose and analyze a precision oscillator approach based upon spins in a solid-state system, in particular, the nitrogen-vacancy defect in single-crystal diamond. We show that this system can have stability approaching portable atomic standards and is readily incorporable as a chip-scale device. Using a pulsed spin-echo technique, we anticipate an Allan deviation of σy=10-7τ-1/2 limited by thermally-induced strain variations; in the absence of such thermal fluctuations, the system is limited by spin dephasing and harbors an Allan deviation nearing ˜10-12τ-1/2. Potential improvements based upon advanced diamond material processing, temperature stabilization, and nanophotonic engineering are discussed.

  2. Imaging the dynamics of free-electron Landau states.

    PubMed

    Schattschneider, P; Schachinger, Th; Stöger-Pollach, M; Löffler, S; Steiger-Thirsfeld, A; Bliokh, K Y; Nori, Franco

    2014-08-08

    Landau levels and states of electrons in a magnetic field are fundamental quantum entities underlying the quantum Hall and related effects in condensed matter physics. However, the real-space properties and observation of Landau wave functions remain elusive. Here we report the real-space observation of Landau states and the internal rotational dynamics of free electrons. States with different quantum numbers are produced using nanometre-sized electron vortex beams, with a radius chosen to match the waist of the Landau states, in a quasi-uniform magnetic field. Scanning the beams along the propagation direction, we reconstruct the rotational dynamics of the Landau wave functions with angular frequency ~100 GHz. We observe that Landau modes with different azimuthal quantum numbers belong to three classes, which are characterized by rotations with zero, Larmor and cyclotron frequencies, respectively. This is in sharp contrast to the uniform cyclotron rotation of classical electrons, and in perfect agreement with recent theoretical predictions.

  3. Electronic states of the diatomic antimony fluoride (SbF)

    NASA Astrophysics Data System (ADS)

    Latifzadeh, Lida; Balasubramanian, K.

    1996-07-01

    The potential energy curves of 21 electronic states of SbF and spectroscopic properties of bound states among these have been computed using the complete active space self-consistent field (CASSCF) followed by first- and second-order configuration interaction (FOCI, SOCI) and multireference singles and doubles configuration interaction (MRSDCI) methods. The computed results are in good agreement with the observed values for six states, while the properties of four other states have been computed which are yet to be observed.

  4. 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,...

  5. REFLECTIONS ON THE TWO-STATE ELECTRON TRANSFER MODEL.

    SciTech Connect

    Brunschwig, B.S.

    2000-01-12

    There is general agreement that the two most important factors determining electron transfer rates in solution are the degree of electronic interaction between the donor and acceptor sites, and the changes in the nuclear configurations of the donor, acceptor, and surrounding medium that occur upon the gain or loss of an electron Ll-51. The electronic interaction of the sites will be very weak, and the electron transfer slow, when the sites are far apart or their interaction is symmetry or spin forbidden. Since electron motion is much faster than nuclear motion, energy conservation requires that, prior to the actual electron transfer, the nuclear configurations of the reactants and the surrounding medium adjust from their equilibrium values to a configuration (generally) intermediate between that of the reactants and products. In the case of electron transfer between , two metal complexes in a polar solvent, the nuclear configuration changes involve adjustments in the metal-ligand and intraligand bond lengths and angles, and changes in the orientations of the surrounding solvent molecules. In common with ordinary chemical reactions, an electron transfer reaction can then be described in terms of the motion of the system on an energy surface from the reactant equilibrium configuration (initial state) to the product equilibrium configuration (final state) via the activated complex (transition state) configuration.

  6. Electron states and electron Raman scattering in semiconductor step-quantum well: Electric field effect

    NASA Astrophysics Data System (ADS)

    Betancourt-Riera, Ri.; Betancourt-Riera, Re.; Ferrer-Moreno, L. A.; Jalil, J. M. Nieto

    2017-04-01

    In this work we determine and show the expressions of the electron states of a step-quantum well with the presence of an external electric field, developed in a GaAs / AlGaAs matrix. The electron states are obtained using the envelope function approximation. In this work it is only necessary to consider a single conduction band, which due to the confinement is divided into a subband system, with T = 0K . Expressions for the electron states and the differential cross-section for an intraband electron Raman scattering process of are presented, the net Raman gain is also calculated. In addition, the interpretation of the singularities found in the emission or excitation spectra is given, since several dispersion configurations are discussed. Furthermore, the effects of an electric field on the electron states and on the differential cross section are studied.

  7. Probing the electronic structures of low oxidation-state uranium fluoride molecules UFx- (x=2-4)

    SciTech Connect

    Li, Wei-Li; Hu, Hanshi; Jian, Tian; Lopez, Gary V.; Su, Jing; Li, Jun; Wang, Lai-Sheng

    2013-12-28

    We report the experimental observation of gaseous UFx- (x = 2-4) anions, which are investigated using photoelectron spectroscopy and relativistic quantum chemistry. Vibrationally resolved photoelectron spectra are obtained for all three species and the electron affinities of UFx (x = 2-4) are measured to be 1.16(3), 1.09(3), and 1.58(3) eV, respectively. Significant multi-electron transitions are observed in the photoelectron spectra of U(5f(3)7s(2)) F-2(-), as a result of strong electron correlation effects of the two 7s electrons. The U-F symmetric stretching vibrational modes are resolved for the ground states of all UFx (x = 2-4) neutrals. Theoretical calculations are performed to qualitatively understand the photoelectron spectra. The entire UFx- and UFx (x = 1-6) series are considered theoretically to examine the trends of U-F bonding and the electron affinities as a function of fluorine coordination. The increased U-F bond lengths and decreased bond orders from UF2- to UF4- indicate that the U-F bonding becomes weaker as the oxidation state of U increases from I to III. (C) 2013 AIP Publishing LLC.

  8. Surface-electronic-state effects in electron emission from the Be(0001) surface

    SciTech Connect

    Archubi, C. D.; Gravielle, M. S.; Silkin, V. M.

    2011-07-15

    We study the electron emission produced by swift protons impinging grazingly on a Be(0001) surface. The process is described within a collisional formalism using the band-structure-based (BSB) approximation to represent the electron-surface interaction. The BSB model provides an accurate description of the electronic band structure of the solid and the surface-induced potential. Within this approach we derive both bulk and surface electronic states, with these latter characterized by a strong localization at the crystal surface. We found that such surface electronic states play an important role in double-differential energy- and angle-resolved electron emission probabilities, producing noticeable structures in the electron emission spectra.

  9. Electron-Electron Interaction in Ion-Atom Collisions Studied by Projectile State-Resolved Auger Electron Spectroscopy.

    NASA Astrophysics Data System (ADS)

    Lee, Do-Hyung

    1990-01-01

    This dissertation addresses the problem of dynamic electron-electron interactions in fast ion-atom collisions using projectile Auger electron spectroscopy. The study was carried out by measuring high-resolution projectile KLL Auger electron spectra as a function of projectile energy for the various collision systems of 0.25-2 MeV/u O^{q+} and F^ {q+} incident on H_2 and He targets. The electrons were detected in the beam direction, where the kinematic broadening is minimized. A zero-degree tandem electron spectrometer system was developed and showed the versatility of zero-degree measurements of collisionally-produced atomic states. The zero-degree binary encounter electrons (BEe), quasifree target electrons ionized by the projectiles in head-on collisions, were observed as a strong background in the KLL Auger electron spectrum. They were studied by treating the target ionization as 180^circ Rutherford elastic scattering in the projectile frame, and resulted in a validity test of the impulse approximation (IA) and a way to determine the spectrometer efficiency. An anomalous q-dependence, in which the zero-degree BEe yields increase with decreasing projectile charge state (q), was observed. State-resolved KLL Auger cross sections were determined by using the BEe normalization and thus the cross sections of the electron -electron interactions such as resonant transfer-excitation (RTE), electron-electron excitation (eeE), and electron -electron ionization (eeI) were determined. Projectile 2l capture with 1s to 2p excitation by the captured target electron was observed as an RTE process with Li-like and He-like projectiles and the measured RTEA (RTE followed by Auger decay) cross sections showed good agreement with an RTE-IA treatment and RTE alignment theory. Projectile 1s to 2p excitation by a target electron was observed an an eeE process with Li-like projectiles. Projectile 1s ionization by a target electron was observed as an eeI process with Be-like projectiles

  10. Alternative ground states enable pathway switching in biological electron transfer.

    PubMed

    Abriata, Luciano A; Álvarez-Paggi, Damián; Ledesma, Gabriela N; Blackburn, Ninian J; Vila, Alejandro J; Murgida, Daniel H

    2012-10-23

    Electron transfer is the simplest chemical reaction and constitutes the basis of a large variety of biological processes, such as photosynthesis and cellular respiration. Nature has evolved specific proteins and cofactors for these functions. The mechanisms optimizing biological electron transfer have been matter of intense debate, such as the role of the protein milieu between donor and acceptor sites. Here we propose a mechanism regulating long-range electron transfer in proteins. Specifically, we report a spectroscopic, electrochemical, and theoretical study on WT and single-mutant Cu(A) redox centers from Thermus thermophilus, which shows that thermal fluctuations may populate two alternative ground-state electronic wave functions optimized for electron entry and exit, respectively, through two different and nearly perpendicular pathways. These findings suggest a unique role for alternative or "invisible" electronic ground states in directional electron transfer. Moreover, it is shown that this energy gap and, therefore, the equilibrium between ground states can be fine-tuned by minor perturbations, suggesting alternative ways through which protein-protein interactions and membrane potential may optimize and regulate electron-proton energy transduction.

  11. Search for bound-state electron+positron pair decay

    NASA Astrophysics Data System (ADS)

    Bosch, F.; Hagmann, S.; Hillenbrand, P.-M.; Lane, G. J.; Litvinov, Yu. A.; Reed, M. W.; Sanjari, M. S.; Stöhlker, Th.; Torilov, S. Yu.; Tu, X. L.; Walke, P. M.

    2016-09-01

    The heavy ion storage rings coupled to in-flight radioactive-ion beam facilities, namely the ability to produce and store for extended periods of time radioactive nuclides in high atomic charge states, for the searchof yet unobserved decay mode - bound-state electron-positron pair decay.

  12. Electronic Religion and the Separation of Church and State.

    ERIC Educational Resources Information Center

    Jackson, Gordon

    An examination of the rise of "electronic religion" (religious broadcasting on radio and television) in the United States and the movement's fusing of religious and political issues during the 1980 election year lends credibility to the argument that a clash between church and state is inherent in the political aspects of these…

  13. Electronic states in hybrid boron nitride and graphene structures

    NASA Astrophysics Data System (ADS)

    Zhao, M.; Huang, Y. H.; Ma, F.; Hu, T. W.; Xu, K. W.; Chu, Paul K.

    2013-08-01

    The energy bands and electronic states of hybrid boron nitride (BN) and graphene structures are studied by first principle calculations. The electronic states change from semi-metallic to insulating depending on the number of B and N atoms as well as domain symmetry. When there are unequal numbers of B and N atoms, mid-gap states usually appear around the Fermi level and the corresponding hybrid structure possesses magnetic and semi-metallic properties. However, when the numbers of B and N atoms are equal, a band gap exists indicative of a semiconducting or insulating nature which depends on the structural symmetry.

  14. Reverse quantum state engineering using electronic feedback loops

    NASA Astrophysics Data System (ADS)

    Kießlich, Gerold; Emary, Clive; Schaller, Gernot; Brandes, Tobias

    2012-12-01

    We propose an all-electronic technique to manipulate and control interacting quantum systems by unitary single-jump feedback conditioned on the outcome of a capacitively coupled electrometer and, in particular, a single-electron transistor. We provide a general scheme for stabilizing pure states in the quantum system and use an effective Hamiltonian method for the quantum master equation to elaborate on the nature of stabilizable states and the conditions under which state purification can be achieved. The state engineering within the quantum feedback scheme is shown to be linked with the solution of an inverse eigenvalue problem. Two applications of the feedback scheme are presented in detail: (i) stabilization of delocalized pure states in a single charge qubit and (ii) entanglement stabilization in two coupled charge qubits. In the latter example, we demonstrate the stabilization of a maximally entangled Bell state for certain detector positions and local feedback operations.

  15. Tunable topological states in electron-doped HTT-Pt

    NASA Astrophysics Data System (ADS)

    Zhang, Xiaoming; Wang, Zhenhai; Zhao, Mingwen; Liu, Feng

    2016-04-01

    Modulating topologically nontrivial states in trivial materials is of both scientific and technological interest. Using first-principles calculations, we propose a demonstration of electron-doping- (or gate-voltage-) induced multiple quantum states; namely, quantum spin Hall (QSH) and quantum anomalous Hall (QAH) states, in a single material of the organometallic framework (HTT-Pt) synthesized from triphenylene hexathiol molecules (HTT) and PtC l2 . At a low doping level, the trivial HTT-Pt converts to a QSH insulator protected by time-reversal symmetry (TRS). When the electronic doping concentration is further increased, TRS will be broken, making the HTT-Pt a QAH insulator. The band gaps of these topologically nontrivial states can be as large as 42.5 meV, suggesting robustness at high temperatures. The possibility of switching between the QSH and QAH states offers an intriguing platform for a different device paradigm by interfacing between QSH and QAH states.

  16. Fast electronic resistance switching involving hidden charge density wave states

    NASA Astrophysics Data System (ADS)

    Vaskivskyi, I.; Mihailovic, I. A.; Brazovskii, S.; Gospodaric, J.; Mertelj, T.; Svetin, D.; Sutar, P.; Mihailovic, D.

    2016-05-01

    The functionality of computer memory elements is currently based on multi-stability, driven either by locally manipulating the density of electrons in transistors or by switching magnetic or ferroelectric order. Another possibility is switching between metallic and insulating phases by the motion of ions, but their speed is limited by slow nucleation and inhomogeneous percolative growth. Here we demonstrate fast resistance switching in a charge density wave system caused by pulsed current injection. As a charge pulse travels through the material, it converts a commensurately ordered polaronic Mott insulating state in 1T-TaS2 to a metastable electronic state with textured domain walls, accompanied with a conversion of polarons to band states, and concurrent rapid switching from an insulator to a metal. The large resistance change, high switching speed (30 ps) and ultralow energy per bit opens the way to new concepts in non-volatile memory devices manipulating all-electronic states.

  17. Fast electronic resistance switching involving hidden charge density wave states

    PubMed Central

    Vaskivskyi, I.; Mihailovic, I. A.; Brazovskii, S.; Gospodaric, J.; Mertelj, T.; Svetin, D.; Sutar, P.; Mihailovic, D.

    2016-01-01

    The functionality of computer memory elements is currently based on multi-stability, driven either by locally manipulating the density of electrons in transistors or by switching magnetic or ferroelectric order. Another possibility is switching between metallic and insulating phases by the motion of ions, but their speed is limited by slow nucleation and inhomogeneous percolative growth. Here we demonstrate fast resistance switching in a charge density wave system caused by pulsed current injection. As a charge pulse travels through the material, it converts a commensurately ordered polaronic Mott insulating state in 1T–TaS2 to a metastable electronic state with textured domain walls, accompanied with a conversion of polarons to band states, and concurrent rapid switching from an insulator to a metal. The large resistance change, high switching speed (30 ps) and ultralow energy per bit opens the way to new concepts in non-volatile memory devices manipulating all-electronic states. PMID:27181483

  18. 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.

  19. State-to-state kinetics and transport properties of electronically excited N and O atoms

    NASA Astrophysics Data System (ADS)

    Istomin, V. A.; Kustova, E. V.

    2016-11-01

    A theoretical model of transport properties in electronically excited atomic gases in the state-to-state approach is developed. Different models for the collision diameters of atoms in excited states are discussed, and it is shown that the Slater-like models can be applied for the state-resolved transport coefficient calculations. The influence of collision diameters of N and O atoms with electronic degrees of freedom on the transport properties is evaluated. Different distributions on the electronic energy are considered for the calculation of transport coefficients. For the Boltzmann-like distributions at temperatures greater than 15000 K, an important effect of electronic excitation on the thermal conductivity and viscosity coefficients is found; the coefficients decrease significantly when many electronic states are taken into account. It is shown that under hypersonic reentry conditions the impact of collision diameters on the transport properties is not really important since the populations of high levels behind the shock waves are low.

  20. STEADY-STATE MODEL OF SOLAR WIND ELECTRONS REVISITED

    SciTech Connect

    Yoon, Peter H.; Kim, Sunjung; Choe, G. S.

    2015-10-20

    In a recent paper, Kim et al. put forth a steady-state model for the solar wind electrons. The model assumed local equilibrium between the halo electrons, characterized by an intermediate energy range, and the whistler-range fluctuations. The basic wave–particle interaction is assumed to be the cyclotron resonance. Similarly, it was assumed that a dynamical steady state is established between the highly energetic superhalo electrons and high-frequency Langmuir fluctuations. Comparisons with the measured solar wind electron velocity distribution function (VDF) during quiet times were also made, and reasonable agreements were obtained. In such a model, however, only the steady-state solution for the Fokker–Planck type of electron particle kinetic equation was considered. The present paper complements the previous analysis by considering both the steady-state particle and wave kinetic equations. It is shown that the model halo and superhalo electron VDFs, as well as the assumed wave intensity spectra for the whistler and Langmuir fluctuations, approximately satisfy the quasi-linear wave kinetic equations in an approximate sense, thus further validating the local equilibrium model constructed in the paper by Kim et al.

  1. Alternative ground states enable pathway switching in biological electron transfer

    PubMed Central

    Abriata, Luciano A.; Álvarez-Paggi, Damián; Ledesma, Gabriela N.; Blackburn, Ninian J.; Vila, Alejandro J.; Murgida, Daniel H.

    2012-01-01

    Electron transfer is the simplest chemical reaction and constitutes the basis of a large variety of biological processes, such as photosynthesis and cellular respiration. Nature has evolved specific proteins and cofactors for these functions. The mechanisms optimizing biological electron transfer have been matter of intense debate, such as the role of the protein milieu between donor and acceptor sites. Here we propose a mechanism regulating long-range electron transfer in proteins. Specifically, we report a spectroscopic, electrochemical, and theoretical study on WT and single-mutant CuA redox centers from Thermus thermophilus, which shows that thermal fluctuations may populate two alternative ground-state electronic wave functions optimized for electron entry and exit, respectively, through two different and nearly perpendicular pathways. These findings suggest a unique role for alternative or “invisible” electronic ground states in directional electron transfer. Moreover, it is shown that this energy gap and, therefore, the equilibrium between ground states can be fine-tuned by minor perturbations, suggesting alternative ways through which protein–protein interactions and membrane potential may optimize and regulate electron–proton energy transduction. PMID:23054836

  2. Alternative ground states enable pathway switching in biological electron transfer

    SciTech Connect

    Abriata, Luciano A.; Alvarez-Paggi, Damian; Ledesma, Gabirela N.; Blackburn, Ninian J.; Vila, Alejandro J.; Murgida, Daniel H.

    2012-10-10

    Electron transfer is the simplest chemical reaction and constitutes the basis of a large variety of biological processes, such as photosynthesis and cellular respiration. Nature has evolved specific proteins and cofactors for these functions. The mechanisms optimizing biological electron transfer have been matter of intense debate, such as the role of the protein milieu between donor and acceptor sites. Here we propose a mechanism regulating long-range electron transfer in proteins. Specifically, we report a spectroscopic, electrochemical, and theoretical study on WT and single-mutant CuA redox centers from Thermus thermophilus, which shows that thermal fluctuations may populate two alternative ground-state electronic wave functions optimized for electron entry and exit, respectively, through two different and nearly perpendicular pathways. In conclusion, these findings suggest a unique role for alternative or “invisible” electronic ground states in directional electron transfer. Moreover, it is shown that this energy gap and, therefore, the equilibrium between ground states can be fine-tuned by minor perturbations, suggesting alternative ways through which protein–protein interactions and membrane potential may optimize and regulate electron–proton energy transduction.

  3. Computing electronic structures: A new multiconfiguration approach for excited states

    NASA Astrophysics Data System (ADS)

    Cancès, Éric; Galicher, Hervé; Lewin, Mathieu

    2006-02-01

    We present a new method for the computation of electronic excited states of molecular systems. This method is based upon a recent theoretical definition of multiconfiguration excited states [due to one of us, see M. Lewin, Solutions of the multiconfiguration equations in quantum chemistry, Arch. Rat. Mech. Anal. 171 (2004) 83-114]. Our algorithm, dedicated to the computation of the first excited state, always converges to a stationary state of the multiconfiguration model, which can be interpreted as an approximate excited state of the molecule. The definition of this approximate excited state is variational. An interesting feature is that it satisfies a non-linear Hylleraas-Undheim-MacDonald type principle: the energy of the approximate excited state is an upper bound to the true excited state energy of the N-body Hamiltonian. To compute the first excited state, one has to deform paths on a manifold, like this is usually done in the search for transition states between reactants and products on potential energy surfaces. We propose here a general method for the deformation of paths which could also be useful in other settings. We also compare our method to other approaches used in Quantum Chemistry and give some explanation of the unsatisfactory behaviours which are sometimes observed when using the latters. Numerical results for the special case of two-electron systems are provided: we compute the first singlet excited state potential energy surface of the H2 molecule.

  4. Computing electronic structures: A new multiconfiguration approach for excited states

    SciTech Connect

    Cances, Eric . E-mail: cances@cermics.enpc.fr; Galicher, Herve . E-mail: galicher@cermics.enpc.fr; Lewin, Mathieu . E-mail: lewin@cermic.enpc.fr

    2006-02-10

    We present a new method for the computation of electronic excited states of molecular systems. This method is based upon a recent theoretical definition of multiconfiguration excited states [due to one of us, see M. Lewin, Solutions of the multiconfiguration equations in quantum chemistry, Arch. Rat. Mech. Anal. 171 (2004) 83-114]. Our algorithm, dedicated to the computation of the first excited state, always converges to a stationary state of the multiconfiguration model, which can be interpreted as an approximate excited state of the molecule. The definition of this approximate excited state is variational. An interesting feature is that it satisfies a non-linear Hylleraas-Undheim-MacDonald type principle: the energy of the approximate excited state is an upper bound to the true excited state energy of the N-body Hamiltonian. To compute the first excited state, one has to deform paths on a manifold, like this is usually done in the search for transition states between reactants and products on potential energy surfaces. We propose here a general method for the deformation of paths which could also be useful in other settings. We also compare our method to other approaches used in Quantum Chemistry and give some explanation of the unsatisfactory behaviours which are sometimes observed when using the latter. Numerical results for the special case of two-electron systems are provided: we compute the first singlet excited state potential energy surface of the H {sub 2} molecule.

  5. Charge transfer to ground-state ions produces free electrons

    NASA Astrophysics Data System (ADS)

    You, D.; Fukuzawa, H.; Sakakibara, Y.; Takanashi, T.; Ito, Y.; Maliyar, G. G.; Motomura, K.; Nagaya, K.; Nishiyama, T.; Asa, K.; Sato, Y.; Saito, N.; Oura, M.; Schöffler, M.; Kastirke, G.; Hergenhahn, U.; Stumpf, V.; Gokhberg, K.; Kuleff, A. I.; Cederbaum, L. S.; Ueda, K.

    2017-01-01

    Inner-shell ionization of an isolated atom typically leads to Auger decay. In an environment, for example, a liquid or a van der Waals bonded system, this process will be modified, and becomes part of a complex cascade of relaxation steps. Understanding these steps is important, as they determine the production of slow electrons and singly charged radicals, the most abundant products in radiation chemistry. In this communication, we present experimental evidence for a so-far unobserved, but potentially very important step in such relaxation cascades: Multiply charged ionic states after Auger decay may partially be neutralized by electron transfer, simultaneously evoking the creation of a low-energy free electron (electron transfer-mediated decay). This process is effective even after Auger decay into the dicationic ground state. In our experiment, we observe the decay of Ne2+ produced after Ne 1s photoionization in Ne-Kr mixed clusters.

  6. Charge transfer to ground-state ions produces free electrons

    PubMed Central

    You, D.; Fukuzawa, H.; Sakakibara, Y.; Takanashi, T.; Ito, Y.; Maliyar, G. G.; Motomura, K.; Nagaya, K.; Nishiyama, T.; Asa, K.; Sato, Y.; Saito, N.; Oura, M.; Schöffler, M.; Kastirke, G.; Hergenhahn, U.; Stumpf, V.; Gokhberg, K.; Kuleff, A. I.; Cederbaum, L. S.; Ueda, K

    2017-01-01

    Inner-shell ionization of an isolated atom typically leads to Auger decay. In an environment, for example, a liquid or a van der Waals bonded system, this process will be modified, and becomes part of a complex cascade of relaxation steps. Understanding these steps is important, as they determine the production of slow electrons and singly charged radicals, the most abundant products in radiation chemistry. In this communication, we present experimental evidence for a so-far unobserved, but potentially very important step in such relaxation cascades: Multiply charged ionic states after Auger decay may partially be neutralized by electron transfer, simultaneously evoking the creation of a low-energy free electron (electron transfer-mediated decay). This process is effective even after Auger decay into the dicationic ground state. In our experiment, we observe the decay of Ne2+ produced after Ne 1s photoionization in Ne–Kr mixed clusters. PMID:28134238

  7. Fragmentation pathwaysfor selected electronic states of theacetylene dication

    SciTech Connect

    Osipov, Timur; Rescigno, Thomas N.; Weber, Thorsten; Miyabe,Shungo; Jahnke, T.; Alnaser, A.; Hertlein, Markus P.; Jagutzki, O.; Schmidt, L.Ph.H.; Schoffler, M.; Foucar, L.; Schossler, S.; Havermeier,T.; Odenweller,M.; Voss, S.; Feinberg, Ben; Landers, Alan; Prior, MichaelH.; Dorner, Reinhart; Cocke, C.L.; Belkacem, Ali

    2007-12-18

    Coincident measurement of the Auger electron and fragmention momenta emitted after carbon core-level photoionization of acetylenehas yielded new understanding of how the dication fragments. Ab initiocalculations and experimental data, including body-frame Auger angulardistributions, are used to identify the parent electronic states andtogether yield a comprehensive map of the dissociation pathways whichinclude surface crossings and barriers to direct dissociation. The Augerangular distributions show evidence of core-holelocalization.

  8. Microwave zero-resistance states in a bilayer electron system.

    PubMed

    Wiedmann, S; Gusev, G M; Raichev, O E; Bakarov, A K; Portal, J C

    2010-07-09

    Magnetotransport measurements on a high-mobility electron bilayer system formed in a wide GaAs quantum well reveal vanishing dissipative resistance under continuous microwave irradiation. Profound zero-resistance states (ZRS) appear even in the presence of additional intersubband scattering of electrons. We study the dependence of photoresistance on frequency, microwave power, and temperature. Experimental results are compared with a theory demonstrating that the conditions for absolute negative resistivity correlate with the appearance of ZRS.

  9. 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.

  10. Electron-impact excitation of the low-lying electronic states of formaldehyde

    NASA Technical Reports Server (NTRS)

    Chutjian, A.

    1974-01-01

    Electron-impact excitation has been observed at incident electron energies of 10.1 and 20.1 eV to the first five excited electronic states of formaldehyde lying at and below the 1B2 state at 7.10 eV. These excitations include two new transitions in the energy-loss range 5.6-6.2 eV and 6.7-7.0 eV which have been detected for the first time, either through electron-impact excitation or photon absorption. The differential cross sections of these new excitations are given at scattering angles between 15 and 135 deg. These cross-section ratios peak at large scattering angles - a characteristic of triplet - singlet excitations. The design and performance of the electron-impact spectrometer used in the above observations is outlined and discussed.

  11. Integral cross sections for electron impact excitation of vibrational and electronic states in phenol

    SciTech Connect

    Neves, R. F. C.; Jones, D. B.; Lopes, M. C. A.; Blanco, F.; García, G.; Ratnavelu, K.; Brunger, M. J.

    2015-05-21

    We report on measurements of integral cross sections (ICSs) for electron impact excitation of a series of composite vibrational modes and electronic-states in phenol, where the energy range of those experiments was 15–250 eV. There are currently no other results against which we can directly compare those measured data. We also report results from our independent atom model with screened additivity rule correction computations, namely, for the inelastic ICS (all discrete electronic states and neutral dissociation) and the total ionisation ICS. In addition, for the relevant dipole-allowed excited electronic states, we also report f-scaled Born-level and energy-corrected and f-scaled Born-level (BEf-scaled) ICS. Where possible, our measured and calculated ICSs are compared against one another with the general level of accord between them being satisfactory to within the measurement uncertainties.

  12. Alternative ground states enable pathway switching in biological electron transfer

    DOE PAGES

    Abriata, Luciano A.; Alvarez-Paggi, Damian; Ledesma, Gabirela N.; ...

    2012-10-10

    Electron transfer is the simplest chemical reaction and constitutes the basis of a large variety of biological processes, such as photosynthesis and cellular respiration. Nature has evolved specific proteins and cofactors for these functions. The mechanisms optimizing biological electron transfer have been matter of intense debate, such as the role of the protein milieu between donor and acceptor sites. Here we propose a mechanism regulating long-range electron transfer in proteins. Specifically, we report a spectroscopic, electrochemical, and theoretical study on WT and single-mutant CuA redox centers from Thermus thermophilus, which shows that thermal fluctuations may populate two alternative ground-state electronicmore » wave functions optimized for electron entry and exit, respectively, through two different and nearly perpendicular pathways. In conclusion, these findings suggest a unique role for alternative or “invisible” electronic ground states in directional electron transfer. Moreover, it is shown that this energy gap and, therefore, the equilibrium between ground states can be fine-tuned by minor perturbations, suggesting alternative ways through which protein–protein interactions and membrane potential may optimize and regulate electron–proton energy transduction.« less

  13. Electronic State Decomposition of Energetic Materials and Model Systems

    DTIC Science & Technology

    2010-11-17

    tetrazine1,4-dioxde ( DATO ), is investigated. Although these molecules are based on N -oxides of a tetrazine aromatic heterocyclic ring, their...nitramines, furazan, tetrazines, tetrazine-N oxides, terazoles, PETN, RDX,HMX,CL-20,DAATO,ACTO, DATO ,conical intersections Elliot R Bernstein Colorado State...Tetrazine-N-Oxide Based High Nitrogen Content Energetic Materials from Excited Electronic States," J. Chem. Phys. 131, 194304 (2009). A

  14. Nature of ground and electronic excited states of higher acenes

    PubMed Central

    Yang, Yang; Yang, Weitao

    2016-01-01

    Higher acenes have drawn much attention as promising organic semiconductors with versatile electronic properties. However, the nature of their ground state and electronic excited states is still not fully clear. Their unusual chemical reactivity and instability are the main obstacles for experimental studies, and the potentially prominent diradical character, which might require a multireference description in such large systems, hinders theoretical investigations. Here, we provide a detailed answer with the particle–particle random-phase approximation calculation. The 1Ag ground states of acenes up to decacene are on the closed-shell side of the diradical continuum, whereas the ground state of undecacene and dodecacene tilts more to the open-shell side with a growing polyradical character. The ground state of all acenes has covalent nature with respect to both short and long axes. The lowest triplet state 3B2u is always above the singlet ground state even though the energy gap could be vanishingly small in the polyacene limit. The bright singlet excited state 1B2u is a zwitterionic state to the short axis. The excited 1Ag state gradually switches from a double-excitation state to another zwitterionic state to the short axis, but always keeps its covalent nature to the long axis. An energy crossing between the 1B2u and excited 1Ag states happens between hexacene and heptacene. Further energetic consideration suggests that higher acenes are likely to undergo singlet fission with a low photovoltaic efficiency; however, the efficiency might be improved if a singlet fission into multiple triplets could be achieved. PMID:27528690

  15. Experimental Studies of Interacting Electronic States in NaCs

    NASA Astrophysics Data System (ADS)

    Faust, Carl E.

    This dissertation describes methods and results of spectroscopic studies of the NaCs molecule. NaCs is of particular interest in many labs where experimental studies of ultra-cold molecules are being conducted. Data obtained in the present work will also be useful as benchmarks for various theoretical calculations. Our goals in studying this molecule were to map out high lying electronic states and to understand how these states interact with one another. Sodium and cesium metal were heated in a heat-pipe oven to form a vapor of NaCs molecules. These molecules were excited using narrow band, continuous wave (cw), tunable lasers. We employed the optical-optical double resonance (OODR) technique to obtain Doppler-free spectra of transitions to rotational and vibrational levels of high lying electronic states. One state of particular interest was the 12(0+) electronic state. Rovibrational level energies corresponding to this state were measured and used to generate a potential energy curve using computer programs to implement both the Rydberg-Klein-Rees (RKR) method and the inverted perturbation approach (IPA). By observing fluorescence from the 12(0+) state resolved as a function of wavelength, we determined that this state interacts with the nearby 11(0+) electronic state, which was previously mapped out by Ashman et al. A two-stage coupling model was devised to describe the resolved fluorescence originating from these two interacting states. The electronic states interact via spin-orbit coupling, while the individual rovibrational levels interact via a second mechanism, likely nonadiabatic coupling. This two-stage coupling between the levels of these states causes quantum interference between fluorescence pathways associated with different components of the wavefunctions describing these levels. This interference results in more complicated resolved fluorescence spectra. The model was used to fit parameters describing these interactions so that the resolved

  16. A many-body states picture of electronic friction: The case of multiple orbitals and multiple electronic states.

    PubMed

    Dou, Wenjie; Subotnik, Joseph E

    2016-08-07

    We present a very general form of electronic friction as present when a molecule with multiple orbitals hybridizes with a metal electrode. To develop this picture of friction, we embed the quantum-classical Liouville equation (QCLE) within a classical master equation (CME). Thus, this article extends our previous work analyzing the case of one electronic level, as we may now treat the case of multiple levels and many electronic molecular states. We show that, in the adiabatic limit, where electron transitions are much faster than nuclear motion, the QCLE-CME reduces to a Fokker-Planck equation, such that nuclei feel an average force as well as friction and a random force-as caused by their interaction with the metallic electrons. Finally, we show numerically and analytically that our frictional results agree with other published results calculated using non-equilibrium Green's functions. Numerical recipes for solving this QCLE-CME will be provided in a subsequent paper.

  17. A many-body states picture of electronic friction: The case of multiple orbitals and multiple electronic states

    NASA Astrophysics Data System (ADS)

    Dou, Wenjie; Subotnik, Joseph E.

    2016-08-01

    We present a very general form of electronic friction as present when a molecule with multiple orbitals hybridizes with a metal electrode. To develop this picture of friction, we embed the quantum-classical Liouville equation (QCLE) within a classical master equation (CME). Thus, this article extends our previous work analyzing the case of one electronic level, as we may now treat the case of multiple levels and many electronic molecular states. We show that, in the adiabatic limit, where electron transitions are much faster than nuclear motion, the QCLE-CME reduces to a Fokker-Planck equation, such that nuclei feel an average force as well as friction and a random force—as caused by their interaction with the metallic electrons. Finally, we show numerically and analytically that our frictional results agree with other published results calculated using non-equilibrium Green's functions. Numerical recipes for solving this QCLE-CME will be provided in a subsequent paper.

  18. Ultrafast Spectroscopy of Delocalized Excited States of the Hydrated Electron

    SciTech Connect

    Paul F. Barbara

    2005-09-28

    Research under support of this grant has been focused on the understanding of highly delocalized ''conduction-band-like'' excited states of solvated electrons in bulk water, in water trapped in the core of reverse micelles, and in alkane solvents. We have strived in this work to probe conduction-band-like states by a variety of ultrafast spectroscopy techniques. (Most of which were developed under DOE support in a previous funding cycle.) We have recorded the optical spectrum of the hydrated electron for the first time. This was accomplished by applying a photo-detrapping technique that we had developed in a previous funding cycle, but had not yet been applied to characterize the actual spectrum. In the cases of reverse micelles, we have been investigating the potential role of conduction bands in the electron attachment process and the photoinduced detrapping, and have published two papers on this topic. Finally, we have been exploring solvated electrons in isooctane from various perspectives. All of these results strongly support the conclusion that optically accessible, highly delocalized electronic states exist in these various media.

  19. Status of state electronic disease surveillance systems--United States, 2007.

    PubMed

    2009-07-31

    The National Electronic Disease Surveillance System (NEDSS) is a web-based system that uses standard health information technology (IT) codes to integrate disease surveillance systems, enabling them to transfer public health, laboratory, and clinical data securely from health-care providers to public health departments. Each jurisdictions' system consists of a base system and modules that can be used for specific surveillance purposes. States also use NEDSS-like or other electronic systems to conduct surveillance on specific diseases or conditions. Until recently, no assessment had been done to describe the status and characteristics of state electronic disease surveillance systems. The Council of State and Territorial Epidemiologists (CSTE) conducted such an assessment in August 2007 in all 50 states. This report presents the results of that assessment, which indicated that, in 2007, state electronic disease surveillance systems varied widely and were in various stages of implementation. Each state had either custom-built systems or purchased systems that were customizable, with associated disease modules to meet its own surveillance needs. As interoperability becomes the standard for electronic data sharing, more states will face customization costs and the need to hire more technical specialists who can manage health information and exchange. Further collaboration and support from surveillance and health-care IT stakeholders with public health will be needed to improve the efficacy and quality of electronic disease surveillance systems.

  20. Controlling autoionization in strontium two-electron-excited states

    NASA Astrophysics Data System (ADS)

    Fields, Robert; Zhang, Xinyue; Dunning, F. Barry; Yoshida, Shuhei; Burgdörfer, Joachim

    2016-05-01

    One challenge in engineering long-lived two-electron-excited states, i.e., so-called planetary atoms, is autoionization. Autoionization, however, can be suppressed if the outermost electron is placed in a high- n, n ~ 300 - 600 , high- L state because such states have only a very small overlap with the inner electron, even when this is also excited to a state of relatively high n and hence of relatively long lifetime. Here the L-dependence of the autoionization rate for high- n strontium Rydberg atoms is examined during excitation of the core ion 5 s 2S1 / 2 - 5 p 2P3 / 2 transition. Measurements in which the angular momentum of the Rydberg electron is controlled using a pulsed electric field show that the autoionization rate decreases rapidly with increasing L and becomes very small for values larger than ~ 20 . The data are analyzed with the aid of calculations undertaken using complex scaling. Research supported by the NSF and Robert A. Welch Foundation.

  1. Tuning ground states and excitations in complex electronic materials

    SciTech Connect

    Bishop, A.R.

    1996-09-01

    Modern electronic materials are characterized by a great variety of broken-symmetry ground states and excitations. Their control requires understanding and tuning underlying driving forces of spin-charge-lattice coupling, critical to macroscopic properties and applications. We report representative model calculations which demonstrate some of the richness of the phenomena and the challenges for successful microscopic modeling.

  2. 45 CFR 265.6 - Must States file reports electronically?

    Code of Federal Regulations, 2010 CFR

    2010-10-01

    ... 45 Public Welfare 2 2010-10-01 2010-10-01 false Must States file reports electronically? 265.6 Section 265.6 Public Welfare Regulations Relating to Public Welfare OFFICE OF FAMILY ASSISTANCE (ASSISTANCE PROGRAMS), ADMINISTRATION FOR CHILDREN AND FAMILIES, DEPARTMENT OF HEALTH AND HUMAN SERVICES...

  3. Determining the Origins of Electronic States in Semiconductor Nanostructures

    SciTech Connect

    Goldman, Rachel S.; Johnson, H. T.

    2014-12-15

    With support from this program, we have generated key results in quantum dot (QD) formation, strain/electronic coupling, measurement and modeling of confined states, and examination of the influence of QDs on thermoelectric and photovoltaic properties of nanocomposite structures. This final report contains a description of our key findings followed by a list of personnel supported and publications generated.

  4. Spilling of electronic states in Pb quantum wells

    NASA Astrophysics Data System (ADS)

    Jałochowski, M.; Palotás, K.; Krawiec, M.

    2016-01-01

    Energy-dependent apparent step heights of two-dimensional ultrathin Pb islands grown on the Si(111)6 ×6 -Au surface have been investigated by a combination of scanning tunneling microscopy, first-principles density-functional theory, and the particle-in-a-box model calculations. The apparent step height shows the thickness- and energy-dependent oscillatory behaviors, which are directly related to the spilling of electron states into the vacuum exhibiting a quantum size effect. This has been unambiguously proven by extensive first-principles scanning tunneling microscopy and spectroscopy simulations. An electronic contribution to the apparent step height is directly determined. At certain energies it reaches values as high as a half of the atomic contribution. The applicability of the particle-in-a-box model to the spilling of electron states is also discussed.

  5. Internal conversion from excited electronic states of 229Th ions

    NASA Astrophysics Data System (ADS)

    Bilous, Pavlo V.; Kazakov, Georgy A.; Moore, Iain D.; Schumm, Thorsten; Pálffy, Adriana

    2017-03-01

    The process of internal conversion from excited electronic states is investigated theoretically for the case of the vacuum-ultraviolet nuclear transition of 229Th. Due to the very low transition energy, the 229Th nucleus offers the unique possibility to open the otherwise forbidden internal conversion nuclear decay channel for thorium ions via optical laser excitation of the electronic shell. We show that this feature can be exploited to investigate the isomeric state properties via observation of internal conversion from excited electronic configurations of +Th and Th+2 ions. A possible experimental realization of the proposed scenario at the nuclear laser spectroscopy facility IGISOL in Jyväskylä, Finland, is discussed.

  6. Electronic density of states in sequence dependent DNA molecules

    NASA Astrophysics Data System (ADS)

    de Oliveira, B. P. W.; Albuquerque, E. L.; Vasconcelos, M. S.

    2006-09-01

    We report in this work a numerical study of the electronic density of states (DOS) in π-stacked arrays of DNA single-strand segments made up from the nucleotides guanine G, adenine A, cytosine C and thymine T, forming a Rudin-Shapiro (RS) as well as a Fibonacci (FB) polyGC quasiperiodic sequences. Both structures are constructed starting from a G nucleotide as seed and following their respective inflation rules. Our theoretical method uses Dyson's equation together with a transfer-matrix treatment, within an electronic tight-binding Hamiltonian model, suitable to describe the DNA segments modelled by the quasiperiodic chains. We compared the DOS spectra found for the quasiperiodic structure to those using a sequence of natural DNA, as part of the human chromosome Ch22, with a remarkable concordance, as far as the RS structure is concerned. The electronic spectrum shows several peaks, corresponding to localized states, as well as a striking self-similar aspect.

  7. 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.

  8. 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.

  9. (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.

  10. Targeting excited states in all-trans polyenes with electron-pair states

    NASA Astrophysics Data System (ADS)

    Boguslawski, Katharina

    2016-12-01

    Wavefunctions restricted to electron pair states are promising models for strongly correlated systems. Specifically, the pair Coupled Cluster Doubles (pCCD) ansatz allows us to accurately describe bond dissociation processes and heavy-element containing compounds with multiple quasi-degenerate single-particle states. Here, we extend the pCCD method to model excited states using the equation of motion (EOM) formalism. As the cluster operator of pCCD is restricted to electron-pair excitations, EOM-pCCD allows us to target excited electron-pair states only. To model singly excited states within EOM-pCCD, we modify the configuration interaction ansatz of EOM-pCCD to contain also single excitations. Our proposed model represents a simple and cost-effective alternative to conventional EOM-CC methods to study singly excited electronic states. The performance of the excited state models is assessed against the lowest-lying excited states of the uranyl cation and the two lowest-lying excited states of all-trans polyenes. Our numerical results suggest that EOM-pCCD including single excitations is a good starting point to target singly excited states.

  11. Targeting excited states in all-trans polyenes with electron-pair states.

    PubMed

    Boguslawski, Katharina

    2016-12-21

    Wavefunctions restricted to electron pair states are promising models for strongly correlated systems. Specifically, the pair Coupled Cluster Doubles (pCCD) ansatz allows us to accurately describe bond dissociation processes and heavy-element containing compounds with multiple quasi-degenerate single-particle states. Here, we extend the pCCD method to model excited states using the equation of motion (EOM) formalism. As the cluster operator of pCCD is restricted to electron-pair excitations, EOM-pCCD allows us to target excited electron-pair states only. To model singly excited states within EOM-pCCD, we modify the configuration interaction ansatz of EOM-pCCD to contain also single excitations. Our proposed model represents a simple and cost-effective alternative to conventional EOM-CC methods to study singly excited electronic states. The performance of the excited state models is assessed against the lowest-lying excited states of the uranyl cation and the two lowest-lying excited states of all-trans polyenes. Our numerical results suggest that EOM-pCCD including single excitations is a good starting point to target singly excited states.

  12. Foucault's Pendulum, Analog for an Electron Spin State

    NASA Astrophysics Data System (ADS)

    Linck, Rebecca

    2012-11-01

    The classical Lagrangian that describes the coupled oscillations of Foucault's pendulum presents an interesting analog to an electron's spin state in an external magnetic field. With a simple modification, this classical Lagrangian yields equations of motion that directly map onto the Schrodinger-Pauli Equation. This analog goes well beyond the geometric phase, reproducing a broad range of behavior from Zeeman-like frequency splitting to precession of the spin state. By demonstrating that unmeasured spin states can be fully described in classical terms, this research opens the door to using the tools of classical physics to examine an inherently quantum phenomenon.

  13. The low-lying electronic states of ReB.

    PubMed

    Borin, Antonio Carlos; Gobbo, João Paulo; Castro, César Augusto Milani

    2014-07-01

    The ground and low-lying electronic states of ReB were studied at the CASPT2//CASSCF level (multiconfigurational second-order perturbation theory) and quadruple-ζ ANO-RCC basis sets. Spectroscopic constants, potential energy curves, wavefunctions, and Mulliken population analysis are given. The ground state of ReB is of X(5)Σ(+) symmetry (R e  = 1.817 Å, ω e  = .909 cm(-1), and μ = 2.87 D), giving rise to a Ω = 0(+) ground state after including spin-orbit coupling.

  14. The electronic properties of superatom states of hollow molecules.

    PubMed

    Feng, Min; Zhao, Jin; Huang, Tian; Zhu, Xiaoyang; Petek, Hrvoje

    2011-05-17

    Electronic and optical properties of molecules and molecular solids are traditionally considered from the perspective of the frontier orbitals and their intermolecular interactions. How molecules condense into crystalline solids, however, is mainly attributed to the long-range polarization interaction. In this Account, we show that long-range polarization also introduces a distinctive set of diffuse molecular electronic states, which in quantum structures or solids can combine into nearly-free-electron (NFE) bands. These NFE properties, which are usually associated with good metals, are vividly evident in sp(2) hybridized carbon materials, specifically graphene and its derivatives. The polarization interaction is primarily manifested in the screening of an external charge at a solid/vacuum interface. It is responsible for the universal image potential and the associated unoccupied image potential (IP) states, which are observed even at the He liquid/vacuum interface. The molecular electronic properties that we describe are derived from the IP states of graphene, which float above and below the molecular plane and undergo free motion parallel to it. Rolling or wrapping a graphene sheet into a nanotube or a fullerene transforms the IP states into diffuse atom-like orbitals that are bound primarily to hollow molecular cores, rather than the component atoms. Therefore, we named them the superatom molecular orbitals (SAMOs). Like the excitonic states of semiconductor nanostructures or the plasmonic resonances of metallic nanoparticles, SAMOs of fullerene molecules, separated by their van der Waals distance, can combine to form diatomic molecule-like orbitals of C(60) dimers. For larger aggregates, they form NFE bands of superatomic quantum structures and solids. The overlap of the diffuse SAMO wavefunctions in van der Waals solids provides a different paradigm for band formation than the valence or conduction bands formed by interaction of the more tightly bound

  15. Foucault's pendulum, a classical analog for the electron spin state

    NASA Astrophysics Data System (ADS)

    Linck, Rebecca A.

    Spin has long been regarded as a fundamentally quantum phenomena that is incapable of being described classically. To bridge the gap and show that aspects of spin's quantum nature can be described classically, this work uses a classical Lagrangian based on the coupled oscillations of Foucault's pendulum as an analog for the electron spin state in an external magnetic field. With this analog it is possible to demonstrate that Foucault's pendulum not only serves as a basis for explaining geometric phase, but is also a basis for reproducing a broad range of behavior from Zeeman-like frequency splitting to precession of the spin state. By demonstrating that unmeasured electron spin states can be fully described in classical terms, this research opens the door to using the tools of classical physics to examine an inherently quantum phenomenon.

  16. Calculation of electron scattering from the ground state of ytterbium

    SciTech Connect

    Bostock, Christopher J.; Fursa, Dmitry V.; Bray, Igor

    2011-05-15

    We report on the application of the convergent close-coupling method, in both relativistic and nonrelativistic formulations, to electron scattering from ytterbium. Angle-differential and integrated cross sections are presented for elastic scattering and excitation of the states (6s6p){sup 3}P{sub 0,1,2}, (6s6p){sup 1}P{sub 1}{sup o}, (6s7p){sup 1}P{sub 1}{sup o}, and (6s5d){sup 1}D{sub 2}{sup e} for a range of incident electron energies. We also present calculations of the total cross section, and angle-differential Stokes parameters for excitation of the (6s6p){sup 3}P{sub 1}{sup o} state from the ground state. A comparison is made with the relativistic distorted-wave method and experiments.

  17. Electronic states of PF 2 and PF +2

    NASA Astrophysics Data System (ADS)

    Latifzadeh, Lida; Balasubramanian, K.

    1994-10-01

    The ground and excited electronic states of PF 2 and PF +2 have been investigated using the complete active space self-consistent field (CASSCF) followed by multi-reference singles and doubles configuration interaction (MRSDCI) methods that include up to 1.2 million configurations. These states include X 2B 1, 4A 2, 2A 1(I), 2A 1(II), 2A 2, 2B 2(I), 2B 2(II), 4B 1, 2B 1(II) for PF 2 and 1A 1, 3B 1, 1B 1 for PF +2. Both all-electron computations employing large basis sets and relativistic effective core potentials using valence basis sets were carried out. The spectroscopic properties were determined for the bound states. The dissociation energy of PFF is obtained using the full second-order configuration interaction (SOCI) and CASSCF/MRSDCI methods.

  18. Optical limiting and picosecond relaxation of carbocyanines upper electronic states

    NASA Astrophysics Data System (ADS)

    Oulianov, D. A.; Dvornikov, A. S.; Rentzepis, P. M.

    2002-05-01

    Nonlinear absorption, anomalous fluorescence and relaxation of high-lying electronic states in six carbocyanine dyes, including cryptocyanine (DCI), DDI, DTDCI, DTTCI, DOTCI and HDIDCI, in solution and in polymer, were studied by means of picosecond transient absorption spectroscopy and nonlinear transmission experiments. Absorption cross-sections of the S 1→S n transition, and decay rates of the second singlet excited state, S 2, were measured. All dyes showed strong reverse saturable absorption in the 450-600 nm region with large excited to ground state absorption cross-section ratios. For DTDCI this ratio, at 470 nm, was measured to be 350, which is the largest ever reported. All molecules have shown strong optical limiting effect. However, in all molecules except DCI a saturation of the optical limiting process was observed as expected, owing to relatively long, up to 17.5 ps, lifetime of the S 2 state. The S 2 state fluorescence quantum yields were also measured.

  19. Kinetic and electron-electron energies for convex sums of ground state densities with degeneracies and fractional electron number

    SciTech Connect

    Levy, Mel E-mail: mlevy@tulane.edu; Anderson, James S. M.; Zadeh, Farnaz Heidar; Ayers, Paul W. E-mail: mlevy@tulane.edu

    2014-05-14

    Properties of exact density functionals provide useful constraints for the development of new approximate functionals. This paper focuses on convex sums of ground-level densities. It is observed that the electronic kinetic energy of a convex sum of degenerate ground-level densities is equal to the convex sum of the kinetic energies of the individual degenerate densities. (The same type of relationship holds also for the electron-electron repulsion energy.) This extends a known property of the Levy-Valone Ensemble Constrained-Search and the Lieb Legendre-Transform refomulations of the Hohenberg-Kohn functional to the individual components of the functional. Moreover, we observe that the kinetic and electron-repulsion results also apply to densities with fractional electron number (even if there are no degeneracies), and we close with an analogous point-wise property involving the external potential. Examples where different degenerate states have different kinetic energy and electron-nuclear attraction energy are given; consequently, individual components of the ground state electronic energy can change abruptly when the molecular geometry changes. These discontinuities are predicted to be ubiquitous at conical intersections, complicating the development of universally applicable density-functional approximations.

  20. Low-lying electronic states of LiF molecule with inner electrons correlation

    NASA Astrophysics Data System (ADS)

    Wan, Ming-jie; Huang, Duo-hui; Yang, Jun-sheng; Cao, Qi-long; Jin, Cheng-guo; Wang, Fan-hou

    2015-06-01

    The potential energy curves and dipole moments of the low-lying electronic states of LiF molecule are performed by using highly accurate multi-reference configuration interaction with Awcv5z basis sets. 1s, the inner shell of Li is considered as the closed orbit, which is used to characterise the spectroscopic properties of a manifold of singlet and triplet states. 16 electronic states correlate with two lowest dissociation channels Li(2S)+F(2P) and Li(2P)+F(2P) are investigated. Spectroscopic parameters of the ground state X1Σ+ have been evaluated and critically compared with the available experimental values and the other theoretical data. However, spectroscopic parameters of 13Π, 11Δ, 11Σ-, 11Π, 13Σ+, 23Σ+, 13Δ, 13Σ-, 23Π, 21Π, 33Π, 31Π and 33Σ+ states are studied for the first time. These 13 excited states have shallow potential wells, and the dispersion coefficients of these excited states are predicted. In additional, oscillator strengths of excited states at equilibrium distances are also predicted.

  1. 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.

  2. Electron teleportation via Majorana bound states in a mesoscopic superconductor.

    PubMed

    Fu, Liang

    2010-02-05

    Zero-energy Majorana bound states in superconductors have been proposed to be potential building blocks of a topological quantum computer, because quantum information can be encoded nonlocally in the fermion occupation of a pair of spatially separated Majorana bound states. However, despite intensive efforts, nonlocal signatures of Majorana bound states have not been found in charge transport. In this work, we predict a striking nonlocal phase-coherent electron transfer process by virtue of tunneling in and out of a pair of Majorana bound states. This teleportation phenomenon only exists in a mesoscopic superconductor because of an all-important but previously overlooked charging energy. We propose an experimental setup to detect this phenomenon in a superconductor-quantum-spin-Hall-insulator-magnetic-insulator hybrid system.

  3. Dynamics and spectroscopy of CH₂OO excited electronic states.

    PubMed

    Kalinowski, Jaroslaw; Foreman, Elizabeth S; Kapnas, Kara M; Murray, Craig; Räsänen, Markku; Gerber, R Benny

    2016-04-28

    The excited states of the Criegee intermediate CH2OO are studied in molecular dynamics simulations using directly potentials from multi-reference perturbation theory (MR-PT2). The photoexcitation of the species is simulated, and trajectories are propagated in time on the excited state. Some of the photoexcitation events lead to direct fragmentation of the molecule, but other trajectories describe at least several vibrations in the excited state, that may terminate by relaxation to the ground electronic state. Limits on the role of non-adiabatic contributions to the process are estimated by two different simulations, one that forces surface-hopping at potential crossings, and another that ignores surface hopping altogether. The effect of non-adiabatic transitions is found to be small. Spectroscopic implications and consequences for the interpretation of experimental results are discussed.

  4. Controlled interaction of surface quantum-well electronic states.

    PubMed

    Seufert, Knud; Auwärter, Willi; García de Abajo, F J; Ecija, David; Vijayaraghavan, Saranyan; Joshi, Sushobhan; Barth, Johannes V

    2013-01-01

    We report on the construction of well-defined surface quantum well arrangements by combining self-assembly protocols and molecular manipulation procedures. After the controlled removal of individual porphyrin molecules from dense-packed arrays on Ag(111), the surface state electrons are confined at the bare silver patches. These act as quantum wells that show well-defined unoccupied bound surface states. Scanning tunneling spectroscopy and complementary boundary element method calculations are performed to characterize the interaction between the bound states of adjacent quantum wells and reveal a hybridization of wave functions resulting in bonding and antibonding states. The interwell coupling can be tuned by the deliberate choice of the molecules acting as potential barriers. The fabrication method is shown to be ideally suited to engineer specific configurations as one-dimensional chains or two-dimensional artificial molecules.

  5. 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.

  6. Evolution of electronic states in fullerenes with size

    NASA Astrophysics Data System (ADS)

    Dong, Jianjun; Drabold, David A.

    1996-04-01

    The electronic density of states (DOS) of fullerenes is studied in this paper. The DOS of small fullerences (C_60 and C_240) is computed with exact diagonalization, while the DOS of large fullerences (C_540, C_960, C_2169 and C_3840) is computed with a newly developed ``Order N" electronic structure method: the maximum entropy method (Maxent) footnote D.A. Drabold, O.F. Sankey, Phys. Rev. Lett. 70 3631,(1995). The projected DOS at different types of sites (pentagon site and facet center hexagon site) is also computed with Maxent. We illustrate the size dependence and the cluster to crystal evolution. footnote D.A. Drabold, P.Ordejón, J. Dong and R.M. Martin, Solid State Commun.,96 833, (1995). We observe that the DOS closely approximates graphite for relaxed C_2160 and C_3840.

  7. 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.

  8. 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

  9. Understanding x-ray driven impulsive electronic state redistribution using a three-state model

    NASA Astrophysics Data System (ADS)

    Ware, Matthew R.; Cryan, James; Bucksbaum, Philip H.

    2016-05-01

    The natural timescale for electron motion is extremely fast; electrons can move across molecular bonds in less than a femtosecond. To understand this fast motion and the role of electronic coherence, we are interested in creating a superposition of valence excited states through excitation with a broad bandwidth (>5eV) laser pulse. In the x-ray regime, the molecular ground state can couple to valence-excited states through an intermediate autoionizing resonance in a process known as stimulated x-ray Raman scattering (SXRS). X-rays excite electrons from the highly localized K-shells in a molecule, creating a superposition of valence-excited states initially localized around a target atom in the molecule. Coherences between states in the superposition will subsequently drive charge transfer as the wavepacket spreads out across the molecule. We use an effective 3-state model coupling the ground, auto-ionizing, and valence-excited states in diatomic systems to study the cross-section of SXRS as function of x-ray intensity, central frequency, bandwidth, and chirp. We also make observations on how the x-ray parameters affect the degree of initial localization to an atom of the wavepacket created in SXRS. This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division.

  10. Electronic thermal conductivity in a superconducting vortex state

    NASA Astrophysics Data System (ADS)

    Adachi, H.; Miranovic, P.; Ichioka, M.; Machida, K.

    2007-10-01

    The longitudinal component of the electronic thermal conductivity κxx in a superconducting vortex state is calculated as a function of magnetic field B. Calculations are performed by taking account of the spatial dependence of normal Green's function g, which was neglected in the previous studies using the Brandt-Pesch-Tewordt method. We discuss the possibility of using κxx(B) as a probe of the pair potential symmetry.

  11. Glycine in an electronically excited state: ab initio electronic structure and dynamical calculations.

    PubMed

    Muchová, Eva; Slavícek, Petr; Sobolewski, Andrzej L; Hobza, Pavel

    2007-06-21

    The goal of this study is to explore the photochemical processes following optical excitation of the glycine molecule into its two low-lying excited states. We employed electronic structure methods at various levels to map the PES of the ground state and the two low-lying excited states of glycine. It follows from our calculations that the photochemistry of glycine can be regarded as a combination of photochemical behavior of amines and carboxylic acid. The first channel (connected to the presence of amino group) results in ultrafast decay, while the channels characteristic for the carboxylic group occur on a longer time scale. Dynamical calculations provided the branching ratio for these channels. We also addressed the question whether conformationally dependent photochemistry can be observed for glycine. While electronic structure calculations favor this possibility, the ab initio multiple spawning (AIMS) calculations showed only minor relevance of the reaction path resulting in conformationally dependent dynamics.

  12. Liquid-state polaron theory of the hydrated electron revisited

    NASA Astrophysics Data System (ADS)

    Donley, James P.; Heine, David R.; Tormey, Caleb A.; Wu, David T.

    2014-07-01

    The quantum path integral/classical liquid-state theory of Chandler and co-workers, created to describe an excess electron in solvent, is re-examined for the hydrated electron. The portion that models electron-water density correlations is replaced by two equations: the range optimized random phase approximation (RO-RPA), and the Donley, Rajasekaran, and Liu (DRL) approximation to the "two-chain" equation, both shown previously to describe accurately the static structure and thermodynamics of strongly charged polyelectrolyte solutions. The static equilibrium properties of the hydrated electron are analyzed using five different electron-water pseudopotentials. The theory is then compared with data from mixed quantum/classical Monte Carlo and molecular dynamics simulations using these same pseudopotentials. It is found that the predictions of the RO-RPA and DRL-based polaron theories are similar and improve upon previous theory, with values for almost all properties analyzed in reasonable quantitative agreement with the available simulation data. Also, it is found using the Larsen, Glover, and Schwartz pseudopotential that the theories give values for the solvation free energy that are at least three times larger than that from experiment.

  13. Liquid-state polaron theory of the hydrated electron revisited

    SciTech Connect

    Donley, James P.; Heine, David R.; Tormey, Caleb A.; Wu, David T.

    2014-07-14

    The quantum path integral/classical liquid-state theory of Chandler and co-workers, created to describe an excess electron in solvent, is re-examined for the hydrated electron. The portion that models electron-water density correlations is replaced by two equations: the range optimized random phase approximation (RO-RPA), and the Donley, Rajasekaran, and Liu (DRL) approximation to the “two-chain” equation, both shown previously to describe accurately the static structure and thermodynamics of strongly charged polyelectrolyte solutions. The static equilibrium properties of the hydrated electron are analyzed using five different electron-water pseudopotentials. The theory is then compared with data from mixed quantum/classical Monte Carlo and molecular dynamics simulations using these same pseudopotentials. It is found that the predictions of the RO-RPA and DRL-based polaron theories are similar and improve upon previous theory, with values for almost all properties analyzed in reasonable quantitative agreement with the available simulation data. Also, it is found using the Larsen, Glover, and Schwartz pseudopotential that the theories give values for the solvation free energy that are at least three times larger than that from experiment.

  14. Model for primary electron transfer and coupling of electronic states at reaction centers of purple bacteria

    NASA Astrophysics Data System (ADS)

    Pavlovich, V. S.

    2006-05-01

    A detailed derivation is presented for relations making it possible to describe the effect of temperature on the halfwidth of the P960 and P870 absorption bands and also on the electron transfer (ET) rate at reaction centers (RCs) of the purple bacteria Rps. viridis and Rb. sphaeroides. Primary electron transfer is considered as a resonant nonradiative transition between P* and P+B L - states (where P is a special pair, BL is an additional bacteriochlorophyll in the L branch of the reaction center). It has been shown that the vibrational hα mode with frequency 130 150 cm-1 controls primary electron transfer. It has been found that the matrix element of the electronic transition between the states P* and P+B L - is equal to 12.7 ± 0.9 and 12.0 ± 1.2 cm-1 for Rps. viridis and Rb. sphaeroides respectively. The mechanism is discussed for electron transport from P* and BL and then to bacteriopheophytin HL.

  15. Integral elastic, electronic-state, ionization, and total cross sections for electron scattering with furfural

    NASA Astrophysics Data System (ADS)

    Jones, D. B.; da Costa, R. F.; Varella, M. T. do N.; Bettega, M. H. F.; Lima, M. A. P.; Blanco, F.; García, G.; Brunger, M. J.

    2016-04-01

    We report absolute experimental integral cross sections (ICSs) for electron impact excitation of bands of electronic-states in furfural, for incident electron energies in the range 20-250 eV. Wherever possible, those results are compared to corresponding excitation cross sections in the structurally similar species furan, as previously reported by da Costa et al. [Phys. Rev. A 85, 062706 (2012)] and Regeta and Allan [Phys. Rev. A 91, 012707 (2015)]. Generally, very good agreement is found. In addition, ICSs calculated with our independent atom model (IAM) with screening corrected additivity rule (SCAR) formalism, extended to account for interference (I) terms that arise due to the multi-centre nature of the scattering problem, are also reported. The sum of those ICSs gives the IAM-SCAR+I total cross section for electron-furfural scattering. Where possible, those calculated IAM-SCAR+I ICS results are compared against corresponding results from the present measurements with an acceptable level of accord being obtained. Similarly, but only for the band I and band II excited electronic states, we also present results from our Schwinger multichannel method with pseudopotentials calculations. Those results are found to be in good qualitative accord with the present experimental ICSs. Finally, with a view to assembling a complete cross section data base for furfural, some binary-encounter-Bethe-level total ionization cross sections for this collision system are presented.

  16. Theory of electron transfer and molecular state in DNA

    NASA Astrophysics Data System (ADS)

    Endres, Robert Gunter

    2002-09-01

    In this thesis, a mechanism for long-range electron transfer in DNA and a systematic search for high conductance DNA are developed. DNA is well known for containing the genetic code of all living species. On the other hand, there are some experimental indications that DNA can mediate effectively long-range electron transfer leading to the concept of chemistry at a distance. This can be important for DNA damage and healing. In the first part of the thesis, a possible mechanism for long-range electron transfer is introduced. The weak distance dependent electron transfer was experimentally observed using transition metal intercalators for donor and acceptor. In our model calculations, the transfer is mediated by the molecular analogue of a Kondo bound state well known from solid state physics of mixed-valence rare-earth compounds. We believe this is quite realistic, since localized d orbitals of the transition metal ions could function as an Anderson impurity embedded in a reservoir of rather delocalized molecular orbitals of the intercalator ligands and DNA pi orbitals. The effective Anderson model is solved with a physically intuitive variational ansatz as well as with the essentially exact DMRG method. The electronic transition matrix element, which is important because it contains the donor-acceptor distance dependence, is obtained with the Mulliken-Hush algorithm as well as from Born-Oppenheimer potential energy surfaces. Our possible explanation of long-range electron transfer is put in context to other more conventional mechanisms which also could lead to similar behavior. Another important issue of DNA is its possible use for nano-technology. Although DNA's mechanical properties are excellent, the question whether it can be conducting and be used for nano-wires is highly controversial. Experimentally, DNA shows conducting, semi-conducting and insulating properties. Motivated by these wide ranging experimental results on the conductivity of DNA, we have

  17. 75 FR 3463 - Cross-Media Electronic Reporting Rule State Authorized Program Revision Approval: State of North...

    Federal Register 2010, 2011, 2012, 2013, 2014

    2010-01-21

    ... AGENCY Cross-Media Electronic Reporting Rule State Authorized Program Revision Approval: State of North...'s approval, under regulations for Cross-Media Electronic Reporting, of the State of North Carolina's..., the final Cross-Media Electronic Reporting Rule (CROMERR) was published in the Federal Register (70...

  18. 75 FR 1617 - Cross-Media Electronic Reporting Rule State Authorized Program Revision Approval: State of New York

    Federal Register 2010, 2011, 2012, 2013, 2014

    2010-01-12

    ... AGENCY Cross-Media Electronic Reporting Rule State Authorized Program Revision Approval: State of New...'s approval, under regulations for Cross-Media Electronic Reporting, of the State of New York's..., the final Cross-Media Electronic Reporting Rule (CROMERR) was published in the Federal Register (70...

  19. Exploring the electronic states of iodocarbyne: a theoretical contribution.

    PubMed

    Alves, Tiago Vinicius; Ornellas, Fernando R

    2014-05-28

    A manifold of electronic states correlating with the two lowest-lying dissociation channels of the iodocarbyne (CI) species is theoretically characterized for the first time in the literature. A contrast between the Λ + S and the relativistic (Ω) descriptions clearly shows the effect of perturbations on electronic states above 20 000 cm(-1) and the potential difficulties to detect them experimentally. For the bound states, spectroscopic parameters were evaluated, as well as the dipole moment functions. Similarly to CO, the polarity predicted for this iodocarbyne is C(δ-)I(δ+); as illustrated in the text, this is also the case for the other halocarbynes. As a potential mechanism for the experimental spectroscopic characterization of CI, we suggest the radiative association between C and I atoms, with light emitted in the red region of the visible spectra. Transition probabilities were also evaluated predicting very weak intensities. For the states 1/2(II) and 3/2(II), we have estimated radiative lifetimes of 7.1 and 714 ms, respectively.

  20. Single electron probes of fractional quantum hall states

    NASA Astrophysics Data System (ADS)

    Venkatachalam, Vivek

    When electrons are confined to a two dimensional layer with a perpendicular applied magnetic field, such that the ratio of electrons to flux quanta (nu) is a small integer or simple rational value, these electrons condense into remarkable new phases of matter that are strikingly different from the metallic electron gas that exists in the absence of a magnetic field. These phases, called integer or fractional quantum Hall (IQH or FQH) states, appear to be conventional insulators in their bulk, but behave as a dissipationless metal along their edge. Furthermore, electrical measurements of such a system are largely insensitive to the detailed geometry of how the system is contacted or even how large the system is... only the order in which contacts are made appears to matter. This insensitivity to local geometry has since appeared in a number of other two and three dimensional systems, earning them the classification of "topological insulators" and prompting an enormous experimental and theoretical effort to understand their properties and perhaps manipulate these properties to create robust quantum information processors. The focus of this thesis will be two experiments designed to elucidate remarkable properties of the metallic edge and insulating bulk of certain FQH systems. To study such systems, we can use mesoscopic devices known as single electron transistors (SETs). These devices operate by watching single electrons hop into and out of a confining box and into a nearby wire (for measurement). If it is initially unfavorable for an electron to leave the box, it can be made favorable by bringing another charge nearby, modifying the energy of the confined electron and pushing it out of the box and into the nearby wire. In this way, the SET can measure nearby charges. Alternatively, we can heat up the nearby wire to make it easier for electrons to enter and leave the box. In this way, the SET is a sensitive thermometer. First, by operating the SET as an

  1. Squeezed states of electrons and transitions of the density of states

    NASA Technical Reports Server (NTRS)

    Lee, Seung Joo; Um, Chung IN

    1993-01-01

    Electron systems which have low dimensional properties have been constructed by squeezing the motion in zero, one, or two-directions. An isolated quantum dot is modeled by a potential box with delta-profiled, penetrable potential walls embedded in a large outer box with infinitely high potential walls which represent the world function with respect to vacuum. We show the smooth crossover of the density of states from the three-dimensional to the quasi-zero dimensional electron gas.

  2. Electronic excited states and relaxation dynamics in polymer heterojunction systems

    NASA Astrophysics Data System (ADS)

    Ramon, John Glenn Santos

    , we examine the effect of the nanoscale interfacial morphology and solvation on the electronic excited states of TFB/F8BT. Here, we employ time-dependent density functional theory (TD-DFT) to investigate the relevant excited states of two stacking configurations. We show that the calculated states agree with the excited states responsible for the experimentally observed emission peaks and that these states are blue shifted relative to those of the isolated chain. Furthermore, slight lateral shifts in the stacking orientation not only shift the excited state energies; more importantly, they alter the nature of these states altogether. Lastly, we see that solvation greatly stabilizes the charge-transfer states.

  3. On the Electron Gas Heat Capacity in Undergraduate Solid State

    NASA Astrophysics Data System (ADS)

    Hasbun, Javier

    2013-03-01

    In undergraduate solid state physics the electronic energy, Uel, is calculated through the Fermi distribution function while the energy is weighted with the density of states. The electronic heat capacity is the derivative of the electronic energy with respect to temperature. Through this process, it is possible to obtain a low temperature approximation for the heat capacity, Cel that's proportional to the temperature. It is of interest to do a numerical calculation of Uel from which the numerical Cel is extracted. However, the result obtained, while agreeing with the low temperature approximation, has a slope that's substantially different. The disagreement appears large as the temperature is increased from zero K. Here we show that the reason has to do with the constancy of the Fermi level. By including the self consistent behavior of the chemical potential, the deviation from zero Kelvin is much improved and the result seems to make better sense. The lesson learned is significant enough to be of great pedagogical importance as regards the heat capacity calculation and the behavior of the chemical potential with temperature.

  4. Efficient numerical simulation of electron states in quantum wires

    NASA Technical Reports Server (NTRS)

    Kerkhoven, Thomas; Galick, Albert T.; Ravaioli, Umberto; Arends, John H.; Saad, Youcef

    1990-01-01

    A new algorithm is presented for the numerical simulation of electrons in a quantum wire as described by a two-dimensional eigenvalue problem for Schroedinger's equation coupled with Poisson's equation. Initially, the algorithm employs an underrelaxed fixed point iteration to generate an approximation which is reasonably close to the solution. Subsequently, this approximate solution is employed as an initial guess for a Jacobian-free implementation of an approximate Newton method. In this manner the nonlinearity in the model is dealt with effectively. The effectiveness of this approach is demonstrated in a set of numerical experiments which study the electron states on the cross section of a quantum wire structure based on III-V semiconductors at 4.2 and 77 K.

  5. Invisible Electronic States and Their Dynamics Revealed by Perturbations

    NASA Astrophysics Data System (ADS)

    Merer, Anthony J.

    2011-06-01

    Sooner or later everyone working in the field of spectroscopy encounters perturbations. These can range in size from a small shift of a single rotational level to total destruction of the vibrational and rotational patterns of an electronic state. To some workers perturbations are a source of terror, but to others they are the most fascinating features of molecular spectra, because they give information about molecular dynamics, and about states that would otherwise be invisible as a result of unfavorable selection rules. An example of the latter is the essentially complete characterization of the tilde{b}^3A_2 state of SO_2 from the vibronic perturbations it causes in the tilde{a}^3B_1 state. The S_1-trans state of acetylene is a beautiful example of dynamics in action. The level patterns of the three bending vibrations change dramatically with increasing vibrational excitation as a result of the vibrational angular momentum and the approach to the isomerization barrier. Several vibrational levels of the S_1-cis isomer, previously thought to be unobservable, can now be assigned. They obtain their intensity through interactions with nearby levels of the trans isomer.

  6. The electronic states of 2-furanmethanol (furfuryl alcohol) studied by photon absorption and electron impact spectroscopies

    NASA Astrophysics Data System (ADS)

    Giuliani, A.; Walker, I. C.; Delwiche, J.; Hoffmann, S. V.; Limão-Vieira, P.; Mason, N. J.; Heyne, B.; Hoebeke, M.; Hubin-Franskin, M.-J.

    2003-10-01

    The photoelectron spectrum of 2-furanmethanol (furfuryl alcohol) has been measured for ionization energies between 8 and 11.2 eV and the first three ionization bands assigned to π3, π2, and no ionizations in order of increasing binding energy. The photoabsorption spectrum has been recorded in the gas phase using both a synchrotron radiation source (5-9.91 eV, 248-125 nm) and electron energy-loss spectroscopy under electric-dipole conditions (5-10.9 eV, 248-90 nm). The (UV) absorption spectrum has also been recorded in solution (4.2-6.36 eV, 292-195 nm). The electronic excitation spectrum appears to be dominated by transitions between π and π* orbitals in the aromatic ring, leading to the conclusion that the frontier molecular orbitals of furan are affected only slightly on replacement of a H atom by the -CH2OH group. Additional experiments investigating electron impact at near-threshold energies have revealed two low-lying triplet states and at least one electron/molecule shape resonance. Dissociative electron attachment also shows to be widespread in furfuryl alcohol.

  7. Direct Imaging of Electron States in Open Quantum Dots

    NASA Astrophysics Data System (ADS)

    Aoki, N.; Brunner, R.; Burke, A. M.; Akis, R.; Meisels, R.; Ferry, D. K.; Ochiai, Y.

    2012-03-01

    We use scanning gate microscopy to probe the ballistic motion of electrons within an open GaAs/AlGaAs quantum dot. Conductance maps are recorded by scanning a biased tip over the open quantum dot while a magnetic field is applied. We show that, for specific magnetic fields, the measured conductance images resemble the classical transmitted and backscattered trajectories and their quantum mechanical analogue. In addition, we prove experimentally, with this direct measurement technique, the existence of pointer states. The demonstrated direct imaging technique is essential for the fundamental understanding of wave function scarring and quantum decoherence theory.

  8. Electronic states of InSe/GaSe superlattice

    NASA Astrophysics Data System (ADS)

    Erkoç, Ş.; Allahverdi, K.; Ibrahim, Z.

    1994-06-01

    Analysis of recent publications revealed an increasing interest in epitaxial growth of InSe/GaSe superlattice. Within the effective mass theory we carried out self-consistent calculations of the confined and itinerant electronic states, potential profile and charge density distribution of InSe/GaSe superlattice, where the InSe layers are the well and the GaSe layers the barrier. Calculations were performed for three types of doping: uniform, modulated in the well, and modulated in the barrier. It has been found that the Coulomb interaction in the well and barrier forces the formation of localized states in the barrier region. The possibility of an insulator-metal transition in InSe/GaSe superlattice is predicted for modulation doping in the barrier and for a doping level n = 10 19cm-3. A decrease of the barrier height has been found for modulation doping in the well.

  9. 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.

  10. Semiclassical dynamics of electron wave packet states with phase vortices.

    PubMed

    Bliokh, Konstantin Yu; Bliokh, Yury P; Savel'ev, Sergey; Nori, Franco

    2007-11-09

    We consider semiclassical higher-order wave packet solutions of the Schrödinger equation with phase vortices. The vortex line is aligned with the propagation direction, and the wave packet carries a well-defined orbital angular momentum (OAM) variant Planck's over 2pil (l is the vortex strength) along its main linear momentum. The probability current coils around the momentum in such OAM states of electrons. In an electric field, these states evolve like massless particles with spin l. The magnetic-monopole Berry curvature appears in momentum space, which results in a spin-orbit-type interaction and a Berry/Magnus transverse force acting on the wave packet. This brings about the OAM Hall effect. In a magnetic field, there is a Zeeman interaction, which, can lead to more complicated dynamics.

  11. Detection of pulsed neutrons with solid-state electronics

    NASA Astrophysics Data System (ADS)

    Chatzakis, J.; Rigakis, I.; Hassan, S. M.; Clark, E. L.; Lee, P.

    2016-09-01

    Measurements of the spatial and time-resolved characteristics of pulsed neutron sources require large area detection materials and fast circuitry that can process the electronic pulses readout from the active region of the detector. In this paper, we present a solid-state detector based on the nuclear activation of materials by neutrons, and the detection of the secondary particle emission of the generated radionuclides’ decay. The detector utilizes a microcontroller that communicates using a modified SPI protocol. A solid-state, pulse shaping filter follows a charge amplifier, and it is designed as an inexpensive, low-noise solution for measuring pulses measured by a digital counter. An imaging detector can also be made by using an array of these detectors. The system can communicate with an interface unit and pass an image to a personal computer.

  12. Semiclassical Dynamics of Electron Wave Packet States with Phase Vortices

    SciTech Connect

    Bliokh, Konstantin Yu.; Bliokh, Yury P.; Savel'ev, Sergey; Nori, Franco

    2007-11-09

    We consider semiclassical higher-order wave packet solutions of the Schroedinger equation with phase vortices. The vortex line is aligned with the propagation direction, and the wave packet carries a well-defined orbital angular momentum (OAM) ({Dirac_h}/2{pi})l (l is the vortex strength) along its main linear momentum. The probability current coils around the momentum in such OAM states of electrons. In an electric field, these states evolve like massless particles with spin l. The magnetic-monopole Berry curvature appears in momentum space, which results in a spin-orbit-type interaction and a Berry/Magnus transverse force acting on the wave packet. This brings about the OAM Hall effect. In a magnetic field, there is a Zeeman interaction, which, can lead to more complicated dynamics.

  13. Modeling the high-energy electronic state manifold of adenine: Calibration for nonlinear electronic spectroscopy

    SciTech Connect

    Nenov, Artur Giussani, Angelo; Segarra-Martí, Javier; Jaiswal, Vishal K.; Rivalta, Ivan; Cerullo, Giulio; Mukamel, Shaul; Garavelli, Marco E-mail: marco.garavelli@ens-lyon.fr

    2015-06-07

    Pump-probe electronic spectroscopy using femtosecond laser pulses has evolved into a standard tool for tracking ultrafast excited state dynamics. Its two-dimensional (2D) counterpart is becoming an increasingly available and promising technique for resolving many of the limitations of pump-probe caused by spectral congestion. The ability to simulate pump-probe and 2D spectra from ab initio computations would allow one to link mechanistic observables like molecular motions and the making/breaking of chemical bonds to experimental observables like excited state lifetimes and quantum yields. From a theoretical standpoint, the characterization of the electronic transitions in the visible (Vis)/ultraviolet (UV), which are excited via the interaction of a molecular system with the incoming pump/probe pulses, translates into the determination of a computationally challenging number of excited states (going over 100) even for small/medium sized systems. A protocol is therefore required to evaluate the fluctuations of spectral properties like transition energies and dipole moments as a function of the computational parameters and to estimate the effect of these fluctuations on the transient spectral appearance. In the present contribution such a protocol is presented within the framework of complete and restricted active space self-consistent field theory and its second-order perturbation theory extensions. The electronic excited states of adenine have been carefully characterized through a previously presented computational recipe [Nenov et al., Comput. Theor. Chem. 1040–1041, 295-303 (2014)]. A wise reduction of the level of theory has then been performed in order to obtain a computationally less demanding approach that is still able to reproduce the characteristic features of the reference data. Foreseeing the potentiality of 2D electronic spectroscopy to track polynucleotide ground and excited state dynamics, and in particular its expected ability to provide

  14. 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.

  15. Benchmarking electronic-state excitation cross sections for electron-N{sub 2} collisions

    SciTech Connect

    Kato, Hidetoshi; Suzuki, Daisuke; Ohkawa, Mizuha; Hoshino, Masamitsu; Tanaka, Hiroshi; Campbell, Laurence; Brunger, Michael J.

    2010-04-15

    We report differential cross sections for electron impact excitation of the a {sup 1{Pi}}{sub g}, C {sup 3{Pi}}{sub u}, E {sup 3{Sigma}}{sub g}{sup +}, a{sup ''} {sup 1{Sigma}}{sub g}{sup +}, b {sup 1{Pi}}{sub u}, c{sub 3} {sup 1{Pi}}{sub u}, o{sub 3} {sup 1{Pi}}{sub u}, b{sup '} {sup 1{Sigma}}{sub u}{sup +}, c{sub 4}{sup '} {sup 1{Sigma}}{sub u}{sup +}, G {sup 3{Pi}}{sub u}, and F {sup 3{Pi}}{sub u} electronic states in N{sub 2}. The incident electron energies are 20, 30, and 40 eV, while the scattered electron angles are 10 deg. and 20 deg. These kinematic conditions were specifically targeted in order to try and shed new light on the worrying discrepancies that exist in the literature for the a {sup 1{Pi}}{sub g}, C {sup 3{Pi}}{sub u}, E {sup 3{Sigma}}{sub g}{sup +}, and a{sup ''} {sup 1{Sigma}}{sub g}{sup +} cross sections, and in general the present measurements confirm that those from the more recent results of the University of California, Fullerton, and the Jet Propulsion Laboratory [M. A. Khakoo, P. V. Johnson, I. Ozkay, P. Yan, S. Trajmar, and I. Kanik, Phys. Rev. A 71, 062703 (2005); C. P. Malone, P. V. Johnson, I. Kanik, B. Ajdari, and M. A. Khakoo, Phys. Rev. A 79, 032704 (2009)] are reliable. In addition, we provide a rigorous cross-check for the remaining seven electronic states, where the only recent comprehensive study is from Khakoo and colleagues [Phys. Rev. A 77, 012704 (2008)]. Here, however, some of those cross sections are confirmed and others are not, suggesting that further work is still needed.

  16. Interaction of Pd electron states with adsorbed hydrogen

    NASA Astrophysics Data System (ADS)

    Solov'ev, S. M.; Pettenkofer, C.; Pronin, I. I.; Potekhina, N. D.; Petrov, V. N.

    2013-02-01

    Investigations of electrons excited into image states (IS) of Pd clusters and their interaction with adsorbed hydrogen using photoelectron (PE) spectroscopy with synchrotron radiation is presented. Pd clusters were deposited on pyrolytic graphite surfaces which were used as inert substrates. PE spectra measured for Pd clusters at low photon energies show additional peaks at energies of ~ 4.7 and 5.25 eV that corresponds to Pd image states at energies EIS - Evac ≈ - 0.75 ± 0.1 eV and EIS - Evac ≈ - 0.2 ± 0.1 eV. After hydrogen adsorption on graphite with Pd clusters the H-induced features: positive peaks at energy - 2 eV, - 3.5 eV, - 7 eV and a small negative peak at - 4.6 eV, were observed in the valence band spectra of Pd below EF. While the peaks at - 3.5 eV and - 2 eV are the result of the formation of H-induced states in the SBZ the - 7 eV peak is due to strong interaction of Pd clusters with hydrogen producing a H―Pd bonding adsorbate state. It is proposed that a charge transfer from IS2 to Pd-H bond dominates over the H- anion neutralization via transfer of excess charge from H- to IS1.

  17. Electronic States of IC60BA and PC71BM

    NASA Astrophysics Data System (ADS)

    Sheng, Chun-Qi; Wang, Peng; Shen, Ying; Li, Wen-Jie; Zhang, Wen-Hua; Zhu, Jun-Fa; Lai, Guo-Qiao; Li, Hong-Nian

    2013-11-01

    We investigate the electronic states of IC60BA and PC71BM using first-principles calculations and photoelectron spectroscopy (PES) measurements. The energy level structures for all possible isomers are reported and compared with those of C60, C70 and PC61BM. The attachment of the side chains can raise the LUMO energies and decrease the HOMO-LUMO gaps, and thus helps to increase the power-conversion efficiency of bulk heterojunction solar cells. In the PES studies, we prepared IC60BA and PC71BM films on Si:H(111) substrates to construct adsorbate/substrate interfaces describable with the integer charge-transfer (ICT) model. Successful measurements then revealed that one of the most important material properties for an electron acceptor, the energy of the negative integer charge-transfer state (EICT-), is 4.31 eV below the vacuum level for PC71BM. The EICT- of IC60BA is smaller than 4.14 eV.

  18. Photodissociation of CCH: classical trajectory calculations involving seven electronic states.

    PubMed

    Apaydin, Gökşin; Fink, William H; Jackson, William M

    2004-11-15

    The photodissociation dynamics of ethynyl radical, C(2)H, involving seven electronic states is studied by classical trajectory calculations. Initial values of the trajectories are selected based on relative absorption intensities calculated by Mebel et al. The energies and the derivatives are interpolated by three-dimensional cubic spline interpolator using an extended data pool. Mean square errors and standard deviations in interpolation of energies for 450 data points are found to be in the range 3.1 x 10(-6)-1.4 x 10(-5) and 1.7 x 10(-3)-3.8 x 10(-3) hartrees, respectively. The photofragments of C(2) and H are produced mainly in the X (1)Sigma(g) (+), a (3)Pi(u), b (3)Sigma(g) (-), c (3)Sigma(u) (+), A (1)Pi(u), B (1)Delta(g) electronic states of C(2) as product. The avoided crossings do not appear to be in the main dissociation pathways. The internal distributions are in good accord with the experimental results where comparison is possible, suggesting that the fragmentation mechanism of C(2)H(2) into C(2) and H is a two step process involving C(2)H radical as an intermediate with a life time long enough to allow complete collection of the phase space in the experiments.

  19. Photodissociation of CCH: Classical trajectory calculations involving seven electronic states

    NASA Astrophysics Data System (ADS)

    Apaydın, Gökşin; Fink, William H.; Jackson, William M.

    2004-11-01

    The photodissociation dynamics of ethynyl radical, C2H, involving seven electronic states is studied by classical trajectory calculations. Initial values of the trajectories are selected based on relative absorption intensities calculated by Mebel et al. The energies and the derivatives are interpolated by three-dimensional cubic spline interpolator using an extended data pool. Mean square errors and standard deviations in interpolation of energies for 450 data points are found to be in the range 3.1×10-6-1.4×10-5 and 1.7×10-3-3.8×10-3 hartrees, respectively. The photofragments of C2 and H are produced mainly in the X 1Σg+, a 3Πu, b 3Σg-, c 3Σu+, A 1Πu, B 1Δg electronic states of C2 as product. The avoided crossings do not appear to be in the main dissociation pathways. The internal distributions are in good accord with the experimental results where comparison is possible, suggesting that the fragmentation mechanism of C2H2 into C2 and H is a two step process involving C2H radical as an intermediate with a life time long enough to allow complete collection of the phase space in the experiments.

  20. Electronic states and spin-orbit splitting of lanthanum dimer

    NASA Astrophysics Data System (ADS)

    Liu, Yang; Wu, Lu; Zhang, Chang-Hua; Krasnokutski, Serge A.; Yang, Dong-Sheng

    2011-07-01

    Lanthanum dimer (La2) was studied by mass-analyzed threshold ionization (MATI) spectroscopy and a series of multi-configuration ab initio calculations. The MATI spectrum exhibits three band systems originating from ionization of the neutral ground electronic state, and each system shows vibrational frequencies of the neutral molecule and singly charged cation. The three ionization processes are La2+ (a2∑g+) ← La2 (X1∑g+), La2+ (b2Π3/2, u) ← La2 (X1∑g+), and La2+ (b2Π1/2, u) ← La2 (X1∑g+), with the ionization energies of 39 046, 40 314, and 40 864 cm-1, respectively. The vibrational frequency of the X1Σg+ state is 207 cm-1, and those of the a2Σg+, b2Π3/2, u and b2Π1/2, u are 235.7, 242.2, and 240 cm-1. While X1Σg+ is the ground state of the neutral molecule, a2Σg+ and b2Πu are calculated to be the excited states of the cation. The spin-orbit splitting in the b2Πu ion is 550 cm-1. An X4Σg- state of La2+ was predicted by theory, but not observed by the experiment. The determination of a singlet ground state of La2 shows that lanthanum behaves differently from scandium and yttrium.

  1. Electronic spin state of iron in lower mantle perovskite

    SciTech Connect

    Li, J.; Struzhkin, V.; Mao, H.-k.; Shu, J.; Hemley, R.; Fei, Y.; Mysen, B.; Dera, P.; Parapenka, V.; Shen, G.

    2010-11-16

    The electronic spin state of iron in lower mantle perovskite is one of the fundamental parameters that governs the physics and chemistry of the most voluminous and massive shell in the Earth. We present experimental evidence for spin-pairing transition in aluminum-bearing silicate perovskite (Mg,Fe)(Si,Al)O{sub 3} under the lower mantle pressures. Our results demonstrate that as pressure increases, iron in perovskite transforms gradually from the initial high-spin state toward the final low-spin state. At 100 GPa, both aluminum-free and aluminum-bearing samples exhibit a mixed spin state. The residual magnetic moment in the aluminum-bearing perovskite is significantly higher than that in its aluminum-free counterpart. The observed spin evolution with pressure can be explained by the presence of multiple iron species and the occurrence of partial spin-paring transitions in the perovskite. Pressure-induced spin-pairing transitions in the perovskite would have important bearing on the magnetic, thermoelastic, and transport properties of the lower mantle, and on the distribution of iron in the Earth's interior. The lower mantle constitutes more than half of the Earth's interior by volume (1), and it is believed to consist predominantly (80-100%) of (Mg,Fe)(Si,Al)O{sub 3} perovskite (hereafter called perovskite), with up to 20% (Mg,Fe)O ferropericlase (2). The electronic spin state of iron has direct influence on the physical properties and chemical behavior of its host phase. Hence, knowledge on the spin state of iron is important for the interpretation of seismic observations, geochemical modeling, and geodynamic simulation of the Earth's deep interior (3, 4). Crystal field theory (4, 5) and band theory (6) predicted that a high-spin to low-spin transition would occur as a result of compression. To date, no experimental data exist on the spin sate of iron in Al-bearing perovskite. To detect possible spinpairing transition of iron in perovskite under the lower mantle

  2. Differential cross sections for electron-impact excitation of the electronic states of pyrimidine

    NASA Astrophysics Data System (ADS)

    Brunger, Michael; Jones, Darryl; Bellm, Susan

    2012-06-01

    Pyrimidine (C4N2H4) is an important molecule, as it forms the basis of larger biomolecules, such as the DNA bases thymine, cytosine and uracil. There is a pressing demand for low-energy electron scattering data from such biological analogs in order to model radiation induced damage [1]. We therefore present the first measurements for absolute differential cross section data for low-energy electron-impact excitation of the electronic states of pyrimidine. The present measurements were performed using a crossed-beam apparatus [2] for incident electron energies ranging between 15 to 50eV while covering a 10 to 90^o angular range. Here the absolute scale has been determined through a normalisation to the recently measured elastic scattering differential cross section data for pyrimidine [3]. [1] F. Ferreira da Silva, D. Almeida, G. Martins, A. R. Milosavljevic, B. P. Marinkovic, S. V. Hoffmann, N. J. Mason, Y. Nunes, G. Garcia and P. Limao-Vieira, Phys Chem Chem Phys 12, 6717 (2010). [2] M. J. Brunger and P. J. O. Teubner, Phys Rev A 41, 1413 (1990). [3] P. Palihawadana, J. Sullivan, M. Brunger, C. Winstead, V. McKoy, G. Garcia, F. Blanco and S. Buckman, Phys Rev A 84, 062702 (2011).

  3. Hamiltonian of a many-electron system with single-electron and electron-pair states in a two-dimensional periodic potential

    NASA Astrophysics Data System (ADS)

    Hai, Guo-Qiang; Peeters, François M.

    2015-01-01

    Based on the metastable electron-pair energy band in a two-dimensional (2D) periodic potential obtained previously by Hai and Castelano [J. Phys.: Condens. Matter 26, 115502 (2014)], we present in this work a Hamiltonian of many electrons consisting of single electrons and electron pairs in the 2D system. The electron-pair states are metastable of energies higher than those of the single-electron states at low electron density. We assume two different scenarios for the single-electron band. When it is considered as the lowest conduction band of a crystal, we compare the obtained Hamiltonian with the phenomenological model Hamiltonian of a boson-fermion mixture proposed by Friedberg and Lee [Phys. Rev. B 40, 6745 (1989)]. Single-electron-electron-pair and electron-pair-electron-pair interaction terms appear in our Hamiltonian and the interaction potentials can be determined from the electron-electron Coulomb interactions. When we consider the single-electron band as the highest valence band of a crystal, we show that holes in this valence band are important for stabilization of the electron-pair states in the system.

  4. Evaluating Electronic Couplings for Excited State Charge Transfer Based on Maximum Occupation Method ΔSCF Quasi-Adiabatic States.

    PubMed

    Liu, Junzi; Zhang, Yong; Bao, Peng; Yi, Yuanping

    2017-02-14

    Electronic couplings of charge-transfer states with the ground state and localized excited states at the donor/acceptor interface are crucial parameters for controlling the dynamics of exciton dissociation and charge recombination processes in organic solar cells. Here we propose a quasi-adiabatic state approach to evaluate electronic couplings through combining maximum occupation method (mom)-ΔSCF and state diabatization schemes. Compared with time-dependent density functional theory (TDDFT) using global hybrid functional, mom-ΔSCF is superior to estimate the excitation energies of charge-transfer states; moreover it can also provide good excited electronic state for property calculation. Our approach is hence reliable to evaluate electronic couplings for excited state electron transfer processes, which is demonstrated by calculations on a typical organic photovoltaic system, oligothiophene/perylenediimide complex.

  5. Electron impact excitation and assignment of the low-lying electronic states of CO2

    NASA Technical Reports Server (NTRS)

    Hall, R. I.; Trajmar, S.

    1973-01-01

    Electron scattering spectra of CO2 are reported in the 7 to 10 eV energy-loss range, at energies of 0.2, 0.35, 0.6, 0.7, and 7.0 eV above threshold, and at a scattering angle of 90 deg. Several new distinct overlapping continua with weak, diffuse bands superimposed are observed to lie in this energy-loss range. The experimental spectra are discussed in the light of recent ab initio configuration-interaction calculations of the vertical transition energies of CO2. The experimental spectra are shown to be consistent with the excitation states of CO2.

  6. Ultrafast excited state relaxation dynamics of electron deficient porphyrins: Conformational and electronic factors

    NASA Astrophysics Data System (ADS)

    Okhrimenko, Albert N.

    Metallo-tetrapyrroles (MTP) are highly stable macrocyclic pi-systems that display interesting properties that make them potential candidates for various applications. Among these applications are optoelectronics, magnetic materials, photoconductive materials, non-linear optical materials and photo tumor therapeutic drugs. These applications are generally related to their high stability and efficient light absorption ability in the visible and near-infrared region of the optical spectrum. Metallo porphyrins are well known and widely studied representatives of metallotetrapyrroles. Electron deficient substituents in the meso positions are well known to greatly influence the interaction between the metal d-orbitals and the nitrogen orbitals of the tetrapyrrole macrocycle. In this work, a series of electron deficient porphyrins has been studied to gain some knowledge about the change in the excited state dynamics with structural and electronic modifications. Among these porphyrins is nickel and iron modified species bearing perfluoro-, perprotio-, p-nitrophenyl- and perfluorophenyl-meso substituents. Ultrafast transient absorption spectrometry has been used as the main research instrument along with other spectroscopic and electrochemical methods. A new technique has been employed to study the photophysical properties of zinc (II) tetraphenylporphine cation radical. It employs a combination of controlled potential coulometry and femtosecond absorption spectrometry. The fast transient lifetime of 17 ps of the pi-cation species originates in very efficient mixing of the a2u HOMO cation orbital that places electronic density mainly on pyrrolic nitrogens and metal d-orbitals. That explains the lack of any emission of the cationic species. This non-radiative decay process might elucidate the processes taking place in photosynthetic systems when electron is removed from porphyrinic moiety and the hole is produced. In this work zinc(II) meso-tetraphenylporphine radial cation

  7. Electron excitation from ground state to first excited state: Bohmian mechanics method

    NASA Astrophysics Data System (ADS)

    Yang, Song; Shuang, Zhao; Fu-Ming, Guo; Yu-Jun, Yang; Su-Yu, Li

    2016-03-01

    The excitation process of electrons from the ground state to the first excited state via the resonant laser pulse is investigated by the Bohmian mechanics method. It is found that the Bohmian particles far away from the nucleus are easier to be excited and are excited firstly, while the Bohmian particles in the ground state is subject to a strong quantum force at a certain moment, being excited to the first excited state instantaneously. A detailed analysis for one of the trajectories is made, and finally we present the space and energy distribution of 2000 Bohmian particles at several typical instants and analyze their dynamical process at these moments. Project supported by the Doctoral Research Start-up Funding of Northeast Dianli University, China (Grant No. BSJXM-201332), the National Natural Science Foundation of China (Grant Nos. 11547114, 11534004, 11474129, 11274141, 11447192, and 11304116), and the Graduate Innovation Fund of Jilin University, China (Grant No. 2015091).

  8. Heavy metal phosphate nanophases in silica: influence of radiolysis probed via f-electron state properties

    SciTech Connect

    Beitz, James V. . E-mail: beitz@anl.gov; Williams, C.W.; Hong, K.-S.; Liu, G.K.

    2005-02-15

    We have assessed the feasibility of carrying out time- and wavelength-resolved laser-induced fluorescence measurements of radiation damage in glassy silica. The consequences of alpha decay of Es-253 in LaPO{sub 4} nanophases embedded in silica were probed based on excitation of 5f states of Cm{sup 3+}, Bk{sup 3+}, and Es{sup 3+} ions. The recorded emission spectra and luminescence decays showed that alpha decay of Es-253 ejected Bk-249 decay daughter ions into the surrounding silica and created radiation damage within the LaPO{sub 4} nanophases. This conclusion is consistent with predictions of an ion transport code commonly used to model ion implantation. Luminescence from the {sup 6}D{sub 7/2} state of Cm{sup 3+}was used as an internal standard. Ion-ion energy transfer dominated the dynamics of the observed emitting 5f states and strongly influenced the intensity of observed spectra. In appropriate sample materials, laser-induced fluorescence provides a powerful method for fundamental investigation of alpha-induced radiation damage in silica.

  9. Electronic states of cuprate superconductors containing halogen or carbon

    NASA Astrophysics Data System (ADS)

    Tohiyama, Takami; Shibata, Yasumasa; Maekawa, Sadamichi

    1996-12-01

    The electronic states of the halo-oxocuprate and oxycarbonate superconductors are examined by means of the ionic and cluster models. The oxycarbonates examined contain the CO3 group on one side of the CuO2 plane. The superconducting critical temperature Tc is found to be correlated with the stability of the Zhang-Rice local singlet in the CuO2 plane. The stability is generally determined by two factors: (1) the energy-level separation between apical ion and in-plane oxygen and (2) the hybridization between apical pz and in-plane orbitals. The former is dominant for the oxycarbonates. It is also found that the CO3 group has no effect on the stabilization. For the halo-oxocuprates, the latter is crucial to stabilize the singlet.

  10. Steady-state and transient electronic dynamics in granular metals

    NASA Astrophysics Data System (ADS)

    Chen, Wei

    In this thesis two very different approaches, steady state and transient, are taken to help understand the electronic dynamics in the nanogranular Cux(SiO2)1-x composite thin films. The electrical conductivity and thermopower are measured from 2 K to room temperature with the Cu volume fraction x varying from 1 down to 0.43. At low temperatures, a T dependence of the electrical conductivity is observed well above the percolation threshold due to the disorder-enhanced electron-electron interaction and as the metal-insulator transition is approached, the electrical conductivity assumes a T1/3 dependence. The thermopower is found to be small and rather insensitive to the degree of disorder in the system. It varies linearly with temperatures at both low and high temperatures. Annealing has considerable influence to the behavior of the electrical conductivity while introducing little changes to the thermopower. Femtosecond pump-probe experiments were performed on a series of Cu x(SiO2)1-x composite films with volume fraction x varying from 0.7 to 1.0 to study the reflectivity change DeltaR/R as a function of composition and temperature. It is discovered that DeltaR/R undergoes drastic changes as the metal content is lowered. Very small amount of SiO 2 inclusions can start to result in qualitatively different Delta R/R behavior from pure Cu. Changes in the dielectric constant of Cu are investigated and possible explanations for the DeltaR/R behaviors in the composite films are discussed.

  11. Electron transport in multiterminal networks of Majorana bound states

    NASA Astrophysics Data System (ADS)

    Weithofer, Luzie; Recher, Patrik; Schmidt, Thomas L.

    2014-11-01

    We investigate electron transport through multiterminal networks hosting Majorana bound states (MBS) in the framework of full counting statistics. In particular, we apply our general results to T-shaped junctions of two Majorana nanowires. When the wires are in the topologically nontrivial regime, three MBS are localized near the outer ends of the wires, while one MBS is localized near the crossing point, and when the lengths of the wires are finite adjacent MBS can overlap. We propose a combination of current and cross-correlation measurements to reveal the predicted coupling of four Majoranas in a topological T junction. Interestingly, we show that the elementary transport processes at the central lead are different compared to the outer leads, giving rise to characteristic nonlocal signatures in electronic transport. We find quantitative agreement between our analytical model and numerical simulations of a tight-binding model. Using the numerical simulations, we discuss the effect of weak disorder on the current and the cross-correlation functions.

  12. Experimental Realization of Nearly Steady-State Toroidal Electron Plasmas

    NASA Astrophysics Data System (ADS)

    Stoneking, M. R.

    2008-11-01

    Non-neutral plasmas are routinely confined in the uniform magnetic field of a Penning-Malmberg trap for arbitrarily long times and approach thermal equilibrium. Theory predicts that dynamically stable and therefore long-lived equilibria exist for non-neutral plasmas confined in the curved, non-uniform field of a toroidal trap, but that ultimately thermal equilibrium states do not exist. On long timescales, the poloidal ExB rotation through the non-uniform toroidal magnetic field leads to magnetic pumping transport. A new experiment has, for the first time, demonstrated the existence of a stable, long-lived (i.e. nearly steady-state) toroidal equilibrium for pure electron plasmas and is poised to observe the magnetic pumping transport mechanism. Electron plasmas with densities of order 10^6 cm-3 are trapped in the Lawrence Non-neutral Torus II for several seconds. LNT II is a high aspect ratio (Ro/a 10), partially toroidal trap (a 270^o arc with Bo=670 G). The m=1 diocotron mode is launched and detected using isolated segments of a fully-sectored conducting boundary and its frequency is used to determine the total trapped charge as a function of time. The observed confinement time ( 3 s) approaches the theoretical limit ( 6 s) set by the magnetic pumping transport mechanism of Crooks and O'Neil. We also present equilibrium modeling and numerical simulation of the toroidal m=1 mode constrained by experimental data. Future work includes the identification of the dominant transport mechanisms via confinement scaling experiments and measurement of the m=2 mode frequency, and development of a strategy for making a transition to fully toroidal confinement. J.P. Marler and M.R. Stoneking, Phys. Rev. Lett. 100, 155001 (2008). S.M. Crooks and T.M. O'Neil, Phys Plamas 3, 2533 (1996).

  13. Final Version: Orbital Specificity in the Unoccupied States of UO2 from Resonant Inverse Photoelectron Spectroscopy

    SciTech Connect

    Tobin, J G; Yu, S W

    2012-03-12

    One of the crucial questions of all actinide electronic structure determinations is the issue of 5f versus 6d character and the distribution of these components across the density of states. Here, a break-though experiment is discussed, which has allowed the direct determination of the U5f and U6d contributions to the unoccupied density of states (UDOS) in Uranium Dioxide. A novel Resonant Inverse Photoelectron (RIPES) and X-ray Emission Spectroscopy (XES) investigation of UO{sub 2} is presented. It is shown that the U5f and U6d components are isolated and identified unambiguously.

  14. 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.

  15. Electron momentum spectroscopy of dimethyl ether taking account of nuclear dynamics in the electronic ground state.

    PubMed

    Morini, Filippo; Watanabe, Noboru; Kojima, Masataka; Deleuze, Michael Simon; Takahashi, Masahiko

    2015-10-07

    The influence of nuclear dynamics in the electronic ground state on the (e,2e) momentum profiles of dimethyl ether has been analyzed using the harmonic analytical quantum mechanical and Born-Oppenheimer molecular dynamics approaches. In spite of fundamental methodological differences, results obtained with both approaches consistently demonstrate that molecular vibrations in the electronic ground state have a most appreciable influence on the momentum profiles associated to the 2b1, 6a1, 4b2, and 1a2 orbitals. Taking this influence into account considerably improves the agreement between theoretical and newly obtained experimental momentum profiles, with improved statistical accuracy. Both approaches point out in particular the most appreciable role which is played by a few specific molecular vibrations of A1, B1, and B2 symmetries, which correspond to C-H stretching and H-C-H bending modes. In line with the Herzberg-Teller principle, the influence of these molecular vibrations on the computed momentum profiles can be unraveled from considerations on the symmetry characteristics of orbitals and their energy spacing.

  16. Electron momentum spectroscopy of dimethyl ether taking account of nuclear dynamics in the electronic ground state

    SciTech Connect

    Morini, Filippo; Deleuze, Michael Simon; Watanabe, Noboru; Kojima, Masataka; Takahashi, Masahiko

    2015-10-07

    The influence of nuclear dynamics in the electronic ground state on the (e,2e) momentum profiles of dimethyl ether has been analyzed using the harmonic analytical quantum mechanical and Born-Oppenheimer molecular dynamics approaches. In spite of fundamental methodological differences, results obtained with both approaches consistently demonstrate that molecular vibrations in the electronic ground state have a most appreciable influence on the momentum profiles associated to the 2b{sub 1}, 6a{sub 1}, 4b{sub 2}, and 1a{sub 2} orbitals. Taking this influence into account considerably improves the agreement between theoretical and newly obtained experimental momentum profiles, with improved statistical accuracy. Both approaches point out in particular the most appreciable role which is played by a few specific molecular vibrations of A{sub 1}, B{sub 1}, and B{sub 2} symmetries, which correspond to C–H stretching and H–C–H bending modes. In line with the Herzberg-Teller principle, the influence of these molecular vibrations on the computed momentum profiles can be unraveled from considerations on the symmetry characteristics of orbitals and their energy spacing.

  17. 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.

  18. 75 FR 983 - Cross-Media Electronic Reporting Rule State Approved Program Revision/Modification Approvals...

    Federal Register 2010, 2011, 2012, 2013, 2014

    2010-01-07

    ... AGENCY Cross-Media Electronic Reporting Rule State Approved Program Revision/Modification Approvals... announces EPA's approval, under regulations for Cross-Media Electronic Reporting, of the State of...@epa.gov . SUPPLEMENTARY INFORMATION: On October 13, 2005, the final Cross-Media Electronic...

  19. 75 FR 69660 - Cross-Media Electronic Reporting Rule State Authorized Program Revision Approval: State of Hawaii

    Federal Register 2010, 2011, 2012, 2013, 2014

    2010-11-15

    ...] [FR Doc No: 2010-28651] ENVIRONMENTAL PROTECTION AGENCY [FRL-9226-9] Cross-Media Electronic Reporting...-Media Electronic Reporting, of the State of Hawaii's request to revise certain of its EPA-authorized...-Media Electronic Reporting Rule (CROMERR) was published in the Federal Register (70 FR 59848)...

  20. Pseudopotential and full-electron DFT calculations of thermodynamic properties of electrons in metals and semiempirical equations of state.

    PubMed

    Levashov, P R; Sin'ko, G V; Smirnov, N A; Minakov, D V; Shemyakin, O P; Khishchenko, K V

    2010-12-22

    In the present work, we compare the thermal contribution of electrons to thermodynamic functions of metals in different models at high densities and electron temperatures. One of the theoretical approaches, the full-potential linear-muffin-tin-orbital method, treats all electrons in the framework of density functional theory (DFT). The other approach, VASP, uses projector-augmented-wave pseudopotentials for the core electrons and considers the valent electrons also in the context of DFT. We analyze the limitations of the pseudopotential approach and compare the DFT results with a finite-temperature Thomas-Fermi model and two semiempirical equations of state.

  1. A combined photoelectron spectroscopy and relativistic ab initio studies of the electronic structures of UFO and UFO(-).

    PubMed

    Roy, Soumendra K; Jian, Tian; Lopez, Gary V; Li, Wei-Li; Su, Jing; Bross, David H; Peterson, Kirk A; Wang, Lai-Sheng; Li, Jun

    2016-02-28

    The observation of the gaseous UFO(-) anion is reported, which is investigated using photoelectron spectroscopy and relativisitic ab initio calculations. Two strong photoelectron bands are observed at low binding energies due to electron detachment from the U-7sσ orbital. Numerous weak detachment bands are also observed due to the strongly correlated U-5f electrons. The electron affinity of UFO is measured to be 1.27(3) eV. High-level relativistic quantum chemical calculations have been carried out on the ground state and many low-lying excited states of UFO to help interpret the photoelectron spectra and understand the electronic structure of UFO. The ground state of UFO(-) is linear with an O-U-F structure and a (3)H4 spectral term derived from a U 7sσ(2)5fφ(1)5fδ(1) electron configuration, whereas the ground state of neutral UFO has a (4)H(7/2) spectral term with a U 7sσ(1)5fφ(1)5fδ(1) electron configuration. Strong electron correlation effects are found in both the anionic and neutral electronic configurations. In the UFO neutral, a high density of electronic states with strong configuration mixing is observed in most of the scalar relativistic and spin-orbit coupled states. The strong electron correlation, state mixing, and spin-orbit coupling of the electronic states make the excited states of UFO very challenging for accurate quantum chemical calculations.

  2. 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.

  3. 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...

  4. 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...

  5. 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...

  6. 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...

  7. Minimal parametrization of an n-electron state

    SciTech Connect

    Kutzelnigg, Werner; Mukherjee, Debashis

    2005-02-01

    The Hamiltonian H for an n-electron system in a finite one-electron basis of dimension m is characterized by d=O(m{sup 4}) matrix elements. The eigenstates of this Hamiltonian - i.e., the full-CI states {psi} - depend, however, on the usually much larger set of N=O(m{sup n}) parameters. One can, nevertheless, write a full-CI state as {psi}=e{sup S}{phi} with {phi} a reference function and S an operator familiar from traditional coupled cluster (TCC) theory. The 'exact' operator S can be expressed (though in an implicit and rather complicated way) in terms of d parameters. An alternative ansatz {psi}=e{sup T}{phi} with T depending in a very simple way on d parameters only (namely, with T having the same structure in Fock space as H) has been studied by Nooijen and by Nakatsuji and been called coupled-cluster with generalized single and double excitations (CCGSD). Nooijen has conjectured that the full-CI equations can be fulfilled with this ansatz. This paper is devoted to a comprehensive analysis of the Nooijen conjecture (NC). Several features make this analysis difficult and even intriguing. (a) One deals with coupled nonlinear systems of equations, for which theorems concerning the existence of their solution are hardly available. (b) There are different possible interpretations of the NC, especially as far as the choice of the reference function {phi} is concerned. (c) There are solutions of the CCGSD equations, for which some elements of T becomes negative infinite, and e{sup T} becomes a projection operator. Such solutions are undesired but difficult to eliminate. We show by direct comparison of the exact wave operator with that of CCGSD theory, for a closed-shell state with {phi} a single Slater determinant, using a perturbation expansion, that CCGSD cannot be exact. This required a reformulation of the CCGSD operator e{sup T} to an equivalent exponential form e{sup R}, with R similar to the S of TCC theory, but with constraints on the cluster amplitudes

  8. 77 FR 58131 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Mississippi

    Federal Register 2010, 2011, 2012, 2013, 2014

    2012-09-19

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Mississippi... . SUPPLEMENTARY INFORMATION: On October 13, 2005, the final Cross-Media Electronic Reporting Rule (CROMERR)...

  9. Separating the Spin States of a Free Electron Beam

    NASA Astrophysics Data System (ADS)

    Rifkin, Neil

    2008-10-01

    In 1922 Otto Stern and Walther Gerlach set out to test the spacial quantization of the electron by passing a beam of neutral silver atoms through a transverse magnetic field. The interaction of the two projections of the electron's magnetic moment with the magnetic field resulted in a splitting of the beam. However, for some sixty years it was generally accepted that the spin of free electrons, and thus their magnetic moment, could not be measured with an experiment similar to that of Stern and Gerlach. The reason being that the lorentz force on charged particles is far greater than the force due to the magnetic moment of the electron, thus blurring any desired results. To reduce the lorentz force, the electrons could be passed through a magnetic field whose gradient is in the direction of the electrons' momentum. This longitudinal Stern-Gerlach device, with a superconducting magnet, could polarize the tails of a low energy electron beam.

  10. 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.

  11. Formation and nonlinear dynamics of the squeezed state of a helical electron beam with additional deceleration

    SciTech Connect

    Egorov, E. N. Koronovskii, A. A.; Kurkin, S. A.; Hramov, A. E.

    2013-11-15

    Results of numerical simulations and analysis of the formation and nonlinear dynamics of the squeezed state of a helical electron beam in a vircator with a magnetron injection gun as an electron source and with additional electron deceleration are presented. The ranges of control parameters where the squeezed state can form in such a system are revealed, and specific features of the system dynamics are analyzed. It is shown that the formation of a squeezed state of a nonrelativistic helical electron beam in a system with electron deceleration is accompanied by low-frequency longitudinal dynamics of the space charge.

  12. Implementation of Inverse Photoelectron Spectroscopy for Measuring the Empty Electronic States of Metal Oxide Surfaces

    DTIC Science & Technology

    2014-11-05

    and initial results on oxidized zirconium have been performed. (a) Papers published in peer-reviewed journals (N/A for none) Enter List of papers...the electronic states of the surface with changes in the photoluminescence spectrum. The results of some of our first experiments on zirconium ...clean” zirconium oxide. The occupied valence electronic states are mainly composed of oxygen 2p electrons. The unoccupied states are zirconium 4d

  13. Two-electron bound states near a Coulomb impurity in gapped graphene

    NASA Astrophysics Data System (ADS)

    De Martino, Alessandro; Egger, Reinhold

    2017-02-01

    We formulate and solve the perhaps simplest two-body bound-state problem for interacting Dirac fermions in two spatial dimensions. A two-body bound state is predicted for gapped graphene monolayers in the presence of weakly repulsive electron-electron interactions and a Coulomb impurity with charge Z e >0 , where the most interesting case corresponds to Z =1 . We introduce a variational Chandrasekhar-Dirac spinor wave function and show the existence of at least one bound state. This state leaves clear signatures accessible by scanning tunneling microscopy. One may thereby obtain direct information about the strength of electron-electron interactions in graphene.

  14. Structural evolution and valence electron-state change during ultra thin silicon-oxide growth

    NASA Astrophysics Data System (ADS)

    Shimizu, A.; Abe, S.; Nakayama, H.; Nishino, T.; Iida, S.

    2000-06-01

    We have studied valence electron-state changes of Si during initial oxidation of Si(111) clean surface, HF-treated Si(001) and Si(111) surfaces by Auger valence electron spectroscopy (AVES). The results showed that the valence electron-state changes during initial oxidation were sensitively reflected in Si[2s,2p,V] (V=3s,3p) AVES spectra and that they depended on both initial surface treatment and surface orientation. The local valence electron-states, local density of states in other words, showed the characteristic-structure evolution depending on the initial surface treatment and surface orientation.

  15. Nonadiabtic electron dynamics in densely quasidegenerate states in highly excited boron cluster

    NASA Astrophysics Data System (ADS)

    Yonehara, Takehiro; Takatsuka, Kazuo

    2016-04-01

    Following the previous study on nonadiabatic reaction dynamics including boron clusters [T. Yonehara and K. Takatsuka, J. Chem. Phys. 137, 22A520 (2012)], we explore deep into highly excited electronic states of the singlet boron cluster (B12) to find the characteristic features of the densely quasi-degenerate electronic state manifold, which undergo very frequent nonadiabatic transitions and thereby intensive electronic state mixing among very many of the relevant states. So much so, isolating the individual adiabatic states and tracking the expected potential energy surfaces both lose the physical sense. This domain of molecular situation is far beyond the realm of the Born-Oppenheimer approximation. To survey such a violent electronic state-mixing, we apply a method of nonadiabatic electron wavepacket dynamics, the semiclassical Ehrenfest method. We have tracked those electron wavepackets and found the electronic state mixing looks like an ultrafast diffusion in the Hilbert space, which results in huge fluctuation. Furthermore, due to such a violent mixing, the quantum phases associated with the electronic states are swiftly randomized, and consequently the coherence among the electronic states are lost quickly. Besides, these highly excited states are mostly of highly poly-radical nature, even in the spin singlet manifold and the number of radicals amounts up to 10 electrons in the sense of unpaired electrons. Thus the electronic states are summarized to be poly-radical and decoherent with huge fluctuation in shorter time scales of vibrational motions. The present numerical study sets a theoretical foundation for unknown molecular properties and chemical reactivity of such densely quasi-degenerate chemical species.

  16. Pulsed-field ionization zero electron kinetic energy spectrum of the ground electronic state of BeOBe+.

    PubMed

    Antonov, Ivan O; Barker, Beau J; Heaven, Michael C

    2011-01-28

    The ground electronic state of BeOBe(+) was probed using the pulsed-field ionization zero electron kinetic energy photoelectron technique. Spectra were rotationally resolved and transitions to the zero-point level, the symmetric stretch fundamental and first two bending vibrational levels were observed. The rotational state symmetry selection rules confirm that the ground electronic state of the cation is (2)Σ(g)(+). Detachment of an electron from the HOMO of neutral BeOBe results in little change in the vibrational or rotational constants, indicating that this orbital is nonbonding in nature. The ionization energy of BeOBe [65480(4) cm(-1)] was refined over previous measurements. Results from recent theoretical calculations for BeOBe(+) (multireference configuration interaction) were found to be in good agreement with the experimental data.

  17. Some Chemical and Electronic Considerations of Solid State Semiconductor Crystals.

    ERIC Educational Resources Information Center

    Hinitz, Herman J.

    1986-01-01

    Describes the trend toward the use of electronic instrumentation to monitor and measure various parameters in chemical reactions. Stresses that a knowledge of the operational relationships involved in such instruments is essential for students beginning in science. Discusses electrostatic charges, semiconductor crystals, electronic conductors,…

  18. STIR: Novel Electronic States by Gating Strongly Correlated Materials

    DTIC Science & Technology

    2016-03-01

    electron behavior which could be modulated by gating: spin liquids (e.g. a layered Sodium Iridate compound) and multiferroics (e.g. Bismuth Ferrite). We...electron behavior which could be modulated by gating: spin liquids (e.g. a layered Sodium Iridate compound) and multiferroics (e.g. Bismuth Ferrite

  19. 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

  20. Nonclassical properties of electronic states of aperiodic chains in a homogeneous electric field

    NASA Astrophysics Data System (ADS)

    Spisak, B. J.; Wołoszyn, M.

    2009-07-01

    The electronic energy levels of one-dimensional aperiodic systems driven by a homogeneous electric field are studied by means of a phase-space description based on the Wigner distribution function. The formulation provides physical insight into the quantum nature of the electronic states for the aperiodic systems generated by the Fibonacci and Thue-Morse sequences. The nonclassical parameter for electronic states is studied as a function of the magnitude of homogeneous electric field to achieve the main result of this work, which is to prove that the nonclassical properties of the electronic states in the aperiodic systems determine the transition probability between electronic states in the region of anticrossings. The localization properties of electronic states and the uncertainty product of momentum and position variables are also calculated as functions of the electric field.

  1. Excited state electron transfer after visible light absorption by the Co(I) state of vitamin B12.

    PubMed

    Achey, Darren; Brigham, Erinn C; DiMarco, Brian N; Meyer, Gerald J

    2014-11-11

    The first example of excited state electron transfer from cob(I)alamin is reported herein. Vitamin B12 was anchored to a mesoporous TiO2 thin film and electrochemically reduced to the cob(I)alamin form. Pulsed laser excitation resulted in rapid excited state electron transfer, ket > 10(8) s(-1), followed by microsecond interfacial charge recombination to re-form cob(I)alamin. The supernucleophilic cob(I)alamin was found to be a potent photoreductant. The yield of excited state electron transfer was found to be excitation wavelength dependent. The implications of this dependence are discussed.

  2. Electron transport in micro to nanoscale solid state networks

    NASA Astrophysics Data System (ADS)

    Fairbanks, Matthew Stetson

    This dissertation focuses on low-dimensional electron transport phenomena in devices ranging from semiconductor electron 'billiards' to semimetal atomic clusters to gold nanoparticles. In each material system, the goal of this research is to understand how carrier transport occurs when many elements act in concert. In the semiconductor electron billiards, magnetoconductance fluctuations, the result of electron quantum interference within the device, are used as a probe of electron transport through arrays of one, two, and three connected billiards. By combining two established analysis techniques, this research demonstrates a novel method for determining the quantum energy level spacing in each of the arrays. That information in turn shows the extent (and limits) of the phase-coherent electron wavefunction in each of the devices. The use of the following two material systems, the semimetal atomic clusters and the gold nanoparticles, is inspired by the electron billiard results. First, the output of the simple, rectangular electron billiards, the magnetoconductance fluctuations, is quite generally found to be fractal. This research addresses the question of what output one might expect from a device with manifestly fractal geometry by simulating the electrical response of fractal resistor networks and by outlining a method to implement such devices in fractal aggregates of semimetal atomic clusters. Second, in gold nanoparticle arrays, the number of array elements can increase by orders of magnitude over the billiard arrays, all with the potential to stay in a similar, phase-coherent transport regime. The last portion of this dissertation details the fabrication of these nanoparticle-based devices and their electrical characteristics, which exhibit strong evidence for electron transport in the Coulomb-blockade regime. A sketch for further 'off-blockade' experiments to realize magnetoconductance fluctuations, i.e. phase-coherent electron phenomena, is presented.

  3. The current state of electronic consultation and electronic referral systems in Canada: an environmental scan.

    PubMed

    Liddy, Clare; Hogel, Matthew; Blazkho, Valerie; Keely, Erin

    2015-01-01

    Access to specialist care is a point of concern for patients, primary care providers, and specialists in Canada. Innovative e-health platforms such as electronic consultation (eConsultation) and referral (eReferral) can improve access to specialist care. These systems allow physicians to communicate asynchronously and could reduce the number of unnecessary referrals that clog wait lists, provide a record of the patient's journey through the referral system, and lead to more efficient visits. Little is known about the current state of eConsultation and eReferral in Canada. The purpose of this work was to identify current systems and gain insight into the design and implementation process of existing systems. An environmental scan approach was used, consisting of a systematic and grey literature review, and targeted semi-structured key informant interviews. Only three eConsultation/eReferral systems are currently in operation in Canada. Four themes emerged from the interviews: eReferral is an end goal for those provinces without an active eReferral system, re-organization of the referral process is a necessity prior to automation, engaging the end-user is essential, and technological incompatibilities are major impediments to progress. Despite the acknowledged need to improve the referral system and increase government spending on health information technology, eConsultation and eReferral systems remain scarce as Canada lags behind the rest of the developed world.

  4. Diagnostics of many-particle electronic states: non-stationary currents and residual charge dynamics

    NASA Astrophysics Data System (ADS)

    Maslova, N. S.; Mantsevich, V. N.; Arseyev, P. I.

    2017-01-01

    We propose the method for identifying many particle electronic states in the system of coupled quantum dots (impurities) with Coulomb correlations. We demonstrate that different electronic states can be distinguished by the complex analysis of localized charge dynamics and non-stationary characteristics. We show that localized charge time evolution strongly depends on the properties of initial state and analyze different time scales in charge kinetics for initially prepared singlet and triplet states. We reveal the conditions for existence of charge trapping effects governed by the selection rules for electron transitions between the states with different occupation numbers.

  5. The Low-Lying Electronic States of LiB

    NASA Technical Reports Server (NTRS)

    Ricca, Alessandra; Bauschlicher, Charles W., Jr.; Langhoff, Stephen R. (Technical Monitor)

    1995-01-01

    The spectroscopic constants for the triplet and singlet states of LiB below about 30 000/ cm are determined using an internally contracted multireference configuration interaction approach in conjunction with [6s 5p 3d 2f] atomic natural orbital basis sets. The ground state is (sup 3)Pi as found in previous work. No excited triplet states are found to be ideal for characterizing the ground state; the (1)(sup 3)Sigma(sup -) state has a transition energy that is too small for many experimental approaches and the (2)(sup 3)Pi and (3)(sup 3)Pi states have bond lengths that are significantly longer than the ground state, resulting in transition intensities that are spread out over many vibrational levels of the ground state.

  6. 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

  7. 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

  8. 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)

  9. Delocalization and occupancy effects of 5f orbitals in plutonium intermetallics using L3-edge resonant X-ray emission spectroscopy

    SciTech Connect

    Booth, C. H.; Medling, S. A.; Jiang, Yu; Bauer, E. D.; Tobash, P. H.; Mitchell, J. N.; Veirs, D. K.; Wall, M. A.; Allen, P. G.; Kas, J. J.; Sokaras, D.; Nordlund, D.; Weng, T. -C.

    2014-06-24

    Although actinide (An) L3 -edge X-ray absorption near-edge structure (XANES) spectroscopy has been very effective in determining An oxidation states in insulating, ionically bonded materials, such as in certain coordination compounds and mineral systems, the technique fails in systems featuring more delocalized 5f orbitals, especially in metals. Recently, actinide L3-edge resonant X-ray emission spec- troscopy (RXES) has been shown to be an effective alternative. This technique is further demonstrated here using a parameterized partial unoccupied density of states method to quantify both occupancy and delocalization of the 5f orbital in ?-Pu, ?-Pu, PuCoGa5 , PuCoIn5 , and PuSb2. These new results, supported by FEFF calculations, highlight the effects of strong correlations on RXES spectra and the technique?s ability to differentiate between f-orbital occupation and delocalization.

  10. State of the Art in Electronic Dosemeters for Neutrons

    NASA Astrophysics Data System (ADS)

    Luszik-Bhadra, Marlies

    2011-05-01

    The paper presents an overview of electronic personal dosemeters for neutrons in mixed neutron/photon fields. The energy response of commercially available electronic dosemeters in quasi-monoenergetic neutron fields and their performance in working places is discussed. The response curves are extended to high-energy neutrons up to 100 MeV, new prototype dosemeters are described and discussed especially for use at high-energy accelerators and in space.

  11. Excited State Electronic Properties of Sodium Iodide and Cesium Iodide

    SciTech Connect

    Campbell, Luke W.; Gao, Fei

    2013-05-01

    We compute from first principles the dielectric function, loss function, lifetime and scattering rate of quasiparticles due to electronic losses, and secondary particle spectrum due to plasmon decay in two scintillating alkali halides, sodium iodide and cesium iodide. Particular emphasis is placed on quasiparticles within several multiples of the band gap from the band edges. A theory for the decay spectra of plasmons and other electronic excitations in crystals is presented. Applications to Monte Carlo radiation transport codes are discussed.

  12. 78 FR 38989 - New Policies and Procedural Requirements for Electronic Submission of State Plans, and Program...

    Federal Register 2010, 2011, 2012, 2013, 2014

    2013-06-28

    ...:// extranet.acf.hhs.gov/oldcdocs/materials.html . DATES: Submit written or electronic comments on the policies...://extranet.acf.hhs.gov/oldcdocs/materials.html . Electronic Submission of Program Progress and Financial... Electronic Submission of State Plans, and Program and Financial Reporting Forms, for Mandatory Grant...

  13. Donor acceptor electronic couplings in π-stacks: How many states must be accounted for?

    NASA Astrophysics Data System (ADS)

    Voityuk, Alexander A.

    2006-04-01

    Two-state model is commonly used to estimate the donor-acceptor electronic coupling Vda for electron transfer. However, in some important cases, e.g. for DNA π-stacks, this scheme fails to provide accurate values of Vda because of multistate effects. The Generalized Mulliken-Hush method enables a multistate treatment of Vda. In this Letter, we analyze the dependence of calculated electronic couplings on the number of the adiabatic states included in the model. We suggest a simple scheme to determine this number. The superexchange correction of the two-state approximation is shown to provide good estimates of the electronic coupling.

  14. Electron-impact excitation of the low-lying electronic states of HCN

    NASA Technical Reports Server (NTRS)

    Chutjian, A.; Tanaka, H.; Srivastava, S. K.; Wicke, B. G.

    1977-01-01

    The first study of the low-energy electron-impact excitation of low-lying electronic transitions in the HCN molecule is reported. Measurements were made at incident electron energies of 11.6 and 21.6 eV in the energy-loss range of 3-10 eV, and at scattering angles of 20-130 deg. Inelastic scattering spectra were placed on the absolute cross-section scale by determining first the ratio of inelastic-to-elastic scattering cross sections, and then separately measuring the absolute elastic scattering cross section. Several new electronic transitions are observed which are intrinsically overlapped in the molecule itself. Assignments of these electronic transitions are suggested. These assignments are based on present spectroscopic and cross-sections measurements, high-energy electron scattering spectra, optical absorption spectra, and ab initio molecular orbital calculations.

  15. Coherent-state description of free-electron lasers

    NASA Astrophysics Data System (ADS)

    Lee, Ching Tsung

    1990-12-01

    It is generally accepted that the overall performance of free-electron lasers (FEL) can be understood without quantum mechanics. However, there are features of FEL such as photon statistics which can only be described quantum-mechanically. Although the majority of quantum-mechanical studies of FEL are devoted to one-particle models, there are also many studies on many-body effects of FEL. Unfortunately, the mathematical derivations of these studies are so complicated that it is not easy to follow the developments with a clearer picture in mind. The origin of the problem is the quantum recoils of the electrons. So we try to gain a clearer picture of the many-body effects by making the recoilless approximation. A simple model of FEL consists of a beam of relativistic electrons propagating through a spatially periodic magnetostatic wiggler field. The resulting laser output is propagating along the same direction as that of the electron beam. Quantum-mechanical analysis of FEL are usually based on the Bambini-Renieri frame which moves in the same direction as the propagating laser beam with a relativistic speed so that: (1) the wiggler field appears almost as a plane-wave radiation, (2) the frequency of the wiggler field coincides with that of the laser, and (3) the electron motion is nonrelativistic. Although in reality the laser beam can only derive its energy at the expense of the kinetic energy of the electrons, it appears in the Bambini-Renieri frame as if the photons of the laser were scattered from the fictitious photons of the wiggler field by the electrons.

  16. Co-Assignment of the Molecular Vibrational Frequencies in Different Electronic States

    NASA Astrophysics Data System (ADS)

    Panchenko, Yurii; Abramenkov, Alexander

    2016-06-01

    Ultrafast electron diffraction experimental data for the structural parameters of molecules in excited electronic states are comparatively uncommon, hence these parameters are largely unknown. However, because differences between the molecular geometries of excited and ground electronic states cause differences in their experimental vibrational spectra it is important to establish a correspondence between the molecular vibrational frequencies in the ground state and those of the excited state of interest. The correct co-assignment of the experimental vibrational frequencies between two different electronic states of a molecule may be determined by the analog of the Duschinsky matrix D. This matrix D is defined as D = (LI)-1LII where LI and LII are the matrices of the vibrational modes of the two states of the molecule under investigation. They are obtained by solving the vibrational problems in the I and II electronic states, respectively. Choosing the dominant elements in columns of the D matrix and permuting these columns to arrange these elements along the diagonal of the transformed matrix Dast makes it possible to establish the correct co-assignment of the calculated frequencies in the two electronic states. The rows of Dast are for the vibrations in the I electronic state, whereas the columns are for vibrations in the II electronic state. The results obtained may be tested by analogous calculations of Dast for isotopologues. The feasibility of co-assignments of the vibrational frequencies in the ground and T_1 and S_1 excited electronic states are demonstrated for trans-C_2O_2F_2. The analogs of the Duschinsky matrix Dast were used to juxtapose the vibrational frequencies of this molecule calculated at the CASPT2/cc-pVTZ level in the S_0, T_1 and S_1 states. F. Duschinsky, Acta Physicochim. URSS, 7(4), 551-566 (1937). Yu. N. Panchenko, Vibrational spectroscopy, 68, 236-240 (2013).

  17. The electronic excited states of green fluorescent protein chromophore models

    NASA Astrophysics Data System (ADS)

    Olsen, Seth Carlton

    We explore the properties of quantum chemical approximations to the excited states of model chromophores of the green fluorescent protein of A. victoria. We calculate several low-lying states by several methods of quantum chemical calculation, including state-averaged complete active space SCF (CASSCF) methods, time dependent density functional theory (TDDFT), equation-of motion coupled cluster (EOM-CCSD) and multireference perturbation theory (MRPT). Amongst the low-lying states we identify the optically bright pipi* state of the molecules and examine its properties. We demonstrate that the state is dominated by a single configuration function. We calculate zero-time approximations to the resonance Raman spectrum of GFP chromophore models, and assign published spectra based upon these.

  18. Present State of Electron Backscatter Diffraction and Prospective Developments

    SciTech Connect

    Schwarzer, R A; Field, D P; Adams, B L; Kumar, M; Schwartz, A J

    2008-10-24

    Electron backscatter diffraction (EBSD), when employed as an additional characterization technique to a scanning electron microscope (SEM), enables individual grain orientations, local texture, point-to-point orientation correlations, and phase identification and distributions to be determined routinely on the surfaces of bulk polycrystals. The application has experienced rapid acceptance in metallurgical, materials, and geophysical laboratories within the past decade (Schwartz et al. 2000) due to the wide availability of SEMs, the ease of sample preparation from the bulk, the high speed of data acquisition, and the access to complementary information about the microstructure on a submicron scale. From the same specimen area, surface structure and morphology of the microstructure are characterized in great detail by the relief and orientation contrast in secondary and backscatter electron images, element distributions are accessed by energy dispersive spectroscopy (EDS), wavelength dispersive spectroscopy (WDS), or cathodoluminescence analysis, and the orientations of single grains and phases can now be determined, as a complement, by EBSD.

  19. Electron density dynamics in the electronic ground state: motion along the Kekulé mode of benzene.

    PubMed

    Schild, Axel; Choudhary, Deepanshu; Sambre, Vaibhav D; Paulus, Beate

    2012-11-26

    If the Born-Oppenheimer approximation is invoked for the description of chemical reactions, the electron density rearranges following the motion of the nuclei. Even though this approach is central to theoretical chemistry, the explicit time dependence of the electron density is rarely studied, especially if the nuclei are treated quantum mechanically. In this article, we model the motion of benzene along the Kekulé vibrational coordinate to simulate the nuclear dynamics and electron density dynamics in the electronic ground state. Details of the change of core, valence, and π electrons are determined and analyzed. We show how the pictures anticipated by drawing Lewis structures of the rearrangement correlate with the time-dependent quantum description of the process.

  20. State of the art of electronic personal dosimeters for neutrons

    NASA Astrophysics Data System (ADS)

    d'Errico, Francesco; Luszik-Bhadra, Marlies; Lahaye, Thierry

    2003-06-01

    Despite a widely recognised need, electronic devices for personal dosimetry of neutrons or mixed neutron-photon fields are still far less established than systems for photon or beta radiations. A large research project is in progress to evaluate different methods currently used or under development for electronic personal dosimetry in mixed neutron-photon fields. The study includes testing in calibration fields as well as in representative workplaces of the nuclear industry. This paper describes the commercial and laboratory systems under investigation and their response characteristics. These were determined so far with measurements using ISO standard monoenergetic beams up to 19 MeV at the PTB in Braunschweig, Germany.

  1. Electron delocalization and aromaticity in low-lying excited states of archetypal organic compounds.

    PubMed

    Feixas, Ferran; Vandenbussche, Jelle; Bultinck, Patrick; Matito, Eduard; Solà, Miquel

    2011-12-14

    Aromaticity is a property usually linked to the ground state of stable molecules. Although it is well-known that certain excited states are unquestionably aromatic, the aromaticity of excited states remains rather unexplored. To move one step forward in the comprehension of aromaticity in excited states, in this work we analyze the electron delocalization and aromaticity of a series of low-lying excited states of cyclobutadiene, benzene, and cyclooctatetraene with different multiplicities at the CASSCF level by means of electron delocalization measures. While our results are in agreement with Baird's rule for the aromaticity of the lowest-lying triplet excited state in annulenes having 4nπ-electrons, they do not support Soncini and Fowler's generalization of Baird's rule pointing out that the lowest-lying quintet state of benzene and septet state of cyclooctatetraene are not aromatic.

  2. Understanding the nuclear initial state with an electron ion collider

    NASA Astrophysics Data System (ADS)

    Toll, Tobias

    2013-09-01

    In these proceedings I describe how a future electron-ion collider will allow us to directly measure the initial spatial distribution of gluons in heavy ions, as well as its variance ("lumpiness") in exclusive diffraction. I show the feasibility of such a measurement by means of simulated data from the novel event generator Sartre.

  3. Electronic absorption and ground state structure of carotenoid molecules.

    PubMed

    Mendes-Pinto, Maria M; Sansiaume, Elodie; Hashimoto, Hideki; Pascal, Andrew A; Gall, Andrew; Robert, Bruno

    2013-09-26

    Predicting the complete electronic structure of carotenoid molecules remains an extremely complex problem, particularly in anisotropic media such as proteins. In this paper, we address the electronic properties of nine relatively simple carotenoids by the combined use of electronic absorption and resonance Raman spectroscopies. Linear carotenoids exhibit an excellent correlation between (i) the inverse of their conjugation chain length N, (ii) the energy of their S0 → S2 electronic transition, and (iii) the position of their ν1 Raman band (corresponding to the stretching mode of their conjugated C═C bonds). For cyclic carotenoids such as β-carotene, this correlation is also observed between the latter two parameters (S0 → S2 energy and ν1 frequency), whereas their "nominal" conjugation length N does not follow the same relationship. We conclude that β-carotene and cyclic carotenoids in general exhibit a shorter effective conjugation length than that expected from their chemical structure. In addition, the effect of solvent polarizability on these molecular parameters was investigated for four of the carotenoids used in this study. We demonstrate that resonance Raman spectroscopy can discriminate between the different effects underlying shifts in the S0 → S2 transition of carotenoid molecules.

  4. Determination and Comparison of Carbonyl Stretching Frequency of a Ketone in Its Ground State and the First Electronic Excited State

    ERIC Educational Resources Information Center

    Bandyopadhyay, Subhajit; Roy, Saswata

    2014-01-01

    This paper describes an inexpensive experiment to determine the carbonyl stretching frequency of an organic keto compound in its ground state and first electronic excited state. The experiment is simple to execute, clarifies some of the fundamental concepts of spectroscopy, and is appropriate for a basic spectroscopy laboratory course. The…

  5. The Low-Lying Electronic States of YCu

    NASA Technical Reports Server (NTRS)

    Ricca, Alessandra; Bauschlicher, Charles W., Jr.; Langhoff, Stephen R. (Technical Monitor)

    1995-01-01

    The spectroscopic constants for the singlet and triplet states of YCu below about 15 000 per centimeter are determined using an internally contracted multireference configuration-interaction approach. These calculations are calibrated by studies of fewer states using higher levels of correlation treatment and/or larger basis sets. The computed T(sub e) values and radiative lifetimes are in reasonable agreement with experiment. The calculations confirm the previous experimental assignment for all but one state, where theory helps resolve between two possible assignments.

  6. Strongly separated pairs of core electrons in computed ground states of small molecules.

    PubMed

    Gottlieb, Alex D; Weishäupl, Rada M

    2013-03-01

    We have performed full configuration interaction computations of the ground states of the molecules Be, BeH2, Li, LiH, B, and BH and verified that the core electrons constitute "separated electron pairs." These separated pairs of core electrons have nontrivial structure; the core pair does not simply occupy a single spatial orbital. Our method of establishing the presence of separated electron pairs is direct and conclusive. We do not fit a separated pair model; we work with the wavefunctions of interest directly. To establish that a given group of spin-orbitals contains a quasi-separated pair, we verify by direct computation that the quantum state of the electrons that occupy those spin-orbitals is nearly a pure 2-electron state.

  7. A multi-state fragment charge difference approach for diabatic states in electron transfer: Extension and automation

    NASA Astrophysics Data System (ADS)

    Yang, Chou-Hsun; Hsu, Chao-Ping

    2013-10-01

    The electron transfer (ET) rate prediction requires the electronic coupling values. The Generalized Mulliken-Hush (GMH) and Fragment Charge Difference (FCD) schemes have been useful approaches to calculate ET coupling from an excited state calculation. In their typical form, both methods use two eigenstates in forming the target charge-localized diabatic states. For problems involve three or four states, a direct generalization is possible, but it is necessary to pick and assign the locally excited or charge-transfer states involved. In this work, we generalize the 3-state scheme for a multi-state FCD without the need of manual pick or assignment for the states. In this scheme, the diabatic states are obtained separately in the charge-transfer or neutral excited subspaces, defined by their eigenvalues in the fragment charge-difference matrix. In each subspace, the Hamiltonians are diagonalized, and there exist off-diagonal Hamiltonian matrix elements between different subspaces, particularly the charge-transfer and neutral excited diabatic states. The ET coupling values are obtained as the corresponding off-diagonal Hamiltonian matrix elements. A similar multi-state GMH scheme can also be developed. We test the new multi-state schemes for the performance in systems that have been studied using more than two states with FCD or GMH. We found that the multi-state approach yields much better charge-localized states in these systems. We further test for the dependence on the number of state included in the calculation of ET couplings. The final coupling values are converged when the number of state included is increased. In one system where experimental value is available, the multi-state FCD coupling value agrees better with the previous experimental result. We found that the multi-state GMH and FCD are useful when the original two-state approach fails.

  8. A multi-state fragment charge difference approach for diabatic states in electron transfer: extension and automation.

    PubMed

    Yang, Chou-Hsun; Hsu, Chao-Ping

    2013-10-21

    The electron transfer (ET) rate prediction requires the electronic coupling values. The Generalized Mulliken-Hush (GMH) and Fragment Charge Difference (FCD) schemes have been useful approaches to calculate ET coupling from an excited state calculation. In their typical form, both methods use two eigenstates in forming the target charge-localized diabatic states. For problems involve three or four states, a direct generalization is possible, but it is necessary to pick and assign the locally excited or charge-transfer states involved. In this work, we generalize the 3-state scheme for a multi-state FCD without the need of manual pick or assignment for the states. In this scheme, the diabatic states are obtained separately in the charge-transfer or neutral excited subspaces, defined by their eigenvalues in the fragment charge-difference matrix. In each subspace, the Hamiltonians are diagonalized, and there exist off-diagonal Hamiltonian matrix elements between different subspaces, particularly the charge-transfer and neutral excited diabatic states. The ET coupling values are obtained as the corresponding off-diagonal Hamiltonian matrix elements. A similar multi-state GMH scheme can also be developed. We test the new multi-state schemes for the performance in systems that have been studied using more than two states with FCD or GMH. We found that the multi-state approach yields much better charge-localized states in these systems. We further test for the dependence on the number of state included in the calculation of ET couplings. The final coupling values are converged when the number of state included is increased. In one system where experimental value is available, the multi-state FCD coupling value agrees better with the previous experimental result. We found that the multi-state GMH and FCD are useful when the original two-state approach fails.

  9. Excited electronic states and spectroscopy of unsymmetrically substituted polyenes

    NASA Astrophysics Data System (ADS)

    Itoh, Takao

    2013-09-01

    α-Methyl-ω-phenylpolyenes, Me-(CH=CH)N-Ph, (MPPNs) with N = 2, 3, and 4 were synthesized. Fluorescence, absorption, and excitation spectra of MPPNs have been measured under different conditions along with those of β-methylstyrene. It is shown that there is a forbidden singlet (π, π*) excited state located at energies below the absorbing state for MPPNs with N = 3 and 4. Excitation energies of these polyenes are determined as a function of N. Quantitative analysis of the temperature dependence of the relative intensity of the fluorescence spectrum and its solvent shift behavior extract estimates of the various physical parameters that characterize excitation energies and excited-state dynamical behavior of MPPN with N = 3. The singlet excited states of the MPPNs were compared with those of the α,ω-diphenylpolyenes and α,ω-dimethylpolyenes.

  10. Excited electronic states and spectroscopy of unsymmetrically substituted polyenes.

    PubMed

    Itoh, Takao

    2013-09-07

    α-Methyl-ω-phenylpolyenes, Me-(CH=CH)N-Ph, (MPPNs) with N = 2, 3, and 4 were synthesized. Fluorescence, absorption, and excitation spectra of MPPNs have been measured under different conditions along with those of β-methylstyrene. It is shown that there is a forbidden singlet (π, π∗) excited state located at energies below the absorbing state for MPPNs with N = 3 and 4. Excitation energies of these polyenes are determined as a function of N. Quantitative analysis of the temperature dependence of the relative intensity of the fluorescence spectrum and its solvent shift behavior extract estimates of the various physical parameters that characterize excitation energies and excited-state dynamical behavior of MPPN with N = 3. The singlet excited states of the MPPNs were compared with those of the α,ω-diphenylpolyenes and α,ω-dimethylpolyenes.

  11. Development of Solid State Electronics for a Spark Chamber

    NASA Astrophysics Data System (ADS)

    Gross, Eisen; Gray, Frederick

    2013-04-01

    Spark chambers have been used to detect charged particles in physics since the early part of the 20^th century. This very crude method can still be very useful in a classroom, museum, or outreach setting to show evidence of such particles. Older electronics such as vacuum tubes and spark gaps have been still used in recent designs, but they are resource-consuming to maintain and are becoming difficult to procure. These designs also used obsolescent electronics for the discriminators in the trigger circuit. A new design will be presented that uses a fast high voltage transistor switch along with modern comparators and programmable logic. Lower trigger latency has been achieved than in the traditional design. The muon imaging efficiency will be presented.

  12. Characterization of the electronic states of the biological relevant SSNO molecule

    NASA Astrophysics Data System (ADS)

    Ayari, Tarek; Hochlaf, Majdi; Mogren Al-Mogren, Muneerah; Francisco, Joseph S.

    2017-02-01

    Using configuration interaction ab initio methods, we investigate the lowest electronic states of doublet and quartet spin multiplicities of SSNO where the one-dimensional cuts of the six-dimensional potential energy surfaces of these electronic states along the stretching and bending coordinates are computed. Mainly, these electronic states are found to be repulsive along the central SN distance. A high density of electronic states is computed even at low excitation energies that may favor their couplings. Therefore, the dynamics of the SSNO electronic states is expected to be very complex. We also characterized the bound electronic states spectroscopically where we derived their equilibrium structures and vibrational frequencies. Our calculations show the importance of taking into account of dynamical correlation, in addition to static correlation, for the accurate description of SSNO electronic excited states and more generally for those of R-NO molecular species. Finally, we highlighted the potential role of SSNO in light-induced NO delivery from SSNO related species in biological media.

  13. Quantum ballistic transport by interacting two-electron states in quasi-one-dimensional channels

    SciTech Connect

    Huang, Danhong; Gumbs, Godfrey; Abranyos, Yonatan; Pepper, Michael; Kumar, Sanjeev

    2015-11-15

    For quantum ballistic transport of electrons through a short conduction channel, the role of Coulomb interaction may significantly modify the energy levels of two-electron states at low temperatures as the channel becomes wide. In this regime, the Coulomb effect on the two-electron states is calculated and found to lead to four split energy levels, including two anticrossing-level and two crossing-level states. Moreover, due to the interplay of anticrossing and crossing effects, our calculations reveal that the ground two-electron state will switch from one anticrossing state (strong confinement) to a crossing state (intermediate confinement) as the channel width gradually increases and then back to the original anticrossing state (weak confinement) as the channel width becomes larger than a threshold value. This switching behavior leaves a footprint in the ballistic conductance as well as in the diffusion thermoelectric power of electrons. Such a switching is related to the triple spin degeneracy as well as to the Coulomb repulsion in the central region of the channel, which separates two electrons away and pushes them to different channel edges. The conductance reoccurrence region expands from the weak to the intermediate confinement regime with increasing electron density.

  14. Electron impact excitation of autoionising states of krypton

    NASA Technical Reports Server (NTRS)

    Srivastava, S. K.; Trajmar, S.

    1978-01-01

    Energy-loss spectra of krypton in the region between 21 and 29 eV have been obtained at electron impact energies of 30, 60 and 100 eV. For each energy, the angular distribution of intensities has been measured at 5, 10 and 15 deg scattering angles. Assignments of spectral features found in this region are suggested and a comparison is made with previous measurements.

  15. Quasi-One-Dimensional Electronic States Inside and Outside Helium-Plated Carbon Nanotubes

    NASA Astrophysics Data System (ADS)

    Motta, M.; Galli, D. E.; Liebrecht, M.; Del Maestro, A.; Cole, M. W.

    2016-10-01

    About one-half a century ago, it was realized that electrons experience a repulsive barrier when approaching the surface of condensed phases of helium, hydrogen, and neon. This led to the proposal and subsequent observation of image-potential surface-bound electronic states, which exhibit intriguing quasi-two-dimensional behavior. In the present work, we report similar quasi-one-dimensional electronic states by exploring single-wall carbon nanotubes coated both inside and outside by thin helium films. Electrons near such structures are localized in the radial direction, but free to move along the nanotube axis. The many-body aspects of the system are discussed qualitatively.

  16. Electronic structure and chemical bonding in the lowest electronic states of TcN.

    PubMed

    Borin, Antonio Carlos; Gobbo, João Paulo

    2009-11-12

    Multiconfiguration second-order perturbation theory, with the inclusion of relativistic effects and spin-orbit coupling, was employed to investigate the nature of the ground and low-lying Lambda-S and Omega states of the TcN molecule. Spectroscopic constants, effective bond order, and potential energy curves for 13 low-lying Lambda-S states and 5 Omega states are given. The computed ground state of TcN is of Omega = 3 symmetry (R(e) = 1.605 A and omega(e) = 1085 cm(-1)), originating mainly from the (3)Delta Lambda-S ground state. This result is contrasted with the nature of the ground state for other VIIB transtion-metal mononitrides, including X(3)Sigma(-) symmetry for MnN and Omega = 0(+) symmetry for ReN, derived also from a X(3)Sigma(-) state.

  17. Bound Electron States in Skew-symmetric Quantum Wire Intersections

    DTIC Science & Technology

    2014-01-01

    in transistors, solar cells , LEDs, and diode lasers. They have also investigated quantum dots as agents for medical imaging and as possible qubits in... solar cells .” Chemical reviews 110.11 (2010): 6873-6890. [9] Bonadeo, Nicolas H., et al. ”Coherent optical control of the quantum state of a single...dots on GaAs /InP , (inset) a single InAs quantum dot. two reasons. First, the superposition of the ground and excited states de- phases more slowly in

  18. The low-lying electronic states of LiC

    NASA Technical Reports Server (NTRS)

    Ricca, Alessandra; Bauschlicher, Charles W., Jr.; Langhoff, Stephen R. (Technical Monitor)

    1995-01-01

    The spectroscopic constants for the doublet and quartet states of LiC below about 30,000/cm are determined using an internally contracted multireference configuration-interaction approach in conjunction with a [6s 5p 3d 2f] atomic natural orbital basis sets. All of the strongly bound states, X(sup 4)(SIGMA)(sup -),(1)(sup 2)(DELTA), (1)(sup 2)(SIGMA)(sup +), and (2)(sup 2) II, very ionic in character. The only bound-bound quartet transition in this energy range is (2)(sup 4)SIGMA(sup -) and Franck-Condon factors, Einstein A values, and lifetimes are reported for this transition.

  19. Quantitative Electron Probe Microanalysis: State of the Art

    NASA Technical Reports Server (NTRS)

    Carpernter, P. K.

    2005-01-01

    Quantitative electron-probe microanalysis (EPMA) has improved due to better instrument design and X-ray correction methods. Design improvement of the electron column and X-ray spectrometer has resulted in measurement precision that exceeds analytical accuracy. Wavelength-dispersive spectrometer (WDS) have layered-dispersive diffraction crystals with improved light-element sensitivity. Newer energy-dispersive spectrometers (EDS) have Si-drift detector elements, thin window designs, and digital processing electronics with X-ray throughput approaching that of WDS Systems. Using these systems, digital X-ray mapping coupled with spectrum imaging is a powerful compositional mapping tool. Improvements in analytical accuracy are due to better X-ray correction algorithms, mass absorption coefficient data sets,and analysis method for complex geometries. ZAF algorithms have ban superceded by Phi(pz) algorithms that better model the depth distribution of primary X-ray production. Complex thin film and particle geometries are treated using Phi(pz) algorithms, end results agree well with Monte Carlo simulations. For geological materials, X-ray absorption dominates the corretions end depends on the accuracy of mass absorption coefficient (MAC) data sets. However, few MACs have been experimentally measured, and the use of fitted coefficients continues due to general success of the analytical technique. A polynomial formulation of the Bence-Albec alpha-factor technique, calibrated using Phi(pz) algorithms, is used to critically evaluate accuracy issues and can be also be used for high 2% relative and is limited by measurement precision for ideal cases, but for many elements the analytical accuracy is unproven. The EPMA technique has improved to the point where it is frequently used instead of the petrogaphic microscope for reconnaissance work. Examples of stagnant research areas are: WDS detector design characterization of calibration standards, and the need for more complete

  20. Combined study of the ground and unoccupied electronic states of graphite by electron energy-loss spectroscopy

    SciTech Connect

    Feng, Zhenbao; Löffler, Stefan; Eder, Franz; Meyer, Jannik C.; Su, Dangsheng; Schattschneider, Peter

    2013-11-14

    Both the unoccupied and ground electronic states of graphite have been studied by electron energy-loss spectroscopy in a transmission electron microscope. Electron energy-loss near-edge structures of the K-edge of carbon have been investigated in detail for scattering angles from 0 to 2.8 mrad. The π{sup *} and σ{sup *} components were separated. The angular and energy dependences of the π{sup *} and σ{sup *} structures were in fair agreement with theory. Electron energy loss Compton spectra of graphite were recorded at scattering angles from 45 to 68 mrad. One Compton scattering spectrum was obtained in 1 min compared with several hours or days using photons. The contributions of core electrons were calculated by the exact Hartree-Slater method in the Compton scattering region. The electron Compton profile for graphite is in good agreement with other conventional Compton profile measurements, as well as with theory, thus establishing the validity of the technique.

  1. Electronic Timekeeping: North Dakota State University Improves Payroll Processing.

    ERIC Educational Resources Information Center

    Vetter, Ronald J.; And Others

    1993-01-01

    North Dakota State University has adopted automated timekeeping to improve the efficiency and effectiveness of payroll processing. The microcomputer-based system accurately records and computes employee time, tracks labor distribution, accommodates complex labor policies and company pay practices, provides automatic data processing and reporting,…

  2. The Low-Lying Electronic States of Mg2(+)

    NASA Technical Reports Server (NTRS)

    Ricca, Alessandra; Bauschlicher, Charles W., Jr.

    1994-01-01

    The low-lying doublet and quartet states of Mg+ have been studied using a multireference configuration interaction approach. The effect of inner-shell correlation has been included using the core-polarization potential method. The computed spectroscopic constants, lifetimes, and oscillator strengths should help resolve the difference between the recent experiments and previous theoretical calculations.

  3. Study of the Electronic Surface State of III - V Compounds

    DTIC Science & Technology

    1976-03-15

    possible reason for the variation in Ep pinning observed by different groups , because EF is very sensitive to small (« 1 monolayer) of oxygen, and... foming a SchPtt.y barrier or by s^l amounts of oxygen. East,nan and cpworkers ba.e ^ alsp reported now finding n-type 3-S’s without surface state

  4. 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.

  5. Ozone absorption spectroscopy in search of low-lying electronic states

    NASA Technical Reports Server (NTRS)

    Anderson, S. M.; Mauersberger, K.

    1995-01-01

    A spectrometer capable of detecting ozone absorption features 9 orders of magnitude weaker than the Hartley band has been employed to investigate the molecule's near-infrared absorption spectrum. At this sensitivity a wealth of information on the low-lying electronically excited states often believed to play a role in atmospheric chemistry is available in the form of vibrational and rotational structure. We have analyzed these spectra using a combination of digital filtering and isotope substitution and find evidence for three electronically excited states below 1.5 eV. The lowest of these states is metastable, bound by approximately 0.1 eV and probably the (3)A2 rather than the (3)B2 state. Its adiabatic electronic energy is 1.24 +/- 0.01 eV, slightly above the dissociation energy of the ground state. Two higher states, at 1.29 +/- 0.03 and 1.48 +/- 0.03 eV are identified as the (3)B2 and the (3)B1, respectively. Combined with other recent theoretical and experimental data on the low-lying electronic states of ozone, these results imply that these are, in fact, the lowest three excited states; that is, there are no electronically excited states of ozone lying below the energy of O(3P) + O2((3)Sigma(-), v = 0). Some of the implications for atmospheric chemistry are considered.

  6. 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.

  7. 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

  8. Spectroscopic properties and potential energy curves of low-lying electronic states of RuC.

    PubMed

    Guo, Rui; Balasubramanian, K

    2004-04-22

    The RuC molecule has been a challenging species due to the open-shell nature of Ru resulting in a large number of low-lying electronic states. We have carried out state-of-the-art calculations using the complete active space multiconfiguration self-consistent field followed by multireference configuration interaction methods that included up to 18 million configurations, in conjunction with relativistic effects. We have computed 29 low-lying electronic states of RuC with different spin multiplicities and spatial symmetries with energy separations less than 38,000 cm(-1). We find two very closely low-lying electronic states for RuC, viz., 1Sigma+ and 3Delta with the 1Sigma+ being stabilized at higher levels of theory. Our computed spectroscopic constants and dipole moments are in good agreement with experiment although we have reported more electronic states than those that have been observed experimentally. Our computations reveal a strongly bound 1Sigma+ state with a large dipole moment which is most likely the experimentally observed ground state and an energetically close 3Delta state with a smaller dipole moment. Overall our computed spectroscopic constants of the excited states with energy separations less than 18,000 cm(-1) agree quite well with those of the corresponding observed states.

  9. Electron Impact Excitation of Xenon from the Ground State and the Metastable State to the 5p57p Levels

    NASA Astrophysics Data System (ADS)

    Chen, Zhan-Bin; Dong, Chen-Zhong; Xie, Lu-You; Jiang, Jun

    2014-03-01

    Electron impact excitation cross sections from the ground state and the lowest metastable state 5p56s J = 2 to the excited states of the 5p57p configuration of xenon are calculated systematically using the fully relativistic distorted wave method. Special attention is paid to the configuration interaction effects in the wave-function expansion of target states. The results are in good agreement with the recent experimental data by Jung et al. [Phys. Rev. A 80 (2009) 062708] over the measured energy range. These accurate theoretical results can be used in the modeling and diagnosis of plasmas containing xenon.

  10. 78 FR 49510 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Montana

    Federal Register 2010, 2011, 2012, 2013, 2014

    2013-08-14

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Montana AGENCY... INFORMATION: On October 13, 2005, the final Cross-Media Electronic Reporting Rule (CROMERR) was published...

  11. 78 FR 35030 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Nevada

    Federal Register 2010, 2011, 2012, 2013, 2014

    2013-06-11

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Nevada AGENCY... . SUPPLEMENTARY INFORMATION: On October 13, 2005, the final Cross-Media Electronic Reporting Rule (CROMERR)...

  12. 76 FR 76971 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Indiana

    Federal Register 2010, 2011, 2012, 2013, 2014

    2011-12-09

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Indiana AGENCY... . SUPPLEMENTARY INFORMATION: On October 13, 2005, the final Cross-Media Electronic Reporting Rule (CROMERR)...

  13. 78 FR 77121 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of New York

    Federal Register 2010, 2011, 2012, 2013, 2014

    2013-12-20

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of New York AGENCY...-Media Electronic Reporting Rule (CROMERR) was published in the Federal Register (70 FR 59848)...

  14. 77 FR 68770 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Vermont

    Federal Register 2010, 2011, 2012, 2013, 2014

    2012-11-16

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Vermont AGENCY... . SUPPLEMENTARY INFORMATION: On October 13, 2005, the final Cross-Media Electronic Reporting Rule (CROMERR)...

  15. 76 FR 25333 - Cross-Media Electronic Reporting: Authorized Program Revision/Modification Approvals, State of...

    Federal Register 2010, 2011, 2012, 2013, 2014

    2011-05-04

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision/ Modification Approvals, State of... final Cross-Media Electronic Reporting Rule (CROMERR) was published in the Federal Register (70 FR...

  16. 77 FR 71792 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Georgia

    Federal Register 2010, 2011, 2012, 2013, 2014

    2012-12-04

    ... From the Federal Register Online via the Government Publishing Office ] ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Georgia AGENCY...@epa.gov . SUPPLEMENTARY INFORMATION: On October 13, 2005, the final Cross-Media Electronic...

  17. 77 FR 25474 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Florida

    Federal Register 2010, 2011, 2012, 2013, 2014

    2012-04-30

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Florida AGENCY... final Cross-Media Electronic Reporting Rule (CROMERR) was published in the Federal Register (70 FR...

  18. 76 FR 76970 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Montana

    Federal Register 2010, 2011, 2012, 2013, 2014

    2011-12-09

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Montana AGENCY... . SUPPLEMENTARY INFORMATION: On October 13, 2005, the final Cross-Media Electronic Reporting Rule (CROMERR)...

  19. 76 FR 76971 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Arkansas

    Federal Register 2010, 2011, 2012, 2013, 2014

    2011-12-09

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Arkansas AGENCY... . SUPPLEMENTARY INFORMATION: On October 13, 2005, the final Cross-Media Electronic Reporting Rule (CROMERR)...

  20. 78 FR 32386 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Arkansas

    Federal Register 2010, 2011, 2012, 2013, 2014

    2013-05-30

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Arkansas AGENCY..., the final Cross-Media Electronic Reporting Rule (CROMERR) was published in the Federal Register (70...

  1. 77 FR 65379 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Wyoming

    Federal Register 2010, 2011, 2012, 2013, 2014

    2012-10-26

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Wyoming AGENCY... 13, 2005, the final Cross-Media Electronic Reporting Rule (CROMERR) was published in the...

  2. 76 FR 25334 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Maryland

    Federal Register 2010, 2011, 2012, 2013, 2014

    2011-05-04

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Maryland AGENCY... . SUPPLEMENTARY INFORMATION: On October 13, 2005, the final Cross-Media Electronic Reporting Rule (CROMERR)...

  3. 76 FR 24020 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Illinois

    Federal Register 2010, 2011, 2012, 2013, 2014

    2011-04-29

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Illinois AGENCY... . SUPPLEMENTARY INFORMATION: On October 13, 2005, the final Cross-Media Electronic Reporting Rule (CROMERR)...

  4. Records for Electronic Databases in the Online Catalog at Middle Tennessee State University

    ERIC Educational Resources Information Center

    Geckle, Beverly J.; Pozzebon, Mary Ellen; Williams, Jo

    2008-01-01

    This article recounts a project at the Middle Tennessee State University library to include records for electronic databases in the online catalog. Although electronic databases are accessible via the library's Databases A-Z list and related subject guides, cataloging these resources also provides access via the online catalog, allowing more of…

  5. A geometrical crossover in excited states of two-electron quantum dots in a magnetic field

    NASA Astrophysics Data System (ADS)

    Nazmitdinov, R. G.; Simonović, N. S.; Plastino, A. R.; Chizhov, A. V.

    2012-11-01

    We use the entanglement measure to study the evolution of quantum correlations in two-electron axially-symmetric parabolic quantum dots under a perpendicular magnetic field. We found that the entanglement indicates on the shape transition in the density distribution of two electrons in the lowest state with zero angular momentum projection at the specific value of the applied magnetic field.

  6. Electronic coupling between ligand and core energy states in dithiolate-monothiolate stabilized Au clusters.

    PubMed

    Ahuja, Tarushee; Wang, Dengchao; Tang, Zhenghua; Robinson, Donald A; Padelford, Jonathan W; Wang, Gangli

    2015-07-15

    Electron transfer activities of metal clusters are fundamentally significant and have promising potential in catalysis, charge or energy storage, sensing, biomedicine and other applications. Strong resonance coupling between the metal core energy states and the ligand molecular orbitals has not been established experimentally, albeit exciting progress has been achieved in the composition and structure determination of these types of nanomaterials recently. In this report, the coupling between core and ligand energy states is demonstrated by the rich electron transfer activities of Au130 clusters. Quantized electron transfers to the core and multi-electron transfers involving the durene-dithiolate ligands were observed at lower and higher potentials, respectively, in voltammetric studies. After a facile multi-electron oxidation from +1.34 to +1.40 V, several reversal reduction processes at more negative potentials, i.e. +0.91 V, +0.18 V and -0.34 V, were observed in an electrochemically irreversible fashion or with sluggish kinetics. The number of electrons and the shifts of the respective reduction potentials in the reversal process were attributed to the electronic coupling or energy relaxation processes. The electron transfer activities and subsequent relaxation processes are drastically reduced at lower temperatures. The time- and temperature-dependent relaxation, involving multiple energy states in the reversal reduction processes upon the oxidation of ligands, reveals the coupling between core and ligand energy states.

  7. Dynamics of the Chemistry of Electronically Excited Atoms in Defined Quantum States.

    DTIC Science & Technology

    1980-08-15

    excited atom concentration by atomic absorption spectroscopy in the vacuum ultraviolet (6). Relatively efficient electronic to vibrational energy transfer...by the use of atomic absorption spectroscopy , permitted observation of both ground and electronically excited state bromine atoms. The deactivation of

  8. Configuring Electronic States in an Atomically Precise Array of Quantum Boxes.

    PubMed

    Nowakowska, Sylwia; Wäckerlin, Aneliia; Piquero-Zulaica, Ignacio; Nowakowski, Jan; Kawai, Shigeki; Wäckerlin, Christian; Matena, Manfred; Nijs, Thomas; Fatayer, Shadi; Popova, Olha; Ahsan, Aisha; Mousavi, S Fatemeh; Ivas, Toni; Meyer, Ernst; Stöhr, Meike; Ortega, J Enrique; Björk, Jonas; Gade, Lutz H; Lobo-Checa, Jorge; Jung, Thomas A

    2016-07-01

    A 2D array of electronically coupled quantum boxes is fabricated by means of on-surface self-assembly assuring ultimate precision of each box. The quantum states embedded in the boxes are configured by adsorbates, whose occupancy is controlled with atomic precision. The electronic interbox coupling can be maintained or significantly reduced by proper arrangement of empty and filled boxes.

  9. 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.

  10. Teleportation of electronic many-qubit states encoded in the electron spin of quantum dots via single photons.

    PubMed

    Leuenberger, Michael N; Flatté, Michael E; Awschalom, D D

    2005-03-18

    We propose a teleportation scheme that relies only on single-photon measurements and Faraday rotation, for teleportation of many-qubit entangled states stored in the electron spins of a quantum dot system. The interaction between a photon and the two electron spins, via Faraday rotation in microcavities, establishes Greenberger-Horne-Zeilinger entanglement in the spin-photon-spin system. The appropriate single-qubit measurements, and the communication of two classical bits, produce teleportation. This scheme provides the essential link between spintronic and photonic quantum information devices by permitting quantum information to be exchanged between them.

  11. Improved Detection of Fast Neutrons with Solid-State Electronics

    NASA Astrophysics Data System (ADS)

    Chatzakis, J.; Hassan, S. M.; Clark, E. L.; Talebitaher, A.; Lee, P.

    2014-02-01

    There is an increasing requirement for alternative and improved detection of fast neutrons due to the renewed interest in neutron diagnostics applications. Some applications require heavily shielded neutron sources that emit a substantial proportion of their emission as fast neutrons and so require high performance fast neutron detectors. In some applications, the detection of neutron bursts from pulsed neutron sources has to be synchronized to the repetition rate of the source. Typical fast neutron detectors incorporate scintillators that are sensitive to all kinds of ionizing radiations as well as neutrons, and their efficiency is low. In this paper, we present a device based on the principle of neutron activation coupled to solid-state p-i-n diodes connected to a charge amplifier. The charge amplifier is specially developed to operate with high capacitance detectors and has been optimized by the aid of the SPICE program. A solid-state pulse shaping filter follows the charge amplifier, as an inexpensive solution, capable to provide pulses that can be counted by a digital counter.

  12. Total electron scattering cross-sections and negative ion states of halogenated methanes

    SciTech Connect

    Underwood-Lemons, T.; Winkler, D.C.; Moore, J.H.; Tossell, J.A.

    1993-12-01

    The interaction of low energy electrons with halogenated methanes plays an important role in both their atmospheric and plasma processing chemistry. In this work, the total electron scattering cross-sections of mixed fluorohalomethanes (CF{sub n}X{sub 4-n}) were measured for incident electrons in the energy range of 0.2-12 eV using electron transmission spectroscopy. Resonances in the scattering cross-sections may be interpreted as the capture of low energy electrons into unoccupied molecular orbitals. To aid in the assignments of the resulting negative ion states, the authors performed quantum mechanical calculations of the electron attachment energies and measured the dissociative attachment cross-sections. The effect of halogen substitution on the orbitals participating in electron capture are examined.

  13. Experimental realization of nearly steady-state toroidal electron plasmas

    SciTech Connect

    Stoneking, M. R.; Ha, B. N.; Smoniewski, J.; Marler, J. P.

    2009-05-15

    Electron plasmas with densities of 5x10{sup 6} cm{sup -3} are trapped in the Lawrence Non-neutral Torus II (LNT II) for times exceeding 1 s. LNT II is a high aspect ratio (R{sub 0}/a > or approx.10) partially toroidal trap (270 deg. arc, B{sub 0}=670 G). The m=1 diocotron mode is launched and detected using isolated segments of a fully sectored conducting boundary and its frequency is used to determine the total trapped charge as a function of time. The observed confinement time ({approx_equal}3 s) approaches the theoretical limit ({approx_equal}6 s) set by the magnetic pumping transport mechanism of Crooks and O'Neil [Phys. Plasmas 3, 2533 (1996)]. We also present equilibrium modeling and numerical simulations of the toroidal m=1 mode constrained by experimental data. Future work includes the identification of the dominant transport mechanisms via confinement scaling experiments and measurement of the m=2 mode frequency and development of a strategy for making a transition to fully toroidal confinement.

  14. Vertically aligned carbon nanofibers: interconnecting solid state electronics with biosystems.

    PubMed

    Cassell, Alan M; Li, Jun; Nguyen-Vu, Thuy-Duong Barbara; Koehne, Jessica E; Chen, Hua; Andrews, Russell; Meyyappan, M

    2009-08-01

    Vertically aligned carbon nanofibers (VACNFs) are grown directly on prefabricated electronic circuits with nanoscale precision. Utilizing the free-standing nanofiber array geometry, we have demonstrated the detection of nucleic acids to construct an ultrasensitive electrochemical sensor. Extending this technology towards in vivo applications, we have modified the free-standing VACNF arrays in order to achieve a multifunctional three dimensional (3-D) matrix that interpenetrates the neuronal network of PC12 cells. We found that PC12 cells cultured on the nanofiber arrays can form an extended neural network upon proper chemical and biochemical modification. The soft 3-D nanofiber array architecture provides a novel platform to fine-tune the topographical, mechanical, chemical, and electrical cues at sub-cellular scales. This biomaterial platform can be used for both fundamental studies of nanomaterial-cell interactions and the development of multifunctional, chronically stable implantable devices. The application of these devices and potential utility as a multifunctional platform for neurophysiology and biochemical studies will be discussed.

  15. Spectroscopic Properties and Potential Energy Curves of Low-lying electronic States of RuC

    SciTech Connect

    Balasubramanian, K; Guo, R

    2003-12-22

    The RuC molecule has been a challenging species due to the open-shell nature of Ru resulting in a large number of low-lying electronic states. We have carried out state-of-the-art calculations using the complete active space multi-configuration self-consistent field (CASSCF) followed by multireference configuration interaction (MRCI) methods that included up 18 million configurations, in conjunction with relativistic effects. We have computed 29 low-lying electronic states of RuC with different spin multiplicities and spatial symmetries with energy separations less than 38 000 cm{sup -1}. We find two very closely low-lying electronic states for RuC, viz., {sup 1}{Sigma}{sup +} and {sup 3}{Delta} with the {sup 1}{Sigma}{sup +} being stabilized at higher levels of theory. Our computed spectroscopic constants and dipole moments are in good agreement with experiment although we have reported more electronic states than those that have been observed experimentally. Our computations reveal a strongly bound X{sup 1}{Sigma}{sup +} state with a large dipole moment and an energetically close {sup 3}{Delta} state with a smaller dipole moment. Overall our computed spectroscopic constants of the excited states with energy separations less than 18000 cm{sup -1} agree quite well with those of the corresponding observed states.

  16. Interface states in two-dimensional electron systems with spin-orbital interaction.

    PubMed

    Sukhanov, Aleksei A; Sablikov, Vladimir A

    2011-10-05

    Interface states at a boundary between regions with different spin-orbit interactions (SOIs) in two-dimensional (2D) electron systems are investigated within the one-band effective mass method with generalized boundary conditions for envelope functions. We have found that the interface states unexpectedly exist even if the effective interface potential equals zero. Depending on the system parameters, the energy of these states can lie in either or both forbidden and conduction bands of bulk states. The interface states have chiral spin texture similar to that of the edge states in 2D topological insulators. However, their energy spectrum is more sensitive to the interfacial potential, the largest effect being produced by the spin-dependent component of the interfacial potential. We have also studied the size quantization of the interface states in a strip of 2D electron gas with SOI and found an unusual (non-monotonic) dependence of the quantization energy on the strip width.

  17. 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.

  18. 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.

  19. 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.

  20. Nonadiabatic excited-state molecular dynamics: Treatment of electronic decoherence

    NASA Astrophysics Data System (ADS)

    Nelson, Tammie; Fernandez-Alberti, Sebastian; Roitberg, Adrian E.; Tretiak, Sergei

    2013-06-01

    Within the fewest switches surface hopping (FSSH) formulation, a swarm of independent trajectories is propagated and the equations of motion for the quantum coefficients are evolved coherently along each independent nuclear trajectory. That is, the phase factors, or quantum amplitudes, are retained. At a region of strong coupling, a trajectory can branch into multiple wavepackets. Directly following a hop, the two wavepackets remain in a region of nonadiabatic coupling and continue exchanging population. After these wavepackets have sufficiently separated in phase space, they should begin to evolve independently from one another, the process known as decoherence. Decoherence is not accounted for in the standard surface hopping algorithm and leads to internal inconsistency. FSSH is designed to ensure that at any time, the fraction of classical trajectories evolving on each quantum state is equal to the average quantum probability for that state. However, in many systems this internal consistency requirement is violated. Treating decoherence is an inherent problem that can be addressed by implementing some form of decoherence correction to the standard FSSH algorithm. In this study, we have implemented two forms of the instantaneous decoherence procedure where coefficients are reinitialized following hops. We also test the energy-based decoherence correction (EDC) scheme proposed by Granucci et al. and a related version where the form of the decoherence time is taken from Truhlar's Coherent Switching with Decay of Mixing method. The sensitivity of the EDC results to changes in parameters is also evaluated. The application of these computationally inexpensive ad hoc methods is demonstrated in the simulation of nonradiative relaxation in two conjugated oligomer systems, specifically poly-phenylene vinylene and poly-phenylene ethynylene. We find that methods that have been used successfully for treating small systems do not necessarily translate to large polyatomic

  1. Ferroelectric-like metallic state in electron doped BaTiO3

    PubMed Central

    Fujioka, J.; Doi, A.; Okuyama, D.; Morikawa, D.; Arima, T.; Okada, K. N.; Kaneko, Y.; Fukuda, T.; Uchiyama, H.; Ishikawa, D.; Baron, A. Q. R.; Kato, K.; Takata, M.; Tokura, Y.

    2015-01-01

    We report that a ferroelectric-like metallic state with reduced anisotropy of polarization is created by the doping of conduction electrons into BaTiO3, on the bases of x-ray/electron diffraction and infrared spectroscopic experiments. The crystal structure is heterogeneous in nanometer-scale, as enabled by the reduced polarization anisotropy. The enhanced infrared intensity of soft phonon along with the resistivity reduction suggests the presence of unusual electron-phonon coupling, which may be responsible for the emergent ferroelectric structure compatible with metallic state. PMID:26289749

  2. The spectroscopy of singlets and triplets excites electronic states, spatial and electronic structure of hydrocarbons and quantum classifications in chemmotology

    NASA Astrophysics Data System (ADS)

    Obukhov, A. E.

    2016-12-01

    In this work we demonstrate the physical foundations of the spectroscopy of the grounds states: E- and X-ray, (RR) Raman scattering the NMR 1H and 13C and IR-, EPR- absorption and the singlets and triplets electronic excited states in the multinuclear hydrocarbons in chemmotology. The parameters of UV-absorption, RR-Raman scattering of light, the fluorescence and the phosphorescence and day-lasers at the pumping laser and lamp, OLEDs and OTETs- are measurements. The spectral-energy properties are briefly studied. The quantum-chemical LCAO-MO SCF expanded-CI PPP/S and INDO/S methods in the electronic and spatial structure hidrocarbons are considered.

  3. Differential cross sections for intermediate-energy electron scattering from α-tetrahydrofurfuryl alcohol: Excitation of electronic-states

    SciTech Connect

    Chiari, L.; Jones, D. B.; Thorn, P. A.; Pettifer, Z.; Duque, H. V.; Silva, G. B. da; Limão-Vieira, P.; Duflot, D.; Hubin-Franskin, M.-J.; Delwiche, J.; Blanco, F.; García, G.; and others

    2014-07-14

    We report on measurements of differential cross sections (DCSs) for electron impact excitation of a series of Rydberg electronic-states in α-tetrahydrofurfuryl alcohol (THFA). The energy range of these experiments was 20–50 eV, while the scattered electron was detected in the 10°–90° angular range. There are currently no other experimental data or theoretical computations against which we can directly compare the present measured results. Nonetheless, we are able to compare our THFA DCSs with earlier cross section measurements for Rydberg-state electronic excitation for tetrahydrofuran, a similar cyclic ether, from Do et al. [J. Chem. Phys. 134, 144302 (2011)]. In addition, “rotationally averaged” elastic DCSs, calculated using our independent atom model with screened additivity rule correction approach are also reported. Those latter results give integral cross sections consistent with the optical theorem, and supercede those from the only previous study of Milosavljević et al. [Eur. Phys. J. D 40, 107 (2006)].

  4. CONDENSED MATTER: ELECTRONIC STRUCTURE, ELECTRICAL, MAGNETIC, AND OPTICAL PROPERTIES: Electronic States of Elliptical Quantum Rings Subjected to a Magnetic Field

    NASA Astrophysics Data System (ADS)

    Li, Hai-Tao; Liu, Li-Zhe; Liu, Jian-Jun

    2008-11-01

    We calculate the energy states and Aharonov-Bohm oscillations of an electron in elliptical quantum rings in the presence of a uniform magnetic Geld by using an exact numerical diagonalization. The calculated results show that the elliptical quantum rings are flatter, larger amplitudes and periods of the Aharonov-Bohm oscillations are observed. In addition, in the limits of a circular quantum ring, the results of our approach are in good agreement with those of earlier theories.

  5. Electron impact excitation and dissociation of N2 via the b 1Pi(u) state

    NASA Technical Reports Server (NTRS)

    Ratliff, J. M.; James, G. K.; Trajmar, S.; Ajello, J. M.; Shemansky, D. E.

    1991-01-01

    Electron impact excitation of the b 1Pi(u) state in N2 plays a prominent role in the dissociation of the molecule and thus in the production of atomic nitrogen in planetary atmospheres. Electron impact excitation cross sections combined with electron-impact-induced fluorescence measurements can yield the corresponding dissociation cross sections. Serious discrepancies exist among excitation cross sections reported in the literature. To clarify the situation, these cross sections were measured at two impact energies using electron energy loss spectroscopy. The new results are in agreement with recent values deduced from optical measurements and fall midway between previous results which are too high or low by factors of 2.

  6. Steady-state hollow electron temperature profiles in the Rijnhuizen Tokamak Project

    SciTech Connect

    Hogeweij, G.M.; Oomens, A.A.; Barth, C.J.; Beurskens, M.N.; Chu, C.C.; van Gelder, J.F.; Lok, J.; Lopes Cardozo, N.J.; Pijper, F.J.; Polman, R.W.; Rommers, J.H.

    1996-01-01

    In the Rijnhuizen Tokamak Project steady-state hollow electron temperature ({ital T}{sub {ital e}}) profiles have been sustained with strong off-axis electron cyclotron heating, creating a region of reversed magnetic shear. In this region the effective electron thermal diffusivity ({chi}{sub {ital e}}{sup {ital pb}}) is close to neoclassical in high density plasmas. For medium density, {chi}{sub {ital e}}{sup {ital pb}} is lower than neoclassical and may even be negative, indicating that off-diagonal elements in the transport matrix drive an electron heat flux up the {ital T}{sub {ital e}} gradient. {copyright} {ital 1996 The American Physical Society.}

  7. Electronic and structural ground state of heavy alkali metals at high pressure

    DOE PAGES

    Fabbris, G.; Lim, J.; Veiga, L. S. I.; ...

    2015-02-17

    Here, alkali metals display unexpected properties at high pressure, including emergence of low symmetry crystal structures, that appear to occur due to enhanced electronic correlations among the otherwise nearly-free conduction electrons. We investigate the high pressure electronic and structural ground state of K, Rb, and Cs using x-ray absorption spectroscopy and x-ray diffraction measurements together with ab initio theoretical calculations. The sequence of phase transitions under pressure observed at low temperature is similar in all three heavy alkalis except for the absence of the oC84 phase in Cs. Both the experimental and theoretical results point to pressure-enhanced localization of themore » valence electrons characterized by pseudo-gap formation near the Fermi level and strong spd hybridization. Although the crystal structures predicted to host magnetic order in K are not observed, the localization process appears to drive these alkalis closer to a strongly correlated electron state.« less

  8. Electronic and structural ground state of heavy alkali metals at high pressure

    SciTech Connect

    Fabbris, G.; Lim, J.; Veiga, L. S. I.; Haskel, D.; Schilling, J. S.

    2015-02-17

    Here, alkali metals display unexpected properties at high pressure, including emergence of low symmetry crystal structures, that appear to occur due to enhanced electronic correlations among the otherwise nearly-free conduction electrons. We investigate the high pressure electronic and structural ground state of K, Rb, and Cs using x-ray absorption spectroscopy and x-ray diffraction measurements together with ab initio theoretical calculations. The sequence of phase transitions under pressure observed at low temperature is similar in all three heavy alkalis except for the absence of the oC84 phase in Cs. Both the experimental and theoretical results point to pressure-enhanced localization of the valence electrons characterized by pseudo-gap formation near the Fermi level and strong spd hybridization. Although the crystal structures predicted to host magnetic order in K are not observed, the localization process appears to drive these alkalis closer to a strongly correlated electron state.

  9. Fabrication and characterization of solid-state nanopores using a field emission scanning electron microscope

    SciTech Connect

    Chang Hung; Iqbal, Samir M.; Stach, Eric A.; King, Alexander H.; Zaluzec, Nestor J.; Bashir, Rashid

    2006-03-06

    The fabrication of solid-state nanopores using the electron beam of a transmission electron microscope (TEM) has been reported in the past. Here, we report a similar method to fabricate solid-state nanopores using the electron source of a conventional field-emission scanning electron microscope (FESEM) instead. Micromachining was used to create initial pore diameters between 50 nm and 200 nm, and controlled pore shrinking to sub 10 nm diameters was performed subsequently during in situ processing in the FESEM. Noticeably, different shrinking behavior was observed when using irradiation from the electron source of the FESEM than the TEM. Unlike previous reports of TEM mediated pore shrinkage, the mechanism of pore shrinkage when using the FESEM could be a result of surface defects generated by radiolysis and subsequent motion of silicon atoms to the pore periphery.

  10. Cyclic electron flow is redox-controlled but independent of state transition

    PubMed Central

    Takahashi, Hiroko; Clowez, Sophie; Wollman, Francis-André; Vallon, Olivier; Rappaport, Fabrice

    2013-01-01

    Photosynthesis is the biological process that feeds the biosphere with reduced carbon. The assimilation of CO2 requires the fine tuning of two co-existing functional modes: linear electron flow, which provides NADPH and ATP, and cyclic electron flow, which only sustains ATP synthesis. Although the importance of this fine tuning is appreciated, its mechanism remains equivocal. Here we show that cyclic electron flow as well as formation of supercomplexes, thought to contribute to the enhancement of cyclic electron flow, are promoted in reducing conditions with no correlation with the reorganization of the thylakoid membranes associated with the migration of antenna proteins towards Photosystems I or II, a process known as state transition. We show that cyclic electron flow is tuned by the redox power and this provides a mechanistic model applying to the entire green lineage including the vast majority of the cases in which state transition only involves a moderate fraction of the antenna. PMID:23760547

  11. Characterization of adsorption and electronic excited states of quercetin on titanium dioxide nanoparticles

    NASA Astrophysics Data System (ADS)

    Zdyb, Agata; Krawczyk, Stanisław

    2016-03-01

    Adsorption of quercetin on colloidal titanium dioxide nanoparticles in ethanol and its excited-state electronic structure were investigated by means of electronic and vibrational spectroscopies. The changes in electronic charge redistribution as reflected by the dipole moment difference, ∆μ, between the ground and excited electronic states were measured with electroabsorption spectroscopy and analyzed using results of TD DFT computations. Adsorption of quercetin causes a red shift of its absorption spectrum. Raman spectra of quercetin analyzed with reference to analogous data for morin indicate binding of quercetin through the hydroxy groups of the catechol moiety. The difference dipole moment, which is 5.5 D in free quercetin, increases to 11.8 D in opposite direction in adsorbed quercetin, and is associated with charge-transfer to the Ti atom. The computed transition energy, intensity, vector Δμ and molecular orbitals involved in the electronic transition at different molecular configurations indicate a bidentate chelating mode of binding of quercetin.

  12. Electron energy-loss spectroscopy of excited states of the pyridine molecules

    NASA Astrophysics Data System (ADS)

    Linert, Ireneusz; Zubek, Mariusz

    2016-04-01

    Electron energy-loss spectra of the pyridine, C5H5N, molecules in the gas phase have been measured to investigate electronic excitation in the energy range 3.5-10 eV. The applied wide range of residual electron energy and the scattering angle range from 10° to 180° enabled to differentiate between optically-allowed and -forbidden transitions. These measurements have allowed vertical excitation energies of the triplet excited states of pyridine to be determined and tentative assignments of these states to be proposed. Some of these states have not been identified in the previous works. 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.

  13. Electronic states at transition metal dichalcogenide lateral heterointerfaces

    NASA Astrophysics Data System (ADS)

    Avalos-Ovando, Oscar; Mastrogiuseppe, Diego; Ulloa, Sergio

    Materials with different band gaps are typically used to create heterostructures that enable band sculpting, depending on different shape and boundaries of the systems. These are used in diode lasers and high-speed transistors devices. Potential material candidates for such heterostructures at the monolayer level are the family of transition-metal dichalcogenides, MX2 (with M=Mo,W and X=S,Se), especially interesting materials with strong spin-orbit coupling and valley degrees of freedom. We consider lateral interfaces between pairs of these materials, and study the effect of different boundary geometries, motivated by recent experimental reports of the growth of such interfaces with different geometries. Using an effective 3-orbital tight-binding model, we focus our attention on monolayer ribbons and triangular flakes. We analyze the formation of edge/interface states for different gap nesting materials. We study the spatial distribution and orbital character of the wave functions throughout, as well as their dependence on interface termination. Supported by NSF DMR-1508325.

  14. Balancing Quality and Access: Reducing State Policy Barriers to Electronically Delivered Higher Education Programs.

    ERIC Educational Resources Information Center

    Johnstone, Sally M.

    This project was designed to increase student access by addressing Western states' regulations on higher education programs delivered electronically across state lines, and to develop and get region-wide agreement on basic quality standards for distance education programs. The project achieved agreement on a set of "Principles of Good…

  15. Electronic interconnects and devices with topological surface states and methods for fabricating same

    DOEpatents

    Yazdani, Ali; Ong, N. Phuan; Cava, Robert J.

    2017-04-04

    An interconnect is disclosed with enhanced immunity of electrical conductivity to defects. The interconnect includes a material with charge carriers having topological surface states. Also disclosed is a method for fabricating such interconnects. Also disclosed is an integrated circuit including such interconnects. Also disclosed is a gated electronic device including a material with charge carriers having topological surface states.

  16. Electronic interconnects and devices with topological surface states and methods for fabricating same

    SciTech Connect

    Yazdani, Ali; Ong, N. Phuan; Cava, Robert J.

    2016-05-03

    An interconnect is disclosed with enhanced immunity of electrical conductivity to defects. The interconnect includes a material with charge carriers having topological surface states. Also disclosed is a method for fabricating such interconnects. Also disclosed is an integrated circuit including such interconnects. Also disclosed is a gated electronic device including a material with charge carriers having topological surface states.

  17. Electronic Properties of Bimetallic Metal-Organic Frameworks (MOFs): Tailoring Density of Electronic States Through MOF Modularity.

    PubMed

    Dolgopolova, Ekaterina A; Brandt, Amy J; Ejegbavwo, Otega; Duke, Audrey S; Maddumapatabandi, Thathsara D; Galhenage, Randima P; Larson, Bryon W; Reid, Obadiah; Ammal, Salai Cheettu; Heyden, Andreas; Chandrashekhar, Mvs; Stavila, Vitalie; Chen, Donna A; Shustova, Natalia B

    2017-03-18

    Development of porous well-defined hybrid materials (e.g., metal-organic frameworks (MOFs)) will add a new dimension to a wide number of applications ranging from supercapacitors and electrodes to "smart" membranes and thermoelectrics. From this perspective, understanding and tailoring electronic properties of MOFs is a key fundamental challenge that could unlock the full potential of these materials. In this work, we focused on the fundamental insights responsible for the electronic properties of three distinct classes of bimetallic systems, Mx-yM'y-MOFs, MxM'y-MOFs, and Mx(ligand-M'y)-MOFs, in which the second metal (M') incorporation occurs through: (i) metal (M) replacement in the framework nodes (type I), (ii) metal node extension (type II), and (iii) metal coordination to the organic ligand (type III), respectively. We employed microwave conductivity, X-ray photoelectron spectroscopy, diffuse reflectance spectroscopy, powder X-ray diffraction, inductively coupled plasma atomic emission spec-troscopy, pressed-pellet conductivity, and theoretical modeling to shed light on the key factors responsible for the tunability of MOF electronic structures. Experimental pre-screening of MOFs was performed based on changes in the density of electronic states near the Fermi edge, which was used as a starting point for further selection of suitable MOFs. As a result, we demonstrated that tailoring of MOF electronic properties could be performed as a function of metal node engineering, framework topology, and/or presence of unsaturated metal sites while preserving framework porosity and structural integrity. These studies unveil the possible pathways for transforming the electronic properties of MOFs from insulating to semiconducting, as well as provide a blueprint for the development of hybrid porous materials with desirable electronic structures.

  18. Spectroscopic properties and potential energy curves of thirty-six electronic states of ZrH

    NASA Astrophysics Data System (ADS)

    Balasubramanian, K.; Wang, J. Z.

    1989-02-01

    Complete active space MCSCF (CASSCF) followed by second-order configuration interaction (SOCI) and relativistic configuration interaction (RCI) calculations are carried out on thirty-six electronic states of ZrH. The spectroscopic properties of these states are calculated which lie below 14000 cm -1. The ground state is found to be a 2Δ 3/2 state with low-lying 2Δ 5/2, 2Π 1/23/2 and 4Φ 3/2, 5/2, 7/2, 9/2 states. The dissociation energy of ZrH is calculated to be 2.64 eV. The ZrH bonding exhibits considerable ionic character and 4d5s5p hybridization in all the electronic states.

  19. Spectroscopic properties and potential energy curves of 28 electronic states of NbH

    NASA Astrophysics Data System (ADS)

    Das, Kalyan K.; Balasubramanian, K.

    1990-12-01

    State-averaged complete active space MCSCF (CASSCF) followed by second-order configuration interaction (SOCI) calculations are carried out on 28 low-lying electronic states of NbH. The ground state of NbH is found to be of 5Δ symmetry ( R e = 1.787 Å, ωe = 1750 cm -1, μe = 2.20 D, De = 2.67 eV) with a very low-lying excited state of 5Π symmetry ( Te = 720 cm -1). There are 14 low-lying bound states below 10 000 cm -1. Many dipole-allowed transitions are predicted for NbH which are yet to be observed. An intense 5Δ(II) ↔ 5Δ transition is predicted in the 21 000 ± 2000 cm -1 region. Mulliken population analyses reveal that the low-lying electronic states of NbH are very ionic (Nb +H -).

  20. Study on the steady operating state of a micro-pulse electron gun

    SciTech Connect

    Kui, Zhou; Xing, Luo; Xiangyang, Lu; Shengwen, Quan; Jifei, Zhao; Ziqin, Yang

    2014-09-15

    Micro-pulse electron gun (MPG) employs the basic concept of multipacting to produce high-current and short-pulse electron beams from a radio-frequency (RF) cavity. The concept of MPG has been proposed for more than two decades. However, the unstable operating state of MPG vastly obstructs its practical applications. This paper presents a study on the steady operating state of a micro-pulse electron gun with theory and experiments. The requirements for the steady operating state are proposed through the analysis of the interaction between the RF cavity and the beam load. Accordingly, a MPG cavity with the frequency of 2856 MHz has been designed, constructed, and tested. Some primary experiments have been finished. Both the unstable and stable operating states of the MPG have been observed. The stable output beam current has been detected at about 3.8 mA. Further experimental study is under way now.

  1. Theoretical calculations on electronic transitions for H/sub 3/, including Rydberg and transition state spectra

    SciTech Connect

    Petsalakis, I.D.; Theodorakopoulos, G.; Wright, J.S.

    1988-12-01

    MRD-CI calculations have been carried out on the ground and excited electronic states of H/sub 3/ for D/sub 3//sub h/, D/sub infinity//sub h/, C/sub infinity//sub v/, and C/sub 2//sub v/ geometries. Dipole transition moments between the various electronic states have been also obtained at the different geometries calculated. The present work provides accurate theoretical information relevant to the transition state spectroscopy of H+H/sub 2/ along a collinear path and also along a perpendicular path. In addition, the present work is the first all-electron configuration interaction treatment of the Rydberg states of H/sub 3/, and the results are in excellent agreement with the observed spectra.

  2. Low-lying singlet and triplet electronic states of RhB.

    PubMed

    Borin, Antonio Carlos; Gobbo, João Paulo

    2008-05-08

    The low-lying XSigma+, a3Delta, A1Delta, b3Sigma+, B1Pi, c3Pi, C1Phi, D1Sigma+, E1Pi, d3Phi, and e3Pi electronic states of RhB have been investigated at the ab initio level, using the multistate multiconfigurational second-order perturbation (MS-CASPT2) theory, with extended atomic basis sets and inclusion of scalar relativistic effects. Among the eleven electronic states included in this work, only three (the X1Sigma+, D1Sigma+, and E1Pi states) have been investigated experimentally. Potential energy curves, spectroscopic constants, dipole moments, binding energies, and chemical bonding aspects are presented for all electronic states.

  3. Exact many-electron ground states on the diamond Hubbard chain

    NASA Astrophysics Data System (ADS)

    Gulacsi, Zsolt; Kampf, Arno; Vollhardt, Dieter

    2008-03-01

    Exact ground states of interacting electrons on the diamond Hubbard chain in a magnetic field are constructed which exhibit a wide range of properties such as flat-band ferromagnetism, correlation induced metallic, half-metallic, or insulating behavior [1]. The properties of these ground states can be tuned by changing the magnetic flux, local potentials, or electron density.The results show that the studied simple one-dimensional structure displays remarkably complex physical properties. The virtue of tuning different ground states through external parameters points to new possibilities for the design of electronic devices which can switch between insulating or conducting and nonmagnetic or (fully or partially spin polarized) ferromagnetic states, open new routes for the design of spin-valve devices and gate induced ferromagnetism. [1] Z. Gulacsi, A. Kampf, D. Vollhardt, Phys. Rev. Lett. 99, 026404(2007).

  4. Enhanced electron attachment to Rydberg states in molecular hydrogen volume discharges

    SciTech Connect

    Pinnaduwage, L.A.; Ding, W.X.; McCorkle, D.L.; Lin, S.H.; Mebel, A.M.; Garscadden, A.

    1999-05-01

    We review recent studies on negative ion formation and studies in other areas that are relevant to the role of high-Rydberg states of H{sub 2} and H{sub 3} in hydrogen negative ion sources. Possible mechanisms for the formation of these excited states are discussed, including the formation of long-lived superexcited (core-excited) Rydberg states. Experimental evidence for negative ion formation via electron attachment to core-excited Rydberg states in a glow discharge apparatus is presented. An expression for the dissociative electron attachment rate constant for Rydberg molecules is derived based on electron capture by a Rydberg molecule due to polarization interaction. {copyright} {ital 1999 American Institute of Physics.}

  5. Electron impact excitation and assignment of the low-lying electronic states of N2O

    NASA Technical Reports Server (NTRS)

    Hall, R. I.; Chutjian, A.; Trajmar, S.

    1973-01-01

    Electron scattering spectra of nitrous oxide are reported in the 5- to 10-eV energy-loss range at scattering angles of 20, 30, 90, and 130 deg at a residual energy of 7.0 eV; and at residual energies of 10.0, 2.0, 1.0, 0.6, and 0.2 eV at a scattering angle of 90 deg. Several new distinct and overlapping continua are observed to lie in this energy-loss range. The experimental spectra are discussed in the light of semiempirical INDO calculations of Chutjian and Segal (1972) of the vertical transition energies of N2O. An assignment of the symmetries of the observed excitations consistent with the experimental and theoretical data is suggested.

  6. Detection of dark states in two-dimensional electronic photon-echo signals via ground-state coherence

    SciTech Connect

    Egorova, Dassia

    2015-06-07

    Several recent experiments report on possibility of dark-state detection by means of so called beating maps of two-dimensional photon-echo spectroscopy [Ostroumov et al., Science 340, 52 (2013); Bakulin et al., Ultrafast Phenomena XIX (Springer International Publishing, 2015)]. The main idea of this detection scheme is to use coherence induced upon the laser excitation as a very sensitive probe. In this study, we investigate the performance of ground-state coherence in the detection of dark electronic states. For this purpose, we simulate beating maps of several models where the excited-state coherence can be hardly detected and is assumed not to contribute to the beating maps. The models represent strongly coupled electron-nuclear dynamics involving avoided crossings and conical intersections. In all the models, the initially populated optically accessible excited state decays to a lower-lying dark state within few hundreds femtoseconds. We address the role of Raman modes and of interstate-coupling nature. Our findings suggest that the presence of low-frequency Raman active modes significantly increases the chances for detection of dark states populated via avoided crossings, whereas conical intersections represent a more challenging task.

  7. Probing Interfacial Electronic States in CdSe Quantum Dots using Second Harmonic Generation Spectroscopy

    DOE PAGES

    Doughty, Benjamin L.; Ma, Yingzhong; Shaw, Robert W

    2015-01-07

    Understanding and rationally controlling the properties of nanomaterial surfaces is a rapidly expanding field of research due to the dramatic role they play on the optical and electronic properties vital to light harvesting, emitting and detection technologies. This information is essential to the continued development of synthetic approaches designed to tailor interfaces for optimal nanomaterial based device performance. In this work, closely spaced electronic excited states in model CdSe quantum dots (QDs) are resolved using second harmonic generation (SHG) spectroscopy, and the corresponding contributions from surface species to these states are assessed. Two distinct spectral features are observed in themore » SHG spectra, which are not readily identified in linear absorption and photoluminescence excitation spectra. These features include a weak band at 395 6 nm, which coincides with transitions to the 2S1/2 1Se state, and a much more pronounced band at 423 4 nm arising from electronic transitions to the 1P3/2 1Pe state. Chemical modification of the QD surfaces through oxidation resulted in disappearance of the SHG band corresponding to the 1P3/2 1Pe state, indicating prominent surface contributions. Signatures of deep trap states localized on the surfaces of the QDs are also observed. We further find that the SHG signal intensities depend strongly on the electronic states being probed and their relative surface contributions, thereby offering additional insight into the surface specificity of SHG signals from QDs.« less

  8. Sulfur-Bridged Terthiophene Dimers: How Sulfur Oxidation State Controls Interchromophore Electronic Coupling.

    PubMed

    Cruz, Chad D; Christensen, Peter R; Chronister, Eric L; Casanova, David; Wolf, Michael O; Bardeen, Christopher J

    2015-10-07

    Symmetric dimers have the potential to optimize energy transfer and charge separation in optoelectronic devices. In this paper, a combination of optical spectroscopy (steady-state and time-resolved) and electronic structure theory is used to analyze the photophysics of sulfur-bridged terthiophene dimers. This class of dimers has the unique feature that the interchromophore (intradimer) electronic coupling can be modified by varying the oxidation state of the bridging sulfur from sulfide (S), to sulfoxide (SO), to sulfone (SO2). Photoexcitation leads to the formation of a delocalized charge resonance state (S1) that relaxes quickly (<10 ps) to a charge-transfer state (S1*). The amount of charge-transfer character in S1* can be enhanced by increasing the oxidation state of the bridging sulfur group as well as the solvent polarity. The S1* state has a decreased intersystem crossing rate when compared to monomeric terthiophene, leading to an enhanced photoluminescence quantum yield. Computational results indicate that electrostatic screening by the bridging sulfur electrons is the key parameter that controls the amount of charge-transfer character. Control of the sulfur bridge oxidation state provides the ability to tune interchromophore interactions in covalent assemblies without altering the molecular geometry or solvent polarity. This capability provides a new strategy for the design of functional supermolecules with applications in organic electronics.

  9. Probing Interfacial Electronic States in CdSe Quantum Dots using Second Harmonic Generation Spectroscopy

    SciTech Connect

    Doughty, Benjamin L.; Ma, Yingzhong; Shaw, Robert W

    2015-01-07

    Understanding and rationally controlling the properties of nanomaterial surfaces is a rapidly expanding field of research due to the dramatic role they play on the optical and electronic properties vital to light harvesting, emitting and detection technologies. This information is essential to the continued development of synthetic approaches designed to tailor interfaces for optimal nanomaterial based device performance. In this work, closely spaced electronic excited states in model CdSe quantum dots (QDs) are resolved using second harmonic generation (SHG) spectroscopy, and the corresponding contributions from surface species to these states are assessed. Two distinct spectral features are observed in the SHG spectra, which are not readily identified in linear absorption and photoluminescence excitation spectra. These features include a weak band at 395 6 nm, which coincides with transitions to the 2S1/2 1Se state, and a much more pronounced band at 423 4 nm arising from electronic transitions to the 1P3/2 1Pe state. Chemical modification of the QD surfaces through oxidation resulted in disappearance of the SHG band corresponding to the 1P3/2 1Pe state, indicating prominent surface contributions. Signatures of deep trap states localized on the surfaces of the QDs are also observed. We further find that the SHG signal intensities depend strongly on the electronic states being probed and their relative surface contributions, thereby offering additional insight into the surface specificity of SHG signals from QDs.

  10. Spectroscopic constants and potential energy curves for 16 electronic states of AsH

    NASA Astrophysics Data System (ADS)

    Balasubramanian, K.; Nannegari, V.

    1989-12-01

    Relativistic complete active space multi-configuration SCF (CASSCF) followed by full secondorder configuration interaction (SOCI) calculations are carried out on 16 electronic states of AsH. Among these are found 11 bound states for which spectroscopic constants are reported. Potential energy curves of all 16 electronic states are computed. Spectroscopic constants of nine new electronic states of AsH which are yet to be observed are reported. The experimentally observed predissociation and Λ-doubling in the A3Π ← X3Σ - system are explained based on theoretical potential energy curves. The dipole moment curves for the low-lying states are presented. The nature of the lowlying electronic states is analyzed through CI wave functions and Mulliken population analyses. The theoretical spectroscopic constants of the X3Σ - state are R e = 1.528 Å, ωe = 2194 cm -1, De = 2.71 eV, μe = 0.18 D, in excellent agreement with the experimental values of R e = 1.535 Å, ωe = 2130 cm -1, and De = 2.80 eV.

  11. Electronic Structure and Oxidation State Changes in the Mn (4) Ca Cluster of Photosystem II

    SciTech Connect

    Yano, J.; Pushkar, Y.; Messinger, J.; Bergmann, U.; Glatzel, P.; Yachandra, V.K.; /SLAC

    2012-08-17

    Oxygen-evolving complex (Mn{sub 4}Ca cluster) of Photosystem II cycles through five intermediate states (S{sub i}-states, i = 0-4) before a molecule of dioxygen is released. During the S-state transitions, electrons are extracted from the OEC, either from Mn or alternatively from a Mn ligand. The oxidation state of Mn is widely accepted as Mn{sub 4}(III{sub 2},IV{sub 2}) and Mn{sub 4}(III,IV{sub 3}) for S{sub 1} and S{sub 2} states, while it is still controversial for the S{sub 0} and S{sub 3} states. We used resonant inelastic X-ray scattering (RIXS) to study the electronic structure of Mn{sub 4}Ca complex in the OEC. The RIXS data yield two-dimensional plots that provide a significant advantage by obtaining both K-edge pre-edge and L-edge-like spectra (metal spin state) simultaneously. We have collected data from PSII samples in the each of the S-states and compared them with data from various inorganic Mn complexes. The spectral changes in the Mn 1s2p{sub 3/2} RIXS spectra between the S-states were compared to those of the oxides of Mn and coordination complexes. The results indicate strong covalency for the electronic configuration in the OEC, and we conclude that the electron is transferred from a strongly delocalized orbital, compared to those in Mn oxides or coordination complexes. The magnitude for the S{sub 0} to S{sub 1}, and S{sub 1} to S{sub 2} transitions is twice as large as that during the S{sub 2} to S{sub 3} transition, indicating that the electron for this transition is extracted from a highly delocalized orbital with little change in charge density at the Mn atoms.

  12. Electronic Structure and Oxidation State Changes in the Mn4Ca Cluster of Photosystem II

    SciTech Connect

    Yano, Junko; Pushkar, Yulia; Messinger, Johannes; Bergmann, Uwe; Glatzel, Pieter; Yachandra, Vittal K

    2007-08-03

    Oxygen-evolving complex (Mn4Ca cluster) of Photosystem II cycles through five intermediate states (Si-states, i =0-4) before a molecule of dioxygen is released. During the S-state transitions, electrons are extracted from the OEC, either from Mn or alternatively from a Mn ligand. The oxidation state of Mn is widely accepted as Mn4(III2,IV2) and Mn4(III,IV3) for S1 and S2 states, while it is still controversial for the S0 and S3 states. We used resonant inelastic X-ray scattering (RIXS) to study the electronic structure of Mn4Ca complex in the OEC. The RIXS data yield two-dimensional plots that provide a significant advantage by obtaining both K-edge pre-edge and L-edge-like spectra (metal spin state) simultaneously. We have collected data from PSII samples in the each of the S-states and compared them with data from various inorganic Mncomplexes. The spectral changes in the Mn 1s2p3/2 RIXS spectra between the S-states were compared to those of the oxides of Mn and coordination complexes. The results indicate strong covalency for the electronic configuration in the OEC, and we conclude that the electron is transferred from a strongly delocalized orbital, compared to those in Mn oxides or coordination complexes. The magnitude for the S0 to S1, and S1 to S2 transitions is twice as large as that during the S2 to S3 transition, indicating that the electron for this transition is extracted from a highly delocalized orbital with little change in charge density at the Mn atoms.

  13. 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

  14. Configuration interaction with Kohn Sham orbitals and their relation to excited electronic states

    NASA Astrophysics Data System (ADS)

    Bouř, Petr

    2001-09-01

    Kohn-Sham (KS) orbitals in CH 2, formaldehyde and acetone molecules were used as reference states for configuration interaction (CI) instead of the usual Hartree-Fock (HF) orbitals. A little difference in overall accuracy of electronic excitation energies was found between these schemes. However, analysis of the wave functions indicated that Slater determinant with the KS orbitals is more suitable for construction of the electronic states. Typically, the main expansion coefficients for the CI/KS procedure were closer to unity than those for HF. The difference was most pronounced for the lowest-energy transitions, while the two methods provided more comparable results for the higher-energy states. Similar behaviour of singlet and triplet states was observed. The results justify the common practice of using the KS determinant as a wave function, for example in sum-over-states theories.

  15. Theoretical Study of Tautomerization Reactions for the Ground and First Excited Electronic States of Adenine

    NASA Technical Reports Server (NTRS)

    Salter, Latasha M.; Chaban, Galina M.; Kwak, Dochan (Technical Monitor)

    2002-01-01

    Geometrical structures and energetic properties for different tautomers of adenine are calculated in this study, using multi-configurational wave functions. Both the ground and the lowest singlet excited state potential energy surfaces are studied. Four tautomeric forms are considered, and their energetic order is found to be different on the ground and the excited state potential energy surfaces. Minimum energy reaction paths are obtained for hydrogen atom transfer (tautomerization) reactions in the ground and the lowest excited electronic states. It is found that the barrier heights and the shapes of the reaction paths are different for the ground and the excited electronic states, suggesting that the probability of such tautomerization reaction is higher on the excited state potential energy surface. This tautomerization process should become possible in the presence of water or other polar solvent molecules and should play an important role in the photochemistry of adenine.

  16. Electron impact ionization of helium from its ground and metastable states

    NASA Astrophysics Data System (ADS)

    Zhang-jin, Chen; Ke-zun, Xu

    1999-05-01

    The triple differential cross sections for the ionization of helium from its ground state 1 1S and metastable states 2 1S and 2 3S in coplanar asymmetric geometry by 150, 250 and 400 eV electrons have been calculated in the BBK model. The present results are compared with the experimental data and/or the other theoretical ones. It has been found that the structures for the metastable states differ markedly from those for the ground state. The collision mechanisms for the new structures appearing in the cross sections for the ionization from metastable states have been analysed. And it has been shown how the intensity of recoil peak changes due to the size of the electron orbital. In addition, the optimal kinematical situations for the cross sections are explored for future experiment.

  17. Spectroscopic Properties and Potential Energy Curves for 21 Electronic States of CrH

    NASA Astrophysics Data System (ADS)

    Dai, D. G.; Balasubramanian, K.

    1993-10-01

    Spectroscopic constants and potential energy curves of 21 electronic states of CrH are obtained using the all-electron complete active space multiconfiguration self-consistent field (CASMCSCF) followed by first-order configuration interaction (FOCI) and full second-order CI (SOCI) and multireference CI including Rydberg states calculations. The ground state of CrH is found to be of 6Σ+ symmetry with re = 1.690 Å, ωe = 1592 cm-1, De = 2.11 eV, and μe = 3.864 D at the SOCI level. Several optical transitions for CrH are predicted. Our computations support the reassignment of the state perturbing the A-X system to 4Σ+ suggested by Ram et al. Our computed spectroscopic constants for the A, X, and a 4Σ+ state are in excellent agreement with the experimental values reported by Ram et al.

  18. Excited state X-ray absorption spectroscopy: Probing both electronic and structural dynamics

    NASA Astrophysics Data System (ADS)

    Neville, Simon P.; Averbukh, Vitali; Ruberti, Marco; Yun, Renjie; Patchkovskii, Serguei; Chergui, Majed; Stolow, Albert; Schuurman, Michael S.

    2016-10-01

    We investigate the sensitivity of X-ray absorption spectra, simulated using a general method, to properties of molecular excited states. Recently, Averbukh and co-workers [M. Ruberti et al., J. Chem. Phys. 140, 184107 (2014)] introduced an efficient and accurate L 2 method for the calculation of excited state valence photoionization cross-sections based on the application of Stieltjes imaging to the Lanczos pseudo-spectrum of the algebraic diagrammatic construction (ADC) representation of the electronic Hamiltonian. In this paper, we report an extension of this method to the calculation of excited state core photoionization cross-sections. We demonstrate that, at the ADC(2)x level of theory, ground state X-ray absorption spectra may be accurately reproduced, validating the method. Significantly, the calculated X-ray absorption spectra of the excited states are found to be sensitive to both geometric distortions (structural dynamics) and the electronic character (electronic dynamics) of the initial state, suggesting that core excitation spectroscopies will be useful probes of excited state non-adiabatic dynamics. We anticipate that the method presented here can be combined with ab initio molecular dynamics calculations to simulate the time-resolved X-ray spectroscopy of excited state molecular wavepacket dynamics.

  19. Excited state X-ray absorption spectroscopy: Probing both electronic and structural dynamics.

    PubMed

    Neville, Simon P; Averbukh, Vitali; Ruberti, Marco; Yun, Renjie; Patchkovskii, Serguei; Chergui, Majed; Stolow, Albert; Schuurman, Michael S

    2016-10-14

    We investigate the sensitivity of X-ray absorption spectra, simulated using a general method, to properties of molecular excited states. Recently, Averbukh and co-workers [M. Ruberti et al., J. Chem. Phys. 140, 184107 (2014)] introduced an efficient and accurate L(2) method for the calculation of excited state valence photoionization cross-sections based on the application of Stieltjes imaging to the Lanczos pseudo-spectrum of the algebraic diagrammatic construction (ADC) representation of the electronic Hamiltonian. In this paper, we report an extension of this method to the calculation of excited state core photoionization cross-sections. We demonstrate that, at the ADC(2)x level of theory, ground state X-ray absorption spectra may be accurately reproduced, validating the method. Significantly, the calculated X-ray absorption spectra of the excited states are found to be sensitive to both geometric distortions (structural dynamics) and the electronic character (electronic dynamics) of the initial state, suggesting that core excitation spectroscopies will be useful probes of excited state non-adiabatic dynamics. We anticipate that the method presented here can be combined with ab initio molecular dynamics calculations to simulate the time-resolved X-ray spectroscopy of excited state molecular wavepacket dynamics.

  20. Spatially inhomogeneous electron state deep in the extreme quantum limit of strontium titanate.

    PubMed

    Bhattacharya, Anand; Skinner, Brian; Khalsa, Guru; Suslov, Alexey V

    2016-09-29

    When an electronic system is subjected to a sufficiently strong magnetic field that the cyclotron energy is much larger than the Fermi energy, the system enters the extreme quantum limit (EQL) and becomes susceptible to a number of instabilities. Bringing a three-dimensional electronic system deeply into the EQL can be difficult however, since it requires a small Fermi energy, large magnetic field, and low disorder. Here we present an experimental study of the EQL in lightly-doped single crystals of strontium titanate. Our experiments probe deeply into the regime where theory has long predicted an interaction-driven charge density wave or Wigner crystal state. A number of interesting features arise in the transport in this regime, including a striking re-entrant nonlinearity in the current-voltage characteristics. We discuss these features in the context of possible correlated electron states, and present an alternative picture based on magnetic-field induced puddling of electrons.

  1. Spatially inhomogeneous electron state deep in the extreme quantum limit of strontium titanate

    NASA Astrophysics Data System (ADS)

    Bhattacharya, Anand; Skinner, Brian; Khalsa, Guru; Suslov, Alexey V.

    2016-09-01

    When an electronic system is subjected to a sufficiently strong magnetic field that the cyclotron energy is much larger than the Fermi energy, the system enters the extreme quantum limit (EQL) and becomes susceptible to a number of instabilities. Bringing a three-dimensional electronic system deeply into the EQL can be difficult however, since it requires a small Fermi energy, large magnetic field, and low disorder. Here we present an experimental study of the EQL in lightly-doped single crystals of strontium titanate. Our experiments probe deeply into the regime where theory has long predicted an interaction-driven charge density wave or Wigner crystal state. A number of interesting features arise in the transport in this regime, including a striking re-entrant nonlinearity in the current-voltage characteristics. We discuss these features in the context of possible correlated electron states, and present an alternative picture based on magnetic-field induced puddling of electrons.

  2. Manifestation of topological surface electron states in the photoelectromagnetic effect induced by terahertz laser radiation

    NASA Astrophysics Data System (ADS)

    Galeeva, A. V.; Egorova, S. G.; Chernichkin, V. I.; Tamm, M. E.; Yashina, L. V.; Rumyantsev, V. V.; Morozov, S. V.; Plank, H.; Danilov, S. N.; Ryabova, L. I.; Khokhlov, D. R.

    2016-09-01

    We demonstrate that measurements of the photoelectromagnetic effect using terahertz laser radiation may provide a unique opportunity to discriminate between the topological surface states and other highly conductive surface electron states. We performed a case study of mixed (Bi{}1-xIn x )2Se3 crystals undergoing a topological phase transformation due to the transition from the inverse to the direct electron energy spectrum in the crystal bulk at variation of the composition x. We show that for the topological insulator phase, the photoelectromagnetic effect amplitude is defined by the number of incident radiation quanta, whereas for the trivial insulator phase, it depends on the power in a laser pulse irrespective of its wavelength. We assume that such behavior is attributed to a strong damping of the electron-electron interaction in the topological insulator phase compared to the trivial insulator.

  3. Spatially inhomogeneous electron state deep in the extreme quantum limit of strontium titanate

    SciTech Connect

    Bhattacharya, Anand; Skinner, Brian; Khalsa, Guru; Suslov, Alexey V.

    2016-09-29

    When an electronic system is subjected to a sufficiently strong magnetic field that the cyclotron energy is much larger than the Fermi energy, the system enters the extreme quantum limit (EQL) and becomes susceptible to a number of instabilities. Bringing a three-dimensional electronic system deeply into the EQL can be difficult however, since it requires a small Fermi energy, large magnetic field, and low disorder. Here we present an experimental study of the EQL in lightly-doped single crystals of strontium titanate. Our experiments probe deeply into the regime where theory has long predicted an interaction-driven charge density wave or Wigner crystal state. A number of interesting features arise in the transport in this regime, including a striking re-entrant nonlinearity in the current-voltage characteristics. As a result, we discuss these features in the context of possible correlated electron states, and present an alternative picture based on magnetic-field induced puddling of electrons.

  4. Ground state of a hydrogen ion molecule immersed in an inhomogeneous electron gas

    NASA Astrophysics Data System (ADS)

    Diaz-Valdes, J.; Gutierrez, F. A.; Matamala, A. R.; Denton, C. D.; Vargas, P.; Valdes, J. E.

    2007-01-01

    In this work we have calculated the ground state energy of the hydrogen molecule, H2+, immersed in the highly inhomogeneous electron gas around a metallic surface within the local density approximation. The molecule is perturbed by the electron density of a crystalline surface of Au <1 0 0> with the internuclear axis parallel to the surface. The surface spatial electron density is calculated through a linearized band structure method (LMTO-DFT). The ground state of the molecule-ion was calculated using the Born-Oppenheimer approximation for a fixed-ion while the screening effects of the inhomogeneous electron gas are depicted by a Thomas-Fermi like electrostatic potential. We found that within our model the molecular ion dissociates at the critical distance of 2.35 a.u. from the first atomic layer of the solid.

  5. Spatially inhomogeneous electron state deep in the extreme quantum limit of strontium titanate

    PubMed Central

    Bhattacharya, Anand; Skinner, Brian; Khalsa, Guru; Suslov, Alexey V.

    2016-01-01

    When an electronic system is subjected to a sufficiently strong magnetic field that the cyclotron energy is much larger than the Fermi energy, the system enters the extreme quantum limit (EQL) and becomes susceptible to a number of instabilities. Bringing a three-dimensional electronic system deeply into the EQL can be difficult however, since it requires a small Fermi energy, large magnetic field, and low disorder. Here we present an experimental study of the EQL in lightly-doped single crystals of strontium titanate. Our experiments probe deeply into the regime where theory has long predicted an interaction-driven charge density wave or Wigner crystal state. A number of interesting features arise in the transport in this regime, including a striking re-entrant nonlinearity in the current–voltage characteristics. We discuss these features in the context of possible correlated electron states, and present an alternative picture based on magnetic-field induced puddling of electrons. PMID:27680386

  6. Studying dissociative electron attachment through formation of heavy-Rydberg ion-pair states

    NASA Astrophysics Data System (ADS)

    Kelley, Michael; Buathong, Sitti; Dunning, F. Barry

    2016-05-01

    Following dissociative electron transfer in collisions between Rydberg atoms and electron-attaching targets, it is possible for the resulting pair of ions to remain electrostatically bound, forming heavy-Rydberg ion-pair states. Precise measurement of the velocity distributions of such ion-pair states provides information concerning the dissociation dynamics of the excited intermediates initially created by electron transfer. Here, electric-field-induced dissociation is used to detect the product ion pairs and observe their velocity distributions. These distributions are analyzed with the aid of a Monte Carlo collision code that models the electron transfer. Measurements with a number of different target species show that through this analysis, dissociation energetics, the branching ratios into different dissociation products, and the lifetimes of the excited intermediates can be examined. Research supported by the Robert A. Welch Foundation.

  7. 26 CFR 5f.103-2 - Public approval of industrial development bonds.

    Code of Federal Regulations, 2013 CFR

    2013-04-01

    ... State constitution, charter or statute) by or under which the governmental unit is created, (B... the United States, the District of Columbia, or any political subdivision thereof. The term “political... governmental unit within a State (counting the State as a governmental unit within such State), then any one...

  8. Non-steady-state transport of superthermal electrons in the plasmasphere

    NASA Technical Reports Server (NTRS)

    Khazanov, George V.; Liemohn, Michael W.; Gombosi, Tamas I.; Nagy, Andrew F.

    1993-01-01

    Numerical solutions to the time-dependent kinetic equation, which describes the transport of superthermal electrons in the splasmasphere between the two conjugate ionospheres, are presented. The model calculates the distribution function as a function of time, field-aligned distance, energy, and pitch-angle. The processes of refilling, depleting, and establishing steady-state conditions of superthermal electrons in the plasmasphere are discussed.

  9. FAST TRACK COMMUNICATION: Fragmentation pathways for selected electronic states of the acetylene dication

    NASA Astrophysics Data System (ADS)

    Osipov, T.; Rescigno, T. N.; Weber, T.; Miyabe, S.; Jahnke, T.; Alnaser, A. S.; Hertlein, M. P.; Jagutzki, O.; Schmidt, L. Ph H.; Schöffler, M.; Foucar, L.; Schössler, S.; Havermeier, T.; Odenweller, M.; Voss, S.; Feinberg, B.; Landers, A. L.; Prior, M. H.; Dörner, R.; Cocke, C. L.; Belkacem, A.

    2008-05-01

    Coincident measurement of the Auger electron and fragment ion momenta emitted after carbon core-level photoionization of acetylene has yielded new understanding of how the dication fragments. Ab initio calculations and experimental data, including body-frame Auger angular distributions, are used to identify the parent electronic states and together yield a comprehensive map of the dissociation pathways which include surface crossings and barriers to direct dissociation. The Auger angular distributions for certain breakup channels show evidence of core-hole localization.

  10. Electronic precursor states of the charge density wave in NbSe 3

    NASA Astrophysics Data System (ADS)

    Schäfer, J.; Rotenberg, Eli; Kevan, S. D.; Blaha, P.; Claessen, R.; Thorne, R. E.

    2002-03-01

    The electron bands of the Peierls compound NbSe3 are mapped with angle-resolved photoemission. Data of the Fermi level crossings show the nesting condition responsible for the charge density wave along the one-dimensional axis. The instability with periodicity q=0.44 Å-1 induces a remnant backfolding of the electron bands in the nominally metallic state high above the critical temperature.

  11. Dynamics of the Chemistry of Electronically Excited Atoms in Defined Quantum States.

    DTIC Science & Technology

    1978-05-01

    laser development . In essence, this research concerns itself with the elucidation of the role of electronic energy in affecting the chemistry or photochemistry of excited halogen atoms and molecules. While much is known about the dynamics of chemical and physical processes which are carried out on the lowest potential energy hypersurface correlating with reactants and products in their electronic ground state, relatively little is known about the dynamics of such phenomena as energy transfer and chemical reactivity on higher-lying potential

  12. Computing the Effects of Strain on Electronic States: A Survey of Methods and Issues

    DTIC Science & Technology

    2012-12-01

    Naval Research Laboratory (NRL) and the NEMO5 code (from Drs. Gerhard Klimeck and James Fonseca, Purdue University) to help in our understanding of...optoelectronics (7, 8). However, even where such effects are absent or negligible, strain still has important effects on the electronic properties ...the community of researchers with interest in accurately computing the electronic structure properties and, in particular, the excited state

  13. Electronic states of MgO: Spectroscopy, predissociation, and cold atomic Mg and O production

    SciTech Connect

    Maatouk, A.; Ben Houria, A.; Yazidi, O.; Jaidane, N.; Hochlaf, M.

    2010-10-14

    We used multiconfigurational methods and a large basis set to compute the potential energy curves of the valence and valence-Rydberg electronic states of MgO molecule. New bound electronic states are found. Using these highly correlated wave functions, we evaluated their mutual spin-orbit couplings and transition moment integrals. For the bound electronic states of MgO, we deduced an accurate set of spectroscopic constants that agree remarkably well with experimental results. Moreover, our potentials, transition moments, and spin-orbit coupling evolutions are incorporated into Fermi golden rule calculations to deduce the radiative lifetimes of MgO(B {sup 1}{Sigma}{sup +}) rovibrational levels and the natural lifetimes of MgO(A {sup 1}{Pi}) vibrational levels, where a good agreement is found with experimental values. Finally, we suggest new routes for the production of cold Mg and O atoms and cold MgO molecules.

  14. Exit charge state dependence of convoy electron production in heavy-ion solid collisions

    SciTech Connect

    Huelskoetter, H.P.; Burgdoerfer, J.; Sellin, I.A.

    1986-01-01

    The dependence of the yield of convoy electrons emitted near the forward direction in collisions involving fast ions and thin solid targets on the emergent projectile charge state is presented and described in terms of primary electron loss events in the solid. The data include a large array of projectiles, projectile energies and charge states, as well as targets ranging in thickness from the non-equilibrium well into the equilibrium thickness region. The description presented is consistent with other experimental and theoretical results indicating that the convoy electron production is closely linked to the ELC process observed in binary ion-atom collisions, with the dominant contribution to the convoy yield stemming from excited states of the projectiles. 22 refs., 3 figs.

  15. 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.

  16. Electronic transport characterization of silicon wafers by spatially resolved steady-state photocarrier radiometric imaging

    SciTech Connect

    Wang, Qian; Li, Bincheng

    2015-09-28

    Spatially resolved steady-state photocarrier radiometric (PCR) imaging technique is developed to characterize the electronic transport properties of silicon wafers. Based on a nonlinear PCR theory, simulations are performed to investigate the effects of electronic transport parameters (the carrier lifetime, the carrier diffusion coefficient, and the front surface recombination velocity) on the steady-state PCR intensity profiles. The electronic transport parameters of an n-type silicon wafer are simultaneously determined by fitting the measured steady-state PCR intensity profiles to the three-dimensional nonlinear PCR model. The determined transport parameters are in good agreement with the results obtained by the conventional modulated PCR technique with multiple pump beam radii.

  17. Decoherence of high-energy electrons in weakly disordered quantum Hall edge states

    NASA Astrophysics Data System (ADS)

    Nigg, Simon E.; Lunde, Anders Mathias

    2016-07-01

    We investigate theoretically the phase coherence of electron transport in edge states of the integer quantum Hall effect at filling factor ν =2 , in the presence of disorder and inter edge state Coulomb interaction. Within a Fokker-Planck approach, we calculate analytically the visibility of the Aharonov-Bohm oscillations of the current through an electronic Mach-Zehnder interferometer. In agreement with recent experiments, we find that the visibility is independent of the energy of the current-carrying electrons injected high above the Fermi sea. Instead, it is the amount of disorder at the edge that sets the phase space available for inter edge state energy exchange and thereby controls the visibility suppression.

  18. State-specific transport properties of partially ionized flows of electronically excited atomic gases

    NASA Astrophysics Data System (ADS)

    Istomin, V. A.; Kustova, E. V.

    2017-03-01

    State-to-state approach for theoretical study of transport properties in atomic gases with excited electronic degrees of freedom of both neutral and ionized species is developed. The dependence of atomic radius on the electronic configuration of excited atoms is taken into account in the transport algorithm. Different cutoff criteria for increasing atomic radius are discussed and the limits of applicability for these criteria are evaluated. The validity of a Slater-like model for the calculation of state-resolved transport coefficients in neutral and ionized atomic gases is shown. For ionized flows, a method of evaluation for effective cross-sections of resonant charge-transfer collisions is suggested. Accurate kinetic theory algorithms for modelling the state-specific transport properties are applied for the prediction of transport coefficients in shock heated flows. Based on the numerical observations, different distributions over electronic states behind the shock front are considered. For the Boltzmann-like distributions at temperatures greater than 14,000 K, an important effect of electronic excitation on the partial thermal conductivity and viscosity coefficients is found for both neutral and ionized atomic gases: increasing radius of excited atoms causes a strong decrease in these transport coefficients. Similarly, the presence of electronically excited states with increased atomic radii leads to reduced diffusion coefficients. Nevertheless the overall impact of increasing effective cross-sections on the transport properties just behind the shock front under hypersonic reentry conditions is found to be minor since the populations of high-lying electronic energy levels behind the shock waves are low.

  19. Adsorption and electronic states of morin on TiO2 nanoparticles

    NASA Astrophysics Data System (ADS)

    Zdyb, Agata; Krawczyk, Stanisław

    2014-10-01

    Low temperature Stark effect spectroscopy has been used to investigate the changes in the electronic charge distribution in the flavonoid morin caused by adsorption to colloidal TiO2 nanoparticles in ethanol. The differences in the permanent dipole moment, Δμ, and in polarizability, Δα, between the ground and excited state were determined. Adsorption causes an increase in both Δμ and Δα of morin but the vector Δμ remains nearly perpendicular to the Ti-dye direction, like in the free molecule. This picture of electron movement on electronic excitation is supported by semiempirical calculations. In contrast to other dyes adsorbed on TiO2, it indicates the indirect effect of chelated Ti atom on morin electronic structure which does not involve the atomic orbitals of the metal, and the electronic structure of adsorbed morin similar to that of the anion.

  20. Evolution of electronic states in n-type copper oxide superconductor via electric double layer gating.

    PubMed

    Jin, Kui; Hu, Wei; Zhu, Beiyi; Kim, Dohun; Yuan, Jie; Sun, Yujie; Xiang, Tao; Fuhrer, Michael S; Takeuchi, Ichiro; Greene, Richard L

    2016-05-25

    The occurrence of electrons and holes in n-type copper oxides has been achieved by chemical doping, pressure, and/or deoxygenation. However, the observed electronic properties are blurred by the concomitant effects such as change of lattice structure, disorder, etc. Here, we report on successful tuning the electronic band structure of n-type Pr2-xCexCuO4 (x = 0.15) ultrathin films, via the electric double layer transistor technique. Abnormal transport properties, such as multiple sign reversals of Hall resistivity in normal and mixed states, have been revealed within an electrostatic field in range of -2 V to + 2 V, as well as varying the temperature and magnetic field. In the mixed state, the intrinsic anomalous Hall conductivity invokes the contribution of both electron and hole-bands as well as the energy dependent density of states near the Fermi level. The two-band model can also describe the normal state transport properties well, whereas the carrier concentrations of electrons and holes are always enhanced or depressed simultaneously in electric fields. This is in contrast to the scenario of Fermi surface reconstruction by antiferromagnetism, where an anti-correlation is commonly expected.

  1. Evolution of electronic states in n-type copper oxide superconductor via electric double layer gating

    NASA Astrophysics Data System (ADS)

    Jin, Kui; Hu, Wei; Zhu, Beiyi; Kim, Dohun; Yuan, Jie; Sun, Yujie; Xiang, Tao; Fuhrer, Michael S.; Takeuchi, Ichiro; Greene, Richard. L.

    2016-05-01

    The occurrence of electrons and holes in n-type copper oxides has been achieved by chemical doping, pressure, and/or deoxygenation. However, the observed electronic properties are blurred by the concomitant effects such as change of lattice structure, disorder, etc. Here, we report on successful tuning the electronic band structure of n-type Pr2‑xCexCuO4 (x = 0.15) ultrathin films, via the electric double layer transistor technique. Abnormal transport properties, such as multiple sign reversals of Hall resistivity in normal and mixed states, have been revealed within an electrostatic field in range of ‑2 V to + 2 V, as well as varying the temperature and magnetic field. In the mixed state, the intrinsic anomalous Hall conductivity invokes the contribution of both electron and hole-bands as well as the energy dependent density of states near the Fermi level. The two-band model can also describe the normal state transport properties well, whereas the carrier concentrations of electrons and holes are always enhanced or depressed simultaneously in electric fields. This is in contrast to the scenario of Fermi surface reconstruction by antiferromagnetism, where an anti-correlation is commonly expected.

  2. Determination of ground and excited state dipole moments via electronic Stark spectroscopy: 5-methoxyindole.

    PubMed

    Wilke, Josefin; Wilke, Martin; Meerts, W Leo; Schmitt, Michael

    2016-01-28

    The dipole moments of the ground and lowest electronically excited singlet state of 5-methoxyindole have been determined by means of optical Stark spectroscopy in a molecular beam. The resulting spectra arise from a superposition of different field configurations, one with the static electric field almost parallel to the polarization of the exciting laser radiation, the other nearly perpendicular. Each field configuration leads to different intensities in the rovibronic spectrum. With an automated evolutionary algorithm approach, the spectra can be fit and the ratio of both field configurations can be determined. A simultaneous fit of two spectra with both field configurations improved the precision of the dipole moment determination by a factor of two. We find a reduction of the absolute dipole moment from 1.59(3) D to 1.14(6) D upon electronic excitation to the lowest electronically excited singlet state. At the same time, the dipole moment orientation rotates by 54(∘) showing the importance of the determination of the dipole moment components. The dipole moment in the electronic ground state can approximately be obtained from a vector addition of the indole and the methoxy group dipole moments. However, in the electronically excited state, vector addition completely fails to describe the observed dipole moment. Several reasons for this behavior are discussed.

  3. Simple relationship between oxidation state and electron affinity in gas-phase metal-oxo complexes.

    PubMed

    Waller, Sarah E; Ray, Manisha; Yoder, Bruce L; Jarrold, Caroline Chick

    2013-12-19

    The photoelectron spectra of WO3H(-) and WO2F(-) are presented and analyzed in the context of a series of previous similar measurements on MO(y)(-) (M = Mo, W; y = 0-3), MO4H(-) and AlMOy(-) (y ≤ 4) complexes. The electronic structures of the WO3H and WO2F anion and neutral complexes were investigated using the B3LYP hybrid density functional method. The spectra of WO3H(-), WO2F(-), and previously measured AlWO3(-) photoelectron spectra show that the corresponding neutrals, in which the transition metal centers are all in a +5 oxidation state, have comparable electron affinities. In addition, the electron affinities fit the general trend of monotonically increasing electron affinity with oxidation state, in spite of the WO3H(-), WO2F(-), and AlWO3(-) having closed shell ground states, suggesting that the oxidation state of the metal atom has more influence than shell closing on the electron affinity of these transition metal-oxo complexes. Results of DFT calculations suggest that the neutrals are pyramidal and the anions are planar. However, the barriers for inversion on the neutral surface are low, and attempts to generate simple Franck-Condon simulations based on simple normal coordinate displacement, ignoring the effects of inversion, are inadequate.

  4. Statistical theory of relaxation of high-energy electrons in quantum Hall edge states

    NASA Astrophysics Data System (ADS)

    Lunde, Anders Mathias; Nigg, Simon E.

    2016-07-01

    We investigate theoretically the energy exchange between the electrons of two copropagating, out-of-equilibrium edge states with opposite spin polarization in the integer quantum Hall regime. A quantum dot tunnel coupled to one of the edge states locally injects electrons at high energy. Thereby a narrow peak in the energy distribution is created at high energy above the Fermi level. A second downstream quantum dot performs an energy-resolved measurement of the electronic distribution function. By varying the distance between the two dots, we are able to follow every step of the energy exchange and relaxation between the edge states, even analytically under certain conditions. In the absence of translational invariance along the edge, e.g., due to the presence of disorder, energy can be exchanged by non-momentum-conserving two-particle collisions. For weakly broken translational invariance, we show that the relaxation is described by coupled Fokker-Planck equations. From these we find that relaxation of the injected electrons can be understood statistically as a generalized drift-diffusion process in energy space for which we determine the drift velocity and the dynamical diffusion parameter. Finally, we provide a physically appealing picture in terms of individual edge-state heating as a result of the relaxation of the injected electrons.

  5. Evolution of electronic states in n-type copper oxide superconductor via electric double layer gating

    PubMed Central

    Jin, Kui; Hu, Wei; Zhu, Beiyi; Kim, Dohun; Yuan, Jie; Sun, Yujie; Xiang, Tao; Fuhrer, Michael S.; Takeuchi, Ichiro; Greene, Richard. L.

    2016-01-01

    The occurrence of electrons and holes in n-type copper oxides has been achieved by chemical doping, pressure, and/or deoxygenation. However, the observed electronic properties are blurred by the concomitant effects such as change of lattice structure, disorder, etc. Here, we report on successful tuning the electronic band structure of n-type Pr2−xCexCuO4 (x = 0.15) ultrathin films, via the electric double layer transistor technique. Abnormal transport properties, such as multiple sign reversals of Hall resistivity in normal and mixed states, have been revealed within an electrostatic field in range of −2 V to + 2 V, as well as varying the temperature and magnetic field. In the mixed state, the intrinsic anomalous Hall conductivity invokes the contribution of both electron and hole-bands as well as the energy dependent density of states near the Fermi level. The two-band model can also describe the normal state transport properties well, whereas the carrier concentrations of electrons and holes are always enhanced or depressed simultaneously in electric fields. This is in contrast to the scenario of Fermi surface reconstruction by antiferromagnetism, where an anti-correlation is commonly expected. PMID:27221198

  6. Hyperfast time-resolved spectroscopy of electron correlation in excited states

    NASA Astrophysics Data System (ADS)

    Nicolaides, Cleanthes A.

    2007-06-01

    As a consequence of continuing developments in the science and technology of techniques that produce and control electromagnetic pulses with frequencies that are found in a broad part of the spectrum, from the ir to the soft X-rays, it is possible to have hyperfast pump-probe time delay spectroscopic techniques capable of time resolving the dynamics of various atomic and molecular systems involving excited states. In this context, it has been demonstrated via first principles solution of the time-dependent Schr"odinger equation (TDSE), that effects which are caused by strong electron correlations in excited states, including the process of autoionization and the formation of resonances, can be time-resolved on a time scale of attoseconds [1-3]. By extending the investigations to polyelectronic atoms, we have obtained new results for various time resolved processes associated with the photo-ejection of inner (2s) electrons and of two electrons (LM) from the thirteen electron atom of Aluminum and with the electron correlation beats in bound and autoionizind states of N^+3 and Al. The theory and computations account for the interference of direct double ionization, inner hole states and Auger decay [4]. [1] C. A. Nicolaides et al, J. Phys. B 35, L271 (2002). [2] Th. Mercouris et al, Phys. Rev. A 69, 032502 (2004). [3] Th. Mercouris, et al, Phys. Rev. A 75, 013407 (2007). [4] Th. Mercouris, Y. Komninos and C. A. Nicolaides, unpublished.

  7. Ab initio study on electronically excited states of lithium isocyanide, LiNC

    NASA Astrophysics Data System (ADS)

    Yasumatsu, Hisato; Jeung, Gwang-Hi

    2014-01-01

    The electronically excited states of the lithium isocyanide molecule, LiNC, were studied by means of ab initio calculations. The bonding nature of LiNC up to ∼10 eV is discussed on the basis of the potential energy surfaces according to the interaction between the ion-pair and covalent states. The ion-pair states are described by Coulomb attractive interaction in the long distance range, while the covalent ones are almost repulsive or bound with a very shallow potential dent. These two states interact each other to form adiabatic potential energy surfaces with non-monotonic change in the potential energy with the internuclear distance.

  8. Entanglement purification and concentration of electron-spin entangled states using quantum-dot spins in optical microcavities

    SciTech Connect

    Wang Chuan; Zhang Yong; Jin Guangsheng

    2011-09-15

    We present an entanglement purification protocol and an entanglement concentration protocol for electron-spin entangled states, resorting to quantum-dot spin and optical-microcavity-coupled systems. The parity-check gates (PCGs) constructed by the cavity-spin-coupling system provide a different method for the entanglement purification of electron-spin entangled states. This protocol can efficiently purify an electron ensemble in a mixed entangled state. The PCGs can also concentrate electron-spin pairs in less-entangled pure states efficiently. The proposed methods are more flexible as only single-photon detection and single-electron detection are needed.

  9. The role of electron equation of state in heating partition of protons in a collisionless plasma

    SciTech Connect

    Parashar, Tulasi N.; Vasquez, Bernard J.; Markovskii, Sergei A.

    2014-02-15

    One of the outstanding questions related to the solar wind is the heating of solar wind plasma. Addressing this question requires a self consistent treatment of the kinetic physics of a collisionless plasma. A hybrid code (with particle ions and fluid electrons) is one of the most convenient computational tools, which allows us to explore self consistent ion kinetics, while saving us computational time as compared to the full particle in cell codes. A common assumption used in hybrid codes is that of isothermal electrons. In this paper, we discuss the role that the equation of state for electrons could potentially play in determining the ion kinetics.

  10. 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.

  11. Electron transfer reactions for image and image-derived states in dielectric thin films.

    PubMed

    Jensen, E T; Sanche, L

    2008-08-21

    We have studied the cross section for electron trapping that occurs at the surfaces and interfaces of a variety of thin dielectric films (n-octane, methanol, n-butanol, and difluoromethane) that are grown on Kr buffer films. When such films are bombarded with electrons of very low incident energies (E less, similar 300 meV), charging cross sections up to the order of 10(-14) cm(2) are measured for submonolayer quantities of a variety of coadsorbed molecules: CH(3)I, CH(3)Br, CH(3)Cl, and CO(2). These huge cross sections are ascribed to the formation of image states at the dielectric film interfaces, which trap incoming electrons and, via coupling to the adsorbate electron affinity levels, dramatically enhance the capture probability. We have also shown that thin film dielectric layer structures can be created which display image-derived states, such as a "quantum well" in a sandwich structure with two "electron barrier" layers surrounding a Kr and adsorbate spacer film. These phenomena are shown to be of a general nature, occurring for a wide variety of molecular thin films, and depend on the dielectric constant and electron affinity of the selected species. We also report the absolute cross section for dissociative electron attachment of submonolayer CH(3)I adsorbed on Kr thin films.

  12. Special Issue of Solid-State Electronics, dedicated to EUROSOI-ULIS 2016

    NASA Astrophysics Data System (ADS)

    Sverdlov, Viktor; Selberherr, Siegfried

    2017-02-01

    The current special issue of Solid-State Electronics includes 29 extended papers presented at the 2016 Second Joint International EUROSOI Workshop and International Conference on Ultimate Integration on Silicon (EUROSOI-ULIS 2016) held in Wien, Austria, on January 25-27, 2016. The papers entering to the special issue have been selected by the EUROSOI-ULIS 2016 Technical Program Committee based on the excellence of abstracts submitted and presentations delivered at the conference. In order to comply with the high standards of Solid-State Electronics the manuscripts went through the standard reviewing procedure.

  13. The dressed states of an electron in a one-dimensional two δ -functions potential

    NASA Astrophysics Data System (ADS)

    Chirilã, C.; Boca, M.; Dinu, V.; Florescu, V.

    2003-11-01

    We study, in the framework of the high-frequency Floquet theory, the one-dimensional system consisting of an electron interacting with a symmetric two δ-functions potential in the presence of an intense monochromatic homogeneous electric field. Most of the results concern the attractive case. They include the dependence of the bound states energies of the dressed potential and of some of its resonances positions on the electric field parameter α_0 (the classical free electron quiver motion amplitude) and on the distance between the two centers and the description of the evolution from resonances to laser induced levels via two antibound states. The repulsive case is described briefly.

  14. Shape transitions in excited states of two-electron quantum dots in a magnetic field

    NASA Astrophysics Data System (ADS)

    Nazmitdinov, R. G.; Simonović, N. S.; Plastino, A. R.; Chizhov, A. V.

    2012-10-01

    We use entanglement to study shape transitions in two-electron axially symmetric parabolic quantum dots in a perpendicular magnetic field. At a specific magnetic field value the dot attains a spherical symmetry. The transition from the axial to the spherical symmetry manifests itself as a drastic change of the entanglement of the lowest state with zero angular momentum projection. While the electrons in such a state are always localized in the plane (x - y) before the transition point, after this point they become localized in the vertical direction.

  15. Time-evolution of electronic states in a Rashba anisotropic two-dimensional quantum dot

    NASA Astrophysics Data System (ADS)

    Amiri, F.; Shirkani, H.; Golshan, M. M.

    2011-10-01

    In this article we present the time evolution of the electronic spin and subbands states, of an electron in an anisotropic two dimensional Rashba quantum dot, to which a magnetic field of arbitrary strength is applied. We also explicitly include the confining (gate) effects as a two dimensional anisotropic harmonic oscillator. From the governing Hamiltonian we compute the time evolution of the initial state, leading to spin and subbands averages as functions of time. Our results indicate that the spin, on the average, precesses about the magnetic field, on an ellipse with intrinsic wobbling. The subbands populations, similar to the case of atom-photon interaction, follow the pattern of collapse-revivals.

  16. State laws prohibiting sales to minors and indoor use of electronic nicotine delivery systems--United States, November 2014.

    PubMed

    Marynak, Kristy; Holmes, Carissa Baker; King, Brian A; Promoff, Gabbi; Bunnell, Rebecca; McAfee, Timothy

    2014-12-12

    Electronic nicotine delivery systems (ENDS), including electronic cigarettes (e-cigarettes) and other devices such as electronic hookahs, electronic cigars, and vape pens, are battery-powered devices capable of delivering aerosolized nicotine and additives to the user. Experimentation with and current use of e-cigarettes has risen sharply among youths and adults in the United States. Youth access to and use of ENDS is of particular concern given the potential adverse effects of nicotine on adolescent brain development. Additionally, ENDS use in public indoor areas might passively expose bystanders (e.g., children, pregnant women, and other nontobacco users) to nicotine and other potentially harmful constituents. ENDS use could have the potential to renormalize tobacco use and complicate enforcement of smoke-free policies. State governments can regulate the sales of ENDS and their use in indoor areas where nonusers might be involuntarily exposed to secondhand aerosol. To learn the current status of state laws regulating the sales and use of ENDS, CDC assessed state laws that prohibit ENDS sales to minors and laws that include ENDS use in conventional smoking prohibitions in indoor areas of private worksites, restaurants, and bars. Findings indicate that as of November 30, 2014, 40 states prohibited ENDS sales to minors, but only three states prohibited ENDS use in private worksites, restaurants, and bars. Of the 40 states that prohibited ENDS sales to minors, 21 did not prohibit ENDS use or conventional smoking in private worksites, restaurants, and bars. Three states had no statewide laws prohibiting ENDS sales to minors and no statewide laws prohibiting ENDS use or conventional smoking in private worksites, restaurants, and bars. According to the Surgeon General, ENDS have the potential for public health harm or public health benefit. The possibility of public health benefit from ENDS could arise only if 1) current smokers use these devices to switch completely

  17. Multi-mode vibronic interactions in the five lowest electronic states of the fluorobenzene radical cation

    NASA Astrophysics Data System (ADS)

    Bâldea, Ioan; Franz, Jan; Szalay, Péter G.; Köppel, Horst

    2006-10-01

    The multi-mode vibronic interactions between the five lowest electronic states of the fluorobenzene radical cation are investigated theoretically, based on ab initio electronic structure data, and employing the linear vibronic coupling model. Low-energy conical intersections, and strong vibronic couplings are found to prevail within the set of X˜-A˜ and B˜-C˜-D˜ cationic states, while the interactions between these two sets of states are found to be rather weak (owing to high-energy conical intersections). The overall intensity distribution of the experimental photoelectron spectrum, as well as the line positions observed in the MATI spectrum, are well reproduced. The vibronic interactions in the X˜-A˜ states are found to be a replica of the multi-mode dynamical Jahn-Teller effect in the parent system, the XE ground state of the benzene radical cation. Ultrafast internal conversion processes within the electronic manifolds in question demonstrate the strength of the nonadiabatic coupling effects and complement the analogous findings for the electronic spectra. The implications for the fluorescence dynamics of the fluorobenzene radical cation are discussed.

  18. Helical edge states and fractional quantum Hall effect in a graphene electron-hole bilayer

    NASA Astrophysics Data System (ADS)

    Sanchez-Yamagishi, Javier D.; Luo, Jason Y.; Young, Andrea F.; Hunt, Benjamin M.; Watanabe, Kenji; Taniguchi, Takashi; Ashoori, Raymond C.; Jarillo-Herrero, Pablo

    2016-10-01

    Helical 1D electronic systems are a promising route towards realizing circuits of topological quantum states that exhibit non-Abelian statistics. Here, we demonstrate a versatile platform to realize 1D systems made by combining quantum Hall (QH) edge states of opposite chiralities in a graphene electron-hole bilayer at moderate magnetic fields. Using this approach, we engineer helical 1D edge conductors where the counterpropagating modes are localized in separate electron and hole layers by a tunable electric field. These helical conductors exhibit strong non-local transport signals and suppressed backscattering due to the opposite spin polarizations of the counterpropagating modes. Unlike other approaches used for realizing helical states, the graphene electron-hole bilayer can be used to build new 1D systems incorporating fractional edge states. Indeed, we are able to tune the bilayer devices into a regime hosting fractional and integer edge states of opposite chiralities, paving the way towards 1D helical conductors with fractional quantum statistics.

  19. Time-resolved fluorescence spectroscopy of high-lying electronic states of Zn-tetraphenylporphyrin

    NASA Astrophysics Data System (ADS)

    Gurzadyan, G. G.; Tran-Thi, T.-H.; Gustavsson, T.

    1998-01-01

    Depopulation of the S2 excited electronic state of the Zn-tetraphenylporphyrin (ZnTPP) was monitored by measuring the decay of S2→S0 and the rise of S1→S0 fluorescence using the up-conversion fluorescence technique with a time-resolution of 120 fs. The lifetime of the S2 electronic state, measured for ZnTPP in ethanol (τS2=2.35 ps) correlates with the risetime of S1→S0 fluorescence. This result demonstrates the depopulation of S2 to S1 via (vibrational) states with lifetimes much shorter than that of S2. The rise time of S2 fluorescence (τv=60-90 fs) was attributed to vibrational relaxation (in S2). Fluorescence anisotropy decay of the S2 state was also studied by measuring the parallel and perpendicular fluorescence components. The high initial anisotropy of r⩾0.7 is interpreted as due to the existence of a degenerate excited electronic state S2 and the corresponding fast decay time τ1=0.2 ps to the electronic dephasing of the degenerate level pair. The long component of the anisotropy decay (τ2≫10 ps) is due to rotational diffusion.

  20. Effects of Electronic-State-Dependent Solute Polarizability: Application to Solute-Pump/Solvent-Probe Spectra.

    PubMed

    Sun, Xiang; Ladanyi, Branka M; Stratt, Richard M

    2015-07-23

    Experimental studies of solvation dynamics in liquids invariably ask how changing a solute from its electronic ground state to an electronically excited state affects a solution's dynamics. With traditional time-dependent-fluorescence experiments, that means looking for the dynamical consequences of the concomitant change in solute-solvent potential energy. But if one follows the shift in the dynamics through its effects on the macroscopic polarizability, as recent solute-pump/solvent-probe spectra do, there is another effect of the electronic excitation that should be considered: the jump in the solute's own polarizability. We examine the spectroscopic consequences of this solute polarizability change in the classic example of the solvation dye coumarin 153 dissolved in acetonitrile. After demonstrating that standard quantum chemical methods can be used to construct accurate multisite models for the polarizabilities of ground- and excited-state solvation dyes, we show via simulation that this polarizability change acts as a contrast agent, significantly enhancing the observable differences in optical-Kerr spectra between ground- and excited-state solutions. A comparison of our results with experimental solute-pump/solvent-probe spectra supports our interpretation and modeling of this spectroscopy. We predict, in particular, that solute-pump/solvent-probe spectra should be sensitive to changes in both the solvent dynamics near the solute and the electronic-state-dependence of the solute's own rotational dynamics.

  1. Influence of a polarizable surrounding on the electronically excited states of aggregated perylene materials.

    PubMed

    Bellinger, Daniel; Settels, Volker; Liu, Wenlan; Fink, Reinhold F; Engels, Bernd

    2016-06-30

    To tune the efficiency of organic semiconductor devices it is important to understand limiting factors as trapping mechanisms for excitons or charges. An understanding of such mechanisms deserves an accurate description of the involved electronical states in the given environment. In this study, we investigate how a polarizable surrounding influences the relative positions of electronically excited states of dimers of different perylene dyes. Polarization effects are particularly interesting for these systems, because gas phase computations predict that the CT states lie slightly above the corresponding Frenkel states. A polarizable environment may change this energy order because CT states are thought to be more sensitive to a polarizable surrounding than Frenkel states. A first insight we got via a TD-HF approach in combination with a polarizable continuum model (PCM). These give limited insights because TD-HF overestimates excitation energies of CT states. However, SCS-CC2 approaches, which are sufficiently accurate, cannot easily be used in combination with continuum solvent models. Hence, we developed two approaches to combine gas phase SCS-CC2 results with solvent effects based on TD-HF computations. Their accuracies were finally checked via ADC(2)//COSMO computations. The results show that for perylene dyes a polarizable surrounding alone does not influence the energetic ordering of CT and Frenkel states. Variations in the energy order of the states only result from nuclear relaxation effects after the excitation process. © 2016 Wiley Periodicals, Inc.

  2. Electronic-state-lifetime interference in the hard-x-ray regime: Argon as a showcase

    NASA Astrophysics Data System (ADS)

    Goldsztejn, G.; Püttner, R.; Journel, L.; Guillemin, R.; Travnikova, O.; Kushawaha, R. K.; Cunha de Miranda, B.; Ismail, I.; Céolin, D.; Piancastelli, M. N.; Simon, M.; Marchenko, T.

    2017-01-01

    Electronic-state-lifetime interference is a phenomenon specific for ionization of atoms and molecules in the hard-x-ray regime. Using resonant K L2 ,3L2 ,3 Auger decay in argon as a showcase, we present a model that allows extracting the interference terms directly from the cross sections of the final electronic states. The analysis provides fundamental information on the excitation and decay processes such as probabilities of various decay paths and the values of the dipole matrix elements for transitions to the excited states. Our results shed light on the interplay between spectator, shake-down, and shake-up processes in the relaxation of deep core-hole states.

  3. Electronic states of alkali metal-NTCDA complexes: A DFT study

    NASA Astrophysics Data System (ADS)

    Tachikawa, Hiroto; Kawabata, Hiroshi

    2015-10-01

    Structures and electronic states of organic-inorganic compound of 1,4,5,8-naphthalene-tetracarboxylic-dianhydride (NTCDA) with alkali metals, Mn(NTCDA) (Mdbnd Li and Na, n = 0-2), have been investigated by means of hybrid density functional theory (DFT) calculations. From the DFT calculations, it was found that the electronic state of the complex at the ground state is characterized by a charge-transfer state expressed by (M)+(NTCDA)-. The alkali metals were bound equivalently to the carbonyl oxygen and ether oxygen atoms of NTCDA. The Cdbnd O double bond character of NTCDA was changed to a C-O single bond like character by the strong interaction of M to the Cdbnd O and O sites. This change was the origin of the red-shift of the IR spectrum. The UV-vis absorption spectra of Mn(NTCDA) were theoretically predicted on the basis of theoretical results.

  4. Activity of upper electron-excited states in bioluminescence of coelenterates

    NASA Astrophysics Data System (ADS)

    Belogurova, N. V.; Alieva, R. R.; Kudryasheva, N. S.

    2009-04-01

    The involvement of upper electron-excited states as the primary excited states into bioluminescence of coelenterates was experimentally verified. A series of fluorescent molecules was used as foreign energy acceptors in this bioluminescent reaction. The fluorescent aromatic compounds - pyrene, 2-methoxy-naphtalene, naphthalene, and 1,4-diphenylbutadiene - were selected, with fluorescent state energies ranging from 26,700 to 32,500 cm -1. Excitation of these molecules by Forster singlet-singlet energy transfer from S of bioluminescence emitter and by light absorption were excluded. The weak sensitized fluorescence of three compounds was found in the course of bioluminescent reaction. Energy of the upper electron-excited states of the bioluminescent emitter was located around 31,000 cm -1. Localization of the primary excitation on a carbonyl group of coelenteramide molecule is discussed. Comparison of the primary excitation in bioluminescent processes of coelenterates and bacteria is provided.

  5. Tight-binding analysis of the electronic states in AlAs with N isoelectronic impurities

    SciTech Connect

    Jo, M.; Mano, T.; Sakuma, Y.; Sakoda, K.

    2014-03-28

    Incorporation of nitrogen (N) atoms into III–V semiconductors significantly changes their electronic structures. The aim of this study was to assess the electronic states in AlAs that contained N impurities. An sp{sup 3}s{sup *} tight-binding model along with valence-force-field strain calculations were used to obtain the energy levels in N-doped AlAs. The calculations showed that an isolated N atom formed a resonant state above the conduction band edge in AlAs. In contrast, NN{sub 1}[110] and NN{sub 4}[220] pairs formed bound states inside the band gap. The formation of two bound states was consistent with the photoluminescence spectrum of N δ-doped AlAs.

  6. Entanglement of two-electron spin states in a double quantum dot

    NASA Astrophysics Data System (ADS)

    Bagrov, V. G.; Gitman, D. M.; Levin, A. D.; Meireles, M. S.

    Recently, an implementation of a universal set of one- and two-quantum-bit gates for quantum computation using spin states of coupled single-electron quantum dots was proposed. It was demonstrated that it is possible to execute a coherent control of a quantum system based on two-electron spin states in a double quantum dot, allowing state preparation, coherent manipulation, and projective readout. This possibility is based on rapid electrical control of the spin exchange interaction. These results motivated us to develop a formal theoretical study of the corresponding model of two coupled spins placed in a magnetic field and subjected to a time-dependent mutual Heisenberg interaction. Using possible exact solutions of the corresponding quantum problem, we study entangling of different separable initial states in this model. It is demonstrated that the entanglement due to a time-dependent Heisenberg interaction is dominating in comparison with the entanglement due to the action of an external magnetic field.

  7. A theoretical study of low-lying electronic states of aminonitrene, phosphinonitrene, and phosphinocarbene

    NASA Astrophysics Data System (ADS)

    Hoffmann, Mark R.; Kuhler, Kathleen

    1991-06-01

    The recently formulated multiconfiguration-based unitary coupled electron pair approximation (UCEPA) is compared with multireference configuration interaction (MR-CISD) calculations, including all single and double excitations, for the molecules in this study. The electronic states of the molecules in this study are not only of experimental interest, but represent a challenge to any formalism to accurately predict the energy separations of the low-lying electronic states. The equilibrium geometries and fundamental vibrational frequencies of the three lowest electronic states (i.e., 1A1, 3A`, and 1A`) of aminonitrene H2N2, and phosphinonitrene, H2PN, have been determined using a split-valence basis with polarization functions on the heavy atoms and a small complete active space self-consistent-field (CASSCF) description of the active space. Both MR-CISD and UCEPA calculations have been performed at the equilibrium structures using larger basis sets to accurately determine the relative energetics of the electronic states. The equilibrium geometries and vibrational frequencies of the two lowest electronic states (i.e., 1A' and 3A`) of phosphinocarbene, H2PCH, have been determined using a larger than double zeta basis set, augmented with polarization and diffuse functions, and a CASSCF description of the active space. Both MR-CISD and UCEPA calculations were performed on the equilibrium structures and predict that the singlet lies between 10.4 and 11.8 kcal/mol lower in energy than the triplet. The use of a generalized valence bond (GVB) reference function within UCEPA is introduced and is shown to be a useful approximation.

  8. State-of-the-art eigensolvers for electronic structure calculations of large scale nano-systems

    SciTech Connect

    Voemel, Christof Tomov, Stanimire Z. Marques, Osni A.; Canning, A. Wang, L.-W. Dongarra, Jack J.

    2008-07-20

    The band edge states determine optical and electronic properties of semiconductor nano-structures which can be computed from an interior eigenproblem. We study the reliability and performance of state-of-the-art iterative eigensolvers on large quantum dots and wires, focusing on variants of preconditioned CG, Lanczos, and Davidson methods. One Davidson variant, the GD + k (Olsen) method, is identified to be as reliable as the commonly used preconditioned CG while consistently being between two and three times faster.

  9. A Prototype System for Electronic Data Interchange among Registrar's Offices of Different States

    NASA Astrophysics Data System (ADS)

    Metz, Igor; Blöchlinger, Adrian; Varveris, Alexandros

    This work presents a prototype system that enables electronic integration of civil status records of the International Commission on Civil Status (ICCS) member states; the pursued issues are involving civil status matters for citizens of member states through their respective Registrars' Offices organization. Phase 1 of the prototype system is presented together with the technical feasibility securely to exchange messages among civil status offices as well as to assure message integrity, authenticity, confidentiality and non-repudiation.

  10. Electronic transition dipole moment and radiative lifetime calculations of sodium dimer ion-pair states.

    PubMed

    Sanli, Aydin; Beser, Bediha; Edwardson, John R; Magnier, Sylvie; Ahmed, Ergin H; Marjatta Lyyra, A

    2015-09-14

    We report here ab initio calculated electronic transition dipole moments for the sodium dimer ion pair states of (1)Σg (+) symmetry. They vary strongly as a function of internuclear distance because of the effect of the Na(+) + Na(-) ion pair potential, which also causes the formation of additional wells and shoulders in the molecular potential energy curves. We also present a computational study of the transition dipole moment matrix elements and lifetimes for these ion-pair states.

  11. Quasicrystalline electronic states of a one-dimensionally modulated Ag film.

    PubMed

    Moras, P; Theis, W; Ferrari, L; Gardonio, S; Fujii, J; Horn, K; Carbone, C

    2006-04-21

    Ag films on GaAs(110) exhibit a one-dimensional quasiperiodic modulation, resulting in a Fibonacci sequence of parallel stripes with two different widths. Valence level photoemission shows that the Ag electronic states acquire a unique character along the quasiperiodic direction, distinctively manifested by a hierarchy of energy level replicas and avoided crossings at characteristic intervals in reciprocal space. These observations demonstrate the strong influence of the one-dimensional quasiperiodic potential on the Ag film states.

  12. Can the lowest two electronic states of Si 2 be ordered?

    NASA Astrophysics Data System (ADS)

    Lüthi, H. P.; McLean, A. D.

    1987-04-01

    Second-order configuration interaction (SOCI) calculations on Si 2 and C 2 in their lowest 3Σ -g and 3Π u, states, combined with experimental data for C 2, lead to a prediction of a near certain 3Σ g-Si 2 ground state with Te = 180 ± 200 cm -1. Enough computed information is now available to guide an experimental search for the bands in the 3Σ -g to 3Π u electronic transition.

  13. Electronic spectra and excited state dynamics of pentafluorophenol: Effects of low-lying πσ∗ states

    NASA Astrophysics Data System (ADS)

    Karmakar, Shreetama; Mukhopadhyay, Deb Pratim; Chakraborty, Tapas

    2015-05-01

    Multiple fluorine atom substitution effect on photophysics of an aromatic chromophore has been investigated using phenol as the reference system. It has been noticed that the discrete vibronic structure of the S1←S0 absorption system of phenol vapor is completely washed out for pentafluorophenol (PFP), and the latter also shows very large Stokes shift in the fluorescence spectrum. For excitations beyond S1 origin, the emission yield of PFP is reduced sharply with increase in excess vibronic energy. However, in a collisional environment like liquid hydrocarbon, the underlying dynamical process that drives the non-radiative decay is hindered drastically. Electronic structure theory predicts a number of low-lying dark electronic states of πσ∗ character in the vicinity of the lowest valence ππ∗ state of this molecule. Tentatively, we have attributed the excitation energy dependent non-radiative decay of the molecule observed only in the gas phase to an interplay between the lowest ππ∗ and a nearby dissociative πσ∗ state. Measurements in different liquids reveal that some of the dark excited states light up with appreciable intensity only in protic liquids like methanol and water due to hydrogen bonding between solute and solvents. Electronic structure theory methods indeed predict that for PFP-(H2O)n clusters (n = 1-11), intensities of a number of πσ∗ states are enhanced with increase in cluster size. In contrast with emitting behavior of the molecule in the gas phase and solutions of nonpolar and polar aprotic liquids, the fluorescence is completely switched off in polar protic liquids. This behavior is a chemically significant manifestation of perfluoro effect, because a very opposite effect occurs in the case of unsubstituted phenol for which fluorescence yield undergoes a very large enhancement in protic liquids. Several dynamical mechanisms have been suggested to interpret the observed photophysical behavior.

  14. Extensive ab initio study of the electronic states of BSe radical including spin-orbit coupling

    NASA Astrophysics Data System (ADS)

    Liu, Siyuan; Zhai, Hongsheng; Liu, Yufang

    2016-06-01

    The internally contracted multi-reference configuration interaction method (MRCI) with Davidson modification and the Douglas-Kroll scalar relativistic correction has been used to calculate the BSe molecule at the level of aug-cc-pV5Z basis set. The calculated electronic states, including 9 doublet and 6 quartet Λ-S states, are correlated to the dissociation limit of B(2Pu) + Se(3Pg) and B(2Pu) + Se(1Dg). The Spin-orbit coupling (SOC) interaction is taken into account via the state interaction approach with the full Breit-Pauli Hamiltonian operator, which causes the entire 15 Λ-S states to split into 32 Ω states. This is the first time that the spin-orbit coupling calculation has been carried out on BSe. The potential energy curves of the Λ-S and Ω electronic states are depicted with the aid of the avoided crossing rule between electronic states of the same symmetry. The spectroscopic constants of the bound Λ-S and Ω states were determined, which are in good agreement with the experimental data. The transition dipole moments (TDMs) and the Franck-Condon factors (FCs) of the transitions from the low-lying bound Ω states A2Π(I)3/2, B2Π(I)1/2 and C2Δ(I)3/2 to the ground state X2Σ+1/2 have also been presented. Based on the previous calculations, the radiative lifetimes of the A2Π(I)3/2, B2Π(I)1/2 and C2Δ(I)3/2 were evaluated.

  15. First-principles equation of state and electronic properties of warm dense oxygen

    SciTech Connect

    Driver, K. P. Soubiran, F.; Zhang, Shuai; Militzer, B.

    2015-10-28

    We perform all-electron path integral Monte Carlo (PIMC) and density functional theory molecular dynamics (DFT-MD) calculations to explore warm dense matter states of oxygen. Our simulations cover a wide density-temperature range of 1–100 g cm{sup −3} and 10{sup 4}–10{sup 9} K. By combining results from PIMC and DFT-MD, we are able to compute pressures and internal energies from first-principles at all temperatures and provide a coherent equation of state. We compare our first-principles calculations with analytic equations of state, which tend to agree for temperatures above 8 × 10{sup 6} K. Pair-correlation functions and the electronic density of states reveal an evolving plasma structure and ionization process that is driven by temperature and density. As we increase the density at constant temperature, we find that the ionization fraction of the 1s state decreases while the other electronic states move towards the continuum. Finally, the computed shock Hugoniot curves show an increase in compression as the first and second shells are ionized.

  16. Bonding and electronic states of boron in silicon nanowires characterized by an infrared synchrotron radiation beam

    NASA Astrophysics Data System (ADS)

    Fukata, N.; Jevasuwan, W.; Ikemoto, Y.; Moriwaki, T.

    2015-04-01

    The infrared synchrotron radiation (IR-SR) beamline of SPring-8 as an IR light source was applied to characterize boron (B) atoms in silicon nanowires (SiNWs). The use of an IR-SR beam with much higher brilliance than conventional IR light sources and a wide range of wavenumbers from visible to far IR regions made it possible to detect a local vibrational mode of B in SiNWs. The use of this technique has also made it possible to detect other IR peaks related to transitions of a bound hole from the ground state of a B acceptor atom to excited states, clarifying the electronic state of B acceptors in SiNWs.The infrared synchrotron radiation (IR-SR) beamline of SPring-8 as an IR light source was applied to characterize boron (B) atoms in silicon nanowires (SiNWs). The use of an IR-SR beam with much higher brilliance than conventional IR light sources and a wide range of wavenumbers from visible to far IR regions made it possible to detect a local vibrational mode of B in SiNWs. The use of this technique has also made it possible to detect other IR peaks related to transitions of a bound hole from the ground state of a B acceptor atom to excited states, clarifying the electronic state of B acceptors in SiNWs. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr00427f

  17. Edge states in twisted bilayer graphene: quantum spin Hall and electron-hole bilayers

    NASA Astrophysics Data System (ADS)

    Sanchez-Yamagishi, Javier D.; Luo, Jason; Watanabe, Kenji; Taniguchi, Takashi; Jarillo-Herrero, Pablo

    2015-03-01

    Twisted bilayer graphene offers a unique platform for studying 1d edge states in a bilayer 2-dimensional electron gas. Despite being spaced by only 0.34 nm, a large interlayer twist decouples the layers in the bulk, while opening the door for interesting interactions at the edges. To probe this physics, we study the electronic transport through quantum Hall edge modes in twisted bilayer graphene devices. Using dual electrostatic gates, we independently control the filling factor of each layer to form different combinations of bilayer edge states while measuring their conductance. The most dramatic transport effects are observed when the layers are doped to have edge states of opposite chiralities, resulting in coexisting electron- and hole-like states. We will present evidence that, in this regime, the twisted bilayer graphene can form a quantum spin Hall state where edge states in each layer counter-propagate in opposite directions with opposite spin polarizations. This bilayer realization offers a flexible system to study quantum spin Hall edge transport as well as to build more complex 1d circuits. We will also discuss the possibility for fractional generalizations of this edge physics and our measurements of the fractional QHE in twisted bilayer graphene.

  18. First-principles equation of state and electronic properties of warm dense oxygen.

    PubMed

    Driver, K P; Soubiran, F; Zhang, Shuai; Militzer, B

    2015-10-28

    We perform all-electron path integral Monte Carlo (PIMC) and density functional theory molecular dynamics (DFT-MD) calculations to explore warm dense matter states of oxygen. Our simulations cover a wide density-temperature range of 1-100 g cm(-3) and 10(4)-10(9) K. By combining results from PIMC and DFT-MD, we are able to compute pressures and internal energies from first-principles at all temperatures and provide a coherent equation of state. We compare our first-principles calculations with analytic equations of state, which tend to agree for temperatures above 8 × 10(6) K. Pair-correlation functions and the electronic density of states reveal an evolving plasma structure and ionization process that is driven by temperature and density. As we increase the density at constant temperature, we find that the ionization fraction of the 1s state decreases while the other electronic states move towards the continuum. Finally, the computed shock Hugoniot curves show an increase in compression as the first and second shells are ionized.

  19. Intermolecular electron transfer from naphthalene derivatives in the higher triplet excited states.

    PubMed

    Sakamoto, Masanori; Cai, Xichen; Hara, Michihiro; Fujitsuka, Mamoru; Majima, Tetsuro

    2004-08-11

    Intermolecular electron transfer (ELT) from a series of naphthalene derivatives (NpD) in the higher triplet excited states (T(n)) to carbon tetrachloride (CCl(4)) in Ar-saturated acetonitrile was observed using the two-color two-laser flash photolysis method. The ELT efficiency depended on the driving force of ELT. Since the ELT from the T(n) state occurred competitively with the internal conversion (IC, T(n) --> T(1)) and the triplet energy transfer (ENT), the ELT became apparent only when sufficient free energy change of ELT was attained. On the other hand, ELT from the T(1) state was not observed, although ELT from the T(1) state with sufficiently long lifetime has a slightly exothermic driving force. The fast ELT from the T(n) state and lack of the reactivity of the T(1) state were explained well by the "sticky" dissociative electron-transfer model based on one-electron reductive attachment to CCl(4) leading to the C-Cl bond cleavage.

  20. Solid effect in the electron spin dressed state: A new approach for dynamic nuclear polarization

    NASA Astrophysics Data System (ADS)

    Weis, V.; Bennati, M.; Rosay, M.; Griffin, R. G.

    2000-10-01

    We describe a new type of solid effect for dynamic nuclear polarization (DNP) that is based on simultaneous, near resonant microwave (mw) and radio frequency (rf) irradiation of a coupled electron nuclear spin system. The interaction of the electron spin with the mw field is treated as an electron spin dressed state. In contrast to the customary laboratory frame solid effect, it is possible to obtain nuclear polarization with the dressed state solid effect (DSSE) even in the absence of nonsecular hyperfine coupling. Efficient, selective excitation of dressed state transitions generates nuclear polarization in the nuclear laboratory frame on a time scale of tens of μs, depending on the strength of the electron-nuclear coupling, the mw and rf offset and field strength. The experiment employs both pulsed mw and rf irradiation at a repetition rate comparable to T1e-1, where T1e is the electronic spin lattice relaxation time. The DSSE is demonstrated on a perdeuterated BDPA radical in a protonated matrix of polystyrene.

  1. Atoms and quantum dots with a large number of electrons: The ground-state energy

    SciTech Connect

    Kunz, Herve; Rueedi, Rico

    2010-03-15

    We compute the ground-state energy of atoms and quantum dots with a large number N of electrons. Both systems are described by a nonrelativistic Hamiltonian of electrons in a d-dimensional space. The electrons interact via the Coulomb potential. In the case of atoms (d=3), the electrons are attracted by the nucleus via the Coulomb potential. In the case of quantum dots (d=2), the electrons are confined by an external potential, whose shape can be varied. We show that the dominant terms of the ground-state energy are those given by a semiclassical Hartree-exchange energy, whose N{yields}{infinity} limit corresponds to Thomas-Fermi theory. This semiclassical Hartree-exchange theory creates oscillations in the ground-state energy as a function of N. These oscillations reflect the dynamics of a classical particle moving in the presence of the Thomas-Fermi potential. The dynamics is regular for atoms and some dots, but in general in the case of dots, the motion contains a chaotic component. We compute the correlation effects. They appear at the order NlnN for atoms, in agreement with available data. For dots, they appear at the order N.

  2. Doubly excited states of ammonia by scattered electron-ion coincidence measurements

    NASA Astrophysics Data System (ADS)

    Yamamoto, Karin; Sakai, Yasuhiro

    2012-03-01

    To obtain information on the optically forbidden doubly excited states of ammonia (NH3), we performed scattered electron-ion coincidence measurements. First, we observed scattered electrons using electron energy-loss spectroscopy and determined the generalized oscillator strength distribution (GOSD) under 200 eV incident electron energy at a scattering angle of 8°. Ionic GOSDs were also determined by combination with the coincidence signal, which was observed by the time-of-flight mass spectrometer at each energy-loss value, for each ion. The total and partial ionic GOSDs were compared with the experimental results of both photon and fast electron impact. Moreover, the neutral GOSD determined by subtracting the total ionic GOSD from the total was compared with previous results. In addition to the optically forbidden doubly excited states, which were identified by Kato et al (2003 J. Phys. B: At. Mol. Opt. Phys. 36 3541) and Ishikawa et al (2008 J. Phys. B: At. Mol. Opt. Phys. 41 195204), we found a new optically forbidden doubly excited state at around 35 eV.

  3. Nyquist noise as probe of hot-electron effects in the ferromagnetic insulating state of manganites

    NASA Astrophysics Data System (ADS)

    Samanta, Sudeshna; Raychaudhuri, Arup K.

    2009-03-01

    Hole-doped rare-earth manganites (like La1-xCaxMnO3) in the ferromagnetic insulating (FMI) state show large non-linear conductance. Such non-linear conductance can arise due to hot-electron effect which originates from decoupling of the electron and lattice temperatures at high power level. The non-linear conductance manifests as electro-resistance or current induced resistance change. We report here low frequency temperature dependent noise measurement which allows us to estimate the electronic temperature by measuring Nyquist noise (``white noise'' in contrast to 1/f noise) in La0.8Ca0.2MnO3 single crystals which has a distinct FMI state below 100K. The measurement was performed with low ac biasing current which was mixed with a high current density d.c that leads to electron heating. We observed that in the insulating state, above a certain input d.c power, the Nyquist noise increases by a large extent and this is coupled to the onset of non-linear conduction as signalled by the power dependence of the differential conductance. The experiment establishes a direct link between hot-electron effect and non-linear conductance.

  4. Photodissociation of carbon dioxide in singlet valence electronic states. II. Five state absorption spectrum and vibronic assignment.

    PubMed

    Grebenshchikov, Sergy Yu

    2013-06-14

    The absorption spectrum of CO2 in the wavelength range 120-160 nm is analyzed by means of quantum mechanical calculations performed using vibronically coupled potential energy surfaces of five singlet valence electronic states and the coordinate dependent transition dipole moment vectors. The thermally averaged spectrum, calculated for T = 190 K via Boltzmann averaging of optical transitions from many initial rotational states, accurately reproduces the experimental spectral envelope, consisting of a low and a high energy band, the positions of the absorption maxima, their FWHMs, peak intensities, and frequencies of diffuse structures in each band. Contributions of the vibronic interactions due to Renner-Teller coupling, conical intersections, and the Herzberg-Teller effect are isolated and the calculated bands are assigned in terms of adiabatic electronic states. Finally, diffuse structures in the calculated bands are vibronically assigned using wave functions of the underlying resonance states. It is demonstrated that the main progressions in the high energy band correspond to consecutive excitations of the pseudorotational motion along the closed loop of the CI seam, and progressions differ in the number of nodes along the radial mode perpendicular to the closed seam. Irregularity of the diffuse peaks in the low energy band is interpreted as a manifestation of the carbene-type "cyclic" OCO minimum.

  5. 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.

  6. 77 FR 13123 - Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Ohio

    Federal Register 2010, 2011, 2012, 2013, 2014

    2012-03-05

    ... From the Federal Register Online via the Government Publishing Office ENVIRONMENTAL PROTECTION AGENCY Cross-Media Electronic Reporting: Authorized Program Revision Approval, State of Ohio AGENCY..., seeh.karen@epa.gov . SUPPLEMENTARY INFORMATION: On October 13, 2005, the final Cross-Media...

  7. Managing Selection for Electronic Resources: Kent State University Develops a New System to Automate Selection

    ERIC Educational Resources Information Center

    Downey, Kay

    2012-01-01

    Kent State University has developed a centralized system that manages the communication and work related to the review and selection of commercially available electronic resources. It is an automated system that tracks the review process, provides selectors with price and trial information, and compiles reviewers' feedback about the resource. It…

  8. Quantum Percolation and Magnetic Nanodroplet States in Electronically Phase-Separated Manganite Nanowires.

    PubMed

    Zhang, Kaixuan; Li, Lin; Li, Hui; Feng, Qiyuan; Zhang, Nan; Cheng, Long; Fan, Xiaodong; Hou, Yubin; Lu, Qingyou; Zhang, Zhenyu; Zeng, Changgan

    2017-03-08

    One-dimensional (1D) confinement has been revealed to effectively tune the properties of materials in homogeneous states. The 1D physics can be further enriched by electronic inhomogeneity, which unfortunately remains largely unknown. Here we demonstrate the ultrahigh sensitivity to magnetic fluctuations and the tunability of phase stability in the electronic transport properties of self-assembled electronically phase-separated manganite nanowires with extreme aspect ratio. The onset of magnetic nanodroplet state, a precursor to the ferromagnetic metallic state, is unambiguously revealed, which is attributed to the small lateral size of the nanowires that is comparable to the droplet size. Moreover, the quasi-1D anisotropy stabilizes thin insulating domains to form intrinsic tunneling junctions in the low temperature range, which is robust even under magnetic field up to 14 T and thus essentially modifies the classic 1D percolation picture to stabilize a novel quantum percolation state. A new phase diagram is therefore established for the manganite system under quasi-1D confinement for the first time. Our findings offer new insight into understanding and manipulating the colorful properties of the electronically phase-separated systems via dimensionality engineering.

  9. Transition operators entering neutrinoless double electron capture to excited nuclear states

    NASA Astrophysics Data System (ADS)

    Vergados, J. D.

    2011-10-01

    We construct the effective transition operators relevant for neutrinoless double electron capture leading to final nuclear states different than 0+. From the structure of these operators we see that if such a process is observed experimentally, it will be very helpful in singling out the very important light neutrino mass contribution from the other lepton violating mechanisms.

  10. Electronic and vibrational spectroscopy of 1-methylthymine and its water clusters: the dark state survives hydration.

    PubMed

    Busker, Matthias; Nispel, Michael; Häber, Thomas; Kleinermanns, Karl; Etinski, Mihajlo; Fleig, Timo

    2008-08-04

    Electronic and vibrational gas phase spectra of 1-methylthymine (1MT) and 1-methyluracil (1MU) and their clusters with water are presented. Mass selective IR/UV double resonance spectra confirm the formation of pyrimidine-water clusters and are compared to calculated vibrational spectra obtained from ab initio calculations. In contrast to Y. He, C. Wu, W. Kong; J. Phys. Chem. A, 2004, 108, 94 we are able to detect 1MT/1MU and their water clusters via resonant two-photon delayed ionization under careful control of the applied water-vapor pressure. The long-living dark electronic state of 1MT and 1MU detected by delayed ionization, survives hydration and the photostability of 1MT/1MU cannot be attributed solely to hydration. Oxygen coexpansions and crossed-beam experiments indicate that the triplet state population is probably small compared to the (1)n pi* and/or hot electronic ground state population. Ab initio theory shows that solvation of 1MT by water does not lead to a substantial modification of the electronic relaxation and quenching of the (1)n pi* state. Relaxation pathways via (1)pi pi*(1)-n pi*(1) and (1)pi pi*-S(0) conical intersections and barriers have been identified, but are not significantly altered by hydration.

  11. Implications of electron attachment to highly-excited states in pulsed-power discharges

    SciTech Connect

    Pinnaduwage, L.A. |

    1997-08-01

    The author points out the possible implications of electron attachment to highly-excited states of molecules in two pulsed power technologies. One involves the pulsed H{sub 2} discharges used for the generation of H ion beams for magnetic fusion energy and particle accelerators. The other is the power modulated plasma discharges used for material processing.

  12. Atomistic simulation of the electronic states of adatoms in monolayer MoS{sub 2}

    SciTech Connect

    Chang, Jiwon; Larentis, Stefano; Tutuc, Emanuel; Register, Leonard F.; Banerjee, Sanjay K.

    2014-04-07

    Using an ab initio density functional theory based electronic structure method, we study the effects of adatoms on the electronic properties of monolayer transition metal dichalcogenide Molybdenum-disulfide (MoS{sub 2}). We consider the 1st (Li, Na, K) and 7th (F, Cl, Br) column atoms and metals (Sc, Ti, Ta, Mo, Pd, Pt, Ag, Au). Three high symmetry sites for the adatom on the surface of monolayer MoS{sub 2} are examined as starting points to search for the most energetically stable configuration for each adatom-monolayer MoS{sub 2} system, as well as the type of associated bonding. For the most stable adatom positions, we characterize the emergence of adatom-induced electronic states including any dopant states.

  13. Electronic states of lithium passivated germanium nanowires: An ab-initio study

    SciTech Connect

    Trejo, A.; Carvajal, E.; Vázquez-Medina, R.; Cruz-Irisson, M.

    2014-05-15

    A study of the electronic and structural properties of germanium nanowires (GeNWs) was performed using the ab-initio Density Functional Theory within the generalized gradient approximation where electron-ion interactions are described by ultrasoft pseudopotentials. To study the effects of the lithium in the surface of the GeNWs we compare the electronic band structures of Hydrogen passivated GeNWs with those of partial and totally Li passivated GeNWs. The nanowires were constructed in the [001], [111] and [110] directions, using the supercell model to create different wire diameters. The results show that in the case of partial Li passivation there are localized orbitals near the valence band maximum, which would create a p-doped-kind of state. The total Li passivation created metallic states for all the wires.

  14. Dynamic tunneling force microscopy for characterizing electronic trap states in non-conductive surfaces

    SciTech Connect

    Wang, R.; Williams, C. C.

    2015-09-15

    Dynamic tunneling force microscopy (DTFM) is a scanning probe technique for real space mapping and characterization of individual electronic trap states in non-conductive films with atomic scale spatial resolution. The method is based upon the quantum mechanical tunneling of a single electron back and forth between a metallic atomic force microscopy tip and individual trap states in completely non-conducting surface. This single electron shuttling is measured by detecting the electrostatic force induced on the probe tip at the shuttling frequency. In this paper, the physical basis for the DTFM method is unfolded through a physical model and a derivation of the dynamic tunneling signal as a function of several experimental parameters is shown. Experimental data are compared with the theoretical simulations, showing quantitative consistency and verifying the physical model used. The experimental system is described and representative imaging results are shown.

  15. Dynamic tunneling force microscopy for characterizing electronic trap states in non-conductive surfaces.

    PubMed

    Wang, R; Williams, C C

    2015-09-01

    Dynamic tunneling force microscopy (DTFM) is a scanning probe technique for real space mapping and characterization of individual electronic trap states in non-conductive films with atomic scale spatial resolution. The method is based upon the quantum mechanical tunneling of a single electron back and forth between a metallic atomic force microscopy tip and individual trap states in completely non-conducting surface. This single electron shuttling is measured by detecting the electrostatic force induced on the probe tip at the shuttling frequency. In this paper, the physical basis for the DTFM method is unfolded through a physical model and a derivation of the dynamic tunneling signal as a function of several experimental parameters is shown. Experimental data are compared with the theoretical simulations, showing quantitative consistency and verifying the physical model used. The experimental system is described and representative imaging results are shown.

  16. Dynamic tunneling force microscopy for characterizing electronic trap states in non-conductive surfaces

    NASA Astrophysics Data System (ADS)

    Wang, R.; Williams, C. C.

    2015-09-01

    Dynamic tunneling force microscopy (DTFM) is a scanning probe technique for real space mapping and characterization of individual electronic trap states in non-conductive films with atomic scale spatial resolution. The method is based upon the quantum mechanical tunneling of a single electron back and forth between a metallic atomic force microscopy tip and individual trap states in completely non-conducting surface. This single electron shuttling is measured by detecting the electrostatic force induced on the probe tip at the shuttling frequency. In this paper, the physical basis for the DTFM method is unfolded through a physical model and a derivation of the dynamic tunneling signal as a function of several experimental parameters is shown. Experimental data are compared with the theoretical simulations, showing quantitative consistency and verifying the physical model used. The experimental system is described and representative imaging results are shown.

  17. The repopulation of electronic states upon vibrational excitation of niobium carbide clusters

    NASA Astrophysics Data System (ADS)

    Chernyy, V.; Logemann, R.; Bakker, J. M.; Kirilyuk, A.

    2016-07-01

    We study the infrared (IR) resonant heating of neutral niobium carbide clusters probed through ultraviolet photoionization spectroscopy. The IR excitation not only changes the photoionization spectra for the photon energies above the ionization threshold, but also modulates ion yield for energies significantly below it. An attempt to describe the experimental spectra using either Fowler's theory or thermally populated vibrational states was not successful. However, the data can be fully modeled by vibrationally and rotationally broadened discrete electronic levels obtained from Density Functional Theory (DFT) calculations. The application of this method to spectra with different IR pulse energies not only yields information about the excited electronic states in the vicinity of the HOMO level, populated by manipulation of the vibrational coordinates of a cluster, but also can serve as an extra indicator for the cluster isomeric structure and corresponding DFT-calculated electronic levels.

  18. Anisotropic electronic state via spontaneous phase separation in strained vanadium dioxide films.

    PubMed

    Liu, M K; Wagner, M; Abreu, E; Kittiwatanakul, S; McLeod, A; Fei, Z; Goldflam, M; Dai, S; Fogler, M M; Lu, J; Wolf, S A; Averitt, R D; Basov, D N

    2013-08-30

    We resolved the enigma of anisotropic electronic transport in strained vanadium dioxide (VO2) films by inquiring into the role that strain plays in the nanoscale phase separation in the vicinity of the insulator-to-metal transition. The root source of the anisotropy was visualized as the formation of a peculiar unidirectional stripe state which accompanies the phase transition. Furthermore, nanoscale infrared spectroscopy unveils distinct facets of electron-lattice interplay at three different stages of the phase transition. These stages include the initial formation of sparse nonpercolating metallic domains without noticeable involvement of the lattice followed by an electron-lattice coupled anisotropic stripe state close to percolation which ultimately evolves into a nearly isotropic rutile metallic phase. Our results provide a unique mesoscopic perspective for the tunable macroscopic phenomena in strained metal oxide films.

  19. Anisotropic Electronic State via Spontaneous Phase Separation in Strained Vanadium Dioxide Films

    NASA Astrophysics Data System (ADS)

    Liu, M. K.; Wagner, M.; Abreu, E.; Kittiwatanakul, S.; McLeod, A.; Fei, Z.; Goldflam, M.; Dai, S.; Fogler, M. M.; Lu, J.; Wolf, S. A.; Averitt, R. D.; Basov, D. N.

    2013-08-01

    We resolved the enigma of anisotropic electronic transport in strained vanadium dioxide (VO2) films by inquiring into the role that strain plays in the nanoscale phase separation in the vicinity of the insulator-to-metal transition. The root source of the anisotropy was visualized as the formation of a peculiar unidirectional stripe state which accompanies the phase transition. Furthermore, nanoscale infrared spectroscopy unveils distinct facets of electron-lattice interplay at three different stages of the phase transition. These stages include the initial formation of sparse nonpercolating metallic domains without noticeable involvement of the lattice followed by an electron-lattice coupled anisotropic stripe state close to percolation which ultimately evolves into a nearly isotropic rutile metallic phase. Our results provide a unique mesoscopic perspective for the tunable macroscopic phenomena in strained metal oxide films.

  20. Integral Cross Sections for Electron Impact Excitation of Rydberg and Valence States of Molecular Nitrogen

    NASA Astrophysics Data System (ADS)

    Malone, C. P.; Johnson, P. V.; Kanik, I.; Liu, X.; Ajdari, B.; Khakoo, M. A.

    2012-06-01

    We present integral cross sections (ICSs) for electron impact excitation of N2 out of the ground state X (v=0), to the b, c3, o3, b', c'4, G, and F electronic states at incident energies ranging between 17.5 eV and 100 eV. The ICSs were derived from the differential cross sections (DCSs) of Khakoo et al. [Phys. Rev. A 77, 012704 (2008)], which were obtained by unfolding energy loss spectra in the ˜12-13.82 eV range. Recently, Heays et al. [Phys. Rev. A 85, 012705 (2012)] measured comparable higher resolution energy loss spectra, with a significantly different apparatus configuration, but in agreement with the Khakoo et al. (2008) spectra. This latter additional effort provided further confidence in the accuracy of the DCSs upon which the present ICS results are based. Of the higher-lying states studied, five are singlet states that radiate to the ground state via dipole allowed transitions. These include the b and b' valence states and the c'4 Rydberg state that give rise to the Birge-Hopfield I, II, and Carroll-Yoshino bands, respectively, all of which are observed in the atmospheres of Earth, Titan, and Triton. The c3 and o3 Rydberg states give rise to the Worley-Jenkins and Worley series of Rydberg bands, respectively. However, these emissions are not readily observed since predissociation for the c3 and o3 states approaches 100%. As such, direct electron excitation measurements, such as those presented here are superior to standard (spontaneous) emission based measurements in this case.

  1. Electronic non-adiabatic states: towards a density functional theory beyond the Born–Oppenheimer approximation

    PubMed Central

    Gidopoulos, Nikitas I.; Gross, E. K. U.

    2014-01-01

    A novel treatment of non-adiabatic couplings is proposed. The derivation is based on a theorem by Hunter stating that the wave function of the complete system of electrons and nuclei can be written, without approximation, as a Born–Oppenheimer (BO)-type product of a nuclear wave function, X(R), and an electronic one, ΦR(r), which depends parametrically on the nuclear configuration R. From the variational principle, we deduce formally exact equations for ΦR(r) and X(R). The algebraic structure of the exact nuclear equation coincides with the corresponding one in the adiabatic approximation. The electronic equation, however, contains terms not appearing in the adiabatic case, which couple the electronic and the nuclear wave functions and account for the electron–nuclear correlation beyond the BO level. It is proposed that these terms can be incorporated using an optimized local effective potential. PMID:24516183

  2. Path integral study of the correlated electronic states of Na4-Na6

    NASA Astrophysics Data System (ADS)

    Hall, Randall W.

    1990-12-01

    Feynman's path integral formulation of quantum mechanics is used to study the correlated electronic states of Na4-Na6. Two types of simulations are performed: in the first, the nuclei are allowed to move at finite temperature in order to find the most stable geometries. In agreement with previous calculations, we find that planar structures are the most stable and that there is significant vibrational amplitude at finite temperatures, indicating that the Born-Oppenheimer surface is relatively flat. In the second type of simulation, the nuclei are held fixed at symmetric and asymmetric geometries and the correlated electron density is found. Our results show that the electrons are localized, rather than delocalized as previous workers have concluded from examination of the single-particle orbitals. We find that the best picture of these clusters is that they contain three-center, two-electron bonds.

  3. Microwave-Induced Oscillations in Magnetocapacitance: Direct Evidence for Nonequilibrium Occupation of Electronic States

    NASA Astrophysics Data System (ADS)

    Dorozhkin, S. I.; Kapustin, A. A.; Umansky, V.; von Klitzing, K.; Smet, J. H.

    2016-10-01

    In a two-dimensional electron system, microwave radiation may induce giant resistance oscillations. Their origin has been debated controversially and numerous mechanisms based on very different physical phenomena have been invoked. However, none of them have been unambiguously experimentally identified, since they produce similar effects in transport studies. The capacitance of a two-subband system is sensitive to a redistribution of electrons over energy states, since it entails a shift of the electron charge perpendicular to the plane. In such a system, microwave-induced magnetocapacitance oscillations have been observed. They can only be accounted for by an electron distribution function oscillating with energy due to Landau quantization, one of the quantum mechanisms proposed for the resistance oscillations.

  4. Tunable Plasmonic Reflection by Bound 1D Electron States in a 2D Dirac Metal

    NASA Astrophysics Data System (ADS)

    Jiang, B.-Y.; Ni, G. X.; Pan, C.; Fei, Z.; Cheng, B.; Lau, C. N.; Bockrath, M.; Basov, D. N.; Fogler, M. M.

    2016-08-01

    We show that the surface plasmons of a two-dimensional Dirac metal such as graphene can be reflected by linelike perturbations hosting one-dimensional electron states. The reflection originates from a strong enhancement of the local optical conductivity caused by optical transitions involving these bound states. We propose that the bound states can be systematically created, controlled, and liquidated by an ultranarrow electrostatic gate. Using infrared nanoimaging, we obtain experimental evidence for the locally enhanced conductivity of graphene induced by a carbon nanotube gate, which supports this theoretical concept.

  5. Solid state oxygen anion and electron mediating membrane and catalytic membrane reactors containing them

    DOEpatents

    Schwartz, Michael; White, James H.; Sammels, Anthony F.

    2000-01-01

    This invention relates to gas-impermeable, solid state materials fabricated into membranes for use in catalytic membrane reactors. This invention particularly relates to solid state oxygen anion- and electron-mediating membranes for use in catalytic membrane reactors for promoting partial or full oxidation of different chemical species, for decomposition of oxygen-containing species, and for separation of oxygen from other gases. Solid state materials for use in the membranes of this invention include mixed metal oxide compounds having the brownmillerite crystal structure.

  6. Solid state oxygen anion and electron mediating membrane and catalytic membrane reactors containing them

    DOEpatents

    Schwartz, Michael; White, James H.; Sammells, Anthony F.

    2005-09-27

    This invention relates to gas-impermeable, solid state materials fabricated into membranes for use in catalytic membrane reactors. This invention particularly relates to solid state oxygen anion- and electron-mediating membranes for use in catalytic membrane reactors for promoting partial or full oxidation of different chemical species, for decomposition of oxygen-containing species, and for separation of oxygen from other gases. Solid state materials for use in the membranes of this invention include mixed metal oxide compounds having the brownmillerite crystal structure.

  7. Electronic spectra and excited-state dynamics of 4-fluoro-N,N-dimethylaniline

    NASA Astrophysics Data System (ADS)

    Fujiwara, Takashige; Reichardt, Christian; Aaron Vogt, R.; Crespo-Hernández, Carlos E.; Zgierski, Marek Z.; Lim, Edward C.

    2013-10-01

    Concerted ultrafast time-resolved spectroscopic experiments and ab initio computational (TDDFT) studies of the electronic transitions of 4-fluoro-N,N-dimethylaniline (FDMA) have been performed to investigate the mechanism of photo-induced intramolecular charge transfer (ICT). The compound FDMA shows dual fluorescence from a ππ∗ state and a closely-lying twisted intramolecular charge transfer (TICT) state in both n-hexane and acetonitrile. The very similar lifetimes observed for the two emission bands indicate that the ππ∗ and the TICT states are effectively in thermal equilibrium at room temperature.

  8. Tunable Plasmonic Reflection by Bound 1D Electron States in a 2D Dirac Metal.

    PubMed

    Jiang, B-Y; Ni, G X; Pan, C; Fei, Z; Cheng, B; Lau, C N; Bockrath, M; Basov, D N; Fogler, M M

    2016-08-19

    We show that the surface plasmons of a two-dimensional Dirac metal such as graphene can be reflected by linelike perturbations hosting one-dimensional electron states. The reflection originates from a strong enhancement of the local optical conductivity caused by optical transitions involving these bound states. We propose that the bound states can be systematically created, controlled, and liquidated by an ultranarrow electrostatic gate. Using infrared nanoimaging, we obtain experimental evidence for the locally enhanced conductivity of graphene induced by a carbon nanotube gate, which supports this theoretical concept.

  9. Electron-phonon interaction in the quantum well state of the 1 ML Na/Cu(111) system

    NASA Astrophysics Data System (ADS)

    Eremeev, S. V.; Rusina, G. G.; Borisova, S. D.; Chulkov, E. V.

    2008-02-01

    The electron-phonon interaction in the quantum well state formed by a Na monolayer coating on Cu(111) is investigated theoretically. The calculations show that the electron-phonon coupling constant γ in this state decreases insignificantly (≈1%) compared to the value of γ for a clean copper surface. The corresponding electron-phonon contribution to the lifetime τ of the quantum well state increases by a factor of 1.5 compared to τ for the clean Cu(111) surface.

  10. Two-state transition between molten globule and unfolded states of acetylcholinesterase as monitored by electron paramagnetic resonance spectroscopy.

    PubMed Central

    Kreimer, D I; Szosenfogel, R; Goldfarb, D; Silman, I; Weiner, L

    1994-01-01

    Cys-231 of Torpedo californica acetylcholinesterase (EC 3.1.1.7) was selectively labeled with the mercury derivative of a stable nitroxyl radical. In 1.5 M guanidinium chloride, this conjugate exists in a molten globule state (MG), whereas in 5 M denaturant, it is in an unfolded state (U). The transition between the two states is reversible. In the MG, the label is highly immobilized, whereas in the U, it is almost freely rotating. The clearly distinct electron paramagnetic resonance (EPR) spectra of the two states permits the study of this transition. Upon elevating the guanidinium chloride concentration, a decrease in the EPR signal of the MG occurs concomitantly with an increase in the U signal, the total intensity of the EPR spectra remaining constant. This behavior is characteristic of a two-state transition. The thermodynamic characteristics of this transition (delta G0 and m), whether estimated directly from the EPR data or from both CD and fluorescence data analyzed by assuming a two-state scheme, are in good agreement. PMID:7991597

  11. 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

  12. 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

  13. 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

  14. 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

  15. 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

  16. 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

  17. 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

  18. 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

  19. 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

  20. 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

  1. 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

  2. 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

  3. 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

  4. A theoretical study on low-lying electronic states and spectroscopic properties of PH

    NASA Astrophysics Data System (ADS)

    Gao, Yufeng; Gao, Tao

    2014-01-01

    The low-lying electronic states (X3∑-, a1Δ, b1Σ+, A3Π, c1Π and 5∑-) of the PH species correlating with the first three dissociation channels have been investigated at the MRCI + Q/aug-cc-PV5Z level of theory. Accurate adiabatic potential energy curves and spectroscopic constants (Te, Re, ωeχe, ωe, Be, De) of these electronic states have been reported. Effect of the spin-orbit coupling on the A3Π and 5∑- states of the PH has been calculated, which lead to the spin-orbit-induced predissociation of the A3Π state. Electronic transition moment, Einstein coefficients and Franck-Condon factors for the A3Π - X3∑- system have been calculated. Dipole moment functions (μe) and radiative lifetime (τv‧) for the A3Π state has also been determined. The radiative lifetime for A3Π - X3∑- transition is computed and compared with the available data.

  5. Doubly excited states of molecular nitrogen by scattered electron-ion coincidence measurements

    NASA Astrophysics Data System (ADS)

    Takahashi, Karin; Hasegawa, Toru; Sakai, Yasuhiro

    2017-03-01

    Scattered electron-ion coincidence measurements were performed on molecular nitrogen (N2) to study the relaxation dynamics of doubly excited states. Doubly excited states are typically so unstable that they result in either auto-ionization or a neutral dissociation. In auto-ionization, ionization and dissociation typically occur. Using a mixed-gas method, we determined the absolute values of the generalized oscillator strength (GOS) distributions using an incident electron energy of 200 eV and a scattering angle of 6°. The GOS distributions of N2+ and N+ were determined by combining the coincidence ion signals, which revealed some doubly excited states of N2. Since electron impact experiments can provide information on optically forbidden transitions, the contribution of optically forbidden states appears in the GOS distributions of both N2+ and N+. We observed auto-ionization and dissociative auto-ionization induced by excitation to the optically forbidden doubly excited states in the range of 30-40 eV.

  6. Imaging electronic trap states in perovskite thin films with combined fluorescence and femtosecond transient absorption microscopy

    DOE PAGES

    Xiao, Kai; Ma, Ying -Zhong; Simpson, Mary Jane; ...

    2016-04-22

    Charge carrier trapping degrades the performance of organometallic halide perovskite solar cells. To characterize the locations of electronic trap states in a heterogeneous photoactive layer, a spatially resolved approach is essential. Here, we report a comparative study on methylammonium lead tri-iodide perovskite thin films subject to different thermal annealing times using a combined photoluminescence (PL) and femtosecond transient absorption microscopy (TAM) approach to spatially map trap states. This approach coregisters the initially populated electronic excited states with the regions that recombine radiatively. Although the TAM images are relatively homogeneous for both samples, the corresponding PL images are highly structured. Themore » remarkable variation in the PL intensities as compared to transient absorption signal amplitude suggests spatially dependent PL quantum efficiency, indicative of trapping events. Furthermore, detailed analysis enables identification of two trapping regimes: a densely packed trapping region and a sparse trapping area that appear as unique spatial features in scaled PL maps.« less

  7. Imaging electronic trap states in perovskite thin films with combined fluorescence and femtosecond transient absorption microscopy

    SciTech Connect

    Xiao, Kai; Ma, Ying -Zhong; Simpson, Mary Jane; Doughty, Benjamin; Yang, Bin

    2016-04-22

    Charge carrier trapping degrades the performance of organometallic halide perovskite solar cells. To characterize the locations of electronic trap states in a heterogeneous photoactive layer, a spatially resolved approach is essential. Here, we report a comparative study on methylammonium lead tri-iodide perovskite thin films subject to different thermal annealing times using a combined photoluminescence (PL) and femtosecond transient absorption microscopy (TAM) approach to spatially map trap states. This approach coregisters the initially populated electronic excited states with the regions that recombine radiatively. Although the TAM images are relatively homogeneous for both samples, the corresponding PL images are highly structured. The remarkable variation in the PL intensities as compared to transient absorption signal amplitude suggests spatially dependent PL quantum efficiency, indicative of trapping events. Furthermore, detailed analysis enables identification of two trapping regimes: a densely packed trapping region and a sparse trapping area that appear as unique spatial features in scaled PL maps.

  8. Cavity quantum electrodynamics with many-body states of a two-dimensional electron gas.

    PubMed

    Smolka, Stephan; Wuester, Wolf; Haupt, Florian; Faelt, Stefan; Wegscheider, Werner; Imamoglu, Ataç

    2014-10-17

    Light-matter interaction has played a central role in understanding as well as engineering new states of matter. Reversible coupling of excitons and photons enabled groundbreaking results in condensation and superfluidity of nonequilibrium quasiparticles with a photonic component. We investigated such cavity-polaritons in the presence of a high-mobility two-dimensional electron gas, exhibiting strongly correlated phases. When the cavity was on resonance with the Fermi level, we observed previously unknown many-body physics associated with a dynamical hole-scattering potential. In finite magnetic fields, polaritons show distinct signatures of integer and fractional quantum Hall ground states. Our results lay the groundwork for probing nonequilibrium dynamics of quantum Hall states and exploiting the electron density dependence of polariton splitting so as to obtain ultrastrong optical nonlinearities.

  9. The electronic structure of VO in its ground and electronically excited states: A combined matrix isolation and quantum chemical (MRCI) study

    SciTech Connect

    Hübner, Olaf; Hornung, Julius; Himmel, Hans-Jörg

    2015-07-14

    The electronic ground and excited states of the vanadium monoxide (VO) molecule were studied in detail. Electronic absorption spectra for the molecule isolated in Ne matrices complement the previous gas-phase spectra. A thorough quantum chemical (multi-reference configuration interaction) study essentially confirms the assignment and characterization of the electronic excitations observed for VO in the gas-phase and in Ne matrices and allows the clarification of open issues. It provides a complete overview over the electronically excited states up to about 3 eV of this archetypical compound.

  10. Standoff Trace Chemical Sensing via Manipulation of Excited Electronic State Lifetimes

    SciTech Connect

    Rudakov, Fedor M

    2013-01-01

    We present a technique for standoff trace chemical sensing that is based on the dependence of excited electronic state lifetimes on the amount of internal vibrational energy. Time resolved photoionization measurements show that the lifetime of the S1 state in N,N-dimethylisopropylamine (DMIPA) decreases exponentially with the amount of energy deposited into vibrational degrees of freedom. This property is employed to acquire spectral signatures of the molecule. Two nanosecond laser pulses are used, one (266 nm) to ionize the molecule through the S1 state and another, with tunable wavelength, to alter the lifetime of the S1 state by depositing energy into vibrations. Reduction of the S1 state lifetime results in a dip in ionization efficiency that is observed by remotely probing the laser-induced plasma with microwave radiation.

  11. Electronic quasiparticles and evolution of Fermi level spin states in thin magnetic layers

    NASA Astrophysics Data System (ADS)

    Schäfer, J.; Hoinkis, M.; Schrupp, D.; Rotenberg, Eli; Blaha, P.; Claessen, R.

    2006-09-01

    Here we report on high-resolution photoemission of iron layers grown on a W(1 1 0) substrate. The evolution of the substrate states upon sub-monolayer adsorption of Fe atoms leads to a shift in surface state binding energy. For thicker (1 1 0) films, sharp metallic surface states are obtained. Their dispersion displays the signature of quasiparticle renormalization due to dressing with excitations. The energy scale is characteristic for the spin wave spectrum in iron, thereby giving evidence of electron-magnon coupling. Furthermore, it is found that quantum well states occur as a function of layer thickness. These modify the spin density of states at the Fermi level in the ferromagnetic film.

  12. Vibronic structure and coupling of higher excited electronic states in carotenoids

    NASA Astrophysics Data System (ADS)

    Krawczyk, Stanisław; Luchowski, Rafał

    2013-03-01

    Absorption spectra of all-trans carotenoids (lycopene, violaxanthin, ζ-carotene) at low temperature exhibit peculiar features in the UV range. The transition to the 11Ag+ state ('cis-band') weakens on cooling, indicating that it is induced by thermal deformations of the conjugated chain. The higher energy band has unique vibrational structure indicating the vibronic coupling of nBu with another electronic state. The electroabsorption spectra point to the electric field-induced mixing of the nBu state with the vibrational continuum of a lower-lying excited state (Fano effect). These observations widen the basis for elucidation of the vibronic coupling effects in the lower excited states.

  13. Probing electronic states of TaC and observation of a stable excited state of TaC- by anion-photoelectron spectroscopy

    NASA Astrophysics Data System (ADS)

    Aravind, G.; Nrisimhamurty, M.; Mane, Rupali G.; Gupta, A. K.; Krishnakumar, E.

    2015-10-01

    We report the experimental value of electron affinity for TaC to be 1.928(0.056) eV by performing photodetachment of its anion at 355 nm. An excited-electronic state of the anion, stable against autodetachment, is observed lying 0.828 eV above the ground-electronic state. Five low-lying electronic states of TaC are observed and identified by comparison with restricted second-order configuration interaction (SOCI) calculations. Vibrational frequencies for the electronic states are obtained from the analysis of the measured data. We also present the results of density functional theory (DFT) calculations performed on the adiabatic electron affinity, yielding a value of 1.9236 eV and vertical detachment energy value of 1.924 eV.

  14. 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.

  15. 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....

  16. 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

  17. Spatially resolved edge currents and guided-wave electronic states in graphene

    NASA Astrophysics Data System (ADS)

    Allen, M. T.; Shtanko, O.; Fulga, I. C.; Akhmerov, A. R.; Watanabe, K.; Taniguchi, T.; Jarillo-Herrero, P.; Levitov, L. S.; Yacoby, A.

    2016-02-01

    Exploiting the light-like properties of carriers in graphene could allow extreme non-classical forms of electronic transport to be realized. In this vein, finding ways to confine and direct electronic waves through nanoscale streams and streamlets, unimpeded by the presence of other carriers, has remained a grand challenge. Inspired by guiding of light in fibre optics, here we demonstrate a route to engineer such a flow of electrons using a technique for mapping currents at submicron scales. We employ real-space imaging of current flow in graphene to provide direct evidence of the confinement of electron waves at the edges of a graphene crystal near charge neutrality. This is achieved by using superconducting interferometry in a graphene Josephson junction and reconstructing the spatial structure of conducting pathways using Fourier methods. The observed edge currents arise from coherent guided-wave states, confined to the edge by band bending and transmitted as plane waves. As an electronic analogue of photon guiding in optical fibres, the observed states afford non-classical means for information transduction and processing at the nanoscale.

  18. Laser-dressing of electronic quantum states in graded semiconductor nanostructures

    NASA Astrophysics Data System (ADS)

    Radu, A.

    2013-03-01

    It is known that a non-resonant laser field will modify the electronic states in a low-dimensional semiconductor very similarly to the laser-dressing of electrons in isolate atoms. Under intense laser field, the energy levels are functions of the laser parameter which depends on the intensity and frequency of the laser but also on the effective mass of the carriers. This aspect is qualitatively different as compared with the laser-dressing of atoms and it was poorly addressed in the literature until now. This work will demonstrate that in compositionally graded quantum wells the gradient of the effective mass will affect the laser dressing of electronic states in a non-trivial manner. The operatorial nature of the laser parameter leads to a surprising result: the electrons in different subbands will feel different laser-dressed confinement potentials. In particular, for a non-graded quantum well the expectation value of the laser parameter will depend on the effective masses of the electron in all distinct layers of the heterostructure.

  19. Aspects of conical intersections: Dynamics, bound states embedded in the continuum and short-lived electronic states

    NASA Astrophysics Data System (ADS)

    Cederbaum, Lorenz

    2007-03-01

    Conical intersections are omnipresent in polyatomic molecules and their presence gives rise to the most severe breakdown of the Born-Oppenheimer approximation. Several general aspects of conical intersections and of the dynamics through them will be addressed. Particular attention will be paid to the question what happens to the potential energy surfaces if the electronic states are metastable. In addition, it is shown that nuclear dynamics on coupled potential surface can lead to bound states embedded in the continuum. Non-Born-Oppenheimer effects are responsible for the binding of these states. Once the Born-Oppenheimer approximation is introduced, these states at best become resonances which decay via potential tunnelling. The tunnelling is completely suppressed by the coupling between the electronic states. Another important issue which will be touched upon is dynamics in the presence of conical intersections in macrosystems. Here, the number of modes is extremely large and, nevertheless, their impact close to the intersections cannot be neglected. It is shown that effective modes can be derived which reproduce exactly the short-time dynamics of the whole macrosystem at low cost. Numerical examples are given. References: H. K"oppel, W. Domcke and L.S. Cederbaum, Adv.Chem.Phys. 57, 59 (1984) G.A. Worth and L.S. Cederbaum, Annu-Rev.Phys.Chem. 55, 127 (2004) L.S. Cederbaum, R.S. Friedman, V.M Ryaboy and N. Moiseyev, Phys.Rev.Lett. 90, 013001 (2003) S. Feuerbacher, T. Sommerfeld and L.S. Cederbaum, J.Chem.Phys. 120, 3201 (2004) L.S. Cederbaum, E. Gindensperger and I. Burghardt, Phys.Rev.Lett. 94, 113003 (2005)

  20. SUPRATHERMAL ELECTRONS IN THE SOLAR CORONA: CAN NONLOCAL TRANSPORT EXPLAIN HELIOSPHERIC CHARGE STATES?

    SciTech Connect

    Cranmer, Steven R.

    2014-08-20

    There have been several ideas proposed to explain how the Sun's corona is heated and how the solar wind is accelerated. Some models assume that open magnetic field lines are heated by Alfvén waves driven by photospheric motions and dissipated after undergoing a turbulent cascade. Other models posit that much of the solar wind's mass and energy is injected via magnetic reconnection from closed coronal loops. The latter idea is motivated by observations of reconnecting jets and also by similarities of ion composition between closed loops and the slow wind. Wave/turbulence models have also succeeded in reproducing observed trends in ion composition signatures versus wind speed. However, the absolute values of the charge-state ratios predicted by those models tended to be too low in comparison with observations. This Letter refines these predictions by taking better account of weak Coulomb collisions for coronal electrons, whose thermodynamic properties determine the ion charge states in the low corona. A perturbative description of nonlocal electron transport is applied to an existing set of wave/turbulence models. The resulting electron velocity distributions in the low corona exhibit mild suprathermal tails characterized by ''kappa'' exponents between 10 and 25. These suprathermal electrons are found to be sufficiently energetic to enhance the charge states of oxygen ions, while maintaining the same relative trend with wind speed that was found when the distribution was assumed to be Maxwellian. The updated wave/turbulence models are in excellent agreement with solar wind ion composition measurements.

  1. Effect of size on electronic states in a strained pyramidal InAs-GaAs quantum dot system

    SciTech Connect

    Ripan, G. H.; Woon, C. Y.; Gopir, G.

    2015-09-25

    The effect of size on electronic states in a strained pyramidal InAs-GaAs quantum dot system was studied. A comparison was made between two InAs quantum pyramids of different sizes embedded inside a cubic GaAs susbtrate material. Strain relaxation was carried out via the Metropolis Monte Carlo method and the calculated local strain tensors were then included to solve the energy values and the wave functions of the electronic states inside the two simulation cube. The 3D finite difference scheme was employed to solve the time independent Schrödinger equation based on the decoupled electron-hole model. Calculated energy values of the four lowest electronic states showed that the transitions between the electron and hole states widen as the size of the dot becomes smaller especially between the ground states. The confinement of electrons and holes become weaker as the size of the dot reduces.

  2. Normal state electronic properties of LaO1-x Fx BiS2 superconductors

    NASA Astrophysics Data System (ADS)

    Querales-Flores, J. D.; Ventura, C. I.; Citro, R.; Rodríguez-Núñez, J. J.

    2016-05-01

    A good description of the electronic structure of BiS2-based superconductors is essential to understand their phase diagram, normal state and superconducting properties. To describe the first reports of normal state electronic structure features from angle resolved photoemission spectroscopy (ARPES) in LaO1-x Fx BiS2, we used a minimal microscopic model to study their low energy properties. It includes the two effective tight-binding bands proposed by Usui et al., Phys. Rev. B, 86, 2012, 220501(R), and we added moderate intra- and inter-orbital electron correlations related to Bi-(pY, pX) and S-(pY, pX) orbitals. We calculated the electron Green's functions using their equations of motion, which we decoupled in second-order of perturbations on the correlations. We determined the normal state spectral density function and total density of states for LaO1-x Fx BiS2, focusing on the description of the k-dependence, effect of doping, and the prediction of the temperature dependence of spectral properties. Including moderate electron correlations, improves the description of the few experimental ARPES and soft X-ray photoemission data available for LaO1-x Fx BiS2. Our analytical approximation enabled us to calculate the spectral density around the conduction band minimum at k→0 =(0.45 π , 0.45 π), and to predict the temperature dependence of the spectral properties at different BZ points, which might be verified by temperature-dependent ARPES.

  3. Pressure-induced phase transition in La1–xSmxO0.5F0.5BiS2

    DOE PAGES

    Fang, Y.; Yazici, D.; White, B. D.; ...

    2015-09-15

    Electrical resistivity measurements on La1–xSmxO0.5F0.5BiS2 (x = 0.1, 0.3, 0.6, 0.8) have been performed under applied pressures up to 2.6 GPa from 2 K to room temperature. The superconducting transition temperature Tc of each sample significantly increases at a Sm-concentration dependent pressure Pt, indicating a pressure-induced phase transition from a low-Tc to a high-Tc phase. At ambient pressure, Tc increases dramatically from 2.8 K at x = 0.1 to 5.4 K at x = 0.8; however, the Tc values at P > Pt decrease slightly with x and Pt shifts to higher pressures with Sm substitution. In the normal state,more » semiconducting-like behavior is suppressed and metallic conduction is induced with increasing pressure in all of the samples. Furthermore, these results suggest that the pressure dependence of Tc for the BiS2-based superconductors is related to the lattice parameters at ambient pressure and enable us to estimate the evolution of Tc for SmO0.5F0.5BiS2 under pressure.« less

  4. Quantization of electronic states in a rare-earth film: Gd/W(110)

    NASA Astrophysics Data System (ADS)

    Rader, O.; Shikin, A. M.

    2001-11-01

    A variety of distinct peaks occurs in photoemission spectra of ultrathin Gd on W(110) depending on the overlayer thickness, in particular a series of sharp peaks inside of a symmetry gap of the W band structure. Our phase-accumulation analysis assigns these structures to quantum-well states hitherto undetected in rare earths. This is of considerable importance since valence electrons mediate the magnetic coupling and determine the magnetic structure of rare-earth metals. As a first example of its impact, we demonstrate how the new quantum-well data help to resolve a current controversy concerning the nature of the Gd electronic structure.

  5. Autoionization resonance states of two-electron atomic systems with finite spherical confinement

    SciTech Connect

    Chakraborty, Sumana; Ho, Y. K.

    2011-09-15

    We investigate the lowest-lying S-wave resonant states of two-electron atoms confined by a spherical quantum cavity under the framework of the stabilization method. Hylleraas-type wave functions (basis length N = 444) taking the correlation effects between all the charged particles into account are used in the present paper. The finite oscillator potential is used to represent the confinement potential. We present the resonant parameters (energies and widths) of the quantum-confined two-electron atoms with different depths and various ranges of the potentials.

  6. Precursor charge state prediction for electron transfer dissociation tandem mass spectra.

    PubMed

    Sharma, Vagisha; Eng, Jimmy K; Feldman, Sergey; von Haller, Priska D; MacCoss, Michael J; Noble, William S

    2010-10-01

    Electron-transfer dissociation (ETD) induces fragmentation along the peptide backbone by transferring an electron from a radical anion to a protonated peptide. In contrast with collision-induced dissociation, side chains and modifications such as phosphorylation are left intact through the ETD process. Because the precursor charge state is an important input to MS/MS sequence database search tools, the ability to accurately determine the precursor charge is helpful for the identification process. Furthermore, because ETD can be applied to large, highly charged peptides, the need for accurate precursor charge state determination is magnified. Otherwise, each spectrum must be searched repeatedly using a large range of possible precursor charge states. To address this problem, we have developed an ETD charge state prediction tool based on support vector machine classifiers that is demonstrated to exhibit superior classification accuracy while minimizing the overall number of predicted charge states. The tool is freely available, open source, cross platform compatible, and demonstrated to perform well when compared with an existing charge state prediction tool. The program is available from http://code.google.com/p/etdz/.

  7. Excited-State Energies and Electronic Couplings of DNA Base Dimers

    SciTech Connect

    Kozak, Christopher R.; Kistler, Kurt A.; Lu, Zhen; Matsika, Spiridoula

    2010-02-04

    The singlet excited electronic states of two π-stacked thymine molecules and their splittings due to electronic coupling have been investigated with a variety of computational methods. Focus has been given on the effect of intermolecular distance on these energies and couplings. Single-reference methods, CIS, CIS(2), EOMCCSD, TDDFT, and the multireference method CASSCF, have been used, and their performance has been compared. It is found that the excited-state energies are very sensitive to the applied method but the couplings are not as sensitive. Inclusion of diffuse functions in the basis set also affects the excitation energies significantly but not the couplings. TDDFT is inadequate in describing the states and their coupling, while CIS(2) gives results very similar to EOM-CCSD. Excited states of cytosine and adenine π-stacked dimers were also obtained and compared with those of thymine dimers to gain a more general picture of excited states in π-stacked DNA base dimers. The coupling is very sensitive to the relative position and orientation of the bases, indicating great variation in the degree of delocalization of the excited states between stacked bases in natural DNA as it fluctuates.

  8. Ground and lowest-lying electronic states of CoN. A multiconfigurational study.

    PubMed

    Gobbo, João Paulo; Borin, Antonio Carlos

    2006-12-28

    The lowest-lying X1Sigma+, a3Phi, b3II, c5Delta, A1Phi, and B1II electronic states of CoN have been investigated at the ab initio MRCI and MS-CASPT2 levels, with extended atomic basis sets and inclusion of scalar relativistic effects. Among the singlet states, the A1Phi and B1II states have been described for the first time. Potential energy curves, excitation energies, spectroscopic constants, and bonding character for all states are reported. Comparison with other early transition-metal nitrides (ScN, TiN, VN, and CrN), isoelectronic (NiC) and isovalent (RhN and IrN) species has been made, besides analyzing the B1II <=> X1+ electronic transition in terms of Franck-Condon factors, Einstein coefficients, and radiative lifetimes. At both levels of theory, the following energetic order has been obtained: X1Sigma+, a3Phi, b3II, c5Delta, A1Phi, and B1II, with good agreement with experimental results. In contrast, previous DFT and MRCI calculations predicted the ground state to be the 5Delta state.

  9. Electronically excited states of membrane fluorescent probe 4-dimethylaminochalcone. Results of quantum chemical calculations.

    PubMed

    Romanov, Alexey N; Gularyan, Samvel K; Polyak, Boris M; Sakovich, Ruslan A; Dobretsov, Gennady E; Sarkisov, Oleg M

    2011-05-28

    Quantum-chemical calculations of ground and excited states for membrane fluorescent probe 4-dimethylaminochalcone (DMAC) in vacuum were performed. Optimized geometries and dipole moments for lowest-lying singlet and triplet states were obtained. The nature of these electronic transitions and the relaxation path in the excited states were determined; changes in geometry and charge distribution were assessed. It was shown that in vacuum the lowest existed level is of (n, π*) nature, and the closest to it is the level of (π, π*) nature; the energy gap between them is narrow. This led to an effective (1)(π, π*) →(1)(n, π*) relaxation. After photoexcitation the molecule undergoes significant transformations, including changes in bond orders, pyramidalization angle of the dimethylamino group, and planarity of the molecule. Its dipole moment rises from 5.5 Debye in the ground state to 17.1 Debye in the (1)(π, π*) state, and then falls to 2 Debye in the (1)(n, π*) state. The excited (1)(n, π*) state is a short living state; it has a high probability of intersystem crossing into the (3)(π, π*) triplet state. This relaxation path explains the low quantum yield of DMAC fluorescence in non-polar media. It is possible that (3)(π, π*) is responsible for observed DMAC phosphorescence.

  10. Triplet excited states of cyclic disulfides and related compounds: electronic structures, geometries, energies, and decay.

    PubMed

    Ginagunta, Saroja; Bucher, Götz

    2011-02-03

    We have performed a computational study on the properties of a series of heterocycles bearing two adjacent heteroatoms, focusing on the structures and electronic properties of their first excited triplet states. If the heteroatoms are both heavy chalcogens (S, Se, or Te) or isoelectronic species, then the lowest excited triplet state usually has (π*, σ*) character. The triplet energies are fairly low (30-50 kcal mol(-1)). The (π*, σ*) triplet states are characterized by a significantly lengthened bond between the two heteroatoms. Thus, in 1,2-dithiolane (1b), the S-S bond length is calculated to be 2.088 Å in the singlet ground state and 2.568 Å in the first triplet excited state. The spin density is predicted to be localized almost exclusively on the sulfur atoms. Replacing one heavy chalcogen atom by an oxygen atom or an NR group results in a significant destabilization of the (π*, σ*) triplet excited state, which then no longer is lower in energy than an open-chain biradical. The size of the heterocyclic ring also contributes to the stability of the (π*, σ*) triplet state, with five-membered rings being more favorable than six-membered rings. Benzoannulation, finally, usually lowers the energy of the (π*, σ*) triplet excited states. If one of the heteroatoms is an oxygen or nitrogen atom, however, the corresponding lowest triplet states are better described as σ,π-biradicals.

  11. Electronic states and potential energy curves of ZrH + and NbH +

    NASA Astrophysics Data System (ADS)

    Das, Kalyan K.; Balasubramanian, K.

    1991-07-01

    State-averaged complete active space MCSCF (CASSCF) followed by second-order configuration interaction (SOCI) calculations are carried out on several low-lying electronic states of ZrH + and NbH +. The ground state of ZrH + is found to be a 3Δ state ( r e = 1.825 Å, ωe = 1752 cm -1) with a very low-lying excited state of 3Φ symmetry ( r e = 1.841 Å, ωe = 1714 cm -1). The NbH + ion has 4Δ state as the ground state ( r e = 1.746 Å, ωe = 1841 cm -1) with a nearly degenerate state of the 4Π symmetry ( r e = 1.768 Å, ωe = 1826 cm -1). The dissociation energies D0 (ZrH +) D0 (NbH +) are calculated to be 56.8 and 54 kcal/mol, compared to experimental values of 54 ± 3 and 53 ± 3 for ZrH + and NbH +, respectively. The nature of low-lying states is analyzed.

  12. Normal-state nodal electronic structure in underdoped high-Tc copper oxides.

    PubMed

    Sebastian, Suchitra E; Harrison, N; Balakirev, F F; Altarawneh, M M; Goddard, P A; Liang, Ruixing; Bonn, D A; Hardy, W N; Lonzarich, G G

    2014-07-03

    An outstanding problem in the field of high-transition-temperature (high-Tc) superconductivity is the identification of the normal state out of which superconductivity emerges in the mysterious underdoped regime. The normal state uncomplicated by thermal fluctuations can be studied using applied magnetic fields that are sufficiently strong to suppress long-range superconductivity at low temperatures. Proposals in which the normal ground state is characterized by small Fermi surface pockets that exist in the absence of symmetry breaking have been superseded by models based on the existence of a superlattice that breaks the translational symmetry of the underlying lattice. Recently, a charge superlattice model that positions a small electron-like Fermi pocket in the vicinity of the nodes (where the superconducting gap is minimum) has been proposed as a replacement for the prevalent superlattice models that position the Fermi pocket in the vicinity of the pseudogap at the antinodes (where the superconducting gap is maximum). Although some ingredients of symmetry breaking have been recently revealed by crystallographic studies, their relevance to the electronic structure remains unresolved. Here we report angle-resolved quantum oscillation measurements in the underdoped copper oxide YBa2Cu3O6 + x. These measurements reveal a normal ground state comprising electron-like Fermi surface pockets located in the vicinity of the nodes, and also point to an underlying superlattice structure of low frequency and long wavelength with features in common with the charge order identified recently by complementary spectroscopic techniques.

  13. Electron-hole asymmetry of the topological surface states in strained HgTe.

    PubMed

    Jost, Andreas; Bendias, Michel; Böttcher, Jan; Hankiewicz, Ewelina; Brüne, Christoph; Buhmann, Hartmut; Molenkamp, Laurens W; Maan, Jan C; Zeitler, Uli; Hussey, Nigel; Wiedmann, Steffen

    2017-03-09

    Topological insulators are a new class of materials with an insulating bulk and topologically protected metallic surface states. Although it is widely assumed that these surface states display a Dirac-type dispersion that is symmetric above and below the Dirac point, this exact equivalence across the Fermi level has yet to be established experimentally. Here, we present a detailed transport study of the 3D topological insulator-strained HgTe that strongly challenges this prevailing viewpoint. First, we establish the existence of exclusively surface-dominated transport via the observation of an ambipolar surface quantum Hall effect and quantum oscillations in the Seebeck and Nernst effect. Second, we show that, whereas the thermopower is diffusion driven for surface electrons, both diffusion and phonon drag contributions are essential for the hole surface carriers. This distinct behavior in the thermoelectric response is explained by a strong deviation from the linear dispersion relation for the surface states, with a much flatter dispersion for holes compared with electrons. These findings show that the metallic surface states in topological insulators can exhibit both strong electron-hole asymmetry and a strong deviation from a linear dispersion but remain topologically protected.

  14. Infrared/ultraviolet quadruple resonance spectroscopy to investigate structures of electronically excited states

    SciTech Connect

    Weiler, M.; Bartl, K.; Gerhards, M.

    2012-03-21

    Molecular beam investigations in combination with IR/UV spectroscopy offer the possibility to obtain structural information on isolated molecules and clusters. One of the demanding tasks is the discrimination of different isomers, e.g., by the use of isomer specific UV excitations. If this discrimination fails due to overlaying UV spectra of different isomers, IR/IR methods offer another possibility. Here, we present a new IR/UV/IR/UV quadruple resonance technique to distinguish between different isomers especially in the electronically excited state. Due to the IR spectra, structural changes and photochemical pathways in excited states can be assigned and identified. The method is applied to the dihydrated cluster of 3-hydroxyflavone which has been investigated as photochemically relevant system and proton wire model in the S{sub 1} state. By applying the new IR/UV/IR/UV technique, we are able to show experimentally that both in the electronic ground (S{sub 0}) and the electronically excited state (S{sub 1}) two isomers have to be assigned.

  15. Electronic and structural properties of low-lying excited states of vitamin B12.

    PubMed

    Lodowski, Piotr; Jaworska, Maria; Kornobis, Karina; Andruniów, Tadeusz; Kozlowski, Pawel M

    2011-11-17

    Time-dependent density functional theory (TD-DFT) has been applied to explore electronically excited states of vitamin B(12) (cyanocobalamin or CNCbl). To explain why the Co-C bond in CNCbl does not undergo photodissociation under conditions of simple photon excitation, electronically excited states have been computed along the Co-C(CN) stretched coordinate. It was found that the repulsive (3)(σ(Co-C) → σ*(Co-C)) triplet state drops in energy as the Co-C(CN) bond lengthens, but it does not become dissociative. Low-lying excited states were also computed as function of two axial bond lengths. Two energy minima have been located on the S(1)/CNCbl, as well as T(1)/CNCbl, surfaces. The full geometry optimization was carried out for each minimum and electronic properties associated with each optimized structure were analyzed in details. One minimum was described as excitation having mixed ππ*/MLCT (metal-to-ligand charge transfer) character, while the second as ligand-to-metal charge transfer (LMCT) transition. Neither of them, however, can be viewed as pure MLCT or LMCT transitions since additional excitation to or from σ-bonds (SB) of N-Co-C unit have also noticeable contributions. Inclusion of solvent altered the character of one of the excitations from ππ*/MLCT/SBLCT to ππ*/LMCT/LSBCT-type, and therefore, both of them gained significant contribution from LMCT/LSBCT transition. Finally, the nature of S(1) electronic state has been comparatively analyzed in CNCbl and MeCbl cobalamins.

  16. Density functional investigation of the electronic structure and charge transfer excited states of a multichromophoric antenna

    NASA Astrophysics Data System (ADS)

    Basurto, Luis; Zope, Rajendra R.; Baruah, Tunna

    2016-05-01

    We report an electronic structure study of a multichromophoric molecular complex containing two of each borondipyrromethane dye, Zn-tetraphenyl-porphyrin, bisphenyl anthracene and a fullerene. The snowflake shaped molecule behaves like an antenna capturing photon at different frequencies and transferring the photon energy to the porphyrin where electron transfer occurs from the porphyrin to the fullerene. The study is performed within density functional formalism using large polarized Guassian basis sets (12,478 basis functions in total). The energies of the HOMO and LUMO states in the complex, as adjudged by the ionization potential and the electron affinity values, show significant differences with respect to their values in participating subunits in isolation. These differences are also larger than the variations of the ionization potential and electron affinity values observed in non-bonded C60-ZnTPP complexes in co-facial arrangement or end-on orientations. An understanding of the origin of these differences is obtained by a systematic study of the effect of structural strain, the presence of ligands, the effect of orbital delocalization on the ionization energy and the electron affinity. Finally, a few lowest charge transfer energies involving electronic transitions from the porphyrin component to the fullerene subunit of the complex are predicted.

  17. Business pluralism of electronic prescriptions: state of development in Europe and the USA.

    PubMed

    Salmivalli, Lauri; Hilmola, Olli-Pekka

    2006-01-01

    In this paper, we analyse the current state of the development of electronic prescriptions in Europe and the USA. These two places have different approaches to the healthcare sector, since in the former one national social insurance usually provides treatment for all of the people (most often only with friction from total costs), but in the latter one the healthcare sector is under free market forces. As our analysis shows in this paper, electronic prescriptions in both of the places have developed in recent years quite favourably, but this development has not produced consistent results, whether electronic prescriptions should be provided by for-profit companies or should they be under strict control of governmental authorities. We base this finding in two empirical observations: (1) in Europe saving potential from electronic prescriptions is estimated to be high, and contains many abstract national economy accounts and (2) leading US companies (providing electronic prescription services) have went been able to increase their revenues significantly, but still their profitability is questionable. We argue that the situation of electronic prescriptions is similar with airline or credit card industry. Both of these are vital for international and local economies, but the business models have developed well after the initial idea.

  18. Ab Initio Investigations of the Excited Electronic States of CaOCa

    NASA Astrophysics Data System (ADS)

    Fawzy, Wafaa M.; Heaven, Michael

    2016-06-01

    Chemical bonding in alkaline earth hypermetalic oxides is of fundamental interest. Previous Ab initio studies of CaOCa predicted a centrosymmetric linear geometry for both the 1Σg^+ ground state and the low lying triplet 3Σu^+ state. However, there have been no reports concerning the higher energy singlet and triplet states. The present work is focused on characterization of the potential energy surface (PES) of the excited 1Σu^+ state (assuming a centrosymmetric linear geometry) and obtaining predictions for the 1Σu^+←1Σg^+ vibronic transitions. We employed the multireference configuration interaction (MRCISD) method with state-averaged, full-valence complete active space self-consistent field (SA-FV-CASSCF) wavefunctions. In these calculations, the active space consisted of ten valence electrons in twelve orbitals, where all the valence electrons were correlated. Contributions of higher excitation and relativistic effects were taken into account using the Davidson correction and the Douglas-Kroll (DK) Hamiltonian, respectively. The correlation-consistent polarized weighed core-valence quadruple zeta basis set (cc-pwCVQZ-DK) was used for all three atoms. The full level of theory is abbreviated as SA-FV-CASSCF (10,12)-MRCISD-Q/cc-pwCVQZ-DK. The calculations were carried out using the MOLPRO2012 suite of programs. For the centrosymmetric linear geometry in all states, initial investigations of one-dimensional radial cuts provided equilibrium bond distances of 2.034 {Å}, 2.034 {Å}, and 1.999 {Å} for the 1Σg^+ , 3Σu^+ , and 1Σu^+ states, respectively. The vertical excitation frequency of the 1Σu^+←1Σg^+ optical transition was calculated to occur at 14801 wn. These predictions were followed by spectroscopic searches by Heaven et al. Indeed, rotationally resolved vibronic progressions were recorded in the vicinity of the predicted electronic band origin. Calculation of the three-dimensional PES showed that the potential minimum in the 1Σu^+ corresponds

  19. Electronic spectra and excited state dynamics of pentafluorophenol: Effects of low-lying πσ{sup ∗} states

    SciTech Connect

    Karmakar, Shreetama; Mukhopadhyay, Deb Pratim; Chakraborty, Tapas

    2015-05-14

    Multiple fluorine atom substitution effect on photophysics of an aromatic chromophore has been investigated using phenol as the reference system. It has been noticed that the discrete vibronic structure of the S{sub 1}←S{sub 0} absorption system of phenol vapor is completely washed out for pentafluorophenol (PFP), and the latter also shows very large Stokes shift in the fluorescence spectrum. For excitations beyond S{sub 1} origin, the emission yield of PFP is reduced sharply with increase in excess vibronic energy. However, in a collisional environment like liquid hydrocarbon, the underlying dynamical process that drives the non-radiative decay is hindered drastically. Electronic structure theory predicts a number of low-lying dark electronic states of πσ{sup ∗} character in the vicinity of the lowest valence ππ{sup ∗} state of this molecule. Tentatively, we have attributed the excitation energy dependent non-radiative decay of the molecule observed only in the gas phase to an interplay between the lowest ππ{sup ∗} and a nearby dissociative πσ{sup ∗} state. Measurements in different liquids reveal that some of the dark excited states light up with appreciable intensity only in protic liquids like methanol and water due to hydrogen bonding between solute and solvents. Electronic structure theory methods indeed predict that for PFP-(H{sub 2}O){sub n} clusters (n = 1-11), intensities of a number of πσ{sup ∗} states are enhanced with increase in cluster size. In contrast with emitting behavior of the molecule in the gas phase and solutions of nonpolar and polar aprotic liquids, the fluorescence is completely switched off in polar protic liquids. This behavior is a chemically significant manifestation of perfluoro effect, because a very opposite effect occurs in the case of unsubstituted phenol for which fluorescence yield undergoes a very large enhancement in protic liquids. Several dynamical mechanisms have been suggested to interpret the

  20. Electronic excitation of ground state atoms by collision with heavy gas particles

    NASA Technical Reports Server (NTRS)

    Hansen, C. Frederick

    1993-01-01

    Most of the important chemical reactions which occur in the very high temperature air produced around space vehicles as they enter the atmosphere were investigated both experimentally and theoretically, to some extent at least. One remaining reaction about which little is known, and which could be quite important at the extremely high temperatures that will be produced by the class of space vehicles now contemplated - such as the AOTV - is the excitation of bound electron states due to collisions between heavy gas particles. Rates of electronic excitation due to free electron collisions are known to be very rapid, but because these collisions quickly equilibrate the free and bound electron energy, the approach to full equilibrium with the heavy particle kinetic energy will depend primarily on the much slower process of bound electron excitation in heavy particle collisions and the subsequent rapid transfer to free electron energy. This may be the dominant mechanism leading to full equilibrium in the gas once the dissociation process has depleted the molecular states so the transfer between molecular vibrational energy and free electron energy is no longer available as a channel for equilibration of free electron and heavy particle kinetic energies. Two mechanisms seem probable in electronic excitation by heavy particle impact. One of these is the collision excitation and deexcitation of higher electronic states which are Rydberg like. A report, entitled 'Semi-Classical Theory of Electronic Excitation Rates', was submitted previously. This presented analytic expressions for the transition probabilities, assuming that the interaction potential is an exponential repulsion with a perturbation ripple due to the dipole-induced dipole effect in the case of neutral-neutral collisions, and to the ion-dipole interaction in the case of ion-neutral collisions. However the above may be, there is little doubt that excitation of ground state species by collision occurs at the

  1. Electron-impact excitation and ionization cross sections for ground state and excited helium atoms

    SciTech Connect

    Ralchenko, Yu. Janev, R.K.; Kato, T.; Fursa, D.V.; Bray, I.; Heer, F.J. de

    2008-07-15

    Comprehensive and critically assessed cross sections for the electron-impact excitation and ionization of ground state and excited helium atoms are presented. All states (atomic terms) with n{<=}4 are treated individually, while the states with n{>=}5 are considered degenerate. For the processes involving transitions to and from n{>=}5 levels, suitable cross section scaling relations are presented. For a large number of transitions, from both ground and excited states, convergent close coupling calculations were performed to achieve a high accuracy of the data. The evaluated/recommended cross section data are presented by analytic fit functions, which preserve the correct asymptotic behavior of the cross sections. The cross sections are also displayed in graphical form.

  2. Excited-state dynamics of oxazole: A combined electronic structure calculations and dynamic simulations study

    NASA Astrophysics Data System (ADS)

    Cao, Jun; Xie, Zhi-Zhong; Yu, Xiaodong

    2016-08-01

    In the present work, the combined electronic structure calculations and surface hopping simulations have been performed to investigate the excited-state decay of the parent oxazole in the gas phase. Our calculations show that the S2 state decay of oxazole is an ultrafast process characterized by the ring-opening and ring-closure of the five-membered oxazole ring, in which the triplet contribution is minor. The ring-opening involves the Osbnd C bond cleavage affording the nitrile ylide and airine intermediates, while the ring-closure gives rise to a bicyclic species through a 2sbnd 5 bond formation. The azirine and bicyclic intermediates in the S0 state are very likely involved in the phototranspositions of oxazoles. This is different from the previous mechanism in which these intermediates in the T1 state have been proposed for these phototranspositions.

  3. Accurate MRCI calculations of the low-lying electronic states of the NCl molecule

    NASA Astrophysics Data System (ADS)

    Song, Ziyue; Shi, Deheng; Sun, Jinfeng; Zhu, Zunlue

    2017-03-01

    Characterization of 22 electronic states of NCl correlating to the two lowest dissociation channels are carried out using high level CASSCF/MRCI calculations with a sextuple-ζ basis set including Davidson modification, core-valence correlation correction and scalar relativistic effects. As far as we know, this radical has never been the preference of theoretical researchers and experimental investigations only concern the ground state and the two low-lying metastable states. Accurate potential energy curves, dissociation energies as well as the equilibrium constants are determined and avoided crossings between the Π symmetry are studied. Moreover, spin-orbit splitting of several states and transition probabilities and radiative lifetimes for some allowed or forbidden transitions are presented.

  4. Turbulent relaxation and meta-stable equilibrium states of an electron plasma

    NASA Astrophysics Data System (ADS)

    Rodgers, Douglas J.

    A Malmberg-Penning electron trap allows for the experimental study of nearly ideal, two-dimensional (2D) inviscid (Euler) hydrodynamics. This is perhaps the simplest case of self organizing nonlinear turbulence, and is therefore a paradigm for dynamo theory, Taylor relaxation, selective decay and other nonlinear fluid processes. The dynamical relaxation of a pure electron plasma in the guiding-center-drift approximation is studied, comparing experiments, numerical simulations and statistical theories of weakly-dissipative 2D turbulence. The nonuniform metastable equilibrium states resulting from turbulent evolution are examined, and are well-described by a maximum entropy principle for constrained circulation, energy, and angular momentum. The turbulent decay of the system is also examined, and a similarity decay law is proposed which incorporates the substantial enstrophy trapped in the metastable equilibrium. This law approaches Batchelor's t-2 self-similar decay in the limit of strong turbulence, and is verified in turbulent evolution in the electron plasma experiment.

  5. Probing the spinor nature of electronic states in nanosize non-collinear magnets

    PubMed Central

    Fischer, Jeison A.; Sandratskii, Leonid M.; Phark, Soo-Hyon; Ouazi, Safia; Pasa, André A.; Sander, Dirk; Parkin, Stuart S. P.

    2016-01-01

    Non-collinear magnetization textures provide a route to novel device concepts in spintronics. These applications require laterally confined non-collinear magnets (NCM). A crucial aspect for potential applications is how the spatial proximity between the NCM and vacuum or another material impacts the magnetization texture on the nanoscale. We focus on a prototypical exchange-driven NCM given by the helical spin order of bilayer Fe on Cu(111). Spin-polarized scanning tunnelling spectroscopy and density functional theory reveal a nanosize- and proximity-driven modification of the electronic and magnetic structure of the NCM in interfacial contact with a ferromagnet or with vacuum. An intriguing non-collinearity between the local magnetization in the sample and the electronic magnetization probed above its surface results. It is a direct consequence of the spinor nature of electronic states in NCM. Our findings provide a possible route for advanced control of nanoscale spin textures by confinement. PMID:27721384

  6. Energy separations for the electronic states of PH -2,PH 2 and PH +2

    NASA Astrophysics Data System (ADS)

    Balasubramanian, K.

    1993-03-01

    All-electron complete-active space multi-configuration self-consistent field (CASSCF) followed by second-order configuration interaction (SOCI) calculations in conjunction with large P(13s10p3d2flg/7s6p3d2flg) and H (10s5p1d/8s5p1d) basis sets are made on the electronic states of PH -2, PH 2 and PH +2. We compute the adiabatic electron affinities of PH 2 and PH. The 3B 1-X 1A 1, 1B 1-X 1A 1 energy separations of PH +2 and the 2A 1-X 2B 1 energy separation of PH 2 are computed.

  7. Lateral quantization of two-dimensional electron states by embedded Ag nanocrystals

    NASA Astrophysics Data System (ADS)

    Van Haesendonck, Chris; Schouteden, Koen

    2013-03-01

    We show that quantization of image-potential state (IS)electrons above the surface of nanostructures can be experimentally achieved by Ag nanocrystals that appear as stacking fault tetrahedrons (SFTs) at Ag(111) surfaces. By means of cryogenic scanning tunneling spectroscopy the n = 1 IS of the Ag(111) surface is revealed to split up in discrete energy levels, which is accompanied by the formation of pronounced standing wave patterns that directly reflect the eigenstates of the SFT surface. The IS confinement behavior is compared to that of the surface state electrons in the SFT surface and can be directly linked to the particle-in-a-box model. ISs provide a novel playground for investigating quantum size effects and defect induced scattering above nanostructured surfaces. This work has been supported by the Research Foundation - Flanders (FWO, Belgium). K.S. is a postdoctoral researcher of the FWO.

  8. Photoelectron spectroscopic study of electronic state and surface structure of In2O3 single crystals

    NASA Astrophysics Data System (ADS)

    Nagata, Takahiro; Bierwagen, Oliver; Galazka, Zbigniew; Imura, Masataka; Ueda, Shigenori; Yoshikawa, Hideki; Yamashita, Yoshiyuki; Chikyow, Toyohiro

    2017-01-01

    The electronic states and band bending behavior of melt-grown In2O3 single crystals were investigated by combining surface-sensitive soft- and bulk-sensitive hard-X-ray photoelectron spectroscopies. The as-grown In2O3 crystal had a higher density of in-gap states related to oxygen vacancies than the In2O3 crystal annealed in air at 1000 °C. Nevertheless, the polished surfaces of both samples had surface electron accumulation layers (SEALs) with similar Fermi level pinning energies at the surface. The estimated peak carrier density at the surface of both samples was 1.2 × 1020 cm-3. The SEALs may originate from defects due to surface polishing or adsorbates.

  9. The effect of charge state on electron excitation by slow protons in simple metal

    NASA Astrophysics Data System (ADS)

    Marouf, S.; Boudouma, Y.; Chami, A. C.

    2016-01-01

    We investigate the energy and angular distributions of conduction band electrons excited by slowly moving protons. An improved method for the description of target response was developed assuming a convenient spherical symmetry of the screened potential. The velocity dependent screening parameter of the trial potential is adjusted in a self-consistent way using an extension of the Friedel sum rule. As positive projectile can be ionized or neutralized by interaction with the target, we should include the different charge states fractions of the protons to determine the doubly differential cross section (DDCS) for the secondary electron emission. A comparison of the double differential cross section using the Density Functional Theory (DFT) is presented. The energy loss of moving proton is also discussed with explicit inclusion of the different charge states and compared to the available experimental data in order to check the validity of the proposed model.

  10. Security aspects of electronic data interchange between a state health department and a hospital emergency department.

    PubMed

    Magnuson, J A; Klockner, Rocke; Ladd-Wilson, Stephen; Zechnich, Andrew; Bangs, Christopher; Kohn, Melvin A

    2004-01-01

    Electronic emergency department reporting provides the potential for enhancing local and state surveillance capabilities for a wide variety of syndromes and reportable conditions. The task of protecting data confidentiality and integrity while developing electronic data interchange between a hospital emergency department and a state public health department proved more complex than expected. This case study reports on the significant challenges that had to be resolved to accomplish this goal; these included application restrictions and incompatibilities, technical malfunctions, changing standards, and insufficient dedicated resources. One of the key administrative challenges was that of coordinating project security with enterprise security. The original project has evolved into an ongoing pilot, with the health department currently receiving secure data from the emergency department at four-hour intervals. Currently, planning is underway to add more emergency departments to the project.

  11. On large amplitude motions of simplest amides in the ground and excited electronic states

    NASA Astrophysics Data System (ADS)

    Tukachev, N. V.; Bataev, V. A.; Godunov, I. A.

    2016-12-01

    For the formamide, acetamide, N-methylformamide and N-methylacetamide molecules in the ground (S0) and lowest excited singlet (S1) and triplet (T1) electronic states equilibrium geometry parameters, harmonic vibrational frequencies, barriers to conformational transitions and conformer energy differences were estimated by means of MP2, CCSD(T), CASSCF, CASPT2 and MRCI ab initio methods. One-, two- and three-dimensional potential energy surface (PES) sections corresponding to different large amplitude motions (LAM) were calculated by means of MP2/aug-cc-pVTZ (S0) and CASPT2/cc-pVTZ (S1,T1). For these molecules, in each excited electronic state six minima were found on 2D PES sections. Using PES sections, different anharmonic vibrational problems were solved and the frequencies of large amplitude vibrations were determined.

  12. Nature of electronic states and optical functions of sodium oxyanionic compounds

    NASA Astrophysics Data System (ADS)

    Zhuravlev, Yu. N.; Korabel'Nikov, D. V.

    2009-01-01

    The band structure, the density of states, the partial electron densities, and optical functions (such as permittivity, refraction index, reflection and absorption coefficients) of sodium nitrite, nitrate, carbonate, chlorate, sulfite, perchlorate, and sulfate are calculated in a local approximation of the density-functional theory using the Troullier-Martins pseudopotentials in the basis of numerical pseudoatomic orbitals. The nature of the upper valence bands and the lower empty bands is established. It is shown that the specific features of the optical functions at energies of up to 8 eV and at E> 8 eV are due to the excitation of electrons into a localized anionic conduction band and into the bands of anion-cation states, respectively. The results are compared to experimental photoelectron spectra and reflection and absorption spectra.

  13. State-selective electron capture in 30- and 100-keV He++He collisions

    NASA Astrophysics Data System (ADS)

    Guo, D. L.; Ma, X.; Zhang, R. T.; Zhang, S. F.; Zhu, X. L.; Feng, W. T.; Gao, Y.; Hai, B.; Zhang, M.; Wang, H. B.; Huang, Z. K.

    2017-01-01

    A combined experimental and theoretical study on single capture in 30- and 100-keV He+ on He collisions was performed. By using a reaction microscope, we obtained the state selective cross sections and the angular-differential cross sections. It was found that the experimental state-selective cross sections were in good agreement with the dynamic screening classical trajectory Monte Carlo calculation for 100-keV He+ incident. The comparisons with various versions of such calculations reveal the roles played by different electron-electron correlation effects. Moreover, a prominent oscillatory structure was observed in the angular-differential cross sections for both projectile energies. With the single capture probability distribution obtained from the classical trajectory Monte Carlo calculation, the oscillation structures can be well explained by atomic-size Fraunhofer-type diffraction.

  14. Lateral quantization of two-dimensional electron states by embedded Ag nanocrystals.

    PubMed

    Schouteden, K; Van Haesendonck, C

    2012-02-17

    We show that quantization of image-potential state (IS) electrons above the surface of nanostructures can be experimentally achieved by Ag nanocrystals that appear as stacking-fault tetrahedrons (SFTs) at Ag(111) surfaces. By means of cryogenic scanning tunneling spectroscopy, the n=1 IS of the Ag(111) surface is revealed to split up in discrete energy levels, which is accompanied by the formation of pronounced standing wave patterns that directly reflect the eigenstates of the SFT surface. The IS confinement behavior is compared to that of the surface state electrons in the SFT surface and can be directly linked to the particle-in-a-box model. ISs provide a novel playground for investigating quantum size effects and defect-induced scattering above nanostructured surfaces.

  15. Controlling Two-Electron Threshold Dynamics in Double Photoionization of Lithium by Initial-State Preparation

    NASA Astrophysics Data System (ADS)

    Zhu, G.; Schuricke, M.; Steinmann, J.; Albrecht, J.; Ullrich, J.; Ben-Itzhak, I.; Zouros, T. J. M.; Colgan, J.; Pindzola, M. S.; Dorn, A.

    2009-09-01

    Double photoionization (DPI) and ionization-excitation (IE) of Li(2s) and Li(2p), state-prepared and aligned in a magneto-optical trap, were explored in a reaction microscope at the free-electron laser in Hamburg (FLASH). From 6 to 12 eV above threshold (ℏω=85, 91 eV), total as well as differential DPI cross sections were observed to critically depend on the initial state and, in particular, on the alignment of the 2p orbital with respect to the VUV-light polarization, whereas no effect is seen for IE. The alignment sensitivity is traced back to dynamical electron correlation at threshold.

  16. Controlling Two-Electron Threshold Dynamics in Double Photoionization of Lithium by Initial-State Preparation

    SciTech Connect

    Zhu, G.; Schuricke, M.; Steinmann, J.; Albrecht, J.; Dorn, A.; Ullrich, J.; Ben-Itzhak, I.; Zouros, T. J. M.; Colgan, J.; Pindzola, M. S.

    2009-09-04

    Double photoionization (DPI) and ionization-excitation (IE) of Li(2s) and Li(2p), state-prepared and aligned in a magneto-optical trap, were explored in a reaction microscope at the free-electron laser in Hamburg (FLASH). From 6 to 12 eV above threshold ((Planck constant/2pi)omega=85, 91 eV), total as well as differential DPI cross sections were observed to critically depend on the initial state and, in particular, on the alignment of the 2p orbital with respect to the VUV-light polarization, whereas no effect is seen for IE. The alignment sensitivity is traced back to dynamical electron correlation at threshold.

  17. Spatial mapping of the electronic states of a one-dimensional system.

    PubMed

    van Houselt, Arie; Oncel, Nuri; Poelsema, Bene; Zandvliet, Harold J W

    2006-07-01

    Using low-temperature scanning tunneling microscopy and spectroscopy, we have recorded spatial maps of confined electronic states in the troughs between self-organized Pt nanowires on Ge(001) that are spaced 2.4 nm apart. Two sub-bands are resolved, which correspond to the lowest energy levels of a quantum mechanical particle in a box. As expected, the spatial dI/dV maps exhibit a maximum and a minimum in the middle of the troughs for the n = 1 and n = 2 states, respectively.

  18. Mechanisms and instrument electronics for the Ohio State Multi-Object Spectrograph (OSMOS)

    NASA Astrophysics Data System (ADS)

    Stoll, R.; Martini, P.; Derwent, M. A.; Gonzalez, R.; O'Brien, T. P.; Pappalardo, D. P.; Pogge, R. W.; Wong, M.-H.; Zhelem, R.

    2010-07-01

    The Ohio State Multi-Object Spectrograph (OSMOS) is a new facility imager and spectrograph for the 2.4m Hiltner telescope at the MDM Observatory. We present a detailed description of the mechanical and electronic solutions employed in OSMOS, many of which have been developed and extensively tested in a large number of instruments built at Ohio State over the past ten years. These solutions include robust aperture wheel and linear stage designs, mechanism control with MicroLYNX programmable logic controllers, and WAGO fieldbus I/O modules.

  19. Inelastic electron scattering to negative parity states of /sup 24/Mg

    SciTech Connect

    Zarek, H.; Yen, S.; Pich, B.O.; Drake, T.E.; Williamson, C.F.; Kowalski, S.; Sargent, C.P.

    1984-05-01

    The electromagnetic form factors for the stronger transitions to negative parity states in /sup 24/Mg were measured for electron energies 90--280 MeV and scattering angles of 90/sup 0/ and 160/sup 0/. The isoscalar K/sup ..pi../ = 0/sup -/ and 3/sup -/ bands show form factors in agreement with open-shell random-phase approximation calculations, even though the parentages of these two bands are radically different. For the isovector negative parity states, a quenching of magnetic strength is observed; its origins are discussed.

  20. Fluctuation of the electronic coupling in DNA: Multistate versus two-state model

    NASA Astrophysics Data System (ADS)

    Voityuk, Alexander A.

    2007-05-01

    The electronic coupling for hole transfer between guanine bases G in the DNA duplex (GT) 6GTG(TG) 6 is studied using a QM/MD approach. The coupling V is calculated for 10 thousand snapshots within the two- and multistate state Generalized Mulliken-Hush model. We find that the two-state scheme considerably underestimates the rate of the hole transfer within the π stack. Moreover, the probability distributions computed with the two- and multistate schemes are quite different. It has been found that large fluctuations of V2, which are at least an order of magnitude larger than its average value, occur roughly every 1 ps.