Theory of interfacial charge-transfer complex photophysics in π-conjugated polymer-fullerene blends

Science.gov (United States)

Aryanpour, K.; Psiachos, D.; Mazumdar, S.

2010-03-01

We present a theory of the electronic structure and photophysics of 1:1 blends of derivatives of polyparaphenylenevinylene and fullerenes [1]. Within the same Coulomb-correlated Hamiltonian applied previously to interacting chains of single-component π-conjugated polymers [2], we find an exciplex state that occurs below the polymer's optical exciton. Weak absorption from the ground state occurs to the exciplex. We explain transient photoinduced absorptions in the blend [3], observed for both above-gap and below-gap photoexcitations, within our theory. Photoinduced absorptions for above-gap photoexcitation are from the optical exciton as well as the exciplex, while for below-gap photoexcitation induced absorptions are from the exciplex alone. In neither case are free polarons generated in the time scale of the experiment. Importantly, the photophysics of films of single-component π-conjugated polymers and blends can both be understood by extending Mulliken's theory of ground state charge-transfer to the case of excited state charge-transfer. [1] K. Aryanpour, D. Psiachos, and S. Mazumdar, arXiv:0908.0366 [2] D. Psiachos and S. Mazumdar, Phys. Rev. B. 79 155106 (2009) [3] T. Drori et al., Phys. Rev. Lett. 101, 037402 (2008)

Symmetric charge transfer cross section of uranium

International Nuclear Information System (INIS)

Shibata, Takemasa; Ogura, Koichi

1995-03-01

Symmetric charge transfer cross section of uranium was calculated under consideration of reaction paths. In the charge transfer reaction a d 3/2 electron in the U atom transfers into the d-electron site of U + ( 4 I 9/2 ) ion. The J value of the U atom produced after the reaction is 6, 5, 4 or 3, at impact energy below several tens eV, only resonant charge transfer in which the product atom is ground state (J=6) takes place. Therefore, the cross section is very small (4-5 x 10 -15 cm 2 ) compared with that considered so far. In the energy range of 100-1000eV the cross section increases with the impact energy because near resonant charge transfer in which an s-electron in the U atom transfers into the d-electron site of U + ion. Charge transfer cross section between U + in the first excited state (289 cm -1 ) and U in the ground state was also obtained. (author)

Collective charge and mass transfer in heavy ion reactions

International Nuclear Information System (INIS)

Hahn, J.

1982-01-01

In this thesis the dynamics of the charge and mass asymmetry degree of freedom was studied in the framework of the fragmentation theory by means of a time-dependent Schroedinger equation. New is the introduction of a friction potential which describes the coupling of these collective degrees of freedom to the not explicitely treated other collective respectively internal degrees of freedom. Thereby it was shown that the measured widths of the isobaric charge distributions in the 86 Kr+sup(92,98)Mo reaction can be explained mainly by the quantum mechanical uncertainty in the charge asymmetry degree of freedom. The charge equilibration occurring at the begin of a deep inelastic collision can therefore by considered as a quantum mechanical, collective, damped motion which is connected with the excitation of the isovector giant dipole resonance of the nucleus-nucleus system. The study of the mass transfer in the reactions 132 Xe+ 120 Sn and 86 Kr+ 166 Er shows, how important at the begin of a deep inelastic collision shell structures and their conservation are for a large part of the reaction, even if the elemental distribution show no maxima in the region of magic shell closures. The experimental width are up to 10 MeV/A well described under conservation of the shell structure. (orig./HSI) [de

Hybrid graphene and graphitic carbon nitride nanocomposite: gap opening, electron-hole puddle, interfacial charge transfer, and enhanced visible light response.

Science.gov (United States)

Du, Aijun; Sanvito, Stefano; Li, Zhen; Wang, Dawei; Jiao, Yan; Liao, Ting; Sun, Qiao; Ng, Yun Hau; Zhu, Zhonghua; Amal, Rose; Smith, Sean C

2012-03-07

Opening up a band gap and finding a suitable substrate material are two big challenges for building graphene-based nanodevices. Using state-of-the-art hybrid density functional theory incorporating long-range dispersion corrections, we investigate the interface between optically active graphitic carbon nitride (g-C(3)N(4)) and electronically active graphene. We find an inhomogeneous planar substrate (g-C(3)N(4)) promotes electron-rich and hole-rich regions, i.e., forming a well-defined electron-hole puddle, on the supported graphene layer. The composite displays significant charge transfer from graphene to the g-C(3)N(4) substrate, which alters the electronic properties of both components. In particular, the strong electronic coupling at the graphene/g-C(3)N(4) interface opens a 70 meV gap in g-C(3)N(4)-supported graphene, a feature that can potentially allow overcoming the graphene's band gap hurdle in constructing field effect transistors. Additionally, the 2-D planar structure of g-C(3)N(4) is free of dangling bonds, providing an ideal substrate for graphene to sit on. Furthermore, when compared to a pure g-C(3)N(4) monolayer, the hybrid graphene/g-C(3)N(4) complex displays an enhanced optical absorption in the visible region, a promising feature for novel photovoltaic and photocatalytic applications. © 2012 American Chemical Society

Charge transfer in gold--alkali-metal systems

International Nuclear Information System (INIS)

Watson, R.E.; Weinert, M.

1994-01-01

Based on conventional electronegativity arguments, gold--alkali-metal compounds are expected to be among the most ''ionic'' of metallic compounds. The concepts of ionicity and charge transfer are difficult to quantify. However, the changes in bonding in the 50/50 Au--alkali-metal systems between the elemental metals and the compounds are so severe that observations can readily be made concerning their character. The results, as obtained from self-consistent electronic-structure calculations, lead to the apparently odd observation that the electron density at the alkali-metal sites in the compound increases significantly and this involves high l componennts in the charge density. This increase, however, can be attributed to Au-like orbitals spatially overlapping the alkali-metal sites. In a chemical sense, it is reasonable to consider the alkali-metal transferring charge to these Au orbitals. While normally the difference in heats of formation between muffin-tin and full-potential calculations for transition-metal--transition-metal and transition-metal--main-group (e.g., Al) compounds having high site symmetry are small, for the gold--alkali-metal systems, the changes in bonding in the compounds cause differences of ∼0.5 eV/atom between the two classes of potential. Any serious estimate of the electronic structure in these systems must account for these aspherical bonding charges. The origin of the semiconducting behavior of the heavy-alkali-metal Au compounds is shown to arise from a combination of the Au-Au separations and the ionic character of the compounds; the light-alkali-metal Au compounds, with their smaller Au-Au separations, do not have a semiconducting gap. Core-level shifts and isomer shifts are also briefly discussed

Calculation of Post-Closure Natural Convection Heat and Mass Transfer in Yucca Mountain Drifts

International Nuclear Information System (INIS)

Webb, S.; Itamura, M.

2004-01-01

Natural convection heat and mass transfer under post-closure conditions has been calculated for Yucca Mountain drifts using the computational fluid dynamics (CFD) code FLUENT. Calculations have been performed for 300, 1000, 3000, and 10,000 years after repository closure. Effective dispersion coefficients that can be used to calculate mass transfer in the drift have been evaluated as a function of time and boundary temperature tilt

Tuning electronic properties of graphene nanoflake polyaromatic hydrocarbon through molecular charge-transfer interactions

Science.gov (United States)

Sharma, Vaishali; Dabhi, Shweta D.; Shinde, Satyam; Jha, Prafulla K.

2018-05-01

By means of first principles calculation we have tuned the electronic properties of graphene nanoflake polyaromatic hydrocarbon via molecular charge transfer. Acceptor/donor Tetracyanoquinodimethane (TCNQ) and Tetrathiafulvalene (TTF) organic molecules are adsorbed on polyaromatic hydrocarbons (PAH) in order to introduce the charge transfer. The substrate's n- or p- type nature depends on the accepting/donating behavior of dopant molecules. Two different classes of PAH (extended form of triangulene) namely Bow-tie graphene nanoflake (BTGNF) and triangular zigzag graphene nanoflake (TZGNF). It is revealed that all the TCNQ and TTF modified graphene nanoflakes exhibit significant changes in HOMO-LUMO gap in range from 0.58 eV to 0.64 eV and 0.01 eV to 0.05 eV respectively. The adsorption energies are in the range of -0.05 kcal/mol to -2.6 kcal/mol. The change in work function is also calculated and discussed, the maximum charge transfer is for TCNQ adsorbed BTGNF. These alluring findings in the tuning of electronic properties will be advantageous for promoting graphene nanoflake polyaromatic hydrocarbon for their applications in electronic devices.

Spontaneous charged lipid transfer between lipid vesicles.

Science.gov (United States)

Richens, Joanna L; Tyler, Arwen I I; Barriga, Hanna M G; Bramble, Jonathan P; Law, Robert V; Brooks, Nicholas J; Seddon, John M; Ces, Oscar; O'Shea, Paul

2017-10-03

An assay to study the spontaneous charged lipid transfer between lipid vesicles is described. A donor/acceptor vesicle system is employed, where neutrally charged acceptor vesicles are fluorescently labelled with the electrostatic membrane probe Fluoresceinphosphatidylethanolamine (FPE). Upon addition of charged donor vesicles, transfer of negatively charged lipid occurs, resulting in a fluorescently detectable change in the membrane potential of the acceptor vesicles. Using this approach we have studied the transfer properties of a range of lipids, varying both the headgroup and the chain length. At the low vesicle concentrations chosen, the transfer follows a first-order process where lipid monomers are transferred presumably through the aqueous solution phase from donor to acceptor vesicle. The rate of transfer decreases with increasing chain length which is consistent with energy models previously reported for lipid monomer vesicle interactions. Our assay improves on existing methods allowing the study of a range of unmodified lipids, continuous monitoring of transfer and simplified experimental procedures.

Interface charge transfer process in ZnO:Mn/ZnS nanocomposites

Energy Technology Data Exchange (ETDEWEB)

Stefan, M.; Toloman, D., E-mail: dana.toloman@itim-cj.ro; Popa, A. [National Institute for R & D of Isotopic and Molecular Technology (Romania); Mesaros, A. [Technical University of Cluj-Napoca, Superconductivity, Spintronics and Surface Science Center – C4S (Romania); Vasile, O. R. [University “Politehnica” from Bucharest, Faculty of Applied Chemistry and Material Science (Romania); Leostean, C.; Pana, O. [National Institute for R & D of Isotopic and Molecular Technology (Romania)

2016-03-15

ZnO:Mn/ZnS nanocomposites were prepared by seed-mediated growth of ZnS QDs onto the preformed ZnO:Mn nanoparticles. The formation of the nanocomposite structure has been evidenced by XRD, HRTEM, and XPS. The architecture of the nanocomposite with outer ZnS QDs around ZnO:Mn cores is sustained by the sulfur and oxygen depth profiles resulted from XPS. When the two components are brought together, the band gap of ZnS component decreases while that of ZnO:Mn increases. It is the result of interface charge transfer from ZnO:Mn to ZnS QDs. Here ZnO:Mn valence states are extended through the interface into unoccupied gap states of ZnS. The energy band setup is modified from a type II into a type I band alignment. The process is accompanied by enhancement of composite UV emission of PL spectra as compared to its counterparts. The charge transfer from valence band also determines the increase of the core-polarization effect of sshell electrons at Mn{sup 2+} nucleus, thus determining the increase of the hyperfine field through the reduction of the covalency degree of Zn(Mn)–O bonds. The quantum confinement in ZnS QDs promotes the ferromagnetic coupling of singly occupied states due to Zn vacancies determining a superparamagnetic behavior of the ensemble. When the nanocomposites are formed, due to interface charge transfer effects, an increased number of filled cation vacancies in ZnS QDs develop, thus disrupting the pre-existing ferromagnetic coupling between spins resulting in a significant reduction of the overall saturation magnetization. The possibility to modulate nanocomposite properties by controlling the interface interactions may be foreseen in these types of materials.

Thermoelastic/plastic analysis of waste-container sleeve: IV. Air gap influence on hole closure. Technical memorandum report (RSI-0019)

International Nuclear Information System (INIS)

Pariseau, W.G.

1975-01-01

A thermoelastic/plastic finite element analysis of the influence of an air-gap on hole closure about a waste-container/sleeve assembly emplaced in a typical repository room (SALT/4T Model) indicates that hole closure would be of the order of hundredths of an inch. Acceptable air-gap width is thus governed by the hole size required for emplacement efficiency. A refined mesh analysis and laboratory testing is suggested in order to further explore the possibility of eliminating the engineering necessity of the sleeve

Impact of exact exchange in the description of the electronic structure of organic charge-transfer molecular crystals

KAUST Repository

Fonari, Alexandr; Sutton, Christopher; Bredas, Jean-Luc; Coropceanu, Veaceslav

2014-01-01

in high-mobility organic crystals. We consider both crystals based on a single molecule, such as pentacene, and crystals based on mixed-stack charge-transfer systems, such as dibenzo-TTF–TCNQ. In the pentacene crystal, the band gap decreases

Photodissociation and charge transfer dynamics of negative ions studied with femtosecond photoelectron spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Zanni, Martin Thomas [Univ. of California, Berkeley, CA (United States)

1999-12-01

This dissertation presents studies aimed at understanding the potential energy surfaces and dynamics of isolated negative ions, and the effects of solvent on each. Although negative ions play important roles in atmospheric and solution phase chemistry, to a large extent the ground and excited state potential energy surfaces of gas phase negative ions are poorly characterized, and solvent effects even less well understood. In an effort to fill this gap, the author's coworkers and the author have developed a new technique, anion femtosecond photoelectron spectroscopy, and applied it to gas phase photodissociation and charge transfer processes. Studies are presented that (1) characterize the ground and excited states of isolated and clustered anions, (2) monitor the photodissociation dynamics of isolated and clustered anions, and (3) explore the charge-transfer-to-solvent states of atomic iodide clustered with polar and non-polar solvents.

Photodissociation and charge transfer dynamics of negative ions studied with femtosecond photoelectron spectroscopy

International Nuclear Information System (INIS)

Zanni, Martin T.

1999-01-01

This dissertation presents studies aimed at understanding the potential energy surfaces and dynamics of isolated negative ions, and the effects of solvent on each. Although negative ions play important roles in atmospheric and solution phase chemistry, to a large extent the ground and excited state potential energy surfaces of gas phase negative ions are poorly characterized, and solvent effects even less well understood. In an effort to fill this gap, the author's coworkers and the author have developed a new technique, anion femtosecond photoelectron spectroscopy, and applied it to gas phase photodissociation and charge transfer processes. Studies are presented that (1) characterize the ground and excited states of isolated and clustered anions, (2) monitor the photodissociation dynamics of isolated and clustered anions, and (3) explore the charge-transfer-to-solvent states of atomic iodide clustered with polar and non-polar solvents

DFT and TD-DFT computation of charge transfer complex between o-phenylenediamine and 3,5-dinitrosalicylic acid

International Nuclear Information System (INIS)

Afroz, Ziya; Zulkarnain,; Ahmad, Afaq; Alam, Mohammad Jane; Faizan, Mohd; Ahmad, Shabbir

2016-01-01

DFT and TD-DFT studies of o-phenylenediamine (PDA), 3,5-dinitrosalicylic acid (DNSA) and their charge transfer complex have been carried out at B3LYP/6-311G(d,p) level of theory. Molecular geometry and various other molecular properties like natural atomic charges, ionization potential, electron affinity, band gap, natural bond orbital (NBO) and frontier molecular analysis have been presented at same level of theory. Frontier molecular orbital and natural bond orbital analysis show the charge delocalization from PDA to DNSA.

Charge Transfer into Aqueous Droplets via Kilovolt Potentials

Science.gov (United States)

Hamlin, B. S.; Rosenberg, E. R.; Ristenpart, W. D.

2012-11-01

When an aqueous droplet immersed in an insulating oil contacts an electrified surface, the droplet acquires net charge. For sufficiently large field strengths, the charged droplet is driven back and forth electrophoretically between the electrodes, in essence ``bouncing'' between them. Although it is clear that the droplet acquires charge, the underlying mechanism controlling the charge transfer process has been unclear. Here we demonstrate that the chemical species present in the droplet strongly affect the charge transfer process into the drop. Using two independent charge measurement techniques, high speed video velocimetry and direct current measurement, we show that the charge acquired during contact is strongly influenced by the droplet pH. We also provide physical evidence that the electrodes undergo electroplating or corrosion for droplets with appropriate chemical species present. Together, the observations strongly suggest that electrochemical reactions govern the charge transfer process into the droplet.

Intramolecular Energy Transfer, Charge Transfer & Hydrogen Bond

Indian Academy of Sciences (India)

Ultrafast Dynamics of Chemical Reactions in Condensed Phase: Intramolecular Energy Transfer, Charge Transfer & Hydrogen Bond · PowerPoint Presentation · Slide 3 · Slide 4 · Slide 5 · Slide 6 · Slide 7 · Slide 8 · Slide 9 · Slide 10 · Slide 11 · Slide 12 · Slide 13 · Slide 14 · Slide 15 · Slide 16 · Slide 17 · Slide 18 · Slide 19.

Long-range corrected DFT calculations of charge-transfer integrals in model metal-free phthalocyanine complexes

Czech Academy of Sciences Publication Activity Database

Mikolajczyk, M. M.; Zalesny, R.; Czyznikowska, Z.; Toman, Petr; Leszczynski, J.; Bartkowiak, W.

2011-01-01

Roč. 17, č. 9 (2011), s. 2143-2149 ISSN 1610-2940 R&D Projects: GA ČR(CZ) GAP205/10/2280; GA MŠk MEB051010 Institutional research plan: CEZ:AV0Z40500505 Keywords : charge-transfer integral * density functional theory * long-range corrected functionals Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 1.797, year: 2011

Charge orders in organic charge-transfer salts

International Nuclear Information System (INIS)

Kaneko, Ryui; Valentí, Roser; Tocchio, Luca F; Becca, Federico

2017-01-01

Motivated by recent experimental suggestions of charge-order-driven ferroelectricity in organic charge-transfer salts, such as κ -(BEDT-TTF) 2 Cu[N(CN) 2 ]Cl, we investigate magnetic and charge-ordered phases that emerge in an extended two-orbital Hubbard model on the anisotropic triangular lattice at 3/4 filling. This model takes into account the presence of two organic BEDT-TTF molecules, which form a dimer on each site of the lattice, and includes short-range intramolecular and intermolecular interactions and hoppings. By using variational wave functions and quantum Monte Carlo techniques, we find two polar states with charge disproportionation inside the dimer, hinting to ferroelectricity. These charge-ordered insulating phases are stabilized in the strongly correlated limit and their actual charge pattern is determined by the relative strength of intradimer to interdimer couplings. Our results suggest that ferroelectricity is not driven by magnetism, since these polar phases can be stabilized also without antiferromagnetic order and provide a possible microscopic explanation of the experimental observations. In addition, a conventional dimer-Mott state (with uniform density and antiferromagnetic order) and a nonpolar charge-ordered state (with charge-rich and charge-poor dimers forming a checkerboard pattern) can be stabilized in the strong-coupling regime. Finally, when electron–electron interactions are weak, metallic states appear, with either uniform charge distribution or a peculiar 12-site periodicity that generates honeycomb-like charge order. (paper)

Gap states of charged soliton in polyacetylene

International Nuclear Information System (INIS)

Lu Dingwei; Liu Jie; Fu Rouli

1988-10-01

By considering the electron interaction in polyacetylene, it is found that two gap states in charged solitons of trans-polyacetylene exist: one is deep level, another is shallow level. The deep one shifts 0.23 ev down (for positive soliton) or up (for negative soliton) from the center of the gap; while the shallow one is 0.06 ev under the bottom of conduction band (positive soliton) or above the top of valence band (negative soliton). These results agree with the absorption spectra of trans-polyacetylene. (author). 5 refs, 4 figs

Bond charges and electronic charge transfer in ternary semiconductors

International Nuclear Information System (INIS)

Pietsch, U.

1986-01-01

By means of a simple molecule-theoretic model of 'linear superposition of two-electron molecules' the bond charges between nearest neighbours and the effective charges of ions are calculated for ternary zinc-blende structure alloys as well as chalcopyrite semiconductors. Taking into account both, the charge transfer among the ions caused by the differences of electronegativities of atoms used and between the bonds created by the internal stress of the lattice a nearly unvaried averaged bond charge amount of the alloy is found, but rather dramatically changed local bond charge parameters in comparison with the respective values of binary compounds used. This fact should influence the noncentral force interaction in such semiconductors. (author)

Impact of charge-transfer excitons in regioregular polythiophene on the charge separation at polythiophene-fullerene heterojunctions

Science.gov (United States)

Polkehn, M.; Tamura, H.; Burghardt, I.

2018-01-01

This study addresses the mechanism of ultrafast charge separation in regioregular oligothiophene-fullerene assemblies representative of poly-3-hexylthiophene (P3HT)-[6,6]-phenyl-C61 butyric acid methyl ester (PCBM) heterojunctions, with special emphasis on the inclusion of charge transfer excitons in the oligothiophene phase. The formation of polaronic inter-chain charge separated species in highly ordered oligothiophene has been demonstrated in recent experiments and could have a significant impact on the net charge transfer to the fullerene acceptor. The present approach combines a first-principles parametrized multi-site Hamiltonian, based on time-dependent density functional theory calculations, with accurate quantum dynamics simulations using the multi-layer multi-configuration time-dependent Hartree method. Quantum dynamical studies are carried out for up to 182 electronic states and 112 phonon modes. The present analysis follows up on our previous study of (Huix-Rotllant et al 2015 J. Phys. Chem. Lett. 6 1702) and significantly expands the scope of this analysis by including the dynamical role of charge transfer excitons. Our investigation highlights the pronounced mixing of photogenerated Frenkel excitons with charge transfer excitons in the oligothiophene domain, and the opening of new transfer channels due the creation of such charge-separated species. As a result, it turns out that the interfacial donor/acceptor charge transfer state can be largely circumvented due to the presence of charge transfer excitons. However, the latter states in turn act as a trap, such that the free carrier yield observed on ultrafast time scales is tangibly reduced. The present analysis underscores the complexity of the transfer pathways at P3HT-PCBM type junctions.

Efficient charge generation by relaxed charge-transfer states at organic interfaces

KAUST Repository

Vandewal, Koen

2013-11-17

Interfaces between organic electron-donating (D) and electron-accepting (A) materials have the ability to generate charge carriers on illumination. Efficient organic solar cells require a high yield for this process, combined with a minimum of energy losses. Here, we investigate the role of the lowest energy emissive interfacial charge-transfer state (CT1) in the charge generation process. We measure the quantum yield and the electric field dependence of charge generation on excitation of the charge-transfer (CT) state manifold via weakly allowed, low-energy optical transitions. For a wide range of photovoltaic devices based on polymer:fullerene, small-molecule:C60 and polymer:polymer blends, our study reveals that the internal quantum efficiency (IQE) is essentially independent of whether or not D, A or CT states with an energy higher than that of CT1 are excited. The best materials systems show an IQE higher than 90% without the need for excess electronic or vibrational energy. © 2014 Macmillan Publishers Limited.

Efficient charge generation by relaxed charge-transfer states at organic interfaces

KAUST Repository

Vandewal, Koen; Albrecht, Steve N.; Hoke, Eric T.; Graham, Kenneth; Widmer, Johannes; Douglas, Jessica D.; Schubert, Marcel; Mateker, William R.; Bloking, Jason T.; Burkhard, George F.; Sellinger, Alan; Frechet, Jean; Amassian, Aram; Riede, Moritz Kilian; McGehee, Michael D.; Neher, Dieter; Salleo, Alberto

2013-01-01

Interfaces between organic electron-donating (D) and electron-accepting (A) materials have the ability to generate charge carriers on illumination. Efficient organic solar cells require a high yield for this process, combined with a minimum of energy losses. Here, we investigate the role of the lowest energy emissive interfacial charge-transfer state (CT1) in the charge generation process. We measure the quantum yield and the electric field dependence of charge generation on excitation of the charge-transfer (CT) state manifold via weakly allowed, low-energy optical transitions. For a wide range of photovoltaic devices based on polymer:fullerene, small-molecule:C60 and polymer:polymer blends, our study reveals that the internal quantum efficiency (IQE) is essentially independent of whether or not D, A or CT states with an energy higher than that of CT1 are excited. The best materials systems show an IQE higher than 90% without the need for excess electronic or vibrational energy. © 2014 Macmillan Publishers Limited.

The description of charge transfer in fast negative ions scattering on water covered Si(100) surfaces

Energy Technology Data Exchange (ETDEWEB)

Chen, Lin; Qiu, Shunli; Liu, Pinyang; Xiong, Feifei; Lu, Jianjie; Liu, Yuefeng; Li, Guopeng; Liu, Yiran; Ren, Fei; Xiao, Yunqing; Gao, Lei; Zhao, Qiushuang; Ding, Bin; Li, Yuan [School of Nuclear Science and Technology, Lanzhou University, 730000 (China); Key Laboratory of Special Function Materials and Structure Design, Ministry of Education, Lanzhou University, 730000 (China); Guo, Yanling, E-mail: guoyanling@lzu.edu.cn [School of Nuclear Science and Technology, Lanzhou University, 730000 (China); Key Laboratory of Special Function Materials and Structure Design, Ministry of Education, Lanzhou University, 730000 (China); Chen, Ximeng, E-mail: chenxm@lzu.edu.cn [School of Nuclear Science and Technology, Lanzhou University, 730000 (China); Key Laboratory of Special Function Materials and Structure Design, Ministry of Education, Lanzhou University, 730000 (China)

2016-11-30

Highlights: • We first observe that negative-ion fractions present no variation with the doping concentration, which is very different from the results of low energy Li neutralization from doped Si samples. • Our work shows that the affinity levels and collision time significantly counteract the band gap effect on negative ion formation. The work will improve our understanding on electron transfer on semiconductor surfaces associated with doping. • In addition, we build a complete theoretical framework to quantitatively calculate the negative-ion fractions. • Our work is related to charge transfer on semiconductor surfaces, which will be of interest to a broad audience due to the wide necessity of the knowledge of charge exchange on semiconductor surfaces in different fields. - Abstract: Doping has significantly affected the characteristics and performance of semiconductor electronic devices. In this work, we study the charge transfer processes for 8.5–22.5 keV C{sup −} and F{sup −} ions scattering on H{sub 2}O-terminated p-type Si(100) surfaces with two different doping concentrations. We find that doping has no influence on negative-ion formation for fast collisions in this relatively high energy range. Moreover, we build a model to calculate negative ion fractions including the contribution from positive ions. The calculations support the nonadiabatic feature of charge transfer.

The charge transfer structure and effective energy transfer in multiplayer assembly film

International Nuclear Information System (INIS)

Li Mingqiang; Jian Xigao

2005-01-01

Charge transfer multiplayer films have been prepared by layer-by-layer self-assembly technique. The films incorporate the rare-earth-containing polyoxometalate K 11 [Eu{PW 11 O 39 } 2 ].nH 2 O and the rich electron polyelectrolyte poly(3-viny-1-methyl-pyridine) quaternary ammonium and display a linear increase in the absorption and film thickness with the number of deposition cycles. Ultraviolet and visible absorption spectra, atomic force micrographs, small-angle X-ray reflectivity measurements, and photoluminescence spectra were used to determine the structure of films. Linear and regular multilayer growth was observed. We can observe the formation of charge transfer complex compound in multiplayer by layer-by-layer assembly method. Most importantly, the luminescence spectra show the charge transfer band in assembly films, which suggest that energy could be effectively transferred to rare earth ions in assembly multiplayer films

Two-Centre Close-Coupling method in charge transfer

Directory of Open Access Journals (Sweden)

Reza Bagheri

2017-09-01

Full Text Available In the present work, the transition matrix elements as well as differential and total scattering cross-sections for positronium formation in Positron-Hydrogen atom collision and hydrogen formation in Positronium-Hydrogen ion collision, through the charge transfer channel by Two-Centre Close-Coupling method up to a first order approximation have been calculated. The charge transfer collision is assumed to be a three-body reaction, while the projectile is a plane wave. Additionally, the hydrogen and positronium atoms are assumed, initially, to be in their ground states. For the case of charge transfer in the scattering of positron by hydrogen atoms, the differential cross sections are plotted for the energy range of 50eV to 10keV, where the Thomas peak is clearly observable. Finally, the total scattering cross-section for the charge transfer in the collision of Positron-Hydrogen and Positronium-Hydrogen ion are plotted as a function of projectile energies and compared with other methods in the literature.

Charge transfer and injection barrier at the metal-organic interfaces

Science.gov (United States)

Yan, Li

2002-09-01

The metal-organic interface plays a critical role in determining the functionality and performance of many innovative organic based devices. It has attracted extensive research interests in recent years. This thesis presents investigations of the electronic structures of organic materials, such as tris-(8-hydroxyquinoline) aluminum (Alq3) and copper phthalocyanine (CuPc), during their interface formation with metals. The characterization is accomplished by X-ray and ultraviolet photoelectron spectroscopes (XPS and UPS) and inverse photoelectron spectroscopy (IPES). As discussed herein, both occupied and unoccupied electronic states at the interfaces are carefully examined in different aspects. In Chapter 4, the charge transfer and chemical reaction at various metal/Alq3 interfaces are investigated using XPS and UPS to study the electron injection into the Alga film. Electron transfer from the low work function metal and Al/LiF(CsF) bilayer to the Alga has been observed. The role of the dielectric and possible chemistry at the interface are discussed in comparison of the low work function metals. Further in Chapter 5, the origin of the metal-interface dipole and the estimation of charge injection barrier is explored using several organic materials. A thermodynamic equilibrium model is extended to explain the relation between the charge transfer process ad the interface dipole. Further, in Chapter 6 the combination of XPS, UPS and IPES detailed the evolution of both occupied and unoccupied energy states during the alkali metal doping. The energy gap modification in organic due to metal doping is observed directly for the spectra. Chapter 7 provides stability study of the organic thin films under x-ray and UV light. The results verify the usability of UPS and XPS for the organic materials used in the thesis. Chapter 7 also shows the secondary ion mass spectroscopy results of metal diffusion in organic thin films.

Beginning-of-life gap closure behaviour of experimental PFBR MOX fuel pin

International Nuclear Information System (INIS)

Jayaraj, V.V.; Padalakshmi, M.; Ojha, B.K.; Padma Prabu, C.; Saravanan, T.; Venkiteswaran, C.N.; Philip, John; Muralidharan, N.G.; Joseph, Jojo; Kasiviswanathan, K.V.; Jayakumar, T.

2011-01-01

Mixed oxide fuel with 22 % and 29% plutonium is chosen as the fuel for PFBR for the two fissile zones. Due to the fabrication tolerances in the pellet diameter, fuel has to be preconditioned at a lower linear power for a brief period before raising the power to the rated value of 450 W/cm. PIE was done on an experimental MOX fuel pin irradiated in FBTR for 13 days at a linear power of 400 W/cm for gap closure studies with the objective of optimising the duration of pre-conditioning before raising the power to the design value of 450 W/cm. X-radiography and remote metallography was done on the fuel pin to estimate the axial fuel column elongation and fuel-clad gap. Remote metallography of the fuel pin cross-sections at five axial locations of the fuel column and the subsequent fuel-clad gap measurement has indicated that the average radial gap has reduced from the pre-irradiation value of 75-110 microns to around 12-13 microns along the entire length of the fuel column. This paper will describe the details of examinations and results of the PIE carried out on the MOX fuel pin. (author)

Charge distribution dependency on gap thickness of CMS endcap RPC

CERN Document Server

Park, Sung Keun

2016-01-01

We present a systematic study of charge distribution dependency of CMS Resistive Plate Chamber (RPC) on gap thickness.Prototypes of double-gap with five different gap thickness from 1.8mm to 1.0mm in 0.2mm steps have been built with 2mm thick phenolic high-pressure-laminated (HPL) plates. The charges of cosmic-muon signals induced on the detector strips are measured as a function of time using two four-channel 400-MHz fresh ADCs. In addition, the arrival time of the muons and the strip cluster sizes are measured by digitizing the signal using a 32-channel voltage-mode front-end-electronics and a 400-MHz 64-channel multi-hit TDC. The gain and the input impedance of the front-end-electronics were 200mV/mV and 20 Ohm, respectively.

Boosting the Visible-Light Photoactivity of BiOCl/BiVO4/N-GQD Ternary Heterojunctions Based on Internal Z-Scheme Charge Transfer of N-GQDs: Simultaneous Band Gap Narrowing and Carrier Lifetime Prolonging.

Science.gov (United States)

Zhu, Mingyue; Liu, Qian; Chen, Wei; Yin, Yuanyuan; Ge, Lan; Li, Henan; Wang, Kun

2017-11-08

The efficient separation of photogenerated electron-hole pairs in photoactive materials is highly desired, allowing their transfer to specific sites for undergoing redox reaction in various applications. The construction of ternary heterojunctions is a practical strategy to enhance the migration of photogenerated electron that realizes the synergistic effect of multicomponents rather than the simple overlay of single component. Here, we demonstrate an available way to fabricate new BiOCl/BiVO 4 /nitrogen-doped graphene quantum dot (N-GQD) ternary heterojunctions that exhibit higher efficiency in charge separation than any binary heterojunction or pure material under visible-light irradiation. UV-vis diffuse reflectance spectroscopy demonstrated that the proposed BiOCl/BiVO 4 /N-GQD ternary heterojunctions possess the narrower band gap energy. More importantly, the ternary heterojunctions reveal the prolonged lifetime of photogenerated charges and enhanced the separation efficiency of photogenerated electron-hole pairs, which may be ascribed to sensitization based on an internal Z-scheme charge transfer at the interface of N-GQDs with oxygen functional groups. Furthermore, we examine the photoactive performance of proposed ternary heterojunctions in aqueous solution by using the photodegradation of bisphenol A as a model system and BiOCl/BiVO 4 /N-GQD ternary heterojunctions also display a dramatically enhanced photodegradation rate. The proposed charge separation and transfer process of BiOCl/BiVO 4 /N-GQD ternary heterojunctions for the enhanced photoactivity were deduced by electrochemical measurements, photoluminescence, and electron spin resonance. The results demonstrate that a Z-scheme charge process was formed between BiOCl/BiVO 4 binary heterojunctions and N-GQDs, leading to an efficient charge carrier separation and strong photocatalytic ability. Notably, this work may assist in a better understanding of the role of N-GQDs in kinds of heterojunctions

Detection of Intramolecular Charge Transfer and Dynamic Solvation in Eosin B by Femtosecond Two-Dimensional Electronic Spectroscopy

Science.gov (United States)

Ghosh, Soumen; Roscioli, Jerome D.; Beck, Warren F.

2014-06-01

We have employed 2D electronic photon echo spectroscopy to study intramolecular charge-transfer dynamics in eosin B. After preparation of the first excited singlet state (S_1) with 40-fs excitation pulses at 520 nm, the nitro group (--NO_2) in eosin B undergoes excited state torsional motion towards a twisted intramolecular charge transfer (TICT) state. As the viscosity of the surrounding solvent increases, the charge-transfer rate decreases because the twisting of the --NO_2 group is hindered. These conclusions are supported by the time evolution of the 2D spectrum, which provides a direct measure of the the ground-to-excited-state energy gap time-correlation function, M(t). In comparison to the inertial and diffusive solvation time scales exhibited by eosin Y, which lacks the nitro group, the M(t) function for eosin B exhibits under the same conditions an additional component on the 150-fs timescale that arises from quenching of the S_1 state by crossing to the TICT state. These results indicate that 2D electronic spectroscopy can be used as a sensitive probe of the rate of charge transfer in a molecular system and of the coupling to the motions of the surrounding solvent. (Supported by grant DE-SC0010847 from the Department of Energy, Office of Basic Energy Sciences, Photosynthetic Systems program.)

Charge transfer complex in diketopyrrolopyrrole polymers and fullerene blends: Implication for organic solar cell efficiency

Science.gov (United States)

Moghe, D.; Yu, P.; Kanimozhi, C.; Patil, S.; Guha, S.

2012-02-01

Copolymers based on diketopyrrolopyrrole (DPP) have recently gained potential in organic photovoltaics. When blended with another acceptor such as PCBM, intermolecular charge transfer occurs which may result in the formation of charge transfer (CT) states. We present here the spectral photocurrent characteristics of two donor-acceptor DPP based copolymers, PDPP-BBT and TDPP-BBT, blended with PCBM to identify the CT states. The spectral photocurrent measured using Fourier-transform photocurrent spectroscopy (FTPS) and monochromatic photocurrent (PC) methods are compared with P3HT:PCBM, where the CT state is well known. PDPP-BBT:PCBM shows a stable CT state while TDPP-BBT does not. Our analysis shows that the larger singlet state energy difference between TDPP-BBT and PCBM along with the lower optical gap of TDPP-BBT obliterates the formation of a midgap CT state resulting in an enhanced photovoltaic efficiency over PDPP-BBT:PCBM.

Collisional charging of individual submillimeter particles: Using ultrasonic levitation to initiate and track charge transfer

Science.gov (United States)

Lee, Victor; James, Nicole M.; Waitukaitis, Scott R.; Jaeger, Heinrich M.

2018-03-01

Electrostatic charging of insulating fine particles can be responsible for numerous phenomena ranging from lightning in volcanic plumes to dust explosions. However, even basic aspects of how fine particles become charged are still unclear. Studying particle charging is challenging because it usually involves the complexities associated with many-particle collisions. To address these issues, we introduce a method based on acoustic levitation, which makes it possible to initiate sequences of repeated collisions of a single submillimeter particle with a flat plate, and to precisely measure the particle charge in situ after each collision. We show that collisional charge transfer between insulators is dependent on the hydrophobicity of the contacting surfaces. We use glass, which we modify by attaching nonpolar molecules to the particle, the plate, or both. We find that hydrophilic surfaces develop significant positive charges after contacting hydrophobic surfaces. Moreover, we demonstrate that charging between a hydrophilic and a hydrophobic surface is suppressed in an acidic environment and enhanced in a basic one. Application of an electric field during each collision is found to modify the charge transfer, again depending on surface hydrophobicity. We discuss these results within the context of contact charging due to ion transfer, and we show that they lend strong support to O H- ions as the charge carriers.

Bridging the Gap in Knowledge Transfer between Academia and Practitioners

Science.gov (United States)

Gera, Rajat

2012-01-01

Purpose: The paper intends to identify the causes or gaps in transfer of managerial knowledge between academia and practitioners and to develop a framework that overcomes the gaps through knowledge management, information technology and human resource practices. The paper aims to suggest a strategic approach based on the knowledge transfer cycle.…

Dynamic response functions, helical gaps, and fractional charges in quantum wires

Science.gov (United States)

Meng, Tobias; Pedder, Christopher J.; Tiwari, Rakesh P.; Schmidt, Thomas L.

We show how experimentally accessible dynamic response functions can discriminate between helical gaps due to magnetic field, and helical gaps driven by electron-electron interactions (''umklapp gaps''). The latter are interesting since they feature gapped quasiparticles of fractional charge e / 2 , and - when coupled to a standard superconductor - an 8 π-Josephson effect and topological zero energy states bound to interfaces. National Research Fund, Luxembourg (ATTRACT 7556175), Deutsche Forschungsgemeinschaft (GRK 1621 and SFB 1143), Swiss National Science Foundation.

Charge-transfer channel in quantum dot-graphene hybrid materials

Science.gov (United States)

Cao, Shuo; Wang, Jingang; Ma, Fengcai; Sun, Mengtao

2018-04-01

The energy band theory of a classical semiconductor can qualitatively explain the charge-transfer process in low-dimensional hybrid colloidal quantum dot (QD)-graphene (GR) materials; however, the definite charge-transfer channels are not clear. Using density functional theory (DFT) and time-dependent DFT, we simulate the hybrid QD-GR nanostructure, and by constructing its orbital interaction diagram, we show the quantitative coupling characteristics of the molecular orbitals (MOs) of the hybrid structure. The main MOs are derived from the fragment MOs (FOs) of GR, and the Cd13Se13 QD FOs merge with the GR FOs in a certain proportion to afford the hybrid system. Upon photoexcitation, electrons in the GR FOs jump to the QD FOs, leaving holes in the GR FOs, and the definite charge-transfer channels can be found by analyzing the complex MOs coupling. The excited electrons and remaining holes can also be localized in the GR or the QD or transfer between the QD and GR with different absorption energies. The charge-transfer process for the selected excited states of the hybrid QD-GR structure are testified by the charge difference density isosurface. The natural transition orbitals, charge-transfer length analysis and 2D site representation of the transition density matrix also verify the electron-hole delocalization, localization, or coherence chacracteristics of the selected excited states. Therefore, our research enhances understanding of the coupling mechanism of low-dimensional hybrid materials and will aid in the design and manipulation of hybrid photoelectric devices for practical application in many fields.

Charge transfer reactions in Xe plasma expansion

International Nuclear Information System (INIS)

Jiao, C. Q.; Garscadden, A.; Ganguly, B. N.

2007-01-01

Charge transfer reactions of fast Xe ions with hydrocarbons including methane (CH 4 ), ethene (C 2 H 4 ), and propane (C 3 H 8 ) are studied by adding these hydrocarbon gases into a cross flowing Xe plasma expansion. Branching ratios and relative reaction rates for the charge transfers of fast Xe + with each of the three hydrocarbon gases are measured under different rf powers of the inductively coupled Xe discharge. For CH 4 /Xe system, we find that fast Xe + reacts readily with CH 4 generating CH 4 + and CH 3 + in a ratio of 1:0.56, with an estimated rate coefficient of (2.3±0.3)x10 -10 cm 3 /s at 75 W rf power which slowly increases to (2.9±0.3)x10 -10 cm 3 /s at 250 W (error bars reflect only the uncertainties due to the unknown extent of the ion recombination that follows the charge transfer reaction). These observed charge transfer reactions are made possible by the kinetically excited Xe ions produced by free expansion of the plasma. For the C 2 H 4 /Xe system product ions C 2 H 4 + and C 2 H 2 + are observed, and for C 3 H 8 /Xe, C 2 H 4 + and C 2 H 5 + and minor product ions including C 2 H 2 + and C 3 H 7 + are observed

Charge-transfer cross sections in collisions of ground-state Ca and H+

Science.gov (United States)

Dutta, C. M.; Oubre, C.; Nordlander, P.; Kimura, M.; Dalgarno, A.

2006-03-01

We have investigated collisions of Ca(4s2) with H+ in the energy range of 200eV/u-10keV/u using the semiclassical molecular-orbital close-coupling (MOCC) method with 18 coupled molecular states ( 11Σ+1 and seven Π+1 states) to determine charge-transfer cross sections. Except for the incoming channel 6Σ+1 , the molecular states all correspond to charge-transfer channels. Inclusion of Ca2+-H- is crucial in the configuration-interaction calculation for generating the molecular wave functions and potentials. Because of the Coulomb attraction, the state separating to Ca2+-H- creates many avoided crossings, even though at infinite separation it lies energetically above all other states that we included. Because of the avoided crossings between the incoming channel 6Σ+1 and the energetically close charge-transfer channel 7Σ+1 the charge-transfer interaction occurs at long range. This makes calculations of charge-transfer cross sections by the MOCC method very challenging. The total charge-transfer cross sections increase monotonically from 3.4×10-15cm2 at 200eV/u to 4.5×10-15cm2 at 10keV/u . Charge transfer occurs mostly to the excited Ca+(5p) state in the entire energy range, which is the sum of the charge transfer to 7Σ+1 and 4Π+1 . It accounts for ˜47% of the total charge transfer cross sections at 200eV/u . However, as the energy increases, transfer to Ca+(4d) increases, and at 10keV/u the charge-transfer cross sections for Ca+(5p) and Ca+(4d) become comparable, each giving ˜38% of the total cross section.

Charge-transfer cross sections in collisions of ground-state Ca and H+

International Nuclear Information System (INIS)

Dutta, C. M.; Oubre, C.; Nordlander, P.; Kimura, M.; Dalgarno, A.

2006-01-01

We have investigated collisions of Ca(4s 2 ) with H + in the energy range of 200 eV/u-10 keV/u using the semiclassical molecular-orbital close-coupling (MOCC) method with 18 coupled molecular states (11 1 Σ + and seven 1 Π + states) to determine charge-transfer cross sections. Except for the incoming channel 6 1 Σ + , the molecular states all correspond to charge-transfer channels. Inclusion of Ca 2+ -H - is crucial in the configuration-interaction calculation for generating the molecular wave functions and potentials. Because of the Coulomb attraction, the state separating to Ca 2+ -H - creates many avoided crossings, even though at infinite separation it lies energetically above all other states that we included. Because of the avoided crossings between the incoming channel 6 1 Σ + and the energetically close charge-transfer channel 7 1 Σ + the charge-transfer interaction occurs at long range. This makes calculations of charge-transfer cross sections by the MOCC method very challenging. The total charge-transfer cross sections increase monotonically from 3.4x10 -15 cm 2 at 200 eV/u to 4.5x10 -15 cm 2 at 10 keV/u. Charge transfer occurs mostly to the excited Ca + (5p) state in the entire energy range, which is the sum of the charge transfer to 7 1 Σ + and 4 1 Π + . It accounts for ∼47% of the total charge transfer cross sections at 200 eV/u. However, as the energy increases, transfer to Ca + (4d) increases, and at 10 keV/u the charge-transfer cross sections for Ca + (5p) and Ca + (4d) become comparable, each giving ∼38% of the total cross section

Quasi-resonant K-K charge transfer

International Nuclear Information System (INIS)

Hagmann, S.; Cocke, C.L.; Richard, P.; Skutlartz, A.; Kelbch, S.; Schmidt-Boecking, H.; Schuch, R.

1983-01-01

The impact parameter dependence, P(b), of single and double K to K charge transfer have been deduced from the coincidences between K-Auger electrons and scattered particles for F 9+ + Ne and F 9+ + Ne collisions at 10 MeV and 4.4 MeV. The 4.4 MeV single K-K transfer probability exhibits oscillations with b. The P(b) for delta-electron emission is also reported. To obtain more details on the mechanism, K-Auger electron-Ne recoil ion coincidences are measured for both F 8+ and F 9+ projectiles. The relative amounts of recoil ions and of satellite and hypersatellite Auger transitions vary substantially with projectile charge state. 11 references, 11 figures

Mass and charge transfer within a floating water bridge

Science.gov (United States)

Fuchs, Elmar C.; Agostinho, Luewton L. F.; Eisenhut, Mathias; Woisetschläger, Jakob

2010-11-01

When high voltage is applied to pure water filled into two beakers close to each other, a connection forms spontaneously, giving the impression of a floating water bridge 1-8. This phenomenon is of special interest, since it comprises a number of phenomena currently tackled in modern water science. In this work, the charge and mass transfer through the water bridge are investigated with schlieren visualization and laser interferometry. It can be shown that the addition of a pH dye increases the H+ and OH- production with subsequent electrolysis, whereas schlieren and interferometric methods reveal another mechanism where charge and mass transfer appear to be coupled. Whereas this mechanism seems to be responsible for the electrolysis-less charge and mass transfer in the water bridge, it is increasingly superseded by the electrochemical mechanism with rising conductivity. Thus it can be shown that a pH dye does only indirectly visualize the charge transfer in the water bridge since it is dragged along with the water flow like any other dye, and additionally promotes conventional electrochemical conduction mechanisms, thereby enhancing electrolysis and reducing the masscoupled charge transport and thus destabilizing the bridge.

Synthesis of Stable Interfaces on SnO2 Surfaces for Charge-Transfer Applications

Science.gov (United States)

Benson, Michelle C.

The commercial market for solar harvesting devices as an alternative energy source requires them to be both low-cost and efficient to replace or reduce the dependence on fossil fuel burning. Over the last few decades there has been promising efforts towards improving solar devices by using abundant and non-toxic metal oxide nanomaterials. One particular metal oxide of interest has been SnO2 due to its high electron mobility, wide-band gap, and aqueous stability. However SnO2 based solar cells have yet to reach efficiency values of other metal oxides, like TiO2. The advancement of SnO2 based devices is dependent on many factors, including improved methods of surface functionalization that can yield stable interfaces. This work explores the use of a versatile functionalization method through the use of the Cu(I)-catalyzed azide-alkyne cycloaddition (CuAAC) reaction. The CuAAC reaction is capable of producing electrochemically, photochemically, and electrocatalytically active surfaces on a variety of SnO2 materials. The resulting charge-transfer characteristics were investigated as well as an emphasis on understanding the stability of the resulting molecular linkage. We determined the CuAAC reaction is able to proceed through both azide-modified and alkyne-modified surfaces. The resulting charge-transfer properties showed that the molecular tether was capable of supporting charge separation at the interface. We also investigated the enhancement of electron injection upon the introduction of an ultra-thin ZrO2 coating on SnO2. Several complexes were used to fully understand the charge-transfer capabilities, including model systems of ferrocene and a ruthenium coordination complex, a ruthenium mononuclear water oxidation catalyst, and a commercial ruthenium based dye.

Effects of Charge-Transfer Excitons on the Photophysics of Organic Semiconductors

Science.gov (United States)

Hestand, Nicholas J.

The field of organic electronics has received considerable attention over the past several years due to the promise of novel electronic materials that are cheap, flexible and light weight. While some devices based on organic materials have already emerged on the market (e.g. organic light emitting diodes), a deeper understanding of the excited states within the condensed phase is necessary both to improve current commercial products and to develop new materials for applications that are currently in the commercial pipeline (e.g. organic photovoltaics, wearable displays, and field effect transistors). To this end, a model for pi-conjugated molecular aggregates and crystals is developed and analyzed. The model considers two types of electronic excitations, namely Frenkel and charge-transfer excitons, both of which play a prominent role in determining the nature of the excited states within tightly-packed organic systems. The former consist of an electron-hole pair bound to the same molecule while in the later the electron and hole are located on different molecules. The model also considers the important nuclear reorganization that occurs when the system switches between electronic states. This is achieved using a Holstein-style Hamiltonian that includes linear vibronic coupling of the electronic states to the nuclear motion associated with the high frequency vinyl-stretching and ring-breathing modes. Analysis of the model reveals spectroscopic signatures of charge-transfer mediated J- and H-aggregation in systems where the photophysical properties are determined primarily by charge-transfer interactions. Importantly, such signatures are found to be sensitive to the relative phase of the intermolecular electron and hole transfer integrals, and the relative energy of the Frenkel and charge-transfer states. When the charge-transfer integrals are in phase and the energy of the charge-transfer state is higher than the Frenkel state, the system exhibits J

Charge transfer through DNA/DNA duplexes and DNA/RNA hybrids: complex theoretical and experimental studies

Czech Academy of Sciences Publication Activity Database

Kratochvílová, Irena; Vala, M.; Weiter, M.; Špérová, M.; Schneider, Bohdan; Páv, Ondřej; Šebera, Jakub; Rosenberg, Ivan; Sychrovský, Vladimír

180-181, Oct-Nov (2013), s. 127-134 ISSN 0301-4622 R&D Projects: GA TA ČR TA01011165; GA ČR(CZ) GAP304/10/1951; GA ČR GA13-27676S; GA ČR GA202/09/0193 Institutional support: RVO:68378271 ; RVO:86652036 ; RVO:61388963 Keywords : charge transfer in oligonucleotides * temperature dependent steady state fluorescence spectroscopy * time-resolved fluorescence spectroscopy Subject RIV: JJ - Other Materials; CC - Organic Chemistry (UOCHB-X) Impact factor: 2.319, year: 2013

Charge transfer cross sections for dysprosium and cerium

Energy Technology Data Exchange (ETDEWEB)

Adachi, Hajime; Tamura, Koji; Okazaki, Tetsuji; Shibata, Takemasa [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

1998-06-01

Symmetric resonant charge transfer cross sections between singly ionized ions and the parent atoms were measured for dysprosium and cerium in the impact energy of 200-2000eV. The cross sections were determined from the ratio between the number of ions produced by charge transfer and those in primary ion beam. The primary ion beam was produced by a laser ion source in which their atoms were ionized by laser resonant photo-ionization. The slow ions produced by charge transfer and fast primary ions were detected with Faraday cups. The obtained cross sections were (1.82{+-}0.14) x 10{sup -14} cm{sup 2} for dysprosium and (0.88{+-}0.12) x 10{sup -14} cm{sup 2} for cerium in the above energy range. The difference of these values can mostly be explained by considering the electron configurations of these atoms and ions. (author)

Charge transfer cross sections for dysprosium and cerium

International Nuclear Information System (INIS)

Adachi, Hajime; Tamura, Koji; Okazaki, Tetsuji; Shibata, Takemasa

1998-06-01

Symmetric resonant charge transfer cross sections between singly ionized ions and the parent atoms were measured for dysprosium and cerium in the impact energy of 200-2000eV. The cross sections were determined from the ratio between the number of ions produced by charge transfer and those in primary ion beam. The primary ion beam was produced by a laser ion source in which their atoms were ionized by laser resonant photo-ionization. The slow ions produced by charge transfer and fast primary ions were detected with Faraday cups. The obtained cross sections were (1.82±0.14) x 10 -14 cm 2 for dysprosium and (0.88±0.12) x 10 -14 cm 2 for cerium in the above energy range. The difference of these values can mostly be explained by considering the electron configurations of these atoms and ions. (author)

Charge Transfer and Catalysis at the Metal Support Interface

Energy Technology Data Exchange (ETDEWEB)

Baker, Lawrence Robert [Univ. of California, Berkeley, CA (United States)

2012-07-31

Kinetic, electronic, and spectroscopic characterization of model Pt–support systems are used to demonstrate the relationship between charge transfer and catalytic activity and selectivity. The results show that charge flow controls the activity and selectivity of supported metal catalysts. This dissertation builds on extensive existing knowledge of metal–support interactions in heterogeneous catalysis. The results show the prominent role of charge transfer at catalytic interfaces to determine catalytic activity and selectivity. Further, this research demonstrates the possibility of selectively driving catalytic chemistry by controlling charge flow and presents solid-state devices and doped supports as novel methods for obtaining electronic control over catalytic reaction kinetics.

Charge-transfer modified embedded atom method dynamic charge potential for Li-Co-O system.

Science.gov (United States)

Kong, Fantai; Longo, Roberto C; Liang, Chaoping; Nie, Yifan; Zheng, Yongping; Zhang, Chenxi; Cho, Kyeongjae

2017-11-29

To overcome the limitation of conventional fixed charge potential methods for the study of Li-ion battery cathode materials, a dynamic charge potential method, charge-transfer modified embedded atom method (CT-MEAM), has been developed and applied to the Li-Co-O ternary system. The accuracy of the potential has been tested and validated by reproducing a variety of structural and electrochemical properties of LiCoO 2 . A detailed analysis on the local charge distribution confirmed the capability of this potential for dynamic charge modeling. The transferability of the potential is also demonstrated by its reliability in describing Li-rich Li 2 CoO 2 and Li-deficient LiCo 2 O 4 compounds, including their phase stability, equilibrium volume, charge states and cathode voltages. These results demonstrate that the CT-MEAM dynamic charge potential could help to overcome the challenge of modeling complex ternary transition metal oxides. This work can promote molecular dynamics studies of Li ion cathode materials and other important transition metal oxides systems that involve complex electrochemical and catalytic reactions.

Voltammetry for the charge transfer at two immiscible electrolyte solutions interface

International Nuclear Information System (INIS)

Kihara, S.; Suzuki, M.; Maeda, K.; Ogura, K.; Matsui, M.; Yoshida, Z.

1989-01-01

The voltammetry for the charge transfer (VCT) at the interface of immicible solutions is a very powerful method for understanding the dynamic features of the charge transfer because of its unmatched advantage that the transfer energy and the number of charges transferred can be measured simultaneously and in situ. In the present paper, several novel systems for electron transfer are outlined, and the following topics are discussed based on results obtained by the current scan polarography at the solution dropping electrode developed as a technique for VCT: the relation between the half-wave potential in VCT for ion transfer and the characteristics of the ion transferred; the relation between the half-wave potential in VCT for electron transfer and the electrochemical nature of a redox couple added in water and that added in organic solution; and the ion transfer through a liquid membrane promoted by electron transfer. Observations are presented and discussion is made on the characteristics of ion transfer polarograms, those of electron transfer polarograms, and ion transfer promoted by electron transfer at a liquid/membrane interface. (N.K.)

Design Review Closure Report for the SY-101 Rapid Transfer System

International Nuclear Information System (INIS)

POWELL, W.J.

1999-01-01

The purpose of this report, is to document closure of design review open items, resulting from design reviews conducted for the SY-101 Respond And Pump In Days (RAPID) Transfer System. Results of the various design reviews were documented in the Design Review Report for The SY-101 Rapid Mitigation System, HNF-4519. In that report, twenty-three open items were identified. In this report the 23 items are reviewed and statused

Design Review Closure Report for the SY-101 Rapid Transfer System

Energy Technology Data Exchange (ETDEWEB)

POWELL, W.J.

1999-11-29

The purpose of this report, is to document closure of design review open items, resulting from design reviews conducted for the SY-101 Respond And Pump In Days (RAPID) Transfer System. Results of the various design reviews were documented in the Design Review Report for The SY-101 Rapid Mitigation System, HNF-4519. In that report, twenty-three open items were identified. In this report the 23 items are reviewed and statused.

Charge-transfer spectra of tetravalent lanthanide ions in oxides

NARCIS (Netherlands)

Hoefdraad, H.E.

The charge-transfer spectra of Ce4+, Pr4+ and Tb4+ in a number of oxides are reported. It is noted that the position of the first charge-transfer band is fixed for the metal ion in an oxygen coordination of VI, but varies in VIII coordination as a function of the host lattice. It is argued that this

Enabling fast charging – A battery technology gap assessment

Energy Technology Data Exchange (ETDEWEB)

Ahmed, Shabbir; Bloom, Ira; Jansen, Andrew N.; Tanim, Tanvir; Dufek, Eric J.; Pesaran, Ahmad; Burnham, Andrew; Carlson, Richard B.; Dias, Fernando; Hardy, Keith; Keyser, Matthew; Kreuzer, Cory; Markel, Anthony; Meintz, Andrew; Michelbacher, Christopher; Mohanpurkar, Manish; Nelson, Paul A.; Robertson, David C.; Scoffield, Don; Shirk, Matthew; Stephens, Thomas; Vijayagopal, Ram; Zhang, Jiucai

2017-11-01

The battery technology literature is reviewed, with an emphasis on key elements that limit extreme fast charging. Key gaps in existing elements of the technology are presented as well as developmental needs. Among these needs are advanced models and methods to detect and prevent lithium plating; new positive-electrode materials which are less prone to stress-induced failure; better electrode designs to accommodate very rapid diffusion in and out of the electrode; measure temperature distributions during fast charge to enable / validate models; and develop thermal management and pack designs to accommodate the higher operating voltage.

Validation of heat transfer models for gap cooling

International Nuclear Information System (INIS)

Okano, Yukimitsu; Nagae, Takashi; Murase, Michio

2004-01-01

For severe accident assessment of a light water reactor, models of heat transfer in a narrow annular gap between overheated core debris and a reactor pressure vessel are important for evaluating vessel integrity and accident management. The authors developed and improved the models of heat transfer. However, validation was not sufficient for applicability of the gap heat flux correlation to the debris cooling in the vessel lower head and applicability of the local boiling heat flux correlations to the high-pressure conditions. Therefore, in this paper, we evaluated the validity of the heat transfer models and correlations by analyses for ALPHA and LAVA experiments where molten aluminum oxide (Al 2 O 3 ) at about 2700 K was poured into the high pressure water pool in a small-scale simulated vessel lower head. In the heating process of the vessel wall, the calculated heating rate and peak temperature agreed well with the measured values, and the validity of the heat transfer models and gap heat flux correlation was confirmed. In the cooling process of the vessel wall, the calculated cooling rate was compared with the measured value, and the validity of the nucleate boiling heat flux correlation was confirmed. The peak temperatures of the vessel wall in ALPHA and LAVA experiments were lower than the temperature at the minimum heat flux point between film boiling and transition boiling, so the minimum heat flux correlation could not be validated. (author)

Twisted intra-molecular charge transfer investigations of semiorganic triglycine phosphate single crystal for non linear optical applications

Science.gov (United States)

Meera, M. R.; Joselin Beaula, T.; Rayar, S. L.; Bena Jothy, V.

2017-09-01

NLO materials are gaining importance in technologies such as optical communication, optical computing and dynamic image processing. Many NLO crystals grown by mixing amino acids with various organic and inorganic acids have been reported in the literature. Hence, glycine mixed semi-organic material will be of special interest as a fundamental building block to develop many complex crystals with improved NLO properties. A semi organic Single crystal of Triglycine Phosphate (TGP) which was grown and spectral analysis have been using FTIR and Raman spectral analysis. Natural Bond Orbital Analysis and the atomic natural charges are also predicted. HOMO LUMO energy gap value suggests the possibility of charge transfer within the molecule.

Spectral Gap Energy Transfer in Atmospheric Boundary Layer

Science.gov (United States)

Bhushan, S.; Walters, K.; Barros, A. P.; Nogueira, M.

2012-12-01

Experimental measurements of atmospheric turbulence energy spectra show E(k) ~ k-3 slopes at synoptic scales (~ 600 km - 2000 km) and k-5/3 slopes at the mesoscales (theory, it is expected that a strong backward energy cascade would develop at the synoptic scale, and that circulation would grow infinitely. To limit this backward transfer, energy arrest at macroscales must be introduced. The most commonly used turbulence models developed to mimic the above energy transfer include the energy backscatter model for 2D turbulence in the horizontal plane via Large Eddy Simulation (LES) models, dissipative URANS models in the vertical plane, and Ekman friction for the energy arrest. One of the controversial issues surrounding the atmospheric turbulence spectra is the explanation of the generation of the 2D and 3D spectra and transition between them, for energy injection at the synoptic scales. Lilly (1989) proposed that the existence of 2D and 3D spectra can only be explained by the presence of an additional energy injection in the meso-scale region. A second issue is related to the observations of dual peak spectra with small variance in meso-scale, suggesting that the energy transfer occurs across a spectral gap (Van Der Hoven, 1957). Several studies have confirmed the spectral gap for the meso-scale circulations, and have suggested that they are enhanced by smaller scale vertical convection rather than by the synoptic scales. Further, the widely accepted energy arrest mechanism by boundary layer friction is closely related to the spectral gap transfer. This study proposes an energy transfer mechanism for atmospheric turbulence with synoptic scale injection, wherein the generation of 2D and 3D spectra is explained using spectral gap energy transfer. The existence of the spectral gap energy transfer is validated by performing LES for the interaction of large scale circulation with a wall, and studying the evolution of the energy spectra both near to and far from the wall

Charge transfer induced activity of graphene for oxygen reduction

International Nuclear Information System (INIS)

Shen, Anli; Xia, Weijun; Dou, Shuo; Wang, Shuangyin; Zhang, Lipeng; Xia, Zhenhai

2016-01-01

Tetracyanoethylene (TCNE), with its strong electron-accepting ability, was used to dope graphene as a metal-free electrocatalyst for the oxygen reduction reaction (ORR). The charge transfer process was observed from graphene to TCNE by x-ray photoelectron spectroscopy and Raman characterizations. Our density functional theory calculations found that the charge transfer behavior led to an enhancement of the electrocatalytic activity for the ORR. (paper)

Charge transfer from and to manganese phthalocyanine: bulk materials and interfaces

Directory of Open Access Journals (Sweden)

Florian Rückerl

2017-08-01

Full Text Available Manganese phthalocyanine (MnPc is a member of the family of transition-metal phthalocyanines, which combines interesting electronic behavior in the fields of organic and molecular electronics with local magnetic moments. MnPc is characterized by hybrid states between the Mn 3d orbitals and the π orbitals of the ligand very close to the Fermi level. This causes particular physical properties, different from those of the other phthalocyanines, such as a rather small ionization potential, a small band gap and a large electron affinity. These can be exploited to prepare particular compounds and interfaces with appropriate partners, which are characterized by a charge transfer from or to MnPc. We summarize recent spectroscopic and theoretical results that have been achieved in this regard.

Does charge transfer correlate with ignition probability?

International Nuclear Information System (INIS)

Holdstock, Paul

2008-01-01

Flammable or explosive atmospheres exist in many industrial environments. The risk of ignition caused by electrostatic discharges is very real and there has been extensive study of the incendiary nature of sparks and brush discharges. It is clear that in order to ignite a gas, an amount of energy needs to be delivered to a certain volume of gas within a comparatively short time. It is difficult to measure the energy released in an electrostatic discharge directly, but it is possible to approximate the energy in a spark generated from a well defined electrical circuit. The spark energy required to ignite a gas, vapour or dust cloud can be determined by passing such sparks through them. There is a relationship between energy and charge in a capacitive circuit and so it is possible to predict whether or not a spark discharge will cause an ignition by measuring the charge transferred in the spark. Brush discharges are in many ways less well defined than sparks. Nevertheless, some work has been done that has established a relationship between charge transferred in brush discharges and the probability of igniting a flammable atmosphere. The question posed by this paper concerns whether such a relationship holds true in all circumstances and if there is a universal correlation between charge transfer and ignition probability. Data is presented on discharges from textile materials that go some way to answering this question.

Enhancing SERS by Means of Supramolecular Charge Transfer

Science.gov (United States)

Wong, Eric; Flood, Amar; Morales, Alfredo

2009-01-01

In a proposed method of sensing small quantities of molecules of interest, surface enhanced Raman scattering (SERS) spectroscopy would be further enhanced by means of intermolecular or supramolecular charge transfer. There is a very large potential market for sensors based on this method for rapid detection of chemical and biological hazards. In SERS, the Raman signals (vibrational spectra) of target molecules become enhanced by factors of the order of 108 when those molecules are in the vicinities of nanostructured substrate surfaces that have been engineered to have plasmon resonances that enhance local electric fields. SERS, as reported in several prior NASA Tech Briefs articles and elsewhere, has remained a research tool and has not yet been developed into a practical technique for sensing of target molecules: this is because the short range (5 to 20 nm) of the field enhancement necessitates engineering of receptor molecules to attract target molecules to the nanostructured substrate surfaces and to enable reliable identification of the target molecules in the presence of interferants. Intermolecular charge-transfer complexes have been used in fluorescence-, photoluminescence-, and electrochemistry-based techniques for sensing target molecules, but, until now, have not been considered for use in SERS-based sensing. The basic idea of the proposed method is to engineer receptor molecules that would be attached to nanostructured SERS substrates and that would interact with the target molecules to form receptor-target supramolecular charge-transfer complexes wherein the charge transfer could be photoexcited.

Integer Charge Transfer and Hybridization at an Organic Semiconductor/Conductive Oxide Interface

KAUST Repository

Gruenewald, Marco; Schirra, Laura K.; Winget, Paul; Kozlik, Michael; Ndione, Paul F.; Sigdel, Ajaya K.; Berry, Joseph J.; Forker, Roman; Bredas, Jean-Luc; Fritz, Torsten; Monti, Oliver L. A.

2015-01-01

with localized states (the shallow donors) in the substrate and charge back-donation, resulting in an effectively integer charge transfer across the interface. Charge transfer is thus not merely a question of locating the Fermi level above the PTCDA electron

Charge transfer devices and their application in physics

Energy Technology Data Exchange (ETDEWEB)

Soroko, L M [Joint Inst. for Nuclear Research, Dubna (USSR)

1979-01-01

Physical properties and technical specifications of charge transfer devices (CTD) are reviewed. The CTD are semiconductor devices based on silicon single crystals. The limiting charge density of the CTD, their efficiency of charge transfer, the background noise and radiation effects are considered. Fast response and low energy consumption are characteristic features of the devices. The application of the CTD in storage devices, real time spectral data processing systems and in streamer chambers is described. The algorithms of topological transformations in the stage of scanning particle track images, which can be realized with the help of the CTD are shortly considered. It is pointed out that applications of the CTD in different fields of science and technology are numerous and expanding.

Static In-wheel Wireless Charging Systems for Electric Vehicles

Directory of Open Access Journals (Sweden)

Chirag Panchal

2017-09-01

Full Text Available Wireless charging is a popular upcoming technology with uses ranging from mobile phone charging through to electric vehicle EV charging. Large air gaps found in current EV wireless charging systems WCS pose a hurdle of its success. Air gaps in WCS cause issues in regards to efficiency power transfer and electromagnetic compatibility EMC leakage issues. A static In-Wheel WCS IW-WCS is presented which significantly reduces the issues associated with large air gaps. A small scale laboratory prototype utilizing a standard 10mm steel reinforced tyre has been created and compared to a typical 30mm air gap. The IW-WCS has been investigated by experimental and finite element method FEM based electro-magnetic field simulation methods to validate performance.

Proton transfer to charged platinum electrodes. A molecular dynamics trajectory study.

Science.gov (United States)

Wilhelm, Florian; Schmickler, Wolfgang; Spohr, Eckhard

2010-05-05

A recently developed empirical valence bond (EVB) model for proton transfer on Pt(111) electrodes (Wilhelm et al 2008 J. Phys. Chem. C 112 10814) has been applied in molecular dynamics (MD) simulations of a water film in contact with a charged Pt surface. A total of seven negative surface charge densities σ between -7.5 and -18.9 µC cm(-2) were investigated. For each value of σ, between 30 and 84 initial conditions of a solvated proton within a water slab were sampled, and the trajectories were integrated until discharge of a proton occurred on the charged surfaces. We have calculated the mean rates for discharge and for adsorption of solvated protons within the adsorbed water layer in contact with the metal electrode as a function of surface charge density. For the less negative values of σ we observe a Tafel-like exponential increase of discharge rate with decreasing σ. At the more negative values this exponential increase levels off and the discharge process is apparently transport limited. Mechanistically, the Tafel regime corresponds to a stepwise proton transfer: first, a proton is transferred from the bulk into the contact water layer, which is followed by transfer of a proton to the charged surface and concomitant discharge. At the more negative surface charge densities the proton transfer into the contact water layer and the transfer of another proton to the surface and its discharge occur almost simultaneously.

A study on gap heat transfer of LWR fuel rods under reactivity initiated accident conditions

International Nuclear Information System (INIS)

Fujishiro, Toshio

1984-03-01

Gap heat transfer between fuel pellet and cladding have a large influence on the LWR fuel behaviors under reactivity initiated accident (RIA) conditions. The objective of the present study is to investigate the effects of gap heat transfer on RIA fuel behaviors based on the results of the gap-gas parameter tests in NSRR and on their analysis with NSR-77 code. Through this study, transient variations of gap heat transfer, the effects of the gap heat transfer on fuel thermal behaviors and on fuel failure, effects of pellet-cladding sticking by eutectic formation, and the effects of cladding collapse under high external pressure have been clearified. The studies have also been performed on the applicability and its limit of modified Ross and Stoute equation which is extensively utilized to evaluate the gap heat transfer coefficient in the present fuel behavior codes. The method to evaluate the gap conductance to the conditions beyond the applicability limit of the Ross and Stoute equation has also been proposed. (author)

Phonons and charge-transfer excitations in HTS superconductors

International Nuclear Information System (INIS)

Bishop, A.R.

1989-01-01

Some of the experimental and theoretical evidence implicating phonons and charge-transfer excitations in HTS superconductors is reviewed. It is suggested that superconductivity may be driven by a synergistic interplay of (anharmonic) phonons and electronic degrees of freedom (e.g., charge fluctuations, excitons). 47 refs., 5 figs

Formation of a ground-state charge-transfer complex in Polyfluorene//[6,6]-Phenyl-C61 butyric acid methyl ester (PCBM) blend films and its role in the function of polymer/PCBM solar cells

Energy Technology Data Exchange (ETDEWEB)

Benson-Smith, J.J.; Bradley, D.D.C.; Nelson, J. [Department of Physics, Imperial College London, London SW7 2BW (United Kingdom); Goris, L.; Vandewal, K.; Haenen, K.; Manca, J.V.; Vanderzande, D. [Institute for Materials Research, Limburgs Universitair Centrum, Wetenschapspark 1, 3590 Diepenbeek (Belgium)

2007-02-12

Evidence is presented for the formation of a weak ground-state charge-transfer complex in the blend films of poly[9,9-dioctylfluorene-co-N-(4-methoxyphenyl)diphenylamine] polymer (TFMO) and [6,6]-phenyl-C{sub 61} butyric acid methyl ester (PCBM), using photothermal deflection spectroscopy (PDS) and photoluminescence (PL) spectroscopy. Comparison of this polymer blend with other polyfluorene polymer/PCBM blends shows that the appearance of this ground-state charge-transfer complex is correlated to the ionization potential of the polymer, but not to the optical gap of the polymer or the surface morphology of the blend film. Moreover, the polymer/PCBM blend films in which this charge-transfer complex is observed also exhibit efficient photocurrent generation in photovoltaic devices, suggesting that the charge-transfer complex may be involved in charge separation. Possible mechanisms for this charge-transfer state formation are discussed as well as the significance of this finding to the understanding and optimization of polymer blend solar cells. (Abstract Copyright [2007], Wiley Periodicals, Inc.)

Mass-transfer studies in an electrochemical reactor with a small interelectrode gap

International Nuclear Information System (INIS)

Colli, A.N.; Toelzer, R.; Bergmann, M.E.H.; Bisang, J.M.

2013-01-01

Highlights: • Turbulence promoters increase from two to eight times the mass-transfer coefficients. • Turbulence promoters become more uniform the mass-transfer distribution. • Expanded plastics with an open structure are appropriate as turbulence promoters. -- Abstract: This paper reports the distribution of the local mass-transfer coefficient along the electrode length for an electrochemical reactor with parallel-plate electrodes and narrow interelectrode gaps of 1 and 2.2 mm, using the reduction of ferricyanide as a test reaction. The studies were performed at different flow rates, Reynolds numbers ranging from 370 to 3700, with the empty reactor and also the interelectrode gap was filled with two types of expanded plastics and a woven plastic mesh as turbulence promoters. The effect of both the interelectrode gap and the partial placing of the turbulence promoter along the electrode length on the mass-transfer behaviour was also analyzed. In all cases the pressure drop across the reactor was measured. A more uniform distribution of the local mass-transfer coefficient, ±15% related to its mean value, and an important increase of the mean mass-transfer coefficient, enhancement factor ranging from 2 to 8, were observed, depending on the type of turbulence promoter, the volumetric flow rate, and the interelectrode gap

Photoinduced partial charge transfer between conjugated polymer and fullerene in solutions

International Nuclear Information System (INIS)

Lin Hongzhen; Weng Yufeng; Huang Hongmin; He Qingguo; Zheng Min; Bai Fenglian

2004-01-01

Photoinduced charge transfer between a conjugated polymer and C 60 and the related processes were investigated in dilute solutions. The substantial fluorescence quenching is correlated with the efficient exciton diffusion within the polymer chains, according to which a sphere-of-action mechanism is proposed. An emissive exciplex was found formed between the conjugated polymer and fullerene in a nonpolar solvent, indicating the occurrence of a photoinduced partial charge transfer process. The low-energy sites in the polymer are believed to play a crucial role in the partial charge transfer. The asymmetry of the exciplex provides a method for evaluating the tendency of photoinduced charge separation between the donor and the acceptor. This method allows screening candidates for photovoltaic applications

Photoinduced electron transfer in covalent ruthenium-anthraquinone dyads: relative importance of driving-force, solvent polarity, and donor-bridge energy gap.

Science.gov (United States)

Hankache, Jihane; Wenger, Oliver S

2012-02-28

Four rigid rod-like molecules comprised of a Ru(bpy)(3)(2+) (bpy = 2,2'-bipyridine) photosensitizer, a 9,10-anthraquinone electron acceptor, and a molecular bridge connecting the two redox partners were synthesized and investigated by optical spectroscopic and electrochemical means. An attempt was made to assess the relative importance of driving-force, solvent polarity, and bridge variation on the rates of photoinduced electron transfer in these molecules. Expectedly, introduction of tert-butyl substituents in the bipyridine ligands of the ruthenium complex and a change in solvent from dichloromethane to acetonitrile lead to a significant acceleration of charge transfer rates. In dichloromethane, photoinduced electron transfer is not competitive with the inherent excited-state deactivation processes of the photosensitizer. In acetonitrile, an increase in driving-force by 0.2 eV through attachment of tert-butyl substituents to the bpy ancillary ligands causes an increase in electron transfer rates by an order of magnitude. Replacement of a p-xylene bridge by a p-dimethoxybenzene spacer entails an acceleration of charge transfer rates by a factor of 3.5. In the dyads from this study, the relative order of importance of individual influences on electron transfer rates is therefore as follows: solvent polarity ≥ driving-force > donor-bridge energy gap.

Complexes with charge transfer and ion-radical salts in catalysis

Energy Technology Data Exchange (ETDEWEB)

Krylov, O V [AN SSSR, Moscow. Inst. Khimicheskoj Fiziki

1978-01-01

Considered are the data experimentally proving formation of complexes with charge transfer as intermediate complexes in homogeneous and heterogeneous catalysis. Catalytic activity correlations with charge transfer energy (and in heterogeneous catalysis with width of semiconductor forbidden band can be useful while selection of catalysts (MoO/sub 3//MgO; V/sub 2/O/sub 5//MgO; MoO/sub 3//Al/sub 2/O/sub 3/; V/sub 2/O/sub 5//Al/sub 2/O/sub 3/). A review of papers on catalytic activity of the previously prepared complexes with charge transfer and ion-radical salts is given. The use of alkali metal complexes with aromatic compounds showed their high activity in hydrogenation reactions and proved principle possibility of activation of hydrogen and hydrocarbons by the systems which do not contain transfer metals.

Characterisation of a CMOS charge transfer device for TDI imaging

International Nuclear Information System (INIS)

Rushton, J.; Holland, A.; Stefanov, K.; Mayer, F.

2015-01-01

The performance of a prototype true charge transfer imaging sensor in CMOS is investigated. The finished device is destined for use in TDI applications, especially Earth-observation, and to this end radiation tolerance must be investigated. Before this, complete characterisation is required. This work starts by looking at charge transfer inefficiency and then investigates responsivity using mean-variance techniques

Space-charge limitation of avalanche growth in narrow-gap resistive plate chambers

CERN Document Server

Williams, M C S

2004-01-01

A big advance in resistive plate chamber technology happened in 1996 with the advent of the multigap resistive plate chamber (MRPC). The MRPC allows us to easily construct detectors with many small gas gaps and thus we obtain good timing together with high detection efficiency. Using this technology, it is now common to build detectors with gas gaps of 200-300 mum in width. This paper examines space-charge limited avalanche growth; this becomes a dominant effect for narrow gap resistive plate chambers. This effect controls gas gain and explains the reason for the excellent behaviour of MRPCs built with this gas gap.

A new technique for the study of charge transfer in multiply charged ion-ion collisions

International Nuclear Information System (INIS)

Shinpaugh, J.L.; Meyer, F.W.; Datz, S.

1994-01-01

While large cross sections (>10 -16 cm 2 ) have been predicted for resonant charge transfer in ion-ion collisions, no experimental data exist for multiply charged systems. A novel technique is being developed at the ORNL ECR facility to allow study of symmetric charge exchange in multiply charged ion-ion collisions using a single ion source. Specific intra-beam charge transfer collisions occurring in a well-defined interaction region labeled by negative high voltage are identified and analyzed by electrostatic analysis in combination with ion time-of-flight coincidence detection of the collision products. Center-of-mass collision energies from 400 to 1000 eV are obtained by varying source and labeling-cell voltages. In addition, by the introduction of a target gas into the high-voltage cell, this labeling-voltage method allows measurement of electron-capture and -loss cross sections for ion-atom collisions. Consequently, higher collision energies can be investigated without the requirement of placing the ECR source on a high-voltage platform

Theoretical treatment of charge transfer processes of relevance to astrophysics

Energy Technology Data Exchange (ETDEWEB)

Krstic, P.S.; Stancil, P.C.; Schultz, D.R.

1997-12-01

Charge transfer is an important process in many astrophysical and atmospheric environments. While numerous experimental and theoretical studies exist for H and He targets, data on other targets, particularly metals and molecules, are sparse. Using a variety of theoretical methods and computational techniques the authors are developing methods to estimate the cross sections for electron capture (charge transfer) in slow collisions of low charge state ions with heavy (Mg, Ca, Fe, Co, Ni and Zn) neutrals. In this ongoing work particular attention is paid to ascertaining the importance of double electron capture.

Theoretical treatment of charge transfer processes of relevance to astrophysics

International Nuclear Information System (INIS)

Krstic, P.S.; Stancil, P.C.; Schultz, D.R.

1997-12-01

Charge transfer is an important process in many astrophysical and atmospheric environments. While numerous experimental and theoretical studies exist for H and He targets, data on other targets, particularly metals and molecules, are sparse. Using a variety of theoretical methods and computational techniques the authors are developing methods to estimate the cross sections for electron capture (charge transfer) in slow collisions of low charge state ions with heavy (Mg, Ca, Fe, Co, Ni and Zn) neutrals. In this ongoing work particular attention is paid to ascertaining the importance of double electron capture

Charge-transfer collisions for polarized ion sources

International Nuclear Information System (INIS)

Schlachter, A.S.

1983-06-01

Charge-transfer processes relevant to polarized ion sources are discussed and results are summarized. The primary atom discussed is hydrogen, with particulr emphasis on H - formation. Heavier negative ions are briefly discussed

Molecular orbital (SCF-Xα-SW) theory of metal-metal charge transfer processes in minerals - II. Application to Fe2+ --> Ti4+ charge transfer transitions in oxides and silicates

Science.gov (United States)

Sherman, David M.

1987-01-01

A molecular orbital description, based on Xα-Scattered wave calculations on a (FeTiO10)14− cluster, is given for Fe2+ → Ti4+ charge transfer transitions in minerals. The calculated energy for the lowest Fe2+ → Ti4+ metal-metal charge transfer transition is 18040 cm−1 in reasonable agreement with energies observed in the optical spectra of Fe-Ti oxides and silicates. As in the case of Fe2+ → Fe3+ charge transfer in mixed-valence iron oxides and silicates, Fe2+ → Ti4+ charge transfer is associated with Fe-Ti bonding across shared polyhedral edges. Such bonding results from the overlap of the Fe(t 2g ) and Ti(t 2g ) 3d orbitals.

Low-Energy Charge Transfer in Multiply-Charged Ion-Atom Collisions Studied with the Combined SCVB-MOCC Approach

Directory of Open Access Journals (Sweden)

B. Zygelman

2002-03-01

Full Text Available A survey of theoretical studies of charge transfer involving collisions of multiply-charged ions with atomic neutrals (H and He is presented. The calculations utilized the quantum-mechanical molecular-orbital close-coupling (MOCC approach where the requisite potential curves and coupling matrix elements have been obtained with the spin-coupled valence bond (SCVB method. Comparison is made among various collision partners, for equicharged systems, where it is illustrated that even for total charge transfer cross sections, scaling-laws do not exist for low-energy collisions (i.e. < 1 keV/amu. While various empirical scaling-laws are well known in the intermediateand high-energy regimes, the multi-electron configurations of the projectile ions results in a rich and varied low-energy dependence, requiring an explicit calculation for each collision-partner pair. Future charge transfer problems to be addressed with the combined SCVB-MOCC approach are briefly discussed.

Charge transfer and ionization occurring in proton- and helium ion-atom collisions

International Nuclear Information System (INIS)

DuBois, R.D.

1985-12-01

Two examples are presented where specific channels have been identified that are responsible for single and double target ionization via direct coulomb ionization or charge transfer processes. Using ratios of absolute cross sections that have been measured for these processes it was shown that an independent electron model should be appropriate for calculating direct double target ionization but generally appears to be inadequate in calculating charge transfer plus ionization and double charge transfer cross sections. At present such detailed information can be obtained only in limited cases. However cross sections with detailed final charge state information should provide stringent tests for present and future theoretical work. 22 refs., 2 figs

Computational Approach to Electron Charge Transfer Reactions

DEFF Research Database (Denmark)

Jónsson, Elvar Örn

-molecular mechanics scheme, and tools to analyse statistical data and generate relative free energies and free energy surfaces. The methodology is applied to several charge transfer species and reactions in chemical environments - chemical in the sense that solvent, counter ions and substrate surfaces are taken...... in to account - which directly influence the reactants and resulting reaction through both physical and chemical interactions. All methods are though general and can be applied to different types of chemistry. First, the basis of the various theoretical tools is presented and applied to several test systems...... and asymmetric charge transfer reactions between several first-row transition metals in water. The results are compared to experiments and rationalised with classical analytic expressions. Shortcomings of the methods are accounted for with clear steps towards improved accuracy. Later the analysis is extended...

Charge transfer properties of pentacene adsorbed on silver: DFT study

Energy Technology Data Exchange (ETDEWEB)

N, Rekha T.; Rajkumar, Beulah J. M., E-mail: beulah-rajkumar@yahoo.co.in [PG & Research Department of Physics, Lady Doak College, Madurai 625002 (India)

2015-06-24

Charge transfer properties of pentacene adsorbed on silver is investigated using DFT methods. Optimized geometry of pentacene after adsorption on silver indicates distortion in hexagonal structure of the ring close to the silver cluster and deviations in co-planarity of carbon atoms due to the variations in bond angles and dihedral angles. Theoretically simulated absorption spectrum has a symmetric surface plasmon resonance peak around 486nm corresponding to the transfer of charge from HOMO-2 to LUMO. Theoretical SERS confirms the process of adsorption, tilted orientation of pentacene on silver surface and the charge transfers reported. Localization of electron density arising from redistribution of electrostatic potential together with a reduced bandgap of pentacene after adsorption on silver suggests its utility in the design of electro active organic semiconducting devices.

Development of heat transfer models for gap cooling

Energy Technology Data Exchange (ETDEWEB)

Kohriyama, Tamio; Murase, Michio; Tamaki, Tomohiko [Institute of Nuclear Safety System Inc., Mihama, Fukui (Japan)

2001-09-01

In a severe accident of a light water reactor (LWR), heat transfer models in a narrow annular gap between superheated core debris and a reactor pressure vessel (RPV) are important to evaluate the integrity of RPV and emergency procedures. This paper discusses the effects of superheat on the heat flux based on existing data. In low superheat conditions, the heat flux in the narrow gap is higher than the heat flux in pool nucleate boiling due to restricted flow area. It approaches the nucleate boiling heat flux as superheat increasing and reaches a critical value subject to the counter-current flow limiting (CCFL) at the top end of the gap. A heat transfer correlation was derived as a function of dimensionless superheat and a Kutateladze-type CCFL correlation was deduced for critical heat flux (CHF) restricted by CCFL, which gave good prediction for a wide range of the CHF data. Effect of an angle of inclination of the gap could also be incorporated in the CCFL correlation. In high superheat conditions, the heat flux in the narrow gap maintains a similar shape to the pool boiling curve but shifts the position to a higher superheated side than the pool boiling except film boiling, which could be expressed by the typical pool film boiling correlation. Incorporating quench test data, the heat flux correlation was derived as a function of dimensionless superheat using the same formula for the low superheat and the Kutateladze-type CCFL correlation was deduced for CHF. The CHF at the high superheat was 3-4 times as large as CHF at the low superheat and this difference was well predicted by different flow patterns in the gap and the balance of pressure gradients between gas and liquid phases. (author)

Dynamical interaction of He atoms with metal surfaces: Charge transfer processes

International Nuclear Information System (INIS)

Flores, F.; Garcia Vidal, F.J.; Monreal, R.

1993-01-01

A self-consistent Kohn-Sham LCAO method is presented to calculate the charge transfer processes between a He * -atom and metal surfaces. Intra-atomic correlation effects are taken into account by considering independently each single He-orbital and by combining the different charge transfer processes into a set of dynamical rate equations for the different ion charge fractions. Our discussion reproduces qualitatively the experimental evidence and gives strong support to the method presented here. (author). 24 refs, 4 figs

Non-Markovian reduced dynamics of ultrafast charge transfer at an oligothiophene–fullerene heterojunction

Energy Technology Data Exchange (ETDEWEB)

Hughes, Keith H., E-mail: keith.hughes@bangor.ac.uk [School of Chemistry, Bangor University, Bangor, Gwynedd LL57 2UW (United Kingdom); Cahier, Benjamin [School of Chemistry, Bangor University, Bangor, Gwynedd LL57 2UW (United Kingdom); Martinazzo, Rocco [Dipartimento di Chimica Università degli Studi di Milano, v. Golgi 19, 20133 Milano (Italy); Tamura, Hiroyuki [WPI-Advanced Institute for Material Research, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577 (Japan); Burghardt, Irene [Institute of Physical and Theoretical Chemistry, Goethe University Frankfurt, Max-von-Laue-Str. 7, 60438 Frankfurt/Main (Germany)

2014-10-17

Highlights: • Quantum dynamical study of exciton dissociation at a heterojunction interface. • The non-Markovian quantum dynamics involves a highly structured spectral density. • Spectral density is reconstructed from an effective mode transformation of the Hamiltonian. • The dynamics is studied using the hierarchical equations of motion approach. • It was found that the temperature has little effect on the charge transfer. - Abstract: We extend our recent quantum dynamical study of the exciton dissociation and charge transfer at an oligothiophene–fullerene heterojunction interface (Tamura et al., 2012) [6] by investigating the process using the non-perturbative hierarchical equations of motion (HEOM) approach. Based upon an effective mode reconstruction of the spectral density the effect of temperature on the charge transfer is studied using reduced density matrices. It was found that the temperature had little effect on the charge transfer and a coherent dynamics persists over the first few tens of femtoseconds, indicating that the primary charge transfer step proceeds by an activationless pathway.

Crystal growth of new charge-transfer salts based on π-conjugated donor molecules

Energy Technology Data Exchange (ETDEWEB)

Morherr, Antonia, E-mail: morherr@stud.uni-frankfurt.de [Physikalisches Institut, Goethe-Universität Frankfurt am Main, 60438 Frankfurt am Main (Germany); Witt, Sebastian [Physikalisches Institut, Goethe-Universität Frankfurt am Main, 60438 Frankfurt am Main (Germany); Chernenkaya, Alisa [Graduate School Materials Science in Mainz, 55128 Mainz (Germany); Institut für Physik, Johannes Gutenberg-Universität, 55099 Mainz (Germany); Bäcker, Jan-Peter [Physikalisches Institut, Goethe-Universität Frankfurt am Main, 60438 Frankfurt am Main (Germany); Schönhense, Gerd [Institut für Physik, Johannes Gutenberg-Universität, 55099 Mainz (Germany); Bolte, Michael [Institut für anorganische Chemie, Goethe-Universität Frankfurt am Main, 60438 Frankfurt am Main (Germany); Krellner, Cornelius [Physikalisches Institut, Goethe-Universität Frankfurt am Main, 60438 Frankfurt am Main (Germany)

2016-09-01

New charge transfer crystals of π-conjugated, aromatic molecules (phenanthrene and picene) as donors were obtained by physical vapor transport. The melting behavior, optimization of crystal growth and the crystal structure are reported for charge transfer salts with (fluorinated) tetracyanoquinodimethane (TCNQ-F{sub x}, x=0, 2, 4), which was used as acceptor material. The crystal structures were determined by single-crystal X-ray diffraction. Growth conditions for different vapor pressures in closed ampules were applied and the effect of these starting conditions for crystal size and quality is reported. The process of charge transfer was investigated by geometrical analysis of the crystal structure and by infrared spectroscopy on single crystals. With these three different acceptor strengths and the two sets of donor materials, it is possible to investigate the distribution of the charge transfer systematically. This helps to understand the charge transfer process in this class of materials with π-conjugated donor molecules.

Experimental evidence of state-selective charge transfer in inductively coupled plasma-atomic emission spectrometry

International Nuclear Information System (INIS)

Chan, George C.-Y.; Hieftje, Gary M.

2004-01-01

State-selective charge-transfer behavior was observed for Fe, Cr, Mn and Cu in inductively coupled plasma (ICP)-atomic emission spectrometry. Charge transfer from Ar + to Fe, Cr and Mn is state-selective because of inefficient collisional mixing of the quasiresonant charge-transfer energy levels with nearby levels. This low efficiency is the consequence of differences in electronic configuration of the core electrons. The reason for state-selective charge-transfer behavior to Cu is not clear, although a tentative explanation based on efficiency of intramultiplet and intermultiplet mixing for this special case is offered

The effect of cathode surface impurities on gap closure

International Nuclear Information System (INIS)

Hinshelwood, D.D.

1983-01-01

Gap closure due to cathode (or anode) plasma motion is often the principal limitation on the pulse length of intense beam diodes and magnetically insulated transmission lines. Since the plasma expansion velocity is typically on the order of the sound speed, a high atomic number plasma is desirable. In recent experiments performed on a Sandia Nereus accelerator (240kV, 50kA, 3-30kA/cm 2 , 70ns) with a parallel plate diode, the cathode plasma was seen to be composed of both the cathode substrate material and constituents (hydrogen and carbon) of surface contaminants such as pump oils. The plasma expansion velocities, inferred from impedance measurements, were 1.5-2 cm/μs and were the same for carbon, aluminum and stainless steel cathodes. This similarity, combined with the temperature estimates of 2-3eV obtained from spectroscopy, implied that the expansion was due to protons from surface contaminants. Similar results were reported from studies of ablatively driven plasmas. In a continuation of the work, the results of time and spatially resolved spectroscopic studies of plasma formed on aluminum cathodes, yielding measurements of the expansion velocities of different components of the cathode plasma, are presented. We have heated stainless steel cathodes in situ to 700 0 C. The Hα line emission was seen to decrease by more than an order of magnitude (becoming lost in the background) when the cathodes were heated but no change in the impedance behavior was observed. Evidently the heating was insufficient to remove the last monolayer, which should contain more than enough hydrogen to close the gap. Preliminary experiments with gold-plated cathodes (which should be more resistant to chemisorption) yielded similar results. Further measurements of plasma formed on heated cathodes are presented

Robust Stacking-Independent Ultrafast Charge Transfer in MoS2/WS2 Bilayers.

Science.gov (United States)

Ji, Ziheng; Hong, Hao; Zhang, Jin; Zhang, Qi; Huang, Wei; Cao, Ting; Qiao, Ruixi; Liu, Can; Liang, Jing; Jin, Chuanhong; Jiao, Liying; Shi, Kebin; Meng, Sheng; Liu, Kaihui

2017-12-26

Van der Waals-coupled two-dimensional (2D) heterostructures have attracted great attention recently due to their high potential in the next-generation photodetectors and solar cells. The understanding of charge-transfer process between adjacent atomic layers is the key to design optimal devices as it directly determines the fundamental response speed and photon-electron conversion efficiency. However, general belief and theoretical studies have shown that the charge transfer behavior depends sensitively on interlayer configurations, which is difficult to control accurately, bringing great uncertainties in device designing. Here we investigate the ultrafast dynamics of interlayer charge transfer in a prototype heterostructure, the MoS 2 /WS 2 bilayer with various stacking configurations, by optical two-color ultrafast pump-probe spectroscopy. Surprisingly, we found that the charge transfer is robust against varying interlayer twist angles and interlayer coupling strength, in time scale of ∼90 fs. Our observation, together with atomic-resolved transmission electron characterization and time-dependent density functional theory simulations, reveals that the robust ultrafast charge transfer is attributed to the heterogeneous interlayer stretching/sliding, which provides additional channels for efficient charge transfer previously unknown. Our results elucidate the origin of transfer rate robustness against interlayer stacking configurations in optical devices based on 2D heterostructures, facilitating their applications in ultrafast and high-efficient optoelectronic and photovoltaic devices in the near future.

Reduced Charge Transfer Exciton Recombination in Organic Semiconductor Heterojunctions by Molecular Doping

Science.gov (United States)

Deschler, Felix; da Como, Enrico; Limmer, Thomas; Tautz, Raphael; Godde, Tillmann; Bayer, Manfred; von Hauff, Elizabeth; Yilmaz, Seyfullah; Allard, Sybille; Scherf, Ullrich; Feldmann, Jochen

2011-09-01

We investigate the effect of molecular doping on the recombination of electrons and holes localized at conjugated-polymer-fullerene interfaces. We demonstrate that a low concentration of p-type dopant molecules (<4% weight) reduces the interfacial recombination via charge transfer excitons and results in a favored formation of separated carriers. This is observed by the ultrafast quenching of photoluminescence from charge transfer excitons and the increase in photoinduced polaron density by ˜70%. The results are consistent with a reduced formation of emissive charge transfer excitons, induced by state filling of tail states.

Charge transfers in complex transition metal alloys (Ti2Fe)

International Nuclear Information System (INIS)

Abramovici, G.

1998-01-01

We introduce a new non-orthogonal tight-binding model, for complex alloys, in which electronic structure is characterized by charge transfers. We give the analytic calculation of a charge transfer, in which overlapping two-center terms are rigorously taken into account. Then, we apply numerically this result to an approximant phase of a quasicrystal of Ti 2 Fe alloy. This model is more particularly adapted to transition metals, and gives realistic densities of states. (orig.)

Ab initio modeling of excitonic and charge-transfer states in organic semiconductors: the PTB1/PCBM low band gap system.

Science.gov (United States)

Borges, Itamar; Aquino, Adélia J A; Köhn, Andreas; Nieman, Reed; Hase, William L; Chen, Lin X; Lischka, Hans

2013-12-11

A detailed quantum chemical simulation of the excitonic and charge-transfer (CT) states of a bulk heterojunction model containing poly(thieno[3,4-b]thiophene benzodithiophene) (PTB1)/[6,6]-phenyl-C61-butyric acid methyl ester (PCBM) is reported. The largest molecular model contains two stacked PTB1 trimer chains interacting with C60 positioned on top of and lateral to the (PTB1)3 stack. The calculations were performed using the algebraic diagrammatic construction method to second order (ADC(2)). One main result of the calculations is that the CT states are located below the bright inter-chain excitonic state, directly accessible via internal conversion processes. The other important aspects of the calculations are the formation of discrete bands of CT states originating from the lateral C60's and the importance of inter-chain charge delocalization for the stability of the CT states. A simple model for the charge separation step is also given, revealing the energetic feasibility of the overall photovoltaic process.

Pressure and gap length dependence of gap breakdown voltage and discharge current of discharge-pumped KrF excimer laser. Hoden reiki KrF laser no zetsuen hakai den prime atsu to reiki denryu no atsuryoku, gap cho izon sei

Energy Technology Data Exchange (ETDEWEB)

Yukimura, K.; Kawakami, H. (Doshisha Univ., Tokyo (Japan)); Hitomi, K. (Kyoto Polytechnic College, Kyoto (Japan))

1991-04-20

On the gap destruction characteristics of UV-preionized discharge-pumped KrF excimer laser (charge transfer type) and the electric characteristics of the excited discharge, studies were made by changing the pressure (1.5-3 atm) and the discharge gap length (14-21 mm) of the discharge medium. (1) Gap breakdown voltage and the maximum current of the excited discharge give a similarity by a product of pressure and the gap length at the charge volatge. (2) Insulation breakdown of the gap occurs at the wave front of the applied voltage and the breakdown time gets delayed by the decreasing voltage applied. By setting the ionization index at constant value 20, the gap breakdown voltage is estimated at the error within 10%. (3) The relation between the maximum current, pressure and the gap length product changes the characteristics by the charge voltage of the primary condenser. With the result combined with the standardization of voltage/current of the excited discharge, the electric characteristics at the specific pressure and gap length can be readily known. 10 refs., 10 figs.

Symmetry-Breaking Charge Transfer in a Zinc Chlorodipyrrin Acceptor for High Open Circuit Voltage Organic Photovoltaics

KAUST Repository

Bartynski, Andrew N.

2015-04-29

© 2015 American Chemical Society. Low open-circuit voltages significantly limit the power conversion efficiency of organic photovoltaic devices. Typical strategies to enhance the open-circuit voltage involve tuning the HOMO and LUMO positions of the donor (D) and acceptor (A), respectively, to increase the interfacial energy gap or to tailor the donor or acceptor structure at the D/A interface. Here, we present an alternative approach to improve the open-circuit voltage through the use of a zinc chlorodipyrrin, ZCl [bis(dodecachloro-5-mesityldipyrrinato)zinc], as an acceptor, which undergoes symmetry-breaking charge transfer (CT) at the donor/acceptor interface. DBP/ZCl cells exhibit open-circuit voltages of 1.33 V compared to 0.88 V for analogous tetraphenyldibenzoperyflanthrene (DBP)/C60-based devices. Charge transfer state energies measured by Fourier-transform photocurrent spectroscopy and electroluminescence show that C60 forms a CT state of 1.45 ± 0.05 eV in a DBP/C60-based organic photovoltaic device, while ZCl as acceptor gives a CT state energy of 1.70 ± 0.05 eV in the corresponding device structure. In the ZCl device this results in an energetic loss between ECT and qVOC of 0.37 eV, substantially less than the 0.6 eV typically observed for organic systems and equal to the recombination losses seen in high-efficiency Si and GaAs devices. The substantial increase in open-circuit voltage and reduction in recombination losses for devices utilizing ZCl demonstrate the great promise of symmetry-breaking charge transfer in organic photovoltaic devices.

Interplay of electronic and geometry shell effects in properties of neutral and charged Sr clusters

DEFF Research Database (Denmark)

Lyalin, Andrey; Solov'yov, Ilia; Solov'yov, Andrey V.

2007-01-01

that the size evolution of structural and electronic properties of strontium clusters is governed by an interplay of the electronic and geometry shell closures. Influence of the electronic shell effects on structural rearrangements can lead to violation of the icosahedral growth motif of strontium clusters......The optimized structure and electronic properties of neutral, singly, and doubly charged strontium clusters have been investigated using ab initio theoretical methods based on density-functional theory. We have systematically calculated the optimized geometries of neutral, singly, and doubly...... charged strontium clusters consisting of up to 14 atoms, average bonding distances, electronic shell closures, binding energies per atom, the gap between the highest occupied and the lowest unoccupied molecular orbitals, and spectra of the density of electronic states (DOS). It is demonstrated...

Intra- and inter-layer charge redistribution in biased bilayer graphene

Directory of Open Access Journals (Sweden)

Rui-Ning Wang

2016-03-01

Full Text Available We investigate the spatial redistribution of the electron density in bilayer graphene in the presence of an interlayer bias within density functional theory. It is found that the interlayer charge redistribution is inhomogeneous between the upper and bottom layers and the transferred charge from the upper layer to the bottom layer linearly increases with the external voltage which further makes the gap at K point linearly increase. However, the band gap will saturate to 0.29 eV in the strong-field regime, but it displays a linear field dependence at the weak-field limit. Due to the AB-stacked way, two carbon atoms per unit cell in the same layer are different and there is also a charge transfer between them, making the widths of π valence bands reduced. In the bottom layer, the charge transfers from the direct atoms which directly face another carbon atom to the indirect atoms facing the center of the hexagon on the opposite layer, while the charge transfers from the indirect atoms to the direct atoms in the upper layer. Furthermore, there is a diploe between the upper and bottom layers which results in the reduction of the interlayer hopping interaction.

Polyoxometalate active charge-transfer material for mediated redox flow battery

Energy Technology Data Exchange (ETDEWEB)

Anderson, Travis Mark; Hudak, Nicholas; Staiger, Chad; Pratt, Harry

2017-01-17

Redox flow batteries including a half-cell electrode chamber coupled to a current collecting electrode are disclosed herein. In a general embodiment, a separator is coupled to the half-cell electrode chamber. The half-cell electrode chamber comprises a first redox-active mediator and a second redox-active mediator. The first redox-active mediator and the second redox-active mediator are circulated through the half-cell electrode chamber into an external container. The container includes an active charge-transfer material. The active charge-transfer material has a redox potential between a redox potential of the first redox-active mediator and a redox potential of the second redox-active mediator. The active charge-transfer material is a polyoxometalate or derivative thereof. The redox flow battery may be particularly useful in energy storage solutions for renewable energy sources and for providing sustained power to an electrical grid.

Charge transfer in chromium-transition metal alloys

International Nuclear Information System (INIS)

Kulakowski, K.; Maksymowicz, A.

1984-07-01

The average T-matrix approximation is applied for calculations of charge transfer of 3d-electrons in transition metal alloys. The role of concentration, long-range and short-range atomic order is investigated. The results are in reasonable agreement with experimental data. (author)

An Electronic Structure Approach to Charge Transfer and Transport in Molecular Building Blocks for Organic Optoelectronics

Science.gov (United States)

Hendrickson, Heidi Phillips

A fundamental understanding of charge separation in organic materials is necessary for the rational design of optoelectronic devices suited for renewable energy applications and requires a combination of theoretical, computational, and experimental methods. Density functional theory (DFT) and time-dependent (TD)DFT are cost effective ab-initio approaches for calculating fundamental properties of large molecular systems, however conventional DFT methods have been known to fail in accurately characterizing frontier orbital gaps and charge transfer states in molecular systems. In this dissertation, these shortcomings are addressed by implementing an optimally-tuned range-separated hybrid (OT-RSH) functional approach within DFT and TDDFT. The first part of this thesis presents the way in which RSH-DFT addresses the shortcomings in conventional DFT. Environmentally-corrected RSH-DFT frontier orbital energies are shown to correspond to thin film measurements for a set of organic semiconducting molecules. Likewise, the improved RSH-TDDFT description of charge transfer excitations is benchmarked using a model ethene dimer and silsesquioxane molecules. In the second part of this thesis, RSH-DFT is applied to chromophore-functionalized silsesquioxanes, which are currently investigated as candidates for building blocks in optoelectronic applications. RSH-DFT provides insight into the nature of absorptive and emissive states in silsesquioxanes. While absorption primarily involves transitions localized on one chromophore, charge transfer between chromophores and between chromophore and silsesquioxane cage have been identified. The RSH-DFT approach, including a protocol accounting for complex environmental effects on charge transfer energies, was tested and validated against experimental measurements. The third part of this thesis addresses quantum transport through nano-scale junctions. The ability to quantify a molecular junction via spectroscopic methods is crucial to their

ARCHITECTURE OF A CHARGE-TRANSFER STATE REGULATING LIGHT HARVESTING IN A PLANT ANTENNA PROTEIN

Energy Technology Data Exchange (ETDEWEB)

Fleming, Graham; Ahn, Tae Kyu; Avenson, Thomas J.; Ballottari, Matteo; Cheng, Yuan-Chung; Niyogi, Krishna K.; Bassi, Roberto; Fleming, Graham R.

2008-04-02

Energy-dependent quenching of excess absorbed light energy (qE) is a vital mechanism for regulating photosynthetic light harvesting in higher plants. All of the physiological characteristics of qE have been positively correlated with charge-transfer between coupled chlorophyll and zeaxanthin molecules in the light-harvesting antenna of photosystem II (PSII). In this work, we present evidence for charge-transfer quenching in all three of the individual minor antenna complexes of PSII (CP29, CP26, and CP24), and we conclude that charge-transfer quenching in CP29 involves a de-localized state of an excitonically coupled chlorophyll dimer. We propose that reversible conformational changes in CP29 can `tune? the electronic coupling between the chlorophylls in this dimer, thereby modulating the energy of the chlorophylls-zeaxanthin charge-transfer state and switching on and off the charge-transfer quenching during qE.

Proton-coupled electron transfer versus hydrogen atom transfer: generation of charge-localized diabatic states.

Science.gov (United States)

Sirjoosingh, Andrew; Hammes-Schiffer, Sharon

2011-03-24

The distinction between proton-coupled electron transfer (PCET) and hydrogen atom transfer (HAT) mechanisms is important for the characterization of many chemical and biological processes. PCET and HAT mechanisms can be differentiated in terms of electronically nonadiabatic and adiabatic proton transfer, respectively. In this paper, quantitative diagnostics to evaluate the degree of electron-proton nonadiabaticity are presented. Moreover, the connection between the degree of electron-proton nonadiabaticity and the physical characteristics distinguishing PCET from HAT, namely, the extent of electronic charge redistribution, is clarified. In addition, a rigorous diabatization scheme for transforming the adiabatic electronic states into charge-localized diabatic states for PCET reactions is presented. These diabatic states are constructed to ensure that the first-order nonadiabatic couplings with respect to the one-dimensional transferring hydrogen coordinate vanish exactly. Application of these approaches to the phenoxyl-phenol and benzyl-toluene systems characterizes the former as PCET and the latter as HAT. The diabatic states generated for the phenoxyl-phenol system possess physically meaningful, localized electronic charge distributions that are relatively invariant along the hydrogen coordinate. These diabatic electronic states can be combined with the associated proton vibrational states to generate the reactant and product electron-proton vibronic states that form the basis of nonadiabatic PCET theories. Furthermore, these vibronic states and the corresponding vibronic couplings may be used to calculate rate constants and kinetic isotope effects of PCET reactions.

Dielectric Losses and Charge Transfer in Antimony-Doped TlGaS2 Single Crystal

Science.gov (United States)

Asadov, S. M.; Mustafaeva, S. N.

2018-03-01

Effect of semimetallic antimony (0.5 mol % Sb) on the dielectric properties and ac-conductivity of TlGaS2-based single crystals grown by the Bridgman-Stockbarger method has been studied. The experimental results on the frequency dispersion of dielectric coefficients and the conductivity of TlGa0.995Sb0.005S2 single crystals allowed the revealing of the dielectric loss nature, the charge transfer mechanism, and the estimation of the parameters of the states localized in the energy gap. The antimony-doping of the TlGaS2 single crystal leads to an increase in the density of states near the Fermi level and a decrease in the average time and average distance of hopes.

Using metal complex-labeled peptides for charge transfer-based biosensing with semiconductor quantum dots

Science.gov (United States)

Medintz, Igor L.; Pons, Thomas; Trammell, Scott A.; Blanco-Canosa, Juan B.; Dawson, Philip E.; Mattoussi, Hedi

2009-02-01

Luminescent colloidal semiconductor quantum dots (QDs) have unique optical and photonic properties and are highly sensitive to charge transfer in their surrounding environment. In this study we used synthetic peptides as physical bridges between CdSe-ZnS core-shell QDs and some of the most common redox-active metal complexes to understand the charge transfer interactions between the metal complexes and QDs. We found that QD emission underwent quenching that was highly dependent on the choice of metal complex used. We also found that quenching traces the valence or number of metal complexes brought into close proximity of the nanocrystal surface. Monitoring of the QD absorption bleaching in the presence of the metal complex provided insight into the charge transfer mechanism. The data suggest that two distinct charge transfer mechanisms can take place. One directly to the QD core states for neutral capping ligands and a second to surface states for negatively charged capping ligands. A basic understanding of the proximity driven charge-transfer and quenching interactions allowed us to construct proteolytic enzyme sensing assemblies with the QD-peptide-metal complex conjugates.

Active pixel sensor with intra-pixel charge transfer

Science.gov (United States)

Fossum, Eric R. (Inventor); Mendis, Sunetra (Inventor); Kemeny, Sabrina E. (Inventor)

2004-01-01

An imaging device formed as a monolithic complementary metal oxide semiconductor integrated circuit in an industry standard complementary metal oxide semiconductor process, the integrated circuit including a focal plane array of pixel cells, each one of the cells including a photogate overlying the substrate for accumulating photo-generated charge in an underlying portion of the substrate, a readout circuit including at least an output field effect transistor formed in the substrate, and a charge coupled device section formed on the substrate adjacent the photogate having a sensing node connected to the output transistor and at least one charge coupled device stage for transferring charge from the underlying portion of the substrate to the sensing node.

Electroluminescence from charge transfer states in Donor/Acceptor solar cells

DEFF Research Database (Denmark)

Sherafatipour, Golenaz; Madsen, Morten

Charge photocurrent generation is a key process in solar energy conversion systems. Effective dissociation of the photo-generated electron-hole pairs (excitons) has a strong influence on the efficiency of the organic solar cells. Charge dissociation takes place at the donor/acceptor interface via...... which the maximum open-circuit voltage can be estimated, and further can be used in the modeling and optimization of the OPV devices. [1] C. Deibe, T. Strobe, and V. Dyakonov, “Role of the charge transfer state in organic donor-acceptor solar cells,” Adv. Mater., vol. 22, pp. 4097–4111, 2010. [2] K...... charge transfer (CT) excitons, which is Coulombically bound interfacial electron- hole pairs residing at the donor/acceptor heterojunctions. The CT state represents an intermediate state between the exciton dissociation and recombination back to the ground state. Since the recombination of photo...

Doping Phosphorene with Holes and Electrons through Molecular Charge Transfer.

Science.gov (United States)

Vishnoi, Pratap; Rajesh, S; Manjunatha, S; Bandyopadhyay, Arkamita; Barua, Manaswee; Pati, Swapan K; Rao, C N R

2017-11-03

An important aspect of phosphorene, the novel two-dimensional semiconductor, is whether holes and electrons can both be doped in this material. Some reports found that only electrons can be preferentially doped into phosphorene. There are some theoretical calculations showing charge-transfer interaction with both tetrathiafulvalene (TTF) and tetracyanoethylene (TCNE). We have carried out an investigation of chemical doping of phosphorene by a variety of electron donor and acceptor molecules, employing both experiment and theory, Raman scattering being a crucial aspect of the study. We find that both electron acceptors and donors interact with phosphorene by charge-transfer, with the acceptors having more marked effects. All the three Raman bands of phosphorene soften and exhibit band broadening on interaction with both donor and acceptor molecules. First-principles calculations establish the occurrence of charge-transfer between phosphorene with donors as well as acceptors. The absence of electron-hole asymmetry is noteworthy. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Temperature-dependent kinetics of charge transfer, hydrogen-atom transfer, and hydrogen-atom expulsion in the reaction of CO+ with CH4 and CD4.

Science.gov (United States)

Melko, Joshua J; Ard, Shaun G; Johnson, Ryan S; Shuman, Nicholas S; Guo, Hua; Viggiano, Albert A

2014-09-18

We have determined the rate constants and branching ratios for the reactions of CO(+) with CH4 and CD4 in a variable-temperature selected ion flow tube. We find that the rate constants are collisional for all temperatures measured (193-700 K for CH4 and 193-500 K for CD4). For the CH4 reaction, three product channels are identified, which include charge transfer (CH4(+) + CO), H-atom transfer (HCO(+) + CH3), and H-atom expulsion (CH3CO(+) + H). H-atom transfer is slightly preferred to charge transfer at low temperature, with the charge-transfer product increasing in contribution as the temperature is increased (H-atom expulsion is a minor product for all temperatures). Analogous products are identified for the CD4 reaction. Density functional calculations on the CO(+) + CH4 reaction were also conducted, revealing that the relative temperature dependences of the charge-transfer and H-atom transfer pathways are consistent with an initial charge transfer followed by proton transfer.

Charge-transfer properties in the gas electron multiplier

International Nuclear Information System (INIS)

Han, Sanghyo; Kim, Yongkyun; Cho, Hyosung

2004-01-01

The charge transfer properties of a gas electron multiplier (GEM) were systematically investigated over a broad range of electric field configurations. The electron collection efficiency and the charge sharing were found to depend on the external fields, as well as on the GEM voltage. The electron collection efficiency increased with the collection field up to 90%, but was essentially independent of the drift field strength. A double conical GEM has a 10% gain increase with time due to surface charging by avalanche ions whereas this effect was eliminated with the cylindrical GEM. The positive-ion feedback is also estimated. (author)

Process techniques of charge transfer time reduction for high speed CMOS image sensors

International Nuclear Information System (INIS)

Cao Zhongxiang; Li Quanliang; Han Ye; Qin Qi; Feng Peng; Liu Liyuan; Wu Nanjian

2014-01-01

This paper proposes pixel process techniques to reduce the charge transfer time in high speed CMOS image sensors. These techniques increase the lateral conductivity of the photo-generated carriers in a pinned photodiode (PPD) and the voltage difference between the PPD and the floating diffusion (FD) node by controlling and optimizing the N doping concentration in the PPD and the threshold voltage of the reset transistor, respectively. The techniques shorten the charge transfer time from the PPD diode to the FD node effectively. The proposed process techniques do not need extra masks and do not cause harm to the fill factor. A sub array of 32 × 64 pixels was designed and implemented in the 0.18 μm CIS process with five implantation conditions splitting the N region in the PPD. The simulation and measured results demonstrate that the charge transfer time can be decreased by using the proposed techniques. Comparing the charge transfer time of the pixel with the different implantation conditions of the N region, the charge transfer time of 0.32 μs is achieved and 31% of image lag was reduced by using the proposed process techniques. (semiconductor devices)

Bane of Hydrogen-Bond Formation on the Photoinduced Charge-Transfer Process in Donor–Acceptor Systems

KAUST Repository

Alsam, Amani Abdu

2017-03-14

Controlling the ultrafast dynamical process of photoinduced charge transfer at donor acceptor interfaces remains a major challenge for physical chemistry and solar cell communities. The process is complicated by the involvement of other complex dynamical processes, including hydrogen bond formation, energy transfer, and solvation dynamics occurring on similar time scales. In this study, we explore the remarkable impact of hydrogen-bond formation on the interfacial charge transfer between a negatively charged electron donating anionic porphyrin and a positively charged electron accepting pi-conjugated polymer, as a model system in solvents with different polarities and capabilities for hydiogen bonding using femtosecond transient absorption spectroscopy. Unlike the conventional understanding of the key role of hydrogen bonding in promoting the charge-transfer process, our steadystate and time-resolved results reveal that the intervening hydrogen-bonding environment and, consequently, the probable longer spacing between the donor and acceptor molecules significantly hinders the charge-transfer process between them. These results show that site-specific hydrogen bonding and geometric considerations between donor and acceptor can be exploited to control both the charge-transfer dynamics and its efficiency not only at donor acceptor interfaces but also in complex biological systems.

Theory and simulation of charge transfer through DNA - nanotube contacts

International Nuclear Information System (INIS)

Rink, Gunda; Kong Yong; Koslowski, Thorsten

2006-01-01

We address the problem of charge transfer between a single-stranded adenine oligomer and semiconducting boron nitride nanotubes from a theoretical and numerical perspective. The model structures have been motivated by computer simulations; sample geometries are used as the input of an electronic structure theory that is based upon an extended Su-Schrieffer-Heeger Hamiltonian. By analyzing the emerging potential energy surfaces, we obtain hole transfer rates via Marcus' theory of charge transfer. In the presence of nanotubes, these rates exceed those of isolated DNA single strands by a factor of up to 10 4 . This enhancement can be rationalized and quantified as a combination of a template effect and the participation of the tube within a superexchange mechanism

Positron Annihilation in Solid Charge-Transfer Complexes

DEFF Research Database (Denmark)

Lévay, B.; Jansen, P.

1979-01-01

Positron lifetime and angular correlation measurements have been carried out on 1:1 charge-transfer complexes, on their pure donor and acceptor components and on the 1:1 M mechanical mixtures of these components. Complex formation reduced the intensity of the long-lifetime component of the donor...

Evaluating the Performance of DFT Functionals in Assessing the Interaction Energy and Ground-State Charge Transfer of Donor/Acceptor Complexes: Tetrathiafulvalene−Tetracyanoquinodimethane (TTF−TCNQ) as a Model Case

KAUST Repository

Sini, Gjergji

2011-03-08

We have evaluated the performance of several density functional theory (DFT) functionals for the description of the ground-state electronic structure and charge transfer in donor/acceptor complexes. The tetrathiafulvalene- tetracyanoquinodimethane (TTF-TCNQ) complex has been considered as a model test case. Hybrid functionals have been chosen together with recently proposed long-range corrected functionals (ωB97X, ωB97X-D, LRC-ωPBEh, and LC-ωPBE) in order to assess the sensitivity of the results to the treatment and magnitude of exact exchange. The results show an approximately linear dependence of the ground-state charge transfer with the HOMO TTF-LUMOTCNQ energy gap, which in turn depends linearly on the percentage of exact exchange in the functional. The reliability of ground-state charge transfer values calculated in the framework of a monodeterminantal DFT approach was also examined. © 2011 American Chemical Society.

Evaluating the Performance of DFT Functionals in Assessing the Interaction Energy and Ground-State Charge Transfer of Donor/Acceptor Complexes: Tetrathiafulvalene−Tetracyanoquinodimethane (TTF−TCNQ) as a Model Case

KAUST Repository

Sini, Gjergji; Sears, John S.; Brédas, Jean-Luc

2011-01-01

We have evaluated the performance of several density functional theory (DFT) functionals for the description of the ground-state electronic structure and charge transfer in donor/acceptor complexes. The tetrathiafulvalene- tetracyanoquinodimethane (TTF-TCNQ) complex has been considered as a model test case. Hybrid functionals have been chosen together with recently proposed long-range corrected functionals (ωB97X, ωB97X-D, LRC-ωPBEh, and LC-ωPBE) in order to assess the sensitivity of the results to the treatment and magnitude of exact exchange. The results show an approximately linear dependence of the ground-state charge transfer with the HOMO TTF-LUMOTCNQ energy gap, which in turn depends linearly on the percentage of exact exchange in the functional. The reliability of ground-state charge transfer values calculated in the framework of a monodeterminantal DFT approach was also examined. © 2011 American Chemical Society.

Tunable band structures in digital oxides with layered crystal habits

Science.gov (United States)

Shin, Yongjin; Rondinelli, James M.

2017-11-01

We use density functional calculations to show that heterovalent cation-order sequences enable control over band-gap variations up to several eV and band-gap closure in the bulk band insulator LaSrAlO4. The band-gap control originates from the internal electric fields induced by the digital chemical order, which induces picoscale band bending; the electric-field magnitude is mainly governed by the inequivalent charged monoxide layers afforded by the layered crystal habit. Charge transfer and ionic relaxations across these layers play secondary roles. This understanding is used to construct and validate a descriptor that captures the layer-charge variation and to predict changes in the electronic gap in layered oxides exhibiting antisite defects and in other chemistries.

Effects of acid concentration on intramolecular charge transfer ...

Indian Academy of Sciences (India)

rate. Time-dependent density functional theory calculations have been performed to understand the observed spectroscopic results. Keywords. Intramolecular charge transfer; absorption and fluorescence; time resolved fluorescence measurements; acid concentration dependence; time-dependent density functional theory.

Energy and charge transfer cascade in methylammonium lead bromide perovskite nanoparticle aggregates.

Science.gov (United States)

Bouduban, Marine E F; Burgos-Caminal, Andrés; Ossola, Rachele; Teuscher, Joël; Moser, Jacques-E

2017-06-01

Highly photoluminescent hybrid lead halide perovskite nanoparticles have recently attracted wide interest in the context of high-stake applications, such as light emitting diodes (LEDs), light emitting transistors and lasers. In addition, they constitute ideal model systems to explore energy and charge transport phenomena occurring at the boundaries of nanocrystalline grains forming thin films in high-efficiency perovskite solar cells (PSCs). Here we report a complete photophysical study of CH 3 NH 3 PbBr 3 perovskite nanoparticles suspended in chlorobenzene and highlight some important interaction properties. Colloidal suspensions under study were constituted of dispersed aggregates of quasi-2D platelets of a range of thicknesses, decorated with 3D-like spherical nanoparticles. These types of nanostructures possess different optical properties that afford a handle for probing them individually. The photophysics of the colloidal particles was studied by femtosecond pump-probe spectroscopy and time-correlated single-photon counting. We show here that a cascade of energy and exciton-mediated charge transfer occurs between nanostructures: upon photoexcitation, localized excitons within one nanostructure can either recombine on a ps timescale, yielding a short-lived emission, or form charge-transfer states (CTSs) across adjacent domains, resulting in longer-lived photoluminescence in the millisecond timescale. Furthermore, CTSs exhibit a clear signature in the form of a strong photoinduced electroabsorption evidenced in femtosecond transient absorption measurements. Charge transfer dynamics at the surface of the nanoparticles have been studied with various quenchers in solution. Efficient hole transfer to N , N , N ', N '-tetrakis(4-methoxyphenyl)benzidine (MeO-TPD) and 1,4-bis(diphenyl-amino)benzene (BDB) donors was attested by the quenching of the nanoparticles emission. The charge transfer rate was limited by the organic layer used to stabilize the nanoparticles

Charge transfer of edge states in zigzag silicene nanoribbons with Stone–Wales defects from first-principles

Energy Technology Data Exchange (ETDEWEB)

Ting, Xie [College of Mathematics and Statistics, Chongqing University, Chongqing 401331 (China); School of Mathematics and Statistic, Chongqing University of Technology, Chongqing 400054 (China); Rui, Wang, E-mail: rcwang@cqu.edu.cn [Institute for Structure and Function and Department of Physics, Chongqing University, Chongqing 400044 (China); State Key Laboratory of Theoretical Physics, Institute of Theoretical Physics, Chinese Academy of Science, Beijing 100190 (China); Shaofeng, Wang [Institute for Structure and Function and Department of Physics, Chongqing University, Chongqing 400044 (China); Xiaozhi, Wu, E-mail: xiaozhiwu@cqu.edu.cn [Institute for Structure and Function and Department of Physics, Chongqing University, Chongqing 400044 (China)

2016-10-15

Highlights: • The properties of SW defects in silicene and ZSNRs are obtained. • The SW defects at the edge of ZSNRs induce a sizable gap. • The charge transfer of edge states is resulted from SW defects in ZSNRS. - Abstract: Stone–Wales (SW) defects are favorably existed in graphene-like materials with honeycomb lattice structure and potentially employed to change the electronic properties in band engineering. In this paper, we investigate structural and electronic properties of SW defects in silicene sheet and its nanoribbons as a function of their concentration using the methods of periodic boundary conditions with first-principles calculations. We first calculate the formation energy, structural properties, and electronic band structures of SW defects in silicene sheet, with dependence on the concentration of SW defects. Our results show a good agreement with available values from the previous first-principles calculations. The energetics, structural aspects, and electronic properties of SW defects with dependence on defect concentration and location in edge-hydrogenated zigzag silicene nanoribbons are obtained. For all calculated concentrations, the SW defects prefer to locate at the edge due to the lower formation energy. The SW defects at the center of silicene nanoribbons slightly influence on the electronic properties, whereas the SW defects at the edge of silicene nanoribbons split the degenerate edge states and induce a sizable gap, which depends on the concentration of defects. It is worth to find that the SW defects produce a perturbation repulsive potential, which leads the decomposed charge of edge states at the side with defect to transfer to the other side without defect.

Predictions of flow and heat transfer in multiple impinging jets with an elliptic-blending second-moment closure

NARCIS (Netherlands)

Thielen, L.; Hanjalić, K.; Jonker, H.; Manceau, R.

2005-01-01

We present numerical computations of flow and heat transfer in multiple jets impinging normally on a flat heated surface, obtained with a new second-moment turbulence closure combined with an elliptic blending model of non-viscous wall blocking effect. This model provides the mean velocity and

High-energy behavior of the charge-transfer cross section in the eikonal approximation

International Nuclear Information System (INIS)

Dewangan, D.P.

1982-01-01

In the now popular version of the eikonal theory of charge transfer, the eikonal wave function does not satisfy the proper boundary conditions and the charge-transfer amplitude is uncertain by an undefined phase factor. The inclusion of the internuclear potential in a consistent way, in the eikonal theory overcomes theses difficulties. However, it also changes the high-energy asymptotic form of proton-hydrogen charge-transfer cross section from sigma/sub eik/ approx.(23/48) sigma/sub BK/ by a small amount to sigma/sub G/approx.(20.109/48)sigma/sub BK/ where sigma/sub BK/ is the Brinkman-Kramers cross section

Present status of heat transfer in narrow gap rectangular channel

International Nuclear Information System (INIS)

Sudo, Yukio; Kaminaga, Masanori

1990-01-01

In the safety evaluation for research nuclear reactors, at the time of abnormal transient change and accidents, after the tripping of a primary coolant pump, such event that the flow direction of coolant in a core reverses from steady downward flow to rising flow is supposed. In this case, the coexisting convection field, in which free convection and forced convection coexist, arises in place of forced convection, and especially in the research reactors using plate type fuel like JRR-3, it is important to grasp the heat transfer characteristics in the coexisting convection field in a narrow channel. Jackson et al. proposed the heat transfer correlation equation which can be applied to wide conditions including the coexisting convection zone, but its applicability to a narrow channel has not been confirmed. Based on the experimental results, in this study, the effect that the decrease of gap exerts to the convection heat transfer characteristics reported so far was investigated. The experiment and the results are reported. In this experiment on the coexisting convection zone in a narrow gap, the effect of main flow acceleration arose sufficiently large as compared with the effect of buoyancy, and heat transfer was promoted. (K.I.)

Natural convection heat transfer of water in a horizontal circular gap

Institute of Scientific and Technical Information of China (English)

SU Guanghui; Kenichiro Sugiyama; WU Yingwei

2007-01-01

An experimental study on the natural convection heat transfer on a horizontal downward facing heated surface in a water gap was carried out under atmospheric pressure conditions. A total of 700 experimental data points were correlated using Rayleigh versus Nusselt number in various forms, based on different independent variables. The effects of different characteristic lengths and film temperatures were discussed. The results show that the buoyancy force acts as a resistance force for natural convecti on beat transfer ona downward facing horizontal heated surface in a confined space. For the estimation of the natural convection heat transfer under the present conditions, empirical correlations in which Nusselt number is expressed as a function of the Rayleigh number, or both Rayleigh and Prandtl numbers, may be used. When it is accurately predicted, the Nusselt number is expressed as a function of the Rayleigh and Prandtl numbers, as well as the gap width-to-heated surface diameter ratio; and uses the temperature difference between the heated surface and the ambient fluid in the definition of Rayleigh number. The characteristic length is the gap size and the film temperature is the average fluid temperature.

Photoinduced charge and energy transfer in dye-doped conjugated polymers

International Nuclear Information System (INIS)

Veldman, Dirk; Bastiaansen, Jolanda J.A.M.; Langeveld-Voss, Bea M.W.; Sweelssen, Joergen; Koetse, Marc M.; Meskers, Stefan C.J.; Janssen, Rene A.J.

2006-01-01

Conjugated polymer-molecular dye blends of MDMO-PPV (poly[2-methoxy-5-(3',7'-dimethyloctyloxy)-1,4-phenylenevinylene]) and PF1CVTP (poly[9,9-dioctylfluorene-2,7-diyl-alt-2,5-bis(2-thienyl-1-cyanovinyl) -1-(3',7= '-dimethyloctyloxy)-4-methoxybenzene-5'',5''-diyl]) with three dipyrrometheneboron difluoride (bodipy) dyes were studied by (time-resolved) fluorescence and photoinduced absorption spectroscopy to determine quantitatively the relation between the electronic HOMO and LUMO levels and the occurrence of energy or charge transfer after optical excitation. We find that for MDMO-PPV photoinduced charge transfer to the dyes occurs, while photoexcitation of PF1CVTP exclusively results in energy transfer. The differences can be rationalized by assuming that the energy of the charge separated state is 0.33-0.45 eV higher than the energy determined from oxidation and reduction potentials of donor and acceptor, respectively. This provides an important design rule to identify appropriate materials for polymer solar cells that can have a high open-circuit voltage

Surface Charge Transfer Doping of Monolayer Phosphorene via Molecular Adsorption.

Science.gov (United States)

He, Yuanyuan; Xia, Feifei; Shao, Zhibin; Zhao, Jianwei; Jie, Jiansheng

2015-12-03

Monolayer phosphorene has attracted much attention owing to its extraordinary electronic, optical, and structural properties. Rationally tuning the electrical transport characteristics of monolayer phosphorene is essential to its applications in electronic and optoelectronic devices. Herein, we study the electronic transport behaviors of monolayer phosphorene with surface charge transfer doping of electrophilic molecules, including 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ), NO2, and MoO3, using density functional theory combined with the nonequilibrium Green's function formalism. F4TCNQ shows optimal performance in enhancing the p-type conductance of monolayer phosphorene. Static electronic properties indicate that the enhancement is originated from the charge transfer between adsorbed molecule and phosphorene layer. Dynamic transport behaviors demonstrate that additional channels for hole transport in host monolayer phosphorene were generated upon the adsorption of molecule. Our work unveils the great potential of surface charge transfer doping in tuning the electronic properties of monolayer phosphorene and is of significance to its application in high-performance devices.

An abnormally slow proton transfer reaction in a simple HBO derivative due to ultrafast intramolecular-charge transfer events.

Science.gov (United States)

Alarcos, Noemí; Gutierrez, Mario; Liras, Marta; Sánchez, Félix; Douhal, Abderrazzak

2015-07-07

We report on the steady-state, picosecond and femtosecond time-resolved studies of a charge and proton transfer dye 6-amino-2-(2'-hydroxyphenyl)benzoxazole (6A-HBO) and its methylated derivative 6-amino-2-(2'-methoxyphenyl)benzoxazole (6A-MBO), in different solvents. With femtosecond resolution and comparison with the photobehaviour of 6A-MBO, we demonstrate for 6A-HBO in solution, the photoproduction of an intramolecular charge-transfer (ICT) process at S1 taking place in ∼140 fs or shorter, followed by solvent relaxation in the charge transferred species. The generated structure (syn-enol charge transfer conformer) experiences an excited-state intramolecular proton-transfer (ESIPT) reaction to produce a keto-type tautomer. This subsequent proton motion occurs in 1.2 ps (n-heptane), 14 ps (DCM) and 35 ps (MeOH). In MeOH, it is assisted by the solvent molecules and occurs through tunneling for which we got a large kinetic isotope effect (KIE) of about 13. For the 6A-DBO (deuterated sample in CD3OD) the global proton-transfer reaction takes place in 200 ps, showing a remarkable slow KIE regime. The slow ESIPT reaction in DCM (14 ps), not through tunnelling as it is not sensitive to OH/OD exchange, has however to overcome an energy barrier using intramolecular as well as solvent coordinates. The rich ESIPT dynamics of 6A-HBO in the used solutions is governed by an ICT reaction, triggered by the amino group, and it is solvent dependent. Thus, the charge injection to a 6A-HBO molecular frame makes the ICT species more stable, and the phenol group less acidic, slowing down the subsequent ESIPT reaction. Our findings bring new insights into the coupling between ICT and ESIPT reactions on the potential-energy surfaces of several barriers.

Photo-induced charge transfer at heterogeneous interfaces: Dye-sensitized tin disulfide, the theory and the experiment

International Nuclear Information System (INIS)

Lanzafame, J.M.

1993-01-01

The study of photo-induced charge transfer is an endeavor that spans the entire industrial period of man's history. Its great importance demands an ever greater understanding of its underlying principles. The work discussed here attempts to probe elementary aspects of the charge transfer process. Investigations into the theory of charge transfer reactions are made in an attempt to isolate the relevant parameters. An analytical discussion is made of a simple Golden Rule type rate equation to describe the transfer kinetics. Then a quantum simulation is carried out to follow the wavefunction propagation as a test of the applicability of the assumptions made in deriving the simpler rate equation. Investigation of charge transfer at surfaces is bet served by the application of ultrafast optical spectroscopies to probe carrier dynamics. A discussion of the properties of the short pulse laser systems employed is included along with a discussion of the different optical spectroscopies available. These tools are then brought to bear upon dye-sensitized SnS 2 , a model system for the study of charge injection processes. The unique properties of the semiconductor are discussed with respect to the charge transfer process. The unique properties of the semiconductor are discussed with respect to the charge transfer process. The optical experiments performed on the dye/SnS 2 systems elucidate the fundamental carrier dynamics and these dynamics are discussed within the theoretical framework to provide a complete picture of the charge transfer kinetics

Super-iron Nanoparticles with Facile Cathodic Charge Transfer

Energy Technology Data Exchange (ETDEWEB)

M Farmand; D Jiang; B Wang; S Ghosh; D Ramaker; S Licht

2011-12-31

Super-irons contain the + 6 valence state of iron. One advantage of this is that it provides a multiple electron opportunity to store additional battery charge. A decrease of particle size from the micrometer to the nanometer domain provides a higher surface area to volume ratio, and opportunity to facilitate charge transfer, and improve the power, voltage and depth of discharge of cathodes made from such salts. However, super-iron salts are fragile, readily reduced to the ferric state, with both heat and contact with water, and little is known of the resultant passivating and non-passivating ferric oxide products. A pathway to decrease the super-iron particle size to the nano-domain is introduced, which overcomes this fragility, and retains the battery capacity advantage of their Fe(VI) valence state. Time and power controlled mechanosynthesis, through less aggressive, dry ball milling, leads to facile charge transfer of super-iron nanoparticles. Ex-situ X-ray Absorption Spectroscopy is used to explore the oxidation state and structure of these iron oxides during discharge and shows the significant change in stability of the ferrate structure to lower oxidation state when the particle size is in the nano-domain.

Charge transfer between O6+ and atomic hydrogen

Science.gov (United States)

Wu, Y.; Stancil, P. C.; Liebermann, H. P.; Buenker, R. J.; Schultz, D. R.; Hui, Y.

2011-05-01

The charge exchange process has been found to play a dominant role in the production of X-rays and/or EUV photons observed in cometary and planetary atmospheres and from the heliosphere. Charge transfer cross sections, especially state-selective cross sections, are necessary parameters in simulations of X-ray emission. In the present work, charge transfer due to collisions of ground state O6+(1s2 1 S) with atomic hydrogen has been investigated theoretically using the quantum-mechanical molecular-orbital close-coupling method (QMOCC). The multi-reference single- and double-excitation configuration interaction approach (MRDCI) has been applied to compute the adiabatic potential and nonadiabatic couplings, and the atomic basis sets used have been optimized with the method proposed previously to obtain precise potential data. Total and state-selective cross sections are calculated for energies between 10 meV/u and 10 keV/u. The QMOCC results are compared to available experimental and theoretical data as well as to new atomic-orbital close-coupling (AOCC) and classical trajectory Monte Carlo (CTMC) calculations. A recommended set of cross sections, based on the MOCC, AOCC, and CTMC calculations, is deduced which should aid in X-ray modeling studies.

Integer Charge Transfer and Hybridization at an Organic Semiconductor/Conductive Oxide Interface

KAUST Repository

Gruenewald, Marco

2015-02-11

We investigate the prototypical hybrid interface formed between PTCDA and conductive n-doped ZnO films by means of complementary optical and electronic spectroscopic techniques. We demonstrate that shallow donors in the vicinity of the ZnO surface cause an integer charge transfer to PTCDA, which is clearly restricted to the first monolayer. By means of DFT calculations, we show that the experimental signatures of the anionic PTCDA species can be understood in terms of strong hybridization with localized states (the shallow donors) in the substrate and charge back-donation, resulting in an effectively integer charge transfer across the interface. Charge transfer is thus not merely a question of locating the Fermi level above the PTCDA electron-transport level but requires rather an atomistic understanding of the interfacial interactions. The study reveals that defect sites and dopants can have a significant influence on the specifics of interfacial coupling and thus on carrier injection or extraction.

Closure of population biobanks and direct-to-consumer genetic testing companies.

Science.gov (United States)

Zawati, Ma'n H; Borry, Pascal; Howard, Heidi Carmen

2011-09-01

Genetic research gained new momentum with the completion of the Human Genome Project in 2003. Formerly centered on the investigation of single-gene disorders, genetic research is increasingly targeting common complex diseases and in doing so is studying the whole genome, the environment and its impact on genomic variation. Consequently, biobanking initiatives have emerged around the world as a tool to sustain such progress. Whether they are small scale or longitudinal, public or private, commercial or non-commercial, biobanks should consider the possibility of closure. Interestingly, while raising important ethical issues, this topic has hardly been explored in the literature. Indeed, ethical issues associated with sale, insolvency, end of funding, or transfer of materials to other entities (which are all issues either related to or possible consequences of closure) are seldom the subject of discussion. In an attempt to fill this gap, this paper will discuss-using population and direct-to-consumer (DTC) genetic testing companies' biobanks as case studies-(1) international and national normative documents addressing the issue of closure and (2) the internal policies of population biobanks and DTC genetic testing companies. The analysis will inform the debate on biobank closure and elucidate the underlying ethical issues, which include, but are not limited to informed consent, storage and privacy.

Charge Transfer Channels in Formation of Exciplex in Polymer Blends

Science.gov (United States)

Dou, Fei; Zhang, Xin-Ping

2011-09-01

The strong dependence of photoluminescence of charge transfer excited states or exciplex in a blend film of poly(9,9'-dioctylfluorene-co-benzothiadiazole) (F8BT) and poly(9,9'-dioctylfluorene-co-bis-N,N'-(4-butylphenyl)-bis-N,N'-phenyl-1,4- phenylenediamine) (PFB) on the excitation wavelengths and morphology is investigated. The experimental results reveal that electron transfer in the LUMOs from PFB to F8BT is more efficient than hole transfer in the HOMOs from PFB to F8BT for the formation of exciplex at the interfacial junctions between these two types of molecules in the blend film. Furthermore, energy transfer from the blue-emitting PFB to the green-emitting F8BT at the interfaces introduces an additional two-step channel and thus enhances the formation of an exciplex. This is important for understanding of charge generation and separation in organic bulk heterojunctions and for design of optoelectronic devices.

Charge Transfer Channels in Formation of Exciplex in Polymer Blends

International Nuclear Information System (INIS)

Dou Fei; Zhang Xin-Ping

2011-01-01

The strong dependence of photoluminescence of charge transfer excited states or exciplex in a blend film of poly(9,9'-dioctylfluorene-co-benzothiadiazole) (F8BT) and poly(9,9'-dioctylfluorene-co-bis-N,N'-(4-butylphenyl)-bis-N,N'-phenyl-1,4- phenylenediamine) (PFB) on the excitation wavelengths and morphology is investigated. The experimental results reveal that electron transfer in the LUMOs from PFB to F8BT is more efficient than hole transfer in the HOMOs from PFB to F8BT for the formation of exciplex at the interfacial junctions between these two types of molecules in the blend film. Furthermore, energy transfer from the blue-emitting PFB to the green-emitting F8BT at the interfaces introduces an additional two-step channel and thus enhances the formation of an exciplex. This is important for understanding of charge generation and separation in organic bulk heterojunctions and for design of optoelectronic devices. (condensed matter: electronic structure, electrical, magnetic, and optical properties)

Predictions for heat transfer characteristics in a natural draft reactor cooling system using a second moment closure turbulence model

International Nuclear Information System (INIS)

Nishimura, M.; Maekawa, I.

2004-01-01

A numerical study is performed on the natural draft reactor cavity cooling system (RCCS). In the cooling system, buoyancy driven heated upward flow could be in the mixed convection regime that is accompanied by heat transfer impairment. Also, the heating wall condition is asymmetric with regard to the channel cross section. These flow regime and thermal boundary conditions may invalidate the use of design correlation. To precisely simulate the flow and thermal fields within the RCCS, the second moment closure turbulence model is applied. Two types of the RCCS channel geometry are selected to make a comparison: an annular duct with fins on the outer surface of the inner circular wall, and a multi-rectangular duct. The prediction shows that the local heat transfer coefficient on the RCCS with finned annular duct is less than 1/6 of that estimated with Dittus-Boelter correlation. Much portion of the natural draft airflow does not contribute cooling at all because mainstream escapes from the narrow gaps between the fins. This result and thus the finned annulus design are unacceptable from the viewpoint for structural integrity of the RCCS wall boundary. The performance of the multi-rectangular duct design is acceptable that the RCCS maximum temperature is less than 400 degree centigrade even when the flow rate is halved from the designed condition. (author)

Charge transfer through DNA/DNA duplexes and DNA/RNA hybrids: complex theoretical and experimental studies.

Science.gov (United States)

Kratochvílová, Irena; Vala, Martin; Weiter, Martin; Špérová, Miroslava; Schneider, Bohdan; Páv, Ondřej; Šebera, Jakub; Rosenberg, Ivan; Sychrovský, Vladimír

2013-01-01

Oligonucleotides conduct electric charge via various mechanisms and their characterization and understanding is a very important and complicated task. In this work, experimental (temperature dependent steady state fluorescence spectroscopy, time-resolved fluorescence spectroscopy) and theoretical (Density Functional Theory) approaches were combined to study charge transfer processes in short DNA/DNA and RNA/DNA duplexes with virtually equivalent sequences. The experimental results were consistent with the theoretical model - the delocalized nature of HOMO orbitals and holes, base stacking, electronic coupling and conformational flexibility formed the conditions for more effective short distance charge transfer processes in RNA/DNA hybrids. RNA/DNA and DNA/DNA charge transfer properties were strongly connected with temperature affected structural changes of molecular systems - charge transfer could be used as a probe of even tiny changes of molecular structures and settings. © 2013. Published by Elsevier B.V. All rights reserved.

Charge transfer in rectifying oxide heterostructures and oxide access elements in ReRAM

Energy Technology Data Exchange (ETDEWEB)

Stefanovich, G. B.; Pergament, A. L.; Boriskov, P. P.; Kuroptev, V. A., E-mail: v.a.kuroptev@gmail.com; Stefanovich, T. G. [Petrozavodsk State University (Russian Federation)

2016-05-15

The main aspects of the synthesis and experimental research of oxide diode heterostructures are discussed with respect to their use as selector diodes, i.e., access elements in oxide resistive memory. It is shown that charge transfer in these materials differs significantly from the conduction mechanism in p–n junctions based on conventional semiconductors (Si, Ge, A{sup III}–B{sup V}), and the model should take into account the electronic properties of oxides, primarily the low carrier drift mobility. It is found that an increase in the forward current requires an oxide with a small band gap (<1.3 eV) in the heterostructure composition. Heterostructures with Zn, In–Zn (IZO), Ti, Ni, and Cu oxides are studied; it is found that the CuO–IZO heterojunction has the highest forward current density (10{sup 4} A/cm{sup 2}).

Heat transfer coefficient for flow boiling in an annular mini gap

Directory of Open Access Journals (Sweden)

Hożejowska Sylwia

2016-01-01

Full Text Available The aim of this paper was to present the concept of mathematical models of heat transfer in flow boiling in an annular mini gap between the metal pipe with enhanced exterior surface and the external glass pipe. The one- and two-dimensional mathematical models were proposed to describe stationary heat transfer in the gap. A set of experimental data governed both the form of energy equations in cylindrical coordinates and the boundary conditions. The models were formulated to minimize the number of experimentally determined constants. Known temperature distributions in the enhanced surface and in the fluid helped to determine, from the Robin condition, the local heat transfer coefficients at the enhanced surface – fluid contact. The Trefftz method was used to find two-dimensional temperature distributions for the thermal conductive filler layer, enhanced surface and flowing fluid. The method of temperature calculation depended on whether the area of single-phase convection ended with boiling incipience in the gap or the two-phase flow region prevailed, with either fully developed bubbly flow or bubbly-slug flow. In the two–phase flow, the fluid temperature was calculated by Trefftz method. Trefftz functions for the Laplace equation and for the energy equation were used in the calculations.

Charge transfer and excitation in high-energy ion-atom collisions

International Nuclear Information System (INIS)

Schlachter, A.S.; Berkner, K.H.; McDonald, R.J.

1986-11-01

Coincidence measurements of charge transfer and simultaneous projectile electron excitation provide insight into correlated two-electron processes in energetic ion-atom collisions. Projectile excitation and electron capture can occur simultaneously in a collision of a highly charged ion with a target atom; this process is called resonant transfer and excitation (RTE). The intermediate excited state which is thus formed can subsequently decay by photon emission or by Auger-electron emission. Results are shown for RTE in both the K shell of Ca ions and the L shell of Nb ions, for simultaneous projectile electron loss and excitation, and for the effect of RTE on electron capture

Radiative charge-transfer lifetime of the excited state of (NaCa)+

International Nuclear Information System (INIS)

Makarov, Oleg P.; Cote, R.; Michels, H.; Smith, W.W.

2003-01-01

New experiments were proposed recently to investigate the regime of cold atomic and molecular ion-atom collision processes in a special hybrid neutral-atom-ion trap under high-vacuum conditions. We study the collisional cooling of laser precooled Ca + ions by ultracold Na atoms. Modeling this process requires knowledge of the radiative lifetime of the excited singlet A 1 Σ + state of the (NaCa) + molecular system. We calculate the rate coefficient for radiative charge transfer using a semiclassical approach. The dipole radial matrix elements between the ground and the excited states, and the potential curves were calculated using complete active space self-consistent field and Moeller-Plesset second-order perturbation theory with an extended Gaussian basis, 6-311+G (3df). The semiclassical charge-transfer rate coefficient was averaged over a thermal Maxwellian distribution. In addition, we also present elastic collision cross sections and the spin-exchange cross section. The rate coefficient for charge transfer was found to be 2.3x10 -16 cm 3 /sec, while those for the elastic and spin-exchange cross sections were found to be several orders of magnitude higher (1.1x10 -8 cm 3 /sec and 2.3x10 -9 cm 3 /sec, respectively). This confirms our assumption that the milli-Kelvin regime of collisional cooling of calcium ions by sodium atoms is favorable with the respect to low loss of calcium ions due to the charge transfer

Charge transfer excitations from excited state Hartree-Fock subsequent minimization scheme

International Nuclear Information System (INIS)

Theophilou, Iris; Tassi, M.; Thanos, S.

2014-01-01

Photoinduced charge-transfer processes play a key role for novel photovoltaic phenomena and devices. Thus, the development of ab initio methods that allow for an accurate and computationally inexpensive treatment of charge-transfer excitations is a topic that nowadays attracts a lot of scientific attention. In this paper we extend an approach recently introduced for the description of single and double excitations [M. Tassi, I. Theophilou, and S. Thanos, Int. J. Quantum Chem. 113, 690 (2013); M. Tassi, I. Theophilou, and S. Thanos, J. Chem. Phys. 138, 124107 (2013)] to allow for the description of intermolecular charge-transfer excitations. We describe an excitation where an electron is transferred from a donor system to an acceptor one, keeping the excited state orthogonal to the ground state and avoiding variational collapse. These conditions are achieved by decomposing the space spanned by the Hartree-Fock (HF) ground state orbitals into four subspaces: The subspace spanned by the occupied orbitals that are localized in the region of the donor molecule, the corresponding for the acceptor ones and two more subspaces containing the virtual orbitals that are localized in the neighborhood of the donor and the acceptor, respectively. Next, we create a Slater determinant with a hole in the subspace of occupied orbitals of the donor and a particle in the virtual subspace of the acceptor. Subsequently we optimize both the hole and the particle by minimizing the HF energy functional in the corresponding subspaces. Finally, we test our approach by calculating the lowest charge-transfer excitation energies for a set of tetracyanoethylene-hydrocarbon complexes that have been used earlier as a test set for such kind of excitations

Charge Separation and Recombination in Small Band Gap Oligomer-Fullerene Triads

NARCIS (Netherlands)

Karsten, Bram P.; Bouwer, Ricardo K. M.; Hummelen, Jan C.; Williams, Rene M.; Janssen, Rene A. J.

2010-01-01

Synthesis and photophysics of a series of thiophene-thienopyrazine small band gap oligomers end-capped at both ends with C(60) are presented In these triads a photoinduced electron transfer reaction occurs between the oligomer as a donor and the fullerene as an acceptor Femtosecond photoinduced

Incorporation of charge transfer into the explicit polarization fragment method by grand canonical density functional theory.

Science.gov (United States)

Isegawa, Miho; Gao, Jiali; Truhlar, Donald G

2011-08-28

Molecular fragmentation algorithms provide a powerful approach to extending electronic structure methods to very large systems. Here we present a method for including charge transfer between molecular fragments in the explicit polarization (X-Pol) fragment method for calculating potential energy surfaces. In the conventional X-Pol method, the total charge of each fragment is preserved, and charge transfer between fragments is not allowed. The description of charge transfer is made possible by treating each fragment as an open system with respect to the number of electrons. To achieve this, we applied Mermin's finite temperature method to the X-Pol wave function. In the application of this method to X-Pol, the fragments are open systems that partially equilibrate their number of electrons through a quasithermodynamics electron reservoir. The number of electrons in a given fragment can take a fractional value, and the electrons of each fragment obey the Fermi-Dirac distribution. The equilibrium state for the electrons is determined by electronegativity equalization with conservation of the total number of electrons. The amount of charge transfer is controlled by re-interpreting the temperature parameter in the Fermi-Dirac distribution function as a coupling strength parameter. We determined this coupling parameter so as to reproduce the charge transfer energy obtained by block localized energy decomposition analysis. We apply the new method to ten systems, and we show that it can yield reasonable approximations to potential energy profiles, to charge transfer stabilization energies, and to the direction and amount of charge transferred. © 2011 American Institute of Physics

Positronium Inhibition and Quenching by Organic Electron Acceptors and Charge Transfer Complexes

DEFF Research Database (Denmark)

Jansen, P.; Eldrup, Morten Mostgaard; Jensen, Bror Skytte

1975-01-01

Positron lifetime measurements were performed on a series of organic electron acceptors and charge-transfer complexes in solution. The acceptors cause both positronium (Ps) inhibition (with maybe one exception) and quenching, but when an acceptor takes part in a charge-transfer complex...... in terms of the spur reaction model of Ps formation. Correlation was also made to gas phase reaction between electron acceptors and free electron, as well as to pulse radiolysis data....

Changes in wetting and contact charge transfer by femtosecond laser-ablation of polyimide

Energy Technology Data Exchange (ETDEWEB)

Guo, X.D., E-mail: xiaodong.guo@uib.no [Department of Physics and Technology, Allegaten 55, 5020 Bergen, University of Bergen (Norway); Dai, Y.; Gong, M. [Department of Physics, Shanghai 200444, Shanghai University (China); Qu, Y.G. [Center for Geobiology, Allegaten 41, 5020 Bergen, University of Bergen (Norway); Helseth, L.E. [Department of Physics and Technology, Allegaten 55, 5020 Bergen, University of Bergen (Norway)

2015-09-15

Highlights: • Laser ablation significantly reduced the triboelectric charging of polyimide films. • Hierarchical micro/nanostructures formed on the surface of the sample. • Structural anisotropy leads to spatially varying contact angles of water droplets. • Raman spectroscopy revealed a carbonization of the polyimide sample. • The corresponding loss of insulation may explain the reduction of charge transfer. - Abstract: In this study it is demonstrated that the triboelectric charging of polyimide thin films is significantly reduced by using a femtosecond laser to nanostructure its. It is found that the contact charge transfer between laser-ablated Kapton and aluminum is almost negligible, and even much lower than the significant current occurring when non-treated Kapton touches the metal. Scanning electron microscopy demonstrates that laser ablation produces a hierarchical micro and nanostructure, and it is found that the structural anisotropy leads to spatially varying contact angles of water droplets residing on the surface. Raman spectra suggest that the centers of the laser-ablated tracks are carbonized; therefore, the loss of insulation can be responsible for the reduction of charge transfer.

Dissociative electron attachment and charge transfer in condensed matter

International Nuclear Information System (INIS)

Bass, A.D.; Sanche, L.

2003-01-01

Experiments using energy-selected beams of electrons incident from vacuum upon thin vapour deposited solids show that, as in the gas-phase, scattering cross sections at low energies are dominated by the formation of temporary negative ions (or resonances) and that molecular damage may be effected via dissociative electron attachment (DEA). Recent results also show that charge transfer between anionic states of target molecules and their environment is often crucial in determining cross sections for electron driven processes. Here, we review recent work from our laboratory, in which charge transfer is observed. For rare gas solids, electron exchange between the electron-exciton complex and either a metal substrate or co-adsorbed molecule enhances the desorption of metastable atoms and/or molecular dissociation. We discuss how transient electron capture by surface electron states of a substrate and subsequent electron transfer to a molecular adsorbate enhances the effective cross sections for DEA. We also consider the case of DEA to CF 2 Cl 2 condensed on water and ammonia ices, where electron exchange between pre-solvated electron states of ice and transient molecular anions can also increase DEA cross sections. Electron transfer from molecular resonances into pre-solvated electron states of ice is also discussed

Risk Factors for Gaps in Care during Transfer from Pediatric to Adult Cystic Fibrosis Programs in the United States.

Science.gov (United States)

Sawicki, Gregory S; Ostrenga, Joshua; Petren, Kristofer; Fink, Aliza K; D'Agostino, Emma; Strassle, Camila; Schechter, Michael S; Rosenfeld, Margaret

2018-02-01

With improved survival into adulthood, the number of dedicated adult cystic fibrosis (CF) care programs has expanded in the United States over the past decade. Transfer from pediatric to adult CF programs represents a potential time for lapses in recommended health care. To describe variability in transfer between pediatric and adult CF care programs and to identify factors associated with prolonged gaps in care. Using the U.S. CF Foundation Patient Registry, we identified individuals with CF who transferred care from a pediatric to an adult CF care program during 2007 to 2013. A gap in care was defined as the time in days between the last recorded pediatric encounter and the first recorded adult encounter. A hierarchical multivariable regression model was applied to investigate the effect of program- and patient-level factors on gaps in care. There were 1,946 individuals at 155 pediatric CF programs who transferred to an adult CF program during the analytic period. The mean age at transfer was 21.1 years, with 68% transferring care between ages 18 and 21 years. The mean gap in care during transfer was 183 days (median, 106 d; range, 2-1,843 d); 47% had a less than 100-day gap, and 13% had a greater than or equal to 365-day gap (prolonged gap). Prolonged gaps in care were more likely to occur among those younger than age 18 years (odds ratio, 3.33; 95% confidence interval, 2.06-5.37) at the time of transfer and those who transferred to an adult program that was in a different city from their pediatric or affiliate program (odds ratio, 2.16; 95% confidence interval, 1.48-3.17). Having any health insurance coverage was associated with decreased likelihood of prolonged gaps (private insurance vs. no insurance [odds ratio, 0.15; 95% confidence interval, 0.09-0.23] or any government insurance versus no insurance [odds ratio, 0.11; 95% confidence interval, 0.07-0.18]). Lung function, nutritional status, and receipt of intravenous antibiotics in the final year of

Theoretical study on production of heavy neutron-rich isotopes around the N=126 shell closure in radioactive beam induced transfer reactions

Directory of Open Access Journals (Sweden)

Long Zhu

2017-04-01

Full Text Available In order to produce more unknown neutron-rich nuclei around N=126, the transfer reactions 136Xe + 198Pt, 136–144Xe + 208Pb, and 132Sn + 208Pb are investigated within the framework of the dinuclear system (DNS model. The influence of neutron excess of projectile on production cross sections of target-like products is studied through the reactions 136,144Xe + 208Pb. We find that the radioactive projectile 144Xe with much larger neutron excess is favorable to produce neutron-rich nuclei with charge number less than the target rather than produce transtarget nuclei. The incident energy dependence of yield distributions of fragments in the reaction 132Sn + 208Pb are also studied. The production cross sections of neutron-rich nuclei with Z=72–77 are predicted in the reactions 136–144Xe + 208Pb and 132Sn + 208Pb. It is noticed that the production cross sections of unknown neutron-rich nuclei in the reaction 144Xe + 208Pb are at least two orders of magnitude larger than those in the reaction 136Xe + 208Pb. The radioactive beam induced transfer reactions 139,144Xe + 208Pb, considering beam intensities proposed in SPIRAL2 (Production System of Radioactive Ion and Acceleration On-Line project as well, for production of neutron-rich nuclei around the N=126 shell closure are investigated for the first time. It is found that, in comparison to the stable beam 136Xe, the radioactive beam 144Xe shows great advantages for producing neutron-rich nuclei with N=126 and the advantages get more obvious for producing nuclei with less charge number.

Optimization of charge transfer and transport processes at the CdSe quantum dots/TiO2 nanorod interface by TiO2 interlayer passivation

International Nuclear Information System (INIS)

Jaramillo-Quintero, O A; Rincon, M E; Triana, M A

2017-01-01

Surface trap states hinder charge transfer and transport properties in TiO 2 nanorods (NRs), limiting its application on optoelectronic devices. Here, we study the interfacial processes between rutile TiO 2 NR and CdSe quantum dots (QDs) using TiO 2 interlayer passivation treatments. Anatase or rutile TiO 2 thin layers were deposited on an NR surface by two wet-chemical deposition treatments. Reduced interfacial charge recombination between NRs and CdSe QDs was observed by electrochemical impedance spectroscopy with the introduction of TiO 2 thin film interlayers compared to bare TiO 2 NRs. These results can be ascribed to in-gap trap state passivation of the TiO 2 NR surface, which led to an increase in open circuit voltage. Moreover, the rutile thin layer was more efficient than anatase to promote a higher photo-excited electron transfer from CdSe QDs to TiO 2 NRs due to a large driving force for charge injection, as confirmed by surface photovoltage spectroscopy. (paper)

Charge-Transfer Complexes Studied by Dynamic Force Spectroscopy

Directory of Open Access Journals (Sweden)

Jurriaan Huskens

2013-03-01

Full Text Available In this paper, the strength and kinetics of two charge-transfer complexes, naphthol-methylviologen and pyrene-methylviologen, are studied using dynamic force spectroscopy. The dissociation rates indicate an enhanced stability of the pyrene-methylviologen complex, which agrees with its higher thermodynamic stability compared to naphthol-methylviologen complex.

Energy and charge transfer in ionized argon coated water clusters

International Nuclear Information System (INIS)

Kočišek, J.; Lengyel, J.; Fárník, M.; Slavíček, P.

2013-01-01

We investigate the electron ionization of clusters generated in mixed Ar-water expansions. The electron energy dependent ion yields reveal the neutral cluster composition and structure: water clusters fully covered with the Ar solvation shell are formed under certain expansion conditions. The argon atoms shield the embedded (H 2 O) n clusters resulting in the ionization threshold above ≈15 eV for all fragments. The argon atoms also mediate more complex reactions in the clusters: e.g., the charge transfer between Ar + and water occurs above the threshold; at higher electron energies above ∼28 eV, an excitonic transfer process between Ar + * and water opens leading to new products Ar n H + and (H 2 O) n H + . On the other hand, the excitonic transfer from the neutral Ar* state at lower energies is not observed although this resonant process was demonstrated previously in a photoionization experiment. Doubly charged fragments (H 2 O) n H 2 2+ and (H 2 O) n 2+ ions are observed and Intermolecular Coulomb decay (ICD) processes are invoked to explain their thresholds. The Coulomb explosion of the doubly charged cluster formed within the ICD process is prevented by the stabilization effect of the argon solvent

Charge transfer in conjugated oligomers encapsulated into carbon nanotubes

Energy Technology Data Exchange (ETDEWEB)

Almadori, Y.; Alvarez, L.; Michel, T.; Le Parc, R.; Bantignies, J.L.; Hermet, P.; Sauvajol, J.L. [Laboratoire Charles Coulomb UMR 5521, Universite Montpellier 2, 34095 Montpellier (France); Laboratoire Charles Coulomb UMR 5521, CNRS, 34095 Montpellier (France); Arenal, R. [Laboratoire d' Etude des Microstructures, CNRS-ONERA, 92322 Chatillon (France); Laboratorio de Microscopias Avanzadas, Instituto de Nanociencia de Aragon, U. Zaragoza, 50018 Zaragoza (Spain); Babaa, R. [Laboratoire de Chimie des Surfaces et Interfaces, CEA, IRAMIS, SPCSI, 91191 Gif-sur-Yvette Cedex (France); Chemical Engineering Department, University of Technology PETRONAS, UTP, Ipoh-Perak (Malaysia); Jouselme, B.; Palacin, S. [Laboratoire de Chimie des Surfaces et Interfaces, CEA, IRAMIS, SPCSI, 91191 Gif-sur-Yvette Cedex (France)

2011-11-15

This study deals with a hybrid system consisting in quaterthiophene derivative encapsulated inside single-walled and multi-walled carbon nanotubes. Investigations of the encapsulation step are performed by transmission electron microscopy. Raman spectroscopy data point out different behaviors depending on the laser excitation energy with respect to the optical absorption of quaterthiophene. At low excitation energy (far from the oligomer resonance window) there is no significant modification of the Raman spectra before and after encapsulation. By contrast, at high excitation energy (close to the oligomer resonance window), Raman spectra exhibit a G-band shift together with an important RBM intensity loss, suggesting a significant charge transfer between the inserted molecule and the host nanotubes. Those results suggest a photo induced process leading to a significant charge transfer. (Copyright copyright 2011 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

Vibrational spectra of charge transfer complexes of lead phthalocyanine

International Nuclear Information System (INIS)

Oza, A.T.; Patel, S.G.; Patel, R.G.; Prajapati, S.M.; Vaidya, Rajiv

2005-01-01

Infrared spectra of six charge transfer complexes of lead phthalocyanine (PbPc), namely, PbPc-I 2 , PbPc-TCNQ, PbPc-DDQ, PbPc-chloranil, PbPc-TCNE and PbPc-TNF, where TCNQ=7,7,8,8-tetracyano-1,4-quinodimethane, DDQ=2,3-dichloro-5,6-dicyano-p-benzoquinone, TCNE=tetracyano-p-ethylene and TNF=2,4,5,7-tetranitro-9-fluorenone have been studied in the range of 400-4000 cm -1 . The analysis of featureless absorption is carried out for studying transition across the Peierls gap of 0.225 eV. The electronic absorption envelopes at 1500, 1100 and 3400 cm -1 are found to have Gaussian shapes and not the degenerate oscillators, as found in purely organic conductors. There is a pairing of two electrons on phthalocyanine ligand as required in Little's model, and consequently, the electronic absorption envelope is a doublet. Electronic absorption envelope is a doublet showing two peaks at 1500 and 1100 cm -1 , indicating a two-electron problem in PbPc. Metal-ligand vibrations between 400 and 700 cm -1 lead to indirect transition between the valence and conduction bands and phonon-mediated coupling between metal chains and the side chains

Symmetric resonance double charge transfer in Kr++ + Kr and Xe++ + Xe systems

International Nuclear Information System (INIS)

Okuno, K.; Koizumi, T.; Kaneko, Y.

1978-01-01

Cross sections of processes Kr ++ + Kr → Ke + Kr ++ and Xe ++ + Xe → Xe + Xe ++ were measured by the injected-ion-drift-tube technique from 0.04 to 20 eV. For both cases, the cross section below 1 eV coincides with the orbiting cross sections with a charge-transfer probability 1/2. Above 1 eV, the energy dependence of the cross sectcion is like that for single charge transfer. Mobilities of Kr ++ and Xe ++ in He are presented also

A two-dimensional position sensitive gas chamber with scanned charge transfer readout

Energy Technology Data Exchange (ETDEWEB)

Gomez, F. E-mail: faustgr@usc.es; Iglesias, A.; Lobato, R.; Mosquera, J.; Pardo, J.; Pena, J.; Pazos, A.; Pombar, M.; Rodriguez, A

2003-10-21

We have constructed and tested a two-dimensional position sensitive parallel-plate gas ionization chamber with scanned charge transfer readout. The scan readout method described here is based on the development of a new position-dependent charge transfer technique. It has been implemented by using gate strips perpendicularly oriented to the collector strips. This solution reduces considerably the number of electronic readout channels needed to cover large detector areas. The use of a 25 {mu}m thick kapton etched circuit allows high charge transfer efficiency with a low gating voltage, consequently needing a very simple commutating circuit. The present prototype covers 8x8 cm{sup 2} with a pixel size of 1.27x1.27 mm{sup 2}. Depending on the intended use and beam characteristics a smaller effective pixel is feasible and larger active areas are possible. This detector can be used for X-ray or other continuous beam intensity profile monitoring.

A two-dimensional position sensitive gas chamber with scanned charge transfer readout

International Nuclear Information System (INIS)

Gomez, F.; Iglesias, A.; Lobato, R.; Mosquera, J.; Pardo, J.; Pena, J.; Pazos, A.; Pombar, M.; Rodriguez, A.

2003-01-01

We have constructed and tested a two-dimensional position sensitive parallel-plate gas ionization chamber with scanned charge transfer readout. The scan readout method described here is based on the development of a new position-dependent charge transfer technique. It has been implemented by using gate strips perpendicularly oriented to the collector strips. This solution reduces considerably the number of electronic readout channels needed to cover large detector areas. The use of a 25 μm thick kapton etched circuit allows high charge transfer efficiency with a low gating voltage, consequently needing a very simple commutating circuit. The present prototype covers 8x8 cm 2 with a pixel size of 1.27x1.27 mm 2 . Depending on the intended use and beam characteristics a smaller effective pixel is feasible and larger active areas are possible. This detector can be used for X-ray or other continuous beam intensity profile monitoring

Charge transfer in pi-stacked systems including DNA

International Nuclear Information System (INIS)

Siebbeles, L.D.A.

2003-01-01

Charge migration in DNA is a subject of intense current study motivated by long-range detection of DNA damage and the potential application of DNA as a molecular wire in nanoscale electronic devices. A key structural element, which makes DNA a medium for long-range charge transfer, is the array of stacked base pairs in the interior of the double helix. The overlapping pi-orbitals of the nucleobases provide a pathway for motion of charge carriers generated on the stack. This 'pi-pathway' resembles the columnarly stacked macrocyclic cores in discotic materials such as triphenylenes. The structure of these pi-stacked systems is highly disordered with dynamic fluctuations occurring on picosecond to nanosecond time scales. Theoretical calculations, concerning the effects of structural disorder and nucleobase sequence in DNA, on the dynamics of charge carriers are presented. Electronic couplings and localization energies of charge carriers were calculated using density functional theory (DFT). Results for columnarly stacked triphenylenes and DNA nucleobases are compared. The results are used to provide insight into the factors that control the mobility of charge carriers. Further, experimental results on the site-selective oxidation of guanine nucleobases in DNA (hot spots for DNA damage) are analyzed on basis of the theoretical results

Ion-atom charge-transfer system for a heavy-ion-beam pumped laser

International Nuclear Information System (INIS)

Ulrich, A.; Gernhaeuser, R.; Kroetz, W.; Wieser, J.; Murnick, D.E.

1994-01-01

An Ar target to which Cs vapor could be added, excited by a pulsed beam of 100-MeV 32 S ions, was studied as a prototype ion-atom charge-transfer system for pumping short-wavelength lasers. Low-velocity Ar 2+ ions were efficiently produced; a huge increase in the intensity of the Ar II 4d-4p spectral lines was observed when Cs vapor was added to the argon. This observation is explained by a selective charge transfer of the Cs 6s electron into the upper levels of the observed transitions. A rate constant of (1.4±0.2)x10 -9 cm 3 /s for the transfer process was determined

CFD analysis of heat transfer in a vertical annular gas gap

International Nuclear Information System (INIS)

Borgohain, A.; Maheshwari, N.K.; Vijayan, P.K.

2011-01-01

Heat transfer analysis in a vertical annulus is carried out by using a CFD code TRIO-U. The results are used to understand heat transfer in the vertical annulus. An experimental study is taken from literature for the CFD analysis. The geometry of the test section of the experiment is simulated in TRIO-U. The operating conditions of the experiment are simulated by imposing appropriate boundary conditions. Three modes of the heat transfer, conduction, radiation and convection in the gas gap are considered in the analysis. From the analysis it is found that TRIO-U can successfully handle all modes heat transfer. The theoretical results for heat transfer have been compared with experimental data. This paper deals with the detailed CFD modelling and analysis. (author)

Dexter energy transfer pathways.

Science.gov (United States)

Skourtis, Spiros S; Liu, Chaoren; Antoniou, Panayiotis; Virshup, Aaron M; Beratan, David N

2016-07-19

Energy transfer with an associated spin change of the donor and acceptor, Dexter energy transfer, is critically important in solar energy harvesting assemblies, damage protection schemes of photobiology, and organometallic opto-electronic materials. Dexter transfer between chemically linked donors and acceptors is bridge mediated, presenting an enticing analogy with bridge-mediated electron and hole transfer. However, Dexter coupling pathways must convey both an electron and a hole from donor to acceptor, and this adds considerable richness to the mediation process. We dissect the bridge-mediated Dexter coupling mechanisms and formulate a theory for triplet energy transfer coupling pathways. Virtual donor-acceptor charge-transfer exciton intermediates dominate at shorter distances or higher tunneling energy gaps, whereas virtual intermediates with an electron and a hole both on the bridge (virtual bridge excitons) dominate for longer distances or lower energy gaps. The effects of virtual bridge excitons were neglected in earlier treatments. The two-particle pathway framework developed here shows how Dexter energy-transfer rates depend on donor, bridge, and acceptor energetics, as well as on orbital symmetry and quantum interference among pathways.

The influence of electric charge transferred during electro-mechanical reshaping on mechanical behavior of cartilage

Science.gov (United States)

Protsenko, Dimitry E.; Lim, Amanda; Wu, Edward C.; Manuel, Cyrus; Wong, Brian J. F.

2011-03-01

Electromechanical reshaping (EMR) of cartilage has been suggested as an alternative to the classical surgical techniques of modifying the shape of facial cartilages. The method is based on exposure of mechanically deformed cartilaginous tissue to a low level electric field. Electro-chemical reactions within the tissue lead to reduction of internal stress, and establishment of a new equilibrium shape. The same reactions offset the electric charge balance between collagen and proteoglycan matrix and interstitial fluid responsible for maintenance of cartilage mechanical properties. The objective of this study was to investigate correlation between the electric charge transferred during EMR and equilibrium elastic modulus. We used a finite element model based on the triphasic theory of cartilage mechanical properties to study how electric charges transferred in the electro-chemical reactions in cartilage can change its mechanical responses to step displacements in unconfined compression. The concentrations of the ions, the strain field and the fluid and ion velocities within the specimen subject to an applied mechanical deformation were estimated and apparent elastic modulus (the ratio of the equilibrium axial stress to the axial strain) was calculated as a function of transferred charge. The results from numerical calculations showed that the apparent elastic modulus decreases with increase in electric charge transfer. To compare numerical model with experimental observation we measured elastic modulus of cartilage as a function of electric charge transferred in electric circuit during EMR. Good correlation between experimental and theoretical data suggests that electric charge disbalance is responsible for alteration of cartilage mechanical properties.

Theoretical studies of charge transfer and proton transfer complex formation between 3,5-dinitrobenzic acid and 1,2-dimethylimidazole

Science.gov (United States)

Afroz, Ziya; Faizan, Mohd.; Alam, Mohammad Jane; Ahmad, Shabbir; Ahmad, Afaq

2018-05-01

Natural atomic charge analysis and molecular electrostatic potential (MEP) surface analysis of hydrogen bonded charge transfer (HBCT) and proton transfer (PT) complex of 3,5-dinitrobenzoic acid (DNBA) and 1,2-dimethylimidazole (DMI) have been investigated by theoretical modelling using widely employed DFT/B3LYP/6-311G(d,p) level of theory. Along with this analysis, Hirshfeld surface study of the intermolecular interactions and associated 2D finger plot for reported PT complex between DNBA and DMI have been explored.

Charge transfer in gas electron multipliers

Energy Technology Data Exchange (ETDEWEB)

Ottnad, Jonathan; Ball, Markus; Ketzer, Bernhard; Ratza, Viktor; Razzaghi, Cina [HISKP, Bonn University, Nussallee 14-16, D-53115 Bonn (Germany)

2015-07-01

In order to efficiently employ a Time Projection Chamber (TPC) at interaction rates higher than ∝1 kHz, as foreseen e.g. in the ALICE experiment (CERN) and at CB-ELSA (Bonn), a continuous operation and readout mode is required. A necessary prerequisite is to minimize the space charge coming from the amplification system and to maintain an excellent spatial and energy resolution. Unfortunately these two goals can be in conflict to each other. Gas Electron Multipliers (GEM) are one candidate to fulfill these requirements. It is necessary to understand the processes within the amplification structure to find optimal operation conditions. To do so, we measure the charge transfer processes in and between GEM foils with different geometries and field configurations, and use an analytical model to describe the results. This model can then be used to predict and optimize the performance. The talk gives the present status of the measurements and describes the model.

Band gap opening of bilayer graphene by F4-TCNQ molecular doping and externally applied electric field.

Science.gov (United States)

Tian, Xiaoqing; Xu, Jianbin; Wang, Xiaomu

2010-09-09

The band gap opening of bilayer graphene with one side surface adsorption of F4-TCNQ is reported. F4-TCNQ doped bilayer graphene shows p-type semiconductor characteristics. With a F4-TCNQ concentration of 1.3 x 10(-10) mol/cm(2), the charge transfer between each F4-TCNQ molecule and graphene is 0.45e, and the built-in electric field, E(bi), between the graphene layers could reach 0.070 V/A. The charge transfer and band gap opening of the F4-TCNQ-doped graphene can be further modulated by an externally applied electric field (E(ext)). At 0.077 V/A, the gap opening at the Dirac point (K), DeltaE(K) = 306 meV, and the band gap, E(g) = 253 meV, are around 71% and 49% larger than those of the pristine bilayer under the same E(ext).

The charge transfer characteristic of tetraphenylporphyrin iron chloride Langmuir–Blodgett films

International Nuclear Information System (INIS)

Du, Y.; Li, Z.H.; Qi, P.; Wang, F.; Liu, D.

2013-01-01

The charge transfer characteristic of tetraphenylporphyrin iron (III) chloride (FeP) Langmuir–Blodgett (LB) films on the surface of the ITO glass electrode was reported. When the cyclic voltammetry (CV) scanning was running, the charge transfer characteristic was controlled by the oxidation–reduction process of Fe(III)/Fe(II). The charge transfer characteristic was related to the following factors: the cross-sectional area, relative to the electrode, of FeP as the electron donor (or acceptor). The greater the cross-sectional area of the aggregation of FeP as the electron donor (or acceptor) was, the larger the number of the donated (or accepted) electrons was. The projected area of the cross-section on the ITO electrode. The greater the projected area was, the larger the number of the donated (or accepted) electrons was. The distance between the center of the electron donor (or acceptor) of FeP and the surface of ITO electrode. The smaller the distance was, the greater the rate of donating (or accepting) electrons was. The monolayer coverage, which formed because of the FeP lying on the ITO surface in the form of the monomer and aggregate, was more sensitive to detect oxygen

Failures of TDDFT in describing the lowest intramolecular charge-transfer excitation in para-nitroanilin

DEFF Research Database (Denmark)

Eriksen, J.J.; Sauer, S.P.A.; Mikkelsen, K.V.

2013-01-01

We investigate the failure of Time{Dependent Density Functional Theory (TDDFT) with the CAM{B3LYP exchange{correlation (xc) functional coupled to the Polarizable Embedding (PE) scheme (PE-CAM-B3LYP) in reproducing the solvatochromic shift of the lowest intense charge{transfer excitation in para...... the electric dipole moments in the gas phase and for 100 solvent congurations. We find that CAM-B3LYP overestimates the amount of charge separation inherent in the ground state and TDDFT/CAM-B3LYP drastically underestimates this amount in the excited charge-transfer state. As the errors in the solvatochromatic...... to benchmark results of TDDFT calculations with CAM-B3LYP for intramolecular charge{transfer excitations in molecular systems similar to pNA against higher{level ab initio wave function methods, like, e.g., CCSD, prior to their use. Using the calculated change in dipole moment upon excitation as a measure...

Verification of Heat and Mass Transfer Closures in Industrial Scale Packed Bed Reactor Simulations

Directory of Open Access Journals (Sweden)

Arpit Singhal

2018-03-01

Full Text Available Particle-resolved direct numerical simulation (PR-DNS is known to provide an accurate detailed insight into the local flow phenomena in static particle arrays. Most PR-DNS studies in literature do not account for reactions taking place inside the porous particles. In this study, PR-DNS is performed for catalytic reactions inside the particles using the multifluid approach where all heat and mass transfer phenomena are directly resolved both inside and outside the particles. These simulation results are then used to verify existing 1D model closures from literature over a number of different reaction parameters including different reaction orders, multiple reactions and reactants, interacting reactions, and reactions involving gas volume generation/consumption inside the particle. Results clearly showed that several modifications to existing 1D model closures are required to reproduce PR-DNS results. The resulting enhanced 1D model was then used to accurately simulate steam methane reforming, which includes all of the aforementioned reaction complexities. The effect of multiple reactants was found to be the most influential in this case.

A study of the flow boiling heat transfer in an annular heat exchanger with a mini gap

Directory of Open Access Journals (Sweden)

Musiał Tomasz

2017-01-01

Full Text Available In this paper the research on flow boiling heat transfer in an annular mini gap was discussed. A one- dimensional mathematical approach was proposed to describe stationary heat transfer in the gap. The mini gap 1 mm wide was created between a metal pipe with enhanced exterior surface and an external tempered glass pipe positioned along the same axis. The experimental test stand consists of several systems: the test loop in which distilled water circulates, the data and image acquisition system and the supply and control system. Known temperature distributions of the metal pipe with enhanced surface and of the working fluid helped to determine, from the Robin boundary condition, the local heat transfer coefficients at the fluid - heated surface contact. In the proposed mathematical model it is assumed that the cylindrical wall is a planar multilayer wall. The numerical results are presented on a chart as function of the heat transfer coefficient along the length of the mini gap.

A low-spin Fe(III) complex with 100-ps ligand-to-metal charge transfer photoluminescence

DEFF Research Database (Denmark)

Chabera, Pavel; Liu, Yizhu; Prakash, Om

2017-01-01

Transition-metal complexes are used as photosensitizers(1), in light-emitting diodes, for biosensing and in photocatalysis(2). A key feature in these applications is excitation from the ground state to a charge-transfer state(3,4); the long charge-transfer-state lifetimes typical for complexes...

Photoinduced charge transfer within polyaniline-encapsulated quantum dots decorated on graphene.

Science.gov (United States)

Nguyen, Kim Truc; Li, Dehui; Borah, Parijat; Ma, Xing; Liu, Zhaona; Zhu, Liangliang; Grüner, George; Xiong, Qihua; Zhao, Yanli

2013-08-28

A new method to enhance the stability of quantum dots (QDs) in aqueous solution by encapsulating them with conducting polymer polyaniline was reported. The polyaniline-encapsulated QDs were then decorated onto graphene through π-π interactions between graphene and conjugated polymer shell of QDs, forming stable polyaniline/QD/graphene hybrid. A testing electronic device was fabricated using the hybrid in order to investigate the photoinduced charge transfer between graphene and encapsulated QDs within the hybrid. The charge transfer mechanism was explored through cyclic voltammetry and spectroscopic studies. The hybrid shows a clear response to the laser irradiation, presenting a great advantage for further applications in optoelectronic devices.

Cost-Effectiveness Comparison of Coupler Designs of Wireless Power Transfer for Electric Vehicle Dynamic Charging

Directory of Open Access Journals (Sweden)

Weitong Chen

2016-11-01

Full Text Available This paper presents a cost-effectiveness comparison of coupler designs for wireless power transfer (WPT, meant for electric vehicle (EV dynamic charging. The design comparison of three common types of couplers is first based on the raw material cost, output power, transfer efficiency, tolerance of horizontal offset, and flux density. Then, the optimal cost-effectiveness combination is selected for EV dynamic charging. The corresponding performances of the proposed charging system are compared and analyzed by both simulation and experimentation. The results verify the validity of the proposed dynamic charging system for EVs.

Gap Resolution

Energy Technology Data Exchange (ETDEWEB)

2017-04-25

Gap Resolution is a software package that was developed to improve Newbler genome assemblies by automating the closure of sequence gaps caused by repetitive regions in the DNA. This is done by performing the follow steps:1) Identify and distribute the data for each gap in sub-projects. 2) Assemble the data associated with each sub-project using a secondary assembler, such as Newbler or PGA. 3) Determine if any gaps are closed after reassembly, and either design fakes (consensus of closed gap) for those that closed or lab experiments for those that require additional data. The software requires as input a genome assembly produce by the Newbler assembler provided by Roche and 454 data containing paired-end reads.

Plasma effect on tunnelling, charge transfer and transient quasimolecular states

International Nuclear Information System (INIS)

Fisher, D V

2003-01-01

The influence of a dense plasma environment on electron tunnelling between two ion potential wells in collectivized states and in charge-transfer collisions is studied. We show that the tunnelling probabilities in dilute plasma (in a close ion-ion collision) and in dense plasma differ strongly. The difference is due to the mixing between Stark components of donor-ion energy levels, caused by the field of spectator ions in a dense plasma. The mixing is determined by an angle α between the nearest-neighbour ion field and the total electric field acting on the donor ion. In close ion-ion binary collisions the mixing may be considered weak. However, for most plasma ions charge transfer, electron state collectivization and transient quasimolecule formation are strongly affected by the field of spectator ions. We derive approximate analytical expressions for the distribution function of α in an ideal plasma and perform molecular dynamics simulations to find the distribution function of α in both ideal and nonideal plasmas. Both α-dependent and average mixing coefficients are determined. We have found that the mixing is strong, even in ideal plasmas, and increases further with an increase in plasma nonideality. It is shown that there is no resonant charge transfer in dense plasmas. The applicability of a transient 'dicenter' quasimolecule model for dense plasmas is discussed

Transfer of energy or charge between quasi-zero-dimensional nanostructures

Czech Academy of Sciences Publication Activity Database

Král, Karel; Menšík, Miroslav

2016-01-01

Roč. 45, č. 4 (2016), s. 243-255 ISSN 2332-4309 R&D Projects: GA ČR(CZ) GA14-05053S; GA MŠk(CZ) LD14011; GA MŠk LH12236 Institutional support: RVO:68378271 ; RVO:61389013 Keywords : charge transfer * electron-phonon interaction * energy transfer * nanostructures * quantum dots Subject RIV: BM - Solid Matter Physics ; Magnetism; CD - Macromolecular Chemistry (UMCH-V) Impact factor: 0.171, year: 2016

Modeling charge transfer at organic donor-acceptor semiconductor interfaces

NARCIS (Netherlands)

Cakir, Deniz; Bokdam, Menno; de Jong, Machiel Pieter; Fahlman, M.; Brocks, G.

2012-01-01

We develop an integer charge transfer model for the potential steps observed at interfaces between donor and acceptor molecular semiconductors. The potential step can be expressed as the difference between the Fermi energy pinning levels of electrons on the acceptor material and holes on the donor

Parallel-plate submicron gap formed by micromachined low-density pillars for near-field radiative heat transfer

International Nuclear Information System (INIS)

Ito, Kota; Miura, Atsushi; Iizuka, Hideo; Toshiyoshi, Hiroshi

2015-01-01

Near-field radiative heat transfer has been a subject of great interest due to the applicability to thermal management and energy conversion. In this letter, a submicron gap between a pair of diced fused quartz substrates is formed by using micromachined low-density pillars to obtain both the parallelism and small parasitic heat conduction. The gap uniformity is validated by the optical interferometry at four corners of the substrates. The heat flux across the gap is measured in a steady-state and is no greater than twice of theoretically predicted radiative heat flux, which indicates that the parasitic heat conduction is suppressed to the level of the radiative heat transfer or less. The heat conduction through the pillars is modeled, and it is found to be limited by the thermal contact resistance between the pillar top and the opposing substrate surface. The methodology to form and evaluate the gap promotes the near-field radiative heat transfer to various applications such as thermal rectification, thermal modulation, and thermophotovoltaics

Parallel-plate submicron gap formed by micromachined low-density pillars for near-field radiative heat transfer

Energy Technology Data Exchange (ETDEWEB)

Ito, Kota, E-mail: kotaito@mosk.tytlabs.co.jp [Toyota Central Research and Development Laboratories, Nagakute, Aichi 480-1192 (Japan); Research Center for Advanced Science and Technology (RCAST), The University of Tokyo, Komaba, Meguro-ku, Tokyo 153-8904 (Japan); Miura, Atsushi; Iizuka, Hideo [Toyota Central Research and Development Laboratories, Nagakute, Aichi 480-1192 (Japan); Toshiyoshi, Hiroshi [Research Center for Advanced Science and Technology (RCAST), The University of Tokyo, Komaba, Meguro-ku, Tokyo 153-8904 (Japan)

2015-02-23

Near-field radiative heat transfer has been a subject of great interest due to the applicability to thermal management and energy conversion. In this letter, a submicron gap between a pair of diced fused quartz substrates is formed by using micromachined low-density pillars to obtain both the parallelism and small parasitic heat conduction. The gap uniformity is validated by the optical interferometry at four corners of the substrates. The heat flux across the gap is measured in a steady-state and is no greater than twice of theoretically predicted radiative heat flux, which indicates that the parasitic heat conduction is suppressed to the level of the radiative heat transfer or less. The heat conduction through the pillars is modeled, and it is found to be limited by the thermal contact resistance between the pillar top and the opposing substrate surface. The methodology to form and evaluate the gap promotes the near-field radiative heat transfer to various applications such as thermal rectification, thermal modulation, and thermophotovoltaics.

Charge transfer in photorechargeable composite films of TiO2 and polyaniline

Science.gov (United States)

Nomiyama, Teruaki; Sasabe, Kenichi; Sakamoto, Kenta; Horie, Yuji

2015-07-01

A photorechargeable battery (PRB) is a photovoltaic device having an energy storage function in a single cell. The photoactive electrode of PRB is a bilayer film consisting of bare porous TiO2 and a TiO2-polyaniline (PANi) mixture that work as a photovoltaic current generator and an electrochemical energy storage by ion dedoping, respectively. To study the charge transfer between TiO2 and PANi, the photorechargeable quantum efficiency QE ([electron count on discharge]/[incident photon count on photocharge]) was measured by varying the thickness LS of the TiO2-PANi mixture. The quantum efficiency QEuv for UV photons had a maximum of ˜7% at LS ˜ 7 µm. The time constant τTP for the charge transfer was about 10-1 s, which was longer ten times or more than the lifetime of excited electrons within TiO2. These facts reveal that the main rate-limiting factor in the photocharging process is the charge transfer between TiO2 and PANi.

Heat transfer from the evaporator outlet to the charge of thermostatic expansion valves

DEFF Research Database (Denmark)

Langmaack, Lasse Nicolai; Knudsen, Hans-Jørgen Høgaard

2006-01-01

outlet with a special mounting strap. The heat transfer is quite complex because it takes place both directly through the contact points between bulb and pipe and indirectly through the mounting strap The TXV has to react to temperature changes at the evaporator outlet. Therefore, the dynamic behavior...... of the valve (and thereby the whole refrigeration system) depends greatly on the heat transfer between the evaporator outlet tube and the charge in the bulb. In this paper a model for the overall heat transfer between the pipe and the charge is presented. Geometrical data and material properties have been kept...... been found to predict the time constant for the temperature development in the bulb within 1-10 %. Furthermore it has been found that app. 20% of the heat transfer takes place trough the mounting strap....

Evidence for charge transfer in Bi-based superconductors studied by positron annihilation

International Nuclear Information System (INIS)

Tang, Z.; Wang, S.J.; Gao, X.H.; Ce, G.C.; Zhao, Z.X.

1993-01-01

We have measured Doppler-broadening annihilation radiation (DBAR) spectra and positron lifetimes in normal and superconducting states for three kinds of Bi-based superconductors: Bi2212, Pb-doped Bi2223, Pb- and F-doped Bi2223. The difference spectra after deconvolution between two states show a sharpening effect with increasing temperature; the F-doped sample has the greatest amplitude in difference spectra but nearly the same positron lifetimes as the Pb-doped sample. The results are interpreted in terms of charge transfer between the Cu-O and Bi-O planes. The role of oxygen defects in charge transfer is discussed. (orig.)

Charge-exchange breakup of the deuteron with the production of two protons and spin structure of the amplitude of the nucleon charge transfer reaction

International Nuclear Information System (INIS)

Glagolev, V.V.; Lyuboshits, V.L.; Lyuboshits, V.V.; Piskunov, N.M.

1999-01-01

In the framework of the impulse approximation, the relation between the effective cross section of the charge-exchange breakup of a fast deuteron d + a → (pp) + b and the effective cross section of the charge transfer process n + a → p + b is discussed. In doing so, the effects of the proton identity (Fermi-statistics) and of the Coulomb and strong interactions of protons in the final state are taken into account. The distribution over relative momenta of the protons, produced in the charge-exchange process d + p → (pp) + n in the forward direction, is investigated. At the transfer momenta being close to zero the effective cross section of the charge-exchange breakup of a fast deuteron, colliding with the proton target, is determined only by the spin-flip part of the amplitude of the charge transfer reaction n + p → p + n at the zero angle. It is shown that the study of the process d + p → (pp) + n in a beam of the polarized (aligned) deuterons allows one, in principle, to separate two spin-dependent terms in the amplitude of the charge transfer reaction n + p → p + n, one of which does not conserve and the other one conserves the projection of the nucleon spin onto the direction of momentum at the transition of the neutron into the proton

Charge ordering and opening of spin gap in NaV2O5

NARCIS (Netherlands)

Mostovoy, M.V.; Khomskii, D.I.

1999-01-01

We argue that the origin of the phase transition in quasi-one-dimensional antiferromagnet NaV2O5 is not the spin-Peierls (SP) instability, but a charge ordering. The opening of the spin gap and the lattice dimerization, characteristic for the spin-Peierls systems, in NaV2O5 result from the interplay

Low-Energy Charge Transfer in Multiply-Charged Ion-Atom Collisions Studied with the Combined SCVB-MOCC Approach

OpenAIRE

Cooper, D. L.; Stancil, P. C.; Turner, A. R.; Wang, J. G.; Clarke, N. J.; Zygelman, B.

2002-01-01

A survey of theoretical studies of charge transfer involving collisions of multiply-charged ions with atomic neutrals (H and He) is presented. The calculations utilized the quantum-mechanical molecular-orbital close-coupling (MOCC) approach where the requisite potential curves and coupling matrix elements have been obtained with the spin-coupled valence bond (SCVB) method. Comparison is made among various collision partners, for equicharged systems, where it is illustrated that even for total...

Possible charge analogues of spin transfer torques in bulk superconductors

Science.gov (United States)

Garate, Ion

2014-03-01

Spin transfer torques (STT) occur when electric currents travel through inhomogeneously magnetized systems and are important for the motion of magnetic textures such as domain walls. Since superconductors are easy-plane ferromagnets in particle-hole (charge) space, it is natural to ask whether any charge duals of STT phenomena exist therein. We find that the superconducting analogue of the adiabatic STT vanishes in a bulk superconductor with a momentum-independent order parameter, while the superconducting counterpart of the nonadiabatic STT does not vanish. This nonvanishing superconducting torque is induced by heat (rather than charge) currents and acts on the charge (rather than spin) degree of freedom. It can become significant in the vicinity of the superconducting transition temperature, where it generates a net quasiparticle charge and alters the dispersion and linewidth of low-frequency collective modes. This work has been financially supported by Canada's NSERC.

Charge-transfer complexes and their role in exciplex emission and near-infrared photovoltaics.

Science.gov (United States)

Ng, Tsz-Wai; Lo, Ming-Fai; Fung, Man-Keung; Zhang, Wen-Jun; Lee, Chun-Sing

2014-08-20

Charge transfer and interactions at organic heterojunctions (OHJs) are known to have critical influences on various properties of organic electronic devices. In this Research News article, a short review is given from the electronic viewpoint on how the local molecular interactions and interfacial energetics at P/N OHJs contribute to the recombination/dissociation of electron-hole pairs. Very often, the P-type materials donate electrons to the N-type materials, giving rise to charge-transfer complexes (CTCs) with a P(δ+) -N(δ-) configuration. A recently observed opposite charge-transfer direction in OHJs is also discussed (i.e., N-type material donates electrons to P-type material to form P(δ-) -N(δ+) ). Recent studies on the electronic structures of CTC-forming material pairs are also summarized. The formation of P(δ-) -N(δ+) -type CTCs and their correlations with exciplex emission are examined. Furthermore, the potential applications of CTCs in NIR photovoltaic devices are reviewed. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Deflection effects and charge transfer in inner-shell vacancy production

International Nuclear Information System (INIS)

Swafford, G.L.

1978-01-01

A method used in the calculation of inner shell ionization in asymmetric ion-atom collisions is extended to include projectile deflection effects and charge transfer to the projectile. Work is done in an independent electron model (Hartree-Fock) for the target, and the interaction is treated with the projectile as a time-dependent perturbation of the system. It is shown tht the time-dependent problem can be solved for the projectile moving along the classical hyperbolic trajectory that results from the nuclear repulsion. The method is very efficient due to the utilization the target-centered expansion of the system wave function. This means that all the required matrix elements can be pretabulated and are then available for use at all impact parameters. The method is first applied to the impact-parameter dependence of K-shell ionization by protons incident upon copper in the energy range 0.5 to 2 MeV. Excellent agreement with the experiments of Andersen et al., is found at the lower energy. Less satisfactory agreement is obtained in the higher energy region. Next the projectile is considered to move in a straight line path with constant velocity, and extend the method to include charge transfer between the target inner shells and the K-shell of the projectile. A critical feature of the results is the recognition of the importance of target continuum states of energy approximately equal to the kinetic energy (in the target frame) of the electron on the projectile. An approach is developed to properly include such resonance states in our pseudostate calculation. Selected numerical results are presented to illustrate the method and to demonstrate the projectile energy and nuclear charge dependence of the charge transfer cross sections

Photosynthesis Revisited: Optimization of Charge and Energy Transfer in Quantum Materials

Science.gov (United States)

Gabor, Nathaniel

2014-03-01

The integration of new nano- and molecular-scale quantum materials into ultra-efficient energy harvesting devices presents significant scientific challenges. Of the many challenges, the most difficult is achieving high photon-to-electron conversion efficiency while maintaining broadband absorption. Due to exciton effects, devices composed of quantum materials may allow near-unity optical absorption efficiency yet require the choice of precisely one fundamental energy (HOMO-LUMO gap). To maximize absorption, the simplest device would absorb at the peak of the solar spectrum, which spans the visible wavelengths. If the peak of the solar spectrum spans the visible wavelengths, then why are terrestrial plants green? Here, I discuss a physical model of photosynthetic absorption and photoprotection in which the cell utilizes active feedback to optimize charge and energy transfer, thus maximizing stored energy rather than absorption. This model, which addresses the question of terrestrial greenness, is supported by several recent results that have begun to unravel the details of photoprotection in higher plants. More importantly, this model indicates a novel route for the design of next-generation energy harvesting systems based on nano- and molecular-scale quantum materials.

Theoretical studies of optics and charge transport in organic conducting oligomers and polymers: Rational design of improved transparent and conducting polymers

Science.gov (United States)

Hutchison, Geoffrey Rogers

Theoretical studies on a variety of oligo- and polyheterocycles elucidate their optical and charge transport properties, suggesting new, improved transparent conductive polymers. First-principles calculations provide accurate methodologies for predicting both optical band gaps of neutral and cationic oligomers and intrinsic charge transfer rates. Multidimensional analysis reveals important motifs in chemical tailorability of oligoheterocycle optical and charge transport properties. The results suggest new directions for design of novel materials. Using both finite oligomer and infinite polymer calculations, the optical band gaps in polyheterocycles follow a modified particle-in-a-box formalism, scaling approximately as 1/N (where N is the number of monomer units) in short chains, saturating for long chains. Calculations demonstrate that band structure changes upon heteroatom substitution, (e.g., from polythiophene to polypyrrole) derive from heteroatom electron affinity. Further investigation of chemical variability in substituted oligoheterocycles using multidimensional statistics reveals the interplay between heteroatom and substituent in correlations between structure and redox/optical properties of neutral and cationic species. A linear correlation between band gaps of neutral and cationic species upon oxidation of conjugated oligomers, shows redshifts of optical absorption for most species and blueshifts for small band gap species. Interstrand charge-transport studies focus on two contributors to hopping-style charge transfer rates: internal reorganization energy and the electronic coupling matrix element. Statistical analysis of chemical variability of reorganization energies in oligoheterocycles proves the importance of reorganization energy in determining intrinsic charge transfer rates (e.g., charge mobility in unsubstituted oligothiophenes). Computed bandwidths across several oligothiophene crystal packing motifs show similar electron and hole bandwidths

Effect of Molecular Packing and Charge Delocalization on the Nonradiative Recombination of Charge-Transfer States in Organic Solar Cells

KAUST Repository

Chen, Xiankai

2016-09-05

In organic solar cells, a major source of energy loss is attributed to nonradiative recombination from the interfacial charge transfer states to the ground state. By taking pentacene–C60 complexes as model donor–acceptor systems, a comprehensive theoretical understanding of how molecular packing and charge delocalization impact these nonradiative recombination rates at donor–acceptor interfaces is provided.

Improving radiation hardness in space-based Charge-Coupled Devices through the narrowing of the charge transfer channel

Science.gov (United States)

Hall, D. J.; Skottfelt, J.; Soman, M. R.; Bush, N.; Holland, A.

2017-12-01

Charge-Coupled Devices (CCDs) have been the detector of choice for imaging and spectroscopy in space missions for several decades, such as those being used for the Euclid VIS instrument and baselined for the SMILE SXI. Despite the many positive properties of CCDs, such as the high quantum efficiency and low noise, when used in a space environment the detectors suffer damage from the often-harsh radiation environment. High energy particles can create defects in the silicon lattice which act to trap the signal electrons being transferred through the device, reducing the signal measured and effectively increasing the noise. We can reduce the impact of radiation on the devices through four key methods: increased radiation shielding, device design considerations, optimisation of operating conditions, and image correction. Here, we concentrate on device design operations, investigating the impact of narrowing the charge-transfer channel in the device with the aim of minimising the impact of traps during readout. Previous studies for the Euclid VIS instrument considered two devices, the e2v CCD204 and CCD273, the serial register of the former having a 50 μm channel and the latter having a 20 μm channel. The reduction in channel width was previously modelled to give an approximate 1.6× reduction in charge storage volume, verified experimentally to have a reduction in charge transfer inefficiency of 1.7×. The methods used to simulate the reduction approximated the charge cloud to a sharp-edged volume within which the probability of capture by traps was 100%. For high signals and slow readout speeds, this is a reasonable approximation. However, for low signals and higher readout speeds, the approximation falls short. Here we discuss a new method of simulating and calculating charge storage variations with device design changes, considering the absolute probability of capture across the pixel, bringing validity to all signal sizes and readout speeds. Using this method, we

Integer charge transfer at the tetrakis(dimethylamino)ethylene/Au interface

DEFF Research Database (Denmark)

Lindell, L.; Unge, Mikael; Osikowicz, W.

2008-01-01

In organic-based electronics, interfacial properties have a profound impact on device performance. The lineup of energy levels is usually dependent on interface dipoles, which may arise from charge transfer reactions. In many applications, metal-organic junctions are prepared under ambient...

Intrinsic localized gap states in IGZO and its parent single crystalline TCOs

Energy Technology Data Exchange (ETDEWEB)

Schmeißer, D.; Haeberle, J.

2016-03-31

We report on the X-ray absorption data for Indium–Gallium–Zink–Oxide thin films, amorphous ZnO films, amorphous SnO{sub x} films, and single crystalline In{sub 2}O{sub 3}, Ga{sub 2}O{sub 3}, ZnO, and SnO{sub 2} data. These absorption data probe the empty conduction band states explicitly. Also they allow for an elemental assignment using resonant excitation to derive the contributions of each metal ion. We find that the lowest states appear right at the Fermi energy and result from configuration interaction induced charge transfer states which we consider as intrinsic gap states. - Highlights: • We identify contributions of localized configuration interaction induced gap states. • Auger profiles taken on metal absorption edges show metallic density of states around E{sub F}. • D-shell opening leads to a charge-transfer state involving metallic d-states.

Impact of Different Standard Type A7A Drum Closure-Ring Practices on Gasket Contraction and Bolt Closure Distance– 15621

Energy Technology Data Exchange (ETDEWEB)

Ketusky, Edward [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Blanton, Paul [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Bobbitt, John H. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

2015-03-11

The Department of Energy, the Savannah River National Laboratory, several manufacturers of specification drums, and the United States Department of Transportation (DOT) are collaborating in the development of a guidance document for DOE contractors and vendors who wish to qualify containers to DOT 7A Type A requirements. Currently, the effort is focused on DOT 7A Type A 208-liter (55-gallons) drums with a standard 12-gauge bolted closure ring. The U.S. requirements, contained in Title 49, Part 178.350 “Specification 7A; general packaging, Type A specifies a competent authority review of the packaging is not required for the transport of (Class 7) radioactive material containing less than Type A quantities of radioactive material. For Type AF drums, a 4 ft. regulatory free drop must be performed, such that the drum “suffers maximum damage.” Although the actual orientation is not defined by the specification, recent studies suggest that maximum damage would result from a shallow angle top impact, where kinetic energy is transferred to the lid, ultimately causing heavy damage to the lid, or even worse, causing the lid to come off. Since each vendor develops closure recommendations/procedures for the drums they manufacture, key parameters applied to drums during closing vary based on vendor. As part of the initial phase of the collaboration, the impact of the closure variants on the ability of the drum to suffer maximum damage is investigated. Specifically, closure testing is performed varying: 1) the amount of torque applied to the closure ring bolt; and, 2) stress relief protocol, including: a) weight of hammer; and, b) orientation that the hammer hits the closure ring. After closure, the amount of drum lid gasket contraction and the distance that the closure bolt moves through the closure ring is measured.

Military Base Closures: Updated Status of Prior Base Realignments and Closures

Science.gov (United States)

As the Department of Defense (DOD) prepares for the 2005 base realignment and closure (BRAC) round, questions continue to be raised about the transfer and environmental cleanup of unneeded property arising from the prior four BRAC rounds and their impact on cost and savings and on local economies.

The tight binding model study of the role of band filling on the charge gap in graphene-on-substrate in paramagnetic state

Science.gov (United States)

Panda, Rudrashish; Sahu, Sivabrata; Rout, G. C.

2017-05-01

We communicate here a tight binding theoretical model study of the band filling effect on the charge gap in graphene-on-substrate. The Hamiltonian consists of nearest neighbor electron hopping and substrate induced gap. Besides this the Coulomb interaction is considered here within mean-field approximation in the paramagnetic limit. The electron occupancies at two sublattices are calculated by Green's function technique and are solved self consistently. Finally the charge gap i.e. Δ ¯=U [ - ] is calculated and computed numerically. The results are reported.

Charge transfer state in DBP:C70 organic solar cells

DEFF Research Database (Denmark)

Sherafatipour, Golenaz; Benduhn, Johannes; Spoltore, Donato

-acceptor interface via delocalized charge-transfer (CT) states, which represents an intermediate state between the exciton dissociation and recombination back to the ground state. In this work we perform the electroluminescence (EL) created by bimolecular free career recombination and sensitive external quantum...

Charge transfer and partial pinning at the contacts as the origin of a double dip in the transfer characteristics of graphene-based field-effect transistors

International Nuclear Information System (INIS)

Di Bartolomeo, Antonio; Giubileo, Filippo; Santandrea, Salvatore; Romeo, Francesco; Citro, Roberta; Schroeder, Thomas; Lupina, Grzegorz

2011-01-01

We discuss the origin of an additional dip other than the charge neutrality point observed in the transfer characteristics of graphene-based field-effect transistors with a Si/SiO 2 substrate used as the back-gate. The double dip is proved to arise from charge transfer between the graphene and the metal electrodes, while charge storage at the graphene/SiO 2 interface can make it more evident. Considering a different Fermi energy from the neutrality point along the channel and partial charge pinning at the contacts, we propose a model which explains all the features observed in the gate voltage loops. We finally show that the double dip enhanced hysteresis in the transfer characteristics can be exploited to realize graphene-based memory devices.

Coupled quantum treatment of vibrationally inelastic and vibronic charge transfer in proton-O2 collisions

International Nuclear Information System (INIS)

Gianturco, F.A.; Palma, A.; Semprini, E.; Stefani, F.; Baer, M.

1990-01-01

A three-dimensional quantum-mechanical study of vibrational, state-resolved differential cross sections (DCS) for the direct inelastic and for the charge-transfer scattering channels has been carried out for the H + +O 2 system. The collision energy considered was E c.m. =23.0 eV, which is the same as that examined by Noll and Toennies in their experiments [J. Chem. Phys. 85, 3313 (1986)]. The scattering treatment employed was the charge-transfer infinite-order sudden approximation (CT IOSA) with the vibrational states correctly expanded over the relevant adiabatic basis for each of the two electronic channels. The state-to-state DCS are found to follow closely the behavior of the experimental quantities, both in the inelastic and the charge-transfer channels. Moreover, a careful comparison between the measured relative probabilities and computed values allows us to test in minute detail the efficiency of the scattering model and the reliability of the potential-energy surfaces employed. It is found that vibrational energy transfer is overestimated in the vibrational inelastic channels while in the charge-transfer inelastic channels the same energy transfer is slightly underestimated by the calculations. The total flux distribution, however, is found to be in very good accord with experiments. Angular distributions are also well reproduced both by the DCS and by the average energy-transfer values. The study of some of the CT IOSA quantities also allows us to establish clearly the importance of nonadiabatic transitions in enhancing vibrational inelasticity in the present system

Radiative heat transfer exceeding the blackbody limit between macroscale planar surfaces separated by a nanosize vacuum gap

Science.gov (United States)

Bernardi, Michael P.; Milovich, Daniel; Francoeur, Mathieu

2016-09-01

Using Rytov's fluctuational electrodynamics framework, Polder and Van Hove predicted that radiative heat transfer between planar surfaces separated by a vacuum gap smaller than the thermal wavelength exceeds the blackbody limit due to tunnelling of evanescent modes. This finding has led to the conceptualization of systems capitalizing on evanescent modes such as thermophotovoltaic converters and thermal rectifiers. Their development is, however, limited by the lack of devices enabling radiative transfer between macroscale planar surfaces separated by a nanosize vacuum gap. Here we measure radiative heat transfer for large temperature differences (~120 K) using a custom-fabricated device in which the gap separating two 5 × 5 mm2 intrinsic silicon planar surfaces is modulated from 3,500 to 150 nm. A substantial enhancement over the blackbody limit by a factor of 8.4 is reported for a 150-nm-thick gap. Our device paves the way for the establishment of novel evanescent wave-based systems.

Classical/quantum correspondence in state selective charge transfer and excitation reactions involving highly charged ions and hydrogen

International Nuclear Information System (INIS)

Purkait, M

2009-01-01

State selective charge transfer and excitation cross sections for collisions of Ne q+ (q = 1-10) with atomic hydrogen are calculated within the framework of Classical Trajectory Monte Carlo (CTMC) method and Boundary Corrected Continuum Intermediate State (BCCIS) approximation.

A schematic model for energy and charge transfer in the chlorophyll complex

DEFF Research Database (Denmark)

Bohr, Henrik; Malik, F.B.

2011-01-01

A theory for simultaneous charge and energy transfer in the carotenoid-chlorophyll-a complex is presented here and discussed. The observed charge transfer process in these chloroplast complexes is reasonably explained in terms of this theory. In addition, the process leads to a mechanism to drive...... an electron in a lower to a higher-energy state, thus providing a mechanism for the ejection of the electron to a nearby molecule (chlorophyll) or into the environment. The observed lifetimes of the electronically excited states are in accord/agreement with the investigations of Sundström et al....... and are in the range of pico-seconds and less. The change in electronic charge distribution in internuclear space as the system undergoes an electronic transition to a higher-energy state could, under appropriate physical conditions, lead to oscillating dipoles capable of transmitting energy from the carotenoid-chlorophylls...

Temperature dependence of positronium reactivities with charge transfer molecules in bilayer membranes

International Nuclear Information System (INIS)

Jean, Y.C.; Yu, C.; Wang, Y.Y.; Yeh, Y.Y.

1984-01-01

Rate constants for positronium atoms reacting chemically with charge-transfer molecules such as p-benzoquinone, nitrobenzene, and coenzyme Q-10 in a model bilayer membrane, dipalmitoylphosphatidylcholine (DPPC), have been measured at temperatures between 23 and 65 0 C. A strong variation of the positronium chemical reactivities, k/sub Ps/ was observed in these systems: k/sub Ps/ increases with increasing temperature until the pretransition temperature of the membrane reaches a maximum value near the main transition temperature and decreases at temperatures higher than the main transition temperature. This variation is interpreted in terms of fluidity and permeability changes associated with the phase transitions of membranes and in terms of charge-transfer-complex formation between the solubilized molecules and the polar head of the membrane. These results demonstrate that positronium and its annihilation characteristics can be employed to investigate charge transport phenomena and microstructural changes of real biological membranes

Evaluation of intramolecular charge transfer state of 4-N, N ...

Indian Academy of Sciences (India)

Abstract. Intramolecular charge transfer of 4-N,N-dimethylamino cinnamaldehyde (DMACA) in vacuum and in five different aprotic solvents has been studied by using time-dependent density functional theory. (TDDFT). Polarizable continuum model (PCM) was employed to consider solvent–solute interactions. The potential ...

Low energy cross section data for ion-molecule reactions in hydrogen systems and for charge transfer of multiply charged ions with atoms and molecules

International Nuclear Information System (INIS)

Okuno, Kazuhiko

2007-04-01

Systematic cross section measurements for ion-molecule reactions in hydrogen systems and for charge transfer of multiply charged ions in low energy collisions with atoms and molecules have been performed continuously by the identical apparatus installed with an octo-pole ion beam guide (OPIG) since 1980 till 2004. Recently, all of accumulated cross section data for a hundred collision systems has been entered into CMOL and CHART of the NIFS atomic and molecular numerical database together with some related cross section data. In this present paper, complicated ion-molecule reactions in hydrogen systems are revealed and the brief outlines of specific properties in low energy charge transfer collisions of multiply charged ions with atoms and molecules are introduced. (author)

Band gap opening in α-graphyne by adsorption of organic molecule

Science.gov (United States)

Majidi, R.; Karami, A. R.

2014-09-01

The lack of a band gap limits the application of graphyne in nanoelectronic devices. We have investigated possibility of opening a band gap in α-graphyne by adsorption of tetracyanoethylene. The electronic property of α-graphyne in the presence of different numbers of tetracyanoethylene has been studied using density functional theory. It is found that charge is transferred from graphyne sheet to tetracyanoethylene molecules. In the presence of this electron acceptor molecule, a semimetal α-graphyne shows semiconducting property. The energy band gap at the Dirac point is enhanced by increasing the number of tetracyanoethylene. Our results provide a simple method to create and control the band gap in α-graphyne.

An impurity-induced gap system as a quantum data bus for quantum state transfer

International Nuclear Information System (INIS)

Chen, Bing; Li, Yong; Song, Z.; Sun, C.-P.

2014-01-01

We introduce a tight-binding chain with a single impurity to act as a quantum data bus for perfect quantum state transfer. Our proposal is based on the weak coupling limit of the two outermost quantum dots to the data bus, which is a gapped system induced by the impurity. By connecting two quantum dots to two sites of the data bus, the system can accomplish a high-fidelity and long-distance quantum state transfer. Numerical simulations for finite system show that the numerical and analytical results of the effective coupling strength agree well with each other. Moreover, we study the robustness of this quantum communication protocol in the presence of disorder in the couplings between the nearest-neighbor quantum dots. We find that the gap of the system plays an important role in robust quantum state transfer

Cell motility in models of wounded human skin is improved by Gap27 despite raised glucose, insulin and IGFBP-5

Energy Technology Data Exchange (ETDEWEB)

Wright, Catherine S.; Berends, Rebecca F. [Department of Life Sciences, School of Health and Life Sciences, Glasgow Caledonian University, 70 Cowcaddens Road, Glasgow G4 0BA (United Kingdom); Flint, David J. [Strathclyde Institute of Pharmacy and Biomedical Sciences, University of Strathclyde, 161 Cathedral Street, Glasgow G4 0RE (United Kingdom); Martin, Patricia E.M., E-mail: Patricia.Martin@gcu.ac.uk [Department of Life Sciences, School of Health and Life Sciences, Glasgow Caledonian University, 70 Cowcaddens Road, Glasgow G4 0BA (United Kingdom)

2013-02-15

Reducing Cx43 expression stimulates skin wound healing. This is mimicked in models when Cx43 function is blocked by the connexin mimetic peptide Gap27. IGF-I also stimulates wound healing with IGFBP-5 attenuating its actions. Further, the IGF-I to IGFBP-5 ratio is altered in diabetic skin, where wound closure is impaired. We investigated whether Gap27 remains effective in augmenting scrape-wound closure in human skin wound models simulating diabetes-induced changes, using culture conditions with raised glucose, insulin and IGFBP-5. Gap27 increased scrape-wound closure in normal glucose and insulin (NGI) and to a lesser extent in high glucose and insulin (HGI). IGF-I enhanced scrape-wound closure in keratinocytes whereas IGFBP-5 inhibited this response. Gap27 overcame the inhibitory effects of IGFBP-5 on IGF-I activity. Connexin-mediated communication (CMC) was reduced in HGI, despite raised Cx43, and Gap27 significantly decreased CMC in NGI and HGI. IGF-I and IGFBP-5 did not affect CMC. IGF-I increased keratinocyte proliferation in NGI, and Gap27 increased proliferation in NGI to a greater extent than in HGI. We conclude that IGF-I and Gap27 stimulate scrape-wound closure by independent mechanisms with Gap27 inhibiting Cx43 function. Gap27 can enhance wound closure in diabetic conditions, irrespective of the IGF-I:IGFBP-5 balance. - Highlights: ► Human organotypic and keratinocyte ‘diabetic’ skin models were used to demonstrate the ability of Gap27 to improve scrape-wound closure. ► Gap27 enhanced scrape-wound closure by reducing Cx43-mediated communication, whereas IGFBP-5 retarded cell migration. ► IGF-I and IGFBP-5 did not affect connexin-mediated pathways. ► Gap27 can override altered glucose, insulin, IGF-I, and IGFBP-5 in ‘diabetic’ skin models and thus has therapeutic potential.

Direct correlation of charge transfer absorption with molecular donor:acceptor interfacial area via photothermal deflection spectroscopy

KAUST Repository

Domingo, Ester

2015-04-09

We show that the Charge Transfer (CT) absorption signal in bulk-heterojunction (BHJ) solar cell blends, measured by photothermal deflection spectroscopy (PDS), is directly proportional to the density of molecular donor/acceptor interfaces. Since the optical transitions from ground state to the interfacial CT state are weakly allowed at photon energies below the optical gap of both donor and acceptor, we can exploit the use of this sensitive linear absorption spectroscopy for such quantification. Moreover, we determine the absolute molar extinction coefficient of the CT transition for an archetypical polymer-fullerene interface. The latter is ~100 times lower than the extinction coefficient of the donor chromophore involved, allowing us to experimentally estimate the transition dipole moment (0.3 D) and the electronic coupling between ground state and CT state to be on the order of 30 meV.

Turn-on fluorescence probes based on pyranine/viologen charge-transfer complexes for the determination of nucleotides

Energy Technology Data Exchange (ETDEWEB)

Schäferling, Michael, E-mail: Michael.schaeferling@utu.fi; Lang, Thomas; Schnettelker, Annette

2014-10-15

The formation of ground state charge-transfer complexes between pyranine (8-hydroxypyrene-1,3,6-trisulfonic acid) and viologen (paraquat) derivatives is utilized for the design of novel fluoroionophores for the determination of phosphate species, particularly of nucleotides. The strong quenching of the pyranine fluorescence by viologen-type charge transfer acceptors can be countermanded if these are functionalized with triethylammonium groups that serve as recognition elements for phosphate anions. We report on the fluorogenic responses of these water-soluble molecular probes in presence of different phosphates. Absorbance measurements give additional information on the charge transfer complex formation and the interaction with nucleotides. The experimental data show that these aggregates form attractive, simple and versatile fluorescence turn-on probes for nucleoside triphosphates. The reversibility of the fluorescence response is demonstrated by means of an enzymatic model assay using ATPase for the decomposition of adenosine triphosphate. - Highlights: • Pyranine/viologen charge-transfer complexes as molecular probe for ATP recognition. • Fluorescence turn on mechanism. • Selective compared to other nucleotides and phosphate anions. • Fast and reversible response applicable to monitor enzymatic reactions.

Study of charge transfer reactions in a microbial fuel cell

Energy Technology Data Exchange (ETDEWEB)

Martin, E.; Savadogo, O. [Ecole Polytechnique, Montreal, PQ (Canada). Dept. de Genie Chimique; National Research Council of Canada, Montreal, PQ (Canada). Biotechnology Research Inst.; Tartakovsky, B. [National Research Council of Canada, Montreal, PQ (Canada). Biotechnology Research Inst.

2008-07-01

Electron transfer reactions in a microbial fuel cell (MFC) were evaluated. The MFC was inoculated with anaerobic mesophilic sludge and operated with carbon felt, carbon cloth, and platinum (Pt) coated carbon cloth. The MFC was then fed with either acetate or glucose as a source of fuel and operated at a temperature of 25 degrees C and a pH of 7. Scanning electron microscopy (SEM) micrographs demonstrated that the micro-organisms colonized the anodes. Cyclic voltammetry and polarization tests were conducted using different fractions of the anodophilic biofilm in order to determine charge transfer routes. The study characterized the electron transfer mechanisms used by the exoelectrogenic micro-organisms to produce electricity. It was concluded that further research is needed to characterize reaction transfer routes. 2 refs., 1 fig.

Layer-dependent surface potential of phosphorene and anisotropic/layer-dependent charge transfer in phosphorene-gold hybrid systems.

Science.gov (United States)

Xu, Renjing; Yang, Jiong; Zhu, Yi; Yan, Han; Pei, Jiajie; Myint, Ye Win; Zhang, Shuang; Lu, Yuerui

2016-01-07

The surface potential and the efficiency of interfacial charge transfer are extremely important for designing future semiconductor devices based on the emerging two-dimensional (2D) phosphorene. Here, we directly measured the strong layer-dependent surface potential of mono- and few-layered phosphorene on gold, which is consistent with the reported theoretical prediction. At the same time, we used an optical way photoluminescence (PL) spectroscopy to probe charge transfer in the phosphorene-gold hybrid system. We firstly observed highly anisotropic and layer-dependent PL quenching in the phosphorene-gold hybrid system, which is attributed to the highly anisotropic/layer-dependent interfacial charge transfer.

H-shaped oligothiophenes with low band gaps and amphoteric redox properties

KAUST Repository

Luo, Jing

2010-12-17

H-shaped bridged oligothiophenes HT-1 and HT-2 were synthesized by two different approaches. Different from normal oligothiophenes, HT-1 and HT-2 showed low band gaps and amphoteric redox behaviors due to intramolecular charge transfer, which is further supported by time-dependent DFT calculations. © 2010 American Chemical Society.

CoPc and CoPcF16 on gold: Site-specific charge-transfer processes

Directory of Open Access Journals (Sweden)

Fotini Petraki

2014-04-01

Full Text Available Interface properties of cobalt(II phthalocyanine (CoPc and cobalt(II hexadecafluoro-phthalocyanine (CoPcF16 to gold are investigated by photo-excited electron spectroscopies (X-ray photoemission spectroscopy (XPS, ultraviolet photoemission spectroscopy (UPS and X-ray excited Auger electron spectroscopy (XAES. It is shown that a bidirectional charge transfer determines the interface energetics for CoPc and CoPcF16 on Au. Combined XPS and XAES measurements allow for the separation of chemical shifts based on different local charges at the considered atom caused by polarization effects. This facilitates a detailed discussion of energetic shifts of core level spectra. The data allow the discussion of site-specific charge-transfer processes.

Hydrogen-transfer and charge-transfer in photochemical and radiation induced reactions. Progress report, November 1, 1975--October 31, 1976

International Nuclear Information System (INIS)

Cohen, S.G.

1976-10-01

The relative importance of light absorption, quenching of triplet, and hydrogen transfer repair has been examined in retardation by mercaptans of photoreduction of aromatic ketones by alcohols. In the reduction of benzophenone by 2-propanol, retardation is efficient and, after correction for the first two effects, is due entirely to hydrogen-transfer repair, as indicated by deuterium labeling. In reduction of acetophenone by α-methylbenzyl alcohol, repair by hydrogen transfer is also operative. In reduction of benzophenone by benzhydrol, retardation is less efficient and is due to quenching, as the ketyl radical does not abstract hydrogen from mercaptan rapidly in competition with coupling. Deuterium isotope effects are discussed in terms of competitive reactions. Photoreduction of benzophenone by 2-butylamine and by triethylamine is retarded by aromatic mercaptans and disulfides. Of the retardation not due to light absorption and triplet quenching by the sulfur compounds, half is due to hydrogen-transfer repair, as indicated by racemization and deuterium labeling. The remainder is attributed to quenching by the sulfur compound of the charge-transfer-complex intermediate. Photoreduction by primary and secondary amines, but not by tertiary amines, is accelerated by aliphatic mercaptans. The acceleration is attributed to catalysis of hydrogen transfer by the mercaptan in the charge-transfer complex. The effect is large in hydrocarbon solvent, less in polar organic solvents and absent in water

Identification of the Heat Transfer Coefficient at the Charge Surface Heated on the Chamber Furnace

Directory of Open Access Journals (Sweden)

Gołdasz A.

2017-06-01

Full Text Available The inverse method was applied to determine the heat flux reaching the charge surface. The inverse solution was based upon finding the minimum of the error norm between the measured and calculated temperatures. The charge temperature field was calculated with the finite element method by solving the heat transfer equation for a square charge made of 15HM steel heated on all its surfaces. On the basis of the mean value of heat flux, the value of the heat transfer coefficient at each surface was determined depending on the surface temperature of the material heated.

Automatically closing swing gate closure assembly

Science.gov (United States)

Chang, Shih-Chih; Schuck, William J.; Gilmore, Richard F.

1988-01-01

A swing gate closure assembly for nuclear reactor tipoff assembly wherein the swing gate is cammed open by a fuel element or spacer but is reliably closed at a desired closing rate primarily by hydraulic forces in the absence of a fuel charge.

27 CFR 27.61 - Containers of distilled spirits to bear closures.

Science.gov (United States)

2010-04-01

... BEER General Requirements Closures for Containers of Distilled Spirits § 27.61 Containers of distilled spirits to bear closures. No person shall transport, buy, possess, or sell, or transfer any imported...

129I Moessbauer spectroscopic study of several n-σ charge-transfer complexes of iodine with thioethers

International Nuclear Information System (INIS)

Sakai, Hiroshi; Matsuyama, Tomochika; Maeda, Yutaka

1986-01-01

129 I Moessbauer studies have been made of n-σ charge-transfer complexes of iodine with thioethers, such as thiane, 1,4-oxathiane, and 1,4-dithiane. The spectra of these complexes consist of two sets of quadrupole octets, corresponding to the bridging and terminal iodine atoms. The transferred charges from the thioethers are localized on the terminal iodine atoms, and the bridging iodine atoms have slightly positive charges. This result can be well explained in terms of a covalent bond between the sulfur and bridging iodine atoms or the MO treatment of a delocalized three-center four-electron bonding. The contributions of the dative structure to the ground state are estimated to be 36, 28, and 24 % for thiane-iodine, 1,4-oxathiane-iodine, and 1,4-dithiane-iodine respectively. The nature of the charge-transfer bond is discussed in comparison with amine-iodine complexes. (author)

Charge-transfer potentials for ionic crystals: Cauchy violation, LO-TO splitting, and the necessity of an ionic reference state.

Science.gov (United States)

Sukhomlinov, Sergey V; Müser, Martin H

2015-12-14

In this work, we study how including charge transfer into force fields affects the predicted elastic and vibrational Γ-point properties of ionic crystals, in particular those of rock salt. In both analytical and numerical calculations, we find that charge transfer generally leads to a negative contribution to the Cauchy pressure, P(C) ≡ C12 - C66, where C12 and C66 are elements of the elastic tensor. This contribution increases in magnitude with pressure for different charge-transfer approaches in agreement with results obtained with density functional theory (DFT). However, details of the charge-transfer models determine the pressure dependence of the longitudinal optical-transverse optical splitting and that for partial charges. These last two quantities increase with density as long as the chemical hardness depends at most weakly on the environment while experiments and DFT find a decrease. In order to reflect the correct trends, the charge-transfer expansion has to be made around ions and the chemical (bond) hardness has to increase roughly exponentially with inverse density or bond lengths. Finally, the adjustable force-field parameters only turn out meaningful, when the expansion is made around ions.

Frenkel and Charge-Transfer Excitations in Donor-acceptor Complexes from Many-Body Green's Functions Theory.

Science.gov (United States)

Baumeier, Björn; Andrienko, Denis; Rohlfing, Michael

2012-08-14

Excited states of donor-acceptor dimers are studied using many-body Green's functions theory within the GW approximation and the Bethe-Salpeter equation. For a series of prototypical small-molecule based pairs, this method predicts energies of local Frenkel and intermolecular charge-transfer excitations with the accuracy of tens of meV. Application to larger systems is possible and allowed us to analyze energy levels and binding energies of excitons in representative dimers of dicyanovinyl-substituted quarterthiophene and fullerene, a donor-acceptor pair used in state of the art organic solar cells. In these dimers, the transition from Frenkel to charge transfer excitons is endothermic and the binding energy of charge transfer excitons is still of the order of 1.5-2 eV. Hence, even such an accurate dimer-based description does not yield internal energetics favorable for the generation of free charges either by thermal energy or an external electric field. These results confirm that, for qualitative predictions of solar cell functionality, accounting for the explicit molecular environment is as important as the accurate knowledge of internal dimer energies.

Realization of a mixed-symmetry superconducting gap in correlated organic metals

Science.gov (United States)

Altmeyer, Michaela; Guterding, Daniel; Jeschke, Harald O.; Diehl, Sandra; Methfessel, Torsten; Tutsch, Ulrich; Schubert, Harald; Lang, Michael; Müller, Jens; Huth, Michael; Jourdan, Martin; Elmers, Hans-Joachim; Valenti, Roser

Recent scanning tunneling spectroscopy measurements on the organic charge tranfer salt κ-(BEDT-TTF)2Cu[N(CN)2]Br show clear evidence of a highly anisotropic gap structure. Based on an ab initio derived model Hamiltonian we employ random phase approximation spin fluctuation theory yielding a composite order parameter of (extended) s+dx2-y2 symmetry. Taking explicitly also the shape of the Fermi surface into account we calculate STS spectra that are in excellent agreement to the experimental observations [1]. Moreover we determine the minimal tight binding model to describe the general lattice structure of these compounds accurately and generate a phase diagram for the gap symmetry by varying the hopping parameters. Based on ab initio derived parameter sets we predict the gap symmetry of other superconducting κ charge transfer salts. This work was supported by Deutsche Forschungsgemeinschaft under Grant No. SFB/TR 49.

Charge Transfer Based Colorimetric Detection of Silver Ion

Energy Technology Data Exchange (ETDEWEB)

Han, Seung Choul; Kim, Kwang Seob; Choi, Soon Kyu; Oh, Jinho; Lee, Jae Wook [Dong-A Univ., Busan (Korea, Republic of)

2014-05-15

We have demonstrated the colorimetric chemosensor for detection of Ag{sup +} via formation of nanoparticles which is based on the intramolecular CT interaction between the electron-rich (2,6-dialkoxynaphthalene; Np) moiety and the electron-deficient (methyl viologen; MV{sup 2+}) moiety of a single sensor molecule. Under irradiation of light, Ag{sup +} was reduced to very small silver nanoparticle by CT interaction in the presence of OEGs as flexible recognition moiety of Ag{sup +} and stabilizer for Ag nanoparticles, thus Ag nanoparticles resulted to reddish brown in the color change of sensor solution, gradually. Therefore, the charge-transfer interaction between an electron-deficient and an electron-rich units existing at a sensor molecule can be regarded as a new and efficient method to construct various colorimetric chemosensors. Donor.acceptor interactions or charge transfer (CT) interactions are an important class of non-covalent interactions and have been widely exploited in self-assembling systems. Beyond molecular chemistry, supramolecular chemistry aims at constituting highly complex, functional chemical systems from components held together by intermolecular forces. Chemosensors are the molecules of abiotic origin that bind selectively and reversibly with the analyte with concomitant change in one or more properties of the system. The recognition and signaling of ionic and neutral species of varying complexity is one of the most intensively studied areas of contemporary supramolecular chemistry.

Mechanism and Dynamics of Charge Transfer in Donor-Bridge-Acceptor Systems

NARCIS (Netherlands)

Gorczak-Vos, N.

2016-01-01

Photoinduced charge transfer in organic materials is a fundamental process in various biological and technological areas. Donor-bridge-acceptor (DBA) molecules are used as model systems in numerous theoretical and experimental work to systematically study and unravel the underlying mechanisms of

Charge transfer between hydrogen(deuterium) ions and atoms in metal vapors

International Nuclear Information System (INIS)

Alvarez T, I.; Cisneros G, C.

1981-01-01

The current state of the experiments on charge transfer between hydrogen (deuterium) ions and atoms in metal vapors are given. Emphasis is given to describing different experimental techniques. The results of calculations if available, are compared with existing experimental data. (author)

ANISOTROPY EFFECTS IN SINGLE-ELECTRON TRANSFER BETWEEN LASER-EXCITED ATOMS AND HIGHLY-CHARGED IONS

NARCIS (Netherlands)

Recent collision experiments are reviewed in which one-electron transfer between laser excited target atoms and (highly charged) keV-ions has been studied. Especially results showing a dependence of the charge exchange on the initial target orbital alignment are discussed. The question to what

Superconductivity and charge transfer excitations in high Tc superconductors

International Nuclear Information System (INIS)

Balseiro, C.A.; Alascio, B.; Gagliano, E.; Rojo, A.

1988-01-01

We present some numerical results to show that in a simple model which includes Cu 3d and O 2p orbitals together with inter and intra atomic correlations pairing between holes can occur due to charge transfer excitations. We present also a simple approximation to derive an effective Hamiltonian containing an interaction between particles which is attractive for some values of the different microscopic parameters

Quantum information transfer between topological and conventional charge qubits

International Nuclear Information System (INIS)

Li Jun; Zou Yan

2016-01-01

We propose a scheme to realize coherent quantum information transfer between topological and conventional charge qubits. We first consider a hybrid system where a quantum dot (QD) is tunnel-coupled to a semiconductor Majorana-hosted nanowire (MNW) via using gated control as a switch, the information encoded in the superposition state of electron empty and occupied state can be transferred to each other through choosing the proper interaction time to make measurements. Then we consider another system including a double QDs and a pair of parallel MNWs, it is shown that the entanglement information transfer can be realized between the two kinds of systems. We also realize long distance quantum information transfer between two quantum dots separated by an MNW, by making use of the nonlocal fermionic level formed with the pared Majorana feimions (MFs) emerging at the two ends of the MNW. Furthermore, we analyze the teleportationlike electron transfer phenomenon predicted by Tewari et al. [Phys. Rev. Lett. 100, 027001 (2008)] in our considered system. Interestingly, we find that this phenomenon exactly corresponds to the case that the information encoded in one QD just returns back to its original place during the dynamical evolution of the combined system from the perspective of quantum state transfer. (paper)

Synthesis and photophysical properties of a novel terephthalic PH sensor based on internal charge transfer

International Nuclear Information System (INIS)

Miladinova, Polya M.

2016-01-01

A novel fluorescence sensing derivative of 2-aminodimethylterephthalate configured as a “fluorophore-receptor” system was synthesized and investigated. Due to the internal charge transfer, the designed fluorophore was able to act as a pH-probe via an “off-on” fluorescence sensing mechanism. The sensor activity toward protons as cations and hydroxide as anions in DMF was studied by monitoring the changes of the fluorescence intensity. Keywords: 2-aminoterephthalic derivative, ICT (internal charge transfer), pH sensor.

Charge Transfer Effect on Raman and Surface Enhanced Raman Spectroscopy of Furfural Molecules.

Science.gov (United States)

Wan, Fu; Shi, Haiyang; Chen, Weigen; Gu, Zhaoliang; Du, Lingling; Wang, Pinyi; Wang, Jianxin; Huang, Yingzhou

2017-08-02

The detection of furfural in transformer oil through surface enhanced Raman spectroscopy (SERS) is one of the most promising online monitoring techniques in the process of transformer aging. In this work, the Raman of individual furfural molecules and SERS of furfural-M x (M = Ag, Au, Cu) complexes are investigated through density functional theory (DFT). In the Raman spectrum of individual furfural molecules, the vibration mode of each Raman peak is figured out, and the deviation from experimental data is analyzed by surface charge distribution. In the SERS of furfural-M x complexes, the influence of atom number and species on SERS chemical enhancement factors (EFs) are studied, and are further analyzed by charge transfer effect. Our studies strengthen the understanding of charge transfer effect in the SERS of furfural molecules, which is important in the online monitoring of the transformer aging process through SERS.

Charge transfer to the continuum by heavy ions in atomic hydrogen

International Nuclear Information System (INIS)

Sellin, I.A.

1981-01-01

Design and installation of an atomic hydrogen target for measurements of charge transfer to the continuum by heavy ions are discussed. The design consists of a tungsten gas cell operated at temperatures of 2500 to 2600 0 K. Initial testing is underway

Photogeneration of free charge carriers in .pi.-conjugated polymers with bulky side groups

Czech Academy of Sciences Publication Activity Database

Menšík, Miroslav; Jex, M.; Pfleger, Jiří; Jung, J.

2012-01-01

Roč. 404, 24 August (2012), s. 48-55 ISSN 0301-0104 R&D Projects: GA ČR(CZ) GAP205/10/2280; GA MŠk(CZ) OC10007 Institutional research plan: CEZ:AV0Z40500505 Institutional support: RVO:61389013 Keywords : photogeneration of free charge carriers * charge transfer states * localized excitation Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 1.957, year: 2012

Effect of Conjugation Length on Photoinduced Charge-Transfer in π-Conjugated Oligomer-Acceptor Dyads

KAUST Repository

Jiang, Junlin

2017-05-25

A series of -conjugated oligomer-acceptor dyads were synthesized that feature oligo(phenylene ethynylene) (OPE) conjugated backbones end-capped with a naphthalene diimide (NDI) acceptor. The OPE segments vary in length from 4 to 8 phenylene ethynene units (PEn-NDI, where n = 4, 6 and 8). Fluorescence and transient absorption spectroscopy reveals that intramolecular OPE NDI charge transfer dominates the deactivation of excited states of the PEn-NDI oligomers. Both charge separation (CS) and charge recombination (CR) are strongly exothermic (G0CS ~ -1.1 and G0CR ~ -2.0 eV), and the driving forces do not vary much across the series because the oxidation and reduction potentials and singlet energies of the OPEs do not vary much with their length. Bimolecular photoinduced charge transfer between model OPEs that do not contain the NDI acceptors with methyl viologen was studied, and the results reveal that the absorption of the cation radical state (OPE+•) remains approximately constant ( ~ 575 nm) regardless of oligomer length. This finding suggests that the cation radical (polaron) of the OPE is relatively localized, effectively occupying a confined segment of n 4 repeat units in the longer oligomers. Photoinduced intramolecular electron transfer dynamics in the PEn-NDI series was investigated by UV-visible femtosecond transient absorption spectroscopy with visible and mid-infrared probes. Charge separation occurs on the 1 – 10 ps timescale, with the rates decreasing slightly with increased oligomer length (βCS ~ 0.15 Å-1). The rate for charge-recombination decreases in the sequence PE4-NDI > PE6-NDI ~ PE8-NDI. The discontinuous distance dependence in the rate for charge recombination may be related to the spatial localization of the positive polaron state in the longer oligomers.

Effect of Conjugation Length on Photoinduced Charge-Transfer in π-Conjugated Oligomer-Acceptor Dyads

KAUST Repository

Jiang, Junlin; Alsam, Amani Abdu; Wang, Shanshan; Aly, Shawkat Mohammede; Pan, Zhenxing; Mohammed, Omar F.; Schanze, Kirk S.

2017-01-01

A series of -conjugated oligomer-acceptor dyads were synthesized that feature oligo(phenylene ethynylene) (OPE) conjugated backbones end-capped with a naphthalene diimide (NDI) acceptor. The OPE segments vary in length from 4 to 8 phenylene ethynene units (PEn-NDI, where n = 4, 6 and 8). Fluorescence and transient absorption spectroscopy reveals that intramolecular OPE NDI charge transfer dominates the deactivation of excited states of the PEn-NDI oligomers. Both charge separation (CS) and charge recombination (CR) are strongly exothermic (G0CS ~ -1.1 and G0CR ~ -2.0 eV), and the driving forces do not vary much across the series because the oxidation and reduction potentials and singlet energies of the OPEs do not vary much with their length. Bimolecular photoinduced charge transfer between model OPEs that do not contain the NDI acceptors with methyl viologen was studied, and the results reveal that the absorption of the cation radical state (OPE+•) remains approximately constant ( ~ 575 nm) regardless of oligomer length. This finding suggests that the cation radical (polaron) of the OPE is relatively localized, effectively occupying a confined segment of n 4 repeat units in the longer oligomers. Photoinduced intramolecular electron transfer dynamics in the PEn-NDI series was investigated by UV-visible femtosecond transient absorption spectroscopy with visible and mid-infrared probes. Charge separation occurs on the 1 – 10 ps timescale, with the rates decreasing slightly with increased oligomer length (βCS ~ 0.15 Å-1). The rate for charge-recombination decreases in the sequence PE4-NDI > PE6-NDI ~ PE8-NDI. The discontinuous distance dependence in the rate for charge recombination may be related to the spatial localization of the positive polaron state in the longer oligomers.

Near thermal charge transfer between Ar+2 and N2

International Nuclear Information System (INIS)

Holzscheiter, H.M.; Church, D.A.

1981-01-01

The near thermal charge transfer reaction of Ar +2 with N 2 has been studied at total pressures below 10 -7 Torr using a stored ion technique. Ar +2 ions produced by electron impact double ionization of Ar gas were selectively stored for times the order of seconds in a split-ring Penning-type ion trap. The decay with time of the initial ion sample number in a mixture of Ar and N 2 gases was fit to the sum of two exponentials, corresponding to different reaction rates for the 3 P and 1 D low-lying Ar +2 levels. The observed Ar +2 number decrease is attributed to the double-charge transfer process Ar +2 +N 2 →Ar+N 2 +2 →Ar+N + +N + in accord with recent flow-tube measurements. A rate constant for the metastable Ar +2 ( 1 D) level reaction with a value k( 1 D)=1.4 x 10 -9 cm 3 /sec is obtained, using the previously measured rate constant for the Ar +2 ( 3 P) state

Charge transfer between acenes and PbS nanocrystals

Energy Technology Data Exchange (ETDEWEB)

Dissanayake, D M N M [Solid State Electronics Laboratory, University of Michigan, Ann Arbor, MI 48109-2122 (United States); Hatton, R A [Department of Chemistry, University of Warwick, Coventry CV4 7AL (United Kingdom); Lutz, T [Departments of Chemistry and Physics, Imperial College, London SW7 2AY (United Kingdom); Curry, R J; Silva, S R P [Advanced Technology Institute, University of Surrey, Guildford GU2 7XH (United Kingdom)], E-mail: ndissa@umich.edu

2009-05-13

Organic-inorganic hybrid heterojunctions have potential as the basis for future photovoltaic devices. Herein, we report the results of investigations exploring the possibility of using pentacene and tetracene as photoelectron donors in conjunction with PbS nanocrystals (PbS-NCs). Photoinduced charge transfer was probed using external quantum efficiency measurements on acene:PbS-NC hybrid photovoltaic devices in conjunction with photoluminescence studies of the corresponding bilayer films. It is shown that photoelectron transfer from pentacene to the PbS-NCs is inefficient as compared to that between tetracene and PbS-NCs. The latter case can be rationalized in terms of the energy level alignment at the heterojunction assuming a common vacuum level. However, in the case of pentacene:PbS-NC junctions an interfacial energy level shift must be considered in order to explain the observations.

Charge-Transfer Processes in Warm Dense Matter: Selective Spectral Filtering for Laser-Accelerated Ion Beams

Science.gov (United States)

Braenzel, J.; Barriga-Carrasco, M. D.; Morales, R.; Schnürer, M.

2018-05-01

We investigate, both experimentally and theoretically, how the spectral distribution of laser accelerated carbon ions can be filtered by charge exchange processes in a double foil target setup. Carbon ions at multiple charge states with an initially wide kinetic energy spectrum, from 0.1 to 18 MeV, were detected with a remarkably narrow spectral bandwidth after they had passed through an ultrathin and partially ionized foil. With our theoretical calculations, we demonstrate that this process is a consequence of the evolution of the carbon ion charge states in the second foil. We calculated the resulting spectral distribution separately for each ion species by solving the rate equations for electron loss and capture processes within a collisional radiative model. We determine how the efficiency of charge transfer processes can be manipulated by controlling the ionization degree of the transfer matter.

Energy gaps, valence and conduction charge densities and optical properties of GaAs1‑xPx

Science.gov (United States)

Al-Hagan, O. A.; Algarni, H.; Bouarissa, N.; Alhuwaymel, T. F.; Ajmal Khan, M.

2018-04-01

The electronic structure and its derived valence and conduction charge distributions along with the optical properties of zinc-blende GaAs1‑xPx ternary alloys have been studied. The calculations are performed using a pseudopotential approach under the virtual crystal approximation (VCA) which takes into account the compositional disorder effect. Our findings are found to be generally in good accord with experiment. The composition dependence of direct and indirect bandgaps showed a clear bandgap bowing. The nature of the gap is found to depend on phosphorous content. The bonding and ionicity of the material of interest have been examined in terms of the anti-symmetric gap and charge densities. The variation in the optical constants versus phosphorous concentration has been discussed. The present investigation may give a useful applications in infrared and visible spectrum light emitters.

Synthetic system mimicking the energy transfer and charge separation of natural photosynthesis

Energy Technology Data Exchange (ETDEWEB)

Gust, D.; Moore, T.A.

1985-05-01

A synthetic molecular triad consisting of a porphyrin P linked to both a quinone Q and a carotenoid polyene C has been prepared as a mimic of natural photosynthesis for solar energy conversion purposes. Laser flash excitation of the porphyrin moiety yields a charge-separated state Csup(+.)-P-Qsup(-.) within 100 ps with a quantum yield of more than 0.25. This charge-separated state has a lifetime on the microsecond time scale in suitable solvents. The triad also models photosynthetic antenna function and photoprotection from singlet oxygen damge. The successful biomimicry of photosynthetic charge separation is in part the result of multistep electron transfers which rapidly separate the charges and leave the system at high potential, but with a considerable barrier to recombination.

Heat Transfer Coefficient at Cast-Mold Interface During Centrifugal Casting: Calculation of Air Gap

Science.gov (United States)

Bohacek, Jan; Kharicha, Abdellah; Ludwig, Andreas; Wu, Menghuai; Karimi-Sibaki, Ebrahim

2018-06-01

During centrifugal casting, the thermal resistance at the cast-mold interface represents a main blockage mechanism for heat transfer. In addition to the refractory coating, an air gap begins to form due to the shrinkage of the casting and the mold expansion, under the continuous influence of strong centrifugal forces. Here, the heat transfer coefficient at the cast-mold interface h has been determined from calculations of the air gap thickness d a based on a plane stress model taking into account thermoelastic stresses, centrifugal forces, plastic deformations, and a temperature-dependent Young's modulus. The numerical approach proposed here is rather novel and tries to offer an alternative to the empirical formulas usually used in numerical simulations for a description of a time-dependent heat transfer coefficient h. Several numerical tests were performed for different coating thicknesses d C, rotation rates Ω, and temperatures of solidus T sol. Results demonstrated that the scenario at the interface is unique for each set of parameters, hindering the possibility of employing empirical formulas without a preceding experiment being performed. Initial values of h are simply equivalent to the ratio of the coating thermal conductivity and its thickness ( 1000 Wm-2 K-1). Later, when the air gap is formed, h drops exponentially to values at least one order of magnitude smaller ( 100 Wm-2 K-1).

Charge and energy transfer interplay in hybrid sensitized solar cells mediated by graphene quantum dots

International Nuclear Information System (INIS)

Mihalache, Iuliana; Radoi, Antonio; Mihaila, Mihai; Munteanu, Cornel; Marin, Alexandru; Danila, Mihai; Kusko, Mihaela; Kusko, Cristian

2015-01-01

Highlights: • We report a one pot synthesis metod of GQD with controlled size and optoelectronic properties. • An improvement of common N3-DSSC characteristics is achieved when GQDs are used as co-sensitiser. • The role of GQD as cosensitisers in hybrid DSSC was investigated and the interplay between charge and energy transfer phenomena mediated by GQDs was demonstrated. • The GQDs presence determines an inhibition of the recombination processes at the TiO 2 /electrolyte interface. - Abstract: We explored the role of graphene quantum dots (GQDs) as co-sensitizers in hybrid dye sensitized solar cell (DSSC) architectures, focusing on various concurring mechanisms, such as: charge transfer, energy transfer and recombination rate, towards light harvesting improvement. GQDs were prepared by the hydrothermal method that allows the tuning of electronic levels and optical properties by employing appropriate precursors and synthesis conditions. The aim was to realize a type II alignment for TiO 2 /GQD/dye hybrid configuration, using standard N3 Ru-dye in order to improve charge transfer. When GQDs were used as co-sensitizers together with N3 Ru-dye, an improvement in power conversion efficiency was achieved, as shown by electrical measurements. The experimental analysis indicates that this improvement arises from the interplay of various mechanisms mediated by GQDs: (i) enhancement of charge separation and collection due to the cascaded alignment of the energy levels; (ii) energy transfer from GQDs to N3 Ru-dye due to the overlap between GQD photoluminescence and N3 Ru-dye absorption spectra; and (iii) reduction of the electron recombination to the redox couple due to the inhibition of the back electron transfer to the electrolyte by the GQDs

Water limits to closing yield gaps

Science.gov (United States)

Davis, Kyle Frankel; Rulli, Maria Cristina; Garrassino, Francesco; Chiarelli, Davide; Seveso, Antonio; D'Odorico, Paolo

2017-01-01

Agricultural intensification is often seen as a suitable approach to meet the growing demand for agricultural products and improve food security. It typically entails the use of fertilizers, new cultivars, irrigation, and other modern technology. In regions of the world affected by seasonal or chronic water scarcity, yield gap closure is strongly dependent on irrigation (blue water). Global yield gap assessments have often ignored whether the water required to close the yield gap is locally available. Here we perform a gridded global analysis (10 km resolution) of the blue water consumption that is needed annually to close the yield gap worldwide and evaluate the associated pressure on renewable freshwater resources. We find that, to close the yield gap, human appropriation of freshwater resources for irrigation would have to increase at least by 146%. Most study countries would experience at least a doubling in blue water requirement, with 71% of the additional blue water being required by only four crops - maize, rice, soybeans, and wheat. Further, in some countries (e.g., Algeria, Morocco, Syria, Tunisia, and Yemen) the total volume of blue water required for yield gap closure would exceed sustainable levels of freshwater consumption (i.e., 40% of total renewable surface and groundwater resources).

Ab Initio Analysis of Auger-Assisted Electron Transfer.

Science.gov (United States)

Hyeon-Deuk, Kim; Kim, Joonghan; Prezhdo, Oleg V

2015-01-15

Quantum confinement in nanoscale materials allows Auger-type electron-hole energy exchange. We show by direct time-domain atomistic simulation and analytic theory that Auger processes give rise to a new mechanism of charge transfer (CT) on the nanoscale. Auger-assisted CT eliminates the renown Marcus inverted regime, rationalizing recent experiments on CT from quantum dots to molecular adsorbates. The ab initio simulation reveals a complex interplay of the electron-hole and charge-phonon channels of energy exchange, demonstrating a variety of CT scenarios. The developed Marcus rate theory for Auger-assisted CT describes, without adjustable parameters, the experimental plateau of the CT rate in the region of large donor-acceptor energy gap. The analytic theory and atomistic insights apply broadly to charge and energy transfer in nanoscale systems.

Charge transfer collisions of Si^3+ with H at low energies

Science.gov (United States)

Joseph, D. C.; Gu, J. P.; Saha, B. C.

2009-11-01

Charge transfer of positively charged ions with atomic hydrogen is important not only in magnetically confined plasmas between impurity ions and H atoms from the chamber walls influences the overall ionization balance and effects the plasma cooling but also in astrophysics, where it plays a key role in determining the properties of the observed gas. It also provides a recombination mechanism for multiply charged ions in X-ray ionized astronomical environments. We report an investigation using the molecular-orbital close-coupling (MOCC) method, both quantum mechanically and semi-classically, in the adiabatic representation. Ab initio adiabatic potentials and coupling matrix elements--radial and angular--are calculated using the MRD-CI method. Comparison of our results with other theoretical as well as experimental findings will be discussed.

Theoretical Study of the Charge-Transfer State Separation within Marcus Theory

DEFF Research Database (Denmark)

Volpi, Riccardo; Nassau, Racine; Nørby, Morten Steen

2016-01-01

We study, within Marcus theory, the possibility of the charge-transfer (CT) state splitting at organic interfaces and a subsequent transport of the free charge carriers to the electrodes. As a case study we analyze model anthracene-C60 interfaces. Kinetic Monte Carlo (KMC) simulations on the cold...... CT state were performed at a range of applied electric fields, and with the fields applied at a range of angles to the interface to simulate the action of the electric field in a bulk heterojunction (BHJ) interface. The results show that the inclusion of polarization in our model increases CT state...... dissociation and charge collection. The effect of the electric field on CT state splitting and free charge carrier conduction is analyzed in detail with and without polarization. Also, depending on the relative orientation of the anthracene and C60 molecules at the interface, CT state splitting shows different...

Charge transfer in dissociating iodomethane and fluoromethane molecules ionized by intense femtosecond X-ray pulses

Directory of Open Access Journals (Sweden)

Rebecca Boll

2016-07-01

Full Text Available Ultrafast electron transfer in dissociating iodomethane and fluoromethane molecules was studied at the Linac Coherent Light Source free-electron laser using an ultraviolet-pump, X-ray-probe scheme. The results for both molecules are discussed with respect to the nature of their UV excitation and different chemical properties. Signatures of long-distance intramolecular charge transfer are observed for both species, and a quantitative analysis of its distance dependence in iodomethane is carried out for charge states up to I21+. The reconstructed critical distances for electron transfer are in good agreement with a classical over-the-barrier model and with an earlier experiment employing a near-infrared pump pulse.

Single-crystal charge transfer interfaces for efficient photonic devices (Conference Presentation)

Science.gov (United States)

Alves, Helena; Pinto, Rui M.; Maçôas, Ermelinda M. S.; Baleizão, Carlos; Santos, Isabel C.

2016-09-01

Organic semiconductors have unique optical, mechanical and electronic properties that can be combined with customized chemical functionality. In the crystalline form, determinant features for electronic applications such as molecular purity, the charge mobility or the exciton diffusion length, reveal a superior performance when compared with materials in a more disordered form. Combining crystals of two different conjugated materials as even enable a new 2D electronic system. However, the use of organic single crystals in devices is still limited to a few applications, such as field-effect transistors. In 2013, we presented the first system composed of single-crystal charge transfer interfaces presenting photoconductivity behaviour. The system composed of rubrene and TCNQ has a responsivity reaching 1 A/W, corresponding to an external quantum efficiency of nearly 100%. A similar approach, with a hybrid structure of a PCBM film and rubrene single crystal also presents high responsivity and the possibility to extract excitons generated in acceptor materials. This strategy led to an extended action towards the near IR. By adequate material design and structural organisation of perylediimides, we demonstrate that is possible to improve exciton diffusion efficiency. More recently, we have successfully used the concept of charge transfer interfaces in phototransistors. These results open the possibility of using organic single-crystal interfaces in photonic applications.

On development of analytical closure relationships for local wall friction, heat and mass transfer coefficients for sub-channel codes

International Nuclear Information System (INIS)

Kornienko, Y.

2000-01-01

The purpose has been to describe an approach suggested for constructing generalized closure relationships for local and subchannel wall friction, heat and mass transfer coefficients, with not only axial and transversal parameters taken into account, but azimuthal substance transfer effects as well. These constitutive relations that are primary for description of one- and two-phase one-dimensional flow models can be derived from the initial 3-D drift flux formulation. The approach is based on the Reynolds flux, boundary layer and generalized coefficient of substance transfer. One more task has been to illustrate the validity of the 'conformity principle' for the limiting cases. The method proposed is based on the similarity theory, boundary layer model, and a phenomenological description of the regularities of the substance transfer (momentum, heat, and mass), as well as on an adequate simulation of the forms of flow structure by a generalized approach to build (an integrated in form and semi-empirical in maintenance structure) analytical relationships for wall friction, heat and mass transfer coefficients. (author)

Charge transfer luminescence of Yb3+ ions in LiY1-xYbxP4O12 phosphates

International Nuclear Information System (INIS)

Stryganyuk, G; Zazubovich, S; Voloshinovskii, A; Pidzyrailo, M; Zimmerer, G; Peters, R; Petermann, K

2007-01-01

Spectral-kinetic studies have been performed for LiY 1-x Yb x P 4 O 12 (x = 0; 0.1; 0.9) phosphates at T = 8-320 K using synchrotron radiation for excitation within the 5-17 eV energy range. Mechanisms for the excitation of Yb 3+ charge transfer and f-f luminescence are discussed. The quasimolecular character of Yb 3+ charge transfer luminescence (CTL) is pointed out. The central Yb 2+ ion and hole delocalized over the surrounding ligands are proposed for consideration as a 'charge transfer cluster' (Yb 2+ CT cluster). Possible mechanisms of Yb 3+ CTL quenching are presumed

Ultrafast spin exchange-coupling torque via photo-excited charge-transfer processes

Science.gov (United States)

Ma, X.; Fang, F.; Li, Q.; Zhu, J.; Yang, Y.; Wu, Y. Z.; Zhao, H. B.; Lüpke, G.

2015-10-01

Optical control of spin is of central importance in the research of ultrafast spintronic devices utilizing spin dynamics at short time scales. Recently developed optical approaches such as ultrafast demagnetization, spin-transfer and spin-orbit torques open new pathways to manipulate spin through its interaction with photon, orbit, charge or phonon. However, these processes are limited by either the long thermal recovery time or the low-temperature requirement. Here we experimentally demonstrate ultrafast coherent spin precession via optical charge-transfer processes in the exchange-coupled Fe/CoO system at room temperature. The efficiency of spin precession excitation is significantly higher and the recovery time of the exchange-coupling torque is much shorter than for the demagnetization procedure, which is desirable for fast switching. The exchange coupling is a key issue in spin valves and tunnelling junctions, and hence our findings will help promote the development of exchange-coupled device concepts for ultrafast coherent spin manipulation.

Probing the N=50 shell gap near $^{78}$Ni

CERN Multimedia

Reiter, P; Blazhev, A A; Franchoo, S; Hadinia, B; Raabe, R; Diriken, J V J; Angus, L J

An experiment is proposed to study the properties of low-lying states close to the N=50 shell gap by single nucleon transfer. The d($^{78}$Zn,p)$\\,^{79}$Zn reaction will be studied using the T-REX silicon-detector array coupled to the MINIBALL $\\gamma$-ray spectrometer. A $^{78}$Zn beam intensity of 5 x 10$^{4}$ pps is expected. The isotope $^{79}$Zn, with Z=30 and N =49, lies two protons above and one neutron below the double-shell closure at $^{78}$Ni. Determination of the single-particle structure of low-lying states in $^{79}$Zn will provide valuable information about the persistence of the N=50 shell gap in this neutron-rich region. In particular the behaviour of the g$_{9/2}$ and d$_{5/2}$ orbitals will be investigated. In total, 27 shifts of beam time are requested. This experiment is envisaged to be the first of a series of measurements on progressively more neutron-rich Zn isotopes.

Development of highly accurate approximate scheme for computing the charge transfer integral

Energy Technology Data Exchange (ETDEWEB)

Pershin, Anton; Szalay, Péter G. [Laboratory for Theoretical Chemistry, Institute of Chemistry, Eötvös Loránd University, P.O. Box 32, H-1518 Budapest (Hungary)

2015-08-21

The charge transfer integral is a key parameter required by various theoretical models to describe charge transport properties, e.g., in organic semiconductors. The accuracy of this important property depends on several factors, which include the level of electronic structure theory and internal simplifications of the applied formalism. The goal of this paper is to identify the performance of various approximate approaches of the latter category, while using the high level equation-of-motion coupled cluster theory for the electronic structure. The calculations have been performed on the ethylene dimer as one of the simplest model systems. By studying different spatial perturbations, it was shown that while both energy split in dimer and fragment charge difference methods are equivalent with the exact formulation for symmetrical displacements, they are less efficient when describing transfer integral along the asymmetric alteration coordinate. Since the “exact” scheme was found computationally expensive, we examine the possibility to obtain the asymmetric fluctuation of the transfer integral by a Taylor expansion along the coordinate space. By exploring the efficiency of this novel approach, we show that the Taylor expansion scheme represents an attractive alternative to the “exact” calculations due to a substantial reduction of computational costs, when a considerably large region of the potential energy surface is of interest. Moreover, we show that the Taylor expansion scheme, irrespective of the dimer symmetry, is very accurate for the entire range of geometry fluctuations that cover the space the molecule accesses at room temperature.

Strategies to enhance the excitation energy-transfer efficiency in a light-harvesting system using the intra-molecular charge transfer character of carotenoids

Energy Technology Data Exchange (ETDEWEB)

Yukihira, Nao [Department of Applied Chemistry for Environment; School of Science and Technology; Kwansei Gakuin University; Sanda; Japan; Sugai, Yuko [Department of Applied Chemistry for Environment; School of Science and Technology; Kwansei Gakuin University; Sanda; Japan; Fujiwara, Masazumi [Department of Applied Chemistry for Environment; School of Science and Technology; Kwansei Gakuin University; Sanda; Japan; Kosumi, Daisuke [Institute of Pulsed Power Science; Kumamoto University; Kumamoto; Japan; Iha, Masahiko [South Product Co. Ltd.; Uruma-shi; Japan; Sakaguchi, Kazuhiko [Department of Chemistry; Graduate School of Science; Osaka City University; Osaka 558-8585; Japan; Katsumura, Shigeo [Department of Chemistry; Graduate School of Science; Osaka City University; Osaka 558-8585; Japan; Gardiner, Alastair T. [Glasgow Biomedical Research Centre; University of Glasgow; 126 University Place; Glasgow, G12 8QQ; UK; Cogdell, Richard J. [Glasgow Biomedical Research Centre; University of Glasgow; 126 University Place; Glasgow, G12 8QQ; UK; Hashimoto, Hideki [Department of Applied Chemistry for Environment; School of Science and Technology; Kwansei Gakuin University; Sanda; Japan

2017-01-01

Fucoxanthin is a carotenoid that is mainly found in light-harvesting complexes from brown algae and diatoms. Due to the presence of a carbonyl group attached to polyene chains in polar environments, excitation produces an excited intra-molecular charge transfer. This intra-molecular charge transfer state plays a key role in the highly efficient (~95%) energy-transfer from fucoxanthin to chlorophyllain the light-harvesting complexes from brown algae. In purple bacterial light-harvesting systems the efficiency of excitation energy-transfer from carotenoids to bacteriochlorophylls depends on the extent of conjugation of the carotenoids. In this study we were successful, for the first time, in incorporating fucoxanthin into a light-harvesting complex 1 from the purple photosynthetic bacterium,Rhodospirillum rubrumG9+ (a carotenoidless strain). Femtosecond pump-probe spectroscopy was applied to this reconstituted light-harvesting complex in order to determine the efficiency of excitation energy-transfer from fucoxanthin to bacteriochlorophyllawhen they are bound to the light-harvesting 1 apo-proteins.

Polarization and charge transfer in the hydration of chloride ions

International Nuclear Information System (INIS)

Zhao Zhen; Rogers, David M.; Beck, Thomas L.

2010-01-01

A theoretical study of the structural and electronic properties of the chloride ion and water molecules in the first hydration shell is presented. The calculations are performed on an ensemble of configurations obtained from molecular dynamics simulations of a single chloride ion in bulk water. The simulations utilize the polarizable AMOEBA force field for trajectory generation and MP2-level calculations are performed to examine the electronic structure properties of the ions and surrounding waters in the external field of more distant waters. The ChelpG method is employed to explore the effective charges and dipoles on the chloride ions and first-shell waters. The quantum theory of atoms in molecules (QTAIM) is further utilized to examine charge transfer from the anion to surrounding water molecules. The clusters extracted from the AMOEBA simulations exhibit high probabilities of anisotropic solvation for chloride ions in bulk water. From the QTAIM analysis, 0.2 elementary charges are transferred from the ion to the first-shell water molecules. The default AMOEBA model overestimates the average dipole moment magnitude of the ion compared to the quantum mechanical value. The average magnitude of the dipole moment of the water molecules in the first shell treated at the MP2-level, with the more distant waters handled with an AMOEBA effective charge model, is 2.67 D. This value is close to the AMOEBA result for first-shell waters (2.72 D) and is slightly reduced from the bulk AMOEBA value (2.78 D). The magnitude of the dipole moment of the water molecules in the first solvation shell is most strongly affected by the local water-water interactions and hydrogen bonds with the second solvation shell, rather than by interactions with the ion.

Evaluation of the Momentum Closure Schemes in MPAS-Ocean

Science.gov (United States)

Zhao, Shimei; Liu, Yudi; Liu, Wei

2018-04-01

In order to compare and evaluate the performances of the Laplacian viscosity closure, the biharmonic viscosity closure, and the Leith closure momentum schemes in the MPAS-Ocean model, a variety of physical quantities, such as the relative reference potential energy (RPE) change, the RPE time change rate (RPETCR), the grid Reynolds number, the root mean square (RMS) of kinetic energy, and the spectra of kinetic energy and enstrophy, are calculated on the basis of results of a 3D baroclinic periodic channel. Results indicate that: 1) The RPETCR demonstrates a saturation phenomenon in baroclinic eddy tests. The critical grid Reynolds number corresponding to RPETCR saturation differs between the three closures: the largest value is in the biharmonic viscosity closure, followed by that in the Laplacian viscosity closure, and that in the Leith closure is the smallest. 2) All three closures can effectively suppress spurious dianeutral mixing by reducing the grid Reynolds number under sub-saturation conditions of the RPETCR, but they can also damage certain physical processes. Generally, the damage to the rotation process is greater than that to the advection process. 3) The dissipation in the biharmonic viscosity closure is strongly dependent on scales. Most dissipation concentrates on small scales, and the energy of small-scale eddies is often transferred to large-scale kinetic energy. The viscous dissipation in the Laplacian viscosity closure is the strongest on various scales, followed by that in the Leith closure. Note that part of the small-scale kinetic energy is also transferred to large-scale kinetic energy in the Leith closure. 4) The characteristic length scale L and the dimensionless parameter D in the Leith closure are inherently coupled. The RPETCR is inversely proportional to the product of D and L. When the product of D and L is constant, both the simulated RPETCR and the inhibition of spurious dianeutral mixing are the same in all tests using the Leith

Analysis of flow boiling heat transfer in narrow annular gaps applying the design of experiments method

Directory of Open Access Journals (Sweden)

Gunar Boye

2015-06-01

Full Text Available The axial heat transfer coefficient during flow boiling of n-hexane was measured using infrared thermography to determine the axial wall temperature in three geometrically similar annular gaps with different widths (s = 1.5 mm, s = 1 mm, s = 0.5 mm. During the design and evaluation process, the methods of statistical experimental design were applied. The following factors/parameters were varied: the heat flux q · = 30 − 190 kW / m 2 , the mass flux m · = 30 − 700 kg / m 2 s , the vapor quality x · = 0 . 2 − 0 . 7 , and the subcooled inlet temperature T U = 20 − 60 K . The test sections with gap widths of s = 1.5 mm and s = 1 mm had very similar heat transfer characteristics. The heat transfer coefficient increases significantly in the range of subcooled boiling, and after reaching a maximum at the transition to the saturated flow boiling, it drops almost monotonically with increasing vapor quality. With a gap width of 0.5 mm, however, the heat transfer coefficient in the range of saturated flow boiling first has a downward trend and then increases at higher vapor qualities. For each test section, two correlations between the heat transfer coefficient and the operating parameters have been created. The comparison also shows a clear trend of an increasing heat transfer coefficient with increasing heat flux for test sections s = 1.5 mm and s = 1.0 mm, but with increasing vapor quality, this trend is reversed for test section 0.5 mm.

Spectroscopic study of the charge-transfer complexes TiCl4/styrene and TiCl4/polystyrene

Science.gov (United States)

Gonçalves, Norberto S.; Noda, Lúcia. K.

2017-10-01

In this work, solutions of TiCl4/styrene and TiCl4/polystyrene charge-transfer complexes in CHCl3 or CDCl3 were investigated by UV-vis, resonance Raman and 1H NMR spectroscopies in order to study their molecular and electronic structures. Both show a yellow colour due to absorption in the 400 nm region, related to a charge-transfer transition. In Raman spectra, as the excitation approaches the resonance region, the primary enhancement of aromatic ring modes was mainly observed, rather than intensification of the vinylic double-bond stretch. Under the experimental conditions it was observed that formation of polystyrene takes place, as showed by 1H NMR spectra, and the most significant interaction occurs at the aromatic ring, as supported by the results from interaction of TiCl4 with polystyrene, as indicated by the charge-transfer band and resonant intensification of the aromatic ring modes.

Communication: Modeling of concentration dependent water diffusivity in ionic solutions: Role of intermolecular charge transfer

Energy Technology Data Exchange (ETDEWEB)

Yao, Yi; Berkowitz, Max L., E-mail: maxb@unc.edu, E-mail: ykanai@unc.edu; Kanai, Yosuke, E-mail: maxb@unc.edu, E-mail: ykanai@unc.edu [Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599 (United States)

2015-12-28

The translational diffusivity of water in solutions of alkali halide salts depends on the identity of ions, exhibiting dramatically different behavior even in solutions of similar salts of NaCl and KCl. The water diffusion coefficient decreases as the salt concentration increases in NaCl. Yet, in KCl solution, it slightly increases and remains above bulk value as salt concentration increases. Previous classical molecular dynamics simulations have failed to describe this important behavior even when polarizable models were used. Here, we show that inclusion of dynamical charge transfer among water molecules produces results in a quantitative agreement with experiments. Our results indicate that the concentration-dependent diffusivity reflects the importance of many-body effects among the water molecules in aqueous ionic solutions. Comparison with quantum mechanical calculations shows that a heterogeneous and extended distribution of charges on water molecules around the ions due to ion-water and also water-water charge transfer plays a very important role in controlling water diffusivity. Explicit inclusion of the charge transfer allows us to model accurately the difference in the concentration-dependent water diffusivity between Na{sup +} and K{sup +} ions in simulations, and it is likely to impact modeling of a wide range of systems for medical and technological applications.

Charge separation and transfer in hybrid type II tunneling structures of CdTe and CdSe nanocrystals

Energy Technology Data Exchange (ETDEWEB)

Gross, Dieter Konrad Michael

2013-11-08

Closely packed nanocrystal systems have been investigated in this thesis with respect to charge separation by charge carrier tunneling. Clustered and layered samples have been analyzed using PL-measurements and SPV-methods. The most important findings are reviewed in the following. A short outlook is also provided for potential further aspects and application of the presented results. The main purpose of this thesis was to find and quantify electronic tunneling transfer in closely packed self-assembled nanocrystal structures presenting quantum mechanical barriers of about 1 nm width. We successfully used hybrid assemblies of CdTe and CdSe nanocrystals where the expected type II alignment between CdTe and CdSe typically leads to a concentration of electrons in CdSe and holes in CdTe nanocrystals. We were able to prove the charge selectivity of the CdTe-CdSe nanocrystal interface which induces charge separation. We mainly investigated the effects related to the electron transfer from CdTe to CdSe nanocrystals. Closely packing was achieved by two independent methods: the disordered colloidal clustering in solution and the layered assembly on dry glass substrates. Both methods lead to an inter-particle distance of about 1 nm of mainly organic material which acts as a tunneling barrier. PL-spectroscopy was applied. The PL-quenching of the CdTe nanocrystals in hybrid assemblies indicates charge separation by electron transfer from CdTe to CdSe nanocrystals. A maximum quenching rate of up to 1/100 ps was measured leading to a significant global PL-quenching of up to about 70 % for the CdTe nanocrystals. It was shown that charge separation dynamics compete with energy transfer dynamics and that charge separation typically dominates. The quantum confinement effect was used to tune the energetic offset between the CdTe and CdSe nanocrystals. We thus observe a correlation of PL-quenching and offset of the energy states for the electron transfer. The investigated PL

Charge separation and transfer in hybrid type II tunneling structures of CdTe and CdSe nanocrystals

International Nuclear Information System (INIS)

Gross, Dieter Konrad Michael

2013-01-01

Closely packed nanocrystal systems have been investigated in this thesis with respect to charge separation by charge carrier tunneling. Clustered and layered samples have been analyzed using PL-measurements and SPV-methods. The most important findings are reviewed in the following. A short outlook is also provided for potential further aspects and application of the presented results. The main purpose of this thesis was to find and quantify electronic tunneling transfer in closely packed self-assembled nanocrystal structures presenting quantum mechanical barriers of about 1 nm width. We successfully used hybrid assemblies of CdTe and CdSe nanocrystals where the expected type II alignment between CdTe and CdSe typically leads to a concentration of electrons in CdSe and holes in CdTe nanocrystals. We were able to prove the charge selectivity of the CdTe-CdSe nanocrystal interface which induces charge separation. We mainly investigated the effects related to the electron transfer from CdTe to CdSe nanocrystals. Closely packing was achieved by two independent methods: the disordered colloidal clustering in solution and the layered assembly on dry glass substrates. Both methods lead to an inter-particle distance of about 1 nm of mainly organic material which acts as a tunneling barrier. PL-spectroscopy was applied. The PL-quenching of the CdTe nanocrystals in hybrid assemblies indicates charge separation by electron transfer from CdTe to CdSe nanocrystals. A maximum quenching rate of up to 1/100 ps was measured leading to a significant global PL-quenching of up to about 70 % for the CdTe nanocrystals. It was shown that charge separation dynamics compete with energy transfer dynamics and that charge separation typically dominates. The quantum confinement effect was used to tune the energetic offset between the CdTe and CdSe nanocrystals. We thus observe a correlation of PL-quenching and offset of the energy states for the electron transfer. The investigated PL

Dynamics of the plasma injected into the gap of a plasma opening switch across a strong magnetic field

International Nuclear Information System (INIS)

Dolgachev, G. I.; Maslennikov, D. D.; Ushakov, A. G.; Fedotkin, A. S.; Khodeev, I. A.; Shvedov, A. A.

2011-01-01

A method is proposed to increase the linear charge density transferred through a plasma opening switch (POS) and, accordingly, reduce the POS diameter by enhancing the external magnetic field in the POS gap. Results are presented from experimental studies of the dynamics of the plasma injected into the POS gap across a strong magnetic field. The possibility of closing the POS gap by the plasma injected across an external magnetic field of up to 60 kG is demonstrated.

Charge separation and transfer in hybrid type II tunneling structures of CdTe and CdSe nanocrystals

Energy Technology Data Exchange (ETDEWEB)

Gross, Dieter Konrad Michael

2013-11-08

Closely packed nanocrystal systems have been investigated in this thesis with respect to charge separation by charge carrier tunneling. Clustered and layered samples have been analyzed using PL-measurements and SPV-methods. The most important findings are reviewed in the following. A short outlook is also provided for potential further aspects and application of the presented results. The main purpose of this thesis was to find and quantify electronic tunneling transfer in closely packed self-assembled nanocrystal structures presenting quantum mechanical barriers of about 1 nm width. We successfully used hybrid assemblies of CdTe and CdSe nanocrystals where the expected type II alignment between CdTe and CdSe typically leads to a concentration of electrons in CdSe and holes in CdTe nanocrystals. We were able to prove the charge selectivity of the CdTe-CdSe nanocrystal interface which induces charge separation. We mainly investigated the effects related to the electron transfer from CdTe to CdSe nanocrystals. Closely packing was achieved by two independent methods: the disordered colloidal clustering in solution and the layered assembly on dry glass substrates. Both methods lead to an inter-particle distance of about 1 nm of mainly organic material which acts as a tunneling barrier. PL-spectroscopy was applied. The PL-quenching of the CdTe nanocrystals in hybrid assemblies indicates charge separation by electron transfer from CdTe to CdSe nanocrystals. A maximum quenching rate of up to 1/100 ps was measured leading to a significant global PL-quenching of up to about 70 % for the CdTe nanocrystals. It was shown that charge separation dynamics compete with energy transfer dynamics and that charge separation typically dominates. The quantum confinement effect was used to tune the energetic offset between the CdTe and CdSe nanocrystals. We thus observe a correlation of PL-quenching and offset of the energy states for the electron transfer. The investigated PL

Momentum transfer in relativistic heavy ion charge-exchange reactions

Science.gov (United States)

Townsend, L. W.; Wilson, J. W.; Khan, F.; Khandelwal, G. S.

1991-01-01

Relativistic heavy ion charge-exchange reactions yield fragments (Delta-Z = + 1) whose longitudinal momentum distributions are downshifted by larger values than those associated with the remaining fragments (Delta-Z = 1, -2,...). Kinematics alone cannot account for the observed downshifts; therefore, an additional contribution from collision dynamics must be included. In this work, an optical model description of collision momentum transfer is used to estimate the additional dynamical momentum downshift. Good agreement between theoretical estimates and experimental data is obtained.

Observation of excited state charge transfer with fs/ps-CARS

International Nuclear Information System (INIS)

Blom, Alex Jason

2009-01-01

Excited state charge transfer processes are studied using the fs/ps-CARS probe technique. This probe allows for multiplexed detection of Raman active vibrational modes. Systems studied include Michler's Ketone, Coumarin 120, 4-dimethylamino-4(prime)-nitrostilbene, and several others. The vibrational spectrum of the para di-substituted benzophenone Michler's Ketone in the first excited singlet state is studied for the first time. It is found that there are several vibrational modes indicative of structural changes of the excited molecule. A combined experimental and theoretical approach is used to study the simplest 7-amino-4-methylcoumarin, Coumarin 120. Vibrations observed in FTIR and spontaneous Raman spectra are assigned using density functional calculations and a continuum solvation model is used to predict how observed modes are affected upon inclusion of a solvent. The low frequency modes of the excited state charge transfer species 4-dimethylamino-4(prime)-nitrostilbene are studied in acetonitrile. Results are compared to previous work on this molecule in the fingerprint region. Finally, several partially completed projects and their implications are discussed. These include the two photon absorption of Coumarin 120, nanoconfinement in cyclodextrin cavities and sensitization of titania nanoparticles

Observation of excited state charge transfer with fs/ps-CARS

Energy Technology Data Exchange (ETDEWEB)

Blom, Alex Jason [Iowa State Univ., Ames, IA (United States)

2009-01-01

Excited state charge transfer processes are studied using the fs/ps-CARS probe technique. This probe allows for multiplexed detection of Raman active vibrational modes. Systems studied include Michler's Ketone, Coumarin 120, 4-dimethylamino-4'-nitrostilbene, and several others. The vibrational spectrum of the para di-substituted benzophenone Michler's Ketone in the first excited singlet state is studied for the first time. It is found that there are several vibrational modes indicative of structural changes of the excited molecule. A combined experimental and theoretical approach is used to study the simplest 7-amino-4-methylcoumarin, Coumarin 120. Vibrations observed in FTIR and spontaneous Raman spectra are assigned using density functional calculations and a continuum solvation model is used to predict how observed modes are affected upon inclusion of a solvent. The low frequency modes of the excited state charge transfer species 4-dimethylamino-4{prime}-nitrostilbene are studied in acetonitrile. Results are compared to previous work on this molecule in the fingerprint region. Finally, several partially completed projects and their implications are discussed. These include the two photon absorption of Coumarin 120, nanoconfinement in cyclodextrin cavities and sensitization of titania nanoparticles.

Charge Transfer in Collisions of S^4+ with H.

Science.gov (United States)

Stancil, P. C.; Turner, A. R.; Cooper, D. L.; Schultz, D. R.; Rakovic, M. J.; Fritsch, W.; Zygelman, B.

2001-05-01

Charge transfer processes due to collisions of ground state S^4+ ions with atomic hydrogen were investigated for energies between 1 meV/u and 10 MeV/u using the quantum-mechanical molecular-orbital close-coupling (MOCC), atomic-orbital close-coupling, classical trajectory Monte Carlo (CTMC), and continuum distorted wave methods. The MOCC calculations utilized ab initio adiabatic potentials and nonadiabatic radial coupling matrix elements obtained with the spin-coupled valence-bond approach. A number of variants of the CTMC approach were explored, including different momentum and radial distributions for the initial state, as well as effective charge and quantum-defect models to determine the corresponding quantum state after capture into final partially-stripped S^3+ excited classical states. Hydrogen target isotope effects were explored and rate coefficients for temperatures between 100 and 10^6 K will be presented

Charge transfer in proton-hydrogen collisions under Debye plasma

Energy Technology Data Exchange (ETDEWEB)

Bhattacharya, Arka [Department of Mathematics, Burdwan University, Golapbag, Burdwan 713 104, West Bengal (India); Kamali, M. Z. M. [Centre for Foundation Studies in Science, University of Malaya, 50603 Kuala Lumpur (Malaysia); Ghoshal, Arijit, E-mail: arijit98@yahoo.com [Department of Mathematics, Burdwan University, Golapbag, Burdwan 713 104, West Bengal (India); Department of Mathematics, Kazi Nazrul University, B.C.W. Campus, Asansol 713 304, West Bengal (India); Institute of Mathematical Sciences, Faculty of Science, University of Malaya, 50603 Kuala Lumpur (Malaysia); Ratnavelu, K. [Department of Mathematics, Kazi Nazrul University, B.C.W. Campus, Asansol 713 304, West Bengal (India)

2015-02-15

The effect of plasma environment on the 1s → nlm charge transfer, for arbitrary n, l, and m, in proton-hydrogen collisions has been investigated within the framework of a distorted wave approximation. The effect of external plasma has been incorporated using Debye screening model of the interacting charge particles. Making use of a simple variationally determined hydrogenic wave function, it has been possible to obtain the scattering amplitude in closed form. A detailed study has been made to investigate the effect of external plasma environment on the differential and total cross sections for electron capture into different angular momentum states for the incident energy in the range of 20–1000 keV. For the unscreened case, our results are in close agreement with some of the most accurate results available in the literature.

Electronic, structural and chemical effects of charge-transfer at organic/inorganic interfaces

Science.gov (United States)

Otero, R.; Vázquez de Parga, A. L.; Gallego, J. M.

2017-07-01

During the last decade, interest on the growth and self-assembly of organic molecular species on solid surfaces spread over the scientific community, largely motivated by the promise of cheap, flexible and tunable organic electronic and optoelectronic devices. These efforts lead to important advances in our understanding of the nature and strength of the non-bonding intermolecular interactions that control the assembly of the organic building blocks on solid surfaces, which have been recently reviewed in a number of excellent papers. To a large extent, such studies were possible because of a smart choice of model substrate-adsorbate systems where the molecule-substrate interactions were purposefully kept low, so that most of the observed supramolecular structures could be understood simply by considering intermolecular interactions, keeping the role of the surface always relatively small (although not completely negligible). On the other hand, the systems which are more relevant for the development of organic electronic devices include molecular species which are electron donors, acceptors or blends of donors and acceptors. Adsorption of such organic species on solid surfaces is bound to be accompanied by charge-transfer processes between the substrate and the adsorbates, and the physical and chemical properties of the molecules cannot be expected any longer to be the same as in solution phase. In recent years, a number of groups around the world have started tackling the problem of the adsorption, self- assembly and electronic and chemical properties of organic species which interact rather strongly with the surface, and for which charge-transfer must be considered. The picture that is emerging shows that charge transfer can lead to a plethora of new phenomena, from the development of delocalized band-like electron states at molecular overlayers, to the existence of new substrate-mediated intermolecular interactions or the strong modification of the chemical

Microchip-calorimetry of organic charge transfer complex which shows superconductivity at low temperatures

Energy Technology Data Exchange (ETDEWEB)

Muraoka, Yuki [Department of Chemistry, Graduate School of Science, Osaka University, Machikaneyama 1-1, Toyonaka, Osaka 560-0043 (Japan); Yamashita, Satoshi [RIKEN, Hirosawa 2-1, Wako, Saitama 351-0198 (Japan); Yamamoto, Takashi [Department of Chemistry, Graduate School of Science, Osaka University, Machikaneyama 1-1, Toyonaka, Osaka 560-0043 (Japan); Nakazawa, Yasuhiro, E-mail: nakazawa@chem.sci.osaka-u.ac.jp [Department of Chemistry, Graduate School of Science, Osaka University, Machikaneyama 1-1, Toyonaka, Osaka 560-0043 (Japan); Institute for Molecular Science, Nishigonaka 38, Myodaiji, Okazaki 444-8585 (Japan)

2012-03-20

Highlights: Black-Right-Pointing-Pointer Organic charge transfer salt of {kappa}-(BEDT-TTF){sub 2}Cu[N(CN){sub 2}]Br shows superconductivity. Black-Right-Pointing-Pointer We succeeded to detect thermal anomaly microchip device TCG3880. Black-Right-Pointing-Pointer Development details of the calorimeter and the detection system is presented. Black-Right-Pointing-Pointer The magnetic fields dependence shows typical character of layered superconductor. - Abstract: We carried out thermodynamic measurements of organic charge transfer complex of {kappa}-(BEDT-TTF){sub 2}Cu[N(CN){sub 2}]Br, where BEDT-TTF is bis(ethylenedithio)tetrathiafulvalene by TCG3880 chip device in order to examine capability of the chip calorimeter at low temperature region and under magnetic fields. TCG3880 chip is mounted on a {sup 3}He cryostat available in combination with a superconductive magnet up to 7 T. Thermal anomalies related to the glass-like freezing of ethylene groups of BEDT-TTF molecules and the superconductive transition were observed. A frequency dependence of the thermal anomaly of the glass formation and a magnetic fields dependence of the thermal anomaly of the superconductive transition are reported. The results presented in this work demonstrate that the TCG3880 is quite useful for thermodynamic investigations of the organic charge transfer complex with much reduced sample quantity as compared with those of relaxation and adiabatic calorimetry.

Doping graphene films via chemically mediated charge transfer

Directory of Open Access Journals (Sweden)

Ishikawa Ryousuke

2011-01-01

Full Text Available Abstract Transparent conductive films (TCFs are critical components of a myriad of technologies including flat panel displays, light-emitting diodes, and solar cells. Graphene-based TCFs have attracted a lot of attention because of their high electrical conductivity, transparency, and low cost. Carrier doping of graphene would potentially improve the properties of graphene-based TCFs for practical industrial applications. However, controlling the carrier type and concentration of dopants in graphene films is challenging, especially for the synthesis of p-type films. In this article, a new method for doping graphene using the conjugated organic molecule, tetracyanoquinodimethane (TCNQ, is described. Notably, TCNQ is well known as a powerful electron accepter and is expected to favor electron transfer from graphene into TCNQ molecules, thereby leading to p-type doping of graphene films. Small amounts of TCNQ drastically improved the resistivity without degradation of optical transparency. Our carrier doping method based on charge transfer has a huge potential for graphene-based TCFs.

Energy transfer between two vacuum-gapped metal plates: Coulomb fluctuations and electron tunneling

Science.gov (United States)

Zhang, Zu-Quan; Lü, Jing-Tao; Wang, Jian-Sheng

2018-05-01

Recent experimental measurements for near-field radiative heat transfer between two bodies have been able to approach the gap distance within 2 nm , where the contributions of Coulomb fluctuation and electron tunneling are comparable. Using the nonequilibrium Green's function method in the G0W0 approximation, based on a tight-binding model, we obtain for the energy current a Caroli formula from the Meir-Wingreen formula in the local equilibrium approximation. Also, the Caroli formula is consistent with the evanescent part of the heat transfer from the theory of fluctuational electrodynamics. We go beyond the local equilibrium approximation to study the energy transfer in the crossover region from electron tunneling to Coulomb fluctuation based on a numerical calculation.

Charge-transfer mobility and electrical conductivity of PANI as conjugated organic semiconductors.

Science.gov (United States)

Zhang, Yahong; Duan, Yuping; Song, Lulu; Zheng, Daoyuan; Zhang, Mingxing; Zhao, Guangjiu

2017-09-21

The intramolecular charge transfer properties of a phenyl-end-capped aniline tetramer (ANIH) and a chloro-substituted derivative (ANICl) as organic semiconductors were theoretically studied through the first-principles calculation based on the Marcus-Hush theory. The reorganization energies, intermolecular electronic couplings, angular resolution anisotropic mobilities, and density of states of the two crystals were evaluated. The calculated results demonstrate that both ANIH and ANICl crystals show the higher electron transfer mobilities than the hole-transfer mobilities, which means that the two crystals should prefer to function as n-type organic semiconductors. Furthermore, the angle dependence mobilities of the two crystals show remarkable anisotropic character. The maximum mobility μ max of ANIH and ANICl crystals is 1.3893 and 0.0272 cm 2 V -1 s -1 , which appear at the orientation angles near 176°/356° and 119°/299° of a conducting channel on the a-b reference plane. It is synthetically evaluated that the ANIH crystal possesses relatively lower reorganization energy, higher electronic coupling, and electron transfer mobility, which means that the ANIH crystal may be the more ideal candidate as a high performance n-type organic semiconductor material. The systematic theoretical studies on organic crystals should be conducive to evaluating the charge-transport properties and designing higher performance organic semiconductor materials.

Reduced Charge Transfer Exciton Recombination in Organic Semiconductor Heterojunctions by Molecular Doping

NARCIS (Netherlands)

Deschler, Felix; Da Como, Enrico; Limmer, Thomas; Tautz, Raphael; Godde, Tillmann; Bayer, Manfred; von Hauff, Elizabeth; Yilmaz, Seyfullah; Allard, Sybille; Scherf, Ullrich; Feldmann, Jochen

2011-01-01

We investigate the effect of molecular doping on the recombination of electrons and holes localized at conjugated-polymer–fullerene interfaces. We demonstrate that a low concentration of p-type dopant molecules (<4% weight) reduces the interfacial recombination via charge transfer excitons and

An insight into the mechanism of charge-transfer of hybrid polymer:ternary/quaternary chalcopyrite colloidal nanocrystals

Directory of Open Access Journals (Sweden)

Parul Chawla

2014-08-01

Full Text Available In this work, we have demonstrated the structural and optoelectronic properties of the surface of ternary/quaternary (CISe/CIGSe/CZTSe chalcopyrite nanocrystallites passivated by tri-n-octylphosphine-oxide (TOPO and tri-n-octylphosphine (TOP and compared their charge transfer characteristics in the respective polymer: chalcopyrite nanocomposites by dispersing them in poly(3-hexylthiophene polymer. It has been found that CZTSe nanocrystallites due to their high crystallinity and well-ordered 3-dimensional network in its pristine form exhibit a higher steric- and photo-stability, resistance against coagulation and homogeneity compared to the CISe and CIGSe counterparts. Moreover, CZTSe nanocrystallites display efficient photoluminescence quenching as evident from the high value of the Stern–Volmer quenching constant (KSV and eventually higher charge transfer efficiency in their respective polymer P3HT:CZTSe composites. We modelled the dependency of the charge transfer from the donor and the charge separation mechanism across the donor–acceptor interface from the extent of crystallinity of the chalcopyrite semiconductors (CISe/CIGSe/CZTSe. Quaternary CZTSe chalcopyrites with their high crystallinity and controlled morphology in conjunction with regioregular P3HT polymer is an attractive candidate for hybrid solar cells applications.

An insight into the mechanism of charge-transfer of hybrid polymer:ternary/quaternary chalcopyrite colloidal nanocrystals.

Science.gov (United States)

Chawla, Parul; Singh, Son; Sharma, Shailesh Narain

2014-01-01

In this work, we have demonstrated the structural and optoelectronic properties of the surface of ternary/quaternary (CISe/CIGSe/CZTSe) chalcopyrite nanocrystallites passivated by tri-n-octylphosphine-oxide (TOPO) and tri-n-octylphosphine (TOP) and compared their charge transfer characteristics in the respective polymer: chalcopyrite nanocomposites by dispersing them in poly(3-hexylthiophene) polymer. It has been found that CZTSe nanocrystallites due to their high crystallinity and well-ordered 3-dimensional network in its pristine form exhibit a higher steric- and photo-stability, resistance against coagulation and homogeneity compared to the CISe and CIGSe counterparts. Moreover, CZTSe nanocrystallites display efficient photoluminescence quenching as evident from the high value of the Stern-Volmer quenching constant (K SV) and eventually higher charge transfer efficiency in their respective polymer P3HT:CZTSe composites. We modelled the dependency of the charge transfer from the donor and the charge separation mechanism across the donor-acceptor interface from the extent of crystallinity of the chalcopyrite semiconductors (CISe/CIGSe/CZTSe). Quaternary CZTSe chalcopyrites with their high crystallinity and controlled morphology in conjunction with regioregular P3HT polymer is an attractive candidate for hybrid solar cells applications.

Coil Design for High Misalignment Tolerant Inductive Power Transfer System for EV Charging

Directory of Open Access Journals (Sweden)

Kafeel Ahmed Kalwar

2016-11-01

Full Text Available The inductive power transfer (IPT system for electric vehicle (EV charging has acquired more research interest in its different facets. However, the misalignment tolerance between the charging coil (installed in the ground and pick-up coil (mounted on the car chassis, has been a challenge and fundamental interest in the future market of EVs. This paper proposes a new coil design QDQ (Quad D Quadrature that maintains the high coupling coefficient and efficient power transfer during reasonable misalignment. The QDQ design makes the use of four adjacent circular coils and one square coil, for both charging and pick-up side, to capture the maximum flux at any position. The coil design has been modeled in JMAG software for calculation of inductive parameters using the finite element method (FEM, and its hardware has been tested experimentally at various misaligned positions. The QDQ coils are shown to be capable of achieving good coupling coefficient and high efficiency of the system until the misalignment displacement reaches 50% of the employed coil size.

A model for the chain-to-plane charge transfer in YBa2Cu3O6+x

International Nuclear Information System (INIS)

Matic, V. M.; Lazarov, N. Dj.; Milic, M.

2012-01-01

A model for the chain-to-plane charge transfer is proposed to account for the two plateaus, at 60 K and at 90 K, of the T c (x) characteristics of the YBa 2 Cu 3 O 6+x high-T c superconductor. It is assumed that the number of holes transferred from a CuO chain of length l to two nearby CuO 2 sheets is proportional to l (that is, to the number of oxygen atoms in the chain), if the chain length is greater than, or equal to, a certain critical chain length, l cr , that is required to trigger the charge transfer process. No holes are assumed to have been transferred from chains of length l cr . The calculated T c (x) dependence is found to be in excellent agreement with the experimentally reported T c (x). The critical chain length parameter is estimated to be equal to l cr = 11 (eleven oxygen atoms in a chain), which is a greater value than that obtained in the previously proposed model for the chain-to-plane charge transfer (l cr = 4). The results obtained out of the proposed model are briefly discussed

Oxidation and metal-insertion in molybdenite surfaces: evaluation of charge-transfer mechanisms and dynamics

Directory of Open Access Journals (Sweden)

Shutthanandan V

2008-06-01

Full Text Available Abstract Molybdenum disulfide (MoS2, a layered transition-metal dichalcogenide, has been of special importance to the research community of geochemistry, materials and environmental chemistry, and geotechnical engineering. Understanding the oxidation behavior and charge-transfer mechanisms in MoS2 is important to gain better insight into the degradation of this mineral in the environment. In addition, understanding the insertion of metals into molybdenite and evaluation of charge-transfer mechanism and dynamics is important to utilize these minerals in technological applications. Furthermore, a detailed investigation of thermal oxidation behavior and metal-insertion will provide a basis to further explore and model the mechanism of adsorption of metal ions onto geomedia. The present work was performed to understand thermal oxidation and metal-insertion processes of molybdenite surfaces. The analysis was performed using atomic force microscopy (AFM, scanning electron microscopy (SEM, transmission electron microscopy (TEM, Rutherford backscattering spectrometry (RBS, and nuclear reaction analysis (NRA. Structural studies using SEM and TEM indicate the local-disordering of the structure as a result of charge-transfer process between the inserted lithium and the molybdenite layer. Selected area electron diffraction measurements indicate the large variations in the diffusivity of lithium confirming that the charge-transfer is different along and perpendicular to the layers in molybdenite. Thermal heating of molybenite surface in air at 400°C induces surface oxidation, which is slow during the first hour of heating and then increases significantly. The SEM results indicate that the crystals formed on the molybdenite surface as a result of thermal oxidation exhibit regular thin-elongated shape. The average size and density of the crystals on the surface is dependent on the time of annealing; smaller size and high density during the first one-hour and

Oxidation and metal-insertion in molybdenite surfaces: evaluation of charge-transfer mechanisms and dynamics.

Science.gov (United States)

Ramana, C V; Becker, U; Shutthanandan, V; Julien, C M

2008-06-05

Molybdenum disulfide (MoS2), a layered transition-metal dichalcogenide, has been of special importance to the research community of geochemistry, materials and environmental chemistry, and geotechnical engineering. Understanding the oxidation behavior and charge-transfer mechanisms in MoS2 is important to gain better insight into the degradation of this mineral in the environment. In addition, understanding the insertion of metals into molybdenite and evaluation of charge-transfer mechanism and dynamics is important to utilize these minerals in technological applications. Furthermore, a detailed investigation of thermal oxidation behavior and metal-insertion will provide a basis to further explore and model the mechanism of adsorption of metal ions onto geomedia.The present work was performed to understand thermal oxidation and metal-insertion processes of molybdenite surfaces. The analysis was performed using atomic force microscopy (AFM), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Rutherford backscattering spectrometry (RBS), and nuclear reaction analysis (NRA).Structural studies using SEM and TEM indicate the local-disordering of the structure as a result of charge-transfer process between the inserted lithium and the molybdenite layer. Selected area electron diffraction measurements indicate the large variations in the diffusivity of lithium confirming that the charge-transfer is different along and perpendicular to the layers in molybdenite. Thermal heating of molybenite surface in air at 400 degrees C induces surface oxidation, which is slow during the first hour of heating and then increases significantly. The SEM results indicate that the crystals formed on the molybdenite surface as a result of thermal oxidation exhibit regular thin-elongated shape. The average size and density of the crystals on the surface is dependent on the time of annealing; smaller size and high density during the first one-hour and significant

Multiconfiguration Pair-Density Functional Theory Outperforms Kohn-Sham Density Functional Theory and Multireference Perturbation Theory for Ground-State and Excited-State Charge Transfer.

Science.gov (United States)

Ghosh, Soumen; Sonnenberger, Andrew L; Hoyer, Chad E; Truhlar, Donald G; Gagliardi, Laura

2015-08-11

The correct description of charge transfer in ground and excited states is very important for molecular interactions, photochemistry, electrochemistry, and charge transport, but it is very challenging for Kohn-Sham (KS) density functional theory (DFT). KS-DFT exchange-correlation functionals without nonlocal exchange fail to describe both ground- and excited-state charge transfer properly. We have recently proposed a theory called multiconfiguration pair-density functional theory (MC-PDFT), which is based on a combination of multiconfiguration wave function theory with a new type of density functional called an on-top density functional. Here we have used MC-PDFT to study challenging ground- and excited-state charge-transfer processes by using on-top density functionals obtained by translating KS exchange-correlation functionals. For ground-state charge transfer, MC-PDFT performs better than either the PBE exchange-correlation functional or CASPT2 wave function theory. For excited-state charge transfer, MC-PDFT (unlike KS-DFT) shows qualitatively correct behavior at long-range with great improvement in predicted excitation energies.

Charge Transfer Effects in Naturally Occurring van der Waals Heterostructures (PbSe )1.16(TiSe2 )m (m =1 , 2)

Science.gov (United States)

Yao, Q.; Shen, D. W.; Wen, C. H. P.; Hua, C. Q.; Zhang, L. Q.; Wang, N. Z.; Niu, X. H.; Chen, Q. Y.; Dudin, P.; Lu, Y. H.; Zheng, Y.; Chen, X. H.; Wan, X. G.; Feng, D. L.

2018-03-01

van der Waals heterostructures (VDWHs) exhibit rich properties and thus has potential for applications, and charge transfer between different layers in a heterostructure often dominates its properties and device performance. It is thus critical to reveal and understand the charge transfer effects in VDWHs, for which electronic structure measurements have proven to be effective. Using angle-resolved photoemission spectroscopy, we studied the electronic structures of (PbSe )1.16(TiSe2 )m (m =1 , 2), which are naturally occurring VDWHs, and discovered several striking charge transfer effects. When the thickness of the TiSe2 layers is halved from m =2 to m =1 , the amount of charge transferred increases unexpectedly by more than 250%. This is accompanied by a dramatic drop in the electron-phonon interaction strength far beyond the prediction by first-principles calculations and, consequently, superconductivity only exists in the m =2 compound with strong electron-phonon interaction, albeit with lower carrier density. Furthermore, we found that the amount of charge transferred in both compounds is nearly halved when warmed from below 10 K to room temperature, due to the different thermal expansion coefficients of the constituent layers of these misfit compounds. These unprecedentedly large charge transfer effects might widely exist in VDWHs composed of metal-semiconductor contacts; thus, our results provide important insights for further understanding and applications of VDWHs.

Total and differential charge transfer cross sections in He{sup 2+}+N{sup 4+} collisions

Energy Technology Data Exchange (ETDEWEB)

Diemar, K. von; Melchert, F.; Huber, K.; Salzborn, E. [Institut fuer Kernphysik, Universitaet Giessen, Giessen (Germany); Trassl, R. [Institut fuer Kernphysik, Universitaet Giessen, Giessen (Germany)]. E-mail: Roland.H.Trassl@strz.uni-giessen.de; Opradolce, L. [Instituto de Astronomia y Fisica del Espacio (CONICET-UBA), Buenos Aires (Argentina); Piacentini, R.D. [Instituto de Fisica Rosario (CONICET-UNR), 2000 Rosario (Argentina)

2001-02-28

Charge transfer in the collision system He{sup 2+}+N{sup 4+} has been investigated both theoretically and experimentally for centre-of-mass energies between 8 and 200 keV. The theoretical calculations of the collision process have been carried out in the semi-classical impact parameter eikonal approach expanding the electronic wavefunction in a multi-state molecular-orbital basis with translation factors. The measurements of the charge-transfer cross sections were performed at an ion-ion crossed-beams experiment. Good agreement between the calculations and the experimental results for both total and differential cross sections is obtained. (author). Letter-to-the-editor.

Electrosynthesis of Copper-Tetracyanoquinodimethane Based on the Coupling Charge Transfer across Water/1,2-Dichloroethane Interface

International Nuclear Information System (INIS)

Huang, Li; Li, Pei; Pamphile, Ndagijimana; Tian, Zhong-Qun; Zhan, Dongping

2014-01-01

Graphical abstract: - Highlights: • Organic semiconductor CuTCNQ is synthesized through electrochemistry of liquid/liquid interface. • A coupling charge transfer (CCT) mechanism is proposed for organic electrosynthesis. • The obtained CuTCNQ has good electrochemical and electronic properties. - Abstract: The organic salt Copper-Tetracyanoquinodimethane (CuTCNQ) is an important semiconductor used in electronics for field-effect transistors, switches and memory devices. Here we present a novel electrosynthetic method of CuTCNQ microneedles based on the coupling charge transfer across water/1,2-dichloroethane (W/1,2-DCE) interface. A HOPG electrode is covered by a small volume of 1,2-DCE solution, which is further covered by an aqueous solution to construct the W/1,2-DCE interface. When TCNQ in 1,2-DCE phase is reduced on HOPG, Cu 2+ in the aqueous solution will transfer across the W/1,2-DCE interface in order to maintain the electric neutrality. Therein CuTCNQ microneedles are formed which have good solid-state electrochemical and electronic properties. This coupling charge transfer mechanism is valuable and broadens the applications of liquid/liquid interface in organic electrosynthesis

Evaluation of gap heat transfer model in ELESTRES for CANDU fuel element under normal operating conditions

International Nuclear Information System (INIS)

Lee, Kang Moon; Ohn, Myung Ryong; Im, Hong Sik; Choi, Jong Hoh; Hwang, Soon Taek

1995-01-01

The gap conductance between the fuel and the sheath depends strongly on the gap width and has a significant influence on the amount of initial stored energy. The modified Ross and Stoute gap conductance model in ELESTRES is based on a simplified thermal deformation model for steady-state fuel temperature calculations. A review on a series of experiments reveals that fuel pellets crack, relocate, and are eccentrically positioned within the sheath rather than solid concentric cylinders. In this paper, the two recently-proposed gap conductance models (offset gap model and relocated gap model) are described and are applied to calculate the fuel-sheath gap conductances under experimental conditions and normal operating conditions in CANDU reactors. The good agreement between the experimentally-inferred and calculated gap conductance values demonstrates that the modified Ross and Stoute model was implemented correctly in ELESTRES. The predictions of the modified Ross and Stoute model provide conservative values for gap heat transfer and fuel surface temperature compared to the offset gap and relocated gap models for a limiting power envelope. 13 figs., 3 tabs., 16 refs. (Author)

Electrostatic sensors applied to the measurement of electric charge transfer in gas-solids pipelines

International Nuclear Information System (INIS)

Woodhead, S R; Denham, J C; Armour-Chelu, D I

2005-01-01

This paper describes the development of a number of electric charge sensors. The sensors have been developed specifically to investigate triboelectric charge transfer which takes place between particles and the pipeline wall, when powdered materials are conveyed through a pipeline using air. A number of industrial applications exist for such gas-solids pipelines, including pneumatic conveyors, vacuum cleaners and dust extraction systems. The build-up of electric charge on pipelines and powdered materials can lead to electrostatic discharge and so is of interest from a safety viewpoint. The charging of powders can also adversely affect their mechanical handling characteristics and so is of interest to handling equipment engineers. The paper presents the design of the sensors, the design of the electric charge test rig and electric charge measurement test results

K-shell-hole production, multiple-hole production, charge transfer, and antisymmetry

International Nuclear Information System (INIS)

Reading, J.F.; Ford, A.L.

1980-01-01

In calculating K-shell-hole production when an ion collides with an atom, account must be taken of the fact that processes involving electrons other than the K-shell electron can occur. For example, after making a K-shell hole an L-shell electron may be knocked into it, or an L-shell vacancy may be produced and the K-shell electron promoted to that vacancy in the ''Fermi sea'' of the target-atom orbitals. In 1973 a theorem was proved by one of the present authors demonstrating that all these multielectron processes cancel in an independent-particle model for the target atom. In this paper it is shown that the same thing occurs for hole production by charge transfer to the ion. The authors demonstrate that multihole production does not obey this simple rule and that the probability for multihole production is not the product of independent single-electron probabilities. The correct expressions that should be used for these processes are given, together with new results for charge-transfer processes accompanied by hole production

Charge transfer in low-energy collisions of H with He+ and H+ with He in excited states

Science.gov (United States)

Loreau, J.; Ryabchenko, S.; Muñoz Burgos, J. M.; Vaeck, N.

2018-04-01

The charge transfer process in collisions of excited (n = 2, 3) hydrogen atoms with He+ and in collisions of excited helium atoms with H+ is studied theoretically. A combination of a fully quantum-mechanical method and a semi-classical approach is employed to calculate the charge-exchange cross sections at collision energies from 0.1 eV u‑1 up to 1 keV u‑1. These methods are based on accurate ab initio potential energy curves and non-adiabatic couplings for the molecular ion HeH+. Charge transfer can occur either in singlet or in triplet states, and the differences between the singlet and triplet spin manifolds are discussed. The dependence of the cross section on the quantum numbers n and l of the initial state is demonstrated. The isotope effect on the charge transfer cross sections, arising at low collision energy when H is substituted by D or T, is investigated. Rate coefficients are calculated for all isotopes up to 106 K. Finally, the impact of the present calculations on models of laboratory plasmas is discussed.

Charge distribution effects in polyatomic reactants involved in simple electron transfer reactions

Czech Academy of Sciences Publication Activity Database

Fawcett, W. R.; Chavis, G. J.; Hromadová, Magdaléna

2008-01-01

Roč. 53, č. 23 (2008), s. 6787-6792 ISSN 0013-4686 Institutional research plan: CEZ:AV0Z40400503 Keywords : electron transfer kinetics * charge distribution effects * double - layer effects in electrode kinetics Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.078, year: 2008

The merits of non-tradable quotas as a domestic policy instrument to prevent firm closure

International Nuclear Information System (INIS)

Hagem, Cathrine

2001-05-01

There is a concern in many countries that a domestic tradable quota system for greenhouse gases, where all emitters must pay for their quotas, may lead to closures of emissions-intensive industrial companies. Allocating quotas free of charge to companies operating in competitive markets has been suggested as a means to reduce the likelihood of closures. Two different designs of quota systems are studied within a two-period model: one where the quotas given free of charge are tradable, and one where the quotas are non-tradable. The two quota systems are compared with respect to their ability both to induce the firms to implement investment in abatement technology and to prevent or postpone closures. (author)

Spin state of negative charge-transfer material SrCoO.sub.3./sub..

Czech Academy of Sciences Publication Activity Database

Kuneš, Jan; Křápek, Vlastimil; Parragh, N.; Sangiovanni, G.; Toschi, A.; Kozhevnikov, A.V.

2012-01-01

Roč. 109, č. 11 (2012), "117206-1"-"117206-5" ISSN 0031-9007 R&D Projects: GA ČR GAP204/10/0284 Keywords : negative charge tranfer * dynamical mean-field theory Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 7.943, year: 2012 http://link.aps.org/doi/10.1103/PhysRevLett.109.117206

Extraordinary Mechanism of the Diels-Alder Reaction: Investigation of Stereochemistry, Charge Transfer, Charge Polarization, and Biradicaloid Formation.

Science.gov (United States)

Sexton, Thomas; Kraka, Elfi; Cremer, Dieter

2016-02-25

The Diels-Alder reaction between 1,3-butadiene and ethene is investigated from far-out in the entrance channel to the very last step in the exit channel thus passing two bifurcation points and extending the range of the reaction valley studied with URVA (Unified Reaction Valley Approach) by 300% compared to previous studies. For the first time, the pre- and postchemical steps of the reaction are analyzed at the same level of theory as the actual chemical processes utilizing the path curvature and its decomposition into internal coordinate or curvilinear coordinate components. A first smaller charge transfer to the dienophile facilitates the rotation of gauche butadiene into its cis form. The actual chemical processes are initiated by a second larger charge transfer to the dienophile that facilitates pyramidalization of the reacting carbon centers, bond equalization, and biradicaloid formation of the reactants. The transition state is aromatically stabilized and moved by five path units into the entrance channel in line with the Hammond-Leffler postulate. The pseudorotation of the boat form into the halfchair of cyclohexene is analyzed. Predictions are made for the Diels-Alder reaction based on a 11-phase mechanism obtained by the URVA analysis.

Modeling of heat and mass transfer processes for the gap-lyophilization system using the mannitol-trehalose-NaCl formulation.

Science.gov (United States)

Kuu, Wei Y; Doty, Mark J; Nisipeanu, Eugen; Rebbeck, Christine L; Cho, Yong K; Smit, Mark H

2014-09-01

Gap freezing (GF) is a new concept that was developed to reduce the primary drying time using an alternative freezing process. The purpose of this investigation was to determine the gap-tray heat transfer coefficient, Kgtr , and to investigate the effect of gap lyophilization on cycle reduction of a mannitol-trehalose-NaCl (MTN) formulation. The values of Kgtr were measured using the product temperature profiles in three different configurations: (1) shelf freezing followed by shelf drying (denoted as SF-SD), (2) GF followed by SD (denoted as GF-SD), and (3) GF followed by gap drying (denoted as GF-GD). For the lyophilization cycle using shelf drying (SF-SD), 80% of the heat transferred during primary drying was from the bottom shelf to the vial, versus 20% via radiation from the top shelf. For the lyophilization cycle using gap drying (GF-GD), only 37% of the heat transferred during primary drying was from the bottom shelf to the vial versus 63% via radiation from the top shelf. Furthermore, GF in conjunction with annealing significantly reduces the dry layer resistance of the MTN formulation, which is the opposite of what was observed with a conventional freezing cycle. © 2014 Wiley Periodicals, Inc. and the American Pharmacists Association.

Density functional theory for the description of charge-transfer processes at TTF/TCNQ interfaces

KAUST Repository

Van Regemorter, Tanguy; Guillaume, Maxime; Sini, Gjergji; Sears, John S.; Geskin, Victor; Bré das, Jean-Luc; Beljonne, David; Cornil, Jé rô me

2012-01-01

In the field of organic electronics, a central issue is to assess how the frontier electronic levels of two adjacent organic layers align with respect to one another at the interface. This alignment can be driven by the presence of a partial charge transfer and the formation of an interface dipole; it plays a key role for instance in determining the rates of exciton dissociation or exciton formation in organic solar cells or light-emitting diodes, respectively. Reliably modeling the processes taking place at these interfaces remains a challenge for the computational chemistry community. Here, we review our recent theoretical work on the influence of the choice of density functional theory (DFT) methodology on the description of the charge-transfer character in the ground state of TTF/ TCNQ model complexes and interfaces. Starting with the electronic properties of the isolated TTF and TCNQ molecules and then considering the charge transfer and resulting interface dipole in TTF/TCNQ donor-acceptor stacks and bilayers, we examine the impact of the choice of DFT functional in describing the interfacial electronic structure. Finally, we employ computations based on periodic boundary conditions to highlight the impact of depolarization effects on the interfacial dipole moment. © Springer-Verlag 2012.

Overcoming the Cut-Off Charge Transfer Bandgaps at the PbS Quantum Dot Interface

KAUST Repository

El-Ballouli, Ala'a O.

2015-11-17

Light harvesting from large size of semiconductor PbS quantum dots (QDs) with a bandgap of less than 1 eV is one of the greatest challenges precluding the development of PbS QD-based solar cells because the interfacial charge transfer (CT) from such QDs to the most commonly used electron acceptor materials is very inefficient, if it occurs at all. Thus, an alternative electron-accepting unit with a new driving force for CT is urgently needed to harvest the light from large-sized PbS QDs. Here, a cationic porphyrin is utilized as a new electron acceptor unit with unique features that bring the donor–acceptor components into close molecular proximity, allowing ultrafast and efficient electron transfer for QDs of all sizes, as inferred from the drastic photoluminescence quenching and the ultrafast formation of the porphyrin anionic species. The time-resolved results clearly demonstrate the possibility of modulating the electron transfer process between PbS QDs and porphyrin moieties not only by the size quantization effect but also by the interfacial electrostatic interaction between the positively charged porphyrin and the negatively charged QDs. This approach provides a new pathway for engineering QD-based solar cells that make the best use of the diverse photons making up the Sun\\'s broad irradiance spectrum.

Density functional theory for the description of charge-transfer processes at TTF/TCNQ interfaces

KAUST Repository

Van Regemorter, Tanguy

2012-09-15

In the field of organic electronics, a central issue is to assess how the frontier electronic levels of two adjacent organic layers align with respect to one another at the interface. This alignment can be driven by the presence of a partial charge transfer and the formation of an interface dipole; it plays a key role for instance in determining the rates of exciton dissociation or exciton formation in organic solar cells or light-emitting diodes, respectively. Reliably modeling the processes taking place at these interfaces remains a challenge for the computational chemistry community. Here, we review our recent theoretical work on the influence of the choice of density functional theory (DFT) methodology on the description of the charge-transfer character in the ground state of TTF/ TCNQ model complexes and interfaces. Starting with the electronic properties of the isolated TTF and TCNQ molecules and then considering the charge transfer and resulting interface dipole in TTF/TCNQ donor-acceptor stacks and bilayers, we examine the impact of the choice of DFT functional in describing the interfacial electronic structure. Finally, we employ computations based on periodic boundary conditions to highlight the impact of depolarization effects on the interfacial dipole moment. © Springer-Verlag 2012.

Overcoming the Cut-Off Charge Transfer Bandgaps at the PbS Quantum Dot Interface

KAUST Repository

El-Ballouli, Ala'a O.; Alarousu, Erkki; Kirmani, Ahmad R.; Amassian, Aram; Bakr, Osman; Mohammed, Omar F.

2015-01-01

Light harvesting from large size of semiconductor PbS quantum dots (QDs) with a bandgap of less than 1 eV is one of the greatest challenges precluding the development of PbS QD-based solar cells because the interfacial charge transfer (CT) from such QDs to the most commonly used electron acceptor materials is very inefficient, if it occurs at all. Thus, an alternative electron-accepting unit with a new driving force for CT is urgently needed to harvest the light from large-sized PbS QDs. Here, a cationic porphyrin is utilized as a new electron acceptor unit with unique features that bring the donor–acceptor components into close molecular proximity, allowing ultrafast and efficient electron transfer for QDs of all sizes, as inferred from the drastic photoluminescence quenching and the ultrafast formation of the porphyrin anionic species. The time-resolved results clearly demonstrate the possibility of modulating the electron transfer process between PbS QDs and porphyrin moieties not only by the size quantization effect but also by the interfacial electrostatic interaction between the positively charged porphyrin and the negatively charged QDs. This approach provides a new pathway for engineering QD-based solar cells that make the best use of the diverse photons making up the Sun's broad irradiance spectrum.

"Inverted" Solvent Effect on Charge Transfer in the Excited State.

Science.gov (United States)

Nau; Pischel

1999-10-04

Faster in cyclohexane than in acetonitrile is the fluorescence quenching of the azoalkane 2,3-diazabicyclo[2.2.2]oct-2-ene (DBO) by amines and sulfides. Although this photoreaction is induced by charge transfer (CT; see picture) and exciplexes are formed, the increase in the dipole moment of the exciplex is not large enough to offset the solvent stabilization of the excited reactants, and an "inverted" solvent effect results.

Charge Transfer and Support Effects in Heterogeneous Catalysis

Energy Technology Data Exchange (ETDEWEB)

Hervier, Antoine [Univ. of California, Berkeley, CA (United States)

2011-12-21

The kinetic, electronic and spectroscopic properties of two-dimensional oxide-supported catalysts were investigated in order to understand the role of charge transfer in catalysis. Pt/TiO₂ nanodiodes were fabricated and used as catalysts for hydrogen oxidation. During the reaction, the current through the diode, as well as its I-V curve, were monitored, while gas chromatography was used to measure the reaction rate. The current and the turnover rate were found to have the same temperature dependence, indicating that hydrogen oxidation leads to the non-adiabatic excitation of electrons in Pt. A fraction of these electrons have enough energy to ballistically transport through Pt and overcome the Schottky barrier at the interface with TiO₂. The yield for this phenomenon is on the order of 10^-4 electrons per product molecule formed, similar to what has been observed for CO oxidation and for the adsorption of many different molecules. The same Pt/TiO₂ system was used to compare currents in hydrogen oxidation and deuterium oxidation. The current through the diode under deuterium oxidation was found to be greater than under hydrogen oxidation by a factor of three. Weighted by the difference in turnover frequencies for the two isotopes, this would imply a chemicurrent yield 5 times greater for D₂ compared to H₂, contrary to what is expected given the higher mass of D₂. Reversible changes in the rectification factor of the diode are observed when switching between D₂ and H₂. These changes are a likely cause for the differences in current between the two isotopes. In the nanodiode experiments, surface chemistry leads to charge flow, suggesting the possibility of creating charge flow to tune surface chemistry. This was done first by exposing a Pt/Si diode to visible light while using it as a catalyst for H₂ oxidation. Absorption of the light in the Si, combined with

Amino-Acid-Induced Preferential Orientation of Perovskite Crystals for Enhancing Interfacial Charge Transfer and Photovoltaic Performance.

Science.gov (United States)

Shih, Yen-Chen; Lan, Yu-Bing; Li, Chia-Shuo; Hsieh, Hsiao-Chi; Wang, Leeyih; Wu, Chih-I; Lin, King-Fu

2017-06-01

Interfacial engineering of perovskite solar cells (PSCs) is attracting intensive attention owing to the charge transfer efficiency at an interface, which greatly influences the photovoltaic performance. This study demonstrates the modification of a TiO 2 electron-transporting layer with various amino acids, which affects charge transfer efficiency at the TiO 2 /CH 3 NH 3 PbI 3 interface in PSC, among which the l-alanine-modified cell exhibits the best power conversion efficiency with 30% enhancement. This study also shows that the (110) plane of perovskite crystallites tends to align in the direction perpendicular to the amino-acid-modified TiO 2 as observed in grazing-incidence wide-angle X-ray scattering of thin CH 3 NH 3 PbI 3 perovskite film. Electrochemical impedance spectroscopy reveals less charge transfer resistance at the TiO 2 /CH 3 NH 3 PbI 3 interface after being modified with amino acids, which is also supported by the lower intensity of steady-state photoluminescence (PL) and the reduced PL lifetime of perovskite. In addition, based on the PL measurement with excitation from different side of the sample, amino-acid-modified samples show less surface trapping effect compared to the sample without modification, which may also facilitate charge transfer efficiency at the interface. The results suggest that appropriate orientation of perovskite crystallites at the interface and trap-passivation are the niche for better photovoltaic performance. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Neutralized ion beam modification of cellulose membranes for study of ion charge effect on ion-beam-induced DNA transfer

Science.gov (United States)

Prakrajang, K.; Sangwijit, K.; Anuntalabhochai, S.; Wanichapichart, P.; Yu, L. D.

2012-02-01

Low-energy ion beam biotechnology (IBBT) has recently been rapidly developed worldwide. Ion-beam-induced DNA transfer is one of the important applications of IBBT. However, mechanisms involved in this application are not yet well understood. In this study plasma-neutralized ion beam was applied to investigate ion charge effect on induction of DNA transfer. Argon ion beam at 7.5 keV was neutralized by RF-driven plasma in the beam path and then bombarded cellulose membranes which were used as the mimetic plant cell envelope. Electrical properties such as impedance and capacitance of the membranes were measured after the bombardment. An in vitro experiment on plasmid DNA transfer through the cellulose membrane was followed up. The results showed that the ion charge input played an important role in the impedance and capacitance changes which would affect DNA transfer. Generally speaking, neutral particle beam bombardment of biologic cells was more effective in inducing DNA transfer than charged ion beam bombardment.

Scientific Computation Application Partnerships in Materials and Chemical Sciences, Charge Transfer and Charge Transport in Photoactivated Systems, Developing Electron-Correlated Methods for Excited State Structure and Dynamics in the NWChem Software Suite

Energy Technology Data Exchange (ETDEWEB)

Cramer, Christopher J. [Univ. of Minnesota, Minneapolis, MN (United States)

2017-11-12

Charge transfer and charge transport in photoactivated systems are fundamental processes that underlie solar energy capture, solar energy conversion, and photoactivated catalysis, both organometallic and enzymatic. We developed methods, algorithms, and software tools needed for reliable treatment of the underlying physics for charge transfer and charge transport, an undertaking with broad applicability to the goals of the fundamental-interaction component of the Department of Energy Office of Basic Energy Sciences and the exascale initiative of the Office of Advanced Scientific Computing Research.

Luminescence and optical spectroscopy of charge transfer processes in solid solutions NiCMg1−CO and NixZn1−xO

International Nuclear Information System (INIS)

Sokolov, V.I.; Pustovarov, V.A.; Churmanov, V.N.; Gruzdev, N.B.; Uimin, M.A.; Byzov, I.V.; Druzhinin, A.V.; Mironova-Ulmane, N.A.

2016-01-01

In this work photoluminescence spectra for Ni c Mg 1−c O and Ni x Zn 1−x O solid solutions with the rock-salt crystal structure were obtained under synchrotron radiation excitation. Periodical peaks in the photoluminescence excitation spectrum of Ni c Mg 1−c O (c=0.008) have been discovered for a wide-gap oxide doped with 3d impurities for the first time. They can be considered as LO phonon repetitions of the narrow zero phonon line resulted from the optical transitions into the p–d charge transfer exciton [d 9 h] state. A close coincidence in energy of different peculiarities in the optical absorption and photoluminescence excitation spectra for the Ni c Mg 1−c O and Ni x Zn 1−x O solid solutions is due to the practically equal interatomic distances Ni–O in the investigated materials. The bulk of new experimental results is the trustworthy evidence that only the p–d charge transfer transitions manifest themselves in the spectral region of 3.5–6.5 eV. - Highlights: • Emission of Ni c Mg 1−c O nanocystals excited by synchrotron radiation is obtained. • LO phonon repetitions have been observed in PLE spectra of Ni c Mg 1−c O firstly for wide gap oxide materials doped with 3d impurities. • The [d 9 h] acceptor exciton state in Ni c Mg 1−c O (c=0.008) are indirectly revealed. • The begin of PLE spectra of Ni x Zn 1−x O are not virtually shifted with a change of composition x. • The near energy coincidence of absorption peaks for nanocrystals NiO and single crystal Ni c Mg 1−c O (c=0.0006) manifests itself.

Through space and through bridge channels of charge transfer at p-n nano-junctions: A DFT study

Energy Technology Data Exchange (ETDEWEB)

Dandu, Naveen [Department of Chemistry and Biochemistry, NDSU, Fargo, ND 58108 (United States); Tretiak, Sergei [Theoretical Division, Center for Nonlinear Studies (CNLS) and Center for Integrated Nanotechnologies (CINT), Los Alamos National Laboratory, Los Alamos, 57069, NM 87454 (United States); Kilina, Svetlana [Department of Chemistry and Biochemistry, NDSU, Fargo, ND 58108 (United States); Kilin, Dmitri, E-mail: Dmitri.Kilin@ndsu.edu [Department of Chemistry and Biochemistry, NDSU, Fargo, ND 58108 (United States)

2016-12-20

Highlights: • Properties of interacting QDs depend on the fashion of interaction: through-bond or through-space. • The disconnected and undoped dimer models shows FÓ§rster band formation. • Dimer models with some doping exhibit degenerate charge-transfer excitons. • p- and n-doped qds shows polarization at the interface. • A photoexcitation polarizes p-n interface, in relation to phototovoltaic effect. - Abstract: Details of charge density distribution at p-n nano interface are analyzed with density functional theory techniques using model system of dimers of doped silicon quantum dots interacting through bond and through space. Spatial distributions of transition densities between the ground and excited states suggest the character of essential electronic excitations, which have a FÓ§rster, bound, unbound, or charge transfer character. A redistribution of electronic density from n-impurities to p-impurities results in a ground state polarization and creates an offset of energies of the bands localized on p-doped quantum dot and the bands localized on n-doped quantum dot. Although impurities contribute very few orbitals to the total density, a ground state charge redistribution and polarization are both responsible for the presence of a large number of charge transfer excitations involving solely silicon orbitals.

Ultrafast dynamics of solvation and charge transfer in a DNA-based biomaterial.

Science.gov (United States)

Choudhury, Susobhan; Batabyal, Subrata; Mondol, Tanumoy; Sao, Dilip; Lemmens, Peter; Pal, Samir Kumar

2014-05-01

Charge migration along DNA molecules is a key factor for DNA-based devices in optoelectronics and biotechnology. The association of a significant amount of water molecules in DNA-based materials for the intactness of the DNA structure and their dynamic role in the charge-transfer (CT) dynamics is less documented in contemporary literature. In the present study, we have used a genomic DNA-cetyltrimethyl ammonium chloride (CTMA) complex, a technological important biomaterial, and Hoechest 33258 (H258), a well-known DNA minor groove binder, as fluorogenic probe for the dynamic solvation studies. The CT dynamics of CdSe/ZnS quantum dots (QDs; 5.2 nm) embedded in the as-prepared and swollen biomaterial have also been studied and correlated with that of the timescale of solvation. We have extended our studies on the temperature-dependent CT dynamics of QDs in a nanoenvironment of an anionic, sodium bis(2-ethylhexyl)sulfosuccinate reverse micelle (AOT RMs), whereby the number of water molecules and their dynamics can be tuned in a controlled manner. A direct correlation of the dynamics of solvation and that of the CT in the nanoenvironments clearly suggests that the hydration barrier within the Arrhenius framework essentially dictates the charge-transfer dynamics. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Refrigerant charge, pressure drop, and condensation heat transfer in flattened tubes

Energy Technology Data Exchange (ETDEWEB)

Wilson, M J; Newell, T A; Chato, J C [University of Illinois, Urbana, IL (United States). Dept. of Mechanical and Industrial Engineering; Infante Ferreira, C A [Delft University of Technology (Netherlands). Laboratory for Refrigeration and Indoor Climate Control

2003-06-01

Horizontal smooth and microfinned copper tubes with an approximate diameter of 9 mm were successively flattened in order to determine changes in flow field characteristics as a round tube is altered into a flattened tube profile. Refrigerants R134a and R410A were investigated over a mass flux range from 75 to 400 kg m{sup -2} s{sup -}2{sup 1} and a quality range from approximately 10-80%. For a given refrigerant mass flow rate, the results show that a significant reduction in refrigerant charge is possible. Pressure drop results show increases of pressure drop at a given mass flux and quality as a tube profile is flattened. Heat transfer results indicate enhancement of the condensation heat transfer coefficient as a tube is flattened. Flattened tubes with an 18{sup o} helix angle displayed the highest heat transfer coefficients. Smooth tubes and axial microfin tubes displayed similar levels of heat transfer enhancement. Heat transfer enhancement is dependent on the mass flux, quality and tube profile. (author)

Highly mobile charge-transfer excitons in two-dimensional WS2/tetracene heterostructures

Science.gov (United States)

Zhu, Tong; Yuan, Long; Zhao, Yan; Zhou, Mingwei; Wan, Yan; Mei, Jianguo; Huang, Libai

2018-01-01

Charge-transfer (CT) excitons at heterointerfaces play a critical role in light to electricity conversion using organic and nanostructured materials. However, how CT excitons migrate at these interfaces is poorly understood. We investigate the formation and transport of CT excitons in two-dimensional WS2/tetracene van der Waals heterostructures. Electron and hole transfer occurs on the time scale of a few picoseconds, and emission of interlayer CT excitons with a binding energy of ~0.3 eV has been observed. Transport of the CT excitons is directly measured by transient absorption microscopy, revealing coexistence of delocalized and localized states. Trapping-detrapping dynamics between the delocalized and localized states leads to stretched-exponential photoluminescence decay with an average lifetime of ~2 ns. The delocalized CT excitons are remarkably mobile with a diffusion constant of ~1 cm2 s−1. These highly mobile CT excitons could have important implications in achieving efficient charge separation. PMID:29340303

Quasi-four-body treatment of charge transfer in the collision of protons with atomic helium: I. Thomas related mechanisms

Science.gov (United States)

Safarzade, Zohre; Fathi, Reza; Shojaei Akbarabadi, Farideh; Bolorizadeh, Mohammad A.

2018-04-01

The scattering of a completely bare ion by atoms larger than hydrogen is at least a four-body interaction, and the charge transfer channel involves a two-step process. Amongst the two-step interactions of the high-velocity single charge transfer in an anion-atom collision, there is one whose amplitude demonstrates a peak in the angular distribution of the cross sections. This peak, the so-called Thomas peak, was predicted by Thomas in a two-step interaction, classically, which could also be described through three-body quantum mechanical models. This work discusses a four-body quantum treatment of the charge transfer in ion-atom collisions, where two-step interactions illustrating a Thomas peak are emphasized. In addition, the Pauli exclusion principle is taken into account for the initial and final states as well as the operators. It will be demonstrated that there is a momentum condition for each two-step interaction to occur in a single charge transfer channel, where new classical interactions lead to the Thomas mechanism.

Theoretical perspectives on electron transfer and charge separation events in photochemical water cleavage systems

International Nuclear Information System (INIS)

Kozak, J.J.; Lenoir, P.M.; Musho, M.K.; Tembe, B.L.

1984-01-01

We study in this paper the dynamics induced by models for photochemical water cleavage systems, focusing on the spatial and temporal factors influencing electron transfer and charge separation processes in such systems. The reaction-diffusion theory is formulated in full generality and the consequences explored in a number of spatio-temporal regimes, viz. the spatially homogeneous system in the long-time limit (i.e. the steady state for a well-stirred system), the spatially homogeneous system in evolution, and the spatially inhomogeneous system in evolution (where, in the latter study, we consider electron transfer at the cluster surface to be governed by a rate constant that reflects the localized nature of such processes). The results of numerical simulations are presented for all three cases and used to highlight the importance of heterogeneous environments in enhancing the cage escape yield of charge separated species, and to demonstrate the dependence of the hydrogen yield on the localization of electron-transfer processes in the vicinity of the microcatalyst surface

An accurate and linear-scaling method for calculating charge-transfer excitation energies and diabatic couplings

Energy Technology Data Exchange (ETDEWEB)

Pavanello, Michele [Department of Chemistry, Rutgers University, Newark, New Jersey 07102-1811 (United States); Van Voorhis, Troy [Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139-4307 (United States); Visscher, Lucas [Amsterdam Center for Multiscale Modeling, VU University, De Boelelaan 1083, 1081 HV Amsterdam (Netherlands); Neugebauer, Johannes [Theoretische Organische Chemie, Organisch-Chemisches Institut der Westfaelischen Wilhelms-Universitaet Muenster, Corrensstrasse 40, 48149 Muenster (Germany)

2013-02-07

Quantum-mechanical methods that are both computationally fast and accurate are not yet available for electronic excitations having charge transfer character. In this work, we present a significant step forward towards this goal for those charge transfer excitations that take place between non-covalently bound molecules. In particular, we present a method that scales linearly with the number of non-covalently bound molecules in the system and is based on a two-pronged approach: The molecular electronic structure of broken-symmetry charge-localized states is obtained with the frozen density embedding formulation of subsystem density-functional theory; subsequently, in a post-SCF calculation, the full-electron Hamiltonian and overlap matrix elements among the charge-localized states are evaluated with an algorithm which takes full advantage of the subsystem DFT density partitioning technique. The method is benchmarked against coupled-cluster calculations and achieves chemical accuracy for the systems considered for intermolecular separations ranging from hydrogen-bond distances to tens of Angstroms. Numerical examples are provided for molecular clusters comprised of up to 56 non-covalently bound molecules.

Excited State Structural Dynamics of Carotenoids and ChargeTransfer Systems

Energy Technology Data Exchange (ETDEWEB)

Van Tassle, Aaron Justin [Univ. of California, Berkeley, CA (United States)

2006-01-01

This dissertation describes the development andimplementation of a visible/near infrared pump/mid-infrared probeapparatus. Chapter 1 describes the background and motivation ofinvestigating optically induced structural dynamics, paying specificattention to solvation and the excitation selection rules of highlysymmetric molecules such as carotenoids. Chapter 2 describes thedevelopment and construction of the experimental apparatus usedthroughout the remainder of this dissertation. Chapter 3 will discuss theinvestigation of DCM, a laser dye with a fluorescence signal resultingfrom a charge transfer state. By studying the dynamics of DCM and of itsmethyl deuterated isotopomer (an otherwise identical molecule), we areable to investigate the origins of the charge transfer state and provideevidence that it is of the controversial twisted intramolecular (TICT)type. Chapter 4 introduces the use of two-photon excitation to the S1state, combined with one-photon excitation to the S2 state of thecarotenoid beta-apo-8'-carotenal. These 2 investigations show evidencefor the formation of solitons, previously unobserved in molecular systemsand found only in conducting polymers Chapter 5 presents an investigationof the excited state dynamics of peridinin, the carotenoid responsiblefor the light harvesting of dinoflagellates. This investigation allowsfor a more detailed understanding of the importance of structuraldynamics of carotenoids in light harvesting.

GapBlaster-A Graphical Gap Filler for Prokaryote Genomes.

Directory of Open Access Journals (Sweden)

Pablo H C G de Sá

Full Text Available The advent of NGS (Next Generation Sequencing technologies has resulted in an exponential increase in the number of complete genomes available in biological databases. This advance has allowed the development of several computational tools enabling analyses of large amounts of data in each of the various steps, from processing and quality filtering to gap filling and manual curation. The tools developed for gap closure are very useful as they result in more complete genomes, which will influence downstream analyses of genomic plasticity and comparative genomics. However, the gap filling step remains a challenge for genome assembly, often requiring manual intervention. Here, we present GapBlaster, a graphical application to evaluate and close gaps. GapBlaster was developed via Java programming language. The software uses contigs obtained in the assembly of the genome to perform an alignment against a draft of the genome/scaffold, using BLAST or Mummer to close gaps. Then, all identified alignments of contigs that extend through the gaps in the draft sequence are presented to the user for further evaluation via the GapBlaster graphical interface. GapBlaster presents significant results compared to other similar software and has the advantage of offering a graphical interface for manual curation of the gaps. GapBlaster program, the user guide and the test datasets are freely available at https://sourceforge.net/projects/gapblaster2015/. It requires Sun JDK 8 and Blast or Mummer.

Exciplex: An Intermolecular Charge-Transfer Approach for TADF.

Science.gov (United States)

Sarma, Monima; Wong, Ken-Tsung

2018-04-03

Organic materials that display thermally activated delayed fluorescence (TADF) are a striking class of functional materials that have witnessed a booming progress in recent years. In addition to pure TADF emitters achieved by the subtle manipulations of intramolecular charge transfer processes with sophisticated molecular structures, a new class of efficient TADF-based OLEDs with emitting layer formed by blending electron donor and acceptor molecules that involve intermolecular charge transfer have also been fabricated. In contrast to pure TADF materials, the exciplex-based systems can realize small ΔEST (0-0.05 eV) much more easily since the electron and hole are positioned on two different molecules, thereby giving small exchange energy. Consequently, exciplex-based OLEDs have the prospective to maximize the TADF contribution and achieve theoretical 100% internal quantum efficiency. Therefore, the challenging issue of achieving small ΔEST in organic systems could be solved. In this article, we summarize and discuss the latest and most significant developments regarding these rapidly evolving functional materials, wherein the majority of the reported exciplex forming systems are categorized into two sub-groups, viz. (a) exciplex as TADF emitters and (b) those as hosts for fluorescent, phosphorescent and TADF dopants according to their structural features and applications. The working mechanisms of the direct electroluminescence from the donor/acceptor interface and the exciplex-forming systems as co-host for the realization of high efficiency OLEDs are reviewed and discussed. This article delivers a summary of the current progresses and achievements of exciplex-based researches and points out the future challenges to trigger more research endeavors to this growing field.

Numerical analysis of turbulent flow and heat transfer in a square sectioned U-bend duct by elliptic-blending second moment closure

International Nuclear Information System (INIS)

Shin, Jong Keun; Choi, Young Don; An, Jeong Soo

2007-01-01

A second moment turbulence closure using the elliptic-blending equation is introduced to analyze the turbulence and heat transfer in a square sectioned U-bend duct flow. The turbulent heat flux model based on the elliptic concept satisfies the near-wall balance between viscous diffusion, viscous dissipation and temperature-pressure gradient correlation, and also has the characteristics of approaching its respective conventional high Reynolds number model far away from the wall. Also, the traditional GGDH heat flux model is compared with the present elliptic concept-based heat flux model. The turbulent heat flux models are closely linked to the elliptic blending second moment closure which is used for the prediction of Reynolds stresses. The predicted results show their reasonable agreement with experimental data for a square sectioned U-bend duct flow field adopted in the present study

Physical adsorption and charge transfer of molecular Br2 on graphene.

Science.gov (United States)

Chen, Zheyuan; Darancet, Pierre; Wang, Lei; Crowther, Andrew C; Gao, Yuanda; Dean, Cory R; Taniguchi, Takashi; Watanabe, Kenji; Hone, James; Marianetti, Chris A; Brus, Louis E

2014-03-25

We present a detailed study of gaseous Br2 adsorption and charge transfer on graphene, combining in situ Raman spectroscopy and density functional theory (DFT). When graphene is encapsulated by hexagonal boron nitride (h-BN) layers on both sides, in a h-BN/graphene/h-BN sandwich structure, it is protected from doping by strongly oxidizing Br2. Graphene supported on only one side by h-BN shows strong hole doping by adsorbed Br2. Using Raman spectroscopy, we determine the graphene charge density as a function of pressure. DFT calculations reveal the variation in charge transfer per adsorbed molecule as a function of coverage. The molecular adsorption isotherm (coverage versus pressure) is obtained by combining Raman spectra with DFT calculations. The Fowler-Guggenheim isotherm fits better than the Langmuir isotherm. The fitting yields the adsorption equilibrium constant (∼0.31 Torr(-1)) and repulsive lateral interaction (∼20 meV) between adsorbed Br2 molecules. The Br2 molecule binding energy is ∼0.35 eV. We estimate that at monolayer coverage each Br2 molecule accepts 0.09 e- from single-layer graphene. If graphene is supported on SiO2 instead of h-BN, a threshold pressure is observed for diffusion of Br2 along the (somewhat rough) SiO2/graphene interface. At high pressure, graphene supported on SiO2 is doped by adsorbed Br2 on both sides.

Active pixel sensor having intra-pixel charge transfer with analog-to-digital converter

Science.gov (United States)

Fossum, Eric R. (Inventor); Mendis, Sunetra K. (Inventor); Pain, Bedabrata (Inventor); Nixon, Robert H. (Inventor); Zhou, Zhimin (Inventor)

2003-01-01

An imaging device formed as a monolithic complementary metal oxide semiconductor integrated circuit in an industry standard complementary metal oxide semiconductor process, the integrated circuit including a focal plane array of pixel cells, each one of the cells including a photogate overlying the substrate for accumulating photo-generated charge in an underlying portion of the substrate, a readout circuit including at least an output field effect transistor formed in the substrate, and a charge coupled device section formed on the substrate adjacent the photogate having a sensing node connected to the output transistor and at least one charge coupled device stage for transferring charge from the underlying portion of the substrate to the sensing node and an analog-to-digital converter formed in the substrate connected to the output of the readout circuit.

Photoinduced Charge Transfer from Titania to Surface Doping Site.

Science.gov (United States)

Inerbaev, Talgat; Hoefelmeyer, James D; Kilin, Dmitri S

2013-05-16

We evaluate a theoretical model in which Ru is substituting for Ti at the (100) surface of anatase TiO 2 . Charge transfer from the photo-excited TiO 2 substrate to the catalytic site triggers the photo-catalytic event (such as water oxidation or reduction half-reaction). We perform ab-initio computational modeling of the charge transfer dynamics on the interface of TiO 2 nanorod and catalytic site. A slab of TiO 2 represents a fragment of TiO 2 nanorod in the anatase phase. Titanium to ruthenium replacement is performed in a way to match the symmetry of TiO 2 substrate. One molecular layer of adsorbed water is taken into consideration to mimic the experimental conditions. It is found that these adsorbed water molecules saturate dangling surface bonds and drastically affect the electronic properties of systems investigated. The modeling is performed by reduced density matrix method in the basis of Kohn-Sham orbitals. A nano-catalyst modeled through replacement defect contributes energy levels near the bottom of the conduction band of TiO 2 nano-structure. An exciton in the nano-rod is dissipating due to interaction with lattice vibrations, treated through non-adiabatic coupling. The electron relaxes to conduction band edge and then to the Ru cite with faster rate than hole relaxes to the Ru cite. These results are of the importance for an optimal design of nano-materials for photo-catalytic water splitting and solar energy harvesting.

Four- and six-charge transfer reactions induced by 52Cr, 56Fe, 63Cu in rare-earths

International Nuclear Information System (INIS)

Mouchaty, G.

1977-01-01

The cross sections for transfer reactions in which 4 and 6 charges are gained by Sm and Nd targets have been measured, the projectiles being 52 Cr and 56 Fe at 343 and 377 MeV. These energies correspond to 1.5B, B being the interaction barrier. The results obtained indicate that the cross section increases when the number of charges transferred and the mass of the projectile are increased. The angular distributions and recoil ranges at each angle of 151 Dy produced through 52 Cr+ 148 Sm, 52 Cr+ 144 Nd, 56 Fe+ 144 Nd, 63 Cu+ 144 Nd reactions were determined for incident energies equivalent to 1.5B. After transformation into the c.m. system, the angular distributions exhibit a maximum close to 155 0 and a tail at small angles. The position of the maximum is independent of the incident ion and of the number of transferred charges. The analysis of the energy distributions indicate that the observed reactions can be explained by a two-step process: a transfer of nucleons followed by an evaporation step. The number of nucleons transferred in the 1st step and the associated excitation energies are higher for the events corresponding to the tail than for those corresponding to the maximum [fr

Study on charge transfer reaction of several organic molecules with accelerated rare gas ions

International Nuclear Information System (INIS)

Takahasi, Makoto; Okuda, Sachiko; Arai, Eiichi; Ichinose, Akira; Takakubo, Masaaki.

1984-01-01

Observing the charge transfer mass spectra of ethylbenzene, cyclobutane and methanol in Ar and Xe ion impacts, we investigated the dependence of the secondary ion peak intensities (normalized to primary ion current and target pressure) on the translational energy of primary ions (0-3500 eV).In the case of ethylbenzene, several maxima of the secondary i on peak intensities were observed in Ar and Xe ion impacts. The correlation between the maxima and the primary ion energy was examined in terms of near adiabatic theory of Massey. Supplementary studies on the energy distribution of primary ion, charge transfer cross section between methanol and Xe ion, and final product analysis in rare gas ion irradiation on cyclobutane were described. (author)

Radioactive beam EXperiments at ISOLDE : Coulomb excitation and neutron transfer reactions of exotic nuclei.

CERN Multimedia

Kugler, E; Ratzinger, U; Wenander, F J C

2002-01-01

% IS347 \\\\ \\\\We propose to perform a pilot experiment to study very neutron rich (A<32) Na-Mg and (A<52) K-Ca isotopes in the region around the neutron shell closures of N=20 and N=28 after Coulomb excitation and neutron transfer, and to demonstrate highly efficient and cost-effective ways to bunch, charge-state breed and accelerate already existing mass-separated singly-charged radioactive ion beams. \\\\ \\\\To do this we plan to accelerate the ISOLDE beams up to 2~MeV/u by means of a novel acceleration scheme and to install an efficient $\\gamma$-ray array for low-multiplicity events around the target position.

Near-surface gravity actuated pipe (GAP{sup TM}) system for Brazilian deepwater fluid transfer

Energy Technology Data Exchange (ETDEWEB)

Fromage, Lionel; Brown, Paul A. [SBM Offshore (Monaco)

2009-12-19

The recent discovery of new deep water and ultra-deep water oil and gas fields offshore Brazil, including pre-salt reservoirs, has become a focal point for field development Operators and Contractors. The aggressive nature of fluids (sour, high density) in combination with deeper waters implies potential flow assurance issues. These issues challenge riser and pipeline technology to find cost effective solutions for hydrocarbon fluid transfer in field development scenarios involving phased tied-back. The near-surface GAP{sup TM}, system (Gravity Actuated Pipe{sup TM}), which has been in operation for more than two years on the Kikeh field offshore Malaysia in 1325 m of water between a Dry Tree Unit (SPAR) and a turret-moored FPSO, is considered to meet these challenges since such a product is quasi independent of water depth and takes advantage of being near surface to optimize flow assurance. Furthermore the GAP{sup TM} has undergone technical upgrades when compared to the Kikeh project in order to make it suitable for the more hostile met ocean conditions offshore Brazil. This paper presents the design features, the construction and assembly plans in Brazil and the offshore installation of a GAP fluid transfer system for operation in Brazilian deep waters. (author)

Negative thermal expansion induced by intermetallic charge transfer.

Science.gov (United States)

Azuma, Masaki; Oka, Kengo; Nabetani, Koichiro

2015-06-01

Suppression of thermal expansion is of great importance for industry. Negative thermal expansion (NTE) materials which shrink on heating and expand on cooling are therefore attracting keen attention. Here we provide a brief overview of NTE induced by intermetallic charge transfer in A-site ordered double perovskites SaCu 3 Fe 4 O 12 and LaCu 3 Fe 4- x Mn x O 12 , as well as in Bi or Ni substituted BiNiO 3 . The last compound shows a colossal dilatometric linear thermal expansion coefficient exceeding -70 × 10 -6 K -1 near room temperature, in the temperature range which can be controlled by substitution.

Theoretical investigation of the charge-transfer properties in different meso-linked zinc porphyrins for highly efficient dye-sensitized solar cells.

Science.gov (United States)

Namuangruk, Supawadee; Sirithip, Kanokkorn; Rattanatwan, Rattanawelee; Keawin, Tinnagon; Kungwan, Nawee; Sudyodsuk, Taweesak; Promarak, Vinich; Surakhot, Yaowarat; Jungsuttiwong, Siriporn

2014-06-28

The charge transfer effect of different meso-substituted linkages on porphyrin analogue 1 (A1, B1 and C1) was theoretically investigated using density functional theory (DFT) and time-dependent DFT (TDDFT) calculations. The calculated geometry parameters and natural bond orbital analysis reveal that the twisted conformation between porphyrin macrocycle and meso-substituted linkages leads to blocking of the conjugation of the conjugated backbone, and the frontier molecular orbital plot shows that the intramolecular charge transfer of A1, B1 and C1 hardly takes place. In an attempt to improve the photoinduced intramolecular charge transfer ability of the meso-linked zinc porphyrin sensitizer, a strong electron-withdrawing group (CN) was introduced into the anchoring group of analogue 1 forming analogue 2 (A2, B2 and C2). The density difference plot of A2, B2 and C2 shows that the charge transfer properties dramatically improved. The electron injection process has been performed using TDDFT; the direct charge-transfer transition in the A2-(TiO2)38 interacting system takes place; our results strongly indicated that introducing electron-withdrawing groups into the acceptor part of porphyrin dyes can fine-tune the effective conjugation length of the π-spacer and improve intramolecular charge transfer properties, consequently inducing the electron injection process from the anchoring group of the porphyrin dye to the (TiO2)38 surface which may improve the conversion efficiency of the DSSCs. Our calculated results can provide valuable information and a promising outlook for computation-aided sensitizer design with anticipated good properties in further experimental synthesis.

Collisions of fast multicharged ions in gas targets: charge transfer and ionization

International Nuclear Information System (INIS)

Schlachter, A.S.

1981-05-01

Measurements of cross sections for charge transfer and ionization of H 2 and rare-gas targets have been made with fast, highly stripped projectiles in charge states as high as 59+. We have found an empirical scaling rule for electron-capture cross section in H 2 valid at energies above 275 keV/amu. Similar scaling might exist for other target gases. Cross sections are generally in good agreement with theory. We have found a scaling rule for electron loss from H in collisions with a fast highly stripped projectile, based on Olson's classical-trajectory Monte-Carlo calculations, and confirmed by measurements in an H 2 target. We have found a similar scaling rule for net ionization of rare-gas targets, based on Olson's CTMC calculations and the independent-electron model. Measurements are essentially consistent with the scaled cross sections. Calculations and measurements of recoil-ion charge-state spectra show large cross sections for the production of highly charged slow recoil ions

Structural dynamics of a noncovalent charge transfer complex from femtosecond stimulated Raman spectroscopy.

Science.gov (United States)

Fujisawa, Tomotsumi; Creelman, Mark; Mathies, Richard A

2012-09-06

Femtosecond stimulated Raman spectroscopy is used to examine the structural dynamics of photoinduced charge transfer within a noncovalent electron acceptor/donor complex of pyromellitic dianhydride (PMDA, electron acceptor) and hexamethylbenzene (HMB, electron donor) in ethylacetate and acetonitrile. The evolution of the vibrational spectrum reveals the ultrafast structural changes that occur during the charge separation (Franck-Condon excited state complex → contact ion pair) and the subsequent charge recombination (contact ion pair → ground state complex). The Franck-Condon excited state is shown to have significant charge-separated character because its vibrational spectrum is similar to that of the ion pair. The charge separation rate (2.5 ps in ethylacetate and ∼0.5 ps in acetonitrile) is comparable to solvation dynamics and is unaffected by the perdeuteration of HMB, supporting the dominant role of solvent rearrangement in charge separation. On the other hand, the charge recombination slows by a factor of ∼1.4 when using perdeuterated HMB, indicating that methyl hydrogen motions of HMB mediate the charge recombination process. Resonance Raman enhancement of the HMB vibrations in the complex reveals that the ring stretches of HMB, and especially the C-CH(3) deformations are the primary acceptor modes promoting charge recombination.

Telephone switchboard closure | 19 December

CERN Multimedia

2014-01-01

Exceptionally, the telephone switchboard will close at 4 p.m. on Friday, 19 December, instead of the usual time of 6 p.m., to allow time for closing all systems properly before the annual closure. Therefore, switchboard operator assistance to transfer calls from/to external lines will stop. All other phone services will run as usual.

Crossed beam study of He+-O2 charge transfer reactions in the collision energy range 0.5-200 eV

International Nuclear Information System (INIS)

Bischof, G.; Linder, F.

1986-01-01

Energy spectra and angular distributions of the O + and O 2 + product ions resulting from the He + -O 2 charge transfer reaction have been measured in the collision energy range 0.5-200 eV using the crossed-beam method. The O 2 + ions represent only a minor fraction of the reaction products (0.2-0.6% over the energy range measured). In the dissociative charge transfer reaction, four main processes are identified leading to O+O + reaction products in different electronic states. Two different mechanisms can be distinguished, each being responsible for two of the observed processes: (i) a long-distance energy-resonant charge transfer process involving the c 4 Σsub(u) - (upsilon'=0) state of O 2 + and (ii) a slightly exothermic charge transfer process via the (III) 2 PIsub(u) state of O 2 + (with the exothermicity depending on the collision energy). Angle-integrated branching ratios and partial cross sections (in absolute units) have been determined. The branching ratios of the individual processes show a pronounced dependence on the collision energy. At low energies, the O + product ions are preferentially formed in the 2 P 0 and 2 D 0 excited states. The angular distributions of the O + product ions show an anisotropic behaviour indicating an orientation-dependent charge transfer probability in the He + -O 2 reaction. (orig.)

The Development of Layered Photonic Band Gap Structures Using a Micro-Transfer Molding Technique

International Nuclear Information System (INIS)

Kevin Jerome Sutherland

2001-01-01

Photonic band gap (PBG) crystals are periodic dielectric structures that manipulate electromagnetic radiation in a manner similar to semiconductor devices manipulating electrons. Whereas a semiconductor material exhibits an electronic band gap in which electrons cannot exist, similarly, a photonic crystal containing a photonic band gap does not allow the propagation of specific frequencies of electromagnetic radiation. This phenomenon results from the destructive Bragg diffraction interference that a wave propagating at a specific frequency will experience because of the periodic change in dielectric permitivity. This gives rise to a variety of optical applications for improving the efficiency and effectiveness of opto-electronic devices. These applications are reviewed later. Several methods are currently used to fabricate photonic crystals, which are also discussed in detail. This research involves a layer-by-layer micro-transfer molding ((mu)TM) and stacking method to create three-dimensional FCC structures of epoxy or titania. The structures, once reduced significantly in size can be infiltrated with an organic gain media and stacked on a semiconductor to improve the efficiency of an electronically pumped light-emitting diode. Photonic band gap structures have been proven to effectively create a band gap for certain frequencies of electro-magnetic radiation in the microwave and near-infrared ranges. The objective of this research project was originally two-fold: to fabricate a three dimensional (3-D) structure of a size scaled to prohibit electromagnetic propagation within the visible wavelength range, and then to characterize that structure using laser dye emission spectra. As a master mold has not yet been developed for the micro transfer molding technique in the visible range, the research was limited to scaling down the length scale as much as possible with the current available technology and characterizing these structures with other methods

The Development of Layered Photonic Band Gap Structures Using a Micro-Transfer Molding Technique

Energy Technology Data Exchange (ETDEWEB)

Sutherland, Kevin Jerome [Iowa State Univ., Ames, IA (United States)

2001-01-01

Photonic band gap (PBG) crystals are periodic dielectric structures that manipulate electromagnetic radiation in a manner similar to semiconductor devices manipulating electrons. Whereas a semiconductor material exhibits an electronic band gap in which electrons cannot exist, similarly, a photonic crystal containing a photonic band gap does not allow the propagation of specific frequencies of electromagnetic radiation. This phenomenon results from the destructive Bragg diffraction interference that a wave propagating at a specific frequency will experience because of the periodic change in dielectric permitivity. This gives rise to a variety of optical applications for improving the efficiency and effectiveness of opto-electronic devices. These applications are reviewed later. Several methods are currently used to fabricate photonic crystals, which are also discussed in detail. This research involves a layer-by-layer micro-transfer molding ({mu}TM) and stacking method to create three-dimensional FCC structures of epoxy or titania. The structures, once reduced significantly in size can be infiltrated with an organic gain media and stacked on a semiconductor to improve the efficiency of an electronically pumped light-emitting diode. Photonic band gap structures have been proven to effectively create a band gap for certain frequencies of electro-magnetic radiation in the microwave and near-infrared ranges. The objective of this research project was originally two-fold: to fabricate a three dimensional (3-D) structure of a size scaled to prohibit electromagnetic propagation within the visible wavelength range, and then to characterize that structure using laser dye emission spectra. As a master mold has not yet been developed for the micro transfer molding technique in the visible range, the research was limited to scaling down the length scale as much as possible with the current available technology and characterizing these structures with other methods.

Ambiguity in knowledge transfer: The role of theory-practice gap.

Science.gov (United States)

Cheraghi, Mohammad Ali; Salsali, Mahvash; Safari, Mahmoud

2010-01-01

In spite of much literature written about the theory-practice gap in the international nursing journals, there is evidence that indicates this subject has not been probed comprehensively since nursing education was transferred to universities in Iran. In the recent years, the public and the government have criticized Iranian nurses because of poor quality of patient care. Although this subject has been lamented by some researchers, there is no comprehensive work on how this gap resulted. In the process of a larger study on "nursing knowledge translation to practice", of one PhD thesis, this process was explored. Using grounded theory analysis, indepth interviews were undertaken with a purposive sample of 29 nurses, with different levels of experience, from the school of nursing in Tehran University of Medical Sciences in 2006 from January to August. Data were analyzed using the constant comparative method. Three main themes emerging from this study included clinical behavior structure, paradoxical knowledge and practice, and divergent nursing organization. It seems that nursing education with some praxis and paradoxes in the realm of nursing knowledge and practice, along with divergent organizational structure have decreased nurses' ability in applying their professional knowledge and skills in order to bridge the gap between theory and practice. Moreover, in spite of increased academic input into nursing education, clinical behaviors of both education and practice settings was perceived as "traditional routine-based".

Synthesis and Exciton Dynamics of Donor-Orthogonal Acceptor Conjugated Polymers: Reducing the Singlet–Triplet Energy Gap

KAUST Repository

Freeman, David M. E.; Musser, Andrew J.; Frost, Jarvist M.; Stern, Hannah L.; Forster, Alexander K.; Fallon, Kealan J.; Rapidis, Alexandros G.; Cacialli, Franco; McCulloch, Iain; Clarke, Tracey M.; Friend, Richard H.; Bronstein, Hugo

2017-01-01

The presence of energetically low-lying triplet states is a hallmark of organic semiconductors. Even though they present a wealth of interesting photophysical properties, these optically dark states significantly limit optoelectronic device performance. Recent advances in emissive charge-transfer molecules have pioneered routes to reduce the energy gap between triplets and

Synthesis and Exciton Dynamics of Donor-Orthogonal Acceptor Conjugated Polymers: Reducing the Singlet–Triplet Energy Gap

KAUST Repository

Freeman, David M. E.

2017-06-09

The presence of energetically low-lying triplet states is a hallmark of organic semiconductors. Even though they present a wealth of interesting photophysical properties, these optically dark states significantly limit optoelectronic device performance. Recent advances in emissive charge-transfer molecules have pioneered routes to reduce the energy gap between triplets and

Charge-Transfer-Induced p-Type Channel in MoS2 Flake Field Effect Transistors.

Science.gov (United States)

Min, Sung-Wook; Yoon, Minho; Yang, Sung Jin; Ko, Kyeong Rok; Im, Seongil

2018-01-31

The two-dimensional transition-metal dichalcogenide semiconductor MoS 2 has received extensive attention for decades because of its outstanding electrical and mechanical properties for next-generation devices. One weakness of MoS 2 , however, is that it shows only n-type conduction, revealing its limitations for homogeneous PN diodes and complementary inverters. Here, we introduce a charge-transfer method to modify the conduction property of MoS 2 from n- to p-type. We initially deposited an n-type InGaZnO (IGZO) film on top of the MoS 2 flake so that electron charges might be transferred from MoS 2 to IGZO during air ambient annealing. As a result, electron charges were depleted in MoS 2 . Such charge depletion lowered the MoS 2 Fermi level, which makes hole conduction favorable in MoS 2 when optimum source/drain electrodes with a high work function are selected. Our IGZO-supported MoS 2 flake field effect transistors (FETs) clearly display channel-type conversion from n- to p-channel in this way. Under short- and long-annealing conditions, n- and p-channel MoS 2 FETs are achieved, respectively, and a low-voltage complementary inverter is demonstrated using both channels in a single MoS 2 flake.

Band gap opening in silicene on MgBr2(0001) induced by Li and Na

KAUST Repository

Zhu, Jiajie

2014-11-12

Silicene consists of a monolayer of Si atoms in a buckled honeycomb structure and is expected to be well compatible with the current Si-based technology. However, the band gap is strongly influenced by the substrate. In this context, the structural and electronic properties of silicene on MgBr2(0001) modified by Li and Na are investigated by first-principles calculations. Charge transfer from silicene (substrate) to substrate (silicene) is found for substitutional doping (intercalation). As compared to a band gap of 0.01 eV on the pristine substrate, strongly enhanced band gaps of 0.65 eV (substitutional doping) and 0.24 eV (intercalation) are achieved. The band gap increases with the dopant concentration.

Excitation and charge transfer in low-energy hydrogen atom collisions with neutral iron

Science.gov (United States)

Barklem, P. S.

2018-05-01

Data for inelastic processes due to hydrogen atom collisions with iron are needed for accurate modelling of the iron spectrum in late-type stars. Excitation and charge transfer in low-energy Fe+H collisions is studied theoretically using a previously presented method based on an asymptotic two-electron linear combination of atomic orbitals model of ionic-covalent interactions in the neutral atom-hydrogen-atom system, together with the multi-channel Landau-Zener model. An extensive calculation including 166 covalent states and 25 ionic states is presented and rate coefficients are calculated for temperatures in the range 1000-20 000 K. The largest rates are found for charge transfer processes to and from two clusters of states around 6.3 and 6.6 eV excitation, corresponding in both cases to active 4d and 5p electrons undergoing transfer. Excitation and de-excitation processes among these two sets of states are also significant. Full Tables and rate coefficient data are only available at the CDS via anonymous ftp to cdsarc.u-strasbg.fr (130.79.128.5) or via http://cdsarc.u-strasbg.fr/viz-bin/qcat?J/A+A/612/A90

Mechanism of the Primary Charge Transfer Reaction in the Cytochrome bc1 Complex

DEFF Research Database (Denmark)

Barragan, Angela M; Schulten, Klaus; Solov'yov, Ilia A

2016-01-01

, the quinol-protein interaction, which initiates the Q-cycle, has not yet been completely described. Furthermore, the initial charge transfer reactions of the Q-cycle lack a physical description. The present investigation utilizes classical molecular dynamics simulations in tandem with quantum density...

Transfer of momentum, mass and charge in heavy ion collisions

International Nuclear Information System (INIS)

Beck, F.; Feldmeier, H.; Dworzecka, M.

1979-01-01

A model for the first two phases of heavy ion collisions based on the transport of single nucleons through the window between the two scattering nuclei is described in some detail. It is pointed out that the model can account simultaneously for a large portion of the energy transfer from relative to intrinsic motion and for the observed variances in mass and charge numbers for reaction times up to the order of 10 -21 s. (P.L.)

Modified silicone sling assisted temporalis muscle transfer in the management of lagophthalmos

Directory of Open Access Journals (Sweden)

Ramesh C Gupta

2014-01-01

Full Text Available Aim : To evaluate the efficacy of modified temporalis muscle transfer (TMT by silicone sling for the management of paralytic lagophthalmos. Settings and Design: Prospective interventional study. Materials and Methods : Ten patients of lagophthalmos due to facial palsy underwent modified TMT using silicone sling. The patients were followed-up for a period of 3 months. Palpebral aperture in primary gaze and during eye closure were assessed both pre- and postoperatively along with problems associated with lagophthalmos like exposure keratopathy and lacrimation. Statistical Analysis : Paired t-test was applied to measure the statistical outcome. Results : Eight patients achieved full correction of lagophthalmos with no lid gap on closing the eye. The mean (standard deviation (SD lid gap on eye closure was 7.7 (0.86 mm preoperatively, 0.5 (0.47 mm at 1 st postoperative day, and 0.7 (0.75 mm at 3 rd month. There was a reduction in mean lid gap on eye closure of 7 mm at 3 months (P < 0.0001 which is highly significant. The mean (SD vertical interpalpebral distance during primary gaze was 12.05 (1.12 mm preoperatively, 10 (0.94 mm at 1 st postoperative day, and 10.35 (1.08 mm at 3 rd month. There was a reduction in mean vertical inter palpebral distance of 1.7 mm at 3 months (P = 0.001 which is significant. Exposure keratitis decreased in five out of six patients at 3 months. Conclusion : Modified TMT by silicone sling is a useful procedure with lesser morbidity and good outcomes for the treatment of paralytic lagophthalmos due to long standing facial palsy.

Engineering Interfacial Charge Transfer in CsPbBr3 Perovskite Nanocrystals by Heterovalent Doping

KAUST Repository

Begum, Raihana; Parida, Manas R.; Abdelhady, Ahmed L.; Banavoth, Murali; AlYami, Noktan; Ahmed, Ghada H.; Hedhili, Mohamed N.; Bakr, Osman; Mohammed, Omar F.

2016-01-01

Since compelling device efficiencies of perovskite solar cells have been achieved, investigative efforts have turned to understand other key challenges in these systems, such as engineering interfacial energy-level alignment and charge transfer (CT

Charge-Transfer Supra-Amphiphiles Built by Water-Soluble Tetrathiafulvalenes and Viologen-Containing Amphiphiles: Supramolecular Nanoassemblies with Modifiable Dimensions.

Science.gov (United States)

Lv, Zhong-Peng; Chen, Bin; Wang, Hai-Ying; Wu, Yue; Zuo, Jing-Lin

2015-08-05

In this study, multidimensional nanoassemblies with various morphologies such as nanosheets, nanorods, and nanofibers are developed via charge-transfer interaction and supra-amphiphile self-assembling in aqueous phase. The charge-transfer interactions between tetrathiafulvalene derivatives (TTFs) and methyl viologen derivatives (MVs) have been confirmed by the characteristic charger-transfer absorption. (1) H NMR and electrospray ionizsation mass spectrometry (ESI-MS) analyses also indicate supra-amphiphiles are formed by the combination of TTFs and MVs head group through charge-transfer interaction and Coulombic force. X-ray single crystal structural studies, transmission electron microscopy (TEM), and scanning electron microscopy (SEM) reveal that both linkage pattern of TTFs in hydrophilic part and alkane chain structure in hydrophobic part have significant influence on nanoassemblies morphology and microstructure. Moreover, gold nanoparticles (AuNPs) are introduced in the above supramolecular nanoassemblies to construct a supra-amphiphile-driven organic-AuNPs assembly system. AuNPs could be assembled into 1D-3D structures by adding different amount of MVs. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Oxygen-assisted charge transfer between ZnO quantum dots and graphene.

Science.gov (United States)

Guo, Wenhao; Xu, Shuigang; Wu, Zefei; Wang, Ning; Loy, M M T; Du, Shengwang

2013-09-23

Efficient charge transfer between ZnO quantum dots (QDs) and graphene is demonstrated by decorating ZnO QDs on top of graphene, with the assistance of oxygen molecules from the air. The electrical response of the device to UV light is greatly enhanced, and a photoconductive gain of up to 10(7) can be obtained. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Collisions of highly stripped ions at MeV energies in gas targets: charge transfer and ionization

International Nuclear Information System (INIS)

Schlachter, A.S.

1980-01-01

Cross sections have been measured for charge transfer and ionization in H 2 and rare-gas targets by fast, highly ionized carbon, iron, niobium, and lead ions in charge states +3 to +59, with energies in the range 0.1 to 4.8 MeV/amu. Experimental results are compared with classical-trajectory calculations; agreement is generally good. For a given target, the cross sections for net ionization reduce to a common curve when plotted as cross section divided by charge state versus energy per nucleon divided by charge state

Experimental study on in-vessel debris coolability; experiments on heat transfer in downward-facing hemicircular gap

Energy Technology Data Exchange (ETDEWEB)

Suh, Kune Yull; Kim, Yong Hoon; Kim, Seong Joong; Lee, Seung Dong [Seoul National University, Seoul (Korea)

2002-03-01

Experiments were performed to measure the CHF and the critical power and to investigate the heat transfer mechanism in the narrow gap with 2D slice test sections. Test parameters in this study included the gap size of 1, 2, 5, and 10mm and the system pressure from 0.1 to 1.0 MPa. The CHF was measured for the distilled water. Results of this study may be summarized as follows. 1) In the narrow gap size of 1 and 2mm, the CHF occurs at the bottom and propagates upwards as the inclination angle relative to gravitational force increases. 2) Dryout is the limiting heat transfer mechanism in the 2D sliced experiments, and the CHF reaches 80-90% of the 3D CHFG value. 3) In the narrow gap size of 1 and 2mm the CHF values lie on the order of 104 kW/m2, while in the gap sizes of 5 and 10mm the CHF values have an order of 105 kW/m2. 4) The flow visualization study revealed that the shape of bubble is elliptic and the hydrodynamic bubble diameter exceeds the size of 20mm. 5) In analyzing the CHF with the inclination angle of the heated surface in the narrow gap size of 1 and 2mm, there exists a transition angle in the vicinity of 20-30 .deg.. From the region of the inclination angle of 0 .deg. C to 20 .deg. C or 30 .deg. C, the dryout mechanism may be directly applicable. On the contrary the transition angle is not conspicuously seen in the gap sizes of 5 and 10mm in which dominant mechanism is closer to pool boiling. 27 refs., 29 figs., 8 tabs. (Author)

Excited State Structural Dynamics of Carotenoids and Charge Transfer Systems

International Nuclear Information System (INIS)

Van Tassle, Aaron Justin

2006-01-01

This dissertation describes the development and implementation of a visible/near infrared pump/mid-infrared probe apparatus. Chapter 1 describes the background and motivation of investigating optically induced structural dynamics, paying specific attention to solvation and the excitation selection rules of highly symmetric molecules such as carotenoids. Chapter 2 describes the development and construction of the experimental apparatus used throughout the remainder of this dissertation. Chapter 3 will discuss the investigation of DCM, a laser dye with a fluorescence signal resulting from a charge transfer state. By studying the dynamics of DCM and of its methyl deuterated isotopomer (an otherwise identical molecule), we are able to investigate the origins of the charge transfer state and provide evidence that it is of the controversial twisted intramolecular (TICT) type. Chapter 4 introduces the use of two-photon excitation to the S1 state, combined with one-photon excitation to the S2 state of the carotenoid beta-apo-8'-carotenal. These 2 investigations show evidence for the formation of solitons, previously unobserved in molecular systems and found only in conducting polymers Chapter 5 presents an investigation of the excited state dynamics of peridinin, the carotenoid responsible for the light harvesting of dinoflagellates. This investigation allows for a more detailed understanding of the importance of structural dynamics of carotenoids in light harvesting

Transitional nuclei near shell closures

Energy Technology Data Exchange (ETDEWEB)

Mukherjee, G. [Variable Energy Cyclotron Centre, 1/AF Bidhan Nagar, Kolkata 700064 (India); Pai, H. [Variable Energy Cyclotron Centre, 1/AF Bidhan Nagar, Kolkata 700064, India and Present Address: Institut für Kernphysik, Technische Universität Darmstadt, Schlossgartenstrasse 9, 64289 Darmstadt (Germany)

2014-08-14

High spin states in Bismuth and Thallium nuclei near the Z = 82 shell closure and Cesium nuclei near the N = 82 shell closure in A = 190 and A = 130 regions, respectively, have been experimentally investigated using heavy-ion fusion evaporation reaction and by detecting the gamma rays using the Indian National Gamma Array (INGA). Interesting shape properties in these transitional nuclei have been observed. The results were compared with the neighboring nuclei in these two regions. The total Routhian surface (TRS) calculations have been performed for a better understanding of the observed properties. In mass region A = 190, a change in shape from spherical to deformed has been observd around neutron number N = 112 for the Bi (Z = 83) isotopes with proton number above the magic gap Z = 82, whereas, the shape of Tl (Z = 81) isotopes with proton number below the magic gap Z = 82 remains stable as a function of neutron number. An important transition from aplanar to planar configuration of angular momentum vectors leading to the occurance of nuclar chirality and magnetic rotation, respectively, has been proposed for the unique parity πh{sub 11/2}⊗νh{sub 11/2} configuration in Cs isotopes in the mass region A ∼ 130 around neutron number N = 79. These results are in commensurate with the TRS calculations.

The determination of the conduction mechanism and optical band gap of fluorescein sodium salt

International Nuclear Information System (INIS)

Yakuphanoglu, Fahrettin; Sekerci, Memet; Evin, Ertan

2006-01-01

The electrical conductivity and optical properties of fluorescein sodium salt in the temperature range of 295-370 K have been investigated. Various conduction models described in the literature were used to elucidate the charge transport mechanism of the compound. It is found that the charge transfer mechanism of the compound is understood in terms of grain boundary scattering. It can be evaluated that the obtained electronic parameters such as mobility, conductivity at room temperature, activation energy and optical band gap suggest that the compound is an organic semiconductor

D- production by multiple charge-transfer collisions in metal-vapor targets. [1 to 50 keV D/sup +/

Energy Technology Data Exchange (ETDEWEB)

Schlachter, A.S.

1977-09-01

A beam of D/sup -/ions can be produced by multiple charge-transfer collisions of a D/sup +/ beam in a thick metal-vapor target. Cross sections and equilibrium charge-state fractions are presented and discussed.

Charge transfer and bond lengths in YBa2Cu3-xMxO6+y

International Nuclear Information System (INIS)

Jorgensen, J.D.; Rhyne, J.J.; Neumann, D.A.; Miceli, P.F.; Tarascon, J.M.; Greene, L.H.; Barboux, P.

1989-01-01

We discuss the effects of doping on the Cu chain sites in YBa 2 Cu 3-x M x O 6+y . The relationship between bond lengths obtained from neutron scattering and charge transfer is evaluated in terms of bond valence. In particular, it is concluded that removing an oxygen from the chains transfers one electron to the planes. 24 refs., 3 figs

Field-induced Gap and Quantized Charge Pumping in Nano-helix

Energy Technology Data Exchange (ETDEWEB)

Qi, Xiao-Liang; /Stanford U., Phys. Dept. /Tsinghua U., Beijing; Zhang, Shou-Cheng; /Stanford U., Phys. Dept.

2010-02-15

We propose several novel physical phenomena based on nano-scale helical wires. Applying a static electric field transverse to the helical wire induces a metal to insulator transition, with the band gap determined by the applied voltage. Similar idea can be applied to 'geometrically' constructing one-dimensional systems with arbitrary external potential. With a quadrupolar electrode configuration, the electric field could rotate in the transverse plane, leading to a quantized dc charge current proportional to the frequency of the rotation. Such a device could be used as a new standard for the high precession measurement of the electric current. The inverse effect implies that passing an electric current through a helical wire in the presence of a transverse static electric field can lead to a mechanical rotation of the helix. This effect can be used to construct nano-scale electro-mechanical motors. Finally, our methodology also enables new ways of controlling and measuring the electronic properties of helical biological molecules such as the DNA.

Quantum computing based on space states without charge transfer

International Nuclear Information System (INIS)

Vyurkov, V.; Filippov, S.; Gorelik, L.

2010-01-01

An implementation of a quantum computer based on space states in double quantum dots is discussed. There is no charge transfer in qubits during a calculation, therefore, uncontrolled entanglement between qubits due to long-range Coulomb interaction is suppressed. Encoding and processing of quantum information is merely performed on symmetric and antisymmetric states of the electron in double quantum dots. Other plausible sources of decoherence caused by interaction with phonons and gates could be substantially suppressed in the structure as well. We also demonstrate how all necessary quantum logic operations, initialization, writing, and read-out could be carried out in the computer.

State-selective charge transfer and excitation in ion-ion interactions at intermediate and high energies

International Nuclear Information System (INIS)

Samanta, R; Purkait, M

2012-01-01

Boundary Corrected Continuum Intermediate State (BCCIS) approximation and Classical Trajectory Monte Carlo (CTMC) methods are applied to calculate the charge transfer and excitation cross sections for ion-ion collisions.

Energy and charge transfer dynamics between Alq3 and CdSeS nanocrystals.

Science.gov (United States)

Zhang, Shuping; Liu, Yuqiang; Yang, Yanqiang

2010-03-01

The photoluminescence properties of the blend films consisting of organic small molecules and nanocrystals (NCs)--Alq3 and CdSeS NCs--were studied by steady-state and time-resolved photoluminescence (PL) spectroscopy with different excited wavelengths. Both the fluorescence intensity and lifetime are intensively dependent on the NC concentration. The detailed analysis of experiment data proves that Forster energy transfer from the Alq3 to the NCs exists simultaneously with the charge transfer and both compete with each other in the blend films.

Simple heuristic derivation of some charge-transfer probabilities at asymptotically high incident velocities

International Nuclear Information System (INIS)

Spruch, L.; Shakeshaft, R.

1984-01-01

For asymptotically high incident velocities we provide simple, heuristic, almost classical, derivations of the cross section for forward charge transfer, and of the ratio of the cross section for capture to the elastic-scattering cross section for the projectile scattered through an angle close to π/3

Single Molecule Spectroelectrochemistry of Interfacial Charge Transfer Dynamics In Hybrid Organic Solar Cell

Energy Technology Data Exchange (ETDEWEB)

Pan, Shanlin [Univ. of Alabama, Tuscaloosa, AL (United States)

2014-11-16

Our research under support of this DOE grant is focused on applied and fundamental aspects of model organic solar cell systems. Major accomplishments are: 1) we developed a spectroelectorchemistry technique of single molecule single nanoparticle method to study charge transfer between conjugated polymers and semiconductor at the single molecule level. The fluorescence of individual fluorescent polymers at semiconductor surfaces was shown to exhibit blinking behavior compared to molecules on glass substrates. Single molecule fluorescence excitation anisotropy measurements showed the conformation of the polymer molecules did not differ appreciably between glass and semiconductor substrates. The similarities in molecular conformation suggest that the observed differences in blinking activity are due to charge transfer between fluorescent polymer and semiconductor, which provides additional pathways between states of high and low fluorescence quantum efficiency. Similar spectroelectrochemistry work has been done for small organic dyes for understand their charge transfer dynamics on various substrates and electrochemical environments; 2) We developed a method of transferring semiconductor nanoparticles (NPs) and graphene oxide (GO) nanosheets into organic solvent for a potential electron acceptor in bulk heterojunction organic solar cells which employed polymer semiconductor as the electron donor. Electron transfer from the polymer semiconductor to semiconductor and GO in solutions and thin films was established through fluorescence spectroscopy and electroluminescence measurements. Solar cells containing these materials were constructed and evaluated using transient absorption spectroscopy and dynamic fluorescence techniques to understand the charge carrier generation and recombination events; 3) We invented a spectroelectorchemistry technique using light scattering and electroluminescence for rapid size determination and studying electrochemistry of single NPs in an

Dependence of charge transfer phenomena during solid-air two-phase flow on particle disperser

Science.gov (United States)

Tanoue, Ken-ichiro; Suedomi, Yuuki; Honda, Hirotaka; Furutani, Satoshi; Nishimura, Tatsuo; Masuda, Hiroaki

2012-12-01

An experimental investigation of the tribo-electrification of particles has been conducted during solid-air two-phase turbulent flow. The current induced in a metal plate by the impact of polymethylmethacrylate (PMMA) particles in a high-speed air flow was measured for two different plate materials. The results indicated that the contact potential difference between the particles and a stainless steel plate was positive, while for a nickel plate it was negative. These results agreed with theoretical contact charge transfer even if not only the particle size but also the kind of metal plate was changed. The specific charge of the PMMA particles during solid-air two-phase flow using an ejector, a stainless steel branch pipe, and a stainless steel straight pipe was measured using a Faraday cage. Although the charge was negative in the ejector, the particles had a positive specific charge at the outlet of the branch pipe, and this positive charge increased in the straight pipe. The charge decay along the flow direction could be reproduced by the charging and relaxation theory. However, the proportional coefficients in the theory changed with the particle size and air velocity. Therefore, an unexpected charge transfer occurred between the ejector and the branch pipe, which could not be explained solely by the contact potential difference. In the ejector, an electrical current in air might have been produced by self-discharge of particles with excess charge between the nickel diffuser in the ejector and the stainless steel nozzle or the stainless steel pipe due to a reversal in the contact potential difference between the PMMA and the stainless steel. The sign of the current depended on the particle size, possibly because the position where the particles impacted depended on their size. When dual coaxial glass pipes were used as a particle disperser, the specific charge of the PMMA particles became more positive along the particle flow direction due to the contact

Impact of speciation on the electron charge transfer properties of nanodiamond drug carriers.

Science.gov (United States)

Sun, Baichuan; Barnard, Amanda S

2016-08-07

Unpassivated diamond nanoparticles (bucky-diamonds) exhibit a unique surface reconstruction involving graphitization of certain crystal facets, giving rise to hybrid core-shell particles containing both aromatic and aliphatic carbon. Considerable effort is directed toward eliminating the aromatic shell, but persistent graphitization of subsequent subsurface-layers makes perdurable purification a challenge. In this study we use some simple statistical methods, in combination with electronic structure simulations, to predict the impact of different fractions of aromatic and aliphatic carbon on the charge transfer properties of the ensembles of bucky-diamonds. By predicting quality factors for a variety of cases, we find that perfect purification is not necessary to preserve selectivity, and there is a clear motivation for purifying samples to improve the sensitivity of charge transfer reactions. This may prove useful in designing drug delivery systems where the release of (selected) drugs needs to be sensitive to specific conditions at the point of delivery.

Size-Induced Segregation in the Stepwise Microhydration of Hydantoin and Its Role in Proton-Induced Charge Transfer

Science.gov (United States)

Calvo, Florent; Bacchus-Montabonel, Marie-Christine

2018-01-01

Recent photochemistry experiments provided evidence for the formation of hydantoin by irradiation of interstellar ice analogues. The significance of these results and the importance of hydantoin in prebiotic chemistry and polypeptide synthesis motivate the present theoretical investigation, in which we analyzed the effects of stepwise hydration on the electronic and thermodynamical properties of the structure of microhydrated hydantoin using a variety of computational approaches. We generally find microhydration to proceed around the hydantoin heterocycle until 5 water molecules are reached, at which stage hydration becomes segregated with a water cluster forming aside the heterocycle. The reactivity of microhydrated hydantoin caused by an impinging proton was evaluated through charge transfer collision cross sections for microhydrated compounds but also for hydantoin on icy grains modeled using a cluster approach mimicking the true hexagonal ice surface. The effects of hydration on charge transfer efficiency are mostly significant when few water molecules are present, and they progressively weaken and stabilize in larger clusters. On the ice substrate, charge transfer essentially contributes to a global increase in the cross sections.

Electronic and vibronic properties of a discotic liquid-crystal and its charge transfer complex

Energy Technology Data Exchange (ETDEWEB)

Haverkate, Lucas A.; Mulder, Fokko M. [Reactor Institute Delft, Faculty of Applied Sciences, Delft University of Technology, Mekelweg 15, 2629JB Delft (Netherlands); Zbiri, Mohamed, E-mail: zbiri@ill.fr; Johnson, Mark R. [Institut Laue Langevin, 38042 Grenoble Cedex 9 (France); Carter, Elizabeth [Vibrational Spectroscopy Facility, School of Chemistry, The University of Sydney, NSW 2008 (Australia); Kotlewski, Arek; Picken, S. [ChemE-NSM, Faculty of Chemistry, Delft University of Technology, 2628BL/136 Delft (Netherlands); Kearley, Gordon J. [Bragg Institute, Australian Nuclear Science and Technology Organisation, Menai, NSW 2234 (Australia)

2014-01-07

Discotic liquid crystalline (DLC) charge transfer (CT) complexes combine visible light absorption and rapid charge transfer characteristics, being favorable properties for photovoltaic (PV) applications. We present a detailed study of the electronic and vibrational properties of the prototypic 1:1 mixture of discotic 2,3,6,7,10,11-hexakishexyloxytriphenylene (HAT6) and 2,4,7-trinitro-9-fluorenone (TNF). It is shown that intermolecular charge transfer occurs in the ground state of the complex: a charge delocalization of about 10{sup −2} electron from the HAT6 core to TNF is deduced from both Raman and our previous NMR measurements [L. A. Haverkate, M. Zbiri, M. R. Johnson, B. Deme, H. J. M. de Groot, F. Lefeber, A. Kotlewski, S. J. Picken, F. M. Mulder, and G. J. Kearley, J. Phys. Chem. B 116, 13098 (2012)], implying the presence of permanent dipoles at the donor-acceptor interface. A combined analysis of density functional theory calculations, resonant Raman and UV-VIS absorption measurements indicate that fast relaxation occurs in the UV region due to intramolecular vibronic coupling of HAT6 quinoidal modes with lower lying electronic states. Relatively slower relaxation in the visible region the excited CT-band of the complex is also indicated, which likely involves motions of the TNF nitro groups. The fast quinoidal relaxation process in the hot UV band of HAT6 relates to pseudo-Jahn-Teller interactions in a single benzene unit, suggesting that the underlying vibronic coupling mechanism can be generic for polyaromatic hydrocarbons. Both the presence of ground state CT dipoles and relatively slow relaxation processes in the excited CT band can be relevant concerning the design of DLC based organic PV systems.

Study of subshell gap around N = 70 for neutron-rich nuclei

International Nuclear Information System (INIS)

Hemalatha, M.

2011-01-01

The study and search for new regions of shell closure for nuclei away from stability is a topic of current interest both experimentally and theoretically. There have been few studies predicting a weak spherical subshell gap of 110 Zr (N = 70), for example. This is supported by a recent study indicating that the spherical N = 70 shell gap may not have a large effect at N = 68 for Zr isotopes. It would be, therefore, interesting to know whether there is a subshell closure at N = 70 in the neutron rich region and also for the very neutron-rich nuclei, 110 Zr

Atomic and electronic structure of trilayer graphene/SiC(0001): Evidence of Strong Dependence on Stacking Sequence and charge transfer.

Science.gov (United States)

Pierucci, Debora; Brumme, Thomas; Girard, Jean-Christophe; Calandra, Matteo; Silly, Mathieu G; Sirotti, Fausto; Barbier, Antoine; Mauri, Francesco; Ouerghi, Abdelkarim

2016-09-15

The transport properties of few-layer graphene are the directly result of a peculiar band structure near the Dirac point. Here, for epitaxial graphene grown on SiC, we determine the effect of charge transfer from the SiC substrate on the local density of states (LDOS) of trilayer graphene using scaning tunneling microscopy/spectroscopy and angle resolved photoemission spectroscopy (ARPES). Different spectra are observed and are attributed to the existence of two stable polytypes of trilayer: Bernal (ABA) and rhomboedreal (ABC) staking. Their electronic properties strongly depend on the charge transfer from the substrate. We show that the LDOS of ABC stacking shows an additional peak located above the Dirac point in comparison with the LDOS of ABA stacking. The observed LDOS features, reflecting the underlying symmetry of the two polytypes, were reproduced by explicit calculations within density functional theory (DFT) including the charge transfer from the substrate. These findings demonstrate the pronounced effect of stacking order and charge transfer on the electronic structure of trilayer or few layer graphene. Our approach represents a significant step toward understand the electronic properties of graphene layer under electrical field.

Geometry and quadratic nonlinearity of charge transfer complexes in solution: A theoretical study

International Nuclear Information System (INIS)

Mukhopadhyay, S.; Ramasesha, S.; Pandey, Ravindra; Das, Puspendu K.

2011-01-01

In this paper, we have computed the quadratic nonlinear optical (NLO) properties of a class of weak charge transfer (CT) complexes. These weak complexes are formed when the methyl substituted benzenes (donors) are added to strong acceptors like chloranil (CHL) or di-chloro-di-cyano benzoquinone (DDQ) in chloroform or in dichloromethane. The formation of such complexes is manifested by the presence of a broad absorption maximum in the visible range of the spectrum where neither the donor nor the acceptor absorbs. The appearance of this visible band is due to CT interactions, which result in strong NLO responses. We have employed the semiempirical intermediate neglect of differential overlap (INDO/S) Hamiltonian to calculate the energy levels of these CT complexes using single and double configuration interaction (SDCI). The solvent effects are taken into account by using the self-consistent reaction field (SCRF) scheme. The geometry of the complex is obtained by exploring different relative molecular geometries by rotating the acceptor with respect to the fixed donor about three different axes. The theoretical geometry that best fits the experimental energy gaps, β HRS and macroscopic depolarization ratios is taken to be the most probable geometry of the complex. Our studies show that the most probable geometry of these complexes in solution is the parallel displaced structure with a significant twist in some cases.

Imidazole as a parent π-conjugated backbone in charge-transfer chromophores

Directory of Open Access Journals (Sweden)

Jiří Kulhánek

2012-01-01

Full Text Available Research activities in the field of imidazole-derived push–pull systems featuring intramolecular charge transfer (ICT are reviewed. Design, synthetic pathways, linear and nonlinear optical properties, electrochemistry, structure–property relationships, and the prospective application of such D-π-A organic materials are described. This review focuses on Y-shaped imidazoles, bi- and diimidazoles, benzimidazoles, bis(benzimidazoles, imidazole-4,5-dicarbonitriles, and imidazole-derived chromophores chemically bound to a polymer chain.

Chemical and physical investigations on the charge transfer interaction of organic donors with iodine and its application as non-traditional organic conductors

Science.gov (United States)

Refat, Moamen S.; Sharshar, T.; Adam, Abdel Majid A.; Elsabawy, Khaled M.; Hemeda, O. M.

2014-09-01

The iso-leucine-iodide and methionine-iodide charge-transfer complexes were prepared and characterized using different spectroscopic techniques. The iodide charge-transfer complexes were synthesized by grinding KI-I2-amino acid with 1:1:1 M ratio in presence of few drops of methanol solvent. The structures of both solid amino acid iodide charge-transfer complexes are discussed with the help of the obtained results of the infrared and Raman laser spectra, Uv-vis. electronic spectra and thermal analyses. The electrical properties (AC resistivity and dielectric constant) of both complexes were investigated. The positron annihilation Doppler broadening (PADB) spectroscopies were also used to probe the structural changes of both complexes. The PADB line-shape parameters (S and W) were found to be dependent on the structure, electronic configuration of the charge transfer complex. The PADB technique is a powerful tool to probe the structural features of the KI-I2-amino acid complexes.

Charge-Transfer States in Organic Solar Cells: Understanding the Impact of Polarization, Delocalization, and Disorder

KAUST Repository

Zheng, Zilong

2017-05-08

We investigate the impact of electronic polarization, charge delocalization, and energetic disorder on the charge-transfer (CT) states formed at a planar C60/pentacene interface. The ability to examine large complexes containing up to seven pentacene molecules and three C60 molecules allows us to take explicitly into account the electronic polarization effects. These complexes are extracted from a bilayer architecture modeled by molecular dynamics simulations and evaluated by means of electronic-structure calculations based on long-range-separated functionals (ωB97XD and BNL) with optimized range-separation parameters. The energies of the lowest charge-transfer states derived for the large complexes are in very good agreement with the experimentally reported values. The average singlet-triplet energy splittings of the lowest CT states are calculated not to exceed 10 meV. The rates of geminate recombination as well as of dissociation of the triplet excitons are also evaluated. In line with experiment, our results indicate that the pentacene triplet excitons generated through singlet fission can dissociate into separated charges on a picosecond time scale, despite the fact that their energy in C60/pentacene heterojunctions is slightly lower than the energies of the lowest CT triplet states.

Charge-transfer collisions involving few-electron systems

International Nuclear Information System (INIS)

Kirchner, T.

2016-01-01

Ion-atom collision systems that involve more than one electron constitute nonseparable few-body problems, whose full solution is difficult to say the least. At impact energies well below 1 keV/amu an expansion of the stationary scattering wave function in terms of a limited number of products of nuclear and molecular state wave functions (amended to satisfy scattering boundary conditions) is feasible and usually sufficient to obtain accurate charge-transfer cross sections provided the electronic wave functions include configuration interaction. At energies above 1 keV/amu this approach becomes inefficient and close-coupling methods within the semi classical approximation are better suited to treat the problem. For bare-ion collisions from helium target atoms explicit solutions of the two-electron time-dependent Schrödinger equation can be achieved, but are computationally costly and cannot be extended to problems which involve more than two electrons.

Direct evidence of charge separation in a metal-organic framework: efficient and selective photocatalytic oxidative coupling of amines via charge and energy transfer.

Science.gov (United States)

Xu, Caiyun; Liu, Hang; Li, Dandan; Su, Ji-Hu; Jiang, Hai-Long

2018-03-28

The selective aerobic oxidative coupling of amines under mild conditions is an important laboratory and commercial procedure yet a great challenge. In this work, a porphyrinic metal-organic framework, PCN-222, was employed to catalyze the reaction. Upon visible light irradiation, the semiconductor-like behavior of PCN-222 initiates charge separation, evidently generating oxygen-centered active sites in Zr-oxo clusters indicated by enhanced porphyrin π-cation radical signals. The photogenerated electrons and holes further activate oxygen and amines, respectively, to give the corresponding redox products, both of which have been detected for the first time. The porphyrin motifs generate singlet oxygen based on energy transfer to further promote the reaction. As a result, PCN-222 exhibits excellent photocatalytic activity, selectivity and recyclability, far superior to its organic counterpart, for the reaction under ambient conditions via combined energy and charge transfer.

Bane of Hydrogen-Bond Formation on the Photoinduced Charge-Transfer Process in Donor–Acceptor Systems

KAUST Repository

Alsam, Amani Abdu; Adhikari, Aniruddha; Parida, Manas R.; Aly, Shawkat Mohammede; Bakr, Osman; Mohammed, Omar F.

2017-01-01

Controlling the ultrafast dynamical process of photoinduced charge transfer at donor acceptor interfaces remains a major challenge for physical chemistry and solar cell communities. The process is complicated by the involvement of other complex

Influence of Coherent Tunneling and Incoherent Hopping on the Charge Transfer Mechanism in Linear Donor-Bridge-Acceptor Systems.

Science.gov (United States)

Li, Guangqi; Govind, Niranjan; Ratner, Mark A; Cramer, Christopher J; Gagliardi, Laura

2015-12-17

The mechanism of charge transfer has been observed to change from tunneling to hopping with increasing numbers of DNA base pairs in polynucleotides and with the length of molecular wires. The aim of this paper is to investigate this transition by examining the population dynamics using a tight-binding Hamiltonian with model parameters to describe a linear donor-bridge-acceptor (D-B-A) system. The model includes a primary vibration and an electron-vibration coupling at each site. A further coupling of the primary vibration with a secondary phonon bath allows the system to dissipate energy to the environment and reach a steady state. We apply the quantum master equation (QME) approach, based on second-order perturbation theory in a quantum dissipative system, to examine the dynamical processes involved in charge-transfer and follow the population transfer rate at the acceptor, ka, to shed light on the transition from tunneling to hopping. With a small tunneling parameter, V, the on-site population tends to localize and form polarons, and the hopping mechanism dominates the transfer process. With increasing V, the population tends to be delocalized and the tunneling mechanism dominates. The competition between incoherent hopping and coherent tunneling governs the mechanism of charge transfer. By varying V and the total number of sites, we also examine the onset of the transition from tunneling to hopping with increasing length.

Columbia River Component Data Gap Analysis

Energy Technology Data Exchange (ETDEWEB)

L. C. Hulstrom

2007-10-23

This Data Gap Analysis report documents the results of a study conducted by Washington Closure Hanford (WCH) to compile and reivew the currently available surface water and sediment data for the Columbia River near and downstream of the Hanford Site. This Data Gap Analysis study was conducted to review the adequacy of the existing surface water and sediment data set from the Columbia River, with specific reference to the use of the data in future site characterization and screening level risk assessments.

Charge imbalance

International Nuclear Information System (INIS)

Clarke, J.

1981-01-01

This article provides a long theoretical development of the main ideas of charge imbalance in superconductors. Concepts of charge imbalance and quasiparticle charge are introduced, especially in regards to the use of tunnel injection in producing and detecting charge imbalance. Various mechanisms of charge relaxation are discussed, including inelastic scattering processes, elastic scattering in the presence of energy-gap anisotropy, and various pair-breaking mechanisms. In each case, present theories are reviewed in comparison with experimental data

Models of charge transport and transfer in molecular switch tunnel junctions of bistable catenanes and rotaxanes

International Nuclear Information System (INIS)

Flood, Amar H.; Wong, Eric W.; Stoddart, J. Fraser

2006-01-01

The processes by which charge transfer can occur play a foundational role in molecular electronics. Here we consider simplified models of the transfer processes that could be present in bistable molecular switch tunnel junction (MSTJ) devices during one complete cycle of the device from its low- to high- and back to low-conductance state. The bistable molecular switches, which are composed of a monolayer of either switchable catenanes or rotaxanes, exist in either a ground-state co-conformation or a metastable one in which the conduction properties of the two co-conformations, when measured at small biases (+0.1 V), are significantly different irrespective of whether transport is dominated by tunneling or hopping. The voltage-driven generation (±2 V) of molecule-based redox states, which are sufficiently long-lived to allow the relative mechanical movements necessary to switch between the two co-conformations, rely upon unequal charge transfer rates on to and/or off of the molecules. Surface-enhanced Raman spectroscopy has been used to image the ground state of the bistable rotaxane in MSTJ-like devices. Consideration of these models provide new ways of looking at molecular electronic devices that rely, not only on nanoscale charge-transport, but also upon the bustling world of molecular motion in mechanically interlocked bistable molecules

Quantitative analysis of charge trapping and classification of sub-gap states in MoS2 TFT by pulse I-V method

Science.gov (United States)

Park, Junghak; Hur, Ji-Hyun; Jeon, Sanghun

2018-04-01

The threshold voltage instabilities and huge hysteresis of MoS2 thin film transistors (TFTs) have raised concerns about their practical applicability in next-generation switching devices. These behaviors are associated with charge trapping, which stems from tunneling to the adjacent trap site, interfacial redox reaction and interface and/or bulk trap states. In this report, we present quantitative analysis on the electron charge trapping mechanism of MoS2 TFT by fast pulse I-V method and the space charge limited current (SCLC) measurement. By adopting the fast pulse I-V method, we were able to obtain effective mobility. In addition, the origin of the trap states was identified by disassembling the sub-gap states into interface trap and bulk trap states by simple extraction analysis. These measurement methods and analyses enable not only quantitative extraction of various traps but also an understanding of the charge transport mechanism in MoS2 TFTs. The fast I-V data and SCLC data obtained under various measurement temperatures and ambient show that electron transport to neighboring trap sites by tunneling is the main charge trapping mechanism in thin-MoS2 TFTs. This implies that interfacial traps account for most of the total sub-gap states while the bulk trap contribution is negligible, at approximately 0.40% and 0.26% in air and vacuum ambient, respectively. Thus, control of the interface trap states is crucial to further improve the performance of devices with thin channels.

Fragment-orbital tunneling currents and electronic couplings for analysis of molecular charge-transfer systems.

Science.gov (United States)

Hwang, Sang-Yeon; Kim, Jaewook; Kim, Woo Youn

2018-04-04

In theoretical charge-transfer research, calculation of the electronic coupling element is crucial for examining the degree of the electronic donor-acceptor interaction. The tunneling current (TC), representing the magnitudes and directions of electron flow, provides a way of evaluating electronic couplings, along with the ability of visualizing how electrons flow in systems. Here, we applied the TC theory to π-conjugated organic dimer systems, in the form of our fragment-orbital tunneling current (FOTC) method, which uses the frontier molecular-orbitals of system fragments as diabatic states. For a comprehensive test of FOTC, we assessed how reasonable the computed electronic couplings and the corresponding TC densities are for the hole- and electron-transfer databases HAB11 and HAB7. FOTC gave 12.5% mean relative unsigned error with regard to the high-level ab initio reference. The shown performance is comparable with that of fragment-orbital density functional theory, which gave the same error by 20.6% or 13.9% depending on the formulation. In the test of a set of nucleobase π stacks, we showed that the original TC expression is also applicable to nondegenerate cases under the condition that the overlap between the charge distributions of diabatic states is small enough to offset the energy difference. Lastly, we carried out visual analysis on the FOTC densities of thiophene dimers with different intermolecular alignments. The result depicts an intimate topological connection between the system geometry and electron flow. Our work provides quantitative and qualitative grounds for FOTC, showing it to be a versatile tool in characterization of molecular charge-transfer systems.

Synthesis, growth, structural modeling and physio-chemical properties of a charge transfer molecule: Guanidinium tosylate

Science.gov (United States)

Era, Paavai; Jauhar, RO. MU.; Vinitha, G.; Murugakoothan, P.

2018-05-01

An organic nonlinear optical material, guanidinium tosylate was synthesized adopting slow evaporation method and the crystals were harvested from aqueous methanolic medium with dimensions 13 × 9 × 3 mm3. Constitution of crystalline material was confirmed by single crystal X-ray diffraction study. The title compound crystallizes in the monoclinic crystal system with space group P21/c. The UV-vis-NIR spectral study of the grown crystal exhibits high transparency of 80% in the entire visible region with lower cut-off wavelength at 282 nm. Optimized molecular geometry of the grown crystal was obtained using density functional theory (DFT) and the frontier energy gaps calculated from the DFT aids to understand the charge transfer taking place in the molecule. The dielectric properties were studied as a function of temperature and frequency to find the charge distribution within the crystal. The titular compound is thermally stable up to 230 °C assessed by thermogravimetric and differential thermal analysis. Anisotropy in the mechanical behavior was observed while measuring for individual planes. The laser induced surface damage threshold of the grown crystal was measured to be 0.344 GW/cm2 for 1064 nm Nd:YAG laser radiation. Z-scan technique confirms the third-order nonlinear optical property with the ascertained nonlinear refractive index (n2), nonlinear absorption coefficient (β) and third order nonlinear susceptibility (χ(3)). Optical limiting study divulges that the transmitted output power step-up linearly with the increase of the input power at lower power realms and saturates from the threshold 24.95 mW/cm2 and amplitude 0.23 mW/cm2.

Syntheses of planar 1,5,2,4,6,8-dithiotetrazocine derivatives and thermodynamic study on intermolecular charge transfer for developing efficient organic solar cell

Energy Technology Data Exchange (ETDEWEB)

Zhang, Chao-Zhi, E-mail: zhangchaozhi@nuist.edu.cn [Department of Chemistry, Nanjing University of Information Science & Technology, Nanjing 210044 (China); Shen, Dan [Department of Chemistry, Nanjing University of Information Science & Technology, Nanjing 210044 (China); Yuan, Yang [Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Nanjing University of Information Science & Technology, Nanjing 210044 (China); Song, Ming-Xia; Li, Shi-Juan [Department of Chemistry, Nanjing University of Information Science & Technology, Nanjing 210044 (China); Cao, Hui, E-mail: yccaoh@hotmail.com [Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, Nanjing University of Information Science & Technology, Nanjing 210044 (China)

2016-07-01

A series of planar 1,5,2,4,6,8-dithiotetrazocine derivatives were synthesized for study on charge transfer at donor/acceptor interface. The fluorescence quenching spectra, and the highest occupied molecular orbital (−6.10 ∼ −6.25 eV) and the lowest unoccupied molecular orbital (−3.45 ∼ −3.58 eV) energy levels of these 1,5,2,4,6,8-dithiotetrazocine derivatives show that they would be potential acceptor materials. Based on theoretical calculations, thermodynamic study on charge transfer at donor/acceptor interface was carried out. The results of experiments and theoretical calculations show that the electrons could transfer spontaneously from poly(3-hexylthiophene) to these acceptors. The percentages of fluorescence quenching increase with negative Gibbs free energy values increasing in the charge transfer procedures. Therefore, short circuit current values of organic solar cells would increase with the Gibbs free energy values increasing. This paper suggests a useful way for developing efficient organic solar cells. - Highlights: • Syntheses of planar 1,5,2,4,6,8-dithiotetrazocine derivatives for develop effective acceptor. • Electrons at excited state in P3HT could transfer spontaneously to these acceptors. • Thermodynamic study on charge transfer at donor/acceptor interface. • Short circuit currents would be predicted by Gibbs free energy in procedure of charge transfer.

Modeling the effect of shunt current on the charge transfer efficiency of an all-vanadium redox flow battery

Science.gov (United States)

Chen, Yong-Song; Ho, Sze-Yuan; Chou, Han-Wen; Wei, Hwa-Jou

2018-06-01

In an all-vanadium redox flow battery (VRFB), a shunt current is inevitable owing to the electrically conductive electrolyte that fills the flow channels and manifolds connecting cells. The shunt current decreases the performance of a VRFB stack as well as the energy conversion efficiency of a VRFB system. To understand the shunt-current loss in a VRFB stack with various designs and operating conditions, a mathematical model is developed to investigate the effects of the shunt current on battery performance. The model is calibrated with experimental data under the same operating conditions. The effects of the battery design, including the number of cells, state of charge (SOC), operating current, and equivalent resistance of the electrolytes in the flow channels and manifolds, on the shunt current are analyzed and discussed. The charge-transfer efficiency is calculated to investigate the effects of the battery design parameters on the shunt current. When the cell number is increased from 5 to 40, the charge transfer efficiency is decreased from 0.99 to a range between 0.76 and 0.88, depending on operating current density. The charge transfer efficiency can be maintained at higher than 0.9 by limiting the cell number to less than 20.

Charge transfer to a dielectric target by guided ionization waves using electric field measurements

NARCIS (Netherlands)

Slikboer, E.T.; Garcia-Caurel, E.; Guaitella, O.; Sobota, A.

2017-01-01

A kHz-operated atmospheric pressure plasma jet is investigated by measuring charge transferred to a dielectric electro-optic surface (BSO crystal) allowing for the measurement of electric field by exploiting the Pockels effect. The electric field values, distribution of the surface discharge and

Surface characterization and surface electronic structure of organic quasi-one-dimensional charge transfer salts

DEFF Research Database (Denmark)

Sing, M.; Schwingenschlögl, U.; Claessen, R.

2003-01-01

We have thoroughly characterized the surfaces of the organic charge-transfer salts TTF-TCNQ and (TMTSF)(2)PF6 which are generally acknowledged as prototypical examples of one-dimensional conductors. In particular x-ray-induced photoemission spectroscopy turns out to be a valuable nondestructive...

Charge transfer through single molecule contacts: How reliable are rate descriptions?

Directory of Open Access Journals (Sweden)

Denis Kast

2011-08-01

Full Text Available Background: The trend for the fabrication of electrical circuits with nanoscale dimensions has led to impressive progress in the field of molecular electronics in the last decade. However, a theoretical description of molecular contacts as the building blocks of future devices is challenging, as it has to combine the properties of Fermi liquids in the leads with charge and phonon degrees of freedom on the molecule. Outside of ab initio schemes for specific set-ups, generic models reveal the characteristics of transport processes. Particularly appealing are descriptions based on transfer rates successfully used in other contexts such as mesoscopic physics and intramolecular electron transfer. However, a detailed analysis of this scheme in comparison with numerically exact solutions is still elusive.Results: We show that a formulation in terms of transfer rates provides a quantitatively accurate description even in domains of parameter space where strictly it is expected to fail, e.g., at lower temperatures. Typically, intramolecular phonons are distributed according to a voltage driven steady state that can only roughly be captured by a thermal distribution with an effective elevated temperature (heating. An extension of a master equation for the charge–phonon complex, to effectively include the impact of off-diagonal elements of the reduced density matrix, provides very accurate solutions even for stronger electron–phonon coupling.Conclusion: Rate descriptions and master equations offer a versatile model to describe and understand charge transfer processes through molecular junctions. Such methods are computationally orders of magnitude less expensive than elaborate numerical simulations that, however, provide exact solutions as benchmarks. Adjustable parameters obtained, e.g., from ab initio calculations allow for the treatment of various realizations. Even though not as rigorously formulated as, e.g., nonequilibrium Green’s function

Crystalline structure of the marketed form of Rifampicin: a case of conformational and charge transfer polymorphism

Science.gov (United States)

de Pinho Pessoa Nogueira, Luciana; de Oliveira, Yara S.; de C. Fonseca, Jéssica; Costa, Wendell S.; Raffin, Fernanda N.; Ellena, Javier; Ayala, Alejandro Pedro

2018-03-01

Rifampicin is a semi-synthetic drug derived from rifamycin B, and currently integrates the fixed dose combination tablet formulations used in the treatment of tuberculosis. It is also used in the leprosy polychemotherapy and prophylaxis, which are diseases classified as neglected according to the World Health Organization. Rifampicin is a polymorphic drug and its desirable polymorphic form is labeled as II, being the main goal of this study the elucidation of its crystalline structure. Polymorph II is characterized by two molecules with different conformations in the asymmetric unit and the following lattice parameters: a = 14.0760 (10) Å, b = 17.5450 (10) Å, c = 17.5270 (10) Å, β = 92.15°. Differently to the previously reported structures, a charge transference from the hydroxyl group of the naphthoquinone of one conformer to the nitrogen of the piperazine group of the second conformer was observed. The relevance of the knowledge of this crystalline structure, which is the preferred polymorph for pharmaceutical formulations, was evidenced by analyzing raw materials with polymorphic mixtures. Thus, the results presented in this contribution close an old information gap allowing the complete solid-state characterization of rifampicin.

A Comparative Study of Power Supply Architectures In Wireless Electric Vehicle Charging Systems

Science.gov (United States)

Esteban, Bryan

Wireless inductive power transfer is a transformational and disruptive technology that enables the reliable and efficient transfer of electrical power over large air gaps for a host of unique applications. One such application that is now gaining much momentum worldwide is the wireless charging of electric vehicles (EVs). This thesis examines two of the primary power supply topologies being predominantly used for EV charging, namely the SLC and the LCL resonant full bridge inverter topologies. The study of both of these topologies is presented in the context of designing a 3 kW, primary side controlled, wireless EV charger with nominal operating parameters of 30 kHz centre frequency and range of coupling in the neighborhood of .18-.26. A comparison of both topologies is made in terms of their complexity, cost, efficiency, and power quality. The aim of the study is to determine which topology is better for wireless EV charging.

Modeling the radiation transfer of discontinuous canopies: results for gap probability and single-scattering contribution

Science.gov (United States)

Zhao, Feng; Zou, Kai; Shang, Hong; Ji, Zheng; Zhao, Huijie; Huang, Wenjiang; Li, Cunjun

2010-10-01

In this paper we present an analytical model for the computation of radiation transfer of discontinuous vegetation canopies. Some initial results of gap probability and bidirectional gap probability of discontinuous vegetation canopies, which are important parameters determining the radiative environment of the canopies, are given and compared with a 3- D computer simulation model. In the model, negative exponential attenuation of light within individual plant canopies is assumed. Then the computation of gap probability is resolved by determining the entry points and exiting points of the ray with the individual plants via their equations in space. For the bidirectional gap probability, which determines the single-scattering contribution of the canopy, a gap statistical analysis based model was adopted to correct the dependence of gap probabilities for both solar and viewing directions. The model incorporates the structural characteristics, such as plant sizes, leaf size, row spacing, foliage density, planting density, leaf inclination distribution. Available experimental data are inadequate for a complete validation of the model. So it was evaluated with a three dimensional computer simulation model for 3D vegetative scenes, which shows good agreement between these two models' results. This model should be useful to the quantification of light interception and the modeling of bidirectional reflectance distributions of discontinuous canopies.

A statewide teleradiology system reduces radiation exposure and charges in transferred trauma patients.

Science.gov (United States)

Watson, Justin J J; Moren, Alexis; Diggs, Brian; Houser, Ben; Eastes, Lynn; Brand, Dawn; Bilyeu, Pamela; Schreiber, Martin; Kiraly, Laszlo

2016-05-01

Trauma transfer patients routinely undergo repeat imaging because of inefficiencies within the radiology system. In 2009, the virtual private network (VPN) telemedicine system was adopted throughout Oregon allowing virtual image transfer between hospitals. The startup cost was a nominal $3,000 per hospital. A retrospective review from 2007 to 2012 included 400 randomly selected adult trauma transfer patients based on a power analysis (200 pre/200 post). The primary outcome evaluated was reduction in repeat computed tomography (CT) scans. Secondary outcomes included cost savings, emergency department (ED) length of stay (LOS), and spared radiation. All data were analyzed using Mann-Whitney U and chi-square tests. P less than .05 indicated significance. Spared radiation was calculated as a weighted average per body region, and savings was calculated using charges obtained from Oregon Health and Science University radiology current procedural terminology codes. Four-hundred patients were included. Injury Severity Score, age, ED and overall LOS, mortality, trauma type, and gender were not statistically different between groups. The percentage of patients with repeat CT scans decreased after VPN implementation: CT abdomen (13.2% vs 2.8%, P < .01) and cervical spine (34.4% vs 18.2%, P < .01). Post-VPN, the total charges saved in 2012 for trauma transfer patients was $333,500, whereas the average radiation dose spared per person was 1.8 mSV. Length of stay in the ED for patients with Injury Severity Score less than 15 transferring to the ICU was decreased (P < .05). Implementation of a statewide teleradiology network resulted in fewer total repeat CT scans, significant savings, decrease in radiation exposure, and decreased LOS in the ED for patients with less complex injuries. The potential for health care savings by widespread adoption of a VPN is significant. Copyright © 2016 Elsevier Inc. All rights reserved.

Heat transfer to surface and gaps of RSI tile arrays in turbulent flow at Mach 10.3

Science.gov (United States)

Throckmorton, D. A.

1974-01-01

Heat transfer to gap walls and surface of a simulated reusable surface insulation (RSI) tile array are presented. The data were obtained in the thick, turbulent tunnel wall boundary layer of the Langley Continuous Flow Hypersonic Tunnel at a freestream Mach number of 10.3 and a freestream unit Reynolds number of one million. Pertinent test variables were: (1) tile array orientation (staggered and in-line), (2) gap width, (3) flow angularity, and (4) tile mismatch.

Solvent control of charge transfer excited state relaxation pathways in [Fe(2,2 '-bipyridine)(CN)4]2-

DEFF Research Database (Denmark)

Kjær, Kasper Skov; Kunnus, Kristjan; Harlang, Tobias C. B.

2018-01-01

The excited state dynamics of solvated [Fe(bpy)(CN)4]2-, where bpy = 2,2'-bipyridine, show significant sensitivity to the solvent Lewis acidity. Using a combination of optical absorption and X-ray emission transient spectroscopies, we have previously shown that the metal to ligand charge transfer...... the MLCT excited state relaxation dynamics of [Fe(bpy)(CN)4]2- in water, a strong Lewis acid solvent. The charge-transfer excited state is now found to decay in less than 100 femtoseconds, forming a quasi-stable metal centered excited state with a 13 picosecond lifetime. We find that this MC excited state...... developed for solar applications....

Ab initio study of charge transfer between lithium and aromatic hydrocarbons. Can the results be directly transferred to the lithium-graphene interaction?

Science.gov (United States)

Sadlej-Sosnowska, N

2014-08-28

We have used electronic density calculations to study neutral complexes of Li with aromatic hydrocarbons. The charge transferred between a Li atom and benzene, coronene, circumcoronene, and circumcircumcoronene has been studied by ab initio methods (at the HF and MP2 level). Toward this aim, the method of integrating electron density in two cuboid fragments of space was applied. One of the fragments was constructed so that it enclosed the bulk of the electron density of lithium; the second, the bulk of the electron density of hydrocarbon. It was found that for each complex two conformations were identified: the most stable with a greater vertical Li-hydrocarbon distance, on the order of 2.5 Å, and another of higher energy with a corresponding distance less than 2 Å. In all cases the transfer of a fractional number, 0.1-0.3 electrons, between Li and hydrocarbon was found; however, the direction of the transfer was not the same in all complexes investigated. The structures of complexes of the first configuration could be represented as Li(σ-)···AH(σ+), whereas the opposite direction of charge transfer was found for complexes of the second configuration, with higher energy. The directions of the dipole moments in the complexes supported these conclusions because they directly measure the redistribution of electron density in a complex with respect to substrates.

Photocatalytic hydrogen generation enhanced by band gap narrowing and improved charge carrier mobility in AgTaO3 by compensated co-doping.

Science.gov (United States)

Li, Min; Zhang, Junying; Dang, Wenqiang; Cushing, Scott K; Guo, Dong; Wu, Nianqiang; Yin, Penggang

2013-10-14

The correlation of the electronic band structure with the photocatalytic activity of AgTaO3 has been studied by simulation and experiments. Doping wide band gap oxide semiconductors usually introduces discrete mid-gap states, which extends the light absorption but has limited benefit for photocatalytic activity. Density functional theory (DFT) calculations show that compensated co-doping in AgTaO3 can overcome this problem by increasing the light absorption and simultaneously improving the charge carrier mobility. N/H and N/F co-doping can delocalize the discrete mid-gap states created by sole N doping in AgTaO3, which increases the band curvature and the electron-to-hole effective mass ratio. In particular, N/F co-doping creates a continuum of states that extend the valence band of AgTaO3. N/F co-doping thus improves the light absorption without creating the mid-gap states, maintaining the necessary redox potentials for water splitting and preventing from charge carrier trapping. The experimental results have confirmed that the N/F-codoped AgTaO3 exhibits a red-shift of the absorption edge in comparison with the undoped AgTaO3, leading to remarkable enhancement of photocatalytic activity toward hydrogen generation from water.

State-selective charge transfer cross sections for light ion impact of atomic hydrogen

Energy Technology Data Exchange (ETDEWEB)

Schultz, D. R. [University of North Texas; Stancil, Phillip C. [University of Georgia, Athens; Havener, C. C. [Oak Ridge National Laboratory (ORNL)

2015-01-01

Owing to the utility of diagnosing plasma properties such as impurity concentration and spatial distribution, and plasma temperature and rotation, by detection of photon emission following capture of electrons from atomic hydrogen to excited states of multiply charged ions, new calculations of state-selective charge transfer involving light ions have been carried out using the atomic orbital close-coupling and the classical trajectory Monte Carlo methods. By comparing these with results of other approaches applicable in a lower impact energy regime, and by benchmarking them using key experimental data, knowledge of the cross sections can be made available across the range parameters needed by fusion plasma diagnostics.

Spectroscopic and theoretical investigations on intramolecular charge transfer phenomenon in 1-3-dioxolane derivative

Science.gov (United States)

Zhang, Zhiyong; Zhang, Zhongzhi; Luo, Yijing; Sun, Shanshan; Zhang, Guangqing

2018-02-01

High fluorescence quantum yield (FQY) and large Stokes shift (SS) cannot be easily achieved simultaneously by traditional PICT or TICT fluorescent probe. However, an 1-3-dioxolane derivative named 5-methyl-8,9-dihydro-5H-[1,3]dioxolo[4,5-b]carbazol-6(7H)-one (MDDCO) features both high FQY and large SS. The purpose of this study is to search the mechanism behind this phenomenon by theoretical method. Simulated structure changes and charge transfer suggest ICT process in MDDCO is similar to PLICT (Planarized Intramolecular Charge Transfer) process. Calculated UV-Vis spectra and fluorescence spectra show that PLICT-like state (S1 state) of MDDCO leads to large SS. Computed transient-absorption spectra and radiative decay rates indicate that PLICT-like state is key factor for high FQY of MDDCO. These findings suggest that PLICT-like state in 1,3-dioxolane derivatives can achieve both large SS and high FQY, which presents a new method for high-performance fluorescent probe design.

Oxidation and Metal-Insertion in Molybdenite Surfaces: Evaluation of Charge-Transfer Mechanisms and Dynamics

Energy Technology Data Exchange (ETDEWEB)

Ramana, Chintalapalle V.; Becker, U.; Shutthanandan, V.; Julien, C. M.

2008-06-05

Molybdenum sulfide (MoS2), an important representative member of the layered transition-metal dichalcogenides, has been of special importance to the research community of geochemistry, materials and environmental chemistry, and industrial science and technology. Understanding the oxidation behavior and charge-transfer mechanisms in MoS2 is important to gain better insight into the degradation of this mineral in the environment. On the other hand understanding the insertion of metals into molybdenite and evaluation of charge-transfer mechanism and dynamics is quite important to utilize these minerals in technological applications. Furthermore, such a detailed investigation of thermal oxidation behavior and intercalation process will provide a basis to further explore and model the mechanism of adsorption of metal ions on to geomedia. Therefore, the present work was performed to understand the oxidation and intercalation processes of molybdenite surfaces. The results obtained, using a wide variety of analytical techniques, are presented and discussed in this paper.

Charge transfer dynamics from adsorbates to surfaces with single active electron and configuration interaction based approaches

Energy Technology Data Exchange (ETDEWEB)

Ramakrishnan, Raghunathan, E-mail: r.ramakrishnan@unibas.ch [Institute of Physical Chemistry, National Center for Computational Design and Discovery of Novel Materials (MARVEL), Department of Chemistry, University of Basel, Klingelbergstrasse 80, CH-4056 Basel (Switzerland); Nest, Mathias [Theoretische Chemie, Technische Universität München, Lichtenbergstr. 4, 85747 Garching (Germany)

2015-01-13

Highlights: • We model electron dynamics across cyano alkanethiolates attached to gold cluster. • We present electron transfer time scales from TD-DFT and TD-CI based simulations. • Both DFT and CI methods qualitatively predict the trend in time scales. • TD-CI predicts the experimental relative time scale very accurately. - Abstract: We employ wavepacket simulations based on many-body time-dependent configuration interaction (TD-CI), and single active electron theories, to predict the ultrafast molecule/metal electron transfer time scales, in cyano alkanethiolates bonded to model gold clusters. The initial states represent two excited states where a valence electron is promoted to one of the two virtual π{sup ∗} molecular orbitals localized on the cyanide fragment. The ratio of the two time scales indicate the efficiency of one charge transfer channel over the other. In both our one-and many-electron simulations, this ratio agree qualitatively with each other as well as with the previously reported experimental time scales (Blobner et al., 2012), measured for a macroscopic metal surface. We study the effect of cluster size and the description of electron correlation on the charge transfer process.

Multiple nucleon transfer in damped nuclear collisions. [Lectures, mass charge, and linear and angular momentum transport

Energy Technology Data Exchange (ETDEWEB)

Randrup, J.

1979-07-01

This lecture discusses a theory for the transport of mass, charge, linear, and angular momentum and energy in damped nuclear collisions, as induced by multiple transfer of individual nucleons. 11 references.

On the charge transfer between single-walled carbon nanotubes and graphene

International Nuclear Information System (INIS)

Rao, Rahul; Pierce, Neal; Dasgupta, Archi

2014-01-01

It is important to understand the electronic interaction between single-walled carbon nanotubes (SWNTs) and graphene in order to use them efficiently in multifunctional hybrid devices. Here, we deposited SWNT bundles on graphene-covered copper and SiO 2 substrates by chemical vapor deposition and investigated the charge transfer between them by Raman spectroscopy. Our results revealed that, on both copper and SiO 2 substrates, graphene donates electrons to the SWNTs, resulting in p-type doped graphene and n-type doped SWNTs.

Lifetimes of partial charge transfer exciplexes of 9-cyanophenanthrene and 9-cyanoanthracene

OpenAIRE

Dolotova, Elena; Dogadkin, Denis; Soboleva, Irina; Kuzmin, Michael; Nicolet, Olivier; Vauthey, Eric

2003-01-01

The fluorescence decays of several exciplexes with partial charge transfer have been investigated in solvents of various polarity. The measured lifetimes are found to be in reasonable agreement with the activation enthalpy and entropy of exciplex decay obtained earlier from the temperature dependence of the exciplex emission quantum yields. For exciplexes with 9-cyanophenanthrene substantial contribution of the higher local excited state into the exciplex electronic structure is found and bor...

The role of remote closure in the perception of occlusion at junctions and illusory contours.

Science.gov (United States)

Gillam, Barbara J; Grove, Philip M; Layden, Jessica

2010-01-01

Abstract. Perceived occlusion at T-junctions or illusory contours at implicit T-junctions are often modelled by using edge information without surface context. We explored the effect of closure on perceived occlusion at T-junctions. Two vertical lines separated by a gap each had six abutting horizontal lines on opposite sides forming T-junctions. These lines were either closed or not closed into pairs at the stem ends of the Ts. In experiment 1, closed T-junction stems gave a much stronger sense of occlusion at the vertical lines than unclosed ones, even though closure information was remote from the putative occlusion and local T-junction information remained constant. When the outer two T-junctions were converted to L-junctions, perceived occlusion considerably diminished. The effect of closure on illusory-contour strength for stimuli like those of experiment 1 but with the vertical lines omitted was explored in experiment 2. The two sets of horizontal lines, separated by a gap, were either closed or not closed into pairs at their outer ends. Illusory-contour strength along the vertical alignments was much greater for closed pairs. Line terminations on both sides of the gap enhanced illusory-contour strength, but whether they were collinear or not had little effect.

Charge separation in branched TiO_2 nanorod array homojunction aroused by quantum effect for enhanced photocatalytic decomposition of gaseous benzene

International Nuclear Information System (INIS)

Wang, Xiaoxia; Ni, Qian; Zeng, Dawen; Liao, Guanglan; Xie, Changsheng

2016-01-01

Highlights: • Charge separation in homojunction based on the broadened band gap by quantum effect. • Absolute charge separation by the passivation effect of TiO_2 nanorod. • Long-distance electron transfer behavior in photocatalysis. • Roughed surface for enhanced light harvesting by light trapping effect. - Abstract: As known, the electron transfer behavior in photocatalysis is short-distance transportation, which leads the photo-induced electrons and holes to be localized. The temporarily separated electrons and holes will recombine with each other in the localized region. In this paper, we successfully achieved electron transfer in a homojunction of branched rutile TiO_2 nanorod @nanoparticle core-shell architecture by quantum confinement effect aroused by the nanoparticle, which is proved by the blue-shifting in UV–vis absorption spectrum of the homojunction. Meanwhile, an absolute charge separation is also achieved by the long-distance electron transfer along the single-crystalline rutile TiO_2 nanorod as uninterrupted high-speed electron transfer channel to FTO substrates. Based on the effective charge separation, the photocatalytic decomposition of gaseous benzene by the homojunction is significantly enhanced, yielding 10 times CO_2 than that of the nanorod array. This homojunction interfacial charge separation, aroused by quantum effect, through long-distance transfer along the single-crystalline nanorod gives us inspiration to achieve efficient charge separation with defect-less interfaces, which might can be utilized for real-time environmental abatement and energy generation simultaneously.

Laser-induced charge transfer in the CH6+ quasimolecule

International Nuclear Information System (INIS)

Errea, L.F.; Mendez, L.; Riera, A.

1985-01-01

The charge transfer cross section is calculated for C 6+ +CH(1s) collisions, through photon assisted 5gsigma--6hsigma, 5gsigma--4fsigma, 5gsigma--4fπ, and 5gsigma--4dsigma transitions. The theory developed by Copeland and Tang, and ourselves, is employed, and the validity of the approximations used is tested. The four processes considered have widely different characteristics with regards to the laser wavelength needed, the collision dynamics and the applicability of back-of-the-envelope estimates based on the Landau--Zener approximation. We point out the relevance of those processes to the impurity diagnostics of magnetically confined fusion plasmas and to the development of short wavelength lasers

Laser-induced charge transfer in the HeH2+ quasimolecule

International Nuclear Information System (INIS)

Errea, L.F.; Mendez, L.; Riera, A.

1983-01-01

In a recent publication, the charge transfer cross section for He 2+ +H(ls) collisions through photon-assisted 2psigma--3dsigma transitions was calculated; this calculation, however, contained several errors whose quantitative--even qualitative effect on the results is not obvious. We present a correct evaluation of this laser-induced cross section, which turns out to be larger, and present a maximum for longer wavelengths, than the values previously reported. In addition, we have checked the applicability of perturbation theory, of the stationary phase, uniform and Landau--Zener approximations, and the importance of potentially competitive photon-assisted reactions

Intra-molecular Charge Transfer and Electron Delocalization in Non-fullerene Organic Solar Cells

Energy Technology Data Exchange (ETDEWEB)

Wu, Qinghe [Department of Chemistry, Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province, Shantou University, Guangdong 515063, P. R. China; Zhao, Donglin [Department of Chemistry, The James Franck Institute, The University of Chicago, 929 E 57th Street, Chicago, Illinois 60637, United States; Goldey, Matthew B. [Institute for Molecular Engineering, The University of Chicago, 5747 South Ellis Avenue, Chicago, Illinois 60637, United States; Filatov, Alexander S. [Department of Chemistry, The James Franck Institute, The University of Chicago, 929 E 57th Street, Chicago, Illinois 60637, United States; Sharapov, Valerii [Department of Chemistry, The James Franck Institute, The University of Chicago, 929 E 57th Street, Chicago, Illinois 60637, United States; Colón, Yamil J. [Institute for Molecular Engineering, Materials Science Division, Argonne National Laboratory, 9700 Cass Avenue, Lemont, Illinois 60439, United States; Institute for Molecular Engineering, The University of Chicago, 5747 South Ellis Avenue, Chicago, Illinois 60637, United States; Cai, Zhengxu [Department of Chemistry, The James Franck Institute, The University of Chicago, 929 E 57th Street, Chicago, Illinois 60637, United States; Chen, Wei [Institute for Molecular Engineering, Materials Science Division, Argonne National Laboratory, 9700 Cass Avenue, Lemont, Illinois 60439, United States; Institute for Molecular Engineering, The University of Chicago, 5747 South Ellis Avenue, Chicago, Illinois 60637, United States; de Pablo, Juan [Institute for Molecular Engineering, Materials Science Division, Argonne National Laboratory, 9700 Cass Avenue, Lemont, Illinois 60439, United States; Institute for Molecular Engineering, The University of Chicago, 5747 South Ellis Avenue, Chicago, Illinois 60637, United States; Galli, Giulia [Institute for Molecular Engineering, Materials Science Division, Argonne National Laboratory, 9700 Cass Avenue, Lemont, Illinois 60439, United States; Institute for Molecular Engineering, The University of Chicago, 5747 South Ellis Avenue, Chicago, Illinois 60637, United States; Yu, Luping [Department of Chemistry, The James Franck Institute, The University of Chicago, 929 E 57th Street, Chicago, Illinois 60637, United States

2018-03-02

Two types of electron acceptors were synthesized by coupling two kinds of electron-rich cores with four equivalent perylene diimides (PDIs) at the a position. With fully aromatic cores, TPB and TPSe have pi-orbitals spread continuously over the whole aromatic conjugated backbone, unlike TPC and TPSi, which contain isolated PDI units due to the use of a tetrahedron carbon or silicon linker. Density functional theory calculations of the projected density of states showed that the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) for TPB are localized in separate regions of space. Further, the LUMO of TPB shows a greater contribution from the orbitals belonging to the connective core of the molecules than that of TPC. Overall, the properties of the HOMO and LUMO point at increased intra-molecular delocalization of negative charge carriers for TPB and TPSe than for TPC and TPSi and hence at a more facile intra-molecular charge transfer for the former. The film absorption and emission spectra showed evidences for the inter -molecular electron delocalization in TPB and TPSe, which is consistent with the network structure revealed by X-ray diffraction studies on single crystals of TPB. These features benefit the formation of charge transfer states and/or facilitate charge transport. Thus, higher electron mobility and higher charge dissociation probabilities under J(sc) condition were observed in blend films of TPB:PTB7-Th and TPSe:PTB7-Th than those in TPC:PTB7Th and TPSi:PTB7-Th blend films. As a result, the J(sc) and fill factor values of 15.02 mA/cm(2), 0.58 and 14.36 mA/cm(2), 0.55 for TPB- and TPSe-based solar cell are observed, whereas those for TPC and TPSi are 11.55 mA/cm2, 0.47 and 10.35 mA/cm(2), 0.42, respectively.

Determination of charge transfer resistance and capacitance of microbial fuel cell through a transient response analysis of cell voltage.

Science.gov (United States)

Ha, Phuc Thi; Moon, Hyunsoo; Kim, Byung Hong; Ng, How Yong; Chang, In Seop

2010-03-15

An alternative method for determining the charge transfer resistance and double-layer capacitance of microbial fuel cells (MFCs), easily implemented without a potentiostat, was developed. A dynamic model with two parameters, the charge transfer resistance and double-layer capacitance of electrodes, was derived from a linear differential equation to depict the current generation with respect to activation overvoltage. This model was then used to fit the transient cell voltage response to the current step change during the continuous operation of a flat-plate type MFC fed with acetate. Variations of the charge transfer resistance and the capacitance value with respect to the MFC design conditions (biocatalyst existence and electrode area) and operating parameters (acetate concentration and buffer strength in the catholyte) were then determined to elucidate the validity of the proposed method. This model was able to describe the dynamic behavior of the MFC during current change in the activation loss region; having an R(2) value of over 0.99 in most tests. Variations of the charge transfer resistance value (thousands of Omega) according to the change of the design factors and operational factors were well-correlated with the corresponding MFC performances. However, though the capacitance values (approximately 0.02 F) reflected the expected trend according to the electrode area change and catalyst property, they did not show significant variation with changes in either the acetate concentration or buffer strength. (c) 2009 Elsevier B.V. All rights reserved.

Modelling of the concentration-time relationship based on global diffusion-charge transfer parameters in a flow-by reactor with a 3D electrode

International Nuclear Information System (INIS)

Nava, J.L.; Sosa, E.; Carreno, G.; Ponce-de-Leon, C.; Oropeza, M.T.

2006-01-01

A concentration versus time relationship model based on the isothermal diffusion-charge transfer mechanism was developed for a flow-by reactor with a three-dimensional (3D) reticulated vitreous carbon (RVC) electrode. The relationship was based on the effectiveness factor (η) which lead to the simulation of the concentration decay at different electrode polarisation conditions, i.e. -0.1, -0.3 and -0.59 V versus SCE; the charge transfer process was used for the former and mix and a mass transport control was used for the latter. Charge transfer and mass transport parameters were estimated from experimental data using Electrochemical Impedance Spectroscopy (EIS) and Linear Voltammetry (LV) techniques, respectively

Modelling of the concentration-time relationship based on global diffusion-charge transfer parameters in a flow-by reactor with a 3D electrode

Energy Technology Data Exchange (ETDEWEB)

Nava, J.L. [Universidad Autonoma Metropolitana-Iztapalapa, Departamento de Quimica, Av. San Rafael Atlixco 186, A.P. 55-534, C.P. 09340, Mexico D.F. (Mexico); Sosa, E. [Instituto Mexicano del Petroleo, Programa de Investigacion en Ingenieria Molecular, Eje Central 152, C.P. 07730, Mexico D.F. (Mexico); Carreno, G. [Universidad de Guanajuato, Facultad de Ingenieria en Geomatica e Hidraulica, Av. Juarez 77, C.P. 36000, Guanajuato, Gto. (Mexico); Ponce-de-Leon, C. [Electrochemical Engineering Group, School of Engineering Sciences, University of Southampton, Highfield, Southampton SO17 1BJ (United Kingdom)]. E-mail: capla@soton.ac.uk; Oropeza, M.T. [Centro de Graduados e Investigacion del Instituto Tecnologico de Tijuana, Blvd. Industrial, s/n, C.P. 22500, Tijuana B.C. (Mexico)

2006-05-25

A concentration versus time relationship model based on the isothermal diffusion-charge transfer mechanism was developed for a flow-by reactor with a three-dimensional (3D) reticulated vitreous carbon (RVC) electrode. The relationship was based on the effectiveness factor ({eta}) which lead to the simulation of the concentration decay at different electrode polarisation conditions, i.e. -0.1, -0.3 and -0.59 V versus SCE; the charge transfer process was used for the former and mix and a mass transport control was used for the latter. Charge transfer and mass transport parameters were estimated from experimental data using Electrochemical Impedance Spectroscopy (EIS) and Linear Voltammetry (LV) techniques, respectively.

Site-dependent charge transfer at the Pt(111)-ZnPc interface and the effect of iodine

International Nuclear Information System (INIS)

Ahmadi, Sareh; Wojek, Bastian M.; Noël, Quentin; Göthelid, Mats; Agnarsson, Björn; Bidermane, Ieva; Sun, Chenghua

2014-01-01

The electronic structure of ZnPc, from sub-monolayers to thick films, on bare and iodated Pt(111) is studied by means of X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, and scanning tunneling microscopy. Our results suggest that at low coverage ZnPc lies almost parallel to the Pt(111) substrate, in a non-planar configuration induced by Zn-Pt attraction, leading to an inhomogeneous charge distribution within the molecule and an inhomogeneous charge transfer to the molecule. ZnPc does not form a complete monolayer on the Pt surface, due to a surface-mediated intermolecular repulsion. At higher coverage ZnPc adopts a tilted geometry, due to a reduced molecule-substrate interaction. Our photoemission results illustrate that ZnPc is practically decoupled from Pt, already from the second layer. Pre-deposition of iodine on Pt hinders the Zn-Pt attraction, leading to a non-distorted first layer ZnPc in contact with Pt(111)-I(√3×√3) or Pt(111)-I(√7×√7), and a more homogeneous charge distribution and charge transfer at the interface. On increased ZnPc thickness iodine is dissolved in the organic film where it acts as an electron acceptor dopant

Computational models of an inductive power transfer system for electric vehicle battery charge

Science.gov (United States)

Anele, A. O.; Hamam, Y.; Chassagne, L.; Linares, J.; Alayli, Y.; Djouani, K.

2015-09-01

One of the issues to be solved for electric vehicles (EVs) to become a success is the technical solution of its charging system. In this paper, computational models of an inductive power transfer (IPT) system for EV battery charge are presented. Based on the fundamental principles behind IPT systems, 3 kW single phase and 22 kW three phase IPT systems for Renault ZOE are designed in MATLAB/Simulink. The results obtained based on the technical specifications of the lithium-ion battery and charger type of Renault ZOE show that the models are able to provide the total voltage required by the battery. Also, considering the charging time for each IPT model, they are capable of delivering the electricity needed to power the ZOE. In conclusion, this study shows that the designed computational IPT models may be employed as a support structure needed to effectively power any viable EV.

Computational models of an inductive power transfer system for electric vehicle battery charge

International Nuclear Information System (INIS)

Anele, A O; Hamam, Y; Djouani, K; Chassagne, L; Alayli, Y; Linares, J

2015-01-01

One of the issues to be solved for electric vehicles (EVs) to become a success is the technical solution of its charging system. In this paper, computational models of an inductive power transfer (IPT) system for EV battery charge are presented. Based on the fundamental principles behind IPT systems, 3 kW single phase and 22 kW three phase IPT systems for Renault ZOE are designed in MATLAB/Simulink. The results obtained based on the technical specifications of the lithium-ion battery and charger type of Renault ZOE show that the models are able to provide the total voltage required by the battery. Also, considering the charging time for each IPT model, they are capable of delivering the electricity needed to power the ZOE. In conclusion, this study shows that the designed computational IPT models may be employed as a support structure needed to effectively power any viable EV. (paper)

Heat exchange between a microparticle and plasma. Contribution of charge transfer processes

International Nuclear Information System (INIS)

Uglov, A.A.; Gnedovets, A.G.

1983-01-01

Heat- and mass-transfer in interaction of a microparticle with a dense plasma have been considered analytically. At that, calculation methods developed as applied to probe diagnostics of slightly ionized plasma are also used in the case of relatively high degrees of ionization, at which heat flows of plasma charged particles Qe and Qi become comparable with molecular ones. High efficiency of energy transfer during electron and ion collisions with a microparticle is due to the following: 1) effective cross section of ion collision with a microparticle, which acquires in a quasineutral plasma the potential phisub(f) < 0, surpasses the geometric one; the maximum contribution of electron and ion constituent is achieved when the cross section ion collisions with a microparticle is linearly connected with its potential, 2) with a charged microparticle electrons from distribution function ''tail'' collide, their energy exceeds potential barrier near the surface and, consequently, the mean heat energy; 3) besides the energy of a microparticle thermal movement during electron recombination and ion neutralization on its surface the heat Qsub(e) and Qsub(i), which considerably exceed the heat of molecular adsorption and mean heat energy of plasma particles at kT approximately 1 eV, are transmitted to the microparticle

Pit closures - effects and alternatives

Energy Technology Data Exchange (ETDEWEB)

Stott, A G

1987-02-01

During the last decade, British Coal has closed around 100 mines. This article illustrates the effect of pit closures on the colliery's workforce, and the local community and its economy. Working conditions at Newmarket Colliery and the Selby coalfield are compared within the context of British Coal's national transfer market. British Coal's transfer benefits include resettlement payments and mortgage subsidies. The job creation venture of British Coal Enterprise Ltd. has helped to create over 3700 new jobs in 264 projects, involving a total investment of 38 M pounds sterling. The article also discusses deputies' qualifications and prospects for recently qualified management staff, and gives a comparison of losses suffered by the different mining unions.

Transverse Schottky spectra and beam transfer functions of coasting ion beams with space charge

International Nuclear Information System (INIS)

Paret, Stefan

2010-01-01

A study of the transverse dynamics of coasting ion beams with moderate space charge is presented in this work. From the dispersion relation with linear space charge, an analytic model describing the impact of space charge on transverse beam transfer functions (BTFs) and the stability limits of a beam is derived. The dielectric function obtained in this way is employed to describe the transverse Schottky spectra with linear space charge as well. The difference between the action of space charge and impedances is highlighted. The setup and the results of an experiment performed in the heavy ion synchrotron SIS-18 at GSI to detect space-charge effects at different beam intensities are explicated. The measured transverse Schottky spectra and BTFs are compared with the linear space-charge model. The stability diagrams constructed from the BTFs are presented. The space-charge parameters evaluated from the Schottky and BTF measurements are compared with estimations based on measured beam parameters. The impact of collective effects on the Schottky and BTF diagnostics is also investigated through numerical simulations. For this purpose the self-field of beams with linear and non-linear transverse density-distributions is computed on a twodimensional grid. The noise of the random particle distribution causes fluctuations of the dipole moment of the beam which produce the Schottky spectrum. BTFs are simulated by exciting the beam with transverse kicks. The simulation results are used to verify the space-charge model. (orig.)

Transverse Schottky spectra and beam transfer functions of coasting ion beams with space charge

Energy Technology Data Exchange (ETDEWEB)

Paret, Stefan

2010-02-22

A study of the transverse dynamics of coasting ion beams with moderate space charge is presented in this work. From the dispersion relation with linear space charge, an analytic model describing the impact of space charge on transverse beam transfer functions (BTFs) and the stability limits of a beam is derived. The dielectric function obtained in this way is employed to describe the transverse Schottky spectra with linear space charge as well. The difference between the action of space charge and impedances is highlighted. The setup and the results of an experiment performed in the heavy ion synchrotron SIS-18 at GSI to detect space-charge effects at different beam intensities are explicated. The measured transverse Schottky spectra and BTFs are compared with the linear space-charge model. The stability diagrams constructed from the BTFs are presented. The space-charge parameters evaluated from the Schottky and BTF measurements are compared with estimations based on measured beam parameters. The impact of collective effects on the Schottky and BTF diagnostics is also investigated through numerical simulations. For this purpose the self-field of beams with linear and non-linear transverse density-distributions is computed on a twodimensional grid. The noise of the random particle distribution causes fluctuations of the dipole moment of the beam which produce the Schottky spectrum. BTFs are simulated by exciting the beam with transverse kicks. The simulation results are used to verify the space-charge model. (orig.)

Muon transfer from muonic hydrogen to heavier atoms; Transfert de charge muonique

Energy Technology Data Exchange (ETDEWEB)

Dupays, A

2004-06-01

This work concerns muon transfer from muonic hydrogen to heavier atoms. Recently, a method of measurement of the hyperfine structure of ground-state muonic hydrogen based on the collision energy dependence of the muon transfer rate to oxygen has been proposed. This proposal is based on measurements which where performed at the Paul Scherrer Institute in the early nineties which indicate that the muon transfer from muonic hydrogen to oxygen increases by a factor of 4 going from thermal to 0.12 eV energies. The motivation of our calculations was to confirm this behaviour. To study the collision energy dependence of the muon transfer rate, we have used a time-independent close-coupling method. We have set up an hyperspherical elliptic formalism valid for nonzero total angular momentum which allows accurate computations of state-to-state reactive and charge exchange processes. We have applied this formalism to muon-transfer process to oxygen and neon. The comparison with experimental results is in both cases excellent. Finally, the neon transfer rate dependence with energy suggests to use neon instead of oxygen to perform a measurement of the hyperfine structure of muonic hydrogen. The results of accurate calculations of the muon transfer rates from muonic protium and deuterium atoms to nitrogen, oxygen and neon are also reported. Very good agreement with measured rates is obtained and for the three systems, the isotopic effect is perfectly reproduced. (author)

Charge transfer in carbon nanotube actuators investigated using in situ Raman spectroscopy

International Nuclear Information System (INIS)

Gupta, S.; Hughes, M.; Windle, A.H.; Robertson, J.

2004-01-01

Charge transfer dynamics on the surface of single-wall carbon nanotube sheets is investigated using in situ Raman spectroscopy in order to understand the actuation mechanism of an electrochemical actuator and to determine associated parameters. We built an actuator from single-wall carbon nanotube mat and studied its actuation in several alkali metal (Li, Na, and K) and alkaline earth (Ca) halide and sulfate solutions in order to clarify the role of counterion as mobile ions in the film. The variation of bonding with applied potential was monitored using in situ Raman spectroscopy. This is because Raman can detect changes in C-C bond length: the radial breathing mode at ∼190 cm-1 varies inversely with the nanotube diameter, and the G band at ∼1590 cm-1 varies with the axial bond length. In addition, the intensities of both the modes vary with the emptying/depleting or filling of the bonding and antibonding states due to electrochemical charge injection. We discussed the variation of peak height and wave numbers of these modes providing valuable information concerning electrochemical charge injection on the carbon nanotube mat surface. We found in-plane microscopic compressive strain (∼-0.25%) and the equivalent charge transfer per carbon atom (f c ∼-0.005) as an upper bound for the actuators studied hereby. It is demonstrated that though the present analysis does comply with the proposition for the actuation principle made earlier, the quantitative estimates are significantly lower if compared with those of reported values. Furthermore, the extent of variation, i.e., coupled electro-chemo-mechanical response of single-wall carbon nanotubes (SWNT) mat depended upon the type of counterion used (Group I versus Group II). The cyclic voltammetry and ac electrochemical impedance spectroscopy results were described briefly, which help to demonstrate well-developed capacitive behavior of SWNT mat and to estimate the specific capacitances as well. Summarizing, the

Absolute Charge Transfer and Fragmentation Cross Sections in He2+-C60 Collisions

International Nuclear Information System (INIS)

Rentenier, A.; Moretto-Capelle, P.; Bordenave-Montesquieu, D.; Bordenave-Montesquieu, A.; Ruiz, L. F.; Diaz-Tendero, S.; Alcami, M.; Martin, F.; Zarour, B.; Hanssen, J.; Hervieux, P.-A.; Politis, M. F.

2008-01-01

We have determined absolute charge transfer and fragmentation cross sections in He 2+ +C 60 collisions in the impact-energy range 0.1-250 keV by using a combined experimental and theoretical approach. We have found that the cross sections for the formation of He + and He 0 are comparable in magnitude, which cannot be explained by the sole contribution of pure single and double electron capture but also by contribution of transfer-ionization processes that are important even at low impact energies. The results show that multifragmentation is important only at impact energies larger than 40 keV; at lower energies, sequential C 2 evaporation is the dominant process

Angular distribution in proton-hydrogen charge-transfer collisions