New Estimates of Inferred Ionic Charge States for Solar Energetic Particle Events with ACE and STEREO

NASA Astrophysics Data System (ADS)

Labrador, A. W.; Sollitt, L. S.; Cohen, C. M.; Cummings, A. C.; Leske, R. A.; Mason, G. M.; Mewaldt, R. A.; Stone, E.; von Rosenvinge, T. T.; Wiedenbeck, M. E.

2012-12-01

Solar energetic particle (SEP) mean ionic charge states can depend on source temperatures and populations (e.g. seed populations) and conditions during acceleration and transport such as stripping. Multi-spacecraft observations of charge states from widely separated spacecraft may reveal evidence for seed populations that vary with longitude. In this presentation, we report new estimates of inferred high energy ionic charge states using the Sollitt et al. (2008) method that fits SEP energy-dependent decay times for SEP event elements to derive mean charge states. In the method, intensity decay times during SEP events are fitted for each element for various energies, and then the energy dependence of the decay times is fitted for each element. Finally, charge-to-mass ratios relative to that of a calibration element (carbon in this case) are obtained, and when Q(C)=5.9 is assumed for calibration, mean charge states for other elements can be inferred. Previously, ACE/SIS and ACE/ULEIS data were applied to three SEP events (Nov. 6, 1997; Nov. 4, 2001; Apr. 21, 2002) with this method, and last year, we reported new results for the Dec. 6, 2006 SEP event compatible with SAMPEX/MAST results. Additional work continues to generalize and extend the software to use publicly available online data from ACE and the two STEREO spacecraft. Energy ranges are those covered by the instruments on ACE (e.g. reference element C at <.1 MeV/nuc from ULEIS to ~64 MeV/nuc from SIS) and on STEREO (e.g. C at 3.2 - 33 MeV/nuc from LET). Initial candidate SEP events for multi-spacecraft charge state estimates are those of Mar. 8, 2011, Mar. 21, 2011, Jan. 24, 2012, and Mar. 4, 2012. Results from events observed by single spacecraft may also be reported.

Field-induced exciton dissociation in PTB7-based organic solar cells

NASA Astrophysics Data System (ADS)

Gerhard, Marina; Arndt, Andreas P.; Bilal, Mühenad; Lemmer, Uli; Koch, Martin; Howard, Ian A.

2017-05-01

The physics of charge separation in organic semiconductors is a topic of ongoing research of relevance to material and device engineering. Herein, we present experimental observations of the field and temperature dependence of charge separation from singlet excitons in PTB7 and PC71BM , and from charge-transfer states created across interfaces in PTB 7 /PC71BM bulk heterojunction solar cells. We obtain this experimental data by time-resolving the near infrared emission of the states from 10 K to room temperature and electric fields from 0 to 2.5 MVcm -1 . Examining how the luminescence is quenched by field and temperature gives direct insight into the underlying physics. We observe that singlet excitons can be split by high fields, and that disorder broadens the high threshold fields needed to split the excitons. Charge-transfer (CT) states, on the other hand, can be separated by both field and temperature. Also, the data imply a strong reduction of the activation barrier for charge splitting from the CT state relative to the exciton state. The observations provided herein of the field-dependent separation of CT states as a function of temperature offer a rich data set against which theoretical models of charge separation can be rigorously tested; it should be useful for developing the more advanced theoretical models of charge separation.

FIRST-PRINCIPLES CALCULATIONS OF CHARGE STATES AND FORMATION ENERGIES OF Mg, Al, and Be TRANSMUTANTS IN 3C-SiC

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

Hu, Shenyang Y.; Setyawan, Wahyu; Jiang, Weilin

2014-08-28

The Vienna Ab-initio Simulation Package (VASP) is employed to calculate charge states and the formation energies of Mg, Al and Be transmutants at different lattice sites in 3C-SiC. The results provide important information on the dependence of the most stable charge state and formation energy of Mg, Al, Be and vacancies on electron potentials.

Photo-dynamics of roseoflavin and riboflavin in aqueous and organic solvents

NASA Astrophysics Data System (ADS)

Zirak, P.; Penzkofer, A.; Mathes, T.; Hegemann, P.

2009-03-01

Roseoflavin (8-dimethylamino-8-demethyl- D-riboflavin) and riboflavin in aqueous and organic solvents are studied by optical absorption spectroscopy, fluorescence spectroscopy, and fluorescence decay kinetics. Solvent polarity dependent absorption shifts are observed. The fluorescence quantum yields are solvent dependent. For roseoflavin the fluorescence decay shows a bi-exponential dependence (ps to sub-ps time constant, and 100 ps to a few ns time constant). The roseoflavin photo-dynamics is explained in terms of fast intra-molecular charge transfer (diabatic electron transfer) from the dimethylamino electron donor group to the pteridin carbonyl electron acceptor followed by intra-molecular charge recombination. The fast fluorescence component is due to direct locally-excited-state emission, and the slow fluorescence component is due to delayed locally-excited-state emission and charge transfer state emission. The fluorescence decay of riboflavin is mono-exponential. The S 1-state potential energy surface is determined by vibronic relaxation and solvation dynamics due to excited-state dipole moment changes (adiabatic optical electron transfer).

Method and apparatus for controlling battery charging in a hybrid electric vehicle

DOEpatents

Phillips, Anthony Mark; Blankenship, John Richard; Bailey, Kathleen Ellen; Jankovic, Miroslava

2003-06-24

A starter/alternator system (24) for hybrid electric vehicle (10) having an internal combustion engine (12) and an energy storage device (34) has a controller (30) coupled to the starter/alternator (26). The controller (30) has a state of charge manager (40) that monitors the state of charge of the energy storage device. The controller has eight battery state-of-charge threshold values that determine the hybrid operating mode of the hybrid electric vehicle. The value of the battery state-of-charge relative to the threshold values is a factor in the determination of the hybrid mode, for example; regenerative braking, charging, battery bleed, boost. The starter/alternator may be operated as a generator or a motor, depending upon the mode.

Charge density dependent mobility of organic hole-transporters and mesoporous TiO₂ determined by transient mobility spectroscopy: implications to dye-sensitized and organic solar cells.

PubMed

Leijtens, Tomas; Lim, Jongchul; Teuscher, Joël; Park, Taiho; Snaith, Henry J

2013-06-18

Transient mobility spectroscopy (TMS) is presented as a new tool to probe the charge carrier mobility of commonly employed organic and inorganic semiconductors over the relevant range of charge densities. The charge density dependence of the mobility of semiconductors used in hybrid and organic photovoltaics gives new insights into charge transport phenomena in solid state dye sensitized solar cells. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

A simple model of solvent-induced symmetry-breaking charge transfer in excited quadrupolar molecules

NASA Astrophysics Data System (ADS)

Ivanov, Anatoly I.; Dereka, Bogdan; Vauthey, Eric

2017-04-01

A simple model has been developed to describe the symmetry-breaking of the electronic distribution of AL-D-AR type molecules in the excited state, where D is an electron donor and AL and AR are identical acceptors. The origin of this process is usually associated with the interaction between the molecule and the solvent polarization that stabilizes an asymmetric and dipolar state, with a larger charge transfer on one side than on the other. An additional symmetry-breaking mechanism involving the direct Coulomb interaction of the charges on the acceptors is proposed. At the same time, the electronic coupling between the two degenerate states, which correspond to the transferred charge being localised either on AL or AR, favours a quadrupolar excited state with equal amount of charge-transfer on both sides. Because of these counteracting effects, symmetry breaking is only feasible when the electronic coupling remains below a threshold value, which depends on the solvation energy and the Coulomb repulsion energy between the charges located on AL and AR. This model allows reproducing the solvent polarity dependence of the symmetry-breaking reported recently using time-resolved infrared spectroscopy.

On the nature of high field charge transport in reinforced silicone dielectrics: Experiment and simulation

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

Huang, Yanhui, E-mail: huangy12@rpi.edu; Schadler, Linda S.

The high field charge injection and transport properties in reinforced silicone dielectrics were investigated by measuring the time-dependent space charge distribution and the current under dc conditions up to the breakdown field and were compared with the properties of other dielectric polymers. It is argued that the energy and spatial distribution of localized electronic states are crucial in determining these properties for polymer dielectrics. Tunneling to localized states likely dominates the charge injection process. A transient transport regime arises due to the relaxation of charge carriers into deep traps at the energy band tails and is successfully verified by amore » Monte Carlo simulation using the multiple-hopping model. The charge carrier mobility is found to be highly heterogeneous due to the non-uniform trapping. The slow moving electron packet exhibits a negative field dependent drift velocity possibly due to the spatial disorder of traps.« less

Voltage-Dependent Charge Storage in Cladded Zn0.56Cd0.44Se Quantum Dot MOS Capacitors for Multibit Memory Applications

NASA Astrophysics Data System (ADS)

Khan, J.; Lingalugari, M.; Al-Amoody, F.; Jain, F.

2013-11-01

As conventional memories approach scaling limitations, new storage methods must be utilized to increase Si yield and produce higher on-chip memory density. Use of II-VI Zn0.56Cd0.44Se quantum dots (QDs) is compatible with epitaxial gate insulators such as ZnS-ZnMgS. Voltage-dependent charging effects in cladded Zn0.56Cd0.44Se QDs are presented in a conventional metal-oxide-semiconductor capacitor structure. Charge storage capabilities in Si and ZnMgS QDs have been reported by various researchers; this work is focused on II-VI material Zn0.56Cd0.44Se QDs nucleated using photoassisted microwave plasma metalorganic chemical vapor deposition. Using capacitance-voltage hysteresis characterization, the multistep charging and discharging capabilities of the QDs at room temperature are presented. Three charging states are presented within a 10 V charging voltage range. These characteristics exemplify discrete charge states in the QD layer, perfect for multibit, QD-functionalized high-density memory applications. Multiple charge states with low operating voltage provide device characteristics that can be used for multibit storage by allowing varying charges to be stored in a QD layer based on the applied "write" voltage.

Space charge in nanostructure resonances

NASA Astrophysics Data System (ADS)

Price, Peter J.

1996-10-01

In quantum ballistic propagation of electrons through a variety of nanostructures, resonance in the energy-dependent transmission and reflection probabilities generically is associated with (1) a quasi-level with a decay lifetime, and (2) a bulge in electron density within the structure. It can be shown that, to a good approximation, a simple formula in all cases connects the density of states for the latter to the energy dependence of the phase angles of the eigen values of the S-matrix governing the propagation. For both the Lorentzian resonances (normal or inverted) and for the Fano-type resonances, as a consequence of this eigen value formula, the space charge due to filled states over the energy range of a resonance is just equal (for each spin state) to one electron charge. The Coulomb interaction within this space charge is known to 'distort' the electrical characteristics of resonant nanostructures. In these systems, however, the exchange effect should effectively cancel the interaction between states with parallel spins, leaving only the anti-parallel spin contribution.

Criminal Charges for Child Harm from Substance Use in Pregnancy.

PubMed

Angelotta, Cara; Appelbaum, Paul S

2017-06-01

Despite the opposition of medical and public health professionals, several state legislatures are considering laws that permit child abuse charges for substance use during pregnancy. We reviewed legal decisions regarding women charged with a crime against a fetus or child as a result of substance use during pregnancy. We identified 24 judicial opinions published between 1977 and 2015 in cases involving 29 women prosecuted in 19 states. Charges included child endangerment, child abuse, drug delivery, attempted aggravated child abuse, chemical endangerment of a child, child neglect, child mistreatment, homicide, manslaughter, and reckless injury to a child. The substances related to the charges included cocaine, heroin, methamphetamine, marijuana, and prescription pills. Proceedings resulted in dismissal of the charges or convictions overturned for 86.2 percent of the women. In all of the cases, the judicial decision depended on the disposition of the question of whether, for the purpose of adjudicating the criminal charges, a fetus is a child. The balance in the courts in favor of treating substance use during pregnancy as a medical problem depends on the definition of a child for the purposes of criminal statutes. Professional advocacy may best be directed at state legislatures. © 2017 American Academy of Psychiatry and the Law.

Conducting ion tracks generated by charge-selected swift heavy ions

NASA Astrophysics Data System (ADS)

Gupta, Srashti; Gehrke, H. G.; Krauser, J.; Trautmann, C.; Severin, D.; Bender, M.; Rothard, H.; Hofsäss, H.

2016-08-01

Conducting ion tracks in tetrahedral amorphous carbon (ta-C) thin films were generated by irradiation with swift heavy ions of well-defined charge state. The conductivity of tracks and the surface topography of the films, showing characteristic hillocks at each track position, were investigated using conductive atomic force microscopy measurements. The dependence of track conductivity and hillock size on the charge state of the ions was studied using 4.6 MeV/u Pb ions of charge state 53+, 56+ and 60+ provided by GANIL, as well as 4.8 MeV/u Bi and Au ions of charge state from 50+ to 61+ and 4.2 MeV/u 238U ions in equilibrium charge state provided by UNILAC of GSI. For the charge state selection at GSI, an additional stripper-foil system was installed at the M-branch that now allows routine irradiations with ions of selected charge states. The conductivity of tracks in ta-C increases significantly when the charge state increases from 51+ to 60+. However, the conductivity of individual tracks on the same sample still shows large variations, indicating that tracks formed in ta-C are either inhomogeneous or the conductivity is limited by the interface between ion track and Si substrate.

Heat loss distribution: Impedance and thermal loss analyses in LiFePO4/graphite 18650 electrochemical cell

NASA Astrophysics Data System (ADS)

Balasundaram, Manikandan; Ramar, Vishwanathan; Yap, Christopher; Lu, Li; Tay, Andrew A. O.; Palani, Balaya

2016-10-01

We report here thermal behaviour and various components of heat loss of 18650-type LiFePO4/graphite cell at different testing conditions. In this regard, the total heat generated during charging and discharging processes at various current rates (C) has been quantified in an Accelerating Rate Calorimeter experiment. Irreversible heat generation, which depends on applied current and internal cell resistance, is measured under corresponding charge/discharge conditions using intermittent pulse techniques. On the other hand, reversible heat generation which depends on entropy changes of the electrode materials during the cell reaction is measured from the determination of entropic coefficient at various states of charge/discharge. The contributions of irreversible and reversible heat generation to the total heat generation at both high and low current rates are evaluated. At every state of charge/discharge, the nature of the cell reaction is found to be either exothermic or endothermic which is especially evident at low C rates. In addition, electrochemical impedance spectroscopy measurements are performed on above 18650 cells at various states of charge to determine the components of internal resistance. The findings from the impedance and thermal loss analysis are helpful for understanding the favourable states of charge/discharge for battery operation, and designing better thermal management systems.

Convergence of the Light-Front Coupled-Cluster Method in Scalar Yukawa Theory

NASA Astrophysics Data System (ADS)

Usselman, Austin

We use Fock-state expansions and the Light-Front Coupled-Cluster (LFCC) method to study mass eigenvalue problems in quantum field theory. Specifically, we study convergence of the method in scalar Yukawa theory. In this theory, a single charged particle is surrounded by a cloud of neutral particles. The charged particle can create or annihilate neutral particles, causing the n-particle state to depend on the n + 1 and n - 1-particle state. Fock state expansion leads to an infinite set of coupled equations where truncation is required. The wave functions for the particle states are expanded in a basis of symmetric polynomials and a generalized eigenvalue problem is solved for the mass eigenvalue. The mass eigenvalue problem is solved for multiple values for the coupling strength while the number of particle states and polynomial basis order are increased. Convergence of the mass eigenvalue solutions is then obtained. Three mass ratios between the charged particle and neutral particles were studied. This includes a massive charged particle, equal masses and massive neutral particles. Relative probability between states can also be explored for more detailed understanding of the process of convergence with respect to the number of Fock sectors. The reliance on higher order particle states depended on how large the mass of the charge particle was. The higher the mass of the charged particle, the more the system depended on higher order particle states. The LFCC method solves this same mass eigenvalue problem using an exponential operator. This exponential operator can then be truncated instead to form a finite system of equations that can be solved using a built in system solver provided in most computational environments, such as MatLab and Mathematica. First approximation in the LFCC method allows for only one particle to be created by the new operator and proved to be not powerful enough to match the Fock state expansion. The second order approximation allowed one and two particles to be created by the new operator and converged to the Fock state expansion results. This showed the LFCC method to be a reliable replacement method for solving quantum field theory problems.

Thermodynamics of emergent magnetic charge screening in artificial spin ice

DOE PAGES

Farhan, Alan; Scholl, Andreas; Petersen, Charlotte F.; ...

2016-09-01

Electric charge screening is a fundamental principle governing the behaviour in a variety of systems in nature. Through reconfiguration of the local environment, the Coulomb attraction between electric charges is decreased, leading, for example, to the creation of polaron states in solids or hydration shells around proteins in water. Here, we directly visualize the real-time creation and decay of screened magnetic charge configurations in a two-dimensional artificial spin ice system, the dipolar dice lattice. By comparing the temperature dependent occurrence of screened and unscreened emergent magnetic charge defects, we determine that screened magnetic charges are indeed a result of localmore » energy reduction and appear as a transient minimum energy state before the system relaxes towards the predicted ground state. These results highlight the important role of emergent magnetic charges in artificial spin ice, giving rise to screened charge excitations and the emergence of exotic low-temperature configurations.« less

Thermodynamics of emergent magnetic charge screening in artificial spin ice

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

Farhan, Alan; Scholl, Andreas; Petersen, Charlotte F.

Electric charge screening is a fundamental principle governing the behaviour in a variety of systems in nature. Through reconfiguration of the local environment, the Coulomb attraction between electric charges is decreased, leading, for example, to the creation of polaron states in solids or hydration shells around proteins in water. Here, we directly visualize the real-time creation and decay of screened magnetic charge configurations in a two-dimensional artificial spin ice system, the dipolar dice lattice. By comparing the temperature dependent occurrence of screened and unscreened emergent magnetic charge defects, we determine that screened magnetic charges are indeed a result of localmore » energy reduction and appear as a transient minimum energy state before the system relaxes towards the predicted ground state. These results highlight the important role of emergent magnetic charges in artificial spin ice, giving rise to screened charge excitations and the emergence of exotic low-temperature configurations.« less

Photoinduced transition to charge-ordered phases from dynamical localization in the metallic phase of α -(BEDT-TTF)2I3

NASA Astrophysics Data System (ADS)

Oya, Koudai; Takahashi, Akira

2018-03-01

From theory, we investigate charge localization induced by higher-frequency off-resonance light-pulse excitation in the metallic phase of α -(BEDT-TTF) 2I3 by numerically solving the time-dependent Schrödinger equation in the quarter-filled extended Hubbard model for the material. Around e a A(max )=1 , where e a A(max ) is the maximum amplitude of the dimensionless vector potential of the pump pulse, the charge distribution is significantly changed by photoexcitation, and the light-pulse-induced collective charge oscillations continue after photoexcitation. Furthermore, the charge dynamics depend strongly on the polarization direction of the pump pulse. These results are consistent with experiment. The magnitudes of the effective transfer integrals are reduced by strong photoexcitation, and this precursory phenomenon for dynamical localization is mainly driven by a photoinduced change in the ratio of the effective transfer integrals between the two strongest bonds. For e a A(max )≳2 , the photoinduced transition to the charge-ordered state, which can be regarded as a light-dressed state, occurs because of dynamical localization. Furthermore, the type of photogenerated charge-ordered state can be controlled by choosing e a A(max ) and the polarization direction.

How Many Parameters Actually Affect the Mobility of Conjugated Polymers?

NASA Astrophysics Data System (ADS)

Fornari, Rocco P.; Blom, Paul W. M.; Troisi, Alessandro

2017-02-01

We describe charge transport along a polymer chain with a generic theoretical model depending in principle on tens of parameters, reflecting the chemistry of the material. The charge carrier states are obtained from a model Hamiltonian that incorporates different types of disorder and electronic structure (e.g., the difference between homo- and copolymer). The hopping rate between these states is described with a general rate expression, which contains the rates most used in the literature as special cases. We demonstrate that the steady state charge mobility in the limit of low charge density and low field ultimately depends on only two parameters: an effective structural disorder and an effective electron-phonon coupling, weighted by the size of the monomer. The results support the experimental observation [N. I. Craciun, J. Wildeman, and P. W. M. Blom, Phys. Rev. Lett. 100, 056601 (2008), 10.1103/PhysRevLett.100.056601] that the mobility in a broad range of (polymeric) semiconductors follows a universal behavior, insensitive to the chemical detail.

Lowest energy Frenkel and charge transfer exciton intermixing in one-dimensional copper phthalocyanine molecular lattice

NASA Astrophysics Data System (ADS)

Bondarev, I. V.; Popescu, A.; Younts, R. A.; Hoffman, B.; McAfee, T.; Dougherty, D. B.; Gundogdu, K.; Ade, H. W.

2016-11-01

We report the results of the combined experimental and theoretical studies of the low-lying exciton states in crystalline copper phthalocyanine. We derive the eigen energy spectrum for the two lowest intramolecular Frenkel excitons coupled to the intermolecular charge transfer exciton state and compare it with temperature dependent optical absorption spectra measured experimentally, to obtain the parameters of the Frenkel-charge-transfer exciton intermixing. The two Frenkel exciton states are spaced apart by 0.26 eV, and the charge transfer exciton state is 50 meV above the lowest Frenkel exciton. Both Frenkel excitons are strongly mixed with the charge transfer exciton, showing the coupling constant 0.17 eV which agrees with earlier experimental measurements. These results can be used for the proper interpretation of the physical properties of crystalline phthalocyanines.

Ellipticity-dependent of multiple ionisation methyl iodide cluster using 532 nm nanosecond laser

NASA Astrophysics Data System (ADS)

Tang, Bin; Zhao, Wuduo; Wang, Weiguo; Hua, Lei; Chen, Ping; Hou, Keyong; Huang, Yunguang; Li, Haiyang

2016-03-01

The dependence of multiply charged ions on laser ellipticity in methyl iodide clusters with 532 nm nanosecond laser was measured using a time-of-flight mass spectrometer. The intensities of multiply charged ions Iq+(q = 2-4) with circularly polarised laser pulse were clearly higher than those with linearly polarised laser pulse but the intensity of single charged ions I+ was inverse. And the dependences of ions on the optical polarisation state were investigated and a flower petal and square distribution for single charged ions (I+, C+) and multiply charged ions (I2+, I3+, I4+, C2+) were observed, respectively. A theoretical calculation was also proposed to simulate the distributions of ions and theoretical results fitted well with the experimental ones. It indicated that the high multiphoton ionisation probability in the initial stage would result in the disintegration of big clusters into small ones and suppress the production of multiply charged ions.

Energy-Dependent Ionization States of Shock-Accelerated Particles in the Solar Corona

NASA Technical Reports Server (NTRS)

Reames, Donald V.; Ng, C. K.; Tylka, A. J.

2000-01-01

We examine the range of possible energy dependence of the ionization states of ions that are shock-accelerated from the ambient plasma of the solar corona. If acceleration begins in a region of moderate density, sufficiently low in the corona, ions above about 0.1 MeV/amu approach an equilibrium charge state that depends primarily upon their speed and only weakly on the plasma temperature. We suggest that the large variations of the charge states with energy for ions such as Si and Fe observed in the 1997 November 6 event are consistent with stripping in moderately dense coronal. plasma during shock acceleration. In the large solar-particle events studied previously, acceleration occurs sufficiently high in the corona that even Fe ions up to 600 MeV/amu are not stripped of electrons.

Study of photon emission by electron capture during solar nuclei acceleration, 1: Temperature-dependent cross section for charge changing processes

NASA Technical Reports Server (NTRS)

Perez-Peraza, J.; Alvarez, M.; Laville, A.; Gallegos, A.

1985-01-01

The study of charge changing cross sections of fast ions colliding with matter provides the fundamental basis for the analysis of the charge states produced in such interactions. Given the high degree of complexity of the phenomena, there is no theoretical treatment able to give a comprehensive description. In fact, the involved processes are very dependent on the basic parameters of the projectile, such as velocity charge state, and atomic number, and on the target parameters, the physical state (molecular, atomic or ionized matter) and density. The target velocity, may have also incidence on the process, through the temperature of the traversed medium. In addition, multiple electron transfer in single collisions intrincates more the phenomena. Though, in simplified cases, such as protons moving through atomic hydrogen, considerable agreement has been obtained between theory and experiments However, in general the available theoretical approaches have only limited validity in restricted regions of the basic parameters. Since most measurements of charge changing cross sections are performed in atomic matter at ambient temperature, models are commonly based on the assumption of targets at rest, however at Astrophysical scales, temperature displays a wide range in atomic and ionized matter. Therefore, due to the lack of experimental data , an attempt is made here to quantify temperature dependent cross sections on basis to somewhat arbitrary, but physically reasonable assumptions.

Charge Separation and Exciton Dynamics at Polymer/ZnO Interface from First-Principles Simulations.

PubMed

Wu, Guangfen; Li, Zi; Zhang, Xu; Lu, Gang

2014-08-07

Charge separation and exciton dynamics play a crucial role in determining the performance of excitonic photovoltaics. Using time-dependent density functional theory with a range-separated exchange-correlation functional as well as nonadiabatic ab initio molecular dynamics, we have studied the formation and dynamics of charge-transfer (CT) excitons at polymer/ZnO interface. The interfacial atomic structure, exciton density of states and conversions between exciton species are examined from first-principles. The exciton dynamics exhibits both adiabatic and nonadiabatic characters. While the adiabatic transitions are facilitated by C═C vibrations along the polymer (P3HT) backbone, the nonadiabatic transitions are realized by exciton hopping between the excited states. We find that the localized ZnO surface states lead to localized low-energy CT states and poor charge separation. In contrast, the surface states of crystalline C60 are indistinguishable from the bulk states, resulting in delocalized CT states and efficient charge separation in polymer/fullerene (P3HT/PCBM) heterojunctions. The hot CT states are found to cool down in an ultrafast time scale and may not play a major role in charge separation of P3HT/ZnO. Finally we suggest that the dimensions of nanostructured acceptors can be tuned to obtain both efficient charge separation and high open circuit voltages.

Electronic properties of B and Al doped graphane: A hybrid density functional study

NASA Astrophysics Data System (ADS)

Mapasha, R. E.; Igumbor, E.; Andriambelaza, N. F.; Chetty, N.

2018-04-01

Using a hybrid density functional theory approach parametrized by Heyd, Scuseria and Ernzerhof (HSE06 hybrid functional), we study the energetics, structural and electronic properties of a graphane monolayer substitutionally doped with the B (BCH) and Al (AlCH) atoms. The BCH defect can be integrated within a graphane monolayer at a relative low formation energy, without major structural distortions and symmetry breaking. The AlCH defect relaxes outward of the monolayer and breaks the symmetry. The density of states plots indicate that BCH doped graphane monolayer is a wide band gap semiconductor, whereas the AlCH defect introduces the spin dependent mid gap states at the vicinity of the Fermi level, revealing a metallic character with the pronounced magnetic features. We further examine the response of the Al dependent spin states on the multiple charge states doping. We find that the defect formation energy, structural and electronic properties can be altered via charge state modulation. The +1 charge doping opens an energy band gap of 1.75 eV. This value corresponds to the wavelength in the visible spectrum, suggesting an ideal material for solar cell absorbers. Our study fine tunes the graphane band gap through the foreign atom doping as well as via defect charge state modulation.

Coherent and Semiclassical States of a Charged Particle in a Constant Electric Field

NASA Astrophysics Data System (ADS)

Adorno, T. C.; Pereira, A. S.

2018-05-01

The method of integrals of motion is used to construct families of generalized coherent states of a nonrelativistic spinless charged particle in a constant electric field. Families of states, differing in the values of their standard deviations at the initial time, are obtained. Depending on the initial values of the standard deviations, and also on the electric field, it turns out to be possible to identify some families with semiclassical states.

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

NASA Astrophysics Data System (ADS)

Yang, Chou-Hsun; Hsu, Chao-Ping

2013-10-01

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

Sulfonium Ion Derivatization, Isobaric Stable Isotope Labeling and Data Dependent CID- and ETD-MS/MS for Enhanced Phosphopeptide Quantitation, Identification and Phosphorylation Site Characterization

PubMed Central

Lu, Yali; Zhou, Xiao; Stemmer, Paul M.; Reid, Gavin E.

2014-01-01

An amine specific peptide derivatization strategy involving the use of novel isobaric stable isotope encoded ‘fixed charge’ sulfonium ion reagents, coupled with an analysis strategy employing capillary HPLC, ESI-MS, and automated data dependent ion trap CID-MS/MS, -MS3, and/or ETD-MS/MS, has been developed for the improved quantitative analysis of protein phosphorylation, and for identification and characterization of their site(s) of modification. Derivatization of 50 synthetic phosphopeptides with S,S′-dimethylthiobutanoylhydroxysuccinimide ester iodide (DMBNHS), followed by analysis using capillary HPLC-ESI-MS, yielded an average 2.5-fold increase in ionization efficiencies and a significant increase in the presence and/or abundance of higher charge state precursor ions compared to the non-derivatized phosphopeptides. Notably, 44% of the phosphopeptides (22 of 50) in their underivatized states yielded precursor ions whose maximum charge states corresponded to +2, while only 8% (4 of 50) remained at this maximum charge state following DMBNHS derivatization. Quantitative analysis was achieved by measuring the abundances of the diagnostic product ions corresponding to the neutral losses of ‘light’ (S(CH3)2) and ‘heavy’ (S(CD3)2) dimethylsulfide exclusively formed upon CID-MS/MS of isobaric stable isotope labeled forms of the DMBNHS derivatized phosphopeptides. Under these conditions, the phosphate group stayed intact. Access for a greater number of peptides to provide enhanced phosphopeptide sequence identification and phosphorylation site characterization was achieved via automated data-dependent CID-MS3 or ETD-MS/MS analysis due to the formation of the higher charge state precursor ions. Importantly, improved sequence coverage was observed using ETD-MS/MS following introduction of the sulfonium ion fixed charge, but with no detrimental effects on ETD fragmentation efficiency. PMID:21952753

Describing long-range charge-separation processes with subsystem density-functional theory

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

Solovyeva, Alisa; Neugebauer, Johannes, E-mail: j.neugebauer@uni-muenster.de; Pavanello, Michele, E-mail: m.pavanello@rutgers.edu

2014-04-28

Long-range charge-transfer processes in extended systems are difficult to describe with quantum chemical methods. In particular, cost-effective (non-hybrid) approximations within time-dependent density functional theory (DFT) are not applicable unless special precautions are taken. Here, we show that the efficient subsystem DFT can be employed as a constrained DFT variant to describe the energetics of long-range charge-separation processes. A formal analysis of the energy components in subsystem DFT for such excitation energies is presented, which demonstrates that both the distance dependence and the long-range limit are correctly described. In addition, electronic couplings for these processes as needed for rate constants inmore » Marcus theory can be obtained from this method. It is shown that the electronic structure of charge-separated states constructed by a positively charged subsystem interacting with a negatively charged one is difficult to converge — charge leaking from the negative subsystem to the positive one can occur. This problem is related to the delocalization error in DFT and can be overcome with asymptotically correct exchange–correlation (XC) potentials or XC potentials including a sufficiently large amount of exact exchange. We also outline an approximate way to obtain charge-transfer couplings between locally excited and charge-separated states.« less

Voltage-induced Metal-Insulator Transitions in Perovskite Oxide Thin Films Doped with Strongly Correlelated Electrons

NASA Astrophysics Data System (ADS)

Wang, Yudi; Gil Kim, Soo; Chen, I.-Wei

2007-03-01

We have observed a reversible metal-insulator transition in perovskite oxide thin films that can be controlled by charge trapping pumped by a bipolar voltage bias. In the as-fabricated state, the thin film is metallic with a very low resistance comparable to that of the metallic bottom electrode, showing decreasing resistance with decreasing temperature. This metallic state switches to a high-resistance state after applying a voltage bias: such state is non-ohmic showing a negative temperature dependence of resistance. Switching at essentially the same voltage bias was observed down to 2K. The metal-insulator transition is attributed to charge trapping that disorders the energy of correlated electron states in the conduction band. By increasing the amount of charge trapped, which increases the disorder relative to the band width, increasingly more insulating states with a stronger temperature dependence of resistivity are accessed. This metal-insulator transition provides a platform to engineer new nonvolatile memory that does not require heat (as in phase transition) or dielectric breakdown (as in most other oxide resistance devices).

Ionization, evaporation and fragmentation of C60 in collisions with highly charged C, O and F ions—effect of projectile charge state.

NASA Astrophysics Data System (ADS)

Kelkar, A. H.; Misra, D.; Tribedi, L. C.

2007-09-01

We study the various inelastic processes such ionization, fragmentation and evaporation of C60 molecule in collisions with fast heavy ions. We have used 2.33 MeV/u C, O and F projectile ion beams. Various ionization and fragmentation products were detected using time-of-flight mass spectrometer. The multiply charged C60r+ ions were detected for maximum r = 4. The projectile charge state (qp) dependence of the single and double ionization cross sections is well reproduced by a model based on the giant dipole plasmon resonance (GDPR). The qp-dependence of the fragmentation yields, was found to be linear. Variation of relative yields of the evaporation products of C602+ (i.e. C582+, C562+ etc) and C603+ (i.e. C583+, C563+ etc) with qp has also been investigated for various projectiles.

Charge transfer transitions in optical spectra of NicMg1-cO oxides

NASA Astrophysics Data System (ADS)

Churmanov, V. N.; Sokolov, V. I.; Pustovarov, V. A.; Gruzdev, N. B.; Uimin, M. A.; Byzov, I. V.; Druzhinin, A. V.; Korolyov, A. V.; Kim, G. A.; Zatsepin, A. F.; Kuznetsova, J. A.

2017-04-01

Radiative recombination with charge transfer was observed in NicMg1-cO (c = 0.008) oxides over the 8-300 K temperature range. This recombination occurs as a result of strong hybridization of the Ni2+ ion 3d-states and the band states. The charge transfer radiation excitation spectrum shows vibrational LO repeats of two exciton lines having charge transfer energy intervals of about 35 meV. The NiO nanocrystal absorption spectrum shows two weak peaks with energies of 3.510 and 3.543 eV, which are highly dependent on temperature. They are interpreted as charge transfer excitons at the edge of NiO fundamental absorption. The distance between the charge transfer exciton lines in the NicMg1-cO oxide spectra are caused by spin-orbit splitting of the valence band peak that was formed by the p-states of the oxygen ion.

Interlayer‐State‐Coupling Dependent Ultrafast Charge Transfer in MoS2/WS2 Bilayers

PubMed Central

Zhang, Jin; Hong, Hao; Lian, Chao; Ma, Wei; Xu, Xiaozhi; Zhou, Xu; Fu, Huixia

2017-01-01

Light‐induced interlayer ultrafast charge transfer in 2D heterostructures provides a new platform for optoelectronic and photovoltaic applications. The charge separation process is generally hypothesized to be dependent on the interlayer stackings and interactions, however, the quantitative characteristic and detailed mechanism remain elusive. Here, a systematical study on the interlayer charge transfer in model MoS2/WS2 bilayer system with variable stacking configurations by time‐dependent density functional theory methods is demonstrated. The results show that the slight change of interlayer geometry can significantly modulate the charge transfer time from 100 fs to 1 ps scale. Detailed analysis further reveals that the transfer rate in MoS2/WS2 bilayers is governed by the electronic coupling between specific interlayer states, rather than the interlayer distances, and follows a universal dependence on the state‐coupling strength. The results establish the interlayer stacking as an effective freedom to control ultrafast charge transfer dynamics in 2D heterostructures and facilitate their future applications in optoelectronics and light harvesting. PMID:28932669

Local Time-Dependent Charging in a Perovskite Solar Cell.

PubMed

Bergmann, Victor W; Guo, Yunlong; Tanaka, Hideyuki; Hermes, Ilka M; Li, Dan; Klasen, Alexander; Bretschneider, Simon A; Nakamura, Eiichi; Berger, Rüdiger; Weber, Stefan A L

2016-08-03

Efficient charge extraction within solar cells explicitly depends on the optimization of the internal interfaces. Potential barriers, unbalanced charge extraction, and interfacial trap states can prevent cells from reaching high power conversion efficiencies. In the case of perovskite solar cells, slow processes happening on time scales of seconds cause hysteresis in the current-voltage characteristics. In this work, we localized and investigated these slow processes using frequency-modulation Kelvin probe force microscopy (FM-KPFM) on cross sections of planar methylammonium lead iodide (MAPI) perovskite solar cells. FM-KPFM can map the charge density distribution and its dynamics at internal interfaces. Upon illumination, space charge layers formed at the interfaces of the selective contacts with the MAPI layer within several seconds. We observed distinct differences in the charging dynamics at the interfaces of MAPI with adjacent layers. Our results indicate that more than one process is involved in hysteresis. This finding is in agreement with recent simulation studies claiming that a combination of ion migration and interfacial trap states causes the hysteresis in perovskite solar cells. Such differences in the charging rates at different interfaces cannot be separated by conventional device measurements.

Non-equilibrium dynamics in disordered materials: Ab initio molecular dynamics simulations

NASA Astrophysics Data System (ADS)

Ohmura, Satoshi; Nagaya, Kiyonobu; Shimojo, Fuyuki; Yao, Makoto

2015-08-01

The dynamic properties of liquid B2O3 under pressure and highly-charged bromophenol molecule are studied by using molecular dynamics (MD) simulations based on density functional theory (DFT). Diffusion properties of covalent liquids under high pressure are very interesting in the sense that they show unexpected pressure dependence. It is found from our simulation that the magnitude relation of diffusion coefficients for boron and oxygen in liquid B2O3 shows the anomalous pressure dependence. The simulation clarified the microscopic origin of the anomalous diffusion properties. Our simulation also reveals the dissociation mechanism in the coulomb explosion of the highly-charged bromophenol molecule. When the charge state n is 6, hydrogen atom in the hydroxyl group dissociates at times shorter than 20 fs while all hydrogen atoms dissociate when n is 8. After the hydrogen dissociation, the carbon ring breaks at about 100 fs. There is also a difference on the mechanism of the ring breaking depending on charge states, in which the ring breaks with expanding (n = 6) or shrink (n = 8).

Solute location in a nanoconfined liquid depends on charge distribution

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

Harvey, Jacob A.; Thompson, Ward H., E-mail: wthompson@ku.edu

2015-07-28

Nanostructured materials that can confine liquids have attracted increasing attention for their diverse properties and potential applications. Yet, significant gaps remain in our fundamental understanding of such nanoconfined liquids. Using replica exchange molecular dynamics simulations of a nanoscale, hydroxyl-terminated silica pore system, we determine how the locations explored by a coumarin 153 (C153) solute in ethanol depend on its charge distribution, which can be changed through a charge transfer electronic excitation. The solute position change is driven by the internal energy, which favors C153 at the pore surface compared to the pore interior, but less so for the more polar,more » excited-state molecule. This is attributed to more favorable non-specific solvation of the large dipole moment excited-state C153 by ethanol at the expense of hydrogen-bonding with the pore. It is shown that a change in molecule location resulting from shifts in the charge distribution is a general result, though how the solute position changes will depend upon the specific system. This has important implications for interpreting measurements and designing applications of mesoporous materials.« less

Pressure dependence of excited-state charge-carrier dynamics in organolead tribromide perovskites

NASA Astrophysics Data System (ADS)

Liu, X. C.; Han, J. H.; Zhao, H. F.; Yan, H. C.; Shi, Y.; Jin, M. X.; Liu, C. L.; Ding, D. J.

2018-05-01

Excited-state charge-carrier dynamics governs the performance of organometal trihalide perovskites (OTPs) and is strongly influenced by the crystal structure. Characterizing the excited-state charge-carrier dynamics in OTPs under high pressure is imperative for providing crucial insights into structure-property relations. Here, we conduct in situ high-pressure femtosecond transient absorption spectroscopy experiments to study the excited-state carrier dynamics of CH3NH3PbBr3 (MAPbBr3) under hydrostatic pressure. The results indicate that compression is an effective approach to modulate the carrier dynamics of MAPbBr3. Across each pressure-induced phase, carrier relaxation, phonon scattering, and Auger recombination present different pressure-dependent properties under compression. Responsiveness is attributed to the pressure-induced variation in the lattice structure, which also changes the electronic band structure. Specifically, simultaneous prolongation of carrier relaxation and Auger recombination is achieved in the ambient phase, which is very valuable for excess energy harvesting. Our discussion provides clues for optimizing the photovoltaic performance of OTPs.

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

NASA Astrophysics Data System (ADS)

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.

Evidences for vertical charge dipole formation in charge-trapping memories and its impact on reliability

NASA Astrophysics Data System (ADS)

Padovani, Andrea; Arreghini, Antonio; Vandelli, Luca; Larcher, Luca; bosch, Geert Van den; Houdt, Jan Van

2012-07-01

We demonstrate the formation of a vertical charge dipole in the nitride layer of TaN/Al2O3/Si3N4/SiO2/Si memories and use dedicated experiments and device simulations to investigate its dependence on program and erase conditions. We show that the polarity of the dipole depends on the program/erase operation sequence and demonstrate that it is at the origin of the charge losses observed during retention. This dipole severely affects the retention of mildly programmed and erased states, representing a serious reliability concern especially for multi-level applications.

Photoinduced ultrafast charge-order melting: Charge-order inversion and nonthermal effects

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

van Veenendaal, Michel

2016-09-01

The effect of photoexcitation is studied for a system with checkerboard charge order induced by displacements of ligands around a metal site. The motion of the ligands is treated classically and the electronic charges are simplified to two-level molecular bond charges. The calculations are done for a checkerboard charge-ordered system with about 100 000 ligand oscillators coupled to a fixed-temperature bath. The initial photoexcitation is followed by a rapid decrease in the charge-order parameter within 50–100 femtoseconds while leaving the correlation length almost unchanged. Depending on the fluence, a complete melting of the charge order occurs in less than amore » picosecond. While for low fluences, the system returns to its original state, for full melting, it recovers to its broken-symmetry state leading to an inversion of the charge order. For small long-range interactions, recovery can be slow due to domain formation.« less

Photoinduced ultrafast charge-order melting: Charge-order inversion and nonthermal effects

DOE PAGES

van Veenendaal, Michel

2016-09-01

The effect of photoexcitation is studied for a system with checkerboard charge order induced by displacements of ligands around a metal site. The motion of the ligands is treated classically and the electronic charges are simplified to two-level molecular bond charges. The calculations are done for a checkerboard charge-ordered system with about 100 000 ligand oscillators coupled to a fixed-temperature bath. The initial photoexcitation is followed by a rapid decrease in the charge-order parameter within 50–100 femtoseconds while leaving the correlation length almost unchanged. Depending on the fluence, a complete melting of the charge order occurs in less than amore » picosecond. While for low fluences, the system returns to its original state, for full melting, it recovers to its broken-symmetry state leading to an inversion of the charge order. Finally, for small long-range interactions, recovery can be slow due to domain formation.« less

Electron Transfer Dissociation: Effects of Cation Charge State on Product Partitioning in Ion/Ion Electron Transfer to Multiply Protonated Polypeptides

PubMed Central

Liu, Jian; McLuckey, Scott A.

2012-01-01

The effect of cation charge state on product partitioning in the gas-phase ion/ion electron transfer reactions of multiply protonated tryptic peptides, model peptides, and relatively large peptides with singly charged radical anions has been examined. In particular, partitioning into various competing channels, such as proton transfer (PT) versus electron transfer (ET), electron transfer with subsequent dissociation (ETD) versus electron transfer with no dissociation (ET,noD), and fragmentation of backbone bonds versus fragmentation of side chains, was measured quantitatively as a function of peptide charge state to allow insights to be drawn about the fundamental aspects of ion/ion reactions that lead to ETD. The ET channel increases relative to the PT channel, ETD increases relative to ET,noD, and fragmentation at backbone bonds increases relative to side-chain cleavages as cation charge state increases. The increase in ET versus PT with charge state is consistent with a Landau-Zener based curve-crossing model. An optimum charge state for ET is predicted by the model for the ground state-to-ground state reaction. However, when the population of excited product ion states is considered, it is possible that a decrease in ET efficiency as charge state increases will not be observed due to the possibility of the population of excited electronic states of the products. Several factors can contribute to the increase in ETD versus ET,noD and backbone cleavage versus side-chain losses. These factors include an increase in reaction exothermicity and charge state dependent differences in precursor and product ion structures, stabilities, and sites of protonation. PMID:23264749

Mirror Charge Radii and the Neutron Equation of State

NASA Astrophysics Data System (ADS)

Brown, B. Alex

2017-09-01

The differences in the charge radii of mirror nuclei are shown to be proportional to the derivative of the neutron equation of state and the symmetry energy at nuclear matter saturation density. This derivative is important for constraining the neutron equation of state for use in astrophysics. The charge radii of several neutron-rich nuclei are already measured to the accuracy of about 0.005 fm. Experiments at isotope-separator and radioactive-beam facilities are needed to measure the charge radii of the corresponding proton-rich mirror nuclei to a similar accuracy. It is also shown that neutron skins of nuclei with N =Z depend upon the value of the symmetry energy at a density of 0.10 nucleons /fm3 .

Two-leg ladder systems with dipole–dipole Fermion interactions

NASA Astrophysics Data System (ADS)

Mosadeq, Hamid; Asgari, Reza

2018-05-01

The ground-state phase diagram of a two-leg fermionic dipolar ladder with inter-site interactions is studied using density matrix renormalization group (DMRG) techniques. We use a state-of-the-art implementation of the DMRG algorithm and finite size scaling to simulate large system sizes with high accuracy. We also consider two different model systems and explore stable phases in half and quarter filling factors. We find that in the half filling, the charge and spin gaps emerge in a finite value of the dipole–dipole and on-site interactions. In the quarter filling case, s-wave superconducting state, charge density wave, homogenous insulating and phase separation phases occur depend on the interaction values. Moreover, in the dipole–dipole interaction, the D-Mott phase emerges when the hopping terms along the chain and rung are the same, whereas, this phase has been only proposed for the anisotropic Hubbard model. In the half filling case, on the other hand, there is either charge-density wave or charged Mott order phase depends on the orientation of the dipole moments of the particles with respect to the ladder geometry.

The effect of solvent relaxation time constants on free energy gap law for ultrafast charge recombination following photoinduced charge separation.

PubMed

Mikhailova, Valentina A; Malykhin, Roman E; Ivanov, Anatoly I

2018-05-16

To elucidate the regularities inherent in the kinetics of ultrafast charge recombination following photoinduced charge separation in donor-acceptor dyads in solutions, the simulations of the kinetics have been performed within the stochastic multichannel point-transition model. Increasing the solvent relaxation time scales has been shown to strongly vary the dependence of the charge recombination rate constant on the free energy gap. In slow relaxing solvents the non-equilibrium charge recombination occurring in parallel with solvent relaxation is very effective so that the charge recombination terminates at the non-equilibrium stage. This results in a crucial difference between the free energy gap laws for the ultrafast charge recombination and the thermal charge transfer. For the thermal reactions the well-known Marcus bell-shaped dependence of the rate constant on the free energy gap is realized while for the ultrafast charge recombination only a descending branch is predicted in the whole area of the free energy gap exceeding 0.2 eV. From the available experimental data on the population kinetics of the second and first excited states for a series of Zn-porphyrin-imide dyads in toluene and tetrahydrofuran solutions, an effective rate constant of the charge recombination into the first excited state has been calculated. The obtained rate constant being very high is nearly invariable in the area of the charge recombination free energy gap from 0.2 to 0.6 eV that supports the theoretical prediction.

Defect charge states in Si doped hexagonal boron-nitride monolayer

NASA Astrophysics Data System (ADS)

Mapasha, R. E.; Molepo, M. P.; Andrew, R. C.; Chetty, N.

2016-02-01

We perform ab initio density functional theory calculations to investigate the energetics, electronic and magnetic properties of isolated stoichiometric and non-stoichiometric substitutional Si complexes in a hexagonal boron-nitride monolayer. The Si impurity atoms substituting the boron atom sites SiB giving non-stoichiometric complexes are found to be the most energetically favourable, and are half-metallic and order ferromagnetically in the neutral charge state. We find that the magnetic moments and magnetization energies increase monotonically when Si defects form a cluster. Partial density of states and standard Mulliken population analysis indicate that the half-metallic character and magnetic moments mainly arise from the Si 3p impurity states. The stoichiometric Si complexes are energetically unfavorable and non-magnetic. When charging the energetically favourable non-stoichiometric Si complexes, we find that the formation energies strongly depend on the impurity charge states and Fermi level position. We also find that the magnetic moments and orderings are tunable by charge state modulation q  =  -2, -1, 0, +1, +2. The induced half-metallic character is lost (retained) when charging isolated (clustered) Si defect(s). This underlines the potential of a Si doped hexagonal boron-nitride monolayer for novel spin-based applications.

Understanding the free energy barrier and multiple timescale dynamics of charge separation in organic photovoltaic cells.

PubMed

Yan, Yaming; Song, Linze; Shi, Qiang

2018-02-28

By employing several lattice model systems, we investigate the free energy barrier and real-time dynamics of charge separation in organic photovoltaic (OPV) cells. It is found that the combined effects of the external electric field, entropy, and charge delocalization reduce the free energy barrier significantly. The dynamic disorder reduces charge carrier delocalization and results in the increased charge separation barrier, while the effect of static disorder is more complicated. Simulation of the real-time dynamics indicates that the free charge generation process involves multiple time scales, including an ultrafast component within hundreds of femtoseconds, an intermediate component related to the relaxation of the hot charge transfer (CT) state, and a slow component on the time scale of tens of picoseconds from the thermally equilibrated CT state. Effects of hot exciton dissociation as well as its dependence on the energy offset between the Frenkel exciton and the CT state are also analyzed. The current results indicate that only a small energy offset between the band gap and the lowest energy CT state is needed to achieve efficient free charge generation in OPV devices, which agrees with recent experimental findings.

Understanding the free energy barrier and multiple timescale dynamics of charge separation in organic photovoltaic cells

NASA Astrophysics Data System (ADS)

Yan, Yaming; Song, Linze; Shi, Qiang

2018-02-01

By employing several lattice model systems, we investigate the free energy barrier and real-time dynamics of charge separation in organic photovoltaic (OPV) cells. It is found that the combined effects of the external electric field, entropy, and charge delocalization reduce the free energy barrier significantly. The dynamic disorder reduces charge carrier delocalization and results in the increased charge separation barrier, while the effect of static disorder is more complicated. Simulation of the real-time dynamics indicates that the free charge generation process involves multiple time scales, including an ultrafast component within hundreds of femtoseconds, an intermediate component related to the relaxation of the hot charge transfer (CT) state, and a slow component on the time scale of tens of picoseconds from the thermally equilibrated CT state. Effects of hot exciton dissociation as well as its dependence on the energy offset between the Frenkel exciton and the CT state are also analyzed. The current results indicate that only a small energy offset between the band gap and the lowest energy CT state is needed to achieve efficient free charge generation in OPV devices, which agrees with recent experimental findings.

Single and multiple ionization of C60 fullerenes and collective effects in collisions with highly charged C, F, and Si ions with energy 3 MeV/u

NASA Astrophysics Data System (ADS)

Kelkar, A. H.; Kadhane, U.; Misra, D.; Gulyas, L.; Tribedi, L. C.

2010-10-01

We have measured absolute cross sections for single, double, triple, and quadruple ionization of C60 in collisions with 3 MeV/u C, F, and Si projectile ions at various projectile charge states. The experiment was performed using the recoil-ion time-of-flight technique. Projectile charge state dependence of the ionization yields was compared mainly with a model based on the giant dipole plasmon resonance (GDPR). In some cases, the continuum-distorted-wave-eikonal-initial-state (CDW-EIS) model which is normally applied for ion-atom collisions was also used as a reference. An excellent qualitative agreement between the experimental data for single and double ionization and the GDPR model predictions was found for all projectile charge states.

Energy gap law of electron transfer in nonpolar solvents.

PubMed

Tachiya, M; Seki, Kazuhiko

2007-09-27

We investigate the energy gap law of electron transfer in nonpolar solvents for charge separation and charge recombination reactions. In polar solvents, the reaction coordinate is given in terms of the electrostatic potentials from solvent permanent dipoles at solutes. In nonpolar solvents, the energy fluctuation due to solvent polarization is absent, but the energy of the ion pair state changes significantly with the distance between the ions as a result of the unscreened strong Coulomb potential. The electron transfer occurs when the final state energy coincides with the initial state energy. For charge separation reactions, the initial state is a neutral pair state, and its energy changes little with the distance between the reactants, whereas the final state is an ion pair state and its energy changes significantly with the mutual distance; for charge recombination reactions, vice versa. We show that the energy gap law of electron-transfer rates in nonpolar solvents significantly depends on the type of electron transfer.

Asymptotics of quasi-classical localized states in 2D system of charged hard-core bosons

NASA Astrophysics Data System (ADS)

Panov, Yu. D.; Moskvin, A. S.

2018-05-01

The continuous quasi-classical two-sublattice approximation is constructed for the 2D system of charged hard-core bosons to explore metastable inhomogeneous states analogous to inhomogeneous localized excitations in magnetic systems. The types of localized excitations are determined by asymptotic analysis and compared with numerical results. Depending on the homogeneous ground state, the excitations are the ferro and antiferro type vortices, the skyrmion-like topological excitations or linear domain walls.

Effect of trap states and microstructure on charge carrier conduction mechanism through semicrystalline poly(vinyl alcohol) granular film

NASA Astrophysics Data System (ADS)

Das, A. K.; Bhowmik, R. N.; Meikap, A. K.

2018-05-01

We report a comprehensive study on hysteresis behaviour of current-voltage characteristic and impedance spectroscopy of granular semicrystalline poly(vinyl alcohol) (PVA) film. The charge carrier conduction mechanism and charge traps of granular PVA film by measuring and analyzing the temperature dependent current-voltage characteristic indicate a bi-stable electronic state in the film. A sharp transformation of charge carrier conduction mechanism from Poole-Frenkel emission to space charge limited current mechanism has been observed. An anomalous oscillatory behaviour of current has been observed due to electric pulse effect on the molecular chain of the polymer. Effect of microstructure on charge transport mechanism has been investigated from impedance spectroscopy analysis. An equivalent circuit model has been proposed to explain the result.

Detonation propagation in annular arcs of condensed phase explosives

NASA Astrophysics Data System (ADS)

Ioannou, Eleftherios; Schoch, Stefan; Nikiforakis, Nikolaos; Michael, Louisa

2017-11-01

We present a numerical study of detonation propagation in unconfined explosive charges shaped as an annular arc (rib). Steady detonation in a straight charge propagates at constant speed, but when it enters an annular section, it goes through a transition phase and eventually reaches a new steady state of constant angular velocity. This study examines the speed of the detonation wave along the annular charge during the transition phase and at steady state, as well as its dependence on the dimensions of the annulus. The system is modeled using a recently proposed diffuse-interface formulation which allows for the representation of a two-phase explosive and of an additional inert material. The explosive considered is the polymer-bonded TATB-based LX-17 and is modeled using two Jones-Wilkins-Lee (JWL) equations of state and the ignition and growth reaction rate law. Results show that steady state speeds are in good agreement with experiment. In the transition phase, the evolution of outer detonation speed deviates from the exponential bounded growth function suggested by previous studies. We propose a new description of the transition phase which consists of two regimes. The first regime is caused by local effects at the outer edge of the annulus and leads to a dependence of the outer detonation speed on the angular position along the arc. The second regime is induced by effects originating from the inner edge of the annular charge and leads to the deceleration of the outer detonation until steady state is reached. The study concludes with a parametric study where the dependence of the steady state and the transition phase on the dimensions of the annulus is investigated.

Absolute calibration of a multichannel plate detector for low energy O, O-, and O+

NASA Astrophysics Data System (ADS)

Stephen, T. M.; Peko, B. L.

2000-03-01

Absolute detection efficiencies of a commercial multichannel plate detector have been measured for O, O+, and O-, impacting at normal incidence for energies ranging from 30-1000 eV. In addition, the detection efficiencies for O relative to its ions are presented, as they may have a more universal application. The absolute detection efficiencies are strongly energy dependent and significant differences are observed for the various charge states at lower energies. The detection efficiencies for the different charge states appear to converge at higher energies. The strongest energy dependence is for O+; the detection efficiency varies by three orders of magnitude across the energy range studied. The weakest dependence is for O-, which varies less than one order of magnitude.

Multi-charge-state molecular dynamics and self-diffusion coefficient in the warm dense matter regime

NASA Astrophysics Data System (ADS)

Fu, Yongsheng; Hou, Yong; Kang, Dongdong; Gao, Cheng; Jin, Fengtao; Yuan, Jianmin

2018-01-01

We present a multi-ion molecular dynamics (MIMD) simulation and apply it to calculating the self-diffusion coefficients of ions with different charge-states in the warm dense matter (WDM) regime. First, the method is used for the self-consistent calculation of electron structures of different charge-state ions in the ion sphere, with the ion-sphere radii being determined by the plasma density and the ion charges. The ionic fraction is then obtained by solving the Saha equation, taking account of interactions among different charge-state ions in the system, and ion-ion pair potentials are computed using the modified Gordon-Kim method in the framework of temperature-dependent density functional theory on the basis of the electron structures. Finally, MIMD is used to calculate ionic self-diffusion coefficients from the velocity correlation function according to the Green-Kubo relation. A comparison with the results of the average-atom model shows that different statistical processes will influence the ionic diffusion coefficient in the WDM regime.

Intramolecular Charge Transfer States in the Condensed Phase

NASA Astrophysics Data System (ADS)

Williams, C. F.; Herbert, J. M.

2009-06-01

Time-Dependent Density Functional Theory (TDDFT) with long range corrected functionals can give accurate results for the energies of electronically excited states involving Intramolecular Charge Transfer (ICT) in large molecules. If this is combined with a Molecular Mechanics (MM) representation of the surrounding solvent this technique can be used to interpret the results of condensed phase UV-Vis Spectroscopy. Often the MM region is represented by a set of point charges, however this means that the solvent cannot repolarize to adapt to the new charge distribution as a result of ICT and so the excitation energies to ICT states are overestimated. To solve this problem an algorithm that interfaces TDDFT with the polarizable force-field AMOEBA is presented; the effect of solvation on charge transfer in species such as 4,4'dimethylaminobenzonitrile (DMABN) is discussed. M.A. Rohrdanz, K.M. Martins, and J.M. Herbert, J. Chem. Phys. 130 034107 (2008).

Gap state charge induced spin-dependent negative differential resistance in tunnel junctions

NASA Astrophysics Data System (ADS)

Jiang, Jun; Zhang, X.-G.; Han, X. F.

2016-04-01

We propose and demonstrate through first-principles calculation a new spin-dependent negative differential resistance (NDR) mechanism in magnetic tunnel junctions (MTJ) with cubic cation disordered crystals (CCDC) AlO x or Mg1-x Al x O as barrier materials. The CCDC is a class of insulators whose band gap can be changed by cation doping. The gap becomes arched in an ultrathin layer due to the space charge formed from metal-induced gap states. With an appropriate combination of an arched gap and a bias voltage, NDR can be produced in either spin channel. This mechanism is applicable to 2D and 3D ultrathin junctions with a sufficiently small band gap that forms a large space charge. It provides a new way of controlling the spin-dependent transport in spintronic devices by an electric field. A generalized Simmons formula for tunneling current through junction with an arched gap is derived to show the general conditions under which ultrathin junctions may exhibit NDR.

Time-resolved electric force microscopy of charge trapping in polycrystalline pentacene.

PubMed

Jaquith, Michael; Muller, Erik M; Marohn, John A

2007-07-12

Here we introduce time-resolved electric force microscopy measurements to directly and locally probe the kinetics of charge trap formation in a polycrystalline pentacene thin-film transistor. We find that the trapping rate depends strongly on the initial concentration of free holes and that trapped charge is highly localized. The observed dependence of trapping rate on the hole chemical potential suggests that the trapping process should not be viewed as a filling of midgap energy levels, but instead as a process in which the very creation of trapped states requires the presence of free holes.

The impact of hot charge carrier mobility on photocurrent losses in polymer-based solar cells

PubMed Central

Philippa, Bronson; Stolterfoht, Martin; Burn, Paul L.; Juška, Gytis; Meredith, Paul; White, Ronald D.; Pivrikas, Almantas

2014-01-01

A typical signature of charge extraction in disordered organic systems is dispersive transport, which implies a distribution of charge carrier mobilities that negatively impact on device performance. Dispersive transport has been commonly understood to originate from a time-dependent mobility of hot charge carriers that reduces as excess energy is lost during relaxation in the density of states. In contrast, we show via photon energy, electric field and film thickness independence of carrier mobilities that the dispersive photocurrent in organic solar cells originates not from the loss of excess energy during hot carrier thermalization, but rather from the loss of carrier density to trap states during transport. Our results emphasize that further efforts should be directed to minimizing the density of trap states, rather than controlling energetic relaxation of hot carriers within the density of states. PMID:25047086

Single and multiple ionization of C{sub 60} fullerenes and collective effects in collisions with highly charged C, F, and Si ions with energy 3 MeV/u

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

Kelkar, A. H.; Kadhane, U.; Misra, D.

2010-10-15

We have measured absolute cross sections for single, double, triple, and quadruple ionization of C{sub 60} in collisions with 3 MeV/u C, F, and Si projectile ions at various projectile charge states. The experiment was performed using the recoil-ion time-of-flight technique. Projectile charge state dependence of the ionization yields was compared mainly with a model based on the giant dipole plasmon resonance (GDPR). In some cases, the continuum-distorted-wave-eikonal-initial-state (CDW-EIS) model which is normally applied for ion-atom collisions was also used as a reference. An excellent qualitative agreement between the experimental data for single and double ionization and the GDPR modelmore » predictions was found for all projectile charge states.« less

Simultaneous specimen current and time-dependent cathodoluminescence measurements on gallium nitride

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

Campo, E. M., E-mail: e.campo@bangor.ac.uk; Hopkins, L.; Pophristic, M.

2016-06-28

Time-dependent cathodoluminescence (CL) and specimen current (SC) are monitored to evaluate trapping behavior and evolution of charge storage. Examination of CL and SC suggests that the near band edge emission in GaN is reduced primarily by the activation of traps upon irradiation, and Gallium vacancies are prime candidates. At the steady state, measurement of the stored charge by empiric-analytical methods suggests that all available traps within the interaction volume have been filled, and that additional charge is being stored interstitially, necessarily beyond the interaction volume. Once established, the space charge region is responsible for the steady state CL emission and,more » prior to build up, it is responsible for the generation of diffusion currents. Since the non-recombination effects resulting from diffusion currents that develop early on are analogous to those leading to device failure upon aging, this study is fundamental toward a holistic insight into optical properties in GaN.« less

Quantum mechanical/molecular mechanical/continuum style solvation model: time-dependent density functional theory.

PubMed

Thellamurege, Nandun M; Cui, Fengchao; Li, Hui

2013-08-28

A combined quantum mechanical/molecular mechanical/continuum (QM/MMpol/C) style method is developed for time-dependent density functional theory (TDDFT, including long-range corrected TDDFT) method, induced dipole polarizable force field, and induced surface charge continuum model. Induced dipoles and induced charges are included in the TDDFT equations to solve for the transition energies, relaxed density, and transition density. Analytic gradient is derived and implemented for geometry optimization and molecular dynamics simulation. QM/MMpol/C style DFT and TDDFT methods are used to study the hydrogen bonding of the photoactive yellow protein chromopore in ground state and excited state.

Cycle of charge carrier states with formation and extinction of a floating gate in an ambipolar tetracyanoquaterthienoquinoid-based field-effect transistor

NASA Astrophysics Data System (ADS)

Itoh, Takuro; Toyota, Taro; Higuchi, Hiroyuki; Matsushita, Michio M.; Suzuki, Kentaro; Sugawara, Tadashi

2017-03-01

A tetracyanoquaterthienoquinoid (TCT4Q)-based field effect transistor is characterized by the ambipolar transfer characteristics and the facile shift of the threshold voltage induced by the bias stress. The trapping and detrapping kinetics of charge carriers was investigated in detail by the temperature dependence of the decay of source-drain current (ISD). We found a repeatable formation of a molecular floating gate is derived from a 'charge carrier-and-gate' cycle comprising four stages, trapping of mobile carriers, formation of a floating gate, induction of oppositely charged mobile carriers, and recombination between mobile and trapped carriers to restore the initial state.

Investigation of ground state charge transfer complex between paracetamol and p-chloranil through DFT and UV-visible studies

NASA Astrophysics Data System (ADS)

Shukla, Madhulata; Srivastava, Nitin; Saha, Satyen

2012-08-01

The present report deals with the theoretical investigation on ground state structure and charge transfer (CT) transitions in paracetamol (PA)/p-chloranil (CA) complex using Density Functional Theory (DFT) and Time Dependent Density Functional Theory (TD-DFT) method. It is found that Cdbnd O bond length of p-chloranil increases on complexation with paracetamol along with considerable amount of charge transfer from PA to CA. TD-DFT calculations have been performed to analyse the observed UV-visible spectrum of PA-CA charge transferred complex. Interestingly, in addition to expected CT transition, a weak symmetry relieved π-π* transition in the chloranil is also observed.

Quantum State Transmission in a Superconducting Charge Qubit-Atom Hybrid

PubMed Central

Yu, Deshui; Valado, María Martínez; Hufnagel, Christoph; Kwek, Leong Chuan; Amico, Luigi; Dumke, Rainer

2016-01-01

Hybrids consisting of macroscopic superconducting circuits and microscopic components, such as atoms and spins, have the potential of transmitting an arbitrary state between different quantum species, leading to the prospective of high-speed operation and long-time storage of quantum information. Here we propose a novel hybrid structure, where a neutral-atom qubit directly interfaces with a superconducting charge qubit, to implement the qubit-state transmission. The highly-excited Rydberg atom located inside the gate capacitor strongly affects the behavior of Cooper pairs in the box while the atom in the ground state hardly interferes with the superconducting device. In addition, the DC Stark shift of the atomic states significantly depends on the charge-qubit states. By means of the standard spectroscopic techniques and sweeping the gate voltage bias, we show how to transfer an arbitrary quantum state from the superconducting device to the atom and vice versa. PMID:27922087

Estimation of ion charge states using Van Allen Probes-RBSPICE: a case study

NASA Astrophysics Data System (ADS)

Farinas Perez, G.; Sibeck, D. G.

2017-12-01

We use data from the RBSPICE instrument aboard the Van Allen Probes spacecraft to identify particle injection events with ion drift echoes. We calculate the arrival time and drift period of the protons, helium and oxygen for every energy channel of the RBSPICE instrument. The ions drift period depends upon their energy and charge, as we know the particle energy and the time drift period, the charge state can be estimated for a dipolar magnetic field model. A drift-echo event occurred in May 23, 2013 at 0400 UT is analyzed.

Fuzzy control of battery chargers

NASA Astrophysics Data System (ADS)

Aldridge, Jack

1996-03-01

The increasing reliance on battery power for portable terrestrial purposes, such as portable tools, portable computers, and telecommunications, provides motivation to optimize the battery charging process with respect to speed of charging and charging cycle lifetime of the battery. Fuzzy control, implemented on a small microcomputer, optimizes charging in the presence of nonlinear effects and large uncertainty in the voltage vs. charge state characteristics for the battery. Use of a small microcontroller makes possible a small, capable, and affordable package for the charger. Microcontroller-based chargers provide improved performance by adjusting both charging voltage and charging current during the entire charging process depending on a current estimate of the state of charge of the battery. The estimate is derived from the zero-current voltage of the battery and the temperature and their rates of change. All of these quantities are uncertain due to the variation in condition between the individual cells in a battery, the rapid and nonlinear dependence of the fundamental electrochemistry on the internal temperature, and the placement of a single temperature sensor within the battery package. While monitoring the individual cell voltages and temperatures would be desirable, cost and complexity considerations preclude the practice. NASA has developed considerable technology in batteries for supplying significant amounts of power for spacecraft and in fuzzy control techniques for the space applications. In this paper, we describe how we are using both technologies to build an optimal charger prototype as a precursor to a commercial version.

TDDFT study of twisted intramolecular charge transfer and intermolecular double proton transfer in the excited state of 4‧-dimethylaminoflavonol in ethanol solvent

NASA Astrophysics Data System (ADS)

Wang, Ye; Shi, Ying; Cong, Lin; Li, Hui

2015-02-01

Time-dependent density functional theory method at the def-TZVP/B3LYP level was employed to investigate the intramolecular and intermolecular hydrogen bonding dynamics in the first excited (S1) state of 4‧-dimethylaminoflavonol (DMAF) monomer and in ethanol solution. In the DMAF monomer, we demonstrated that the intramolecular charge transfer (ICT) takes place in the S1 state. This excited state ICT process was followed by intramolecular proton transfer. Our calculated results are in good agreement with the mechanism proposed in experimental work. For the hydrogen-bonded DMAF-EtOH complex, it was demonstrated that the intermolecular hydrogen bonds can induce the formation of the twisted intramolecular charge transfer (TICT) state and the conformational twisting is along the C3-C4 bond. Moreover, the intermolecular hydrogen bonds can also facilitate the intermolecular double proton transfer in the TICT state. A stepwise intermolecular double proton transfer process was revealed. Therefore, the intermolecular hydrogen bonds can alter the mechanism of intramolecular charge transfer and proton transfer in the excited state for the DMAF molecule.

Specimen charging in X-ray absorption spectroscopy: correction of total electron yield data from stabilized zirconia in the energy range 250-915 eV.

PubMed

Vlachos, Dimitrios; Craven, Alan J; McComb, David W

2005-03-01

The effects of specimen charging on X-ray absorption spectroscopy using total electron yield have been investigated using powder samples of zirconia stabilized by a range of oxides. The stabilized zirconia powder was mixed with graphite to minimize the charging but significant modifications of the intensities of features in the X-ray absorption near-edge fine structure (XANES) still occurred. The time dependence of the charging was measured experimentally using a time scan, and an algorithm was developed to use this measured time dependence to correct the effects of the charging. The algorithm assumes that the system approaches the equilibrium state by an exponential decay. The corrected XANES show improved agreement with the electron energy-loss near-edge fine structure obtained from the same samples.

State of Charge estimation of lithium ion battery based on extended Kalman filtering algorithm

NASA Astrophysics Data System (ADS)

Yang, Fan; Feng, Yiming; Pan, Binbiao; Wan, Renzhuo; Wang, Jun

2017-08-01

Accurate estimation of state-of-charge (SOC) for lithium ion battery is crucial for real-time diagnosis and prognosis in green energy vehicles. In this paper, a state space model of the battery based on Thevenin model is adopted. The strategy of estimating state of charge (SOC) based on extended Kalman fil-ter is presented, as well as to combine with ampere-hour counting (AH) and open circuit voltage (OCV) methods. The comparison between simulation and experiments indicates that the model’s performance matches well with that of lithium ion battery. The algorithm of extended Kalman filter keeps a good accura-cy precision and less dependent on its initial value in full range of SOC, which is proved to be suitable for online SOC estimation.

Laser ion source activities at Brookhaven National Laboratory

DOE PAGES

Kanesue, Takeshi; Okamura, Masahiro

2015-07-31

In Brookhaven National Laboratory (BNL), we have been developing laser ion sources for diverse accelerators. Tabletop Nd:YAG lasers with up to several Joules of energy are mainly used to create ablation plasmas for stable operations. The obtained charge states depend on laser power density and target species. Two types of ion extraction schemes, Direct Plasma Injection Scheme (DPIS) and conventional static extraction, are used depending on application. We optimized and select a suitable laser irradiation condition and a beam extraction scheme to meet the requirement of the following accelerator system. We have demonstrated to accelerate more than 5 x 10more » 10 of C 6+ ions using the DPIS. We successfully commissioned low charge ion beam provider to the user facilities in BNL. As a result, to achieve higher current, higher charge state and lower emittance, further studies will continue.« less

Extremely large nonsaturating magnetoresistance and ultrahigh mobility due to topological surface states in the metallic Bi2Te3 topological insulator

NASA Astrophysics Data System (ADS)

Shrestha, K.; Chou, M.; Graf, D.; Yang, H. D.; Lorenz, B.; Chu, C. W.

2017-05-01

Weak antilocalization (WAL) effects in Bi2Te3 single crystals have been investigated at high and low bulk charge-carrier concentrations. At low charge-carrier density the WAL curves scale with the normal component of the magnetic field, demonstrating the dominance of topological surface states in magnetoconductivity. At high charge-carrier density the WAL curves scale with neither the applied field nor its normal component, implying a mixture of bulk and surface conduction. WAL due to topological surface states shows no dependence on the nature (electrons or holes) of the bulk charge carriers. The observations of an extremely large nonsaturating magnetoresistance and ultrahigh mobility in the samples with lower carrier density further support the presence of surface states. The physical parameters characterizing the WAL effects are calculated using the Hikami-Larkin-Nagaoka formula. At high charge-carrier concentrations, there is a greater number of conduction channels and a decrease in the phase coherence length compared to low charge-carrier concentrations. The extremely large magnetoresistance and high mobility of topological insulators have great technological value and can be exploited in magnetoelectric sensors and memory devices.

Elucidation of the role of metal-to-ring charge-transfer excited states in the deactivation of photoexcited ruthenium porphyrin carbonyl complexes

NASA Astrophysics Data System (ADS)

Rodriguez, Juan; McDowell, Lynda; Holten, Dewey

1988-06-01

Deactivation of the lowest excited triplet state, 3(π, π*), of the Ru(II) porphyrins RuP(CO)(L) is more strongly dependent on temperature than decay of 3(π, π*) in Pt(II)P and H 2P (metal-free) complexes containing the same macrocycle P. This and other observations support the proposal that 3(π, π*) in the RuP(CO)(L) complexes decays in part via a metal-to-ring (d, π*) charge-transfer excited state at higher energy.

Pseudo-direct bandgap transitions in silicon nanocrystals: effects on optoelectronics and thermoelectrics

NASA Astrophysics Data System (ADS)

Singh, Vivek; Yu, Yixuan; Sun, Qi-C.; Korgel, Brian; Nagpal, Prashant

2014-11-01

While silicon nanostructures are extensively used in electronics, the indirect bandgap of silicon poses challenges for optoelectronic applications like photovoltaics and light emitting diodes (LEDs). Here, we show that size-dependent pseudo-direct bandgap transitions in silicon nanocrystals dominate the interactions between (photoexcited) charge carriers and phonons, and hence the optoelectronic properties of silicon nanocrystals. Direct measurements of the electronic density of states (DOS) for different sized silicon nanocrystals reveal that these pseudo-direct transitions, likely arising from the nanocrystal surface, can couple with the quantum-confined silicon states. Moreover, we demonstrate that since these transitions determine the interactions of charge carriers with phonons, they change the light emission, absorption, charge carrier diffusion and phonon drag (Seebeck coefficient) in nanoscaled silicon semiconductors. Therefore, these results can have important implications for the design of optoelectronics and thermoelectric devices based on nanostructured silicon.While silicon nanostructures are extensively used in electronics, the indirect bandgap of silicon poses challenges for optoelectronic applications like photovoltaics and light emitting diodes (LEDs). Here, we show that size-dependent pseudo-direct bandgap transitions in silicon nanocrystals dominate the interactions between (photoexcited) charge carriers and phonons, and hence the optoelectronic properties of silicon nanocrystals. Direct measurements of the electronic density of states (DOS) for different sized silicon nanocrystals reveal that these pseudo-direct transitions, likely arising from the nanocrystal surface, can couple with the quantum-confined silicon states. Moreover, we demonstrate that since these transitions determine the interactions of charge carriers with phonons, they change the light emission, absorption, charge carrier diffusion and phonon drag (Seebeck coefficient) in nanoscaled silicon semiconductors. Therefore, these results can have important implications for the design of optoelectronics and thermoelectric devices based on nanostructured silicon. Electronic supplementary information (ESI) available. See DOI: 10.1039/c4nr04688a

Impact of Various Charge States of Hydrogen on Passivation of Dislocation in Silicon

NASA Astrophysics Data System (ADS)

Song, Lihui; Lou, Jingjing; Fu, Jiayi; Ji, Zhenguo

2018-03-01

Dislocation, one of typical crystallographic defects in silicon, is detrimental to the minority carrier lifetime of silicon wafer. Hydrogen passivation is able to reduce the recombination activity of dislocation, however, the passivation efficacy is strongly dependent on the experimental conditions. In this paper, a model based on the theory of hydrogen charge state control is proposed to explain the passivation efficacy of dislocation correlated to the peak temperature of thermal annealing and illumination intensity. Experimental results support the prediction of the model that a mix of positively charged hydrogen and negatively charged hydrogen at certain ratio can maximise the passivation efficacy of dislocation, leading to a better power conversion efficiency of silicon solar cell with dislocation in it.

A unitary convolution approximation for the impact-parameter dependent electronic energy loss

NASA Astrophysics Data System (ADS)

Schiwietz, G.; Grande, P. L.

1999-06-01

In this work, we propose a simple method to calculate the impact-parameter dependence of the electronic energy loss of bare ions for all impact parameters. This perturbative convolution approximation (PCA) is based on first-order perturbation theory, and thus, it is only valid for fast particles with low projectile charges. Using Bloch's stopping-power result and a simple scaling, we get rid of the restriction to low charge states and derive the unitary convolution approximation (UCA). Results of the UCA are then compared with full quantum-mechanical coupled-channel calculations for the impact-parameter dependent electronic energy loss.

dc Resistivity of Quantum Critical, Charge Density Wave States from Gauge-Gravity Duality

NASA Astrophysics Data System (ADS)

Amoretti, Andrea; Areán, Daniel; Goutéraux, Blaise; Musso, Daniele

2018-04-01

In contrast to metals with weak disorder, the resistivity of weakly pinned charge density waves (CDWs) is not controlled by irrelevant processes relaxing momentum. Instead, the leading contribution is governed by incoherent, diffusive processes which do not drag momentum and can be evaluated in the clean limit. We compute analytically the dc resistivity for a family of holographic charge density wave quantum critical phases and discuss its temperature scaling. Depending on the critical exponents, the ground state can be conducting or insulating. We connect our results to dc electrical transport in underdoped cuprate high Tc superconductors. We conclude by speculating on the possible relevance of unstable, semilocally critical CDW states to the strange metallic region.

dc Resistivity of Quantum Critical, Charge Density Wave States from Gauge-Gravity Duality.

PubMed

Amoretti, Andrea; Areán, Daniel; Goutéraux, Blaise; Musso, Daniele

2018-04-27

In contrast to metals with weak disorder, the resistivity of weakly pinned charge density waves (CDWs) is not controlled by irrelevant processes relaxing momentum. Instead, the leading contribution is governed by incoherent, diffusive processes which do not drag momentum and can be evaluated in the clean limit. We compute analytically the dc resistivity for a family of holographic charge density wave quantum critical phases and discuss its temperature scaling. Depending on the critical exponents, the ground state can be conducting or insulating. We connect our results to dc electrical transport in underdoped cuprate high T_{c} superconductors. We conclude by speculating on the possible relevance of unstable, semilocally critical CDW states to the strange metallic region.

Ultrafast investigation of photoinduced charge transfer in aminoanthraquinone pharmaceutical product

NASA Astrophysics Data System (ADS)

Zhang, Song; Sun, Simei; Zhou, Miaomiao; Wang, Lian; Zhang, Bing

2017-02-01

We investigated the mechanism of intramolecular charge transfer and the following radiationless dynamics of the excited states of 1-aminoanthraquinone using steady state and time-resolved absorption spectroscopy combined with quantum chemical calculations. Following photoexcitation with 460 nm, conformational relaxation via twisting of the amino group, charge transfer and the intersystem crossing (ISC) processes have been established to be the major relaxation pathways responsible for the ultrafast nonradiative of the excited S1 state. Intramolecular proton transfer, which could be induced by intramolecular hydrogen bonding is inspected and excluded. Time-dependent density functional theory (TDDFT) calculations reveal the change of the dipole moments of the S0 and S1 states along the twisted coordinate of the amino group, indicating the mechanism of twisted intra-molecular charge transfer (TICT). The timescale of TICT is measured to be 5 ps due to the conformational relaxation and a barrier on the S1 potential surface. The ISC from the S1 state to the triplet manifold is a main deactivation pathway with the decay time of 28 ps. Our results observed here have yield a physically intuitive and complete picture of the photoinduced charge transfer and radiationless dynamics in anthraquinone pharmaceutial products.

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

Ohmura, Satoshi; Nagaya, Kiyonobu; Yao, Makoto

The dynamic properties of liquid B{sub 2}O{sub 3} under pressure and highly-charged bromophenol molecule are studied by using molecular dynamics (MD) simulations based on density functional theory (DFT). Diffusion properties of covalent liquids under high pressure are very interesting in the sense that they show unexpected pressure dependence. It is found from our simulation that the magnitude relation of diffusion coefficients for boron and oxygen in liquid B{sub 2}O{sub 3} shows the anomalous pressure dependence. The simulation clarified the microscopic origin of the anomalous diffusion properties. Our simulation also reveals the dissociation mechanism in the coulomb explosion of the highly-chargedmore » bromophenol molecule. When the charge state n is 6, hydrogen atom in the hydroxyl group dissociates at times shorter than 20 fs while all hydrogen atoms dissociate when n is 8. After the hydrogen dissociation, the carbon ring breaks at about 100 fs. There is also a difference on the mechanism of the ring breaking depending on charge states, in which the ring breaks with expanding (n = 6) or shrink (n = 8)« less

Mapping of Residues Forming the Voltage Sensor of the Voltage-Dependent Anion-Selective Channel

NASA Astrophysics Data System (ADS)

Thomas, Lorie; Blachly-Dyson, Elizabeth; Colombini, Marco; Forte, Michael

1993-06-01

Voltage-gated ion-channel proteins contain "voltage-sensing" domains that drive the conformational transitions between open and closed states in response to changes in transmembrane voltage. We have used site-directed mutagenesis to identify residues affecting the voltage sensitivity of a mitochondrial channel, the voltage-dependent anion-selective channel (VDAC). Although charge changes at many sites had no effect, at other sites substitutions that increased positive charge also increased the steepness of voltage dependance and substitutions that decreased positive charge decreased voltage dependance by an appropriate amount. In contrast to the plasma membrane K^+ and Na^+ channels, these residues are distributed over large parts of the VDAC protein. These results have been used to define the conformational transitions that accompany voltage gating of an ion channel. This gating mechanism requires the movement of large portions of the VDAC protein through the membrane.

Transition from direct to inverted charge transport Marcus regions in molecular junctions via molecular orbital gating

NASA Astrophysics Data System (ADS)

Yuan, Li; Wang, Lejia; Garrigues, Alvar R.; Jiang, Li; Annadata, Harshini Venkata; Anguera Antonana, Marta; Barco, Enrique; Nijhuis, Christian A.

2018-04-01

Solid-state molecular tunnel junctions are often assumed to operate in the Landauer regime, which describes essentially activationless coherent tunnelling processes. In solution, on the other hand, charge transfer is described by Marcus theory, which accounts for thermally activated processes. In practice, however, thermally activated transport phenomena are frequently observed also in solid-state molecular junctions but remain poorly understood. Here, we show experimentally the transition from the Marcus to the inverted Marcus region in a solid-state molecular tunnel junction by means of intra-molecular orbital gating that can be tuned via the chemical structure of the molecule and applied bias. In the inverted Marcus region, charge transport is incoherent, yet virtually independent of temperature. Our experimental results fit well to a theoretical model that combines Landauer and Marcus theories and may have implications for the interpretation of temperature-dependent charge transport measurements in molecular junctions.

Coexistence of charge order and antiferromagnetism in (TMTTF)2SbF6: NMR study

NASA Astrophysics Data System (ADS)

Nomura, K.; Yamamoto, M.; Matsunaga, N.; Hirose, S.; Shimohara, N.; Satoh, T.; Isome, T.; Liu, Y.; Kawamoto, A.

2015-03-01

The electronic state of (TMTTF)2SbF6 was investigated by the 1H and 13C NMR measurements. The temperature dependence of T1-1 in 1H NMR shows a sharp peak associated with the antiferromagnetic transition at TAF=6 K. The temperature dependence of T1-1 is described by the power law T2.4 below TAF. This suggests the nodal gapless spin wave excitation in antiferromagnetic phase. In 13C NMR, two sharp peaks at high temperature region, associated with the inner and the outer carbon sites in TMTTF dimer, split into four peaks below 150 K. It indicates that the charge disproportionation occurs. The degree of charge disproportionation Δρ is estimated as (0.25±0.09)e from the chemical shift difference. This value of Δρ is consistent with that obtained from the infrared spectroscopy. In the antiferromagnetic state (AFI), the observed line shape is well fitted by eight Lorentzian peaks. This suggests that the charge order with the same degree still remains in the AF state. From the line assignment, the AF staggered spin amplitude is obtained as 0.70 μB and 0.24 μB at the charge rich and the poor sites, respectively. These values corresponding to almost 1 μB per dimer are quite different from 0.11 μB of another AF (AFII) state in (TMTTF)2Br with effective higher pressure. As a result, it is understood that the antiferromagnetic staggered spin order is stabilized on the CO state in the AFI phase of (TMTTF)2SbF6.

Effect of Single-Electron Interface Trapping in Decanano MOSFETs: A 3D Atomistic Simulation Study

NASA Technical Reports Server (NTRS)

Asenov, Asen; Balasubramaniam, R.; Brown, A. R.; Davies, J. H.

2000-01-01

We study the effect of trapping/detrapping of a single-electron in interface states in the channel of n-type MOSFETs with decanano dimensions using 3D atomistic simulation techniques. In order to highlight the basic dependencies, the simulations are carried out initially assuming continuous doping charge, and discrete localized charge only for the trapped electron. The dependence of the random telegraph signal (RTS) amplitudes on the device dimensions and on the position of the trapped charge in the channel are studied in detail. Later, in full-scale, atomistic simulations assuming discrete charge for both randomly placed dopants and the trapped electron, we highlight the importance of current percolation and of traps with strategic position where the trapped electron blocks a dominant current path.

Charge-state distribution of Li ions from the β decay of laser-trapped 6He atoms

NASA Astrophysics Data System (ADS)

Hong, R.; Leredde, A.; Bagdasarova, Y.; Fléchard, X.; García, A.; Knecht, A.; Müller, P.; Naviliat-Cuncic, O.; Pedersen, J.; Smith, E.; Sternberg, M.; Storm, D. Â. W.; Swanson, H. Â. E.; Wauters, F.; Zumwalt, D.

2017-11-01

The accurate determination of atomic final states following nuclear β decay plays an important role in several experiments. In particular, the charge state distributions of ions following nuclear β decay are important for determinations of the β -ν angular correlation with improved precision. Beyond the hydrogenic cases, the decay of neutral 6He presents the simplest case. Our measurement aims at providing benchmarks to test theoretical calculations. The kinematics of Lin + ions produced following the β decay of 6He within an electric field were measured using 6He atoms in the metastable (1 s 2 s ,S31) and (1 s 2 p ,P32) states confined by a magneto-optical trap. The electron shakeoff probabilities were deduced, including their dependence on ion energy. We find significant discrepancies on the fractions of Li ions in the different charge states with respect to a recent calculation.

Quark charge retention in final state hadrons from deep inelastic muon scattering

NASA Astrophysics Data System (ADS)

Albanese, J. P.; Arneodo, M.; Arvidson, A.; Aubert, J. J.; Becks, K. H.; Bee, C.; Benchouk, C.; Bird, I.; Blum, D.; Böhm, E.; de Bouard, X.; Brasse, F. W.; Braun, H.; Broll, C.; Brown, S.; Brück, H.; Calen, H.; Callebaut, D.; Carr, J.; Chima, J. S.; Clifft, R.; Cobb, J. H.; Coignet, G.; Combley, F.; Coughlan, J.; Court, G. R.; D'Agostini, G.; Dahlgren, S.; Davies, J. K.; Dau, W. D.; Dengler, F.; Derado, I.; Dobinson, R. W.; Dosselli, U.; Dreyer, T.; Drees, J.; Dumont, J. J.; Düren, M.; Eckardt, V.; Edwards, A.; Edwards, M.; Ernst, T.; Eszes, G.; Favier, J.; Ferrero, M. I.; Figiel, J.; Flauger, W.; Foster, J.; Gabathuler, E.; Gamet, R.; Gayler, J.; Geddes, N.; Giubellino, P.; Gössling, C.; Grafström, P.; Grard, F.; Gustafsson, L.; Haas, J.; Hagberg, E.; Hasert, F. J.; Hayman, P.; Heusse, P.; Hoppe, C.; Jaffré, M.; Jachołkowska, A.; Janata, F.; Jancso, G.; Johnson, A. S.; Kabuss, E. M.; Kellner, G.; Korbel, V.; Krüger, J.; Kullander, S.; Landgraf, U.; Lanske, D.; Loken, J.; Long, K.; Maire, M.; Manz, A.; Mohr, W.; Montanet, F.; Montgomery, H. E.; Mount, R. P.; Nagy, E.; Nassalski, J.; Norton, P. R.; Oakham, F. G.; Osborne, A. M.; Pascaud, C.; Paul, L.; Payre, P.; Peroni, C.; Pessard, H.; Pettingale, J.; Pönsgen, B.; Pötsch, M.; Preissner, H.; Renton, P.; Ribarics, P.; Rith, K.; Rondio, E.; Schlagböhmer, A.; Schmitz, N.; Schneegans, M.; Schröder, T.; Schultze, K.; Shiers, J.; Sloan, T.; Stier, H. E.; Stockhausen, W.; Studt, M.; Taylor, G.; Thénard, J. M.; Thompson, J. C.; de la Torre, A.; Toth, J.; Urban, L.; Wahlen, H.; Wallucks, W.; Whalley, M.; Williams, W. S. C.; Wheeler, S.; Wimpenny, S.; Windmolders, R.; Wolf, G.; Zank, P.; European Muon Collaboration

1984-08-01

The net charge of final state hadrons in both the current and target fragmentation regions has been measured in 280 GeV/ c muon-proton scattering experiment. A clean kinematic separation of the two regions in the centre-of-mass rapidity is demonstrated. The dependence on xBj of the mean net charges is found to be consistent with a large contribution of sea quarks at small xBj and with the dominance of valence quarks at large xBj thus giving clear confirmation of the quarck- parton model. It is also shown that the lending forward hadron has a high probability of containing the struck quark.

Electro-thermal battery model identification for automotive applications

NASA Astrophysics Data System (ADS)

Hu, Y.; Yurkovich, S.; Guezennec, Y.; Yurkovich, B. J.

This paper describes a model identification procedure for identifying an electro-thermal model of lithium ion batteries used in automotive applications. The dynamic model structure adopted is based on an equivalent circuit model whose parameters are scheduled on the state-of-charge, temperature, and current direction. Linear spline functions are used as the functional form for the parametric dependence. The model identified in this way is valid inside a large range of temperatures and state-of-charge, so that the resulting model can be used for automotive applications such as on-board estimation of the state-of-charge and state-of-health. The model coefficients are identified using a multiple step genetic algorithm based optimization procedure designed for large scale optimization problems. The validity of the procedure is demonstrated experimentally for an A123 lithium ion iron-phosphate battery.

Optical properties and electronic energy relaxation of metallic Au144(SR)60 nanoclusters.

PubMed

Yi, Chongyue; Tofanelli, Marcus A; Ackerson, Christopher J; Knappenberger, Kenneth L

2013-12-04

Electronic energy relaxation of Au144(SR)60(q) ligand-protected nanoclusters, where SR = SC6H13 and q = -1, 0, +1, and +2, was examined using femtosecond time-resolved transient absorption spectroscopy. The observed differential transient spectra contained three distinct components: (1) transient bleaches at 525 and 600 nm, (2) broad visible excited-state absorption (ESA), and (3) stimulated emission (SE) at 670 nm. The bleach recovery kinetics depended upon the excitation pulse energy and were thus attributed to electron-phonon coupling typical of metallic nanostructures. The prominent bleach at 525 nm was assigned to a core-localized plasmon resonance (CLPR). ESA decay kinetics were oxidation-state dependent and could be described using a metal-sphere charging model. The dynamics, emission energy, and intensity of the SE peak exhibited dielectric-dependent responses indicative of Superatom charge transfer states. On the basis of these data, the Au144(SR)60 system is the smallest-known nanocluster to exhibit quantifiable electron dynamics and optical properties characteristic of metals.

Testing time-dependent density functional theory with depopulated molecular orbitals for predicting electronic excitation energies of valence, Rydberg, and charge-transfer states and potential energies near a conical intersection

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

Li, Shaohong L.; Truhlar, Donald G., E-mail: truhlar@umn.edu

2014-09-14

Kohn-Sham (KS) time-dependent density functional theory (TDDFT) with most exchange-correlation functionals is well known to systematically underestimate the excitation energies of Rydberg and charge-transfer excited states of atomic and molecular systems. To improve the description of Rydberg states within the KS TDDFT framework, Gaiduk et al. [Phys. Rev. Lett. 108, 253005 (2012)] proposed a scheme that may be called HOMO depopulation. In this study, we tested this scheme on an extensive dataset of valence and Rydberg excitation energies of various atoms, ions, and molecules. It is also tested on a charge-transfer excitation of NH{sub 3}-F{sub 2} and on the potentialmore » energy curves of NH{sub 3} near a conical intersection. We found that the method can indeed significantly improve the accuracy of predicted Rydberg excitation energies while preserving reasonable accuracy for valence excitation energies. However, it does not appear to improve the description of charge-transfer excitations that are severely underestimated by standard KS TDDFT with conventional exchange-correlation functionals, nor does it perform appreciably better than standard TDDFT for the calculation of potential energy surfaces.« less

Electrodynamics in cylindrical symmetry in the magnetic plasma state

NASA Astrophysics Data System (ADS)

López-Bara, F. I.; López-Aguilar, F.

2018-05-01

Excited states in magnetic structures of the so-called spin-ices and in some artificial magnetic materials present a behaviour as being a magnetic neutral plasma. In this state the electromagnetic waves in confined systems (waveguides) filled with materials with magnetic charges are able to transmit information and energy. In the natural spin-ices, the difficulty is the very low temperature for which these magnetic entities appear, whose phenomenology under the electromagnetic interaction is that of solids containing magnetic charges. However, similar behaviour may be present in other compounds at higher temperatures, even at room temperature and they are named artificial spin-ice compounds. This analysis is addressed to obtain theoretical results about magnetic responses and frequency-dependent magnetricity. The key physical magnitudes are the plasmon frequency () which is related to the cut-off frequency in a wave guide and the effective inertial masses () of these magnetic charges. All properties of the electromagnetic propagation in these compounds with effective magnetic monopoles depend on and m. This is carried out including the dissipative forces among magnetic charges which give new characteristic features to the electromagnetic propagation. The main goal of this work is the analysis of these electromagnetic properties in order to find possible circuital applications of these materials to be utilized by devices.

Spectroscopic fingerprints for charge localization in the organic semiconductor (DOEO)4[HgBr4]·TCE

NASA Astrophysics Data System (ADS)

Koplak, Oksana V.; Chernenkaya, Alisa; Medjanik, Katerina; Brambilla, Alberto; Gloskovskii, Andrei; Calloni, Alberto; Elmers, Hans-Joachim; Schönhense, Gerd; Ciccacci, Franco; Morgunov, Roman B.

2015-05-01

Changes of the electronic structure accompanied by charge localization and a transition to an antiferromagnetic ground state were observed in the organic semiconductor (DOEO)4[HgBr4]·TCE. Localization starts in the temperature region of about 150 K and the antiferromagnetic state occurs below 60 K. The magnetic moment of the crystal contains contributions of inclusions (droplets), and individual paramagnetic centers formed by localized holes and free charge carriers at 2 K. Two types of inclusions of 100-400 nm and 2-5 nm sizes were revealed by transmission electron microscopy. Studying the temperature- and angular dependence of electron spin resonance (ESR) spectra revealed fingerprints of antiferromagnetic contributions as well as paramagnetic resonance spectra of individual localized charge carriers. The results point on coexistence of antiferromagnetic long and short range order as evident from a second ESR line. Photoelectron spectroscopy in the VUV, soft and hard X-ray range shows temperature-dependent effects upon crossing the critical temperatures around 60 K and 150 K. The substantially different probing depths of soft and hard X-ray photoelectron spectroscopy yield information on the surface termination. The combined investigation using complementary methods at the same sample reveals the close relation of changes in the transport properties and in the energy distribution of electronic states.

Temperature Dependence of Electric Transport in Few-layer Graphene under Large Charge Doping Induced by Electrochemical Gating

PubMed Central

Gonnelli, R. S.; Paolucci, F.; Piatti, E.; Sharda, Kanudha; Sola, A.; Tortello, M.; Nair, Jijeesh R.; Gerbaldi, C.; Bruna, M.; Borini, S.

2015-01-01

The temperature dependence of electric transport properties of single-layer and few-layer graphene at large charge doping is of great interest both for the study of the scattering processes dominating the conductivity at different temperatures and in view of the theoretically predicted possibility to reach the superconducting state in such extreme conditions. Here we present the results obtained in 3-, 4- and 5-layer graphene devices down to 3.5 K, where a large surface charge density up to about 6.8·1014 cm−2 has been reached by employing a novel polymer electrolyte solution for the electrochemical gating. In contrast with recent results obtained in single-layer graphene, the temperature dependence of the sheet resistance between 20 K and 280 K shows a low-temperature dominance of a T2 component – that can be associated with electron-electron scattering – and, at about 100 K, a crossover to the classic electron-phonon regime. Unexpectedly, this crossover does not show any dependence on the induced charge density, i.e. on the large tuning of the Fermi energy. PMID:25906088

Frequency-dependent local field factors in dielectric liquids by a polarizable force field and molecular dynamics simulations

NASA Astrophysics Data System (ADS)

Davari, Nazanin; Haghdani, Shokouh; Åstrand, Per-Olof

2015-12-01

A force field model for calculating local field factors, i.e. the linear response of the local electric field for example at a nucleus in a molecule with respect to an applied electric field, is discussed. It is based on a combined charge-transfer and point-dipole interaction model for the polarizability, and thereby it includes two physically distinct terms for describing electronic polarization: changes in atomic charges arising from transfer of charge between the atoms and atomic induced dipole moments. A time dependence is included both for the atomic charges and the atomic dipole moments and if they are assumed to oscillate with the same frequency as the applied electric field, a model for frequency-dependent properties are obtained. Furthermore, if a life-time of excited states are included, a model for the complex frequency-dependent polariability is obtained including also information about excited states and the absorption spectrum. We thus present a model for the frequency-dependent local field factors through the first molecular excitation energy. It is combined with molecular dynamics simulations of liquids where a large set of configurations are sampled and for which local field factors are calculated. We are normally not interested in the average of the local field factor but rather in configurations where it is as high as possible. In electrical insulation, we would like to avoid high local field factors to reduce the risk for electrical breakdown, whereas for example in surface-enhanced Raman spectroscopy, high local field factors are desired to give dramatically increased intensities.

Interfacial Electron Transfer at Sensitized Nanocrystalline TiO2 Electrolyte Interfaces: Influence of Surface Electric Fields and Lewis-Acidic Cations

NASA Astrophysics Data System (ADS)

Barr, Timothy J.

Interfacial electron transfer reactions facilitate charge separation and recombination in dye-sensitized solar cells (DSSCs). Understanding what controls these electron transfer reactions is necessary to develop efficient DSSCs. Gerischer proposed a theory for interfacial electron transfer where the rate constant was related to the energetic overlap between the donor and acceptor states. The present work focuses on understanding how the composition of the CH3CN electrolyte influenced this overlap. It was found that the identity of the electrolyte cation tuned the energetic position of TiO2 electron acceptor states, similar to how pH influences the flatband potential of bulk semiconductors in aqueous electrolytes. For example, the onset for absorption changes, that were attributed to electrons in the TiO2 thin film, were 0.5 V more positive in Mg2+ containing electrolyte than TBA+, where TBA+ is tetrabutylammonium. Similar studies performed on mesoporous, nanocrystalline SnO2 thin films reported a similar cation dependence, but also found evidence for electrons that did not absorb in the visible region that were termed ‘phantom electrons.’. Electron injection is known to generate surface electric fields on the order of 2 MV/cm. The rearrangement of cations in response to surface electric fields, termed screening, was investigated. It was found that magnitude of the electric field and the screening dynamics were dependent on the identity of the electrolyte cation. The rate of charge recombination to the anionic iodide/triiodide redox mediator correlated with the screening ability of the cation, and was initially thought to control charge recombination. However, it was difficult to determine whether electron diffusion or driving force were also cation dependent. Therefore, a in-lab built apparatus, termed STRiVE, was constructed that could disentangle the influence electron diffusion, driving force, and electric fields had on charge recombination. It was found that electron diffusion was independent of the electrolyte cation. Furthermore, charge recombination displayed the same cation-sensitivity using both anionic and cationic redox mediators, indicating electric fields did not cause the cation-dependence of charge recombination. Instead, it was found that the electrolyte cation tuned the energetic position of the TiO2 acceptor states and modulated the driving force for charge recombination.

Exploration of charge states of balanol analogues acting as ATP-competitive inhibitors in kinases.

PubMed

Hardianto, Ari; Yusuf, Muhammad; Liu, Fei; Ranganathan, Shoba

2017-12-28

(-)-Balanol is an ATP mimic that inhibits protein kinase C (PKC) isozymes and cAMP-dependent protein kinase (PKA) with limited selectivity. While PKA is a tumour promoter, PKC isozymes act as tumour promoters or suppressors, depending on the cancer type. In particular, PKCε is frequently implicated in cancer promotion, making it a potential target for anticancer drugs. To improve isozyme selectivity of balanol, exhaustive structural and activity relationship (SAR) studies have been performed in the last two decades, but with limited success. More recently, fluorination on balanol has shown improved selectivity for PKCε, although the fluorine effect is not yet clearly understood. Understanding the origin to this fluorine-based selectivity will be valuable for designing better balanol-based ATP mimicking inhibitors. Computational approaches such as molecular dynamics (MD) simulations can decipher the fluorine effect, provided that correct charges have been assigned to a ligand. Balanol analogues have multiple ionisable functional groups and the effect of fluorine substitutions on the exact charge state of each analogue bound to PKA and to PKCε needs to be thoroughly investigated in order to design highly selective inhibitors for therapeutic applications. We explored the charge states of novel fluorinated balanol analogues using MD simulations. For different potential charge states of these analogues, Molecular Mechanics Generalized Born Surface Area (MMGBSA) binding energy values were computed. This study suggests that balanol and the most potent fluorinated analogue (5S fluorine substitution on the azepane ring), have charges on the azepane ring (N1), and the phenolic (C6''OH) and the carboxylate (C15''O 2 H) groups on the benzophenone moiety, when bound to PKCε as well as PKA. To the best our knowledge, this is the first study showing that the phenolate group is charged in balanol and its analogues binding to the ATP site of PKCε. Correct charge assignments of ligands are important to obtain predicted binding energy values from MD simulations that reflect experimental values. Both fluorination and the local enzymatic environment of the ATP site can influence the exact charge states of balanol analogues. Overall, this study is highly valuable for further rational design of potent balanol analogues selective to PKCε.

A simple model of electron beam initiated dielectric breakdown

NASA Technical Reports Server (NTRS)

Beers, B. L.; Daniell, R. E.; Delmer, T. N.

1985-01-01

A steady state model that describes the internal charge distribution of a planar dielectric sample exposed to a uniform electron beam was developed. The model includes the effects of charge deposition and ionization of the beam, separate trap-modulated mobilities for electrons and holes, electron-hole recombination, and pair production by drifting thermal electrons. If the incident beam current is greater than a certain critical value (which depends on sample thickness as well as other sample properties), the steady state solution is non-physical.

High magnetic field magnetoresistance anomalies in the charge density wave state of the quasi-two dimensional bronze KMo6O{17}

NASA Astrophysics Data System (ADS)

Guyot, H.; Dumas, J.; Marcus, J.; Schlenker, C.; Vignolles, D.

2005-12-01

We report high magnetic field magnetoresistance measurements performed in pulsed fields up to 55 T on the quasi-two dimensional charge density wave conductor KMo{6}O{17}. Magnetoresistance curves show several anomalies below 28 T. First order transitions to smaller gap states take place at low temperature above 30 T. A phase diagram T(B) has been obtained. The angular dependence of the anomalies is reported.

Charge carrier dynamics in organic semiconductors and their donor-acceptor composites: Numerical modeling of time-resolved photocurrent

NASA Astrophysics Data System (ADS)

Johnson, Brian; Kendrick, Mark J.; Ostroverkhova, Oksana

2013-09-01

We present a model that describes nanosecond (ns) time-scale photocurrent dynamics in functionalized anthradithiophene (ADT) films and ADT-based donor-acceptor (D/A) composites. By fitting numerically simulated photocurrents to experimental data, we quantify contributions of multiple pathways of charge carrier photogeneration to the photocurrent, as well as extract parameters that characterize charge transport (CT) in organic films including charge carrier mobilities, trap densities, hole trap depth, and trapping and recombination rates. In pristine ADT films, simulations revealed two competing charge photogeneration pathways: fast, occurring on picosecond (ps) or sub-ps time scales with efficiencies below 10%, and slow, which proceeds at the time scale of tens of nanoseconds, with efficiencies of about 11%-12%, at the applied electric fields of 40-80 kV/cm. The relative contribution of these pathways to the photocurrent was electric field dependent, with the contribution of the fast process increasing with applied electric field. However, the total charge photogeneration efficiency was weakly electric field dependent exhibiting values of 14%-20% of the absorbed photons. The remaining 80%-86% of the photoexcitation did not contribute to charge carrier generation at these time scales. In ADT-based D/A composites with 2 wt.% acceptor concentration, an additional pathway of charge photogeneration that proceeds via CT exciton dissociation contributed to the total charge photogeneration. In the composite with the functionalized pentacene (Pn) acceptor, which exhibits strong exciplex emission from a tightly bound D/A CT exciton, the contribution of the CT state to charge generation was small, ˜8%-12% of the total number of photogenerated charge carriers, dependent on the electric field. In contrast, in the composite with PCBM acceptor, the CT state contributed about a half of all photogenerated charge carriers. In both D/A composites, the charge carrier mobilities were reduced and trap densities and average trap depths were increased, as compared to a pristine ADT donor film. A considerably slower recombination of free holes with trapped electrons was found in the composite with the PCBM acceptor, which led to slower decays of the transient photocurrent and considerably higher charge retention, as compared to a pristine ADT donor film and the composite with the functionalized Pn acceptor.

Spin Solid versus Magnetic Charge Ordered State in Artificial Honeycomb Lattice of Connected Elements

PubMed Central

Glavic, Artur; Summers, Brock; Dahal, Ashutosh; Kline, Joseph; Van Herck, Walter; Sukhov, Alexander; Ernst, Arthur

2018-01-01

Abstract The nature of magnetic correlation at low temperature in two‐dimensional artificial magnetic honeycomb lattice is a strongly debated issue. While theoretical researches suggest that the system will develop a novel zero entropy spin solid state as T → 0 K, a confirmation to this effect in artificial honeycomb lattice of connected elements is lacking. This study reports on the investigation of magnetic correlation in newly designed artificial permalloy honeycomb lattice of ultrasmall elements, with a typical length of ≈12 nm, using neutron scattering measurements and temperature‐dependent micromagnetic simulations. Numerical modeling of the polarized neutron reflectometry data elucidates the temperature‐dependent evolution of spin correlation in this system. As temperature reduces to ≈7 K, the system tends to develop novel spin solid state, manifested by the alternating distribution of magnetic vortex loops of opposite chiralities. Experimental results are complemented by temperature‐dependent micromagnetic simulations that confirm the dominance of spin solid state over local magnetic charge ordered state in the artificial honeycomb lattice with connected elements. These results enable a direct investigation of novel spin solid correlation in the connected honeycomb geometry of 2D artificial structure. PMID:29721429

Universal Binding and Recoil Corrections to Bound State g Factors in Hydrogenlike Ions

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

Eides, Michael I.; Martin, Timothy J. S.

2010-09-03

The leading relativistic and recoil corrections to bound state g factors of particles with arbitrary spin are calculated. It is shown that these corrections are universal for any spin and depend only on the free particle gyromagnetic ratios. To prove this universality we develop nonrelativistic quantum electrodynamics (NRQED) for charged particles with an arbitrary spin. The coefficients in the NRQED Hamiltonian for higher spin particles are determined only by the requirements of Lorentz invariance and local charge conservation in the respective relativistic theory. For spin one charged particles, the NRQED Hamiltonian follows from the renormalizable QED of the charged vectormore » bosons. We show that universality of the leading relativistic and recoil corrections can be explained with the help of the Bargmann-Michael-Telegdi equation.« less

Continuous distribution of emission states from single CdSe/ZnS quantum dots.

PubMed

Zhang, Kai; Chang, Hauyee; Fu, Aihua; Alivisatos, A Paul; Yang, Haw

2006-04-01

The photoluminescence dynamics of colloidal CdSe/ZnS/streptavidin quantum dots were studied using time-resolved single-molecule spectroscopy. Statistical tests of the photon-counting data suggested that the simple "on/off" discrete state model is inconsistent with experimental results. Instead, a continuous emission state distribution model was found to be more appropriate. Autocorrelation analysis of lifetime and intensity fluctuations showed a nonlinear correlation between them. These results were consistent with the model that charged quantum dots were also emissive, and that time-dependent charge migration gave rise to the observed photoluminescence dynamics.

Charge-transfer photodissociation of adsorbed molecules via electron image states

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

Jensen, E. T.

The 248 and 193 nm photodissociations of submonolayer quantities of CH{sub 3}Br and CH{sub 3}I adsorbed on thin layers of n-hexane indicate that the dissociation is caused by dissociative electron attachment from subvacuum level photoelectrons created in the copper substrate. The characteristics of this photodissociation-translation energy distributions and coverage dependences show that the dissociation is mediated by an image potential state which temporarily traps the photoelectrons near the n-hexane-vacuum interface, and then the charge transfers from this image state to the affinity level of a coadsorbed halomethane which then dissociates.

Calorimetric determination of thermal parameters for the Li/BrCl in SOCl2 (BCX) chemistry

NASA Technical Reports Server (NTRS)

Darcy, Eric C.; Kalu, Eric E.; White, Ralph E.

1990-01-01

The heat capacity of a Li-BCX DD-cell was found to be dependent on its state of charge by drop calorimetry measurements. The method of drop calorimetry involves measuring the energy (joules) gained or lost from a sample that is transferred from a bath at temperature A to one at temperature B. The thermoneutral potential is defined as the cell potential where the cell electrochemical reactions are neither exothermic nor endothermic. A Hart scientific calorimeter system, Model No. S77XX, designed for heat conduction calorimetry and drop calorimetry was used. Calorimetric analysis yielded a thermoneutral potential of 4.14 volts and a cell heat capacity dependent on the state of charge.

Two Components of Voltage-Dependent Inactivation in Cav1.2 Channels Revealed by Its Gating Currents

PubMed Central

Ferreira, Gonzalo; Ríos, Eduardo; Reyes, Nicolás

2003-01-01

Voltage-dependent inactivation (VDI) was studied through its effects on the voltage sensor in Cav1.2 channels expressed in tsA 201 cells. Two kinetically distinct phases of VDI in onset and recovery suggest the presence of dual VDI processes. Upon increasing duration of conditioning depolarizations, the half-distribution potential (V1/2) of intramembranous mobile charge was negatively shifted as a sum of two exponential terms, with time constants 0.5 s and 4 s, and relative amplitudes near 50% each. This kinetics behavior was consistent with that of increment of maximal charge related to inactivation (Qn). Recovery from inactivation was also accompanied by a reduction of Qn that varied with recovery time as a sum of two exponentials. The amplitudes of corresponding exponential terms were strongly correlated in onset and recovery, indicating that channels recover rapidly from fast VDI and slowly from slow VDI. Similar to charge “immobilization,” the charge moved in the repolarization (OFF) transient became slower during onset of fast VDI. Slow VDI had, instead, hallmarks of interconversion of charge. Confirming the mechanistic duality, fast VDI virtually disappeared when Li+ carried the current. A nine-state model with parallel fast and slow inactivation pathways from the open state reproduces most of the observations. PMID:12770874

Excited state properties of peridinin: Observation of a solvent dependence of the lowest excited singlet state lifetime and spectral behavior unique among carotenoids

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

Bautista, J.A.; Connors, R.E.; Raju, B.B.

1999-10-14

The spectroscopic properties and dynamic behavior of peridinin in several different solvents were studied by steady-state absorption, fluorescence, and transient optical spectroscopy. The lifetime of the lowest excited singlet state of peridinin is found to be strongly dependent on solvent polarity and ranges from 7 ps in the strongly polar solvent trifluoroethanol to 172 ps in the nonpolar solvents cyclohexane and benzene. The lifetimes show no obvious correlation with solvent polarizability, and hydrogen bonding of the solvent molecules to peridinin is not an important factor in determining the dynamic behavior of the lowest excited singlet state. The wavelengths of emissionmore » maxima, the quantum yields of fluorescence, and the transient absorption spectra are also affected by the solvent environment. A model consistent with the data and supported by preliminary semiempirical calculations invokes the presence of a charge transfer state in the excited state manifold of peridinin to account for the observations. The charge transfer state most probably results from the presence of the lactone ring in the {pi}-electron conjugation of peridinin analogous to previous findings on aminocoumarins and related compounds. The behavior of peridinin reported here is highly unusual for carotenoids, which generally show little dependence of the spectral properties and lifetimes of the lowest excited singlet state on the solvent environment.« less

Dynamics of the Rydberg state population of slow highly charged ions impinging a solid surface at arbitrary collision geometry

NASA Astrophysics Data System (ADS)

Nedeljković, N. N.; Majkić, M. D.; Božanić, D. K.; Dojčilović, R. J.

2016-06-01

We consider the population dynamics of the intermediate Rydberg states of highly charged ions (core charge Z\\gg 1, principal quantum number {n}{{A}}\\gg 1) interacting with solid surfaces at arbitrary collision geometry. The recently developed resonant two-state vector model for the grazing incidence (2012 J. Phys. B: At. Mol. Opt. Phys. 45 215202) is extended to the quasi-resonant case and arbitrary angle of incidence. According to the model, the population probabilities depend both on the projectile parallel and perpendicular velocity components, in a complementary way. A cascade neutralization process for {{{Xe}}}Z+ ions, for Z=15{--}45, interacting with a conductive-surface is considered by taking into account the population dynamics. For an arbitrary collision geometry and given range of ionic velocities, a micro-staircase model for the simultaneous calculation of the kinetic energy gain and the charge state of the ion in front of the surface is proposed. The relevance of the obtained results for the explanation of the formation of nanostructures on solid surfaces by slow highly charged ions for normal incidence geometry is briefly discussed.

Ion Current Rectification, Limiting and Overlimiting Conductances in Nanopores

PubMed Central

van Oeffelen, Liesbeth; Van Roy, Willem; Idrissi, Hosni; Charlier, Daniel; Lagae, Liesbet; Borghs, Gustaaf

2015-01-01

Previous reports on Poisson-Nernst-Planck (PNP) simulations of solid-state nanopores have focused on steady state behaviour under simplified boundary conditions. These are Neumann boundary conditions for the voltage at the pore walls, and in some cases also Donnan equilibrium boundary conditions for concentrations and voltages at both entrances of the nanopore. In this paper, we report time-dependent and steady state PNP simulations under less restrictive boundary conditions, including Neumann boundary conditions applied throughout the membrane relatively far away from the nanopore. We simulated ion currents through cylindrical and conical nanopores with several surface charge configurations, studying the spatial and temporal dependence of the currents contributed by each ion species. This revealed that, due to slow co-diffusion of oppositely charged ions, steady state is generally not reached in simulations or in practice. Furthermore, it is shown that ion concentration polarization is responsible for the observed limiting conductances and ion current rectification in nanopores with asymmetric surface charges or shapes. Hence, after more than a decade of collective research attempting to understand the nature of ion current rectification in solid-state nanopores, a relatively intuitive model is retrieved. Moreover, we measured and simulated current-voltage characteristics of rectifying silicon nitride nanopores presenting overlimiting conductances. The similarity between measurement and simulation shows that overlimiting conductances can result from the increased conductance of the electric double-layer at the membrane surface at the depletion side due to voltage-induced polarization charges. The MATLAB source code of the simulation software is available via the website http://micr.vub.ac.be. PMID:25978328

Applicability of post-ionization theory to laser-assisted field evaporation of magnetite

DOE PAGES

Schreiber, Daniel K.; Chiaramonti, Ann N.; Gordon, Lyle M.; ...

2014-12-15

Analysis of the mean Fe ion charge state from laser-assisted field evaporation of magnetite (Fe3O4) reveals unexpected trends as a function of laser pulse energy that break from conventional post-ionization theory for metals. For Fe ions evaporated from magnetite, the effects of post-ionization are partially offset by the increased prevalence of direct evaporation into higher charge states with increasing laser pulse energy. Therefore the final charge state is related to both the field strength and the laser pulse energy, despite those variables themselves being intertwined when analyzing at a constant detection rate. Comparison of data collected at different base temperaturesmore » also show that the increased prevalence of Fe2+ at higher laser energies is possibly not a direct thermal effect. Conversely, the ratio of 16O+:16O2+ is well-correlated with field strength and unaffected by laser pulse energy on its own, making it a better overall indicator of the field evaporation conditions than the mean Fe charge state. Plotting the normalized field strength versus laser pulse energy also elucidates a non-linear dependence, in agreement with previous observations on semiconductors, that suggests a field-dependent laser absorption efficiency. Together these observations demonstrate that the field evaporation process for laser-pulsed oxides exhibits fundamental differences from metallic specimens that cannot be completely explained by post-ionization theory. Further theoretical studies, combined with detailed analytical observations, are required to understand fully the field evaporation process of non-metallic samples.« less

Comparative study of mobility extraction methods in p-type polycrystalline silicon thin film transistors

NASA Astrophysics Data System (ADS)

Liu, Kai; Liu, Yuan; Liu, Yu-Rong; En, Yun-Fei; Li, Bin

2017-07-01

Channel mobility in the p-type polycrystalline silicon thin film transistors (poly-Si TFTs) is extracted using Hoffman method, linear region transconductance method and multi-frequency C-V method. Due to the non-negligible errors when neglecting the dependence of gate-source voltage on the effective mobility, the extracted mobility results are overestimated using linear region transconductance method and Hoffman method, especially in the lower gate-source voltage region. By considering of the distribution of localized states in the band-gap, the frequency independent capacitance due to localized charges in the sub-gap states and due to channel free electron charges in the conduction band were extracted using multi-frequency C-V method. Therefore, channel mobility was extracted accurately based on the charge transport theory. In addition, the effect of electrical field dependent mobility degradation was also considered in the higher gate-source voltage region. In the end, the extracted mobility results in the poly-Si TFTs using these three methods are compared and analyzed.

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

NASA Astrophysics Data System (ADS)

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.

Effects of Charge State on Fragmentation Pathways, Dynamics, and Activation Energies of Ubiquitin Ions Measured by Blackbody Infrared Radiative Dissociation

PubMed Central

Jockusch, Rebecca A.; Schnier, Paul D.; Price, William D.; Strittmatter, Eric. F.; Demirev, Plamen A.; Williams*, Evan R.

2005-01-01

Blackbody infrared radiative dissociation spectra of the (M + 5H)5+ through (M + 11H)11+ ions of the protein ubiquitin (8.6 kDa) formed by electrospray ionization were measured in a Fourier-transform mass spectrometer. The 5+ ion dissociates exclusively by loss of water and/or ammonia, whereas the 11+ charge state dissociates only by formation of complementary y and b ions. These two processes are competitive for intermediate charge state ions, with the formation of y and b ions increasingly favored for the higher charge states. The y and b ions are formed by cleavage of the backbone amide bond on the C-terminal side of acidic residues exclusively, with cleavage adjacent to aspartic acid favored. Thermal unimolecular dissociation rate constants for the dissociation of each of these charge states were measured. From the temperature dependence of these rates, Arrhenius activation parameters in the rapid energy exchange limit are obtained. The activation energies (Ea) and preexponential factors (A) for the 5+, 8+, and 9+ ions are 1.2 eV and 1012 s−1, respectively. These values for the 6+ and 7+ ions are 0.9–1.0 eV and 109 s−1, and those for the 10+ and 11+ ions are 1.6 eV and 1016–1017 s−1. Thus, with the exception of the 5+ ion, the higher charge states of ubiquitin have larger dissociation activation energies than the lower charge states. The different A factors observed for production of y and b ions from different precursor charge states indicate that they are formed by different mechanisms, ranging from relatively complex rearrangements to direct bond cleavages. These results clearly demonstrate that the relative dissociation rates of large biomolecule ions by themselves are not necessarily a reliable indicator of their relative dissociation energies, even when similar fragment ions are formed. PMID:9075403

Effects of charge state on fragmentation pathways, dynamics, and activation energies of ubiquitin ions measured by blackbody infrared radiative dissociation.

PubMed

Jockusch, R A; Schnier, P D; Price, W D; Strittmatter, E F; Demirev, P A; Williams, E R

1997-03-15

Blackbody infrared radiative dissociation spectra of the (M + 5H)5+ through (M + 11H)11+ ions of the protein ubiquitin (8.6 kDa) formed by electrospray ionization were measured in a Fourier-transform mass spectrometer. The 5+ ion dissociates exclusively by loss of water and/or ammonia, whereas the 11+ charge state dissociates only by formation of complementary y and b ions. These two processes are competitive for intermediate charge state ions, with the formation of y and b ions increasingly favored for the higher charge states. The y and b ions are formed by cleavage of the backbone amide bond on the C-terminal side of acidic residues exclusively, with cleavage adjacent to aspartic acid favored. Thermal unimolecular dissociation rate constants for the dissociation of each of these charge states were measured. From the temperature dependence of these rates, Arrhenius activation parameters in the rapid energy exchange limit are obtained. The activation energies (Ea) and preexponential factors (A) for the 5+, 8+, and 9+ ions are 1.2 eV and 10(12) s-1, respectively. These values for the 6+ and 7+ ions are 0.9-1.0 eV and 10(9) s-1, and those for the 10+ and 11+ ions are 1.6 eV and 10(16)-10(17) s-1. Thus, with the exception of the 5+ ion, the higher charge states of ubiquitin have larger dissociation activation energies than the lower charge states. The different A factors observed for production of y and b ions from different precursor charge states indicate that they are formed by different mechanisms, ranging from relatively complex rearrangements to direct bond cleavages. These results clearly demonstrate that the relative dissociation rates of large biomolecule ions by themselves are not necessarily a reliable indicator of their relative dissociation energies, even when similar fragment ions are formed.

Direct Measurement of Nuclear Dependence of Charged Current Quasielasticlike Neutrino Interactions Using MINERvA

NASA Astrophysics Data System (ADS)

Betancourt, M.; Ghosh, A.; Walton, T.; Altinok, O.; Bellantoni, L.; Bercellie, A.; Bodek, A.; Bravar, A.; Cai, T.; Martinez Caicedo, D. A.; Carneiro, M. F.; Dytman, S. A.; Díaz, G. A.; Felix, J.; Fields, L.; Fine, R.; Galindo, R.; Gallagher, H.; Ghosh, A.; Golan, T.; Gran, R.; Harris, D. A.; Higuera, A.; Hurtado, K.; Kiveni, M.; Kleykamp, J.; Le, T.; Maher, E.; Manly, S.; Mann, W. A.; Marshall, C. M.; McFarland, K. S.; McGivern, C. L.; McGowan, A. M.; Messerly, B.; Miller, J.; Mislivec, A.; Morfín, J. G.; Mousseau, J.; Naples, D.; Nelson, J. K.; Norrick, A.; Nuruzzaman, Patrick, C. E.; Perdue, G. N.; Ramírez, M. A.; Ren, L.; Rimal, D.; Rodrigues, P. A.; Ruterbories, D.; Schellman, H.; Sobczyk, J. T.; Solano Salinas, C. J.; Sánchez Falero, S.; Valencia, E.; Wolcott, J.; Wospakrik, M.; Yaeggy, B.; Minerva Collaboration

2017-08-01

Charged-current νμ interactions on carbon, iron, and lead with a final state hadronic system of one or more protons with zero mesons are used to investigate the influence of the nuclear environment on quasielasticlike interactions. The transferred four-momentum squared to the target nucleus, Q2, is reconstructed based on the kinematics of the leading proton, and differential cross sections versus Q2 and the cross-section ratios of iron, lead, and carbon to scintillator are measured for the first time in a single experiment. The measurements show a dependence on the atomic number. While the quasielasticlike scattering on carbon is compatible with predictions, the trends exhibited by scattering on iron and lead favor a prediction with intranuclear rescattering of hadrons accounted for by a conventional particle cascade treatment. These measurements help discriminate between different models of both initial state nucleons and final state interactions used in the neutrino oscillation experiments.

Band dependence of charge density wave in quasi-one-dimensional Ta2NiSe7 probed by orbital magnetoresistance

NASA Astrophysics Data System (ADS)

He, Jiaming; Zhang, Yiran; Wen, Libin; Yang, Yusen; Liu, Jinyu; Wu, Yueshen; Lian, Hailong; Xing, Hui; Wang, Shun; Mao, Zhiqiang; Liu, Ying

2017-07-01

Ta2NiSe7 is a quasi-one-dimensional (quasi-1D) transition-metal chalcogenide with Ta and Ni chain structures. An incommensurate charge-density wave (CDW) in this quasi-1D structure was well studied previously using tunnelling spectrum, X-ray, and electron diffraction, whereas its transport property and the relation to the underlying electronic states remain to be explored. Here, we report our results of the magnetoresistance (MR) on Ta2NiSe7. A breakdown of Kohler's rule is found upon entering the CDW state. Concomitantly, a clear change in curvature in the field dependence of MR is observed. We show that the curvature change is well described by the two-band orbital MR, with the hole density being strongly suppressed in the CDW state, indicating that the p orbitals from Se atoms dominate the change in transport through CDW transition.

Coverage Dependent Charge Reduction of Cationic Gold Clusters on Surfaces Prepared Using Soft Landing of Mass-selected Ions

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

Johnson, Grant E.; Priest, Thomas A.; Laskin, Julia

2012-11-29

The ionic charge state of monodisperse cationic gold clusters on surfaces may be controlled by selecting the coverage of mass-selected ions soft landed onto a substrate. Polydisperse diphosphine-capped gold clusters were synthesized in solution by reduction of chloro(triphenylphosphine)gold(I) with borane tert-butylamine in the presence of 1,3-bis(diphenylphosphino)propane. The polydisperse gold clusters were introduced into the gas phase by electrospray ionization and mass selection was employed to select a multiply charged cationic cluster species (Au11L53+, m/z = 1409, L = 1,3-bis(diphenylphosphino)propane) which was delivered to the surfaces of four different self-assembled monolayers on gold (SAMs) at coverages of 1011 and 1012 clusters/mm2.more » Employing the spatial profiling capabilities of in-situ time-of-flight secondary ion mass spectrometry (TOF-SIMS) it is shown that, in addition to the chemical functionality of the monolayer (as demonstrated previously: ACS Nano, 2012, 6, 573) the coverage of cationic gold clusters on the surface may be used to control the distribution of ionic charge states of the soft-landed multiply charged clusters. In the case of a 1H,1H,2H,2H-perfluorodecanethiol SAM (FSAM) almost complete retention of charge by the deposited Au11L53+ clusters was observed at a lower coverage of 1011 clusters/mm2. In contrast, at a higher coverage of 1012 clusters/mm2, pronounced reduction of charge to Au11L52+ and Au11L5+ was observed on the FSAM. When soft landed onto 16- and 11-mercaptohexadecanoic acid surfaces on gold (16,11-COOH-SAMs), the mass-selected Au11L53+ clusters exhibited partial reduction of charge to Au11L52+ at lower coverage and additional reduction of charge to both Au11L52+ and Au11L5+ at higher coverage. The reduction of charge was found to be more pronounced on the surface of the shorter (thinner) C11 than the longer (thicker) C16-COOH-SAM. On the surface of the 1-dodecanethiol (HSAM) monolayer, the most abundant charge state was found to be Au11L52+ at lower coverage and Au11L5+ at higher coverage, respectively. A coverage-dependent electron tunneling mechanism is proposed to account for the observed reduction of charge of mass-selected multiply charged gold clusters soft landed on SAMs. The results demonstrate that one of the critical parameters that influence the chemical and physical properties of supported metal clusters, ionic charge state, may be controlled by selecting the coverage of charged species soft landed onto surfaces.« less

Quantitative analysis of intramolecular exciplex and electron transfer in a double-linked zinc porphyrin-fullerene dyad.

PubMed

Al-Subi, Ali Hanoon; Niemi, Marja; Tkachenko, Nikolai V; Lemmetyinen, Helge

2012-10-04

Photoinduced charge transfer in a double-linked zinc porphyrin-fullerene dyad is studied. When the dyad is excited at the absorption band of the charge-transfer complex (780 nm), an intramolecular exciplex is formed, followed by the complete charge separated (CCS) state. By analyzing the results obtained from time-resolved transient absorption and emission decay measurements in a range of solvents with different polarities, we derived a dependence between the observable lifetimes and internal parameters controlling the reaction rate constants based on the semiquantum Marcus electron-transfer theory. The critical value of the solvent polarity was found to be ε(r) ≈ 6.5: in solvents with higher dielectric constants, the energy of the CCS state is lower than that of the exciplex and the relaxation takes place via the CCS state predominantly, whereas in solvents with lower polarities the energy of the CCS state is higher and the exciplex relaxes directly to the ground state. In solvents with moderate polarities the exciplex and the CCS state are in equilibrium and cannot be separated spectroscopically. The degree of the charge shift in the exciplex relative to that in the CCS state was estimated to be 0.55 ± 0.02. The electronic coupling matrix elements for the charge recombination process and for the direct relaxation of the exciplex to the ground state were found to be 0.012 ± 0.001 and 0.245 ± 0.022 eV, respectively.

Passivating the sulfur vacancy in monolayer MoS2

NASA Astrophysics Data System (ADS)

Lu, Haichang; Kummel, Andrew; Robertson, John

2018-06-01

Various methods to passivate the sulfur vacancy in 2D MoS2 are modeled using density functional theory (DFT) to understand the passivation mechanism at an atomic scale. First, the organic super acid, bis(trifluoromethane)sulfonimide (TFSI) is a strong protonating agent, and it is experimentally found to greatly increase the photoluminescence efficiency. DFT simulations find that the effectiveness of passivation depends critically on the charge state and number of hydrogens donated by TFSI since this determines the symmetry of the defect complex. A symmetrical complex is formed by three hydrogen atoms bonding to the defect in a -1 charge state, and this gives no bandgap states and a Fermi level in the midgap. However, a charge state of +1 gives a lower symmetry complex with one state in the gap. One or two hydrogens also give complexes with gap states. Second, passivation by O2 can provide partial passivation by forming a bridge bond across the S vacancy, but it leaves a defect state in the lower bandgap. On the other hand, substitutional additions do not shift the vacancy states out of the gap.

Extension of the self-consistent-charge density-functional tight-binding method: third-order expansion of the density functional theory total energy and introduction of a modified effective coulomb interaction.

PubMed

Yang, Yang; Yu, Haibo; York, Darrin; Cui, Qiang; Elstner, Marcus

2007-10-25

The standard self-consistent-charge density-functional-tight-binding (SCC-DFTB) method (Phys. Rev. B 1998, 58, 7260) is derived by a second-order expansion of the density functional theory total energy expression, followed by an approximation of the charge density fluctuations by charge monopoles and an effective damped Coulomb interaction between the atomic net charges. The central assumptions behind this effective charge-charge interaction are the inverse relation of atomic size and chemical hardness and the use of a fixed chemical hardness parameter independent of the atomic charge state. While these approximations seem to be unproblematic for many covalently bound systems, they are quantitatively insufficient for hydrogen-bonding interactions and (anionic) molecules with localized net charges. Here, we present an extension of the SCC-DFTB method to incorporate third-order terms in the charge density fluctuations, leading to chemical hardness parameters that are dependent on the atomic charge state and a modification of the Coulomb scaling to improve the electrostatic treatment within the second-order terms. These modifications lead to a significant improvement in the description of hydrogen-bonding interactions and proton affinities of biologically relevant molecules.

Gravitational memory charges of supertranslation and superrotation on Rindler horizons

NASA Astrophysics Data System (ADS)

Hotta, Masahiro; Trevison, Jose; Yamaguchi, Koji

2016-10-01

In a Rindler-type coordinate system spanned in a region outside of a black hole horizon, we have nonvanishing classical holographic charges as soft hairs on the horizon for stationary black holes. Taking a large black hole mass limit, the spacetimes with the charges are described by asymptotic Rindler metrics. We construct a general theory of gravitational holographic charges for a (1 +3 )-dimensional linearized gravity field in the Minkowski background with Rindler horizons. Although matter crossing a Rindler horizon causes horizon deformation and a time-dependent coordinate shift—that is, gravitational memory—the supertranslation and superrotation charges on the horizon can be defined during and after its passage through the horizon. It is generally proven that holographic states on the horizon cannot store any information about absorbed perturbative gravitational waves. However, matter crossing the horizon really excites holographic states. By using gravitational memory operators, which consist of the holographic charge operators, we suggest a resolution of the no-cloning paradox of quantum information between matter falling into the horizon and holographic charges on the horizon from the viewpoint of the contextuality of quantum measurement.

Emergence of Landauer transport from quantum dynamics: A model Hamiltonian approach

NASA Astrophysics Data System (ADS)

Pal, Partha Pratim; Ramakrishna, S.; Seideman, Tamar

2018-04-01

The Landauer expression for computing current-voltage characteristics in nanoscale devices is efficient but not suited to transient phenomena and a time-dependent current because it is applicable only when the charge carriers transition into a steady flux after an external perturbation. In this article, we construct a very general expression for time-dependent current in an electrode-molecule-electrode arrangement. Utilizing a model Hamiltonian (consisting of the subsystem energy levels and their electronic coupling terms), we propagate the Schrödinger wave function equation to numerically compute the time-dependent population in the individual subsystems. The current in each electrode (defined in terms of the rate of change of the corresponding population) has two components, one due to the charges originating from the same electrode and the other due to the charges initially residing at the other electrode. We derive an analytical expression for the first component and illustrate that it agrees reasonably with its numerical counterpart at early times. Exploiting the unitary evolution of a wavefunction, we construct a more general Landauer style formula and illustrate the emergence of Landauer transport from our simulations without the assumption of time-independent charge flow. Our generalized Landauer formula is valid at all times for models beyond the wide-band limit, non-uniform electrode density of states and for time and energy-dependent electronic coupling between the subsystems. Subsequently, we investigate the ingredients in our model that regulate the onset time scale of this steady state. We compare the performance of our general current expression with the Landauer current for time-dependent electronic coupling. Finally, we comment on the applicability of the Landauer formula to compute hot-electron current arising upon plasmon decoherence.

Emergence of Landauer transport from quantum dynamics: A model Hamiltonian approach.

PubMed

Pal, Partha Pratim; Ramakrishna, S; Seideman, Tamar

2018-04-14

The Landauer expression for computing current-voltage characteristics in nanoscale devices is efficient but not suited to transient phenomena and a time-dependent current because it is applicable only when the charge carriers transition into a steady flux after an external perturbation. In this article, we construct a very general expression for time-dependent current in an electrode-molecule-electrode arrangement. Utilizing a model Hamiltonian (consisting of the subsystem energy levels and their electronic coupling terms), we propagate the Schrödinger wave function equation to numerically compute the time-dependent population in the individual subsystems. The current in each electrode (defined in terms of the rate of change of the corresponding population) has two components, one due to the charges originating from the same electrode and the other due to the charges initially residing at the other electrode. We derive an analytical expression for the first component and illustrate that it agrees reasonably with its numerical counterpart at early times. Exploiting the unitary evolution of a wavefunction, we construct a more general Landauer style formula and illustrate the emergence of Landauer transport from our simulations without the assumption of time-independent charge flow. Our generalized Landauer formula is valid at all times for models beyond the wide-band limit, non-uniform electrode density of states and for time and energy-dependent electronic coupling between the subsystems. Subsequently, we investigate the ingredients in our model that regulate the onset time scale of this steady state. We compare the performance of our general current expression with the Landauer current for time-dependent electronic coupling. Finally, we comment on the applicability of the Landauer formula to compute hot-electron current arising upon plasmon decoherence.

Simulation of perturbation produced by an absorbing spherical body in collisionless plasma

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

Krasovsky, V. L., E-mail: vkrasov@iki.rssi.ru; Kiselyov, A. A., E-mail: alexander.kiselyov@stonehenge-3.net.ru; Dolgonosov, M. S.

2017-01-15

A steady plasma state reached in the course of charging of an absorbing spherical body is found using computational methods. Numerical simulations provide complete information on this process, thereby allowing one to find the spatiotemporal dependences of the physical quantities and observe the kinetic phenomena accompanying the formation of stable electron and ion distributions in phase space. The distribution function of trapped ions is obtained, and their contribution to the screening of the charged sphere is determined. The sphere charge and the charge of the trapped-ion cloud are determined as functions of the unperturbed plasma parameters.

Negative differential electrolyte resistance in a solid-state nanopore resulting from electroosmotic flow bistability.

PubMed

Luo, Long; Holden, Deric A; White, Henry S

2014-03-25

A solid-state nanopore separating two aqueous solutions containing different concentrations of KCl is demonstrated to exhibit negative differential resistance (NDR) when a constant pressure is applied across the nanopore. NDR refers to a decrease in electrical current when the voltage applied across the nanopore is increased. NDR results from the interdependence of solution flow (electroosmotic and pressure-engendered) with the distributions of K+ and Cl- within the nanopore. A switch from a high-conductivity state to a low-conductivity state occurs over a very narrow voltage window (<2 mV) that depends on the nanopore geometry, electrolyte concentration, and nanopore surface charge density. Finite element simulations based on a simultaneous solution of the Navier-Stokes, Poisson, and Nernst-Planck equations demonstrate that NDR results from a positive feedback mechanism between the ion distributions and electroosmotic flow, yielding a true bistability in fluid flow and electrical current at a critical applied voltage, i.e., the NDR "switching potential". Solution pH and Ca2+ were separately employed as chemical stimuli to investigate the dependence of the NDR on the surface charge density. The NDR switching potential is remarkably sensitive to the surface charge density, and thus to pH and the presence of Ca2+, suggesting possible applications in chemical sensing.

Remarks on thermalization in 2D CFT

NASA Astrophysics Data System (ADS)

de Boer, Jan; Engelhardt, Dalit

2016-12-01

We revisit certain aspects of thermalization in 2D conformal field theory (CFT). In particular, we consider similarities and differences between the time dependence of correlation functions in various states in rational and non-rational CFTs. We also consider the distinction between global and local thermalization and explain how states obtained by acting with a diffeomorphism on the ground state can appear locally thermal, and we review why the time-dependent expectation value of the energy-momentum tensor is generally a poor diagnostic of global thermalization. Since all 2D CFTs have an infinite set of commuting conserved charges, generic initial states might be expected to give rise to a generalized Gibbs ensemble rather than a pure thermal ensemble at late times. We construct the holographic dual of the generalized Gibbs ensemble and show that, to leading order, it is still described by a Banados-Teitelboim-Zanelli black hole. The extra conserved charges, while rendering c <1 theories essentially integrable, therefore seem to have little effect on large-c conformal field theories.

Revealing energy level structure of individual quantum dots by tunneling rate measured by single-electron sensitive electrostatic force spectroscopy.

PubMed

Roy-Gobeil, Antoine; Miyahara, Yoichi; Grutter, Peter

2015-04-08

We present theoretical and experimental studies of the effect of the density of states of a quantum dot (QD) on the rate of single-electron tunneling that can be directly measured by electrostatic force microscopy (e-EFM) experiments. In e-EFM, the motion of a biased atomic force microscope cantilever tip modulates the charge state of a QD in the Coulomb blockade regime. The charge dynamics of the dot, which is detected through its back-action on the capacitavely coupled cantilever, depends on the tunneling rate of the QD to a back-electrode. The density of states of the QD can therefore be measured through its effect on the energy dependence of tunneling rate. We present experimental data on individual 5 nm colloidal gold nanoparticles that exhibit a near continuous density of state at 77 K. In contrast, our analysis of already published data on self-assembled InAs QDs at 4 K clearly reveals discrete degenerate energy levels.

Quantum Mechanical Calculations of Free Energy and Open-Circuit Voltage in Lattice Modeled Organic Photovoltaic Devices

NASA Astrophysics Data System (ADS)

Lankevich, Vladimir; Bittner, Eric

In organic photovoltaic devices (OPVs), initially bound electron and hole can take many different paths to dissociate and become free charge carriers. This leads to the increase in their density of states and therefore increase in the entropy of the system. Accurate description of the energy barriers that charges have to overcome, therefore requires calculation of the free energy. Free energy of an OPV is directly related to its open-circuit voltage and depends only on few important parameters such as average life-time of a charge-transfer state, average energy of the charge-transfer state and energetic disorder in the system. We extend these ideas to the quantum mechanical simulations of the dissociation in the lattice modeled bulk-heterojunction system. We observe average excitonic and free energies that agree with theoretical predictions and the number of experimental results from previous studies. We study effects of the energy disorder and importance of the dimensionality and morphology in materials such as polymer-fullerene blends.

Charge dependence of the plasma travel length in atmospheric-pressure plasma

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

Yambe, Kiyoyuki; Konda, Kohmei; Masuda, Seiya

Plasma plume is generated using a quartz tube, helium gas, and foil electrode by applying AC high voltage under the atmosphere. The plasma plume is released into the atmosphere from inside of the quartz tube and is seen as the continuous movement of the plasma bullet. The travel length of plasma bullet is defined from plasma energy and force due to electric field. The drift velocity of plasma bullet has the upper limit under atmospheric-pressure because the drift velocity is determined from the balance between electric field and resistive force due to collisions between plasma and air. The plasma plumemore » charge depends on the drift velocity. Consequently, in the laminar flow of helium gas flow state, the travel length of the plasma plume logarithmically depends on the plasma plume charge which changes with both the electric field and the resistive force.« less

Ligand-dependent exciton dynamics and photovoltaic properties of PbS quantum dot heterojunction solar cells.

PubMed

Chang, Jin; Ogomi, Yuhei; Ding, Chao; Zhang, Yao Hong; Toyoda, Taro; Hayase, Shuzi; Katayama, Kenji; Shen, Qing

2017-03-01

The surface chemistry of colloidal quantum dots (QDs) plays an important role in determining the photoelectric properties of QD films and the corresponding quantum dot heterojunction solar cells (QDHSCs). To investigate the effects of the ligand structure on the photovoltaic performance and exciton dynamics of QDHSCs, PbS QDHSCs were fabricated by the solid state ligand exchange method with mercaptoalkanoic acid as the cross-linking ligand. Temperature-dependent photoluminescence and ultrafast transient absorption spectra show that the electronic coupling and charge transfer rate within QD ensembles were monotonically enhanced as the ligand length decreased. However, in practical QDHSCs, the second shortest ligand 3-mercaptopropionic acid (MPA) showed higher power conversion efficiency than the shortest ligand thioglycolic acid (TGA). This could be attributed to the difference in their surface trap states, supported by thermally stimulated current measurements. Moreover, compared with the non-conjugated ligand MPA, the conjugated ligand 4-mercaptobenzoic acid (MBA) introduces less trap states and has a similar charge transfer rate in QD ensembles, but has poor photovoltaic properties. This unexpected result could be contributed by the QD-ligand orbital mixing, leading to the charge transfer from QDs to ligands instead of charge transfer between adjacent QDs. This work highlights the significant effects of ligand structures on the photovoltaic properties and exciton dynamics of QDHSCs, which would shed light on the further development of QD-based photoelectric devices.

The nature and role of trap states in a dendrimer-based organic field-effect transistor explosive sensor

NASA Astrophysics Data System (ADS)

Tang, Guoqiang; Chen, Simon S. Y.; Lee, Kwan H.; Pivrikas, Almantas; Aljada, Muhsen; Burn, Paul L.; Meredith, Paul; Shaw, Paul E.

2013-06-01

We report the fabrication and charge transport characterization of carbazole dendrimer-based organic field-effect transistors (OFETs) for the sensing of explosive vapors. After exposure to para-nitrotoluene (pNT) vapor, the OFET channel carrier mobility decreases due to trapping induced by the absorbed pNT. The influence of trap states on transport in devices before and after exposure to pNT vapor has been determined using temperature-dependent measurements of the field-effect mobility. These data clearly show that the absorption of pNT vapor into the dendrimer active layer results in the formation of additional trap states. Such states inhibit charge transport by decreasing the density of conducting states.

Charge transport study in bis{2-(2-hydroxyphenyl) benzoxazolate} zinc [Zn(hpb)2

NASA Astrophysics Data System (ADS)

Rai, Virendra Kumar; Srivastava, Ritu; Chauhan, Gayatri; Kumar, Arunandan; Kamalasanan, M. N.

2008-10-01

The nature of the electrical transport mechanism for carrier transport in pure bis {2-(2-hydroxyphenyl) benzoxazolate} zinc [Zn(hpb)2] has been studied by current voltage measurements of samples at different thicknesses and at different temperatures. Hole-only devices show ohmic conduction at low voltages and space charge conduction at high voltages. The space charge conduction is clearly identifiable with a square law dependence of current on voltage as well as the scaling of current inversely with the cube of thickness. With a further increase in voltage, the current increases with a Vm dependence with m varying with temperature typical of trap limited conduction with an exponential distribution of trap states. From the square law region the effective charge carrier mobility of holes has been evaluated as 2.5 × 10-11 m2 V-1 s-1. Electron-only devices however show electrode limited conduction, which was found to obey the Scott Malliaras model of charge injection.

Localization of holes near charged defects in orbitally degenerate, doped Mott insulators

NASA Astrophysics Data System (ADS)

Avella, Adolfo; Oleś, Andrzej M.; Horsch, Peter

2018-05-01

We study the role of charged defects, disorder and electron-electron (e-e) interactions in a multiband model for t2g electrons in vanadium perovskites R1-xCaxVO3 (R = La,…,Y). By means of unrestricted Hartree-Fock calculations, we find that the atomic multiplet structure persists up to 50% Ca doping. Using the inverse participation number, we explore the degree of localization and its doping dependence for all electronic states. The observation of strongly localized wave functions is consistent with our conjecture that doped holes form spin-orbital polarons that are strongly bound to the charged Ca2+ defects. Interestingly, the long-range e-e interactions lead to a discontinuity in the wave function size across the chemical potential, where the electron removal states are more localized than the addition states.

Charge-state distribution of Li ions from the β decay of laser-trapped He 6 atoms

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

Hong, R.; Leredde, A.; Bagdasarova, Y.

The accurate determination of atomic final states following nuclear β decay plays an important role in several experiments. In particular, the charge state distributions of ions following nuclear β decay are important for determinations of the β-ν angular correlation with improved precision. Also, beyond the hydrogenic cases, the decay of neutral 6He presents the simplest case. Our measurement aims at providing benchmarks to test theoretical calculations. The kinematics of Li n+ ions produced following the β decay of 6He within an electric field were measured using 6He atoms in the metastable (1s2s, 3S 1) and (1s2p, 3P 2) states confinedmore » by a magneto-optical trap. The electron shakeoff probabilities were deduced, including their dependence on ion energy. Finally, we find significant discrepancies on the fractions of Li ions in the different charge states with respect to a recent calculation.« less

Charge-state distribution of Li ions from the β decay of laser-trapped He 6 atoms

DOE PAGES

Hong, R.; Leredde, A.; Bagdasarova, Y.; ...

2017-11-13

The accurate determination of atomic final states following nuclear β decay plays an important role in several experiments. In particular, the charge state distributions of ions following nuclear β decay are important for determinations of the β-ν angular correlation with improved precision. Also, beyond the hydrogenic cases, the decay of neutral 6He presents the simplest case. Our measurement aims at providing benchmarks to test theoretical calculations. The kinematics of Li n+ ions produced following the β decay of 6He within an electric field were measured using 6He atoms in the metastable (1s2s, 3S 1) and (1s2p, 3P 2) states confinedmore » by a magneto-optical trap. The electron shakeoff probabilities were deduced, including their dependence on ion energy. Finally, we find significant discrepancies on the fractions of Li ions in the different charge states with respect to a recent calculation.« less

A Combined Theoretical and Experimental Study of Dissociation of Charge Transfer States at the Donor-Acceptor Interface of Organic Solar Cells.

PubMed

Tscheuschner, Steffen; Bässler, Heinz; Huber, Katja; Köhler, Anna

2015-08-13

The observation that in efficient organic solar cells almost all electron-hole pairs generated at the donor-acceptor interface escape from their mutual coulomb potential remains to be a conceptual challenge. It has been argued that it is the excess energy dissipated in the course of electron or hole transfer at the interface that assists this escape process. The current work demonstrates that this concept is unnecessary to explain the field dependence of electron-hole dissociation. It is based upon the formalism developed by Arkhipov and co-workers as well as Baranovskii and co-workers. The key idea is that the binding energy of the dissociating "cold" charge-transfer state is reduced by delocalization of the hole along the polymer chain, quantified in terms of an "effective mass", as well as the fractional strength of dipoles existent at the interface in the dark. By covering a broad parameter space, we determine the conditions for efficient electron-hole dissociation. Spectroscopy of the charge-transfer state on bilayer solar cells as well as measurements of the field dependence of the dissociation yield over a broad temperature range support the theoretical predictions.

Structural insight of the charge-ordering phenomena in manganites

NASA Astrophysics Data System (ADS)

Garcia, Joaquin

2005-03-01

Recent experiments using x-ray absorption spectroscopy (XAS) and x-ray resonant scattering (XRS) techniques show that the conventional description of the so-called charge ordering phases of manganites in terms of Mn^3+/Mn^4+ ionic ordering is far from reality. I present here the XRS study of the low temperature phase of Nd0.5Sr0.5MnO3 manganite. Strong resonances are observed in the energy dependent spectra of (300), (030) and (05/20) reflections. Their azimuthal and polarization dependencies are well explained by the anisotropy of the local geometrical structure. Two different Mn sites were found. One of them is surrounded by a tetragonal distorted oxygen octahedron, whereas the other site has a nearly regular octahedral environment. The charge separation between the intermediate valence states is less than 0.2 e-. The analysis performed resolves some of the apparent contradictions with previous XRS and XAS experiments in manganites. These results joined to those recently obtained on the Verwey transition in magnetite indicate that the electronic states in transition-metal oxides need to be described in terms of band states instead of localized ones. Colaborators: G. Sub'ias, J. Blasco, M. G. Proietti, M. S'anchez and J. Herrero-Martin

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

Mironov, Alexey Yu.; Silevitch, Daniel M.; Proslier, Thomas

Three decades after the prediction of charge-vortex duality in the critical vicinity of the two-dimensional superconductor-insulator transition (SIT), one of the fundamental implications of this duality-the charge Berezinskii-Kosterlitz-Thouless (BKT) transition that should occur on the insulating side of the SIT-has remained unobserved. The dual picture of the process points to the existence of a superinsulating state endowed with zero conductance at finite temperature. Here, we report the observation of the charge BKT transition on the insulating side of the SIT in 10 nm thick NbTiN films, identified by the BKT critical behavior of the temperature and magnetic field dependent resistance,more » and map out the magnetic-field dependence of the critical temperature of the charge BKT transition. Finally, we ascertain the effects of the finite electrostatic screening length and its divergence at the magnetic field-tuned approach to the superconductor-insulator transition.« less

Experimental exploration of the Mulliken-Hush relationship for intramolecular electron transfer reactions.

PubMed

Mukherjee, Tamal; Ito, Naoki; Gould, Ian R

2011-03-17

The Mulliken-Hush (M-H) relationship provides the critical link between optical and thermal electron transfer processes, and yet very little direct experimental support for its applicability has been provided. Dicyanovinylazaadamantane (DCVA) represents a simple two-state (neutral/charge-transfer) intramolecular electron transfer system that exhibits charge-transfer absorption and emission spectra that are readily measurable in solvents with a wide range of polarities. In this regard it represents an ideal model system for studying the factors that control both optical charge separation (absorption) and recombination (emission) processes in solution. Here we explore the applicability of the M-H relation to quantitative descriptions of the optical charge-transfer processes in DCVA. For DCVA, the measured radiative rate constants exhibit a linear dependence on transition energy, and transition dipole moments exhibit an inverse dependence on transition energy, consistent with the M-H relationship.

Charged anisotropic matter with linear or nonlinear equation of state

NASA Astrophysics Data System (ADS)

Varela, Victor; Rahaman, Farook; Ray, Saibal; Chakraborty, Koushik; Kalam, Mehedi

2010-08-01

Ivanov pointed out substantial analytical difficulties associated with self-gravitating, static, isotropic fluid spheres when pressure explicitly depends on matter density. Simplifications achieved with the introduction of electric charge were noticed as well. We deal with self-gravitating, charged, anisotropic fluids and get even more flexibility in solving the Einstein-Maxwell equations. In order to discuss analytical solutions we extend Krori and Barua’s method to include pressure anisotropy and linear or nonlinear equations of state. The field equations are reduced to a system of three algebraic equations for the anisotropic pressures as well as matter and electrostatic energy densities. Attention is paid to compact sources characterized by positive matter density and positive radial pressure. Arising solutions satisfy the energy conditions of general relativity. Spheres with vanishing net charge contain fluid elements with unbounded proper charge density located at the fluid-vacuum interface. Notably the electric force acting on these fluid elements is finite, although the acting electric field is zero. Net charges can be huge (1019C) and maximum electric field intensities are very large (1023-1024statvolt/cm) even in the case of zero net charge. Inward-directed fluid forces caused by pressure anisotropy may allow equilibrium configurations with larger net charges and electric field intensities than those found in studies of charged isotropic fluids. Links of these results with charged strange quark stars as well as models of dark matter including massive charged particles are highlighted. The van der Waals equation of state leading to matter densities constrained by cubic polynomial equations is briefly considered. The fundamental question of stability is left open.

Investigation of the charge-orbital ordering mechanism in single-layered Pr0.5Ca1.5MnO4

NASA Astrophysics Data System (ADS)

Rangkuti, C. N.; Majidi, M. A.

2018-04-01

Motivated by the experimental study of half-doped single-layered Pr0.5Ca1.5MnO4 showing charge, orbital, and spin orderings [1], we propose a model to theoretically study the system to explain such ordering phenomena. The ground state electron configuration reveals that the charges form a checkerboard pattern with alternating Mn3+/Mn4+ sites, while the orbitals are aligned in zigzag chains [1, 2]. We calculate the ground state energy of this system to find the most preferable configuration by comparing three types of configurations (charge-unordered, charge-ordered, and charge-orbital-ordered states). The calculations are based on a tight-binding model representing effective electron hoppings among Mn ions in MnO2-plane. We take into account the horizontally- and vertically-oriented orbital and spin degrees of freedom at Mn sites. We assume that the hopping integral values depend on the relative orientation between the corresponding orbitals of adjacent Mn ions. The interaction terms we incorporate into our effective Hamiltonian include inter-orbital, intra-orbital Hubbard repulsions, and Jahn-Teller distortion [2]. We absorb the exchange interaction between spins into local self-energy that we calculate within dynamical mean field algorithm [2]. Within our model we show a circumstance in which the charge-orbital ordered configuration has the lowest energy, consistent with the ground state ordering revealed by the experimental data.

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

PubMed

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.

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

NASA Astrophysics Data System (ADS)

Sukhomlinov, Sergey V.; Müser, Martin H.

2015-12-01

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, PC ≡ 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.

Integrative Approach with Electrophysiological and Theoretical Methods Reveals a New Role of S4 Positively Charged Residues in PKD2L1 Channel Voltage-Sensing.

PubMed

Numata, Tomohiro; Tsumoto, Kunichika; Yamada, Kazunori; Kurokawa, Tatsuki; Hirose, Shinichi; Nomura, Hideki; Kawano, Mitsuhiro; Kurachi, Yoshihisa; Inoue, Ryuji; Mori, Yasuo

2017-08-29

Numerical model-based simulations provide important insights into ion channel gating when experimental limitations exist. Here, a novel strategy combining numerical simulations with patch clamp experiments was used to investigate the net positive charges in the putative transmembrane segment 4 (S4) of the atypical, positively-shifted voltage-dependence of polycystic kidney disease 2-like 1 (PKD2L1) channel. Charge-neutralising mutations (K452Q, K455Q and K461Q) in S4 reduced gating charges, positively shifted the Boltzmann-type activation curve [i.e., open probability (P open )-V curve] and altered the time-courses of activation/deactivation of PKD2L1, indicating that this region constitutes part of a voltage sensor. Numerical reconstruction of wild-type (WT) and mutant PKD2L1-mediated currents necessitated, besides their voltage-dependent gating parameters, a scaling factor that describes the voltage-dependence of maximal conductance, G max . Subsequent single-channel conductance (γ) measurements revealed that voltage-dependence of G max in WT can be explained by the inward-rectifying property of γ, which is greatly changed in PKD2L1 mutants. Homology modelling based on PKD2 and Na V Ab structures suggest that such voltage dependence of P open and γ in PKD2L1 could both reflect the charged state of the S4 domain. The present conjunctive experimental and theoretical approaches provide a framework to explore the undetermined mechanism(s) regulating TRP channels that possess non-classical voltage-dependent properties.

Charge transfer fluorescence and 34 nm exciton diffusion length in polymers with electron acceptor end traps

DOE PAGES

Zaikowski, Lori; Mauro, Gina; Bird, Matthew; ...

2014-12-22

Photoexcitation of conjugated poly-2,7-(9,9-dihexylfluorene) polyfluorenes with naphthylimide (NI) and anthraquinone (AQ) electron-acceptor end traps produces excitons that form charge transfer states at the end traps. Intramolecular singlet exciton transport to end traps was examined by steady state fluorescence for polyfluorenes of 17 to 127 repeat units in chloroform, dimethylformamide (DMF), tetrahydrofuran (THF), and p-xylene. End traps capture excitons and form charge transfer (CT) states at all polymer lengths and in all solvents. The CT nature of the end-trapped states is confirmed by their fluorescence spectra, solvent and trap group dependence and DFT descriptions. Quantum yields of CT fluorescence are asmore » large as 46%. This strong CT emission is understood in terms of intensity borrowing. Energies of the CT states from onsets of the fluorescence spectra give the depths of the traps which vary with solvent polarity. For NI end traps the trap depths are 0.06 (p-xylene), 0.13 (THF) and 0.19 eV (CHCl 3). For AQ, CT fluorescence could be observed only in p-xylene where the trap depth is 0.27 eV. Quantum yields, emission energies, charge transfer energies, solvent reorganization and vibrational energies were calculated. Fluorescence measurements on chains >100 repeat units indicate that end traps capture ~50% of the excitons, and that the exciton diffusion length L D =34 nm, which is much larger than diffusion lengths reported in polymer films or than previously known for diffusion along isolated chains. As a result, the efficiency of exciton capture depends on chain length, but not on trap depth, solvent polarity or which trap group is present.« less

Resonant charge exchange for H-H+ in Debye plasmas

NASA Astrophysics Data System (ADS)

Laricchiuta, Annarita; Colonna, Gianpiero; Capitelli, Mario; Kosarim, Alexander; Smirnov, Boris M.

2017-11-01

The dynamics of resonant charge exchange in proton-hydrogen collisions embedded in plasma is investigated in the framework of the asymptotic approach, modified to account for the effect of Debye-Hückel screening in particle interactions. The cross sections exhibit a marked dependence on the Debye length in regimes of severe plasma confinement. Processes involving excited states H( n)-H+ are also discussed.

Dispersive electron transport in tris(8-hydroxyquinoline) aluminum (Alq3) probed by impedance spectroscopy.

PubMed

Berleb, Stefan; Brütting, Wolfgang

2002-12-31

Electron transport in tris(8-hydroxyquinoline) aluminum (Alq3) is investigated by impedance spectroscopy under conditions of space-charge limited conduction (SCLC). Existing SCLC models are extended to include the field dependence of the charge carrier mobility and energetically distributed trap states. The dispersive nature of electron transport is revealed by a frequency-dependent mobility with a dispersion parameter alpha in the range 0.4-0.5, independent of temperature. This indicates that positional rather than energetic disorder is the dominant mechanism for the dispersive transport of electrons in Alq3.

Multiple Gas-Phase Conformations of a Synthetic Linear Poly(acrylamide) Polymer Observed Using Ion Mobility-Mass Spectrometry.

PubMed

Haler, Jean R N; Far, Johann; Aqil, Abdelhafid; Claereboudt, Jan; Tomczyk, Nick; Giles, Kevin; Jérôme, Christine; De Pauw, Edwin

2017-11-01

Ion mobility-mass spectrometry (IM-MS) has emerged as a powerful separation and identification tool to characterize synthetic polymer mixtures and topologies (linear, cyclic, star-shaped,…). Electrospray coupled to IM-MS already revealed the coexistence of several charge state-dependent conformations for a single charge state of biomolecules with strong intramolecular interactions, even when limited resolving power IM-MS instruments were used. For synthetic polymers, the sample's polydispersity allows the observation of several chain lengths. A unique collision cross-section (CCS) trend is usually observed when increasing the degree of polymerization (DP) at constant charge state, allowing the deciphering of different polymer topologies. In this paper, we report multiple coexisting CCS trends when increasing the DP at constant charge state for linear poly(acrylamide) PAAm in the gas phase. This is similar to observations on peptides and proteins. Biomolecules show in addition population changes when collisionally heating the ions. In the case of synthetic PAAm, fragmentation occurred before reaching the energy for conformation conversion. These observations, which were made on two different IM-MS instruments (SYNAPT G2 HDMS and high resolution multi-pass cyclic T-Wave prototype from Waters), limit the use of ion mobility for synthetic polymer topology interpretations to polymers where unique CCS values are observed for each DP at constant charge state. Graphical Abstract ᅟ.

Multiple Gas-Phase Conformations of a Synthetic Linear Poly(acrylamide) Polymer Observed Using Ion Mobility-Mass Spectrometry

NASA Astrophysics Data System (ADS)

Haler, Jean R. N.; Far, Johann; Aqil, Abdelhafid; Claereboudt, Jan; Tomczyk, Nick; Giles, Kevin; Jérôme, Christine; De Pauw, Edwin

2017-08-01

Ion mobility-mass spectrometry (IM-MS) has emerged as a powerful separation and identification tool to characterize synthetic polymer mixtures and topologies (linear, cyclic, star-shaped,…). Electrospray coupled to IM-MS already revealed the coexistence of several charge state-dependent conformations for a single charge state of biomolecules with strong intramolecular interactions, even when limited resolving power IM-MS instruments were used. For synthetic polymers, the sample's polydispersity allows the observation of several chain lengths. A unique collision cross-section (CCS) trend is usually observed when increasing the degree of polymerization (DP) at constant charge state, allowing the deciphering of different polymer topologies. In this paper, we report multiple coexisting CCS trends when increasing the DP at constant charge state for linear poly(acrylamide) PAAm in the gas phase. This is similar to observations on peptides and proteins. Biomolecules show in addition population changes when collisionally heating the ions. In the case of synthetic PAAm, fragmentation occurred before reaching the energy for conformation conversion. These observations, which were made on two different IM-MS instruments (SYNAPT G2 HDMS and high resolution multi-pass cyclic T-Wave prototype from Waters), limit the use of ion mobility for synthetic polymer topology interpretations to polymers where unique CCS values are observed for each DP at constant charge state. [Figure not available: see fulltext.

Photoinduced intramolecular charge transfer (ICT) reaction in trans-methyl p-(dimethylamino) cinnamate: A combined fluorescence measurement and quantum chemical calculations

NASA Astrophysics Data System (ADS)

Chakraborty, Amrita; Kar, Samiran; Guchhait, Nikhil

2006-01-01

The photophysical behaviour of trans-methyl p-(dimethylamino) cinnamate ( t-MDMAC) donor-acceptor system has been investigated by steady-state absorption and emission spectroscopy and quantum chemical calculations. The molecule t-MDMAC shows an emission from the locally excited state in non-polar solvents. In addition to weak local emission, a strong solvent dependent red shifted fluorescence in polar aprotic solvents is attributed to highly polar intramolecular charge transfer state. However, the formation of hydrogen-bonded clusters with polar protic solvents has been suggested from a linear correlation between the observed red shifted fluorescence band maxima with hydrogen bonding parameters ( α). Calculations by ab initio and density functional theory show that the lone pair electron at nitrogen center is out of plane of the benzene ring in the global minimum ground state structure. In the gas phase, a potential energy surface along the twist coordinate at the donor (-NMe 2) and acceptor (-CH = CHCOOMe) sites shows stabilization of S 1 state and destabilization S 2 and S 0 states. A similar potential energy calculation along the twist coordinate in acetonitrile solvent using non-equilibrium polarized continuum model also shows more stabilization of S 1 state relative to other states and supports solvent dependent red shifted emission properties. In all types of calculations it is found that the nitrogen lone pair is delocalized over the benzene ring in the global minimum ground state and is localized on the nitrogen centre at the 90° twisted configuration. The S 1 energy state stabilization along the twist coordinate at the donor site and localized nitrogen lone pair at the perpendicular configuration support well the observed dual fluorescence in terms of proposed twisted intramolecular charge transfer (TICT) model.

Chemical bonding analysis on amphoteric hydrogen - alkaline earth ammine borohydrides

NASA Astrophysics Data System (ADS)

Kiruthika, S.; Ravindran, P.

2018-04-01

Usually the ions in solid are in the positive oxidation states or in the negative oxidation state depending upon the chemical environment. It is highly unusual for an ion having both positive as well as negative oxidation state in a particular compound. Structural analysis suggest that the alkaline earth ammine borohydrides (AABH) with the chemical formula M (BH4)2(NH3)2 (M = Mg, Ca, or Sr) where hydrogen is present in +1 and -1 oxidation states. In order to understand the oxidation states of hydrogen and also the character of chemical bond present in AABH we have made charge density, electron localization function, Born effective charge, Bader effective charge, and density of states analyses using result from the density functional calculations. Our detailed analyses show that hydrogen is in amphoteric behavior with hydrogen closer to boron is in negative oxidation state and that closer to nitrogen is in the positive oxidation state. Due to the presence of finite covalent bonding between the consitutents in AABH the oxidation state of hydrogen is non-interger value. The confirmation of the presence of amphtoric behavior of hydrogen in AABH has implication in hydrogen storage applications.

Surface Assisted Transient Displacement Charge Technique. II. Effect of Gases on Photoinduced Charge Transfer in Self-Assembled Monolayers

PubMed Central

Krasnoslobodtsev, Alexey V.; Smirnov, Sergei N.

2008-01-01

Surface assisted photoinduced transient displacement charge (SPTDC) technique was used to study charge transfer in self-assembled monolayers of 7-diethylaminocoumarin covalently linked to oxide surface in atmosphere of different gases. The dipole signal was found to be opposite to that in solution and dependent on the nature of gas and its pressure. The results were explained by collision-induced relaxation that impedes uninhibited tilting of molecules onto the surface. Collisions with paramagnetic oxygen induce intersystem crossing to long-lived triplet dipolar states of coumarin with the rate close to the half of that for the collision rate. PMID:16956285

INTERDISCIPLINARY PHYSICS AND RELATED AREAS OF SCIENCE AND TECHNOLOGY: Efficient One-Step Generation of Cluster State with Charge Qubits in Circuit QED

NASA Astrophysics Data System (ADS)

Wang, Yi-Min; Li, Cheng-Zu

2010-01-01

We propose theoretical schemes to generate highly entangled cluster state with superconducting qubits in a circuit QED architecture. Charge qubits are located inside a superconducting transmission line, which serves as a quantum data bus. We show that large clusters state can be efficiently generated in just one step with the long-range Ising-like unitary operators. The quantum operations which are generally realized by two coupling mechanisms: either voltage coupling or current coupling, depend only on global geometric features and are insensitive not only to the thermal state of the transmission line but also to certain random operation errors. Thus high-fidelity one-way quantum computation can be achieved.

Quasi-particle properties from tunneling in the v = 5/2 fractional quantum Hall state.

PubMed

Radu, Iuliana P; Miller, J B; Marcus, C M; Kastner, M A; Pfeiffer, L N; West, K W

2008-05-16

Quasi-particles with fractional charge and statistics, as well as modified Coulomb interactions, exist in a two-dimensional electron system in the fractional quantum Hall (FQH) regime. Theoretical models of the FQH state at filling fraction v = 5/2 make the further prediction that the wave function can encode the interchange of two quasi-particles, making this state relevant for topological quantum computing. We show that bias-dependent tunneling across a narrow constriction at v = 5/2 exhibits temperature scaling and, from fits to the theoretical scaling form, extract values for the effective charge and the interaction parameter of the quasi-particles. Ranges of values obtained are consistent with those predicted by certain models of the 5/2 state.

Kinetics of optically excited charge carriers at the GaN surface: Influence of catalytic Pt nanostructures

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

Winnerl, Andrea, E-mail: andrea.winnerl@wsi.tum.de; Pereira, Rui N.; Stutzmann, Martin

2015-10-21

In this work, we use GaN with different deposited Pt nanostructures as a controllable model system to investigate the kinetics of photo-generated charge carriers in hybrid photocatalysts. We combine conductance and contact potential difference measurements to investigate the influence of Pt on the processes involved in the capture and decay of photo-generated charge carriers at and close to the GaN surface. We found that in the presence of Pt nanostructures the photo-excitation processes are similar to those found in Pt free GaN. However, in GaN with Pt nanostructures, photo-generated holes are preferentially trapped in surface states of the GaN coveredmore » with Pt and/or in electronic states of the Pt and lead to an accumulation of positive charge there, whereas negative charge is accumulated in localized states in a shallow defect band of the GaN covered with Pt. This preferential accumulation of photo-generated electrons close to the surface is responsible for a dramatic acceleration of the turn-off charge transfer kinetics and a stronger dependence of the surface photovoltage on light intensity when compared to a Pt free GaN surface. Our study shows that in hybrid photocatalysts, the metal nanostructures induce a spatially inhomogeneous surface band bending of the semiconductor that promotes a lateral drift of photogenerated charges towards the catalytic nanostructures.« less

Crystallochromy of perylene pigments: Interference between Frenkel excitons and charge-transfer states

NASA Astrophysics Data System (ADS)

Gisslén, Linus; Scholz, Reinhard

2009-09-01

The optical properties of perylene-based pigments are arising from the interplay between neutral molecular excitations and charge transfer between adjacent molecules. In the crystalline phase, these excitations are coupled via electron and hole transfer, two quantities relating directly to the width of the conduction and valence band in the crystalline phase. Based on the crystal structure determined by x-ray diffraction, density-functional theory (DFT) and Hartree-Fock are used for the calculation of the electronic states of a dimer of stacked molecules. The resulting transfer parameters for electron and hole are used in an exciton model for the coupling between Frenkel excitons and charge-transfer states. The deformation of the positively or negatively charged molecular ions with respect to the neutral ground state is calculated with DFT and the geometry in the optically excited state is deduced from time-dependent DFT and constrained DFT. All of these deformations are interpreted in terms of the elongation of an effective internal vibration which is used subsequently in the exciton model for the crystalline phase. A comparison between the calculated dielectric function and the observed optical spectra allows to deduce the relative energetic position of Frenkel excitons and the charge-transfer state involving stack neighbors, a key parameter for various electronic and optoelectronic device applications. For five out of six perylene pigments studied in the present work, this exciton model results in excellent agreement between calculated and observed optical properties.

Synthesis and Photophysical Characterization of an Artificial Photosynthetic Reaction Center Exhibiting Acid-Responsive Regulation of Charge Separation

NASA Astrophysics Data System (ADS)

Pahk, Ian

Non-photochemical quenching (NPQ) is a photoprotective regulatory mechanism essential to the robustness of the photosynthetic apparatus of green plants. Energy flow within the low-light adapted reaction centers is dynamically optimized to match the continuously fluctuating light conditions found in nature. Activated by compartmentalized decreases in pH resulting from photosynthetic activity during periods of elevated photon flux, NPQ induces rapid thermal dissipation of excess excitation energy that would otherwise overwhelm the apparatus's ability to consume it. Consequently, the frequency of charge separation decreases and the formation of potentially deleterious, high-energy intermediates slows, thereby reducing the threat of photodamage by disallowing their accumulation. Herein is described the synthesis and photophysical analysis of a molecular triad that mimics the effects of NPQ on charge separation within the photosynthetic reaction centers. Steady-state absorption and emission, time-resolved fluorescence, and transient absorption spectroscopies were used to demonstrate reversible quenching of the first singlet excited state affecting the quantum yield of charge separation by approximately one order of magnitude. As in the natural system, the populations of unquenched and quenched states and, therefore, the overall yields of charge separation were found to be dependent upon acid concentration.

Search for doubly charged Higgs bosons in like-sign dilepton final states at √s¯= 7 TeV with the ATLAS detector

DOE PAGES

Aad, G.

2012-12-04

A search for doubly-charged Higgs bosons decaying to pairs of electrons and/or muons is presented. The search is performed using a data sample corresponding to an integrated luminosity of 4.7 fb -1 of pp collisions at √s¯ = 7 TeV collected by the ATLAS detector at the LHC. Pairs of prompt, isolated, high-p T leptons with the same electric charge (e ±e ±, e ±μ ±, μ ±μ ±) are selected, and their invariant mass distribution is searched for a narrow resonance. No significant excess over Standard Model background expectations is observed, and limits are placed on the cross sectionmore » times branching ratio for pair production of doubly-charged Higgs bosons. The masses of doubly-charged Higgs bosons are constrained depending on the branching ratio into these leptonic final states. Assuming pair production, coupling to left-handed fermions, and a branching ratio of 100% for each final state, masses below 409 GeV, 375 GeV, and 398 GeV are excluded for e ±e ±, e ±μ ±, and μ ±μ ±, respectively.« less

Charge and pairing dynamics in the attractive Hubbard model: Mode coupling and the validity of linear-response theory

NASA Astrophysics Data System (ADS)

Bünemann, Jörg; Seibold, Götz

2017-12-01

Pump-probe experiments have turned out as a powerful tool in order to study the dynamics of competing orders in a large variety of materials. The corresponding analysis of the data often relies on standard linear-response theory generalized to nonequilibrium situations. Here we examine the validity of such an approach for the charge and pairing response of systems with charge-density wave and (or) superconducting (SC) order. Our investigations are based on the attractive Hubbard model which we study within the time-dependent Hartree-Fock approximation. In particular, we calculate the quench and pump-probe dynamics for SC and charge order parameters in order to analyze the frequency spectra and the coupling of the probe field to the specific excitations. Our calculations reveal that the "linear-response assumption" is justified for small to moderate nonequilibrium situations (i.e., pump pulses) in the case of a purely charge-ordered ground state. However, the pump-probe dynamics on top of a superconducting ground state is determined by phase and amplitude modes which get coupled far from the equilibrium state indicating the failure of the linear-response assumption.

Spin polarized and density modulated phases in symmetric electron-electron and electron-hole bilayers.

PubMed

Kumar, Krishan; Moudgil, R K

2012-10-17

We have studied symmetric electron-electron and electron-hole bilayers to explore the stable homogeneous spin phase and the feasibility of inhomogeneous charge-/spin-density ground states. The former is resolved by comparing the ground-state energies in states of different spin polarizations, while the latter is resolved by searching for a divergence in the wavevector-dependent static charge/spin susceptibility. For this endeavour, we have used the dielectric approach within the self-consistent mean-field theory of Singwi et al. We find that the inter-layer interactions tend to change an abrupt spin-polarization transition of an isolated layer into a nearly gradual one, even though the partially spin-polarized phases are not clearly stable within the accuracy of our calculation. The transition density is seen to decrease with a reduction in layer spacing, implying a suppression of spin polarization by inter-layer interactions. Indeed, the suppression shows up distinctly in the spin susceptibility computed from the spin-polarization dependence of the ground-state energy. However, below a critical layer spacing, the unpolarized liquid becomes unstable against a charge-density-wave (CDW) ground state at a density preceding full spin polarization, with the transition density for the CDW state increasing on further reduction in the layer spacing. Due to attractive e-h correlations, the CDW state is found to be more pronounced in the e-h bilayer. On the other hand, the static spin susceptibility diverges only in the long-wavelength limit, which simply represents a transition to the homogeneous spin-polarized phase.

Pre-Steady-State Kinetics of Ba-Ca Exchange Reveals a Second Electrogenic Step Involved in Ca2+ Translocation by the Na-Ca Exchanger

PubMed Central

Haase, Andreas; Hartung, Klaus

2009-01-01

Kinetic properties of the Na-Ca exchanger (guinea pig NCX1) expressed in Xenopus oocytes were investigated with excised membrane patches in the inside-out configuration and photolytic Ca2+ concentration jumps with either 5 mM extracellular Sr2+ or Ba2+. After a Ca2+ concentration jump on the cytoplasmic side, the exchanger performed Sr-Ca or Ba-Ca exchange. In the Sr-Ca mode, currents are transient and decay in a monoexponential manner similar to that of currents in the Ca-Ca exchange mode described before. Currents recorded in the Ba-Ca mode are also transient, but the decay is biphasic. In the Sr-Ca mode the amount of charge translocated increases at negative potentials in agreement with experiments performed in the Ca-Ca mode. In the Ba-Ca mode the total amount of charge translocated after a Ca2+ concentration jump is ∼4 to 5 times that in Ca-Ca or Sr-Ca mode. In the Ba-Ca mode the voltage dependence of charge translocation depends on the Ca2+ concentration on the cytosolic side before the Ca2+ concentration jump. At low initial Ca2+ levels (∼0.5 μM), charge translocation is voltage independent. At a higher initial concentration (1 μM Ca2+), the amount of charge translocated increases at positive potentials. Biphasic relaxation of the current was also observed in the Ca-Ca mode if the external Ca2+ concentration was reduced to ≤0.5 mM. The results reported here and in previous publications can be described by using a 6-state model with two voltage-dependent conformational transitions. PMID:19486679

Microtubules as mechanical force sensors.

PubMed

Karafyllidis, Ioannis G; Lagoudas, Dimitris C

2007-03-01

Microtubules are polymers of tubulin subunits (dimers) arranged on a hexagonal lattice. Each tubulin dimer comprises two monomers, the alpha-tubulin and beta-tubulin, and can be found in two states. In the first state a mobile negative charge is located into the alpha-tubulin monomer and in the second into the beta-tubulin monomer. Each tubulin dimer is modeled as an electrical dipole coupled to its neighbors by electrostatic forces. The location of the mobile charge in each dimer depends on the location of the charges in the dimer's neighborhood. Mechanical forces that act on the microtubule affect the distances between the dimers and alter the electrostatic potential. Changes in this potential affect the mobile negative charge location in each dimer and the charge distribution in the microtubule. The net effect is that mechanical forces affect the charge distribution in microtubules. We propose to exploit this effect and use microtubules as mechanical force sensors. We model each dimer as a two-state quantum system and, following the quantum computation paradigm, we use discrete quantum random walk on the hexagonal microtubule lattice to determine the charge distribution. Different forces applied on the microtubule are modeled as different coin biases leading to different probability distributions of the quantum walker location, which are directly connected to different charge distributions. Simulation results show that there is a strong indication that microtubules can be used as mechanical force sensors and that they can also detect the force directions and magnitudes.

Out-of-equilibrium spin transport in mesoscopic superconductors.

PubMed

Quay, C H L; Aprili, M

2018-08-06

The excitations in conventional superconductors, Bogoliubov quasi-particles, are spin-[Formula: see text] fermions but their charge is energy-dependent and, in fact, zero at the gap edge. Therefore, in superconductors (unlike normal metals) spin and charge degrees of freedom may be separated. In this article, we review spin injection into conventional superconductors and focus on recent experiments on mesoscopic superconductors. We show how quasi-particle spin transport and out-of-equilibrium spin-dependent superconductivity can be triggered using the Zeeman splitting of the quasi-particle density of states in thin-film superconductors with small spin-mixing scattering. Finally, we address the spin dynamics and the feedback of quasi-particle spin imbalances on the amplitude of the superconducting energy gap.This article is part of the theme issue 'Andreev bound states'. © 2018 The Author(s).

Ab initio modeling of steady-state and time-dependent charge transport in hole-only α-NPD devices

NASA Astrophysics Data System (ADS)

Liu, Feilong; Massé, Andrea; Friederich, Pascal; Symalla, Franz; Nitsche, Robert; Wenzel, Wolfgang; Coehoorn, Reinder; Bobbert, Peter A.

2016-12-01

We present an ab initio modeling study of steady-state and time-dependent charge transport in hole-only devices of the amorphous molecular semiconductor α-NPD [N ,N'-Di(1 -naphthyl)-N ,N'-diphenyl-(1 ,1'-biphenyl)-4 ,4'-diamine] . The study is based on the microscopic information obtained from atomistic simulations of the morphology and density functional theory calculations of the molecular hole energies, reorganization energies, and transfer integrals. Using stochastic approaches, the microscopic information obtained in simulation boxes at a length scale of ˜10 nm is expanded and employed in one-dimensional (1D) and three-dimensional (3D) master-equation modeling of the charge transport at the device scale of ˜100 nm. Without any fit parameter, predicted current density-voltage and impedance spectroscopy data obtained with the 3D modeling are in very good agreement with measured data on devices with different α-NPD layer thicknesses in a wide range of temperatures, bias voltages, and frequencies. Similarly good results are obtained with the computationally much more efficient 1D modeling after optimizing a hopping prefactor.

Probing charge transfer complex states in organic solar cells using photocurrent spectroscopy

NASA Astrophysics Data System (ADS)

Moghe, Dhanashree; Adil, Danish; Kanimozhi, Catherine; Dutta, Gitesh; Patil, Satish; Guha, Suchismita

2013-03-01

Diketopyrrolopyrrole (DPP) containing copolymers-fullerene blends have gained a lot of interest in organic optoelectronics with a great potential in organic photovoltaics (OPVs). The interfacial charge transfer complex (CTC) states formed in donor-acceptor blended OPVs play a major role in the overall efficiency of the device. We investigate the spectral photocurrent characteristics of five DPP based copolymers; two of them being benzothiadiazole and carbazole -based statistical copolymers of DPP. These systems provide a wide range of bandgap energies ranging from ~ 1.4 to 1.7 eV. We use Fourier transform photocurrent spectroscopy (FTPS) and monochromatic photocurrent (PC) to identify the CTC states in these DPP copolymer -fullerene blends. The stability of the CTC state is found to be dependent on the band gap energy difference between the donor copolymer and the acceptor. We support our inferences from theoretical results obtained using density-functional theory (DFT) and time-dependent DFT for two DPP based copolymers The theoretical calculations reveal a higher contribution of the CTC states to the lowest excited state in the phenyl-based DPP monomer, which has a larger bandgap energy compared to the thiophene-based DPP system, in the presence of a fullerene molecule.

Modulation of Molecular Flux Using a Graphene Nanopore Capacitor.

PubMed

Shankla, Manish; Aksimentiev, Aleksei

2017-04-20

Modulation of ionic current flowing through nanoscale pores is one of the fundamental biological processes. Inspired by nature, nanopores in synthetic solid-state membranes are being developed to enable rapid analysis of biological macromolecules and to serve as elements of nanofludic circuits. Here, we theoretically investigate ion and water transport through a graphene-insulator-graphene membrane containing a single, electrolyte-filled nanopore. By means of all-atom molecular dynamics simulations, we show that the charge state of such a graphene nanopore capacitor can regulate both the selectivity and the magnitude of the nanopore ionic current. At a fixed transmembrane bias, the ionic current can be switched from being carried by an equal mixture of cations and anions to being carried almost exclusively by either cationic or anionic species, depending on the sign of the charge assigned to both plates of the capacitor. Assigning the plates of the capacitor opposite sign charges can either increase the nanopore current or reduce it substantially, depending on the polarity of the bias driving the transmembrane current. Facilitated by the changes of the nanopore surface charge, such ionic current modulations are found to occur despite the physical dimensions of the nanopore being an order of magnitude larger than the screening length of the electrolyte. The ionic current rectification is accompanied by a pronounced electro-osmotic effect that can transport neutral molecules such as proteins and drugs across the solid-state membrane and thereby serve as an interface between electronic and chemical signals.

A negative charge in transmembrane segment 1 of domain II of the cockroach sodium channel is critical for channel gating and action of pyrethroid insecticides

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

Du Yuzhe; Song Weizhong; Groome, James R.

2010-08-15

Voltage-gated sodium channels are the primary target of pyrethroids, an important class of synthetic insecticides. Pyrethroids bind to a distinct receptor site on sodium channels and prolong the open state by inhibiting channel deactivation and inactivation. Recent studies have begun to reveal sodium channel residues important for pyrethroid binding. However, how pyrethroid binding leads to inhibition of sodium channel deactivation and inactivation remains elusive. In this study, we show that a negatively charged aspartic acid residue at position 802 (D802) located in the extracellular end of transmembrane segment 1 of domain II (IIS1) is critical for both the action ofmore » pyrethroids and the voltage dependence of channel activation. Charge-reversing or -neutralizing substitutions (K, G, or A) of D802 shifted the voltage dependence of activation in the depolarizing direction and reduced channel sensitivity to deltamethrin, a pyrethroid insecticide. The charge-reversing mutation D802K also accelerated open-state deactivation, which may have counteracted the inhibition of sodium channel deactivation by deltamethrin. In contrast, the D802G substitution slowed open-state deactivation, suggesting an additional mechanism for neutralizing the action of deltamethrin. Importantly, Schild analysis showed that D802 is not involved in pyrethroid binding. Thus, we have identified a sodium channel residue that is critical for regulating the action of pyrethroids on the sodium channel without affecting the receptor site of pyrethroids.« less

Multi-temperature state-dependent equivalent circuit discharge model for lithium-sulfur batteries

NASA Astrophysics Data System (ADS)

Propp, Karsten; Marinescu, Monica; Auger, Daniel J.; O'Neill, Laura; Fotouhi, Abbas; Somasundaram, Karthik; Offer, Gregory J.; Minton, Geraint; Longo, Stefano; Wild, Mark; Knap, Vaclav

2016-10-01

Lithium-sulfur (Li-S) batteries are described extensively in the literature, but existing computational models aimed at scientific understanding are too complex for use in applications such as battery management. Computationally simple models are vital for exploitation. This paper proposes a non-linear state-of-charge dependent Li-S equivalent circuit network (ECN) model for a Li-S cell under discharge. Li-S batteries are fundamentally different to Li-ion batteries, and require chemistry-specific models. A new Li-S model is obtained using a 'behavioural' interpretation of the ECN model; as Li-S exhibits a 'steep' open-circuit voltage (OCV) profile at high states-of-charge, identification methods are designed to take into account OCV changes during current pulses. The prediction-error minimization technique is used. The model is parameterized from laboratory experiments using a mixed-size current pulse profile at four temperatures from 10 °C to 50 °C, giving linearized ECN parameters for a range of states-of-charge, currents and temperatures. These are used to create a nonlinear polynomial-based battery model suitable for use in a battery management system. When the model is used to predict the behaviour of a validation data set representing an automotive NEDC driving cycle, the terminal voltage predictions are judged accurate with a root mean square error of 32 mV.

Fundamental studies on the metal chloride cathodes in sodium batteries

NASA Technical Reports Server (NTRS)

Ratnakumar, B. V.; Attia, A.; Halpert, G.

1990-01-01

The authors report studies of the passivation of the NiCl2 electrode during reduction, its effect on the electrochemical rate kinetics for the reduction, and its dependence on the state of charge of the electrode. NiCl2 exhibits passive behavior more readily at lower states of charge due to a decrease in the electrochemical area, resulting from NaCl deposited during reduction. The passive behavior is evident from the DC polarization curves as well as AC impedance plots at the same potentials, implying a correlation between them. The results of the studies are presented in detail.

Characterisation of retention properties of charge-trapping memory cells at low temperatures

NASA Astrophysics Data System (ADS)

Yurchuk, E.; Bollmann, J.; Mikolajick, T.

2009-09-01

The density of states of deep level centers in silicon oxynitride layer of SONOS memory cells are calculated from temperature dependent retention measurement. The dominating charge loss mechanisms are direct trap-to-band tunneling (TB) and thermally stimulated emission (TE). Retention measurements at low temperatures (80 - 300K) will be dominated by TE from more "shallow" traps with energies below 1eV and by TB. Taking into account both independent and rival processes the density of states could be calculated self consisting. The results are in excellent agreement with elsewhere published data.

Melting of Domain Wall in Charge Ordered Dirac Electron of Organic Conductor α-(BEDT-TTF)2I3

NASA Astrophysics Data System (ADS)

Ohki, Daigo; Matsuno, Genki; Omori, Yukiko; Kobayashi, Akito

2018-05-01

The origin of charge order melting is identified by using the real space dependent mean-field theory in the extended Hubbard model describing an organic Dirac electron system α-(BEDT-TTF)2I3. In this model, the width of a domain wall which arises between different types of the charge ordered phase exhibits a divergent increase with decreasing the strength of electron-electron correlations. By analyzing the finite-size effect carefully, it is shown that the divergence coincides with a topological transition where a pair of Dirac cones merges in keeping with a finite gap. It is also clarified that the gap opening point and the topological transition point are different, which leads to the existence of an exotic massive Dirac electron phase with melted-type domain wall and gapless edge states. The present result also indicated that multiple metastable states are emerged in massive Dirac Electron phase. In the trivial charge ordered phase, the gapless domain-wall bound state takes place instead of the gapless edge states, accompanying with a form change of the domain wall from melted-type into hyperbolic-tangent-type.

A model Ni-Al-Mo superalloy studied by ultraviolet pulsed-laser-assisted local-electrode atom-probe tomography.

PubMed

Tu, Yiyou; Plotnikov, Elizaveta Y; Seidman, David N

2015-04-01

This study investigates the effects of the charge-state ratio of evaporated ions on the accuracy of local-electrode atom-probe (LEAP) tomographic compositional and structural analyses, which employs a picosecond ultraviolet pulsed laser. Experimental results demonstrate that the charge-state ratio is a better indicator of the best atom-probe tomography (APT) experimental conditions compared with laser pulse energy. The thermal tails in the mass spectra decrease significantly, and the mass resolving power (m/Δm) increases by 87.5 and 185.7% at full-width half-maximum and full-width tenth-maximum, respectively, as the laser pulse energy is increased from 5 to 30 pJ/pulse. The measured composition of this alloy depends on the charge-state ratio of the evaporated ions, and the most accurate composition is obtained when Ni2+/Ni+ is in the range of 0.3-20. The γ(f.c.c.)/γ'(L12) interface is quantitatively more diffuse when determined from the measured concentration profiles for higher laser pulse energies. Conclusions of the APT compositional and structural analyses utilizing the same suitable charge-state ratio are more comparable than those collected with the same laser pulse energy.

Understanding the influence of solvent field and fluctuations on the stability of photo-induced charge-separated state in molecular triad

NASA Astrophysics Data System (ADS)

Balamurugan, D.; Aquino, Adelia; Lischka, Hans; Dios, Francis; Flores, Lionel; Cheung, Margaret

2013-03-01

Molecular triad composed of fullerene, porphyrin, and carotene is an artificial analogue of natural photosynthetic system and is considered for applications in solar energy conversion because of its ability to produce long-lived photo-induced charge separated state. The goal of the present multiscale simulation is to understand how the stability of photo-induced charge-separated state in molecular triad is influenced by a polar organic solvent, namely tetrahydrofuran (THF). The multiscale approach is based on combined quantum, classical molecular dynamics, and statistical physics calculations. The quantum chemical calculations were performed on the triad using the second order algebraic diagrammatic perturbation and time-dependent density functional theory. Molecular dynamics simulations were performed on triad in a box of THF solvent with the replica exchange method. The two methods on different length and time scales are bridged through an important sampling technique. We have analyzed the free energy landscape, structural fluctuations, and the long- range electrostatic interactions between triad and solvent molecules. The results suggest that the polarity and re-organization of the solvent is critical in stabilization of charge-separated state in triad. Supported by DOE (DE-FG02-10ER16175)

Dot size effects of nanocrystalline germanium on charging dynamics of memory devices

PubMed Central

2013-01-01

The dot size of nanocrystalline germanium (NC Ge) which impacts on the charging dynamics of memory devices has been theoretically investigated. The calculations demonstrate that the charge stored in the NC Ge layer and the charging current at a given oxide voltage depend on the dot size especially on a few nanometers. They have also been found to obey the tendency of initial increase, then saturation, and lastly, decrease with increasing dot size at any given charging time, which is caused by a compromise between the effects of the lowest conduction states and the capacitance of NC Ge layer on the tunneling. The experimental data from literature have also been used to compare and validate the theoretical analysis. PMID:23305228

Adding high time resolution to charge-state-specific ion energy measurements for pulsed copper vacuum arc plasmas

NASA Astrophysics Data System (ADS)

Tanaka, Koichi; Han, Liang; Zhou, Xue; Anders, André

2015-08-01

Charge-state-resolved ion energy-time distributions of pulsed Cu arc plasma were obtained by using direct (time-dependent) acquisition of the ion detection signal from a commercial ion mass-per-charge and energy-per-charge analyzer. We find a shift of energies of Cu2+, Cu3+ and Cu4+ ions to lower values during the first few hundred microseconds after arc ignition, which is evidence for particle collisions in the plasma. The generation of Cu+ ions in the later part of the pulse, measured by the increase of Cu+ signal intensity and an associated slight reduction of the mean charge state, points to charge exchange reactions between ions and neutrals. At the very beginning of the pulse, when the plasma expands into vacuum and the plasma potential strongly fluctuates, ions with much higher energy (over 200 eV) are observed. Early in the pulse, the ion energies observed are approximately proportional to the ion charge state, and we conclude that the acceleration mechanism is primarily based on acceleration in an electric field. This field is directed away from the cathode, indicative of a potential hump. Measurements by a floating probe suggest that potential structures travel, and ions moving in the traveling field can gain high energies up to a few hundred electron-volts. Later in the pulse, the approximate proportionality is lost, which is related to increased smearing out of different energies due to collisions with neutrals, and/or to a change of the acceleration character from electrostatic to ‘gas-dynamic’, i.e. dominated by pressure gradient.

Structural origins of pH and ionic strength effects on protein stability. Acid denaturation of sperm whale apomyoglobin.

PubMed

Yang, A S; Honig, B

1994-04-15

A recently developed approach to calculate the pH dependence of protein stability from three-dimensional structure information is applied to the analysis of acid denaturation of sperm whale apomyoglobin. The finite difference Poisson-Boltzmann method is used to calculate pKa values and these are used to obtain titration curves for the folded protein as well as for compact intermediates. The total electrostatic free energy change involved in apomyoglobin unfolding is then evaluated. Calculations are carried out of the unfolding free energy of the native (N) and the compact intermediate (I) of apomyoglobin relative to the unfolded state (U) over a range of pH at various ionic strengths. The contributions from key ionizable groups to the unfolding process are discussed. For the acid-induced partial unfolding of apomyoglobin near pH 5, the transition from N to I is found to be driven by three histidines that are exposed when the B, C, D and E helices unfold. Similarly, the unfolding of the compact intermediate I consisting of the A, G and H helices is driven primarily by a few carboxylic acids with low pKa values in the compact state. This picture is in contrast to the view which attributes acid denaturation to electrostatic repulsion resulting from the build up of positive charge. In fact, charge-charge interactions in myoglobin are found to be attractive at all pH values where the protein unfolds. pH-dependent changes in these interactions contribute to acid denaturation but other electrostatic effects, such as hydrogen bonding and solvation, are important as well. The effect of increasing ionic strength on unfolding is attributed to the decrease of attractive charge-charge interactions which destabilize the N state relative to I, but stabilize the I state relative to U by reducing the pKa shifts of a few critical carboxylic acids. The I state is found to be more stable than U at neutral pH thus accounting for its presence as an intermediate on the protein folding pathway. Our results have implications for the origins of compact intermediates or "molten globule" states.

Direct Measurement of Nuclear Dependence of Charged Current Quasielasticlike Neutrino Interactions Using MINERvA

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

Betancourt, M.; Ghosh, A.; Walton, T.

Charged-current νμ interactions on carbon, iron, and lead with a final state hadronic system of one or more protons with zero mesons are used to investigate the influence of the nuclear environment on quasielasticlike interactions. The transferred four-momentum squared to the target nucleus, Q2, is reconstructed based on the kinematics of the leading proton, and differential cross sections versus Q2 and the cross-section ratios of iron, lead, and carbon to scintillator are measured for the first time in a single experiment. The measurements show a dependence on the atomic number. While the quasielasticlike scattering on carbon is compatible with predictions,more » the trends exhibited by scattering on iron and lead favor a prediction with intranuclear rescattering of hadrons accounted for by a conventional particle cascade treatment. These measurements help discriminate between different models of both initial state nucleons and final state interactions used in the neutrino oscillation experiments.« less

Negatively charged excitons and photoluminescence in asymmetric quantum wells

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

Szlufarska, Izabela; Wojs, Arkadiusz; Quinn, John J.

2001-02-15

We study photoluminescence (PL) of charged excitons (X{sup -}) in narrow asymmetric quantum wells in high magnetic fields B. The binding of all X{sup -} states strongly depends on the separation {delta} of electron and hole layers. The most sensitive is the ''bright'' singlet, whose binding energy decreases quickly with increasing {delta} even at relatively small B. As a result, the value of B at which the singlet-triplet crossing occurs in the X{sup -} spectrum also depends on {delta}, and decreases from 35 T in a symmetric 10 nm GaAs well to 16 T for {delta}=0.5 nm. Since the criticalmore » values of {delta} at which different X{sup -} states unbind are surprisingly small compared to the well width, the observation of strongly bound X{sup -} states in an experimental PL spectrum implies virtually no layer displacement in the sample. This casts doubt on the interpretation of PL spectra of heterojunctions in terms of X{sup -} recombination.« less

High open-circuit voltage small-molecule p-DTS(FBTTh 2 ) 2.ICBA bulk heterojunction solar cells – morphology, excited-state dynamics, and photovoltaic performance

DOE PAGES

Ko Kyaw, Aung Ko; Gehrig, Dominik; Zhang, Jie; ...

2014-11-27

The photovoltaic performance of bulk heterojunction solar cells using the solution-processable small molecule donor 7,7'-(4,4-bis(2-ethylhexyl)-4H-silolo[3,2-b:4,5-b']dithiophene-2,6-diyl)bis(6-fluoro-4-(5'-hexyl-[2,2'-bithiophene]-5-yl)benzo[c][1,2,5]thiadiazole) (p-DTS(FBTTh 2) 2 in combination with indene-C60 bis-adduct (ICBA) as an acceptor is systematically optimized by altering the processing conditions. A high open-circuit voltage of 1 V, more than 0.2 V higher than that of a p-DTS(FBTTh 2) 2:PC 70BM blend, is achieved. However, the power conversion efficiency remains around 5% and thus is lower than ~8% previously reported for p-DTS(FBTTh 2) 2:PC 70BM. Transient absorption (TA) pump–probe spectroscopy over a wide spectral (Vis-NIR) and dynamic (fs to μs) range in combination with multivariate curvemore » resolution analysis of the TA data reveals that generation of free charges is more efficient in the blend with PC 70BM as an acceptor. In contrast, blends with ICBA create more coulombically bound interfacial charge transfer (CT) states, which recombine on the sub-nanosecond timescale by geminate recombination. Furthermore, the ns to μs charge carrier dynamics in p-DTS(FBTTh 2) 2:ICBA blends are only weakly intensity dependent implying a significant contribution of recombination from long-lived CT states and trapped charges, while those in p-DTS(FBTTh 2) 2:PC 70BM decay via an intensity-dependent recombination mechanism indicating that spatially separated (free) charge carriers are observed, which can be extracted as photocurrent from the device.« less

Exciton shelves for charge and energy transport in third-generation quantum-dot devices

NASA Astrophysics Data System (ADS)

Goodman, Samuel; Singh, Vivek; Noh, Hyunwoo; Casamada, Josep; Chatterjee, Anushree; Cha, Jennifer; Nagpal, Prashant

2014-03-01

Quantum dots are semiconductor nanocrystallites with size-dependent quantum-confined energy levels. While they have been intensively investigated to utilize hot-carriers for photovoltaic applications, to bridge the mismatch between incident solar photons and finite bandgap of semiconductor photocells, efficient charge or exciton transport in quantum-dot films has proven challenging. Here we show development of new coupled conjugated molecular wires with ``exciton shelves'', or different energy levels, matched with the multiple energy levels of quantum dots. Using single nanoparticle and ensemble device measurements we show successful extraction and transport of both bandedge and high-energy charge carriers, and energy transport of excitons. We demonstrate using measurements of electronic density of states, that careful matching of energy states of quantum-dot with molecular wires is important, and any mismatch can generate midgap states leading to charge recombination and reduced efficiency. Therefore, these exciton-shelves and quantum dots can lead to development of next-generation photovoltaic and photodetection devices using simultaneous transport of bandedge and hot-carriers or energy transport of excitons in these nanostructured solution-processed films.

The low-lying {pi}{sigma}* state and its role in the intramolecular charge transfer of aminobenzonitriles and aminobenzethyne

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

Lee, Jae-Kwang; Fujiwara, Takashige; Kofron, William G.

2008-04-28

Electronic absorption spectra of the low-lying {pi}{pi}* and {pi}{sigma}* states of several aminobenzonitriles and 4-dimethylaminobenzethyne have been studied by time-resolved transient absorption and time-dependent density functional theory calculation. In acetonitrile, the lifetime of the {pi}{sigma}*-state absorption is very short (picoseconds or subpicosecond) for molecules that exhibit intramolecular charge transfer (ICT), and very long (nanoseconds) for those that do not. Where direct comparison of the temporal characteristics of the {pi}{sigma}*-state and the ICT-state transients could be made, the formation rate of the ICT state is identical to the decay rate of the {pi}{sigma}* state within the experimental uncertainty. These results aremore » consistent with the {pi}{sigma}*-mediated ICT mechanism, L{sub a} ({pi}{pi}*){yields}{pi}{sigma}*{yields}ICT, in which the decay rate of the {pi}{sigma}* state is determined by the rate of the solvent-controlled {pi}{sigma}*{yields}ICT charge-shift reaction. The {pi}{pi}*{yields}{pi}{sigma}* state crossing does not occur in 3-dimethylaminobenzonitrile or 2-dimethylaminobenzonitrile, as predicted by the calculation, and 4-aminobenzonitrile and 4-dimethylaminobenzethyne does not exhibit the ICT reaction, consistent with the higher energy of the ICT state relative to the {pi}{sigma}* state.« less

Femtosecond-picosecond laser photolysis studies on the dynamics of excited charge-transfer complexes: Aromatic hydrocarbon-acid anhydride, -tetracyanoethylene, and -tetracyanoquinodimethane systems in acetonitrile solutions

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

Asahi, Tsuyoshi; Mataga, Noboru

1991-03-07

Formation processes of contact ion pairs (CIP) from the excited Franck-Condon (FC) state of charge-transfer (CT) complexes of aromatic hydrocarbons with acid anhydride as well as cyano compound acceptors in acetonitrile solution and charge recombination (CR) rates (k{sub CR}{sup CIP}) of produced CIP states have been investigated by femtosecond and picosecond laser phototlysis and time-resolved absorption spectral measurements covering a wide range of free energy gap-{Delta}G{degree}{sub ip} between the ion pair and the ground state. It has been confirmed that the CIP formation becomes faster and k{sub CR}{sup CIP} of the produced CIP increases with increase of the strengths ofmore » the electron donor (D) and acceptor (A) in the complex, i.e., with decrease of the {minus}{Delta}G{degree}{sub ip} value. This peculiar energy gap dependence of k{sub CR}{sup CIP}, quite different from the bell-shaped one observed in the case of the solvent-separated ion pairs (SSIP) or loose ion pairs (LIP) formed by encounter between fluorescer and quencher in the fluoresence quenching reaction, has been interpreted by assuming the change of electronic and geometrical structures of CIP depending on the strengths of D and A.« less

Study of the dependence of direct soft photon production on the jet characteristics in hadronic Z 0 decays

NASA Astrophysics Data System (ADS)

Abdallah, J.; Abreu, P.; Adam, W.; Adzic, P.; Albrecht, T.; Alemany-Fernandez, R.; Allmendinger, T.; Allport, P. P.; Amaldi, U.; Amapane, N.; Amato, S.; Anashkin, E.; Andreazza, A.; Andringa, S.; Anjos, N.; Antilogus, P.; Apel, W.-D.; Arnoud, Y.; Ask, S.; Asman, B.; Augustin, J. E.; Augustinus, A.; Baillon, P.; Ballestrero, A.; Bambade, P.; Barbier, R.; Bardin, D.; Barker, G. J.; Baroncelli, A.; Battaglia, M.; Baubillier, M.; Becks, K.-H.; Begalli, M.; Behrmann, A.; Ben-Haim, E.; Benekos, N.; Benvenuti, A.; Berat, C.; Berggren, M.; Bertrand, D.; Besancon, M.; Besson, N.; Bloch, D.; Blom, M.; Bluj, M.; Bonesini, M.; Boonekamp, M.; Booth, P. S. L.; Borisov, G.; Botner, O.; Bouquet, B.; Bowcock, T. J. V.; Boyko, I.; Bracko, M.; Brenner, R.; Brodet, E.; Bruckman, P.; Brunet, J. M.; Buschbeck, B.; Buschmann, P.; Calvi, M.; Camporesi, T.; Canale, V.; Carena, F.; Castro, N.; Cavallo, F.; Chapkin, M.; Charpentier, Ph.; Checchia, P.; Chierici, R.; Chliapnikov, P.; Chudoba, J.; Chung, S. U.; Cieslik, K.; Collins, P.; Contri, R.; Cosme, G.; Cossutti, F.; Costa, M. J.; Crennell, D.; Cuevas, J.; D'Hondt, J.; da Silva, T.; da Silva, W.; Della Ricca, G.; de Angelis, A.; de Boer, W.; de Clercq, C.; de Lotto, B.; de Maria, N.; de Min, A.; de Paula, L.; di Ciaccio, L.; di Simone, A.; Doroba, K.; Drees, J.; Eigen, G.; Ekelof, T.; Ellert, M.; Elsing, M.; Espirito Santo, M. C.; Fanourakis, G.; Fassouliotis, D.; Feindt, M.; Fernandez, J.; Ferrer, A.; Ferro, F.; Flagmeyer, U.; Foeth, H.; Fokitis, E.; Fulda-Quenzer, F.; Fuster, J.; Gandelman, M.; Garcia, C.; Gavillet, Ph.; Gazis, E.; Gokieli, R.; Golob, B.; Gomez-Ceballos, G.; Goncalves, P.; Graziani, E.; Grosdidier, G.; Grzelak, K.; Guy, J.; Haag, C.; Hallgren, A.; Hamacher, K.; Hamilton, K.; Haug, S.; Hauler, F.; Hedberg, V.; Hennecke, M.; Hoffman, J.; Holmgren, S.-O.; Holt, P. J.; Houlden, M. A.; Jackson, J. N.; Jarlskog, G.; Jarry, P.; Jeans, D.; Johansson, E. K.; Jonsson, P.; Joram, C.; Jungermann, L.; Kapusta, F.; Katsanevas, S.; Katsoufis, E.; Kernel, G.; Kersevan, B. P.; Kerzel, U.; King, B. T.; Kjaer, N. J.; Kluit, P.; Kokkinias, P.; Kourkoumelis, C.; Kouznetsov, O.; Krumstein, Z.; Kucharczyk, M.; Lamsa, J.; Leder, G.; Ledroit, F.; Leinonen, L.; Leitner, R.; Lemonne, J.; Lepeltier, V.; Lesiak, T.; Liebig, W.; Liko, D.; Lipniacka, A.; Lopes, J. H.; Lopez, J. M.; Loukas, D.; Lutz, P.; Lyons, L.; MacNaughton, J.; Malek, A.; Maltezos, S.; Mandl, F.; Marco, J.; Marco, R.; Marechal, B.; Margoni, M.; Marin, J.-C.; Mariotti, C.; Markou, A.; Martinez-Rivero, C.; Masik, J.; Mastroyiannopoulos, N.; Matorras, F.; Matteuzzi, C.; Mazzucato, F.; Mazzucato, M.; Mc Nulty, R.; Meroni, C.; Migliore, E.; Mitaroff, W.; Mjoernmark, U.; Moa, T.; Moch, M.; Moenig, K.; Monge, R.; Montenegro, J.; Moraes, D.; Moreno, S.; Morettini, P.; Mueller, U.; Muenich, K.; Mulders, M.; Mundim, L.; Murray, W.; Muryn, B.; Myatt, G.; Myklebust, T.; Nassiakou, M.; Navarria, F.; Nawrocki, K.; Nemecek, S.; Nicolaidou, R.; Nikolenko, M.; Oblakowska-Mucha, A.; Obraztsov, V.; Olshevski, A.; Onofre, A.; Orava, R.; Osterberg, K.; Ouraou, A.; Oyanguren, A.; Paganoni, M.; Paiano, S.; Palacios, J. P.; Palka, H.; Papadopoulou, Th. D.; Pape, L.; Parkes, C.; Parodi, F.; Parzefall, U.; Passeri, A.; Passon, O.; Peralta, L.; Perepelitsa, V.; Perrotta, A.; Petrolini, A.; Piedra, J.; Pieri, L.; Pierre, F.; Pimenta, M.; Piotto, E.; Podobnik, T.; Poireau, V.; Pol, M. E.; Polok, G.; Pozdniakov, V.; Pukhaeva, N.; Pullia, A.; Radojicic, D.; Rebecchi, P.; Rehn, J.; Reid, D.; Reinhardt, R.; Renton, P.; Richard, F.; Ridky, J.; Rivero, M.; Rodriguez, D.; Romero, A.; Ronchese, P.; Roudeau, P.; Rovelli, T.; Ruhlmann-Kleider, V.; Ryabtchikov, D.; Sadovsky, A.; Salmi, L.; Salt, J.; Sander, C.; Savoy-Navarro, A.; Schwickerath, U.; Sekulin, R.; Siebel, M.; Sisakian, A.; Smadja, G.; Smirnova, O.; Sokolov, A.; Sopczak, A.; Sosnowski, R.; Spassov, T.; Stanitzki, M.; Stocchi, A.; Strauss, J.; Stugu, B.; Szczekowski, M.; Szeptycka, M.; Szumlak, T.; Tabarelli, T.; Tegenfeldt, F.; Timmermans, J.; Tkatchev, L.; Tobin, M.; Todorovova, S.; Tome, B.; Tonazzo, A.; Tortosa, P.; Travnicek, P.; Treille, D.; Tristram, G.; Trochimczuk, M.; Troncon, C.; Turluer, M.-L.; Tyapkin, I. A.; Tyapkin, P.; Tzamarias, S.; Uvarov, V.; Valenti, G.; van Dam, P.; van Eldik, J.; van Remortel, N.; van Vulpen, I.; Vegni, G.; Veloso, F.; Venus, W.; Verdier, P.; Verzi, V.; Vilanova, D.; Vitale, L.; Vrba, V.; Wahlen, H.; Washbrook, A. J.; Weiser, C.; Wicke, D.; Wickens, J.; Wilkinson, G.; Winter, M.; Witek, M.; Yushchenko, O.; Zalewska, A.; Zalewski, P.; Zavrtanik, D.; Zhuravlov, V.; Zimin, N. I.; Zintchenko, A.; Zupan, M.; DELPHI Collaboration

2010-06-01

An analysis of the direct soft photon production rate as a function of the parent jet characteristics is presented, based on hadronic events collected by the DELPHI experiment at LEP1. The dependences of the photon rates on the jet kinematic characteristics (momentum, mass, etc.) and on the jet charged, neutral and total hadron multiplicities are reported. Up to a scale factor of about four, which characterizes the overall value of the soft photon excess, a similarity of the observed soft photon behavior to that of the inner hadronic bremsstrahlung predictions is found for the momentum, mass, and jet charged multiplicity dependences. However for the dependence of the soft photon rate on the jet neutral and total hadron multiplicities a prominent difference is found for the observed soft photon signal as compared to the expected bremsstrahlung from final state hadrons. The observed linear increase of the soft photon production rate with the jet total hadron multiplicity and its strong dependence on the jet neutral multiplicity suggest that the rate is proportional to the number of quark pairs produced in the fragmentation process, with the neutral pairs being more effectively radiating than the charged ones.

Dielectric relaxation of barium strontium titanate and application to thin films for DRAM capacitors

NASA Astrophysics Data System (ADS)

Baniecki, John David

This thesis examines the issues associated with incorporating the high dielectric constant material Barium Strontium Titanate (BSTO) in to the storage capacitor of a dynamic random access memory (DRAM). The research is focused on two areas: characterizing and understanding the factors that control charge retention in BSTO thin films and modifying the electrical properties using ion implantation. The dielectric relaxation of BSTO thin films deposited by metal-organic chemical vapor deposition (MOCVD) is investigated in the time and frequency domains. It is shown that the frequency dispersion of the complex capacitance of BSTO thin films can be understood in terms of a power-law frequency dependence from 1mHz to 20GHz. From the correspondence between the time and frequency domain measurements, it is concluded that the power-law relaxation currents extend back to the nano second regime of DRAM operation. The temperature, field, and annealing dependence of the dielectric relaxation currents are also investigated and mechanisms for the observed power law relaxation are explored. An equivalent circuit model of a high dielectric constant thin film capacitor is developed based on the electrical measurements and implemented in PSPICE. Excellent agreement is found between the experimental and simulated electrical characteristics showing the utility of the equivalent circuit model in simulating the electrical properties of high dielectric constant thin films. Using the equivalent circuit model, it is shown that the greatest charge loss due to dielectric relaxation occurs during the first read after a refresh time following a write to the opposite logic state for a capacitor that has been written to the same logic state for a long time (opposite state write charge loss). A theoretical closed form expression that is a function of three material parameters is developed which estimates the opposite state write charge loss due to dielectric relaxation. Using the closed form expression, and BSTO thin film electrical characteristics, the charge loss due to dielectric relaxation is estimated to be 6--12% of the initial charge stored on the capacitor plates for MOCVD BSTO thin films with Pt electrodes after a post top electrode anneal in oxygen. In contrast, it is shown that the charge loss due to steady state leakage is only 0.0125--0.125% of the initial charge stored on the capacitor plates. Charge retention is shown to depend strongly on the annealing conditions. Annealing MOCVD BSTO thin films with Pt electrodes in forming gas (95% Ar 5% H2) increases charge loss due to dielectric relaxation to as much as 60%. Ion implantation is used to dope BSTO thin films with Mn. X-ray diffraction and transmission electron microscopy (TEM) shows ion implantation significantly damages the film leaving only short-range order, but post-implant annealing heals the damage. Capacitance recovery after post-implant annealing is as high as 94% for 15 nm BSTO films. At low implant doses, the Mn doped films have substantially lower leakage (up to a factor of ten lower) and only slightly higher relaxation currents and dielectric loss indicating that ion implantation may be a potentially viable way of introducing dopants into high dielectric constant thin films for future DRAM applications.

Pion single and double charge exchange in the resonance region: Dynamical corrections

NASA Astrophysics Data System (ADS)

Johnson, Mikkel B.; Siciliano, E. R.

1983-04-01

We consider pion-nucleus elastic scattering and single- and double-charge-exchange scattering to isobaric analog states near the (3,3) resonance within an isospin invariant framework. We extend previous theories by introducing terms into the optical potential U that are quadratic in density and consistent with isospin invariance of the strong interaction. We study the sensitivity of single and double charge exchange angular distributions to parameters of the second-order potential both numerically, by integrating the Klein-Gordon equation, and analytically, by using semiclassical approximations that explicate the dependence of the exact numerical results to the parameters of U. The magnitude and shape of double charge exchange angular distributions are more sensitive to the isotensor term in U than has been hitherto appreciated. An examination of recent experimental data shows that puzzles in the shape of the 18O(π+, π-)18Ne angular distribution at 164 MeV and in the A dependence of the forward double charge exchange scattering on 18O, 26Mg, 42Ca, and 48Ca at the same energy may be resolved by adding an isotensor term in U. NUCLEAR REACTIONS Scattering theory for elastic, single-, and double-charge-exchange scattering to IAS in the region of the P33 resonance. Second-order effects on charge-exchange calculations of σ(A, θ).

Single crystal structures and theoretical calculations of uranium endohedral metallofullerenes (U@C2n , 2n = 74, 82) show cage isomer dependent oxidation states for U.

PubMed

Cai, Wenting; Morales-Martínez, Roser; Zhang, Xingxing; Najera, Daniel; Romero, Elkin L; Metta-Magaña, Alejandro; Rodríguez-Fortea, Antonio; Fortier, Skye; Chen, Ning; Poblet, Josep M; Echegoyen, Luis

2017-08-01

Charge transfer is a general phenomenon observed for all endohedral mono-metallofullerenes. Since the detection of the first endohedral metallofullerene (EMF), La@C 82 , in 1991, it has always been observed that the oxidation state of a given encapsulated metal is always the same, regardless of the cage size. No crystallographic data exist for any early actinide endohedrals and little is known about the oxidation states for the few compounds that have been reported. Here we report the X-ray structures of three uranium metallofullerenes, U@ D 3h -C 74 , U@ C 2 (5)-C 82 and U@ C 2v (9)-C 82 , and provide theoretical evidence for cage isomer dependent charge transfer states for U. Results from DFT calculations show that U@ D 3h -C 74 and U@ C 2 (5)-C 82 have tetravalent electronic configurations corresponding to U 4+ @ D 3h -C 74 4- and U 4+ @ C 2 (5)-C 82 4- . Surprisingly, the isomeric U@ C 2v (9)-C 82 has a trivalent electronic configuration corresponding to U 3+ @ C 2v (9)-C 82 3- . These are the first X-ray crystallographic structures of uranium EMFs and this is first observation of metal oxidation state dependence on carbon cage isomerism for mono-EMFs.

Numerical experiments on charging of a spherical body in a plasma with Maxwellian distributions of charged particles

NASA Astrophysics Data System (ADS)

Krasovsky, Victor L.; Kiselyov, Alexander A.

2017-12-01

New results of numerical simulation of collisionless plasma perturbation caused by a sphere absorbing electrons and ions are presented. Consideration is given to nonstationary phenomena accompanying the process of charging as well as to plasma steady state reached at long times. Corresponding asymptotic values of charges of the sphere and trapped-ion cloud around it have been found along with self-consistent electric field pattern depending on parameters of the unperturbed plasma. It is established that contribution of the trapped ions to screening of the charged sphere can be quite significant, so that the screening becomes essentially nonlinear in nature. A simple interconnection between the sphere radius, electron and ion Debye lengths has been revealed as the condition for maximum trapped-ion effect. Kinetic structure of the space charge induced in the plasma is discussed with relation to the specific form of the unperturbed charged particle distribution functions.

Electron transfer beyond the static picture: A TDDFT/TD-ZINDO study of a pentacene dimer

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

Reslan, Randa; Lopata, Kenneth; Arntsen, Christopher

2012-12-14

We use time-dependent density functional theory and time-dependent ZINDO (a semi-empirical method) to study transfer of an extra electron between a pair of pentacene molecules. A measure of the electronic transfer integral is computed in a dynamic picture via the vertical excitation energy from a delocalized anionic ground state. With increasing dimer separation, this dynamical measurement of charge transfer is shown to be significantly larger than the commonly used static approximation (i.e., LUMO+1–LUMO of the neutral dimer, or HOMO–LUMO of the charged dimer), up to an order of magnitude higher at 6 Å. These results offer a word of cautionmore » for calculations involving large separations, as in organic photovoltaics, where care must be taken when using a static picture to model charge transfer.« less

Electron transfer beyond the static picture: A TDDFT/TD-ZINDO study of a pentacene dimer

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

Reslan, Randa; Lopata, Kenneth A.; Arntsen, Christopher D.

2012-12-14

We use time-dependent density functional theory and time-dependent ZINDO (a semi-empirical method) to study transfer of an extra electron between a pair of pentacene dimers. A measure of the electronic transfer integral is computed in a dynamic picture via the vertical excitation energy from a delocalized anionic ground state. With increasing dimer separation, this dynamical measurement of charge transfer is shown to be significantly larger than the commonly used static approximation (i.e., LUMO+1 - LUMO of the neutral dimer, or HOMO - LUMO of the charged dimer), up to an order of magnitude higher at 6 Å. These results offermore » a word of caution for calculations involving large separations, as in organic photovoltaics, where care must be taken when using a static picture to model charge transfer.« less

Entanglement scrambling in 2d conformal field theory

DOE PAGES

Asplund, Curtis T.; Bernamonti, Alice; Galli, Federico; ...

2015-09-17

Here, we investigate how entanglement spreads in time-dependent states of a 1+1 dimensional conformal field theory (CFT). The results depend qualitatively on the value of the central charge. In rational CFTs, which have central charge below a critical value, entanglement entropy behaves as if correlations were carried by free quasiparticles. This leads to long-term memory effects, such as spikes in the mutual information of widely separated regions at late times. When the central charge is above the critical value, the quasiparticle picture fails. Assuming no extended symmetry algebra, any theory with c > 1 has diminished memory effects compared tomore » the rational models. In holographic CFTs, with c >> 1, these memory effects are eliminated altogether at strong coupling, but reappear after the scrambling time t ≳ β log c at weak coupling.« less

Fluorescence probe of polypeptide conformational dynamics in gas phase and in solution

NASA Astrophysics Data System (ADS)

Iavarone, Anthony T.; Meinen, Jan; Schulze, Susanne; Parks, Joel H.

2006-07-01

Fluorescence measurements of polypeptides derivatized with the fluorescent dye BODIPY TMR have been used to probe the polypeptide conformational dynamics as a function of temperature and charge state. Measurements of (BODIPY TMR)-[Pro]n-Arg-Trp and (BODIPY TMR)-[Gly-Ser]m-Arg-Trp have been performed for charge states 1+ and 2+ of n = 4 and 10 and m = 2 and 5. The 2+ charge states of both of these polypeptides exhibit similar temperature dependences for equal chain lengths (n = 4, m = 2 and n = 10, m = 5) and suggest conformations dominated by Coulomb repulsion. In the absence of such Coulomb repulsion, the 1+ charge state conformations appear to be characterized by the flexibility of the polypeptide chain for which [Gly-Ser]m > [Pro]n. Comparisons of these gas phase polypeptide measurements with corresponding measurements in solution provide a direct measure of the effects of solvent on the conformational dynamics. The change in fluorescence as a function of temperature in the gas phase is two orders of magnitude greater than that in solution, a dramatic result we attribute to the restrictions on intramolecular dynamics imposed by diffusion-limited kinetics and the lack of shielding by solvent. Measurements were also made of unsolvated Pron peptides without the tryptophan (Trp) residue to isolate the interaction of the fluorescent dye with charges.

Beyond Born-Oppenheimer theory for ab initio constructed diabatic potential energy surfaces of singlet H3+ to study reaction dynamics using coupled 3D time-dependent wave-packet approach.

PubMed

Ghosh, Sandip; Mukherjee, Saikat; Mukherjee, Bijit; Mandal, Souvik; Sharma, Rahul; Chaudhury, Pinaki; Adhikari, Satrajit

2017-08-21

The workability of beyond Born-Oppenheimer theory to construct diabatic potential energy surfaces (PESs) of a charge transfer atom-diatom collision process has been explored by performing scattering calculations to extract accurate integral cross sections (ICSs) and rate constants for comparison with most recent experimental quantities. We calculate non-adiabatic coupling terms among the lowest three singlet states of H 3 + system (1 1 A ' , 2 1 A ' , and 3 1 A ' ) using MRCI level of calculation and solve the adiabatic-diabatic transformation equation to formulate the diabatic Hamiltonian matrix of the same process [S. Mukherjee et al., J. Chem. Phys. 141, 204306 (2014)] for the entire region of nuclear configuration space. The nonadiabatic effects in the D + + H 2 reaction has been studied by implementing the coupled 3D time-dependent wave packet formalism in hyperspherical coordinates [S. Adhikari and A. J. C. Varandas, Comput. Phys. Commun. 184, 270 (2013)] with zero and non-zero total angular momentum (J) on such newly constructed accurate (ab initio) diabatic PESs of H 3 + . We have depicted the convergence profiles of reaction probabilities for the reactive non-charge transfer, non-reactive charge transfer, and reactive charge transfer processes for different collisional energies with respect to the helicity (K) and total angular momentum (J) quantum numbers. Finally, total and state-to-state ICSs are calculated as a function of collision energy for the initial rovibrational state (v = 0, j = 0) of the H 2 molecule, and consequently, those quantities are compared with previous theoretical and experimental results.

Hydrated proton and hydroxide charge transfer at the liquid/vapor interface of water

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

Soniat, Marielle; Rick, Steven W., E-mail: srick@uno.edu; Kumar, Revati

2015-07-28

The role of the solvated excess proton and hydroxide ions in interfacial properties is an interesting scientific question with applications in a variety of aqueous behaviors. The role that charge transfer (CT) plays in interfacial behavior is also an unsettled question. Quantum calculations are carried out on clusters of water with an excess proton or a missing proton (hydroxide) to determine their CT. The quantum results are applied to analysis of multi-state empirical valence bond trajectories. The polyatomic nature of the solvated excess proton and hydroxide ion results in directionally dependent CT, depending on whether a water molecule is amore » hydrogen bond donor or acceptor in relation to the ion. With polyatomic molecules, CT also depends on the intramolecular bond distances in addition to intermolecular distances. The hydrated proton and hydroxide affect water’s liquid/vapor interface in a manner similar to monatomic ions, in that they induce a hydrogen-bonding imbalance at the surface, which results in charged surface waters. This hydrogen bond imbalance, and thus the charged waters at the surface, persists until the ion is at least 10 Å away from the interface.« less

Negative Differential Conductance in Polyporphyrin Oligomers with Nonlinear Backbones.

PubMed

Kuang, Guowen; Chen, Shi Zhang; Yan, Linghao; Chen, Ke Qiu; Shang, Xuesong; Liu, Pei Nian; Lin, Nian

2018-01-17

We study negative differential conductance (NDC) effects in polyporphyrin oligomers with nonlinear backbones. Using a low-temperature scanning tunneling microscope, we selectively controlled the charge transport path in single oligomer wires. We observed robust NDC when charge passed through a T-shape junction, bistable NDC when charge passed through a 90° kink and no NDC when charge passed through a 120° kink. Aided by density functional theory with nonequilibrium Green's functions simulations, we attributed this backbone-dependent NDC to bias-modulated hybridization of the electrode states with the resonant transport molecular orbital. We argue this mechanism is generic in molecular systems, which opens a new route of designing molecular NDC devices.

Charge transfer in iridate-manganite superlattices

DOE PAGES

Okamoto, Satoshi; Nichols, John; Sohn, Changhee; ...

2017-03-03

Charge transfer in superlattices consisting of SrIrOmore » $$_3$$ and SrMnO$$_3$$ is investigated using density functional theory. Despite the nearly identical work function and non-polar interfaces between SrIrO$$_3$$ and SrMnO$$_3$$, rather large charge transfer was experimentally reported between them. Our results provide a qualitative understanding to such experimental reports. We further develop a microscopic model that captures the mechanism behind this phenomenon. This leads to unique strain dependence of such charge transfer in iridate-manganite superlattices. The predicted behavior is consistently verified by experiment. Lastly, our work thus demonstrates a new route to control electronic states in non-polar oxide heterostructures.« less

Lifetime enhancement for multiphoton absorption in intermediate band solar cells

NASA Astrophysics Data System (ADS)

Bezerra, Anibal T.; Studart, Nelson

2017-08-01

A semiconductor structure consisting of two coupled quantum wells embedded into the intrinsic region of a p-i-n junction is proposed as an intermediate band solar cell with a photon ratchet state, which would lead to increasing the cell efficiency. The conduction subband of the right-hand side quantum well works as the intermediated band, whereas the excited conduction subband of the left-hand side quantum well operates as the ratchet state. The photoelectrons in the intermediate band are scattered through the thin wells barrier and accumulated into the ratchet subband. A rate equation model for describing the charge transport properties is presented. The efficiency of the current generation is analyzed by studying the occupation of the wells subbands, taking into account the charge dynamic behavior provided by the electrical contacts connected to the cell. The current generation efficiency depends essentially from the relations between the generation, recombination rates and the scattering rate to the ratchet state. The inclusion of the ratchet states led to both an increase and a decrease in the cell current depending on the transition rates. This suggests that the coupling between the intermediate band and the ratchet state is a key point in developing an efficient solar cell.

Determination of the “NiOOH” charge and discharge mechanisms at ideal activity

DOE PAGES

Merrill, Matthew; Worsley, Marcus; Wittstock, Arne; ...

2014-01-24

Here, optimization of electrodeposition conditions produced Ni(OH) 2 deposits chargeable up to 1.84 ± 0.02 e – per Ni on and the resulting nickel oxide/hydroxide active material could subsequently deliver 1.58 ± 0.02 e – per Ni ion (462 mA h/g) over a potential range <0.2 V. The ability of the “NiOOH” active material to deliver an approximately ideal charge and discharge facilitated a coulometric and thermodynamic analysis through which the charge/discharge mechanisms were determined from known enthalpies of formation. The (dis)charge states were confirmed with in situ Raman spectroscopy. The mechanisms were additionally evaluated with respect to pH andmore » potential dependence, charge quantities, hysteresis, and fluoride ion partial inhibition of the charge mechanism. The results indicate that the “NiOOH” (dis)charges as a solid-state system with mechanisms consistent with known nickel and oxygen redox reactions. A defect chemistry mechanism known for the LiNiO 2 system also occurs for “NiOOH” to cause both high activity and hysteresis. Similar to other cation insertion nickel oxides, the activity of the “NiOOH” mechanism is predominantly due to oxygen redox activity and does not involve the Ni4 + oxidation state. The “NiOOH” was produced from cathodic electrodeposition of Ni(OH) 2 from nickel nitrate solutions onto highly oriented pyrolytic graphite at ideal electrodeposition current efficiencies and the deposition mechanism was also characterized.« less

On the Kendrick Mass Defect Plots of Multiply Charged Polymer Ions: Splits, Misalignments, and How to Correct Them

NASA Astrophysics Data System (ADS)

Fouquet, Thierry N. J.; Cody, Robert B.; Ozeki, Yuka; Kitagawa, Shinya; Ohtani, Hajime; Sato, Hiroaki

2018-05-01

The Kendrick mass defect (KMD) analysis of multiply charged polymeric distributions has recently revealed a surprising isotopic split in their KMD plots—namely a 1/z difference between KMDs of isotopes of an oligomer at charge state z. Relying on the KMD analysis of actual and simulated distributions of poly(ethylene oxide) (PEO), the isotopic split is mathematically accounted for and found to go with an isotopic misalignment in certain cases. It is demonstrated that the divisibility (resp. indivisibility) of the nominal mass of the repeating unit (R) by z is the condition for homolog ions to line up horizontally (resp. misaligned obliquely) in a KMD plot. Computing KMDs using a fractional base unit R/z eventually corrects the misalignments for the associated charge state while using the least common multiple of all the charge states as the divisor realigns all the points at once. The isotopic split itself can be removed by using either a new charge-dependent KMD plot compatible with any fractional base unit or the remainders of KM (RKM) recently developed for low-resolution data all found to be linked in a unified theory. These original applications of the fractional base units and the RKM plots are of importance theoretically to satisfy the basics of a mass defect analysis and practically for a correct data handling of single stage and tandem mass spectra of multiply charged homo- and copolymers.

Communication: The electronic entropy of charged defect formation and its impact on thermochemical redox cycles

NASA Astrophysics Data System (ADS)

Lany, Stephan

2018-02-01

The ideal material for solar thermochemical water splitting, which has yet to be discovered, must satisfy stringent conditions for the free energy of reduction, including, in particular, a sufficiently large positive contribution from the solid-state entropy. By inverting the commonly used relationship between defect formation energy and defect concentration, it is shown here that charged defect formation causes a large electronic entropy contribution manifesting itself as the temperature dependence of the Fermi level. This result is a general feature of charged defect formation and motivates new materials design principles for solar thermochemical hydrogen production.

Communication: The electronic entropy of charged defect formation and its impact on thermochemical redox cycles

DOE PAGES

Lany, Stephan

2018-02-21

The ideal material for solar thermochemical water splitting, which has yet to be discovered, must satisfy stringent conditions for the free energy of reduction, including, in particular, a sufficiently large positive contribution from the solid-state entropy. By inverting the commonly used relationship between defect formation energy and defect concentration, it is shown here that charged defect formation causes a large electronic entropy contribution manifesting itself as the temperature dependence of the Fermi level. This result is a general feature of charged defect formation and motivates new materials design principles for solar thermochemical hydrogen production.

Communication: The electronic entropy of charged defect formation and its impact on thermochemical redox cycles

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

Lany, Stephan

The ideal material for solar thermochemical water splitting, which has yet to be discovered, must satisfy stringent conditions for the free energy of reduction, including, in particular, a sufficiently large positive contribution from the solid-state entropy. By inverting the commonly used relationship between defect formation energy and defect concentration, it is shown here that charged defect formation causes a large electronic entropy contribution manifesting itself as the temperature dependence of the Fermi level. This result is a general feature of charged defect formation and motivates new materials design principles for solar thermochemical hydrogen production.

Single-molecule interfacial electron transfer dynamics in solar energy conversion

NASA Astrophysics Data System (ADS)

Dhital, Bharat

This dissertation work investigated the parameters affecting the interfacial electron transfer (ET) dynamics in dye-semiconductor nanoparticles (NPs) system by using single-molecule fluorescence spectroscopy and imaging combined with electrochemistry. The influence of the molecule-substrate electronic coupling, the molecular structure, binding geometry on the surface and the molecule-attachment surface chemistry on interfacial charge transfer processes was studied on zinc porphyrin-TiO2 NP systems. The fluorescence blinking measurement on TiO2 NP demonstrated that electronic coupling regulates dynamics of charge transfer processes at the interface depending on the conformation of molecule on the surface. Moreover, semiconductor surface charge induced electronic coupling of molecule which is electrostatically adsorbed on the semiconductor surface also predominantly alters the ET dynamics. Furthermore, interfacial electric field and electron accepting state density dependent ET dynamics has been dissected in zinc porphyrin-TiO2 NP system by observing the single-molecule fluorescence blinking dynamics and fluorescence lifetime with and without applied bias. The significant difference in fluorescence fluctuation and lifetime suggested the modulation of charge transfer dynamics at the interface with external electric field perturbation. Quasi-continuous distribution of fluorescence intensity with applied negative potential was attributed to the faster charge recombination due to reduced density of electron accepting states. The driving force and electron accepting state density ET dependent dynamics has also been probed in zinc porphyrin-TiO2 NP and zinc porphyrin-indium tin oxide (ITO) systems. Study of a molecule adsorbed on two different semiconductors (ITO and TiO2), with large difference in electron densities and distinct driving forces, allows us to observe the changes in rates of back electron transfer process reflected by the suppressed fluorescence blinking of molecule on ITO surface. Finally, the electric field effect on the interface properties has been probed by using surface-enhanced Raman spectroscopy and supported by density functional theory calculations in alizarin-TiO2 system. The perturbation, created by the external potential, has been observed to cause a shift and/or splitting interfacial bond vibrational mode, typical indicator of the coupling energy changes between alizarin and TiO2. Such splitting provides evidence for electric field-dependent electronic coupling changes that have a significant impact on the interfacial electron transfer dynamics.

Exploring coherent electron excitation and migration dynamics by electron diffraction with ultrashort X-ray pulses.

PubMed

Yuan, Kai-Jun; Bandrauk, André D

2017-10-04

Exploring ultrafast charge migration is of great importance in biological and chemical reactions. We present a scheme to monitor attosecond charge migration in molecules by electron diffraction with spatial and temporal resolutions from ab initio numerical simulations. An ultraviolet pulse creates a coherent superposition of electronic states, after which a time-delayed attosecond X-ray pulse is used to ionize the molecule. It is found that diffraction patterns in the X-ray photoelectron spectra show an asymmetric structure, which is dependent on the time delay between the pump-probe pulses, encoding the information of molecular orbital symmetry and chemical bonding. We describe these phenomena by developing an electronic time-dependent ultrafast molecular photoionization model of a coherent superposition state. The periodical distortion of electron diffraction patterns illustrates the evolution of the electronic coherence, providing a tool for attosecond imaging of ultrafast molecular reaction processes.

Substitution effects on the absorption spectra of nitrophenolate isomers.

PubMed

Wanko, Marius; Houmøller, Jørgen; Støchkel, Kristian; Suhr Kirketerp, Maj-Britt; Petersen, Michael Åxman; Nielsen, Mogens Brøndsted; Nielsen, Steen Brøndsted; Rubio, Angel

2012-10-05

Charge-transfer excitations highly depend on the electronic coupling between the donor and acceptor groups. Nitrophenolates are simple examples of charge-transfer systems where the degree of coupling differs between ortho, meta and para isomers. Here we report the absorption spectra of the isolated anions in vacuo to avoid the complications of solvent effects. Gas-phase action spectroscopy was done with two different setups, an electrostatic ion storage ring and an accelerator mass spectrometer. The results are interpreted on the basis of CC2 quantum chemical calculations. We identified absorption maxima at 393, 532, and 399 nm for the para, meta, and ortho isomer, respectively, with the charge-transfer transition into the lowest excited singlet state. In the meta isomer, this π-π* transition is strongly redshifted and its oscillator strength reduced, which is related to the pronounced charge-transfer character, as a consequence of the topology of the conjugated π-system. Each isomer's different charge distribution in the ground state leads to a very different solvent shift, which in acetonitrile is bathochromic for the para and ortho, but hypsochromic for the meta isomer.

Laser-induced electron dynamics including photoionization: A heuristic model within time-dependent configuration interaction theory.

PubMed

Klinkusch, Stefan; Saalfrank, Peter; Klamroth, Tillmann

2009-09-21

We report simulations of laser-pulse driven many-electron dynamics by means of a simple, heuristic extension of the time-dependent configuration interaction singles (TD-CIS) approach. The extension allows for the treatment of ionizing states as nonstationary states with a finite, energy-dependent lifetime to account for above-threshold ionization losses in laser-driven many-electron dynamics. The extended TD-CIS method is applied to the following specific examples: (i) state-to-state transitions in the LiCN molecule which correspond to intramolecular charge transfer, (ii) creation of electronic wave packets in LiCN including wave packet analysis by pump-probe spectroscopy, and, finally, (iii) the effect of ionization on the dynamic polarizability of H(2) when calculated nonperturbatively by TD-CIS.

Dangerous liaisons: anion-induced protonation in phosphate-polyamine interactions and their implications for the charge states of biologically relevant surfaces.

PubMed

Laucirica, Gregorio; Marmisollé, Waldemar A; Azzaroni, Omar

2017-03-22

Although not always considered a preponderant interaction, amine-phosphate interactions are omnipresent in multiple chemical and biological systems. This study aims to answer questions that are still pending about their nature and consequences. We focus on the description of the charge state as surface charges constitute directing agents of the interaction of amine groups with either natural or synthetic counterparts. Our results allow us to quantitatively determine the relative affinities of HPO 4 2- and H 2 PO 4 - from the analysis of the influence of phosphates on the zeta-potential of amino-functionalized surfaces in a broad pH range. We show that phosphate anions enhance the protonation of amino groups and, conversely, charged amines induce further proton dissociation of phosphates, yielding a complex dependence of the surface effective charge on the pH and phosphate concentration. We also demonstrate that phosphate-amine interaction is specific and the modulation of surface charge occurs in the physiological phosphate concentration range, emphasizing its biochemical and biotechnological relevance and the importance of considering this veiled association in both in vivo and in vitro studies.

Theoretical investigation of the electron transfer dynamics and photodegradation pathways in a hydrogen-evolving ruthenium-palladium photocatalyst.

PubMed

Staniszewska, Magdalena; Kupfer, Stephan; Guthmuller, Julien

2018-05-16

Time-dependent density functional theory calculations combined with the Marcus theory of electron transfer (ET) were applied on the molecular photocatalyst [(tbbpy)2Ru(tpphz)PdCl2]2+ in order to elucidate the light-induced relaxation pathways populated upon excitation in the longer wavelength range of its absorption spectrum. The computational results show that after the initial excitation, metal (Ru) to ligand (tpphz) charge transfer (MLCT) triplet states are energetically accessible, but that an ET toward the catalytic center (PdCl2) from these states is a slow process, with estimated time constants above 1 ns. Instead, the calculations predict that low-lying Pd-centered states are efficiently populated - associated to an energy transfer toward the catalytic center. Thus, it is postulated that these states lead to the dissociation of a Cl- and are consequently responsible for the experimentally observed degradation of the catalytic center. Following dissociation, it is shown that the ET rates from the MLCT states to the charge separated states are significantly increased (i.e. 10^5-10^6 times larger). This demonstrates that alteration of the catalytic center generates efficient charge separation. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Mesoscopic features of charge generation in organic semiconductors.

PubMed

Savoie, Brett M; Jackson, Nicholas E; Chen, Lin X; Marks, Tobin J; Ratner, Mark A

2014-11-18

CONSPECTUS: In the past two decades, organic materials have been extensively investigated by numerous research groups worldwide for implementation in organic photovoltaic (OPV) devices. The interest in organic semiconductors is spurred by their potential low cost and facile tunability, making OPV devices a potentially disruptive technology. To study OPV operating mechanisms is also to explore a knowledge gap in our general understanding of materials, because both the time scales (femtosecond to microsecond) and length scales (nanometer to micrometer) relevant to OPV functionality occupy a challenging and fascinating space between the traditional regimes of quantum chemistry and solid-state physics. New theoretical frameworks and computational tools are needed to bridge the aforementioned length and time scales, and they must satisfy the criteria of computational tractability for systems involving 10(4)-10(6) atoms, while also maintaining predictive utility. While this challenge is far from solved, advances in density functional theory (DFT) have allowed researchers to investigate the ground- and excited-state properties of many intermediate sized systems (10(2)-10(3) atoms) that provide the outlines of the larger problem. Results on these smaller systems are already sufficient to predict optical gaps and trends in valence band energies, correct erroneous interpretations of experimental data, and develop models for charge generation and transport in OPV devices. The active films of high-efficiency OPV devices are comprised of mesoscopic mixtures of electron donor (D) and electron acceptor (A) species, a "bulk-heterojunction" (BHJ) device, subject to variable degrees of structural disorder. Depending on the degree of intermolecular electronic coupling and energy level alignment, the spatial delocalization of photoexcitations and charge carriers can affect the dynamics of the solar cell. In this Account, we provide an overview of three pivotal characteristics of solar cells that possess strong delocalization dependence: (1) the exciton binding energy, (2) charge transfer at the D-A heterojunction, and (3) the energy landscape in the vicinity of the D-A heterojunction. In each case, the length scale dependence can be assessed through DFT calculations on reference systems, with a view to establishing general trends. Throughout the discussion, we draw from the experimental and theoretical literature to provide a consistent view of what is known about these properties in actual BHJ blends. A consistent interpretation of the results to date affords the following view: transient delocalization effects and resonant charge transfer at the heterojunction are capable of funneling excitations away from trap states and mediating exciton dissociation; these factors alone are capable of explaining the remarkably good charge generation currently achieved in OPV devices. The exciton binding energy likely plays a minimal role in modern OPV devices, since the presence of the heterojunction serves to bypass the costly exciton-to-free-charge transition state.

Tight-binding molecular-dynamics study of point defects in GaAs

NASA Astrophysics Data System (ADS)

Seong, Hyangsuk; Lewis, Laurent J.

1995-08-01

Tight-binding molecular-dynamics simulations at 0 K have been performed in order to study the effect of defects (vacancies and antisites) in different states of charge on the electronic and structural properties of GaAs. Relaxations are fully included in the model, and for each defect we calculate the local atomic structure, the volume change upon relaxing, the formation energy (including chemical potential contributions), and the ionization levels. We find Ga vacancies to relax by an amount which is independent of the state of charge, consistent with positron lifetime measurements. Our calculations also predict Ga vacancies to exhibit a negative-U effect, and to assume a triply negative charge state for most values of the electron chemical potential. The relaxation of As vacancies, on the contrary, depends sensitively on the state of charge. The model confirms the two experimentally observed ionization levels for this defect, just below the conduction-band minimum. Likewise, Ga antisites exhibit large relaxations. In fact, in the neutral state, relaxation is so large that it leads to a ``broken-bond'' configuration, in excellent accord with the first-principles calculations of Zhang and Chadi [Phys. Rev. Lett. 64, 1789 (1990)]. This system also exhibits a negative-U effect, for values of the electron chemical potential near midgap. For As antisites, we find only a weak relaxation, independent of the charge. The model predicts the neutral state of the defect to be the ground state for values of the electron chemical potential near and above midgap, which supports the view that the EL2 defect is a neutral As antisite. Upon comparing the formation energies of the various defects we finally find that, for all values of the atomic chemical potentials, antisites are most likely to occur than vacancies.

Investigating local degradation and thermal stability of charged nickel-based cathode materials through real-time electron microscopy.

PubMed

Hwang, Sooyeon; Kim, Seung Min; Bak, Seong-Min; Cho, Byung-Won; Chung, Kyung Yoon; Lee, Jeong Yong; Chang, Wonyoung; Stach, Eric A

2014-09-10

In this work, we take advantage of in situ transmission electron microscopy (TEM) to investigate thermally induced decomposition of the surface of Li(x)Ni(0.8)Co(0.15)Al(0.05)O2 (NCA) cathode materials that have been subjected to different states of charge (SOC). While uncharged NCA is stable up to 400 °C, significant changes occur in charged NCA with increasing temperature. These include the development of surface porosity and changes in the oxygen K-edge electron energy loss spectra, with pre-edge peaks shifting to higher energy losses. These changes are closely related to O2 gas released from the structure, as well as to phase changes of NCA from the layered structure to the disordered spinel structure, and finally to the rock-salt structure. Although the temperatures where these changes initiate depend strongly on the state of charge, there also exist significant variations among particles with the same state of charge. Notably, when NCA is charged to x = 0.33 (the charge state that is the practical upper limit voltage in most applications), the surfaces of some particles undergo morphological and oxygen K-edge changes even at temperatures below 100 °C, a temperature that electronic devices containing lithium ion batteries (LIB) can possibly see during normal operation. Those particles that experience these changes are likely to be extremely unstable and may trigger thermal runaway at much lower temperatures than would be usually expected. These results demonstrate that in situ heating experiments are a unique tool not only to study the general thermal behavior of cathode materials but also to explore particle-to-particle variations, which are sometimes of critical importance in understanding the performance of the overall system.

Two-loop self-energy in the Lamb shift of the ground and excited states of hydrogenlike ions

NASA Astrophysics Data System (ADS)

Yerokhin, V. A.

2018-05-01

The two-loop self-energy correction to the Lamb shift of hydrogenlike ions is calculated for the 1 s , 2 s , and 2 p1 /2 states and nuclear charge numbers Z =30 -100 . The calculation is performed to all orders in the nuclear binding strength parameter Z α . As compared to previous calculations of this correction, numerical accuracy is improved by an order of magnitude and the region of the nuclear charges is extended. An analysis of the Z dependence of the obtained results demonstrates their consistency with the known Z α -expansion coefficients.

Interactions between charged residues in the transmembrane segments of the voltage-sensing domain in the hERG channel.

PubMed

Zhang, M; Liu, J; Jiang, M; Wu, D-M; Sonawane, K; Guy, H R; Tseng, G-N

2005-10-01

Studies on voltage-gated K channels such as Shaker have shown that positive charges in the voltage-sensor (S4) can form salt bridges with negative charges in the surrounding transmembrane segments in a state-dependent manner, and different charge pairings can stabilize the channels in closed or open states. The goal of this study is to identify such charge interactions in the hERG channel. This knowledge can provide constraints on the spatial relationship among transmembrane segments in the channel's voltage-sensing domain, which are necessary for modeling its structure. We first study the effects of reversing S4's positive charges on channel activation. Reversing positive charges at the outer (K525D) and inner (K538D) ends of S4 markedly accelerates hERG activation, whereas reversing the 4 positive charges in between either has no effect or slows activation. We then use the 'mutant cycle analysis' to test whether D456 (outer end of S2) and D411 (inner end of S1) can pair with K525 and K538, respectively. Other positive charges predicted to be able, or unable, to interact with D456 or D411 are also included in the analysis. The results are consistent with predictions based on the distribution of these charged residues, and confirm that there is functional coupling between D456 and K525 and between D411 and K538.

Electron mobility in the inversion layers of fully depleted SOI films

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

Zaitseva, E. G., E-mail: ZaytsevaElza@yandex.ru; Naumova, O. V.; Fomin, B. I.

The dependences of the electron mobility μ{sub eff} in the inversion layers of fully depleted double–gate silicon-on-insulator (SOI) metal–oxide–semiconductor (MOS) transistors on the density N{sub e} of induced charge carriers and temperature T are investigated at different states of the SOI film (inversion–accumulation) from the side of one of the gates. It is shown that at a high density of induced charge carriers of N{sub e} > 6 × 10{sup 12} cm{sup –2} the μeff(T) dependences allow the components of mobility μ{sub eff} that are related to scattering at surface phonons and from the film/insulator surface roughness to be distinguished.more » The μ{sub eff}(N{sub e}) dependences can be approximated by the power functions μ{sub eff}(N{sub e}) ∝ N{sub e}{sup −n}. The exponents n in the dependences and the dominant mechanisms of scattering of electrons induced near the interface between the SOI film and buried oxide are determined for different N{sub e} ranges and film states from the surface side.« less

Electron quantum dynamics in atom-ion interaction

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

Sabzyan, H., E-mail: sabzyan@sci.ui.ac.ir; Jenabi, M. J.

2016-04-07

Electron transfer (ET) process and its dependence on the system parameters are investigated by solving two-dimensional time-dependent Schrödinger equation numerically using split operator technique. Evolution of the electron wavepacket occurs from the one-electron species hydrogen atom to another bare nucleus of charge Z > 1. This evolution is quantified by partitioning the simulation box and defining regional densities belonging to the two nuclei of the system. It is found that the functional form of the time-variations of these regional densities and the extent of ET process depend strongly on the inter-nuclear distance and relative values of the nuclear charges, whichmore » define the potential energy surface governing the electron wavepacket evolution. Also, the initial electronic state of the single-electron atom has critical effect on this evolution and its consequent (partial) electron transfer depending on its spreading extent and orientation with respect to the inter-nuclear axis.« less

Application of hyperspherical harmonics expansion method to the low-lying bound S-states of exotic two-muon three-body systems

NASA Astrophysics Data System (ADS)

Khan, Md. Abdul

2014-09-01

In this paper, energies of the low-lying bound S-states (L = 0) of exotic three-body systems, consisting a nuclear core of charge +Ze (Z being atomic number of the core) and two negatively charged valence muons, have been calculated by hyperspherical harmonics expansion method (HHEM). The three-body Schrödinger equation is solved assuming purely Coulomb interaction among the binary pairs of the three-body systems XZ+μ-μ- for Z = 1 to 54. Convergence pattern of the energies have been checked with respect to the increasing number of partial waves Λmax. For available computer facilities, calculations are feasible up to Λmax = 28 partial waves, however, calculation for still higher partial waves have been achieved through an appropriate extrapolation scheme. The dependence of bound state energies has been checked against increasing nuclear charge Z and finally, the calculated energies have been compared with the ones of the literature.

Inner-shell excitation and ionic fragmentation of molecules

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

Hitchcock, A.P.; Tyliszczak, T.; Cavell, R.G.

1997-04-01

Inner-shell excitation and associated decay spectroscopies are site specific probes of electronic and geometrical structure and photoionization dynamics. X-ray absorption probes the geometric and electronic structure, while time-of-flight mass spectrometry with multi-coincidence detection provides information on the photofragmentation dynamics of the initially produced inner-shell state. Auger decay of inner-shell excited and ionised states is an efficient source of multiply charged ions. The charge separation and fragmentation of these species, studied by photoelectron-photoion-photoion coincidence (also called charge separation mass spectrometry) gives insights into bonding and electronic structure. In molecules, the dependence of the fragmentation process on the X-ray energy can revealmore » cases of site and/or state selective fragmentation. At the ALS the authors have examined the soft X-ray spectroscopy and ionic fragmentation of a number of molecules, including carboranes, silylenes, phosphorus halides, SF{sub 6} and CO{sub 2}. Their work is illustrated using results from the carborane and PF{sub 3} studies.« less

Projectile-charge-state dependence of 0[degree] binary-encounter electron production in 30-MeV O[sup [ital q]+]+O[sub 2] collisions

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

Zouros, T.J.M.; Richard, P.; Wong, K.L.

Double-differential cross sections (DDCS's) for the production of binary-encounter electrons (BEE's) are reported for 30-MeV O[sup [ital q]+]+O[sub 2] collisions. The BEE DDCS's were measured at [theta]=0[degree] with respect to the beam direction for projectile charge states [ital q]=4--8. The measured BEE DDCS's were found to increase with decreasing charge state in agreement with other recent BEE results employing simpler H[sub 2] and He targets. Impulse-approximation calculations of BEE production for [theta]=0[degree]--45[degree] are also presented, in which it is assumed that target electrons undergo elastic scattering in the screened Coulomb field of the projectile ion. These calculations are shown tomore » be in agreement with our data at [theta]=0[degree] where only 2[ital s] and 2[ital p] target electrons are considered.« less

Experimental and theoretical investigation of radiation and dynamics properties in laser-produced carbon plasmas

NASA Astrophysics Data System (ADS)

Min, Qi; Su, Maogen; Wang, Bo; Cao, Shiquan; Sun, Duixiong; Dong, Chenzhong

2018-05-01

The radiation and dynamics properties of laser-produced carbon plasma in vacuum were studied experimentally with aid of a spatio-temporally resolved emission spectroscopy technique. In addition, a radiation hydrodynamics model based on the fluid dynamic equations and the radiative transfer equation was presented, and calculation of the charge states was performed within the time-dependent collisional radiative model. Detailed temporal and spatial evolution behavior about plasma parameters have been analyzed, such as velocity, electron temperature, charge state distribution, energy level population, and various atomic processes. At the same time, the effects of different atomic processes on the charge state distribution were examined. Finally, the validity of assuming a local thermodynamic equilibrium in the carbon plasma expansion was checked, and the results clearly indicate that the assumption was valid only at the initial (<80 ns) stage of plasma expansion. At longer delay times, it was not applicable near the plasma boundary because of a sharp drop of plasma temperature and electron density.

Electronic properties of disordered Weyl semimetals at charge neutrality

NASA Astrophysics Data System (ADS)

Holder, Tobias; Huang, Chia-Wei; Ostrovsky, Pavel M.

2017-11-01

Weyl semimetals have been intensely studied as a three-dimensional realization of a Dirac-like excitation spectrum where the conduction bands and valence bands touch at isolated Weyl points in momentum space. Like in graphene, this property entails various peculiar electronic properties. However, recent theoretical studies have suggested that resonant scattering from rare regions can give rise to a nonzero density of states even at charge neutrality. Here, we give a detailed account of this effect and demonstrate how the semimetallic nature is suppressed at the lowest scales. To this end, we develop a self-consistent T -matrix approach to investigate the density of states beyond the limit of weak disorder. Our results show a nonvanishing density of states at the Weyl point, which exhibits a nonanalytic dependence on the impurity density. This unusually strong effect of rare regions leads to a revised estimate for the conductivity close to the Weyl point and emphasizes possible deviations from semimetallic behavior in dirty Weyl semimetals at charge neutrality even with very low impurity concentration.

Charge Transfer Enhancement in the D-π-A Type Porphyrin Dyes: A Density Functional Theory (DFT) and Time-Dependent Density Functional Theory (TD-DFT) Study.

PubMed

Kang, Guo-Jun; Song, Chao; Ren, Xue-Feng

2016-11-25

The electronic geometries and optical properties of two D-π-A type zinc porphyrin dyes (NCH₃-YD2 and TPhe-YD) were systematically investigated by density functional theory (DFT) and time-dependent density functional theory (TD-DFT) to reveal the origin of significantly altered charge transfer enhancement by changing the electron donor of the famous porphyrin-based sensitizer YD2-o-C8. The molecular geometries and photophysical properties of dyes before and after binding to the TiO₂ cluster were fully investigated. From the analyses of natural bond orbital (NBO), extended charge decomposition analysis (ECDA), and electron density variations (Δρ) between the excited state and ground state, it was found that the introduction of N(CH₃)₂ and 1,1,2-triphenylethene groups enhanced the intramolecular charge-transfer (ICT) character compared to YD2-o-C8. The absorption wavelength and transition possess character were significantly influenced by N(CH₃)₂ and 1,1,2-triphenylethene groups. NCH₃-YD2 with N(CH₃)₂ groups in the donor part is an effective way to improve the interactions between the dyes and TiO₂ surface, light having efficiency (LHE), and free energy change (ΔG inject ), which is expected to be an efficient dye for use in dye-sensitized solar cells (DSSCs).

Charge movement in gating-locked HCN channels reveals weak coupling of voltage sensors and gate.

PubMed

Ryu, Sujung; Yellen, Gary

2012-11-01

HCN (hyperpolarization-activated cyclic nucleotide gated) pacemaker channels have an architecture similar to that of voltage-gated K(+) channels, but they open with the opposite voltage dependence. HCN channels use essentially the same positively charged voltage sensors and intracellular activation gates as K(+) channels, but apparently these two components are coupled differently. In this study, we examine the energetics of coupling between the voltage sensor and the pore by using cysteine mutant channels for which low concentrations of Cd(2+) ions freeze the open-closed gating machinery but still allow the sensors to move. We were able to lock mutant channels either into open or into closed states by the application of Cd(2+) and measure the effect on voltage sensor movement. Cd(2+) did not immobilize the gating charge, as expected for strict coupling, but rather it produced shifts in the voltage dependence of voltage sensor charge movement, consistent with its effect of confining transitions to either closed or open states. From the magnitude of the Cd(2+)-induced shifts, we estimate that each voltage sensor produces a roughly three- to sevenfold effect on the open-closed equilibrium, corresponding to a coupling energy of ∼1.3-2 kT per sensor. Such coupling is not only opposite in sign to the coupling in K(+) channels, but also much weaker.

Charge storage in oxygen deficient phases of TiO2: defect Physics without defects.

PubMed

Padilha, A C M; Raebiger, H; Rocha, A R; Dalpian, G M

2016-07-01

Defects in semiconductors can exhibit multiple charge states, which can be used for charge storage applications. Here we consider such charge storage in a series of oxygen deficient phases of TiO2, known as Magnéli phases. These Magnéli phases (TinO2n-1) present well-defined crystalline structures, i.e., their deviation from stoichiometry is accommodated by changes in space group as opposed to point defects. We show that these phases exhibit intermediate bands with an electronic quadruple donor transitions akin to interstitial Ti defect levels in rutile TiO2. Thus, the Magnéli phases behave as if they contained a very large pseudo-defect density: ½ per formula unit TinO2n-1. Depending on the Fermi Energy the whole material will become charged. These crystals are natural charge storage materials with a storage capacity that rivals the best known supercapacitors.

The Role of Solution Conditions in the Bacteriophage PP7 Capsid Charge Regulation

DOE PAGES

Nap, Rikkert J.; Bozic, Anze Losdorfer; Szleifer, Igal; ...

2014-10-21

Here, we investigate and quantify the effects of pH and salt concentration on the charge regulation of the bacteriophage PP7 capsid. These effects are found to be extremely important and substantial, introducing qualitative changes in the charge state of the capsid such as a transition from net-positive to net-negative charge depending on the solution pH. The overall charge of the virus capsid arises as a consequence of a complicated balance with the chemical dissociation equilibrium of the amino acids and the electrostatic interaction between them, and the translational entropy of the mobile solution ions, i.e., counterion release. We show thatmore » to properly describe and predict the charging equilibrium of viral capsids in general, one needs to include molecular details as exemplified by the acid-base equilibrium of the detailed distribution of amino acids in the proteinaceous capsid shell.« less

Carrier Propagation Dependence on Applied Potentials in Pentacene Organic Field Effect Transistors Investigated by Impedance Spectroscopy and Electrical Time-of-Flight Techniques

NASA Astrophysics Data System (ADS)

Lin, Jack; Weis, Martin; Taguchi, Dai; Manaka, Takaaki; Iwamoto, Mitsumasa

2011-04-01

Transient measurements of impedance spectroscopy and electrical time-of-flight (TOF) techniques were used for the evaluation of carrier propagation dependence on applied potentials in a pentacene organic field effect transistor (OFET). These techniques are based on carrier propagation, thus isolates the effect of charge density. The intrinsic mobility which is free from contact resistance effects was obtained by measurement of various channel lengths. The obtained intrinsic mobility shows good correspondence with steady-state current-voltage measurement's saturation mobility. However, their power law relations on mobility vs applied potential resulted in different exponents, suggesting different carrier propagation mechanisms, which is attributable to filling of traps or space charge field in the channel region. The hypothesis was verified by a modified electrical TOF experiment which demonstrated how the accumulated charges in the channel influence the effective mobility.

Long-range correction for tight-binding TD-DFT

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

Humeniuk, Alexander; Mitrić, Roland, E-mail: roland.mitric@uni-wuerzburg.de

2015-10-07

We present two improvements to the tight-binding approximation of time-dependent density functional theory (TD-DFTB): First, we add an exact Hartree-Fock exchange term, which is switched on at large distances, to the ground state Hamiltonian and similarly to the coupling matrix that enters the linear response equations for the calculation of excited electronic states. We show that the excitation energies of charge transfer states are improved relative to the standard approach without the long-range correction by testing the method on a set of molecules from the database in Peach et al. [J. Chem. Phys. 128, 044118 (2008)] which are known tomore » exhibit problematic charge transfer states. The degree of spatial overlap between occupied and virtual orbitals indicates where TD-DFTB and long-range corrected TD-DFTB (lc-TD-DFTB) can be expected to produce large errors. Second, we improve the calculation of oscillator strengths. The transition dipoles are obtained from Slater Koster files for the dipole matrix elements between valence orbitals. In particular, excitations localized on a single atom, which appear dark when using Mulliken transition charges, acquire a more realistic oscillator strength in this way. These extensions pave the way for using lc-TD-DFTB to describe the electronic structure of large chromophoric polymers, where uncorrected TD-DFTB fails to describe the high degree of conjugation and produces spurious low-lying charge transfer states.« less

Improved continuum lowering calculations in screened hydrogenic model with l-splitting for high energy density systems

NASA Astrophysics Data System (ADS)

Ali, Amjad; Shabbir Naz, G.; Saleem Shahzad, M.; Kouser, R.; Aman-ur-Rehman; Nasim, M. H.

2018-03-01

The energy states of the bound electrons in high energy density systems (HEDS) are significantly affected due to the electric field of the neighboring ions. Due to this effect bound electrons require less energy to get themselves free and move into the continuum. This phenomenon of reduction in potential is termed as ionization potential depression (IPD) or the continuum lowering (CL). The foremost parameter to depict this change is the average charge state, therefore accurate modeling for CL is imperative in modeling atomic data for computation of radiative and thermodynamic properties of HEDS. In this paper, we present an improved model of CL in the screened hydrogenic model with l-splitting (SHML) proposed by G. Faussurier and C. Blancard, P. Renaudin [High Energy Density Physics 4 (2008) 114] and its effect on average charge state. We propose the level charge dependent calculation of CL potential energy and inclusion of exchange and correlation energy in SHML. By doing this, we made our model more relevant to HEDS and free from CL empirical parameter to the plasma environment. We have implemented both original and modified model of SHML in our code named OPASH and benchmark our results with experiments and other state-of-the-art simulation codes. We compared our results of average charge state for Carbon, Beryllium, Aluminum, Iron and Germanium against published literature and found a very reasonable agreement between them.

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

Lopez-Bezanilla, Alejandro

By means of a multi-scale first-principles approach, a description of the local electronic structure of 2D and narrow phosphorene sheets with various types of modifications is presented. Firtly, a rational argument based on the geometry of the pristine and modified P network, and supported by the Wannier functions formalism is introduced to describe a hybridization model of the P atomic orbitals. Ab initio calculations show that non-isoelectronic foreign atoms form quasi-bound states at varying energy levels and create different polarization states depending on the number of valence electrons between P and the doping atom. The quantum transport properties of modifiedmore » phosphorene ribbons are further described with great accuracy. The distortions on the electronic bands induced by the external species lead to strong backscattering effects on the propagating charge carriers. Depending on the energy of the charge carrier and the type of doping, the conduction may range from the diffusive to the localized regime. Interstitial defects at vacant sites lead to homogeneous transport fingerprints across different types of doping atoms. We suggest that the relatively low values of charge mobility reported in experimental measurements may have its origin in the presence of defects.« less

Electronic structure of charge- and spin-controlled Sr(1-(x+y))La(x+y)Ti(1-x)Cr(x)O3.

PubMed

Iwasawa, H; Yamakawa, K; Saitoh, T; Inaba, J; Katsufuji, T; Higashiguchi, M; Shimada, K; Namatame, H; Taniguchi, M

2006-02-17

We present the electronic structure of Sr(1-(x+y))La(x+y)Ti(1-x)Cr(x)O3 investigated by high-resolution photoemission spectroscopy. In the vicinity of the Fermi level, it was found that the electronic structure was composed of a Cr 3d local state with the t(2g)3 configuration and a Ti 3d itinerant state. The energy levels of these Cr and Ti 3d states are well interpreted by the difference of the charge-transfer energy of both ions. The spectral weight of the Cr 3d state is completely proportional to the spin concentration x irrespective of the carrier concentration y, indicating that the spin density can be controlled by x as desired. In contrast, the spectral weight of the Ti 3d state is not proportional to y, depending on the amount of Cr doping.

Molecular understanding of osmosis in semipermeable membranes.

PubMed

Raghunathan, A V; Aluru, N R

2006-07-14

We investigate single-file osmosis of water through a semipermeable membrane with an uncharged, a positively and a negatively charged nanopore. Molecular dynamics simulations indicate that the osmotic flux through a negatively charged pore (J_) is higher compared to the osmotic flux in a positively charged pore (J+) followed by the osmotic flux in the uncharged pore (J(0)), i.e., J_ > J+ > J(0). The molecular mechanisms governing osmosis, steady state osmosis, and the observed osmotic flux dependence on the nanopore charge are explained by computing all the molecular interactions involved and identifying the molecular interactions that play an important role during and after osmosis. This study helps in a fundamental understanding of osmosis and in the design of advanced nanoporous membranes for various applications of osmosis.

Excited state intramolecular charge transfer reaction in nonaqueous electrolyte solutions: Temperature dependence

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

Pradhan, Tuhin; Gazi, Harun Al Rasid; Biswas, Ranjit

2009-08-07

Temperature dependence of the excited state intramolecular charge transfer reaction of 4-(1-azetidinyl)benzonitrile (P4C) in ethyl acetate (EA), acetonitrile (ACN), and ethanol at several concentrations of lithium perchlorate (LiClO{sub 4}) has been investigated by using the steady state and time resolved fluorescence spectroscopic techniques. The temperature range considered is 267-343 K. The temperature dependent spectral peak shifts and reaction driving force (-{Delta}G{sub r}) in electrolyte solutions of these solvents can be explained qualitatively in terms of interaction between the reactant molecule and ion-atmosphere. Time resolved studies indicate that the decay kinetics of P4C is biexponential, regardless of solvents, LiClO{sub 4} concentrations,more » and temperatures considered. Except at higher electrolyte concentrations in EA, reaction rates in solutions follow the Arrhenius-type temperature dependence where the estimated activation energy exhibits substantial electrolyte concentration dependence. The average of the experimentally measured activation energies in these three neat solvents is found to be in very good agreement with the predicted value based on data in room temperature solvents. While the rate constant in EA shows a electrolyte concentration induced parabolic dependence on reaction driving force (-{Delta}G{sub r}), the former in ethanol and ACN increases only linearly with the increase in driving force (-{Delta}G{sub r}). The data presented here also indicate that the step-wise increase in solvent reorganization energy via sequential addition of electrolyte induces the ICT reaction in weakly polar solvents to crossover from the Marcus inverted region to the normal region.« less

Pressure Dependence of the Charge-Density-Wave Gap in Rare-Earth Tri-Tellurides

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

Sacchetti, A.; /Zurich, ETH; Arcangeletti, E.

2009-12-14

We investigate the pressure dependence of the optical properties of CeTe{sub 3}, which exhibits an incommensurate charge-density-wave (CDW) state already at 300 K. Our data are collected in the mid-infrared spectral range at room temperature and at pressures between 0 and 9 GPa. The energy for the single particle excitation across the CDW gap decreases upon increasing the applied pressure, similarly to the chemical pressure by rare-earth substitution. The broadening of the bands upon lattice compression removes the perfect nesting condition of the Fermi surface and therefore diminishes the impact of the CDW transition on the electronic properties of RTe{submore » 3}.« less

Electronic structure and charge transfer excited states of endohedral fullerene containing electron donoracceptor complexes utilized in organic photovoltaics

NASA Astrophysics Data System (ADS)

Amerikheirabadi, Fatemeh

Organic Donor-Acceptor complexes form the main component of the organic photovoltaic devices (OPVs). The open circuit voltage of OPVs is directly related to the charge transfer excited state energies of these complexes. Currently a large number of different molecular complexes are being tested for their efficiency in photovoltaic devices. In this work, density functional theory as implemented in the NRLMOL code is used to investigate the electronic structure and related properties of these donor-acceptor complexes. The charge transfer excitation energies are calculated using the perturbative delta self-consistent field method recently developed in our group as the standard time dependent density functional approaches fail to accurately provide them. The model photovoltaics systems analyzed are as follows: Sc3N C 80--ZnTPP, Y3 N C80-- ZnTPP and Sc3 N C80-- ZnPc. In addition, a thorough analysis of the isolated donor and acceptor molecules is also provided. The studied acceptors are chosen from a class of fullerenes named trimetallic nitride endohedral fullerenes. These molecules have shown to possess advantages as acceptors such as long lifetimes of the charge-separated states.

State-conditional coherent charge qubit oscillations in a Si/SiGe quadruple quantum dot

NASA Astrophysics Data System (ADS)

Ward, Daniel R.; Kim, Dohun; Savage, Donald E.; Lagally, Max G.; Foote, Ryan H.; Friesen, Mark; Coppersmith, Susan N.; Eriksson, Mark A.

2016-10-01

Universal quantum computation requires high-fidelity single-qubit rotations and controlled two-qubit gates. Along with high-fidelity single-qubit gates, strong efforts have been made in developing robust two-qubit logic gates in electrically gated quantum dot systems to realise a compact and nanofabrication-compatible architecture. Here we perform measurements of state-conditional coherent oscillations of a charge qubit. Using a quadruple quantum dot formed in a Si/SiGe heterostructure, we show the first demonstration of coherent two-axis control of a double quantum dot charge qubit in undoped Si/SiGe, performing Larmor and Ramsey oscillation measurements. We extract the strength of the capacitive coupling between a pair of double quantum dots by measuring the detuning energy shift (≈75 μeV) of one double dot depending on the excess charge configuration of the other double dot. We further demonstrate that the strong capacitive coupling allows fast, state-conditional Landau-Zener-Stückelberg oscillations with a conditional π phase flip time of about 80 ps, showing a promising pathway towards multi-qubit entanglement and control in semiconductor quantum dots.

State-conditional coherent charge qubit oscillations in a Si/SiGe quadruple quantum dot

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

Ward, Daniel R.; Kim, Dohun; Savage, Donald E.

Universal quantum computation requires high-fidelity single-qubit rotations and controlled two-qubit gates. Along with high-fidelity single-qubit gates, strong efforts have been made in developing robust two-qubit logic gates in electrically gated quantum dot systems to realise a compact and nanofabrication-compatible architecture. Here we perform measurements of state-conditional coherent oscillations of a charge qubit. Using a quadruple quantum dot formed in a Si/SiGe heterostructure, we show the first demonstration of coherent two-axis control of a double quantum dot charge qubit in undoped Si/SiGe, performing Larmor and Ramsey oscillation measurements. We extract the strength of the capacitive coupling between a pair of doublemore » quantum dots by measuring the detuning energy shift (≈75 μeV) of one double dot depending on the excess charge configuration of the other double dot. Finally, we further demonstrate that the strong capacitive coupling allows fast, state-conditional Landau–Zener–Stückelberg oscillations with a conditional π phase flip time of about 80 ps, showing a promising pathway towards multi-qubit entanglement and control in semiconductor quantum dots.« less

State-conditional coherent charge qubit oscillations in a Si/SiGe quadruple quantum dot

DOE PAGES

Ward, Daniel R.; Kim, Dohun; Savage, Donald E.; ...

2016-10-18

Universal quantum computation requires high-fidelity single-qubit rotations and controlled two-qubit gates. Along with high-fidelity single-qubit gates, strong efforts have been made in developing robust two-qubit logic gates in electrically gated quantum dot systems to realise a compact and nanofabrication-compatible architecture. Here we perform measurements of state-conditional coherent oscillations of a charge qubit. Using a quadruple quantum dot formed in a Si/SiGe heterostructure, we show the first demonstration of coherent two-axis control of a double quantum dot charge qubit in undoped Si/SiGe, performing Larmor and Ramsey oscillation measurements. We extract the strength of the capacitive coupling between a pair of doublemore » quantum dots by measuring the detuning energy shift (≈75 μeV) of one double dot depending on the excess charge configuration of the other double dot. Finally, we further demonstrate that the strong capacitive coupling allows fast, state-conditional Landau–Zener–Stückelberg oscillations with a conditional π phase flip time of about 80 ps, showing a promising pathway towards multi-qubit entanglement and control in semiconductor quantum dots.« less

Solution Phase Exciton Diffusion Dynamics of a Charge-Transfer Copolymer PTB7 and a Homopolymer P3HT

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

Cho, Sung; Rolczynski, Brian S.; Xu, Tao

2015-06-18

Using ultrafast polarization-controlled transient absorption (TA) measurements, dynamics of the initial exciton states were investigated on the time scale of tens of femtoseconds to about 80 ps in two different types of conjugated polymers extensively used in active layers of organic photovoltaic devices. These polymers are poly(3-fluorothienothiophenebenzodithiophene) (PTB7) and poly-3-hexylthiophene (P3HT), which are charge-transfer polymers and homopolymers, respectively. In PTB7, the initial excitons with excess vibrational energy display two observable ultrafast time constants, corresponding to coherent exciton diffusion before the vibrational relaxation, and followed by incoherent exciton diffusion processes to a neighboring local state after the vibrational relaxation. In contrast,more » P3HT shows only one exciton diffusion or conformational motion time constant of 34 ps, even though its exciton decay kinetics are multiexponential. Based on the experimental results, an exciton dynamics mechanism is conceived taking into account the excitation energy and structural dependence in coherent and incoherent exciton diffusion processes, as well as other possible deactivation processes including the formation of the pseudo-charge-transfer and charge separate states, as well as interchain exciton hopping or coherent diffusion.« less

Solution Phase Exciton Diffusion Dynamics of a Charge-Transfer Copolymer PTB7 and a Homopolymer P3HT.

PubMed

Cho, Sung; Rolczynski, Brian S; Xu, Tao; Yu, Luping; Chen, Lin X

2015-06-18

Using ultrafast polarization-controlled transient absorption (TA) measurements, dynamics of the initial exciton states were investigated on the time scale of tens of femtoseconds to about 80 ps in two different types of conjugated polymers extensively used in active layers of organic photovoltaic devices. These polymers are poly(3-fluorothienothiophenebenzodithiophene) (PTB7) and poly-3-hexylthiophene (P3HT), which are charge-transfer polymers and homopolymers, respectively. In PTB7, the initial excitons with excess vibrational energy display two observable ultrafast time constants, corresponding to coherent exciton diffusion before the vibrational relaxation, and followed by incoherent exciton diffusion processes to a neighboring local state after the vibrational relaxation. In contrast, P3HT shows only one exciton diffusion or conformational motion time constant of 34 ps, even though its exciton decay kinetics are multiexponential. Based on the experimental results, an exciton dynamics mechanism is conceived taking into account the excitation energy and structural dependence in coherent and incoherent exciton diffusion processes, as well as other possible deactivation processes including the formation of the pseudo-charge-transfer and charge separate states, as well as interchain exciton hopping or coherent diffusion.

The Long-Term Performance of Small-Cell Batteries Without Cell-Balancing Electronics

NASA Technical Reports Server (NTRS)

Pearson, C.; Thwaite, C.; Curzon, D.; Rao, G.

2006-01-01

Tests approx.8 yrs ago showed Sony HC do not imbalance. AEA developed a theory (ESPC 2002): a) Self-discharge (SD) decreases with state-of-charge (SOC); b) Cells diverge to a state of dynamic equilibrium; c) Equilibrium spread depends on cell SD uniformity. Balancing model verified against test data. Short-term measures of SD difficult in Sony cells and very small values, depends on technique. Long-term evidence supports lower SD at low SD. Battery testing best proof of performance, typically mission specific tests.

Atomic and electronic structure of trilayer graphene/SiC(0001): Evidence of Strong Dependence on Stacking Sequence and charge transfer.

PubMed

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.

Symmetry lowering of pentacene molecular states interacting with a Cu surface

NASA Astrophysics Data System (ADS)

Baldacchini, Chiara; Mariani, Carlo; Betti, Maria Grazia; Vobornik, Ivana; Fujii, Jun; Annese, Emilia; Rossi, Giorgio; Ferretti, Andrea; Calzolari, Arrigo; di Felice, Rosa; Ruini, Alice; Molinari, Elisa

2007-12-01

Pentacene adsorbed on the Cu(119) vicinal surface forms long-range ordered chain structures. Photoemission spectroscopy measurements and ab initio density functional theory simulations provide consistent evidences that pentacene molecular orbitals mix with the copper bands, giving rise to interaction states localized at the interface. Angular-resolved and polarization dependent photoemission spectroscopy shows that most of the pentacene derived intensity is strongly dichroic. The symmetry of the molecular states of the free pentacene molecules is reduced upon adsorption on Cu(119), as a consequence of the molecule-metal interaction. Theoretical results show a redistribution of the charge density in π molecular states close to the Fermi level, consistent with the photoemission intensities (density of states) and polarization dependence (orbital symmetry).

Charge-state dependence of binary-encounter-electron cross sections and peak energies

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

Hidmi, H.I.; Richard, P.; Sanders, J.M.

The charge-state dependence of the binary-encounter-electron (BEE) double-differential cross section (DDCS) at 0[degree] with respect to the beam direction resulting from collisions of 1 MeV/amu H[sup +], C[sup [ital q]+], N[sup [ital q]+], O[sup [ital q]+], F[sup [ital q]+], Si[sup [ital q]+], and Cl[sup [ital q]+], and 0.5 MeV/amu Cu[sup [ital q]+] with H[sub 2] is reported. The data show an enhancement in the BEE DDCS as the charge state of the projectile is decreased, in agreement with the data reported by Richard [ital et] [ital al]. [J. Phys. B 23, L213 (1990)]. The DDCS enhancement ratios observed for themore » three-electron isoelectronic sequence C[sup 3+]:C[sup 6+], N[sup 4+]:N[sup 7+], O[sup 5+]:O[sup 8+], and F[sup 6+]:F[sup 9+] are about 1.35, whereas a DDCS enhancement of 3.5 was observed for Cu[sup 4+]. The BEE enhancement with increasing electrons on the projectile has been shown by several authors to be due to the non-Coulomb static potential of the projectile and additionally to the [ital e]-[ital e] exchange interaction. An impulse-approximation (IA) model fits the shape of the BEE DDCS and predicts a [ital Z][sub [ital p

Charge-state dynamics in electrostatic force spectroscopy

NASA Astrophysics Data System (ADS)

Ondráček, Martin; Hapala, Prokop; Jelínek, Pavel

2016-07-01

We present a numerical model that allows us to study the response of an oscillating probe in electrostatic force spectroscopy to charge switching in quantum dots at various time scales. The model provides more insight into the behavior of frequency shift and dissipated energy under different scanning conditions when measuring a temporarily charged quantum dot on a surface. Namely, we analyze the dependence of the frequency shift, the dissipated energy, and their fluctuations on the resonance frequency of the tip and on the electron tunneling rates across the tip-quantum dot and quantum dot-sample junctions. We discuss two complementary approaches to simulating the charge dynamics, a stochastic and a deterministic one. In addition, we derive analytic formulas valid for small amplitudes, describing relations between the frequency shift, dissipated energy, and the characteristic rates driving the charging and discharging processes.

Solvent effects in time-dependent self-consistent field methods. I. Optical response calculations

DOE PAGES

Bjorgaard, J. A.; Kuzmenko, V.; Velizhanin, K. A.; ...

2015-01-22

In this study, we implement and examine three excited state solvent models in time-dependent self-consistent field methods using a consistent formalism which unambiguously shows their relationship. These are the linear response, state specific, and vertical excitation solvent models. Their effects on energies calculated with the equivalent of COSMO/CIS/AM1 are given for a set of test molecules with varying excited state charge transfer character. The resulting solvent effects are explained qualitatively using a dipole approximation. It is shown that the fundamental differences between these solvent models are reflected by the character of the calculated excitations.

Total Charge Movement per Channel

PubMed Central

Sigg, Daniel; Bezanilla, Francisco

1997-01-01

One measure of the voltage dependence of ion channel conductance is the amount of gating charge that moves during activation and vice versa. The limiting slope method, introduced by Almers (Almers, W. 1978. Rev. Physiol. Biochem. Pharmacol. 82:96–190), exploits the relationship of charge movement and voltage sensitivity, yielding a lower limit to the range of single channel gating charge displacement. In practice, the technique is plagued by low experimental resolution due to the requirement that the logarithmic voltage sensitivity of activation be measured at very low probabilities of opening. In addition, the linear sequential models to which the original theory was restricted needed to be expanded to accommodate the complexity of mechanisms available for the activation of channels. In this communication, we refine the theory by developing a relationship between the mean activation charge displacement (a measure of the voltage sensitivity of activation) and the gating charge displacement (the integral of gating current). We demonstrate that recording the equilibrium gating charge displacement as an adjunct to the limiting slope technique greatly improves accuracy under conditions where the plots of mean activation charge displacement and gross gating charge displacement versus voltage can be superimposed. We explore this relationship for a wide variety of channel models, which include those having a continuous density of states, nonsequential activation pathways, and subconductance states. We introduce new criteria for the appropriate use of the limiting slope procedure and provide a practical example of the theory applied to low resolution simulation data. PMID:8997663

Insulator-semiconductor interface fixed charges in AlGaN/GaN metal-insulator-semiconductor devices with Al2O3 or AlTiO gate dielectrics

NASA Astrophysics Data System (ADS)

Le, Son Phuong; Nguyen, Duong Dai; Suzuki, Toshi-kazu

2018-01-01

We have investigated insulator-semiconductor interface fixed charges in AlGaN/GaN metal-insulator-semiconductor (MIS) devices with Al2O3 or AlTiO (an alloy of Al2O3 and TiO2) gate dielectrics obtained by atomic layer deposition on AlGaN. Analyzing insulator-thickness dependences of threshold voltages for the MIS devices, we evaluated positive interface fixed charges, whose density at the AlTiO/AlGaN interface is significantly lower than that at the Al2O3/AlGaN interface. This and a higher dielectric constant of AlTiO lead to rather shallower threshold voltages for the AlTiO gate dielectric than for Al2O3. The lower interface fixed charge density also leads to the fact that the two-dimensional electron concentration is a decreasing function of the insulator thickness for AlTiO, whereas being an increasing function for Al2O3. Moreover, we discuss the relationship between the interface fixed charges and interface states. From the conductance method, it is shown that the interface state densities are very similar at the Al2O3/AlGaN and AlTiO/AlGaN interfaces. Therefore, we consider that the lower AlTiO/AlGaN interface fixed charge density is not owing to electrons trapped at deep interface states compensating the positive fixed charges and can be attributed to a lower density of oxygen-related interface donors.

Building better water models using the shape of the charge distribution of a water molecule

NASA Astrophysics Data System (ADS)

Dharmawardhana, Chamila Chathuranga; Ichiye, Toshiko

2017-11-01

The unique properties of liquid water apparently arise from more than just the tetrahedral bond angle between the nuclei of a water molecule since simple three-site models of water are poor at mimicking these properties in computer simulations. Four- and five-site models add partial charges on dummy sites and are better at modeling these properties, which suggests that the shape of charge distribution is important. Since a multipole expansion of the electrostatic potential describes a charge distribution in an orthogonal basis set that is exact in the limit of infinite order, multipoles may be an even better way to model the charge distribution. In particular, molecular multipoles up to the octupole centered on the oxygen appear to describe the electrostatic potential from electronic structure calculations better than four- and five-site models, and molecular multipole models give better agreement with the temperature and pressure dependence of many liquid state properties of water while retaining the computational efficiency of three-site models. Here, the influence of the shape of the molecular charge distribution on liquid state properties is examined by correlating multipoles of non-polarizable water models with their liquid state properties in computer simulations. This will aid in the development of accurate water models for classical simulations as well as in determining the accuracy needed in quantum mechanical/molecular mechanical studies and ab initio molecular dynamics simulations of water. More fundamentally, this will lead to a greater understanding of how the charge distribution of a water molecule leads to the unique properties of liquid water. In particular, these studies indicate that p-orbital charge out of the molecular plane is important.

Charging performance of automotive batteries-An underestimated factor influencing lifetime and reliable battery operation

NASA Astrophysics Data System (ADS)

Sauer, Dirk Uwe; Karden, Eckhard; Fricke, Birger; Blanke, Holger; Thele, Marc; Bohlen, Oliver; Schiffer, Julia; Gerschler, Jochen Bernhard; Kaiser, Rudi

Dynamic charge acceptance and charge acceptance under constant voltage charging conditions are for two reasons essential for lead-acid battery operation: energy efficiency in applications with limited charging time (e.g. PV systems or regenerative braking in vehicles) and avoidance of accelerated ageing due to sulphation. Laboratory tests often use charge regimes which are beneficial for the battery life, but which differ significantly from the operating conditions in the field. Lead-acid batteries in applications with limited charging time and partial-state-of-charge operation are rarely fully charged due to their limited charge acceptance. Therefore, they suffer from sulphation and early capacity loss. However, when appropriate charging strategies are applied most of the lost capacity and thus performance for the user may be recovered. The paper presents several aspects of charging regimes and charge acceptance. Theoretical and experimental investigations show that temperature is the most critical parameter. Full charging within short times can be achieved only at elevated temperatures. A strong dependency of the charge acceptance during charging pulses on the pre-treatment of the battery can be observed, which is not yet fully understood. But these effects have a significant impact on the fuel efficiency of micro-hybrid electric vehicles.

Self-force as probe of internal structure

NASA Astrophysics Data System (ADS)

Isoyama, Soichiro; Poisson, Eric

2012-08-01

The self-force acting on a (scalar or electric) charge held in place outside a massive body contains information about the body’s composition, and can therefore be used as a probe of internal structure. We explore this theme by computing the (scalar or electromagnetic) self-force when the body is a spherical ball of perfect fluid in hydrostatic equilibrium, under the assumption that its rest-mass density and pressure are related by a polytropic equation of state. The body is strongly self-gravitating, and all computations are performed in exact general relativity. The dependence on internal structure is best revealed by expanding the self-force in powers of r-10, with r0 denoting the radial position of the charge outside the body. To the leading order, the self-force scales as r-30 and depends only on the square of the charge and the body’s mass; the leading self-force is universal. The dependence on internal structure is seen at the next order, r-50, through a structure factor that depends on the equation of state. We compute this structure factor for relativistic polytropes, and show that for a fixed mass, it increases linearly with the body’s radius in the case of the scalar self-force, and quadratically with the body’s radius in the case of the electromagnetic self-force. In both cases we find that for a fixed mass and radius, the self-force is smaller if the body is more centrally dense, and larger if the mass density is more uniformly distributed.

In-situ time-of-flight neutron diffraction study of the structure evolution of electrode materials in a commercial battery with LiNi0.8Co0.15Al0.05O2 cathode

NASA Astrophysics Data System (ADS)

Bobrikov, I. A.; Samoylova, N. Yu.; Sumnikov, S. V.; Ivanshina, O. Yu.; Vasin, R. N.; Beskrovnyi, A. I.; Balagurov, A. M.

2017-12-01

A commercial lithium-ion battery with LiNi0.8Co0.15Al0.05O2 (NCA) cathode has been studied in situ using high-intensity and high-resolution neutron diffraction. Structure and phase composition of the battery electrodes have been probed during charge-discharge in different cycling modes. The dependence of the anode composition on the charge rate has been determined quantitatively. Different kinetics of Li (de)intercalation in the graphite anode during charge/discharge process have been observed. Phase separation of the cathode material has not been detected in whole voltage range. Non-linear dependencies of the unit cell parameters, atomic and layer spacing on the lithium content in the cathode have been observed. Measured dependencies of interatomic spacing and interlayer spacing, and unit cell parameters of the cathode structure on the lithium content could be qualitatively explained by several factors, such as variations of oxidation state of cation in oxygen octahedra, Coulomb repulsion of oxygen layers, changes of average effective charge of oxygen layers and van der Waals interactions between MeO2-layers at high level of the NCA delithiation.

Dependence of interface charge trapping on channel engineering in pentacene field effect transistors.

PubMed

Lee, Sunwoo; Park, Junghyuck; Park, In-Sung; Ahn, Jinho

2014-07-01

We investigate the dependence of charge carrier mobility by trap states at various interface regions through channel engineering. Prior to evaluation of interface trap density, the electrical performance in pentaene field effect transistors (FET) with high-k gate oxide are also investigated depending on four channel engineering. As a channel engineering, gas treatment, coatings of thin polymer layer, and chemical surface modification using small molecules were carried out. After channel engineering, the performance of device as well as interface trap density calculated by conductance method are remarkably improved. It is found that the reduced interface trap density is closely related to decreasing the sub-threshold swing and improving the mobility. Particularly, we also found that performance of device such as mobility, subthreshold swing, and interface trap density after gas same is comparable to those of OTS.

Carrier-envelope phase dependence of the directional fragmentation and hydrogen migration in toluene in few-cycle laser fields.

PubMed

Li, Hui; Kling, Nora G; Förg, Benjamin; Stierle, Johannes; Kessel, Alexander; Trushin, Sergei A; Kling, Matthias F; Kaziannis, Spyros

2016-07-01

The dissociative ionization of toluene initiated by a few-cycle laser pulse as a function of the carrier envelope phase (CEP) is investigated using single-shot velocity map imaging. Several ionic fragments, CH3 (+), H2 (+), and H3 (+), originating from multiply charged toluene ions present a CEP-dependent directional emission. The formation of H2 (+) and H3 (+) involves breaking C-H bonds and forming new bonds between the hydrogen atoms within the transient structure of the multiply charged precursor. We observe appreciable intensity-dependent CEP-offsets. The experimental data are interpreted with a mechanism that involves laser-induced coupling of vibrational states, which has been found to play a role in the CEP-control of molecular processes in hydrocarbon molecules, and appears to be of general importance for such complex molecules.

Nickel-cadmium battery system for electric vehicles

NASA Astrophysics Data System (ADS)

Klein, M.; Charkey, A.

A nickel-cadmium battery system has been developed and is being evaluated for electric vehicle propulsion applications. The battery system design features include: (1) air circulation through gaps between cells for thermal management, (2) a metal-gas coulometric fuel gauge for state-of-charge and charge control, and (3) a modified constant current ac/dc power supply for the charger. The battery delivers one and a half to two times the energy density of comparable lead-acid batteries depending on operating conditions.

Pseudo-direct bandgap transitions in silicon nanocrystals: effects on optoelectronics and thermoelectrics.

PubMed

Singh, Vivek; Yu, Yixuan; Sun, Qi-C; Korgel, Brian; Nagpal, Prashant

2014-12-21

While silicon nanostructures are extensively used in electronics, the indirect bandgap of silicon poses challenges for optoelectronic applications like photovoltaics and light emitting diodes (LEDs). Here, we show that size-dependent pseudo-direct bandgap transitions in silicon nanocrystals dominate the interactions between (photoexcited) charge carriers and phonons, and hence the optoelectronic properties of silicon nanocrystals. Direct measurements of the electronic density of states (DOS) for different sized silicon nanocrystals reveal that these pseudo-direct transitions, likely arising from the nanocrystal surface, can couple with the quantum-confined silicon states. Moreover, we demonstrate that since these transitions determine the interactions of charge carriers with phonons, they change the light emission, absorption, charge carrier diffusion and phonon drag (Seebeck coefficient) in nanoscaled silicon semiconductors. Therefore, these results can have important implications for the design of optoelectronics and thermoelectric devices based on nanostructured silicon.

The plasma environment, charge state, and currents of Saturn's C and D rings

NASA Technical Reports Server (NTRS)

Wilson, G. R.

1991-01-01

The charge state and associated currents of Saturn's C an D rings are studied by modeling the flow of ionospheric plasma from the mid- to low-latitude ionosphere to the vicinity of the rings. It is found that the plasma density near the C and D rings, at a given radial location, will experience a one to two order of magnitude diurnal variation. The surface charge density (SCD) of these rings can show significant radial and azimuthal variations due mainly to variation in the plasma density. The SCD also depends on structural features of the rings such as thickness and the nature of the particle size distribution. The associated azimuthal currents carried by these rings also show large diurnal variations resulting in field-aligned currents which close in the ionosphere. The resulting ionospheric electric field will probably not produce a significant amount of plasma convection in the topside ionosphere and inner plasmasphere.

The voltage-dependent anion channel as a biological transistor: theoretical considerations.

PubMed

Lemeshko, V V; Lemeshko, S V

2004-07-01

The voltage-dependent anion channel (VDAC) is a porin of the mitochondrial outer membrane with a bell-shaped permeability-voltage characteristic. This porin restricts the flow of negatively charged metabolites at certain non-zero voltages, and thus might regulate their flux across the mitochondrial outer membrane. Here, we have developed a mathematical model illustrating the possibility of interaction between two steady-state fluxes of negatively charged metabolites circulating across the VDAC in a membrane. The fluxes interact by contributing to generation of the membrane electrical potential with subsequent closure of the VDAC. The model predicts that the VDAC might function as a single-molecule biological transistor and amplifier, because according to the obtained calculations a small change in the flux of one pair of different negatively charged metabolites causes a significant modulation of a more powerful flux of another pair of negatively charged metabolites circulating across the same membrane with the VDAC. Such transistor-like behavior of the VDAC in the mitochondrial outer membrane might be an important principle of the cell energy metabolism regulation under some physiological conditions.

Transient luminescence induced by electrical refilling of charge carrier traps of dislocation network at hydrophilically bonded Si wafers interface

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

Bondarenko, Anton; Vyvenko, Oleg

2014-02-21

Dislocation network (DN) at hydrophilically bonded Si wafers interface is placed in space charge region (SCR) of a Schottky diode at a depth of about 150 nm from Schottky electrode for simultaneous investigation of its electrical and luminescent properties. Our recently proposed pulsed traps refilling enhanced luminescence (Pulsed-TREL) technique based on the effect of transient luminescence induced by refilling of charge carrier traps with electrical pulses is further developed and used as a tool to establish DN energy levels responsible for D1 band of dislocation-related luminescence in Si (DRL). In present work we do theoretical analysis and simulation of trapsmore » refilling kinetics dependence on refilling pulse magnitude (Vp) in two levels model: shallow and deep. The influence of initial charge state of deep level on shallow level occupation-Vp dependence is discussed. Characteristic features predicted by simulations are used for Pulsed-TREL experimental results interpretation. We conclude that only shallow (∼0.1 eV from conduction and valence band) energetic levels in the band gap participate in D1 DRL.« less

Absence of Intramolecular Singlet Fission in Pentacene-Perylenediimide Heterodimers: The Role of Charge Transfer State.

PubMed

Wang, Long; Wu, Yishi; Chen, Jianwei; Wang, Lanfen; Liu, Yanping; Yu, Zhenyi; Yao, Jiannian; Fu, Hongbing

2017-11-16

A new class of donor-acceptor heterodimers based on two singlet fission (SF)-active chromophores, i.e., pentacene (Pc) and perylenediimide (PDI), was developed to investigate the role of charge transfer (CT) state on the excitonic dynamics. The CT state is efficiently generated upon photoexcitation. However, the resulting CT state decays to different energy states depending on the energy levels of the CT state. It undergoes extremely rapid deactivation to the ground state in polar CH 2 Cl 2 , whereas it undergoes transformation to a Pc triplet in nonpolar toluene. The efficient triplet generation in toluene is not due to SF but CT-mediated intersystem crossing. In light of the energy landscape, it is suggested that the deep energy level of the CT state relative to that of the triplet pair state makes the CT state actually serve as a trap state that cannot undergoes an intramolecular singlet fission process. These results provide guidance for the design of SF materials and highlight the requisite for more widely applicable design principles.

pH-Dependent Optical Properties of Synthetic Fluorescent Imidazoles

PubMed Central

Berezin, Mikhail Y.; Kao, Jeff; Achilefu, Samuel

2010-01-01

An imidazole moiety is often found as an integral part of fluorophores in a variety of fluorescent proteins and many such proteins possess pH dependent light emission. In contrast, synthetic fluorescent compounds with incorporated imidazoles are rare and have not been studied as pH probes. In this report, the richness of imidazole optical properties, including pH sensitivity, was demonstrated via a novel imidazole-based fluorophore 1H-imidazol-5-yl-vinyl-benz[e]indolium. Three species corresponding to protonated, neutral and deprotonated imidazoles were identified in the broad range of pH 1-12. The absorption and emission bands of each species were assigned by comparative spectral analysis with synthesized mono- and di-N-methylated fluorescent imidazole analogues. pKa analysis in the ground and the excited states showed photoacidic properties of the fluorescent imidazoles due to the excited state proton transfer (ESPT). This effect was negligible for substituted imidazoles. The assessment of a pH sensitive center in the imidazole ring revealed the switching of the pH sensitive centers from 1-N in the ground state to 3-N in the excited state. The effect was attributed to the unique kind of the excited state charge transfer (ESCT) resulting in a positive charge swapping between two nitrogens. PMID:19212987

Understanding How Isotopes Affect Charge Transfer in P3HT/PCBM: A Quantum Trajectory-Electronic Structure Study with Nonlinear Quantum Corrections

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

Wang, Lei; Jakowski, Jacek; Garashchuk, Sophya

The experimentally observed effect of selective deuterium substitution on the open circuit voltage for a blend of poly(3-hexylthiophene)(P3HT) and [6,6]-phenyl-C 61- butyric acid methyl ester (PCBM) (Nat. Commun. 5:3180, 2014) is explored using a 221-atom model of a polymer-wrapped PCBM molecule. We describe the protonic and deuteronic wavefunctions for the H/D isotopologues of the hexyl side chains within a Quantum Trajectory/Electronic Structure approach where the dynamics is performed with newly developed nonlinear corrections to the quantum forces, necessary to describe the nuclear wavefunctions; the classical forces are generated with a Density Functional Tight Binding method. We used the resulting protonicmore » and deuteronic time-dependent wavefunctions to assess the effects of isotopic substitution (deuteration) on the energy gaps relevant to the charge transfer for the donor and acceptor electronic states. Furthermore, while the isotope effect on the electronic energy levels is found negligible, the quantum-induced fluctuations of the energy gap between the charge transfer and charge separated states due to nuclear wavefunctions may account for experimental trends by promoting charge transfer in P3HT/PCBM and increasing charge recombination on the donor in the deuterium substituted P3HT/PCBM.« less

Understanding How Isotopes Affect Charge Transfer in P3HT/PCBM: A Quantum Trajectory-Electronic Structure Study with Nonlinear Quantum Corrections

DOE PAGES

Wang, Lei; Jakowski, Jacek; Garashchuk, Sophya; ...

2016-08-09

The experimentally observed effect of selective deuterium substitution on the open circuit voltage for a blend of poly(3-hexylthiophene)(P3HT) and [6,6]-phenyl-C 61- butyric acid methyl ester (PCBM) (Nat. Commun. 5:3180, 2014) is explored using a 221-atom model of a polymer-wrapped PCBM molecule. We describe the protonic and deuteronic wavefunctions for the H/D isotopologues of the hexyl side chains within a Quantum Trajectory/Electronic Structure approach where the dynamics is performed with newly developed nonlinear corrections to the quantum forces, necessary to describe the nuclear wavefunctions; the classical forces are generated with a Density Functional Tight Binding method. We used the resulting protonicmore » and deuteronic time-dependent wavefunctions to assess the effects of isotopic substitution (deuteration) on the energy gaps relevant to the charge transfer for the donor and acceptor electronic states. Furthermore, while the isotope effect on the electronic energy levels is found negligible, the quantum-induced fluctuations of the energy gap between the charge transfer and charge separated states due to nuclear wavefunctions may account for experimental trends by promoting charge transfer in P3HT/PCBM and increasing charge recombination on the donor in the deuterium substituted P3HT/PCBM.« less

One-Dimensional Brownian Motion of Charged Nanoparticles along Microtubules: A Model System for Weak Binding Interactions

PubMed Central

Minoura, Itsushi; Katayama, Eisaku; Sekimoto, Ken; Muto, Etsuko

2010-01-01

Abstract Various proteins are known to exhibit one-dimensional Brownian motion along charged rodlike polymers, such as microtubules (MTs), actin, and DNA. The electrostatic interaction between the proteins and the rodlike polymers appears to be crucial for one-dimensional Brownian motion, although the underlying mechanism has not been fully clarified. We examined the interactions of positively-charged nanoparticles composed of polyacrylamide gels with MTs. These hydrophilic nanoparticles bound to MTs and displayed one-dimensional Brownian motion in a charge-dependent manner, which indicates that nonspecific electrostatic interaction is sufficient for one-dimensional Brownian motion. The diffusion coefficient decreased exponentially with an increasing particle charge (with the exponent being 0.10 kBT per charge), whereas the duration of the interaction increased exponentially (exponent of 0.22 kBT per charge). These results can be explained semiquantitatively if one assumes that a particle repeats a cycle of binding to and movement along an MT until it finally dissociates from the MT. During the movement, a particle is still electrostatically constrained in the potential valley surrounding the MT. This entire process can be described by a three-state model analogous to the Michaelis-Menten scheme, in which the two parameters of the equilibrium constant between binding and movement, and the rate of dissociation from the MT, are derived as a function of the particle charge density. This study highlights the possibility that the weak binding interactions between proteins and rodlike polymers, e.g., MTs, are mediated by a similar, nonspecific charge-dependent mechanism. PMID:20409479

One-dimensional Brownian motion of charged nanoparticles along microtubules: a model system for weak binding interactions.

PubMed

Minoura, Itsushi; Katayama, Eisaku; Sekimoto, Ken; Muto, Etsuko

2010-04-21

Various proteins are known to exhibit one-dimensional Brownian motion along charged rodlike polymers, such as microtubules (MTs), actin, and DNA. The electrostatic interaction between the proteins and the rodlike polymers appears to be crucial for one-dimensional Brownian motion, although the underlying mechanism has not been fully clarified. We examined the interactions of positively-charged nanoparticles composed of polyacrylamide gels with MTs. These hydrophilic nanoparticles bound to MTs and displayed one-dimensional Brownian motion in a charge-dependent manner, which indicates that nonspecific electrostatic interaction is sufficient for one-dimensional Brownian motion. The diffusion coefficient decreased exponentially with an increasing particle charge (with the exponent being 0.10 kBT per charge), whereas the duration of the interaction increased exponentially (exponent of 0.22 kBT per charge). These results can be explained semiquantitatively if one assumes that a particle repeats a cycle of binding to and movement along an MT until it finally dissociates from the MT. During the movement, a particle is still electrostatically constrained in the potential valley surrounding the MT. This entire process can be described by a three-state model analogous to the Michaelis-Menten scheme, in which the two parameters of the equilibrium constant between binding and movement, and the rate of dissociation from the MT, are derived as a function of the particle charge density. This study highlights the possibility that the weak binding interactions between proteins and rodlike polymers, e.g., MTs, are mediated by a similar, nonspecific charge-dependent mechanism. Copyright 2010 Biophysical Society. Published by Elsevier Inc. All rights reserved.

Energy relaxation of intense laser pulse-produced plasmas

NASA Astrophysics Data System (ADS)

Shihab, M.; Abou-Koura, G. H.; El-Siragy, N. M.

2016-05-01

We describe a collisional radiative model (CRE) of homogeneously expanded nickel plasmas in vacuum. The CRE model is coupled with two separate electron and ion temperature magneto-hydrodynamic equations. On the output, the model provides the temporal variation of the electron temperature, ion temperature, and average charge state. We demonstrate the effect of three-body recombination ({∝}N_e T^{-9/2}_e) on plasma parameters, as it changes the time dependence of electron temperature from t^{-2} to t^{-1} and exhibits a pronounced effect leading to a freezing feature in the average charge state. In addition, the effect of the three-body recombination on the warm up of ions and delaying the equilibration is addressed.

Molecular structures and excited states of CpM(CO)(2) (Cp = eta(5)-C(5)H(5); M = Rh, Ir) and [Cl(2)Rh(CO)(2)](-). Theoretical evidence for a competitive charge transfer mechanism.

PubMed

Hu, Zhenming; Boyd, Russell J; Nakatsuji, Hiroshi

2002-03-20

Molecular structures and excited states of CpM(CO)(2) (Cp = eta(5)-C(5)H(5); M = Rh, Ir) and [Cl(2)Rh(CO)(2)](-) complexes have been investigated using the B3LYP and the symmetry-adapted cluster (SAC)/SAC-configuration interaction (SAC-CI) theoretical methods. All the dicarbonyl complexes have singlet ground electronic states with large singlet-triplet separations. Thermal dissociations of CO from the parent dicarbonyls are energetically unfavorable. CO thermal dissociation is an activation process for [Cl(2)Rh(CO)(2)](-) while it is a repulsive potential for CpM(CO)(2). The natures of the main excited states of CpM(CO)(2) and [Cl(2)Rh(CO)(2)](-) are found to be quite different. For [Cl(2)Rh(CO)(2)](-), all the strong transitions are identified to be metal to ligand CO charge transfer (MLCT) excitations. A significant feature of the excited states of CpM(CO)(2) is that both MLCT excitation and a ligand Cp to metal and CO charge transfer excitation are strongly mixed in the higher energy states with the latter having the largest oscillator strength. A competitive charge transfer excited state has therefore been identified theoretically for CpRh(CO)(2) and CpIr(CO)(2). The wavelength dependence of the quantum efficiencies for the photoreactions of CpM(CO)(2) reported by Lees et al. can be explained by the existence of two different types of excited states. The origin of the low quantum efficiencies for the C-H/S-H bond activations of CpM(CO)(2) can be attributed to the smaller proportion of the MLCT excitation in the higher energy states.

Mixing of Exciton and Charge-Transfer States in Photosystem II Reaction Centers: Modeling of Stark Spectra with Modified Redfield Theory

PubMed Central

Novoderezhkin, Vladimir I.; Dekker, Jan P.; van Grondelle, Rienk

2007-01-01

We propose an exciton model for the Photosystem II reaction center (RC) based on a quantitative simultaneous fit of the absorption, linear dichroism, circular dichroism, steady-state fluorescence, triplet-minus-singlet, and Stark spectra together with the spectra of pheophytin-modified RCs, and so-called RC5 complexes that lack one of the peripheral chlorophylls. In this model, the excited state manifold includes a primary charge-transfer (CT) state that is supposed to be strongly mixed with the pure exciton states. We generalize the exciton theory of Stark spectra by 1), taking into account the coupling to a CT state (whose static dipole cannot be treated as a small parameter in contrast to usual excited states); and 2), expressing the line shape functions in terms of the modified Redfield approach (the same as used for modeling of the linear responses). This allows a consistent modeling of the whole set of experimental data using a unified physical picture. We show that the fluorescence and Stark spectra are extremely sensitive to the assignment of the primary CT state, its energy, and coupling to the excited states. The best fit of the data is obtained supposing that the initial charge separation occurs within the special-pair PD1PD2. Additionally, the scheme with primary electron transfer from the accessory chlorophyll to pheophytin gave a reasonable quantitative fit. We show that the effectiveness of these two pathways is strongly dependent on the realization of the energetic disorder. Supposing a mixed scheme of primary charge separation with a disorder-controlled competition of the two channels, we can explain the coexistence of fast sub-ps and slow ps components of the Phe-anion formation as revealed by different ultrafast spectroscopic techniques. PMID:17526589

The behavior of exciplex decay processes and interplay of radiationless transition and preliminary reorganization mechanisms of electron transfer in loose and tight pairs of reactants.

PubMed

Kuzmin, Michael G; Soboleva, Irina V; Dolotova, Elena V

2007-01-18

Exciplex emission spectra and rate constants of their decay via internal conversion and intersystem crossing are studied and discussed in terms of conventional radiationless transition approach. Exciplexes of 9-cyanophenanthrene with 1,2,3-trimethoxybenzene and 1,3,5-trimethoxybenzene were studied in heptane, toluene, butyl acetate, dichloromethane, butyronitrile, and acetonitrile. A better description of spectra and rate constants is obtained using 0-0 transition energy and Gauss broadening of vibrational bands rather than the free energy of electron transfer and reorganization energy. The coincidence of parameters describing exciplex emission spectra and dependence of exciplex decay rate constants on energy gap gives the evidence of radiationless quantum transition mechanism rather than thermally activated medium reorganization mechanism of charge recombination in exciplexes and excited charge transfer complexes (contact radical ion pairs) as well as in solvent separated radical ion pairs. Radiationless quantum transition mechanism is shown to provide an appropriate description also for the main features of exergonic excited-state charge separation reactions if fast mutual transformations of loose and tight pairs of reactants are considered. In particular, very fast electron transfer (ET) in tight pairs of reactants with strong electronic coupling of locally excited and charge transfer states can prevent the observation of an inverted region in bimolecular excited-state charge separation even for highly exergonic reactions.

Electrostatic bending response of a charged helix

NASA Astrophysics Data System (ADS)

Zampetaki, A. V.; Stockhofe, J.; Schmelcher, P.

2018-04-01

We explore the electrostatic bending response of a chain of charged particles confined on a finite helical filament. We analyze how the energy difference Δ E between the bent and the unbent helical chain scales with the length of the helical segment and the radius of curvature and identify features that are not captured by the standard notion of the bending rigidity, normally used as a measure of bending tendency in the linear response regime. Using Δ E to characterize the bending response of the helical chain we identify two regimes with qualitatively different bending behaviors for the ground state configuration: the regime of small and the regime of large radius-to-pitch ratio, respectively. Within the former regime, Δ E changes smoothly with the variation of the system parameters. Of particular interest are its oscillations with the number of charged particles encountered for commensurate fillings which yield length-dependent oscillations in the preferred bending direction of the helical chain. We show that the origin of these oscillations is the nonuniformity of the charge distribution caused by the long-range character of the Coulomb interactions and the finite length of the helix. In the second regime of large values of the radius-to-pitch ratio, sudden changes in the ground state structure of the charges occur as the system parameters vary, leading to complex and discontinuous variations in the ground state bending response Δ E .

Tuning the Direction of Intramolecular Charge Transfer and the Nature of the Fluorescent State in a T-Shaped Molecular Dyad.

PubMed

Felouat, Abdellah; D'Aléo, Anthony; Charaf-Eddin, Azzam; Jacquemin, Denis; Le Guennic, Boris; Kim, Eunsun; Lee, Kwang Jin; Woo, Jae Heun; Ribierre, Jean-Charles; Wu, Jeong Weon; Fages, Frédéric

2015-06-18

Controlling photoinduced intramolecular charge transfer at the molecular scale is key to the development of molecular devices for nanooptoelectronics. Here, we describe the design, synthesis, electronic characterization, and photophysical properties of two electron donor-acceptor molecular systems that consist of tolane and BF2-containing curcuminoid chromophoric subunits connected in a T-shaped arrangement. The two π-conjugated segments intersect at the electron acceptor dioxaborine core. From steady-state electronic absorption and fluorescence emission, we find that the photophysics of the dialkylamino-substituted analogue is governed by the occurrence of two closely lying excited states. From DFT calculations, we show that excitation in either of these two states results in a distinct shift of the electron density, whether it occurs along the curcuminoid or tolane moiety. Femtosecond transient absorption spectroscopy confirmed these findings. As a consequence, the nature of the emitting state and the photophysical properties are strongly dependent on solvent polarity. Moreover, these characteristics can also be switched by protonation or complexation at the nitrogen atom of the amino group. These features set new approaches toward the construction of a three-terminal molecular system in which the lateral branch would transduce a change of electronic state and ultimately control charge transport in a molecular-scale device.

Magnetic susceptibility as a direct measure of oxidation state in LiFePO4 batteries and cyclic water gas shift reactors.

PubMed

Kadyk, Thomas; Eikerling, Michael

2015-08-14

The possibility of correlating the magnetic susceptibility to the oxidation state of the porous active mass in a chemical or electrochemical reactor was analyzed. The magnetic permeability was calculated using a hierarchical model of the reactor. This model was applied to two practical examples: LiFePO4 batteries, in which the oxidation state corresponds with the state-of-charge, and cyclic water gas shift reactors, in which the oxidation state corresponds to the depletion of the catalyst. In LiFePO4 batteries phase separation of the lithiated and delithiated phases in the LiFePO4 particles in the positive electrode gives rise to a hysteresis effect, i.e. the magnetic permeability depends on the history of the electrode. During fast charge or discharge, non-uniform lithium distributionin the electrode decreases the hysteresis effect. However, the overall sensitivity of the magnetic response to the state-of-charge lies in the range of 0.03%, which makes practical measurement challenging. In cyclic water gas shift reactors, the sensitivity is 4 orders of magnitude higher and without phase separation, no hysteresis occurs. This shows that the method is suitable for such reactors, in which large changes of the magnetic permeability of the active material occurs.

Probing the solvation structure and dynamics in ionic liquids by time-resolved infrared spectroscopy of 4-(dimethylamino)benzonitrile.

PubMed

Ando, Rômulo A; Brown-Xu, Samantha E; Nguyen, Lisa N Q; Gustafson, Terry L

2017-09-20

In this work we demonstrate the use of the push-pull model system 4-(dimethylamino)benzonitrile (DMABN) as a convenient molecular probe to investigate the local solvation structure and dynamics by means of time-resolved infrared spectroscopy (TRIR). The photochemical features associated with this system provide several advantages due to the high charge separation between the ground and charge transfer states involving the characteristic nitrile bond, and an excited state lifetime that is long enough to observe the slow solvation dynamics in organic solvents and ionic liquids. The conversion from a locally excited state to an intramolecular charge transfer state (LE-ICT) in ionic liquids shows similar kinetic lifetimes in comparison to organic solvents. This similarity confirms that such conversion depends solely on the intramolecular reorganization of DMABN in the excited state, and not by the dynamics of solvation. In contrast, the relative shift of the ν(CN) vibration during the relaxation of the ICT state reveals two distinct lifetimes that are sensitive to the solvent environment. This study reveals a fast time component which is attributed to the dipolar relaxation of the solvent and a slower time component related to the rotation of the dimethylamino group of DMABN.

A Charged Particle Veto Wall for the Large Area Neutron Array (LANA)

NASA Astrophysics Data System (ADS)

Zhu, K.; Chajecki, Z.; Anderson, C.; Bromell, J.; Brown, K.; Crosby, J.; Kodali, S.; Lynch, W. G.; Morfouace, P.; Sweany, S.; Tsang, M. B.; Tsang, C.; Brett, J. J.; Swaim, J. L.

2017-09-01

Comparison of neutrons and protons emitted in heavy ion collisions is one of the observables to probe symmetry energy, which is related to the properties of neutron star. In general, neutrons are difficult to measure and neutron detectors are not as easy to use or as widely available as charged particle detectors. Two neutron walls (NW) called LANA exist at the National Superconducting Cyclotron Laboratory. Although the NSCL NW attains excellent discrimination of γ rays and neutron, it fails to discriminate charged particles from neutrons. To ensure near 100% rejection of charged particles, a Charged Particle Veto Wall (VW) is being jointly built by Michigan State University and Western Michigan University. It will be placed in front of one NW. To increase efficiency in detecting neutrons, the second neutron wall is stacked behind it. In this presentation, I will discuss the design, construction and testing of the VW together with the LANA in preparation of two approved NSCL experiments to probe the density and momentum dependence of the symmetry energy potentials in the equation state of the asymmetric nuclear matter. This material is based upon work supported by the National Science Foundation under Grant No. PHY 1565546.

Excited state intramolecular charge transfer reaction in binary mixtures of water and tertiary butanol (TBA): alcohol mole fraction dependence.

PubMed

Pradhan, Tuhin; Ghoshal, Piue; Biswas, Ranjit

2008-02-07

The excited state intramolecular charge transfer reaction of 4-(1-azetidinyl)benzonitrile (P4C) has been studied in water-tertiary butanol (TBA) mixtures at different alcohol mole fractions by using steady state and time-resolved fluorescence spectroscopy. The ratio between the areas under the locally excited (LE) and charge transferred (CT) emission bands is found to exhibit a sharp rise at alcohol mole fraction approximately 0.04, a value at which several thermodynamic properties of this mixture is known to show anomalous change due to the enhancement of H-bonding network. The radiative rate associated with the LE emission also shows a maximum at this TBA mole fraction. Although the structural transition from the water-like tetrahedral network to the alcohol-like chain is reflected in the red shift of the absorption spectrum up to TBA mole fraction approximately 0.10, the emission bands (both LE and CT) show the typical nonideal alcohol mole fraction dependence at all TBA mole fractions. Quantum yield, CT radiative rate as well as transition moments also exhibit a nonideal alcohol mole fraction dependence. The time-resolved emission decay of P4C has been found to be biexponential at all TBA mole fractions, regardless of emission collection around either the LE or the CT bands. The time constant associated with the slow component (tau(slow)) shows a minimum at TBA mole fraction approximately 0.04, whereas such a minimum for the fast time constant, tau(fast) (representing the rate of LE --> CT conversion reaction) is not observed. The nonobservation of the minimum in tau(fast) might be due to the limited time resolution employed in our experiments.

Pressure dependence of the photocycle kinetics of bacteriorhodopsin.

PubMed Central

Klink, B U; Winter, R; Engelhard, M; Chizhov, I

2002-01-01

The pressure dependence of the photocycle kinetics of bacteriorhodopsin from Halobacterium salinarium was investigated at pressures up to 4 kbar at 25 degrees C and 40 degrees C. The kinetics can be adequately modeled by nine apparent rate constants, which are assigned to irreversible transitions of a single relaxation chain of nine kinetically distinguishable states P(1) to P(9). All states except P(1) and P(9) consist of two or more spectral components. The kinetic states P(2) to P(6) comprise only the two fast equilibrating spectral states L and M. From the pressure dependence, the volume differences DeltaV(o)(LM) between these two spectral states could be determined that range from DeltaV(o)(LM) = -11.4 +/- 0.7 ml/mol (P(2)) to DeltaV(o)(LM) = 14.6 +/- 2.8 mL/mol (P(6)). A model is developed that explains the dependence of DeltaV(o)(LM) on the kinetic state by the electrostriction effect of charges, which are formed and neutralized during the L/M transition. PMID:12496115

Photophysics of detection of explosive vapours via luminescence quenching of thin films: impact of inter-molecular interactions.

PubMed

Shoaee, Safa; Fan, Shengqiang; Burn, Paul L; Shaw, Paul E

2016-09-21

Fluorescence-based detection of explosive analytes requires an understanding of the nature of the excited state responsible for the luminescence response of a sensing material. Many measurements are carried out to elucidate the fundamental photophysical properties of an emissive material in solution. However, simple transfer of the understanding gained from the solution measurements to the solid-state can lead to errors. This is in part due to the absence of inter-molecular interactions of the chromophores in solution, which are present in the solid-state. To understand the role of inter-molecular interactions on the detection of explosive analytes we have chosen dendrimers from two different families, D1 and D2, which allow facile control of the inter-molecular interactions through the choice of dendrons and emissive chromophores. Using ultrafast transient absorption spectroscopy we find that the solution photoinduced absorption (PA) for both materials can be explained in terms of the generation of singlet excitons, which decay to the ground state, or intersystem cross (ISC) to form a triplet exciton. In neat films however, we observe different photophysical behaviours; first, ISC to the triplet state does not occur, and second, depending on the chromophore, charge transfer and charge separated states are formed. Furthermore, we find that when either dendrimer is interfaced with analyte vapour, the singlet state is strongly quenched, generating a charge transfer state that undergoes geminate recombination.

Variable charge transfer state energies at nanostructured pentacene/C60 interfaces

NASA Astrophysics Data System (ADS)

Lin, YunHui L.; Zhang, Fengyu; Kerner, Ross A.; Yang, Terry Chien-Jen; Kahn, Antoine; Rand, Barry P.

2018-05-01

While it has recently been recognized that organic donor-acceptor charge transfer (CT) state energies can vary substantially under different interfacial morphologies, this behavior is under-appreciated in the context of organic singlet fission solar cells where a specific alignment between the triplet state of the fission material and the CT state of the donor-acceptor interface is necessary to the function of the device. In this work, we demonstrate that the CT state energy of a prototypical pentacene-C60 singlet fission system is around 1 eV in most systems, but can vary over 300 meV depending on the composition and morphology of the interface. Moreover, we show that the inclusion of a poly(3-hexylthiophene-2,5-diyl) underlayer, which commonly serves as a triplet blocker and hole collector in pentacene/C60 solar cells, helps promote active layer morphologies with stabilized, low energy CT states. These trends in the interfacial energetics are correlated with structural characterization of the films by atomic force microscopy and x-ray diffraction.

A temperature dependent study on charge dynamics in organic molecular device: Effect of shallow traps on space charge limited behavior

NASA Astrophysics Data System (ADS)

Mukherjee, A. K.; Kavala, A. K.

2014-04-01

Shallow traps play a significant role in influencing charge dynamics through organic molecular thin films, such as pentacene. Sandwich cells of pentacene capped by gold electrodes are an excellent specimen to study the nature of underlying charge dynamics. In this paper, self-consistent numerical simulation of I-V characteristics is performed at various temperatures. The results have revealed negative value of Poole Frenkel coefficient. The location of trap energy level is found to be located at 0.24 eV above the highest occupied molecular orbit (HOMO) level of pentacene. Other physical parameters related to trap levels, such as density of states due to traps and effective carrier density due to traps, have also been estimated in this study.

What Controls the Rate of Ultrafast Charge Transfer and Charge Separation Efficiency in Organic Photovoltaic Blends.

PubMed

Jakowetz, Andreas C; Böhm, Marcus L; Zhang, Jiangbin; Sadhanala, Aditya; Huettner, Sven; Bakulin, Artem A; Rao, Akshay; Friend, Richard H

2016-09-14

In solar energy harvesting devices based on molecular semiconductors, such as organic photovoltaics (OPVs) and artificial photosynthetic systems, Frenkel excitons must be dissociated via charge transfer at heterojunctions to yield free charges. What controls the rate and efficiency of charge transfer and charge separation is an important question, as it determines the overall power conversion efficiency (PCE) of these systems. In bulk heterojunctions between polymer donor and fullerene acceptors, which provide a model system to understand the fundamental dynamics of electron transfer in molecular systems, it has been established that the first step of photoinduced electron transfer can be fast, of order 100 fs. But here we report the first study which correlates differences in the electron transfer rate with electronic structure and morphology, achieved with sub-20 fs time resolution pump-probe spectroscopy. We vary both the fullerene substitution and donor/fullerene ratio which allow us to control both aggregate size and the energetic driving force for charge transfer. We observe a range of electron transfer times from polymer to fullerene, from 240 fs to as short as 37 fs. Using ultrafast electro-optical pump-push-photocurrent spectroscopy, we find the yield of free versus bound charges to be weakly dependent on the energetic driving force, but to be very strongly dependent on fullerene aggregate size and packing. Our results point toward the importance of state accessibility and charge delocalization and suggest that energetic offsets between donor and acceptor levels are not an important criterion for efficient charge generation. This provides design rules for next-generation materials to minimize losses related to driving energy and boost PCE.

Attempt to probe nuclear charge radii by cluster and proton emissions

NASA Astrophysics Data System (ADS)

Qian, Yibin; Ren, Zhongzhou; Ni, Dongdong

2013-05-01

We deduce the rms nuclear charge radii for ground states of light and medium-mass nuclei from experimental data of cluster radioactivity and proton emission in a unified framework. On the basis of the density-dependent cluster model, the calculated decay half-lives are obtained within the modified two-potential approach. The charge distribution of emitted clusters in the cluster decay and that of daughter nuclei in the proton emission are determined to correspondingly reproduce the experimental half-lives within the folding model. The obtained charge distribution is then employed to give the rms charge radius of the studied nuclei. Satisfactory agreement between theory and experiment is achieved for available experimental data, and the present results are found to be consistent with theoretical estimations. This study is expected to be helpful in the future detection of nuclear sizes, especially for these exotic nuclei near the proton dripline.

Microscopic Simulations of Charge Transport in Disordered Organic Semiconductors

PubMed Central

2011-01-01

Charge carrier dynamics in an organic semiconductor can often be described in terms of charge hopping between localized states. The hopping rates depend on electronic coupling elements, reorganization energies, and driving forces, which vary as a function of position and orientation of the molecules. The exact evaluation of these contributions in a molecular assembly is computationally prohibitive. Various, often semiempirical, approximations are employed instead. In this work, we review some of these approaches and introduce a software toolkit which implements them. The purpose of the toolkit is to simplify the workflow for charge transport simulations, provide a uniform error control for the methods and a flexible platform for their development, and eventually allow in silico prescreening of organic semiconductors for specific applications. All implemented methods are illustrated by studying charge transport in amorphous films of tris-(8-hydroxyquinoline)aluminum, a common organic semiconductor. PMID:22076120

Inherent Driving Force for Charge Separation in Curved Stacks of Oligothiophenes

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

Wu, Qin

Coexistence of high local charge mobility and an energy gradient can lead to efficient free charge carrier generation from geminate charge transfer states at the donor–acceptor interface in bulk heterojunction organic photovoltaics. It is, however, not clear what polymer microstructures can support such coexistence. Using recent methods from density functional theory, we propose that a stack of similarly curved oligothiophene chains can deliver the requirements for efficient charge separation. Curved stacks are stable because of the polymer’s strong π-stacking ability and because backbone torsions are flexible in neutral chains. However, energy of a charge in a polymer chain has remarkablymore » stronger dependence on torsions. The trend of increasing planarity in curved stacks effectively creates an energy gradient that drives charge in one direction. The curvature of these partially ordered stacks is found to beneficially interact with fullerenes for charge separation. The curved stacks, therefore, are identified as possible building blocks for interfacial structures that lead to efficient free carrier generation in high-performing organic photovoltaic systems.« less

Inherent Driving Force for Charge Separation in Curved Stacks of Oligothiophenes

DOE PAGES

Wu, Qin

2015-01-30

Coexistence of high local charge mobility and an energy gradient can lead to efficient free charge carrier generation from geminate charge transfer states at the donor–acceptor interface in bulk heterojunction organic photovoltaics. It is, however, not clear what polymer microstructures can support such coexistence. Using recent methods from density functional theory, we propose that a stack of similarly curved oligothiophene chains can deliver the requirements for efficient charge separation. Curved stacks are stable because of the polymer’s strong π-stacking ability and because backbone torsions are flexible in neutral chains. However, energy of a charge in a polymer chain has remarkablymore » stronger dependence on torsions. The trend of increasing planarity in curved stacks effectively creates an energy gradient that drives charge in one direction. The curvature of these partially ordered stacks is found to beneficially interact with fullerenes for charge separation. The curved stacks, therefore, are identified as possible building blocks for interfacial structures that lead to efficient free carrier generation in high-performing organic photovoltaic systems.« less

Initial state q q g correlations as a background for the chiral magnetic effect in collision of small systems

DOE PAGES

Kovner, Alex; Lublinsky, Michael; Skokov, Vladimir

2017-11-13

Motivated by understanding the background to chiral magnetic effect in proton-nucleus collisions from first principles, we compute the three particle correlation in the projectile wave function. We extract the correlations between two quarks and one gluon in the framework of the color glass condensate. This is related to the same-charge correlation of the conventional observable for the chiral magnetic effect. We show that there are two different contributions to this correlation function. One contribution is rapidity-independent and as such can be identified with the pedestal; while the other displays rather strong rapidity dependence. The pedestal contribution and the rapidity-dependent contributionmore » at large rapidity separation between the two quarks result in the negative same charge correlations, while at small rapidity separation the second contribution changes sign. We argue that the computed initial state correlations might be partially responsible for the experimentally observed signal in proton-nucleus collisions.« less

Initial state q q g correlations as a background for the chiral magnetic effect in collision of small systems

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

Kovner, Alex; Lublinsky, Michael; Skokov, Vladimir

Motivated by understanding the background to chiral magnetic effect in proton-nucleus collisions from first principles, we compute the three particle correlation in the projectile wave function. We extract the correlations between two quarks and one gluon in the framework of the color glass condensate. This is related to the same-charge correlation of the conventional observable for the chiral magnetic effect. We show that there are two different contributions to this correlation function. One contribution is rapidity-independent and as such can be identified with the pedestal; while the other displays rather strong rapidity dependence. The pedestal contribution and the rapidity-dependent contributionmore » at large rapidity separation between the two quarks result in the negative same charge correlations, while at small rapidity separation the second contribution changes sign. We argue that the computed initial state correlations might be partially responsible for the experimentally observed signal in proton-nucleus collisions.« less

Initial state q q g correlations as a background for the chiral magnetic effect in collision of small systems

NASA Astrophysics Data System (ADS)

Kovner, Alex; Lublinsky, Michael; Skokov, Vladimir

2017-11-01

Motivated by understanding the background to chiral magnetic effect in proton-nucleus collisions from first principles, we compute the three particle correlation in the projectile wave function. We extract the correlations between two quarks and one gluon in the framework of the color glass condensate. This is related to the same-charge correlation of the conventional observable for the chiral magnetic effect. We show that there are two different contributions to this correlation function. One contribution is rapidity-independent and as such can be identified with the pedestal; while the other displays rather strong rapidity dependence. The pedestal contribution and the rapidity-dependent contribution at large rapidity separation between the two quarks result in the negative same charge correlations, while at small rapidity separation the second contribution changes sign. We argue that the computed initial state correlations might be partially responsible for the experimentally observed signal in proton-nucleus collisions.

Tracking ion irradiation effects using buried interface devices

NASA Astrophysics Data System (ADS)

Cutshall, D. B.; Kulkarni, D. D.; Miller, A. J.; Harriss, J. E.; Harrell, W. R.; Sosolik, C. E.

2018-05-01

We discuss how a buried interface device, specifically a metal-oxide-semiconductor (MOS) capacitor, can be utilized to track effects of ion irradiation on insulators. We show that the exposure of oxides within unfinished capacitor devices to ions can lead to significant changes in the capacitance of the finished devices. For multicharged ions, these capacitive effects can be traced to defect production within the oxide and ultimately point to a role for charge-dependent energy loss. In particular, we attribute the stretchout of the capacitance-voltage curves of MOS devices that include an irradiated oxide to the ion irradiation. The stretchout shows a power law dependence on the multicharged ion charge state (Q) that is similar to that observed for multicharged ion energy loss in other systems.

Spin-dependent recombination probed through the dielectric polarizability

PubMed Central

Bayliss, Sam L.; Greenham, Neil C.; Friend, Richard H.; Bouchiat, Hélène; Chepelianskii, Alexei D

2015-01-01

Despite residing in an energetically and structurally disordered landscape, the spin degree of freedom remains a robust quantity in organic semiconductor materials due to the weak coupling of spin and orbital states. This enforces spin-selectivity in recombination processes which plays a crucial role in optoelectronic devices, for example, in the spin-dependent recombination of weakly bound electron-hole pairs, or charge-transfer states, which form in a photovoltaic blend. Here, we implement a detection scheme to probe the spin-selective recombination of these states through changes in their dielectric polarizability under magnetic resonance. Using this technique, we access a regime in which the usual mixing of spin-singlet and spin-triplet states due to hyperfine fields is suppressed by microwave driving. We present a quantitative model for this behaviour which allows us to estimate the spin-dependent recombination rate, and draw parallels with the Majorana–Brossel resonances observed in atomic physics experiments. PMID:26439933

Large impact of reorganization energy on photovoltaic conversion due to interfacial charge-transfer transitions.

PubMed

Fujisawa, Jun-ichi

2015-05-14

Interfacial charge-transfer (ICT) transitions are expected to be a novel charge-separation mechanism for efficient photovoltaic conversion featuring one-step charge separation without energy loss. Photovoltaic conversion due to ICT transitions has been investigated using several TiO2-organic hybrid materials that show organic-to-inorganic ICT transitions in the visible region. In applications of ICT transitions to photovoltaic conversion, there is a significant problem that rapid carrier recombination is caused by organic-inorganic electronic coupling that is necessary for the ICT transitions. In order to solve this problem, in this work, I have theoretically studied light-to-current conversions due to the ICT transitions on the basis of the Marcus theory with density functional theory (DFT) and time-dependent DFT (TD-DFT) calculations. An apparent correlation between the reported incident photon-to-current conversion efficiencies (IPCE) and calculated reorganization energies was clearly found, in which the IPCE increases with decreasing the reorganization energy consistent with the Marcus theory in the inverted region. This activation-energy dependence was systematically explained by the equation formulated by the Marcus theory based on a simple excited-state kinetic scheme. This result indicates that the reduction of the reorganization energy can suppress the carrier recombination and enhance the IPCE. The reorganization energy is predominantly governed by the structural change in the chemical-adsorption moiety between the ground and ICT excited states. This work provides crucial knowledge for efficient photovoltaic conversion due to ICT transitions.

The Generation of Dehydroalanine Residues in Protonated Polypeptides: Ion/Ion Reactions for Introducing Selective Cleavages

NASA Astrophysics Data System (ADS)

Peng, Zhou; Bu, Jiexun; McLuckey, Scott A.

2017-09-01

We examine a gas-phase approach for converting a subset of amino acid residues in polypeptide cations to dehydroalanine (Dha). Subsequent activation of the modified polypeptide ions gives rise to specific cleavage N-terminal to the Dha residue. This process allows for the incorporation of selective cleavages in the structural characterization of polypeptide ions. An ion/ion reaction within the mass spectrometer between a multiply protonated polypeptide and the sulfate radical anion introduces a radical site into the multiply protonated polypeptide reactant. Subsequent collisional activation of the polypeptide radical cation gives rise to radical side chain loss from one of several particular amino acid side chains (e.g., leucine, asparagine, lysine, glutamine, and glutamic acid) to yield a Dha residue. The Dha residues facilitate preferential backbone cleavages to produce signature c- and z-ions, demonstrated with cations derived from melittin, mechano growth factor (MGF), and ubiquitin. The efficiencies for radical side chain loss and for subsequent generation of specific c- and z-ions have been examined as functions of precursor ion charge state and activation conditions using cations of ubiquitin as a model for a small protein. It is noted that these efficiencies are not strongly dependent on ion trap collisional activation conditions but are sensitive to precursor ion charge state. Moderate to low charge states show the greatest overall yields for the specific Dha cleavages, whereas small molecule losses (e.g., water/ammonia) dominate at the lowest charge states and proton catalyzed amide bond cleavages that give rise to b- and y-ions tend to dominate at high charge states. [Figure not available: see fulltext.

Effect of dielectric stoichiometry and interface chemical state on band alignment between tantalum oxide and platinum

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

Lebedinskii, Yu. Yu.; National Research Nuclear University MEPhI; Chernikova, A. G.

2015-10-05

The tantalum oxide–platinum interface electronic properties determined by X-ray photoelectron spectroscopy are found to depend on the dielectric stoichiometry and platinum chemical state. We demonstrate the slow charging of the tantalum oxide in cases of Ta{sub 2}O{sub 5}/Pt and Ta{sub 2}O{sub 5−y}/Pt interfaces under the X-ray irradiation. This behavior is proposed to be related to the charge accumulation at oxygen vacancies induced traps. Based on the proposed methodology, we define the intrinsic conductive band offset (CBO) ∼1.3 eV (both for Ta{sub 2}O{sub 5}/Pt and Ta{sub 2}O{sub 5−y}/Pt) and CBO after the full saturation of the traps charging ∼0.5 eV, while the lastmore » one defines the energy position of charged traps below the bottom of conduction band. We demonstrate also the pining at the both Ta{sub 2}O{sub 5}/Pt and Ta{sub 2}O{sub 5−y}/Pt interfaces even in the “intrinsic” state, apparently induced by the presence of additional interfacial states. No shifts of Ta4f line and band alignment in over stoichiometric Ta{sub 2}O{sub 5+x}/Pt structure during X-ray irradiation, as well as the absence of pinning, resulting in increase of CBO up to 2.3 eV are found. This behavior is related to the PtO{sub 2} interfacing layer formation at Ta{sub 2}O{sub 5+x}/Pt, blocking the charging of the surface states and associated dipole formation.« less

Effect of molecular properties on the performance of polymer light-emitting diodes

NASA Astrophysics Data System (ADS)

Ramos, Marta M. D.; Almeida, A. M.; Correia, Helena M. G.; Ribeiro, R. Mendes; Stoneham, A. M.

2004-11-01

The performance of a single layer polymer light-emitting diode depends on several interdependent factors, although recombination between electrons and holes within the polymer layer is believed to play an important role. Our aim is to carry out computer experiments in which bipolar charge carriers are injected in polymer networks made of poly(p-phenylene vinylene) chains randomly oriented. In these simulations, we follow the charge evolution in time from some initial state to the steady state. The intra-molecular properties of the polymer molecules obtained from self-consistent quantum molecular dynamics calculations are used in the mesoscopic model. The purpose of the present work is to clarify the effects of intra-molecular charge mobility and energy disorder on recombination efficiency. In particular, we find that charge mobility along the polymer chains has a serious influence on recombination within the polymer layer. Our results also show that energy disorder due to differences in ionization potential and electron affinity of neighbouring molecules affects mainly recombinations that occur near the electrodes at polymer chains parallel to them.

Structure and Electronic Spectra of Purine-Methyl Viologen Charge Transfer Complexes

PubMed Central

Jalilov, Almaz S.; Patwardhan, Sameer; Singh, Arunoday; Simeon, Tomekia; Sarjeant, Amy A.; Schatz, George C.; Lewis, Frederick D.

2014-01-01

The structure and properties of the electron donor-acceptor complexes formed between methyl viologen (MV) and purine nucleosides and nucleotides in water and the solid state have been investigated using a combination of experimental and theoretical methods. Solution studies were performed using UV-vis and 1H NMR spectroscopy. Theoretical calculations were performed within the framework of density functional theory (DFT). Energy decomposition analysis indicates that dispersion and induction (charge-transfer) interactions dominate the total binding energy, whereas electrostatic interactions are largely repulsive. The appearance of charge transfer bands in the absorption spectra of the complexes are well described by time-dependent (TD) DFT and are further explained in terms of the redox properties of purine monomers and solvation effects. Crystal structures are reported for complexes of methyl viologen with the purines 2′-deoxyguanosine 3′-monophosphate GMP (DAD′DAD′ type) and 7-deazaguanosine zG (DAD′ADAD′ type). Comparison of the structures determined in the solid state and by theoretical methods in solution provides valuable insights into the nature of charge-transfer interactions involving purine bases as electron donors. PMID:24294996

Relationship between composition of mixture charged and that in circulation in an auto refrigerant cascade and a J-T refrigerator operating in liquid refrigerant supply mode

NASA Astrophysics Data System (ADS)

Sreenivas, Bura; Nayak, H. Gurudath; Venkatarathnam, G.

2017-01-01

The composition of the refrigerant mixture in circulation during steady state operation of J-T and allied refrigerators is not the same as that charged due to liquid hold up in the heat exchangers and phase separators, as well as the differential solubility of different refrigerant components in the compressor lubricating oil. The performance of refrigerators/liquefiers operating on mixed refrigerant cycles is dependent on the mixture composition. It is therefore important to charge the right mixture that results in an optimum composition in circulation during steady state operation. The relationship between the charged and circulating composition has been experimentally studied in a J-T refrigerator operating in the liquid refrigerant supply (LRS) mode and an auto refrigerant cascade refrigerator (with a phase separator) operating in the gas refrigerant supply (GRS) mode. The results of the study are presented in this work. The results show that the method presented earlier for J-T refrigerators operating in GRS mode is also applicable in the case of refrigerators studied in this work.

Wall-loss distribution of charge breeding ions in an electron cyclotron resonance ion source

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

Jeong, S. C.; Oyaizu, M.; Imai, N.

2011-03-15

The ion loss distribution in an electron cyclotron resonance ion source (ECRIS) was investigated to understand the element dependence of the charge breeding efficiency in an electron cyclotron resonance (ECR) charge breeder. The radioactive {sup 111}In{sup 1+} and {sup 140}Xe{sup 1+} ions (typical nonvolatile and volatile elements, respectively) were injected into the ECR charge breeder at the Tokai Radioactive Ion Accelerator Complex to breed their charge states. Their respective residual activities on the sidewall of the cylindrical plasma chamber of the source were measured after charge breeding as functions of the azimuthal angle and longitudinal position and two-dimensional distributions ofmore » ions lost during charge breeding in the ECRIS were obtained. These distributions had different azimuthal symmetries. The origins of these different azimuthal symmetries are qualitatively discussed by analyzing the differences and similarities in the observed wall-loss patterns. The implications for improving the charge breeding efficiencies of nonvolatile elements in ECR charge breeders are described. The similarities represent universal ion loss characteristics in an ECR charge breeder, which are different from the loss patterns of electrons on the ECRIS wall.« less

0{degree} binary encounter electron production in 30-MeV O{ital {sup q}}{sup +}+H{sub 2}, He, O{sub 2}, Ne, and Ar collisions

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

Zouros, T.J.; Wong, K.L.; Grabbe, S.

Double-differential cross sections (DDCS{close_quote}s) for the production of binary encounter electrons (BEE{close_quote}s) were measured for collisions of 30-MeV O{sup {ital q}+} projectiles with H{sub 2}, He, O{sub 2}, Ne, and Ar targets with {ital q}=4{endash}8 and an electron ejection angle of {theta}=0{degree} with respect to the beam direction. Particular interest focused on (a) the evaluation of the contributions of the different electron subshells of the multielectron targets, O{sub 2}, Ne, and Ar; (b) the study of the well-known enhancement of the BEE DDCS{close_quote}s with decreasing projectile charge-state {ital q}; here this dependence was tested for higher collision energies and newmore » targets; (c) the study of the dependence of the BEE {ital peak} {ital energy} on the particular target and projectile charge state. Results were analyzed in terms of the impulse approximation, in which target electrons in the projectile frame undergo 180{degree} elastic scattering in the field of the projectile ion. The electron scattering calculations were performed in a partial-wave treatment using the Hartree-Fock model. Good agreement with the data was found for the H{sub 2} and He targets, while for the multielectron targets O{sub 2}, Ne, and Ar only electrons whose velocity was lower than the projectile velocity needed to be included for good agreement. All measured BEE DDCS{close_quote}s were found to increase with decreasing projectile charge state, in agreement with other recent BEE results. The BEE peak energies were found to be independent of the projectile charge state for all targets utilized. {copyright} {ital 1996 The American Physical Society.}« less

Synthesis, spectral behaviour and photophysics of donor-acceptor kind of chalcones: Excited state intramolecular charge transfer and fluorescence quenching studies

NASA Astrophysics Data System (ADS)

Pannipara, Mehboobali; Asiri, Abdullah M.; Alamry, Khalid A.; Arshad, Muhammad N.; El-Daly, Samy A.

2015-02-01

The spectral and photophysical properties of two chalcones containing electron donating and accepting groups with intramolecular charge transfer characteristics were synthesized and characterized by 1H NMR, 13C NMR and X-ray crystallography. Both compounds show very strong solvent polarity dependent changes in their photophysical characteristics, namely, remarkable red shift in the emission spectra with increasing solvent polarity, large change in Stokes shift, significant reduction in the fluorescence quantum yield; indicating that the fluorescence states of these compounds are of intramolecular charge transfer (ICT) character. The solvent effect on the photophysical parameters such as singlet absorption, molar absorptivity, oscillator strength, dipole moment, fluorescence spectra, and fluorescence quantum yield of both compounds have been investigated comprehensively. For both dyes, Lippert-Mataga and Reichardt's correlations were used to estimate the difference between the excited and ground state dipole moments (Δμ). The interactions of dyes with colloidal silver nanoparticles (Ag NPs) were also studied in ethanol using steady state fluorescence quenching measurements. The fluorescence quenching data reveal that dynamic quenching and energy transfer play a major role in the fluorescence quenching of dyes by Ag NPs.

Analyzing the equilibrium states of a quasi-neutral spatially inhomogeneous system of charges above a liquid dielectric film based on the first principles of quantum statistics

NASA Astrophysics Data System (ADS)

Lytvynenko, D. M.; Slyusarenko, Yu V.

2017-08-01

A theory of quasi-neutral equilibrium states of charges above a liquid dielectric surface is developed. This theory is based on the first principles of quantum statistics for systems comprising many identical particles. The proposed approach involves applying the variational principle, modified for the considered systems, and the Thomas-Fermi model. In the terms of the developed theory self-consistency equations are obtained. These equations provide the relation between the main parameters describing the system: the potential of the static electric field, the distribution function of charges and the surface profile of the liquid dielectric. The equations are used to study the phase transition in the system to a spatially periodic state. The proposed method can be applied in analyzing the properties of the phase transition in the system in relation to the spatially periodic states of wave type. Using the analytical and numerical methods, we perform a detailed study of the dependence of the critical parameters of such a phase transition on the thickness of the liquid dielectric film. Some stability criteria for the new asymmetric phase of the studied system are discussed.

State selected ion--molecule reactions by a TESICO technique. IV. Relative importance of the two spin-orbit states of Ar/sup +/ in the charge transfer reactions with N/sub 2/ and CO

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

Kato, T.; Tanaka, K.; Koyano, I.

1982-07-01

Charge transfer reactions Ar/sup +/ (/sup 2/P/sub J/)+N/sub 2/..-->..N/sup +//sub 2/+Ar (1) and Ar/sup +/(/sup 2/P/sub J/)+CO..-->..CO/sup +/+Ar (2) have been studied for the two spin-orbit states (J = 3/2 and 1/2) separately using the threshold electron-secondary ion coincidence (TESICO) technique. Relative cross sections for the two states sigma(3/2) and sigma(1/2) have been determined at three collision energies 0.2, 1.4, and 5.8 eV. It has been found that in Reaction (1), sigma(3/2) is larger than sigma (1/2) with ratio sigma(1/2)/sigma(3/2) ranging from 0.5 to 0.8 depending on the collision energy, whereas in Reaction (2), sigma(1/2) is larger than sigma(3/2) withmore » the ratio ranging from 1.2 to 1.6. The implications of these results are discussed with regard to the roles of energy resonance and Franck--Condon factors in charge transfer processes.« less

Carrier-envelope phase dependence of the directional fragmentation and hydrogen migration in toluene in few-cycle laser fields

PubMed Central

Li, Hui; Kling, Nora G.; Förg, Benjamin; Stierle, Johannes; Kessel, Alexander; Trushin, Sergei A.; Kling, Matthias F.; Kaziannis, Spyros

2016-01-01

The dissociative ionization of toluene initiated by a few-cycle laser pulse as a function of the carrier envelope phase (CEP) is investigated using single-shot velocity map imaging. Several ionic fragments, CH3+, H2+, and H3+, originating from multiply charged toluene ions present a CEP-dependent directional emission. The formation of H2+ and H3+ involves breaking C-H bonds and forming new bonds between the hydrogen atoms within the transient structure of the multiply charged precursor. We observe appreciable intensity-dependent CEP-offsets. The experimental data are interpreted with a mechanism that involves laser-induced coupling of vibrational states, which has been found to play a role in the CEP-control of molecular processes in hydrocarbon molecules, and appears to be of general importance for such complex molecules. PMID:26958589

Effect of atomic-scale defects and dopants on phosphorene electronic structure and quantum transport properties

DOE PAGES

Lopez-Bezanilla, Alejandro

2016-01-20

By means of a multi-scale first-principles approach, a description of the local electronic structure of 2D and narrow phosphorene sheets with various types of modifications is presented. Firtly, a rational argument based on the geometry of the pristine and modified P network, and supported by the Wannier functions formalism is introduced to describe a hybridization model of the P atomic orbitals. Ab initio calculations show that non-isoelectronic foreign atoms form quasi-bound states at varying energy levels and create different polarization states depending on the number of valence electrons between P and the doping atom. The quantum transport properties of modifiedmore » phosphorene ribbons are further described with great accuracy. The distortions on the electronic bands induced by the external species lead to strong backscattering effects on the propagating charge carriers. Depending on the energy of the charge carrier and the type of doping, the conduction may range from the diffusive to the localized regime. Interstitial defects at vacant sites lead to homogeneous transport fingerprints across different types of doping atoms. We suggest that the relatively low values of charge mobility reported in experimental measurements may have its origin in the presence of defects.« less

Microscopic signature of insulator-to-metal transition in highly doped semicrystalline conducting polymers in ionic-liquid-gated transistors

NASA Astrophysics Data System (ADS)

Tanaka, Hisaaki; Nishio, Satoshi; Ito, Hiroshi; Kuroda, Shin-ichi

2015-12-01

Electronic state of charge carriers, in particular, in highly doped regions, in thin-film transistors of a semicrystalline conducting polymer poly(2,5-bis(3-alkylthiophene-2-yl)thieno[3,2-b]thiophene), has been studied by using field-induced electron spin resonance (ESR) spectroscopy. By adopting an ionic-liquid gate insulator, a gate-controlled reversible electrochemical hole-doping of the polymer backbone is achieved, as confirmed from the change of the optical absorption spectra. The edge-on molecular orientation in the pristine film is maintained even after the electrochemical doping, which is clarified from the angular dependence of the g value. As the doping level increases, spin 1/2 polarons transform into spinless bipolarons, which is demonstrated from the spin-charge relation showing a spin concentration peak around 1%, contrasting to the monotonic increase in the charge concentration. At high doping levels, a drastic change in the linewidth anisotropy due to the generation of conduction electrons is observed, indicating the onset of metallic state, which is also supported by the temperature dependence of the spin susceptibility and the ESR linewidth. Our results suggest that semicrystalline conducting polymers become metallic with retaining their molecular orientational order, when appropriate doping methods are chosen.

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

PubMed Central

Boll, Rebecca; Erk, Benjamin; Coffee, Ryan; Trippel, Sebastian; Kierspel, Thomas; Bomme, Cédric; Bozek, John D.; Burkett, Mitchell; Carron, Sebastian; Ferguson, Ken R.; Foucar, Lutz; Küpper, Jochen; Marchenko, Tatiana; Miron, Catalin; Patanen, Minna; Osipov, Timur; Schorb, Sebastian; Simon, Marc; Swiggers, Michelle; Techert, Simone; Ueda, Kiyoshi; Bostedt, Christoph; Rolles, Daniel; Rudenko, Artem

2016-01-01

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. PMID:27051675

Programming interfacial energetic offsets and charge transfer in β-Pb 0.33V 2O 5/quantum-dot heterostructures: Tuning valence-band edges to overlap with midgap states

DOE PAGES

Pelcher, Kate E.; Milleville, Christopher C.; Wangoh, Linda; ...

2016-12-06

Here, semiconductor heterostructures for solar energy conversion interface light-harvesting semiconductor nanoparticles with wide-band-gap semiconductors that serve as charge acceptors. In such heterostructures, the kinetics of charge separation depend on the thermodynamic driving force, which is dictated by energetic offsets across the interface. A recently developed promising platform interfaces semiconductor quantum dots (QDs) with ternary vanadium oxides that have characteristic midgap states situated between the valence and conduction bands. In this work, we have prepared CdS/β-Pb 0.33V 2O 5 heterostructures by both linker-assisted assembly and surface precipitation and contrasted these materials with CdSe/β-Pb 0.33V 2O 5 heterostructures prepared by the samemore » methods. Increased valence-band (VB) edge onsets in X-ray photoelectron spectra for CdS/β-Pb 0.33V 2O 5 heterostructures relative to CdSe/β-Pb 0.33V 2O 5 heterostructures suggest a positive shift in the VB edge potential and, therefore, an increased driving force for the photoinduced transfer of holes to the midgap state of β-Pb 0.33V 2O 5. This approach facilitates a ca. 0.40 eV decrease in the thermodynamic barrier for hole injection from the VB edge of QDs suggesting an important design parameter. Transient absorption spectroscopy experiments provide direct evidence of hole transfer from photoexcited CdS QDs to the midgap states of β-Pb 0.33V 2O 5 NWs, along with electron transfer into the conduction band of the β-Pb 0.33V 2O 5 NWs. Hole transfer is substantially faster and occurs at <1-ps time scales, whereas completion of electron transfer requires 5—30 ps depending on the nature of the interface. The differentiated time scales of electron and hole transfer, which are furthermore tunable as a function of the mode of attachment of QDs to NWs, provide a vital design tool for designing architectures for solar energy conversion. More generally, the approach developed here suggests that interfacing semiconductor QDs with transition-metal oxide NWs exhibiting intercalative midgap states yields a versatile platform wherein the thermodynamics and kinetics of charge transfer can be systematically modulated to improve the efficiency of charge separation across interfaces.« less

Programming interfacial energetic offsets and charge transfer in β-Pb 0.33V 2O 5/quantum-dot heterostructures: Tuning valence-band edges to overlap with midgap states

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

Pelcher, Kate E.; Milleville, Christopher C.; Wangoh, Linda

Here, semiconductor heterostructures for solar energy conversion interface light-harvesting semiconductor nanoparticles with wide-band-gap semiconductors that serve as charge acceptors. In such heterostructures, the kinetics of charge separation depend on the thermodynamic driving force, which is dictated by energetic offsets across the interface. A recently developed promising platform interfaces semiconductor quantum dots (QDs) with ternary vanadium oxides that have characteristic midgap states situated between the valence and conduction bands. In this work, we have prepared CdS/β-Pb 0.33V 2O 5 heterostructures by both linker-assisted assembly and surface precipitation and contrasted these materials with CdSe/β-Pb 0.33V 2O 5 heterostructures prepared by the samemore » methods. Increased valence-band (VB) edge onsets in X-ray photoelectron spectra for CdS/β-Pb 0.33V 2O 5 heterostructures relative to CdSe/β-Pb 0.33V 2O 5 heterostructures suggest a positive shift in the VB edge potential and, therefore, an increased driving force for the photoinduced transfer of holes to the midgap state of β-Pb 0.33V 2O 5. This approach facilitates a ca. 0.40 eV decrease in the thermodynamic barrier for hole injection from the VB edge of QDs suggesting an important design parameter. Transient absorption spectroscopy experiments provide direct evidence of hole transfer from photoexcited CdS QDs to the midgap states of β-Pb 0.33V 2O 5 NWs, along with electron transfer into the conduction band of the β-Pb 0.33V 2O 5 NWs. Hole transfer is substantially faster and occurs at <1-ps time scales, whereas completion of electron transfer requires 5—30 ps depending on the nature of the interface. The differentiated time scales of electron and hole transfer, which are furthermore tunable as a function of the mode of attachment of QDs to NWs, provide a vital design tool for designing architectures for solar energy conversion. More generally, the approach developed here suggests that interfacing semiconductor QDs with transition-metal oxide NWs exhibiting intercalative midgap states yields a versatile platform wherein the thermodynamics and kinetics of charge transfer can be systematically modulated to improve the efficiency of charge separation across interfaces.« less

Critical behaviour in charging of electric vehicles

NASA Astrophysics Data System (ADS)

Carvalho, Rui; Buzna, Lubos; Gibbens, Richard; Kelly, Frank

2015-09-01

The increasing penetration of electric vehicles over the coming decades, taken together with the high cost to upgrade local distribution networks and consumer demand for home charging, suggest that managing congestion on low voltage networks will be a crucial component of the electric vehicle revolution and the move away from fossil fuels in transportation. Here, we model the max-flow and proportional fairness protocols for the control of congestion caused by a fleet of vehicles charging on two real-world distribution networks. We show that the system undergoes a continuous phase transition to a congested state as a function of the rate of vehicles plugging to the network to charge. We focus on the order parameter and its fluctuations close to the phase transition, and show that the critical point depends on the choice of congestion protocol. Finally, we analyse the inequality in the charging times as the vehicle arrival rate increases, and show that charging times are considerably more equitable in proportional fairness than in max-flow.

Measurement of the centrality dependence of the charged-particle pseudorapidity distribution in proton-lead collisions at [Formula: see text] TeV with the ATLAS detector.

PubMed

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Zimmermann, R; Zimmermann, S; Zimmermann, S; Zinonos, Z; Ziolkowski, M; Zitoun, R; Zobernig, G; Zoccoli, A; Zur Nedden, M; Zurzolo, G; Zutshi, V; Zwalinski, L

2016-01-01

The centrality dependence of the mean charged-particle multiplicity as a function of pseudorapidity is measured in approximately 1 [Formula: see text]b[Formula: see text] of proton-lead collisions at a nucleon-nucleon centre-of-mass energy of [Formula: see text] [Formula: see text] using the ATLAS detector at the Large Hadron Collider. Charged particles with absolute pseudorapidity less than 2.7 are reconstructed using the ATLAS pixel detector. The [Formula: see text] collision centrality is characterised by the total transverse energy measured in the Pb-going direction of the forward calorimeter. The charged-particle pseudorapidity distributions are found to vary strongly with centrality, with an increasing asymmetry between the proton-going and Pb-going directions as the collisions become more central. Three different estimations of the number of nucleons participating in the [Formula: see text] collision have been carried out using the Glauber model as well as two Glauber-Gribov inspired extensions to the Glauber model. Charged-particle multiplicities per participant pair are found to vary differently for these three models, highlighting the importance of including colour fluctuations in nucleon-nucleon collisions in the modelling of the initial state of [Formula: see text] collisions.

Measurement of the centrality dependence of the charged-particle pseudorapidity distribution in proton–lead collisions at $$\\sqrt{s_{_\\text {NN}}} = 5.02$$ TeV with the ATLAS detector

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

Aad, G.; Abajyan, T.; Abbott, B.

2016-04-01

The centrality dependence of the mean charged-particle multiplicity as a function of pseudorapidity is measured in approximately 1 μb -1 of proton–lead collisions at a nucleon–nucleon centre-of-mass energy ofmore » $$\\sqrt{s_{_\\text {NN}}} = 5.02$$ TeV using the ATLAS detector at the Large Hadron Collider. Charged particles with absolute pseudorapidity less than 2.7 are reconstructed using the ATLAS pixel detector. The ρ + Ρb collision centrality is characterised by the total transverse energy measured in the Pb-going direction of the forward calorimeter. The charged-particle pseudorapidity distributions are found to vary strongly with centrality, with an increasing asymmetry between the proton-going and Pb-going directions as the collisions become more central. Three different estimations of the number of nucleons participating in the ρ + Ρb collision have been carried out using the Glauber model as well as two Glauber–Gribov inspired extensions to the Glauber model. In conclusion, charged-particle multiplicities per participant pair are found to vary differently for these three models, highlighting the importance of including colour fluctuations in nucleon–nucleon collisions in the modelling of the initial state of ρ + Ρb collisions.« less

Uniaxial-Strain-Orientation Dependence of the Competition between Mott and Charge Ordered Phases and their Corresponding Superconductivity of β-(BDA-TTP)2I3

NASA Astrophysics Data System (ADS)

Nuruzzaman, Md.; Yokogawa, Keiichi; Yoshino, Harukazu; Yoshimoto, Haruo; Kikuchi, Koichi; Kaihatsu, Takayuki; Yamada, Jun-ichi; Murata, Keizo

2012-12-01

We studied the electronic transport properties of the charge transfer salt β-(BDA-TTP)2I3 [BDA-TTP: 2,5-bis(1,3-dithian-2-ylidene)-1,3,4,6-tetrathiapentalene] by applying uniaxial strains along the three crystallographic axes, and obtained three corresponding temperature-pressure phase diagrams. Three phase diagrams were quite dependent on the direction of compression. Following the preceding paper by Kikuchi et al., we speculate that the insulating states are of 1/2-filled Mott insulators for the a- and b-axes compressions, and of 1/4-filled charge ordered states for the c-axis compression as well as hydrostatic pressure. The superconducting phase under uniaxial strain was realized with Tc = 5 K at 1.9 GPa along the a-axis and with Tc = 5.6 K at 1.75 GPa along the b-axis. Superconductivity was also reproduced with a Tc of 9.5 K at 1.0 GPa for the c-axis compressions in the range of 0.85 to 1.53 GPa as previously reported. We studied tentative measurement on upper critical fields, Bc2's of these superconductivities and found that the extrapolated values, Bc2(0)'s, exceeded Pauli-limit by about 2--3 times. However, at least in terms of Bc2, the difference in superconductivity associated with two different insulating states was not clear.

Investigations on the defect dipole induced pyroelectric current in multiferroic GdMnO3 system

NASA Astrophysics Data System (ADS)

Pal, A.; Dhana Sekhar, C.; Venimadhav, A.; Prellier, W.; Murugavel, P.

2018-01-01

Pyroelectric current measurements on the orthorhombic GdMnO3 polycrystalline sample are done to explore the intrinsic and extrinsic contributions. The measurements reveal poling temperature dependent pyrocurrent peaks at 20, 50 and 108 K. The pyrocurrent at 20 K and at 108 K are attributed to ferroelectric transition induced by the incommensurate spiral magnetic ordering of Mn spins and the release of trapped charges from the localized states, respectively. A detailed analysis on the broad pyrocurrent signal at 50 K suggests that it could be attributed to the thermally stimulated depolarization current effect due to the relaxation of defect dipoles induced by negatively charged Mn3+ ions and excess holes localized at Mn4+ sites. Importantly, the effect of the electric field due to the defect dipoles on the ferroelectric state is highlighted. The temperature dependent dielectric measurements under the magnetic field brought out the correlation between pyroelectric and dielectric properties. The influence of poling temperature dependent extrinsic effects on pyrocurrent suggests the choice of poling temperature on the study of polarization and the resultant multiferroicity in a spin-driven ferroelectric rare earth manganite system.

Electrokinetic Properties of Fullerene nC60 Nanoparticles: Role of Co-ions and pH

EPA Science Inventory

Environmental exposure, bioavailability, and mobility of nanoparticles (NPs) in part depend on their aggregated state and their surface charge. These fundamental characteristics are functions of the aqueous media in which the particles are suspended. For example, inorganic ions p...

Improvement of Characteristics of Laser Source of Ions Using Two-Element Targets

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

Khaydarov, R. T.

2006-12-04

Two-element plasma ions generated from porous (Ho2O3) and solid (PbMg) targets were studied depending on the target density {rho} and on the fraction of light (Mg) component of the target, using a mass-spectrometer. Oxygen ions with maximal charge is observed for small values of {rho}, while the heavy component of the target Ho has maximal charge for larger values of {rho}. The influence of {rho} to the energy spectra and intensity of plasma ions is also investigated. In the case of solid (PbMg) target the increase of the fraction of Mg leads to the widening of the energy spectra ofmore » Pb ions by more than a factor of two, while the intensity of Pb ions of all charge states does not depend on the Mg fraction. These effects are explained by the friction existing between light and heavy ions during their expansion away from the target.« less

Orbitally dependent kinetic exchange in a heterobimetallic pair: Ferromagnetic spin alignment and magnetic anisotropy in the cyano-bridged Cr(III)Fe(II) dimer

NASA Astrophysics Data System (ADS)

Palii, A. V.; Tsukerblat, B. S.; Verdaguer, M.

2002-11-01

The problem of the kinetic exchange interaction in the cyanide-bridged heterobinuclear dimers involving orbitally degenerate transition metal ions is considered. The developed approach is based on the concept of the effective Hamiltonian of the orbitally dependent kinetic exchange. We deduce this many-electron Hamiltonian on the microscopic background so that all relevant biorbital transfer processes are taken into account as well as the properties of the many-electron states. The bioctahedral cyanide-bridged Cr(III)Fe(II) dimer is considered in detail as an example distinctly exhibiting new quantitative and qualitative features of the orbitally dependent exchange and as a structural unit of three-dimensional ferromagnetic crystals {Fe(II)3)Cr(III)(CN62}[middle dot]13H2O. The proposed mechanism of the kinetic exchange involves the electron transfer from the double occupied t2 orbitals of Fe(II) [ground state 5T2(t2)4e2] to the half occupied t2 orbitals of Cr(III) [ground state 4A2(t2)3] resulting in the charge transfer state 3T1(t2)4Cr(II)- 6A1(t2)3e2 Fe(III) and the transfer between the half-occupied t2 orbitals of the metal ions resulting in the charge transfer state 3T1(t2)4Cr(II)- 4T2(t2)3e2 Fe(III). The effective Hamiltonian of the orbitally dependent exchange for the Cr(III)Fe(II) pair deduced within this theoretical framework describes competitive ferro- and antiferromagnetic contributions arising from these two charge transfer states. This Hamiltonian leads to a complex energy pattern, consisting of two interpenetrating Heisenberg-like schemes, one exhibiting ferromagnetic and another one antiferromagnetic splitting. The condition for the ferromagnetic spin alignment in the ground state is deduced. The orbitally dependent terms of the Hamiltonian are shown to give rise to a strong magnetic anisotropy of the system, this result as well as the condition for the spin alignment in the ground term are shown to be out of the scope of the Goodenough-Kanamori rules. Along with the full spin S the energy levels are labeled by the orbital quantum numbers providing thus the direct information about the magnetic anisotropy of the system. Under a reasonable estimation of the excitation energies based on the optical absorption data we conclude that the kinetic exchange in the cyanide-bridged Cr(III)Fe(II) pair leads to the ferromagnetic spin alignment exhibiting at the same time strong axial magnetic anisotropy with C4 easy axis of magnetization.

Constraining the magnitude of the Chiral Magnetic Effect with Event Shape Engineering in Pb-Pb collisions at √{sNN } = 2.76 TeV

NASA Astrophysics Data System (ADS)

Acharya, S.; Adam, J.; Adamová, D.; Adolfsson, J.; Aggarwal, M. M.; Aglieri Rinella, G.; Agnello, M.; Agrawal, N.; Ahammed, Z.; Ahmad, N.; Ahn, S. U.; Aiola, S.; Akindinov, A.; Al-Turany, M.; Alam, S. N.; Albuquerque, D. S. D.; Aleksandrov, D.; Alessandro, B.; Alfaro Molina, R.; Alici, A.; Alkin, A.; Alme, J.; Alt, T.; Altenkamper, L.; Altsybeev, I.; Alves Garcia Prado, C.; Andrei, C.; Andreou, D.; Andrews, H. A.; Andronic, A.; Anguelov, V.; Anson, C.; Antičić, T.; Antinori, F.; Antonioli, P.; Anwar, R.; Aphecetche, L.; Appelshäuser, H.; Arcelli, S.; Arnaldi, R.; Arnold, O. W.; Arsene, I. C.; Arslandok, M.; Audurier, B.; Augustinus, A.; Averbeck, R.; Azmi, M. D.; Badalà, A.; Baek, Y. W.; Bagnasco, S.; Bailhache, R.; Bala, R.; Baldisseri, A.; Ball, M.; Baral, R. C.; Barbano, A. M.; Barbera, R.; Barile, F.; Barioglio, L.; Barnaföldi, G. G.; Barnby, L. S.; Barret, V.; Bartalini, P.; Barth, K.; Bartsch, E.; Basile, M.; Bastid, N.; Basu, S.; Batigne, G.; Batyunya, B.; Batzing, P. C.; Bazo Alba, J. L.; Bearden, I. G.; Beck, H.; Bedda, C.; Behera, N. K.; Belikov, I.; Bellini, F.; Bello Martinez, H.; Bellwied, R.; Beltran, L. G. E.; Belyaev, V.; Bencedi, G.; Beole, S.; Bercuci, A.; Berdnikov, Y.; Berenyi, D.; Bertens, R. A.; Berzano, D.; Betev, L.; Bhasin, A.; Bhat, I. R.; Bhati, A. K.; Bhattacharjee, B.; Bhom, J.; Bianchi, A.; Bianchi, L.; Bianchi, N.; Bianchin, C.; Bielčík, J.; Bielčíková, J.; Bilandzic, A.; Biro, G.; Biswas, R.; Biswas, S.; Blair, J. T.; Blau, D.; Blume, C.; Boca, G.; Bock, F.; Bogdanov, A.; Boldizsár, L.; Bombara, M.; Bonomi, G.; Bonora, M.; Book, J.; Borel, H.; Borissov, A.; Borri, M.; Botta, E.; Bourjau, C.; Bratrud, L.; Braun-Munzinger, P.; Bregant, M.; Broker, T. A.; Broz, M.; Brucken, E. J.; Bruna, E.; Bruno, G. E.; Budnikov, D.; Buesching, H.; Bufalino, S.; Buhler, P.; Buncic, P.; Busch, O.; Buthelezi, Z.; Butt, J. B.; Buxton, J. T.; Cabala, J.; Caffarri, D.; Caines, H.; Caliva, A.; Calvo Villar, E.; Camerini, P.; Capon, A. A.; Carena, F.; Carena, W.; Carnesecchi, F.; Castillo Castellanos, J.; Castro, A. J.; Casula, E. A. R.; Ceballos Sanchez, C.; Cerello, P.; Chandra, S.; Chang, B.; Chapeland, S.; Chartier, M.; Chattopadhyay, S.; Chattopadhyay, S.; Chauvin, A.; Cheshkov, C.; Cheynis, B.; Chibante Barroso, V.; Chinellato, D. D.; Cho, S.; Chochula, P.; Chojnacki, M.; Choudhury, S.; Chowdhury, T.; Christakoglou, P.; Christensen, C. H.; Christiansen, P.; Chujo, T.; Chung, S. U.; Cicalo, C.; Cifarelli, L.; Cindolo, F.; Cleymans, J.; Colamaria, F.; Colella, D.; Collu, A.; Colocci, M.; Concas, M.; Conesa Balbastre, G.; Conesa Del Valle, Z.; Connors, M. E.; Contreras, J. G.; Cormier, T. M.; Corrales Morales, Y.; Cortés Maldonado, I.; Cortese, P.; Cosentino, M. R.; Costa, F.; Costanza, S.; Crkovská, J.; Crochet, P.; Cuautle, E.; Cunqueiro, L.; Dahms, T.; Dainese, A.; Danisch, M. C.; Danu, A.; Das, D.; Das, I.; Das, S.; Dash, A.; Dash, S.; de, S.; de Caro, A.; de Cataldo, G.; de Conti, C.; de Cuveland, J.; de Falco, A.; de Gruttola, D.; De Marco, N.; de Pasquale, S.; de Souza, R. D.; Degenhardt, H. F.; Deisting, A.; Deloff, A.; Deplano, C.; Dhankher, P.; di Bari, D.; di Mauro, A.; di Nezza, P.; di Ruzza, B.; Diaz Corchero, M. A.; Dietel, T.; Dillenseger, P.; Divià, R.; Djuvsland, Ø.; Dobrin, A.; Domenicis Gimenez, D.; Dönigus, B.; Dordic, O.; Doremalen, L. V. R.; Dubey, A. K.; Dubla, A.; Ducroux, L.; Duggal, A. K.; Dukhishyam, M.; Dupieux, P.; Ehlers, R. J.; Elia, D.; Endress, E.; Engel, H.; Epple, E.; Erazmus, B.; Erhardt, F.; Espagnon, B.; Esumi, S.; Eulisse, G.; Eum, J.; Evans, D.; Evdokimov, S.; Fabbietti, L.; Faivre, J.; Fantoni, A.; Fasel, M.; Feldkamp, L.; Feliciello, A.; Feofilov, G.; Fernández Téllez, A.; Ferreiro, E. G.; Ferretti, A.; Festanti, A.; Feuillard, V. J. G.; Figiel, J.; Figueredo, M. A. S.; Filchagin, S.; Finogeev, D.; Fionda, F. M.; Floris, M.; Foertsch, S.; Foka, P.; Fokin, S.; Fragiacomo, E.; Francescon, A.; Francisco, A.; Frankenfeld, U.; Fronze, G. G.; Fuchs, U.; Furget, C.; Furs, A.; Fusco Girard, M.; Gaardhøje, J. J.; Gagliardi, M.; Gago, A. M.; Gajdosova, K.; Gallio, M.; Galvan, C. D.; Ganoti, P.; Garabatos, C.; Garcia-Solis, E.; Garg, K.; Gargiulo, C.; Gasik, P.; Gauger, E. F.; Gay Ducati, M. B.; Germain, M.; Ghosh, J.; Ghosh, P.; Ghosh, S. K.; Gianotti, P.; Giubellino, P.; Giubilato, P.; Gladysz-Dziadus, E.; Glässel, P.; Goméz Coral, D. M.; Gomez Ramirez, A.; Gonzalez, A. S.; Gonzalez, V.; González-Zamora, P.; Gorbunov, S.; Görlich, L.; Gotovac, S.; Grabski, V.; Graczykowski, L. K.; Graham, K. L.; Greiner, L.; Grelli, A.; Grigoras, C.; Grigoriev, V.; Grigoryan, A.; Grigoryan, S.; Gronefeld, J. M.; Grosa, F.; Grosse-Oetringhaus, J. F.; Grosso, R.; Gruber, L.; Guber, F.; Guernane, R.; Guerzoni, B.; Gulbrandsen, K.; Gunji, T.; Gupta, A.; Gupta, R.; Guzman, I. B.; Haake, R.; Hadjidakis, C.; Hamagaki, H.; Hamar, G.; Hamon, J. C.; Haque, M. R.; Harris, J. W.; Harton, A.; Hassan, H.; Hatzifotiadou, D.; Hayashi, S.; Heckel, S. T.; Hellbär, E.; Helstrup, H.; Herghelegiu, A.; Hernandez, E. G.; Herrera Corral, G.; Herrmann, F.; Hess, B. A.; Hetland, K. F.; Hillemanns, H.; Hills, C.; Hippolyte, B.; Hladky, J.; Hohlweger, B.; Horak, D.; Hornung, S.; Hosokawa, R.; Hristov, P.; Hughes, C.; Humanic, T. J.; Hussain, N.; Hussain, T.; Hutter, D.; Hwang, D. S.; Iga Buitron, S. A.; Ilkaev, R.; Inaba, M.; Ippolitov, M.; Irfan, M.; Islam, M. S.; Ivanov, M.; Ivanov, V.; Izucheev, V.; Jacak, B.; Jacazio, N.; Jacobs, P. M.; Jadhav, M. B.; Jadlovsky, J.; Jaelani, S.; Jahnke, C.; Jakubowska, M. J.; Janik, M. A.; Jayarathna, P. H. S. Y.; Jena, C.; Jena, S.; Jercic, M.; Jimenez Bustamante, R. T.; Jones, P. G.; Jusko, A.; Kalinak, P.; Kalweit, A.; Kang, J. H.; Kaplin, V.; Kar, S.; Karasu Uysal, A.; Karavichev, O.; Karavicheva, T.; Karayan, L.; Karczmarczyk, P.; Karpechev, E.; Kebschull, U.; Keidel, R.; Keijdener, D. L. D.; Keil, M.; Ketzer, B.; Khabanova, Z.; Khan, P.; Khan, S. A.; Khanzadeev, A.; Kharlov, Y.; Khatun, A.; Khuntia, A.; Kielbowicz, M. M.; Kileng, B.; Kim, B.; Kim, D.; Kim, D. J.; Kim, H.; Kim, J. S.; Kim, J.; Kim, M.; Kim, M.; Kim, S.; Kim, T.; Kirsch, S.; Kisel, I.; Kiselev, S.; Kisiel, A.; Kiss, G.; Klay, J. L.; Klein, C.; Klein, J.; Klein-Bösing, C.; Klewin, S.; Kluge, A.; Knichel, M. L.; Knospe, A. G.; Kobdaj, C.; Kofarago, M.; Köhler, M. K.; Kollegger, T.; Kondratiev, V.; Kondratyeva, N.; Kondratyuk, E.; Konevskikh, A.; Konyushikhin, M.; Kopcik, M.; Kour, M.; Kouzinopoulos, C.; Kovalenko, O.; Kovalenko, V.; Kowalski, M.; Koyithatta Meethaleveedu, G.; Králik, I.; Kravčáková, A.; Kreis, L.; Krivda, M.; Krizek, F.; Kryshen, E.; Krzewicki, M.; Kubera, A. M.; Kučera, V.; Kuhn, C.; Kuijer, P. G.; Kumar, A.; Kumar, J.; Kumar, L.; Kumar, S.; Kundu, S.; Kurashvili, P.; Kurepin, A.; Kurepin, A. B.; Kuryakin, A.; Kushpil, S.; Kweon, M. J.; Kwon, Y.; La Pointe, S. L.; La Rocca, P.; Lagana Fernandes, C.; Lai, Y. S.; Lakomov, I.; Langoy, R.; Lapidus, K.; Lara, C.; Lardeux, A.; Lattuca, A.; Laudi, E.; Lavicka, R.; Lea, R.; Leardini, L.; Lee, S.; Lehas, F.; Lehner, S.; Lehrbach, J.; Lemmon, R. C.; Lenti, V.; Leogrande, E.; León Monzón, I.; Lévai, P.; Li, X.; Lien, J.; Lietava, R.; Lim, B.; Lindal, S.; Lindenstruth, V.; Lindsay, S. W.; Lippmann, C.; Lisa, M. A.; Litichevskyi, V.; Llope, W. J.; Lodato, D. F.; Loenne, P. I.; Loginov, V.; Loizides, C.; Loncar, P.; Lopez, X.; López Torres, E.; Lowe, A.; Luettig, P.; Luhder, J. R.; Lunardon, M.; Luparello, G.; Lupi, M.; Lutz, T. H.; Maevskaya, A.; Mager, M.; Mahajan, S.; Mahmood, S. M.; Maire, A.; Majka, R. D.; Malaev, M.; Malinina, L.; Mal'Kevich, D.; Malzacher, P.; Mamonov, A.; Manko, V.; Manso, F.; Manzari, V.; Mao, Y.; Marchisone, M.; Mareš, J.; Margagliotti, G. V.; Margotti, A.; Margutti, J.; Marín, A.; Markert, C.; Marquard, M.; Martin, N. A.; Martinengo, P.; Martinez, J. A. L.; Martínez, M. I.; Martínez García, G.; Martinez Pedreira, M.; Masciocchi, S.; Masera, M.; Masoni, A.; Masson, E.; Mastroserio, A.; Mathis, A. M.; Matuoka, P. F. T.; Matyja, A.; Mayer, C.; Mazer, J.; Mazzilli, M.; Mazzoni, M. A.; Meddi, F.; Melikyan, Y.; Menchaca-Rocha, A.; Meninno, E.; Mercado Pérez, J.; Meres, M.; Mhlanga, S.; Miake, Y.; Mieskolainen, M. M.; Mihaylov, D. L.; Mikhaylov, K.; Milosevic, J.; Mischke, A.; Mishra, A. N.; Miśkowiec, D.; Mitra, J.; Mitu, C. M.; Mohammadi, N.; Mohanty, B.; Mohisin Khan, M.; Montes, E.; Moreira de Godoy, D. A.; Moreno, L. A. P.; Moretto, S.; Morreale, A.; Morsch, A.; Muccifora, V.; Mudnic, E.; Mühlheim, D.; Muhuri, S.; Mukherjee, M.; Mulligan, J. D.; Munhoz, M. G.; Münning, K.; Munzer, R. H.; Murakami, H.; Murray, S.; Musa, L.; Musinsky, J.; Myers, C. J.; Myrcha, J. W.; Nag, D.; Naik, B.; Nair, R.; Nandi, B. K.; Nania, R.; Nappi, E.; Narayan, A.; Naru, M. U.; Natal da Luz, H.; Nattrass, C.; Navarro, S. R.; Nayak, K.; Nayak, R.; Nayak, T. K.; Nazarenko, S.; Nedosekin, A.; Negrao de Oliveira, R. A.; Nellen, L.; Nesbo, S. V.; Ng, F.; Nicassio, M.; Niculescu, M.; Niedziela, J.; Nielsen, B. S.; Nikolaev, S.; Nikulin, S.; Nikulin, V.; Noferini, F.; Nomokonov, P.; Nooren, G.; Noris, J. C. C.; Norman, J.; Nyanin, A.; Nystrand, J.; Oeschler, H.; Oh, S.; Ohlson, A.; Okubo, T.; Olah, L.; Oleniacz, J.; Oliveira da Silva, A. C.; Oliver, M. H.; Onderwaater, J.; Oppedisano, C.; Orava, R.; Oravec, M.; Ortiz Velasquez, A.; Oskarsson, A.; Otwinowski, J.; Oyama, K.; Pachmayer, Y.; Pacik, V.; Pagano, D.; Pagano, P.; Paić, G.; Palni, P.; Pan, J.; Pandey, A. K.; Panebianco, S.; Papikyan, V.; Pappalardo, G. S.; Pareek, P.; Park, J.; Parmar, S.; Passfeld, A.; Pathak, S. P.; Patra, R. N.; Paul, B.; Pei, H.; Peitzmann, T.; Peng, X.; Pereira, L. G.; Pereira da Costa, H.; Peresunko, D.; Perez Lezama, E.; Peskov, V.; Pestov, Y.; Petráček, V.; Petrov, V.; Petrovici, M.; Petta, C.; Pezzi, R. P.; Piano, S.; Pikna, M.; Pillot, P.; Pimentel, L. O. D. L.; Pinazza, O.; Pinsky, L.; Piyarathna, D. B.; Płoskoń, M.; Planinic, M.; Pliquett, F.; Pluta, J.; Pochybova, S.; Podesta-Lerma, P. L. M.; Poghosyan, M. G.; Polichtchouk, B.; Poljak, N.; Poonsawat, W.; Pop, A.; Poppenborg, H.; Porteboeuf-Houssais, S.; Pozdniakov, V.; Prasad, S. K.; Preghenella, R.; Prino, F.; Pruneau, C. A.; Pshenichnov, I.; Puccio, M.; Puddu, G.; Pujahari, P.; Punin, V.; Putschke, J.; Raha, S.; Rajput, S.; Rak, J.; Rakotozafindrabe, A.; Ramello, L.; Rami, F.; Rana, D. B.; Raniwala, R.; Raniwala, S.; Räsänen, S. S.; Rascanu, B. T.; Rathee, D.; Ratza, V.; Ravasenga, I.; Read, K. F.; Redlich, K.; Rehman, A.; Reichelt, P.; Reidt, F.; Ren, X.; Renfordt, R.; Reolon, A. R.; Reshetin, A.; Reygers, K.; Riabov, V.; Ricci, R. A.; Richert, T.; Richter, M.; Riedler, P.; Riegler, W.; Riggi, F.; Ristea, C.; Rodríguez Cahuantzi, M.; Røed, K.; Rogochaya, E.; Rohr, D.; Röhrich, D.; Rokita, P. S.; Ronchetti, F.; Rosas, E. D.; Rosnet, P.; Rossi, A.; Rotondi, A.; Roukoutakis, F.; Roy, A.; Roy, C.; Roy, P.; Rubio Montero, A. J.; Rueda, O. V.; Rui, R.; Rumyantsev, B.; Rustamov, A.; Ryabinkin, E.; Ryabov, Y.; Rybicki, A.; Saarinen, S.; Sadhu, S.; Sadovsky, S.; Šafařík, K.; Saha, S. K.; Sahlmuller, B.; Sahoo, B.; Sahoo, P.; Sahoo, R.; Sahoo, S.; Sahu, P. K.; Saini, J.; Sakai, S.; Saleh, M. A.; Salzwedel, J.; Sambyal, S.; Samsonov, V.; Sandoval, A.; Sarkar, D.; Sarkar, N.; Sarma, P.; Sas, M. H. P.; Scapparone, E.; Scarlassara, F.; Schaefer, B.; Scharenberg, R. P.; Scheid, H. S.; Schiaua, C.; Schicker, R.; Schmidt, C.; Schmidt, H. R.; Schmidt, M. O.; Schmidt, M.; Schmidt, N. V.; Schukraft, J.; Schutz, Y.; Schwarz, K.; Schweda, K.; Scioli, G.; Scomparin, E.; Šefčík, M.; Seger, J. E.; Sekiguchi, Y.; Sekihata, D.; Selyuzhenkov, I.; Senosi, K.; Senyukov, S.; Serradilla, E.; Sett, P.; Sevcenco, A.; Shabanov, A.; Shabetai, A.; Shahoyan, R.; Shaikh, W.; Shangaraev, A.; Sharma, A.; Sharma, A.; Sharma, M.; Sharma, M.; Sharma, N.; Sheikh, A. I.; Shigaki, K.; Shou, Q.; Shtejer, K.; Sibiriak, Y.; Siddhanta, S.; Sielewicz, K. M.; Siemiarczuk, T.; Silaeva, S.; Silvermyr, D.; Silvestre, C.; Simatovic, G.; Simonetti, G.; Singaraju, R.; Singh, R.; Singhal, V.; Sinha, T.; Sitar, B.; Sitta, M.; Skaali, T. B.; Slupecki, M.; Smirnov, N.; Snellings, R. J. M.; Snellman, T. W.; Song, J.; Song, M.; Soramel, F.; Sorensen, S.; Sozzi, F.; Spiriti, E.; Sputowska, I.; Srivastava, B. K.; Stachel, J.; Stan, I.; Stankus, P.; Stenlund, E.; Stocco, D.; Storetvedt, M. M.; Strmen, P.; Suaide, A. A. P.; Sugitate, T.; Suire, C.; Suleymanov, M.; Suljic, M.; Sultanov, R.; Šumbera, M.; Sumowidagdo, S.; Suzuki, K.; Swain, S.; Szabo, A.; Szarka, I.; Tabassam, U.; Takahashi, J.; Tambave, G. J.; Tanaka, N.; Tarhini, M.; Tariq, M.; Tarzila, M. G.; Tauro, A.; Tejeda Muñoz, G.; Telesca, A.; Terasaki, K.; Terrevoli, C.; Teyssier, B.; Thakur, D.; Thakur, S.; Thomas, D.; Thoresen, F.; Tieulent, R.; Tikhonov, A.; Timmins, A. R.; Toia, A.; Torres, S. R.; Tripathy, S.; Trogolo, S.; Trombetta, G.; Tropp, L.; Trubnikov, V.; Trzaska, W. H.; Trzeciak, B. A.; Tsuji, T.; Tumkin, A.; Turrisi, R.; Tveter, T. S.; Ullaland, K.; Umaka, E. N.; Uras, A.; Usai, G. L.; Utrobicic, A.; Vala, M.; van der Maarel, J.; van Hoorne, J. W.; van Leeuwen, M.; Vanat, T.; Vande Vyvre, P.; Varga, D.; Vargas, A.; Vargyas, M.; Varma, R.; Vasileiou, M.; Vasiliev, A.; Vauthier, A.; Vázquez Doce, O.; Vechernin, V.; Veen, A. M.; Velure, A.; Vercellin, E.; Vergara Limón, S.; Vernet, R.; Vértesi, R.; Vickovic, L.; Vigolo, S.; Viinikainen, J.; Vilakazi, Z.; Villalobos Baillie, O.; Villatoro Tello, A.; Vinogradov, A.; Vinogradov, L.; Virgili, T.; Vislavicius, V.; Vodopyanov, A.; Völkl, M. A.; Voloshin, K.; Voloshin, S. A.; Volpe, G.; von Haller, B.; Vorobyev, I.; Voscek, D.; Vranic, D.; Vrláková, J.; Wagner, B.; Wang, H.; Wang, M.; Watanabe, D.; Watanabe, Y.; Weber, M.; Weber, S. G.; Weiser, D. F.; Wenzel, S. C.; Wessels, J. P.; Westerhoff, U.; Whitehead, A. M.; Wiechula, J.; Wikne, J.; Wilk, G.; Wilkinson, J.; Willems, G. A.; Williams, M. C. S.; Willsher, E.; Windelband, B.; Witt, W. E.; Yalcin, S.; Yamakawa, K.; Yang, P.; Yano, S.; Yin, Z.; Yokoyama, H.; Yoo, I.-K.; Yoon, J. H.; Yurchenko, V.; Zaccolo, V.; Zaman, A.; Zampolli, C.; Zanoli, H. J. C.; Zardoshti, N.; Zarochentsev, A.; Závada, P.; Zaviyalov, N.; Zbroszczyk, H.; Zhalov, M.; Zhang, H.; Zhang, X.; Zhang, Y.; Zhang, C.; Zhang, Z.; Zhao, C.; Zhigareva, N.; Zhou, D.; Zhou, Y.; Zhou, Z.; Zhu, H.; Zhu, J.; Zichichi, A.; Zimmermann, A.; Zimmermann, M. B.; Zinovjev, G.; Zmeskal, J.; Zou, S.; Alice Collaboration

2018-02-01

In ultrarelativistic heavy-ion collisions, the event-by-event variation of the elliptic flow v2 reflects fluctuations in the shape of the initial state of the system. This allows to select events with the same centrality but different initial geometry. This selection technique, Event Shape Engineering, has been used in the analysis of charge-dependent two- and three-particle correlations in Pb-Pb collisions at √{sNN } = 2.76 TeV. The two-particle correlator 〈 cos ⁡ (φα -φβ) 〉, calculated for different combinations of charges α and β, is almost independent of v2 (for a given centrality), while the three-particle correlator 〈 cos ⁡ (φα +φβ - 2Ψ2) 〉 scales almost linearly both with the event v2 and charged-particle pseudorapidity density. The charge dependence of the three-particle correlator is often interpreted as evidence for the Chiral Magnetic Effect (CME), a parity violating effect of the strong interaction. However, its measured dependence on v2 points to a large non-CME contribution to the correlator. Comparing the results with Monte Carlo calculations including a magnetic field due to the spectators, the upper limit of the CME signal contribution to the three-particle correlator in the 10-50% centrality interval is found to be 26-33% at 95% confidence level.

Energy and charge transfer dynamics between Alq3 and CdSeS nanocrystals.

PubMed

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.

Unusual Thermoelectric Behavior Indicating a Hopping to Bandlike Transport Transition in Pentacene

NASA Astrophysics Data System (ADS)

Germs, W. Chr.; Guo, K.; Janssen, R. A. J.; Kemerink, M.

2012-07-01

An unusual increase in the Seebeck coefficient with increasing charge carrier density is observed in pentacene thin film transistors. This behavior is interpreted as being due to a transition from hopping transport in static localized states to bandlike transport, occurring at temperatures below ˜250K. Such a transition can be expected for organic materials in which both static energetic disorder and dynamic positional disorder are important. While clearly visible in the temperature and density dependent Seebeck coefficient, the transition hardly shows up in the charge carrier mobility.

Characteristics of dielectric properties and conduction mechanism of TlInS2:Cu single crystals

NASA Astrophysics Data System (ADS)

El-Nahass, M. M.; Ali, H. A. M.; El-Zaidia, E. F. M.

2013-12-01

Single crystals of TlInS2:Cu were grown by the modified Bridgman method. The dielectric behavior of TlInS2:Cu was investigated using the impedance spectroscopy technique. The real (ε1), imaginary (ε2) parts of complex dielectric permittivity and ac conductivity were measured in the frequency range (42-2×105) Hz with a variation of temperature in the range from 291 K to 483 K. The impedance data were presented in Nyquist diagrams for different temperatures. The frequency dependence of σtot (ω) follows the Jonscher's universal dynamic law with the relation σtot (ω)=σdc+Aωs, (where s is the frequency exponent). The mechanism of the ac charge transport across the layers of TlInS2:Cu single crystals was referred to the hopping over localized states near the Fermi level. The examined system exhibits temperature dependence of σac (ω), which showed a linear increase with the increase in temperature at different frequencies. Some parameters were calculated as: the density of localized states near the Fermi level, NF, the average time of charge carrier hopping between localized states, τ, and the average hopping distance, R.

Controllable spin-charge transport in strained graphene nanoribbon devices

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

Diniz, Ginetom S., E-mail: ginetom@gmail.com; Guassi, Marcos R.; Qu, Fanyao

2014-09-21

We theoretically investigate the spin-charge transport in two-terminal device of graphene nanoribbons in the presence of a uniform uniaxial strain, spin-orbit coupling, exchange field, and smooth staggered potential. We show that the direction of applied strain can efficiently tune strain-strength induced oscillation of band-gap of armchair graphene nanoribbon (AGNR). It is also found that electronic conductance in both AGNR and zigzag graphene nanoribbon (ZGNR) oscillates with Rashba spin-orbit coupling akin to the Datta-Das field effect transistor. Two distinct strain response regimes of electronic conductance as function of spin-orbit couplings magnitude are found. In the regime of small strain, conductance ofmore » ZGNR presents stronger strain dependence along the longitudinal direction of strain. Whereas for high values of strain shows larger effect for the transversal direction. Furthermore, the local density of states shows that depending on the smoothness of the staggered potential, the edge states of AGNR can either emerge or be suppressed. These emerging states can be determined experimentally by either spatially scanning tunneling microscope or by scanning tunneling spectroscopy. Our findings open up new paradigms of manipulation and control of strained graphene based nanostructure for application on novel topological quantum devices.« less

Electronic Interactions of Michler's Ketone with DNA Bases in Synthetic Hairpins.

PubMed

Jalilov, Almaz S; Young, Ryan M; Eaton, Samuel W; Wasielewski, Michael R; Lewis, Frederick D

2015-01-01

The mechanism and dynamics of photoinduced electron transfer in two families of DNA hairpins possessing Michler's ketone linkers have been investigated by means of steady state and time-resolved transient absorption and emission spectroscopies. The excited state behavior of the diol linker employed in hairpin synthesis is similar to that of Michler's ketone in methanol solution. Hairpins possessing only a Michler's ketone linker undergo fast singlet state charge separation and charge recombination with an adjacent purine base, attributed to well-stacked ground state conformations, and intersystem crossing to the triplet state, attributed to poorly stacked ground state conformations. The failure of the triplet to undergo electron transfer reactions on the 7 ns time scale of our measurements is attributed to the low triplet energy and reduction potential of the twisted triplet state. Hairpins possessing both a Michler's ketone linker and a perylenediimide base surrogate separated by four base pairs undergo photoinduced hole transport from the diimide to Michler's ketone upon excitation of the diimide. The efficiency of hole transport is dependent upon the sequence of the intervening purine bases. © 2014 The American Society of Photobiology.

Gas-Phase Stability of Negatively Charged Organophosphate Metabolites Produced by Electrospray Ionization and Matrix-Assisted Laser Desorption/Ionization

NASA Astrophysics Data System (ADS)

Asakawa, Daiki; Mizuno, Hajime; Toyo'oka, Toshimasa

2017-12-01

The formation mechanisms of singly and multiply charged organophosphate metabolites by electrospray ionization (ESI) and their gas phase stabilities were investigated. Metabolites containing multiple phosphate groups, such as adenosine 5'-diphosphate (ADP), adenosine 5'-triphosphate (ATP), and D- myo-inositol-1,4,5-triphosphate (IP3) were observed as doubly deprotonated ions by negative-ion ESI mass spectrometry. Organophosphates with multiple negative charges were found to be unstable and often underwent loss of PO3 -, although singly deprotonated analytes were stable. The presence of fragments due to the loss of PO3 - in the negative-ion ESI mass spectra could result in the misinterpretation of analytical results. In contrast to ESI, matrix-assisted laser desorption ionization (MALDI) produced singly charged organophosphate metabolites with no associated fragmentation, since the singly charged anions are stable. The stability of an organophosphate metabolite in the gas phase strongly depends on its charge state. The fragmentations of multiply charged organophosphates were also investigated in detail through density functional theory calculations. [Figure not available: see fulltext.

Critical Nuclear Charge of the Quantum Mechanical Three-Body Problem

NASA Astrophysics Data System (ADS)

Busuttil, Michael; Moini, Amirreza; Drake, Gordon W. F.

2014-05-01

The critical nuclear charge (Zc) for a three-body quantum mechanical system consisting of positive and negative charges is the minimum nuclear charge that can keep the system in a bound state. Here we present a study of the critical nuclear charge for two-electron (heliumlike) systems with infinite nuclear mass, and also a range of reduced mass ratio (μ / m) up to 0.5. The results help to resolve a discrepancy in the literature for the infinite mass case, and they are the first to study the dependence on reduced mass ratio. It was found that Zc has a local maximum with μ / m = 0 . 352 5 . The critical charge for the infinite mass case is found to be Zc = 0 . 911 028 224 076 8 (1 0) . This value is more accurate than any previous value in the literature, and agrees with the upper bound Zc = 0 . 911 03 reported by Baker et al.. The critical nuclear charge outside this range [0.5 - 1.0] still needs to be investigated in future works. Research Supported by NSERC and SHARCNET.

Investigations on the charge transfer mechanism at donor/acceptor interfaces in the quest for descriptors of organic solar cell performance.

PubMed

Muraoka, Azusa; Fujii, Mikiya; Mishima, Kenji; Matsunaga, Hiroki; Benten, Hiroaki; Ohkita, Hideo; Ito, Shinzaburo; Yamashita, Koichi

2018-05-07

Herein, we theoretically and experimentally investigated the mechanisms of charge separation processes of organic thin-film solar cells. PTB7, PTB1, and PTBF2 have been chosen as donors and PC 71 BM has been chosen as an acceptor considering that effective charge generation depends on the difference between the material combinations. Experimental results of transient absorption spectroscopy show that the hot process is a key step for determining external quantum efficiency (EQE) in these systems. From the quantum chemistry calculations, it has been found that EQE tends to increase as the transferred charge, charge transfer distance, and variation of dipole moments between the ground and excited states of the donor/acceptor complexes increase; this indicates that these physical quantities are a good descriptor to assess the donor-acceptor charge transfer quality contributing to the solar cell performance. We propose that designing donor/acceptor interfaces with large values of charge transfer distance and variation of dipole moments of the donor/acceptor complexes is a prerequisite for developing high-efficiency polymer/PCBM solar cells.

Pressure dependence of the optical properties of the charge-density-wave compound LaTe2

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

Lavagnini, M.; Sacchetti, A.; Degiorgi, L.

2009-12-14

We report the pressure dependence of the optical response of LaTe{sub 2}, which is deep in the charge-density-wave (CDW) ground state even at 300 K. The reflectivity spectrum is collected in the mid-infrared spectral range at room temperature and at pressures between 0 and 7 GPa. We extract the energy scale due to the single particle excitation across the CDW gap and the Drude weight. We establish that the gap decreases upon compressing the lattice, while the Drude weight increases. This signals a reduction in the quality of nesting upon applying pressure, therefore inducing a lesser impact of the CDWmore » condensate on the electronic properties of LaTe{sub 2}. The consequent suppression of the CDW gap leads to a release of additional charge carriers, manifested by the shift of weight from the gap feature into the metallic component of the optical response. On the contrary, the power-law behavior, seen in the optical conductivity at energies above the gap excitation and indicating a weakly interacting limit within the Tomonaga-Luttinger liquid scenario, seems to be only moderately dependent on pressure.« less

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

Möller, Christian, E-mail: cmoeller@cismst.de; TU Ilmenau, Institut für Physik, Weimarer Str. 32, 98693 Ilmenau; Bartel, Til

Iron-boron (FeB) pairing is observed in the n-type region of a boron and phosphorus co-doped silicon sample which is unexpected from the FeB pair model of Kimerling and Benton. To explain the experimental data, the existing FeB pair model is extended by taking into account the electronic capture and emission rates at the interstitial iron (Fe{sub i}) trap level as a function of the charge carrier densities. According to this model, the charge state of the Fe{sub i} may be charged in n-type making FeB association possible. Further, FeB pair formation during illumination in p-type silicon is investigated. This permitsmore » the determination of the charge carrier density dependent FeB dissociation rate and in consequence allows to determine the acceptor concentration in the co-doped n-type silicon by lifetime measurement.« less

Ultrafast large-amplitude relocation of electronic charge in ionic crystals

PubMed Central

Zamponi, Flavio; Rothhardt, Philip; Stingl, Johannes; Woerner, Michael; Elsaesser, Thomas

2012-01-01

The interplay of vibrational motion and electronic charge relocation in an ionic hydrogen-bonded crystal is mapped by X-ray powder diffraction with a 100 fs time resolution. Photoexcitation of the prototype material KH2PO4 induces coherent low-frequency motions of the PO4 tetrahedra in the electronically excited state of the crystal while the average atomic positions remain unchanged. Time-dependent maps of electron density derived from the diffraction data demonstrate an oscillatory relocation of electronic charge with a spatial amplitude two orders of magnitude larger than the underlying vibrational lattice motions. Coherent longitudinal optical and tranverse optical phonon motions that dephase on a time scale of several picoseconds, drive the charge relocation, similar to a soft (transverse optical) mode driven phase transition between the ferro- and paraelectric phase of KH2PO4. PMID:22431621

Ab initio characterization of electron transfer coupling in photoinduced systems: generalized Mulliken-Hush with configuration-interaction singles.

PubMed

Chen, Hung-Cheng; Hsu, Chao-Ping

2005-12-29

To calculate electronic couplings for photoinduced electron transfer (ET) reactions, we propose and test the use of ab initio quantum chemistry calculation for excited states with the generalized Mulliken-Hush (GMH) method. Configuration-interaction singles (CIS) is proposed to model the locally excited (LE) and charge-transfer (CT) states. When the CT state couples with other high lying LE states, affecting coupling values, the image charge approximation (ICA), as a simple solvent model, can lower the energy of the CT state and decouple the undesired high-lying local excitations. We found that coupling strength is weakly dependent on many details of the solvent model, indicating the validity of the Condon approximation. Therefore, a trustworthy value can be obtained via this CIS-GMH scheme, with ICA used as a tool to improve and monitor the quality of the results. Systems we tested included a series of rigid, sigma-linked donor-bridge-acceptor compounds where "through-bond" coupling has been previously investigated, and a pair of molecules where "through-space" coupling was experimentally demonstrated. The calculated results agree well with experimentally inferred values in the coupling magnitudes (for both systems studied) and in the exponential distance dependence (for the through-bond series). Our results indicate that this new scheme can properly account for ET coupling arising from both through-bond and through-space mechanisms.

Redox probing study of the potential dependence of charge transport through Li 2O 2

DOE PAGES

Knudsen, Kristian B.; Luntz, Alan C.; Jensen, Søren H.; ...

2015-11-20

In the field of energy storage devices the pursuit for cheap, high energy density, reliable secondary batteries is at the top of the agenda. The Li–O 2 battery is one of the possible technologies that, in theory, should be able to close the gap, which exists between the present state-of-the-art Li-ion technologies and the demand placed on batteries by technologies such as electrical vehicles. Here we present a redox probing study of the charge transfer across the main deposition product lithium peroxide, Li 2O 2, in the Li–O 2 battery using outer-sphere redox shuttles. The change in heterogeneous electron transfermore » exchange rate as a function of the potential and the Li 2O 2 layer thickness (~depth-of-discharge) was determined using electrochemical impedance spectroscopy. In addition, the attenuation of the electron transfer exchange rate with film thickness is dependent on the probing potential, providing evidence that hole transport is the dominant process for charge transfer through Li 2O 2 and showing that the origin of the sudden death observed upon discharge is due to charge transport limitations.« less

Solvent control of charge transfer excited state relaxation pathways in [Fe(2,2'-bipyridine)(CN) 4] 2-

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

Kjær, Kasper S.; Kunnus, Kristjan; Harlang, Tobias C. B.

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 (MLCT) excited state of [Fe(bpy)(CN) 4] 2- has a 19 picosecond lifetime and no discernable contribution from metal centered (MC) states in weak Lewis acid solvents, such as dimethyl sulfoxide and acetonitrile. Here, in the present work, we use the same combination of spectroscopic techniques to measure the MLCT excited state relaxation dynamics of [Fe(bpy)(CN) 4] 2-more » 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 has triplet ( 3MC) character, unlike other reported six-coordinate Fe(II)-centered coordination compounds, which form MC quintet ( 5MC) states. The solvent dependent changes in excited state non-radiative relaxation for [Fe(bpy)(CN) 4] 2- allows us to infer the influence of the solvent on the electronic structure of the complex. Lastly, the robust characterization of the dynamics and optical spectral signatures of the isolated 3MC intermediate provides a strong foundation for identifying 3MC intermediates in the electronic excited state relaxation mechanisms of similar Fe-centered systems being developed for solar applications.« less

Solvent control of charge transfer excited state relaxation pathways in [Fe(2,2'-bipyridine)(CN) 4] 2-

DOE PAGES

Kjær, Kasper S.; Kunnus, Kristjan; Harlang, Tobias C. B.; ...

2018-01-19

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 (MLCT) excited state of [Fe(bpy)(CN) 4] 2- has a 19 picosecond lifetime and no discernable contribution from metal centered (MC) states in weak Lewis acid solvents, such as dimethyl sulfoxide and acetonitrile. Here, in the present work, we use the same combination of spectroscopic techniques to measure the MLCT excited state relaxation dynamics of [Fe(bpy)(CN) 4] 2-more » 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 has triplet ( 3MC) character, unlike other reported six-coordinate Fe(II)-centered coordination compounds, which form MC quintet ( 5MC) states. The solvent dependent changes in excited state non-radiative relaxation for [Fe(bpy)(CN) 4] 2- allows us to infer the influence of the solvent on the electronic structure of the complex. Lastly, the robust characterization of the dynamics and optical spectral signatures of the isolated 3MC intermediate provides a strong foundation for identifying 3MC intermediates in the electronic excited state relaxation mechanisms of similar Fe-centered systems being developed for solar applications.« less

Hard X-ray photoemission study of the Fabre salts (TMTTF)2X (X = SbF6 and PF6)

NASA Astrophysics Data System (ADS)

Medjanik, Katerina; de Souza, Mariano; Kutnyakhov, Dmytro; Gloskovskii, Andrei; Müller, Jens; Lang, Michael; Pouget, Jean-Paul; Foury-Leylekian, Pascale; Moradpour, Alec; Elmers, Hans-Joachim; Schönhense, Gerd

2014-11-01

Core-level photoemission spectra of the Fabre salts with X = SbF6 and PF6 were taken using hard X-rays from PETRA III, Hamburg. In these salts TMTTF layers show a significant stack dimerization with a charge transfer of 1 e per dimer to the anion SbF6 or PF6. At room temperature and slightly below the core-level spectra exhibit single lines, characteristic for a well-screened metallic state. At reduced temperatures progressive charge localization sets in, followed by a 2nd order phase transition into a charge-ordered ground state. In both salts groups of new core-level signals occur, shifted towards lower kinetic energies. This is indicative of a reduced transverse-conductivity across the anion layers, visible as layer-dependent charge depletion for both samples. The surface potential was traced via shifts of core-level signals of an adsorbate. A well-defined potential could be established by a conducting cap layer of 5 nm aluminum which appears "transparent" due to the large probing depth of HAXPES (8-10 nm). At the transition into the charge-ordered phase the fluorine 1 s line of (TMTTF)2SbF6 shifts by 2.8 eV to higher binding energy. This is a spectroscopic fingerprint of the loss of inversion symmetry accompanied by a cooperative shift of the SbF6 anions towards the more positively charged TMTTF donors. This shift does not occur for the X = PF6 compound, most likely due to smaller charge disproportion or due to the presence of charge disorder.

Local charge-density change and superconductivity: A positron study

NASA Astrophysics Data System (ADS)

Jean, Y. C.; Sundar, C. S.; Bharathi, A.; Kyle, J.; Nakanishi, H.; Tseng, P. K.; Hor, P. H.; Meng, R. L.; Huang, Z. J.; Chu, C. W.; Wang, Z. Z.; Turchi, P. E. A.; Howell, R. H.; Wachs, A. L.; Fluss, M. J.

1990-03-01

The temperature dependence between 10 and 300 K of the positron lifetime was measured in the high-temperature superconductors YBA2(Cu1-xMx)3O6+δ, where M=Zn and Ga with x=0.0 to 0.07 and δ>0.8. In the undoped and Ga-doped samples, the positron lifetime in the Bloch state, τb, was observed to decrease below Tc. In the Zn-doped samples, a dramatic x-dependent temperature variation of τb was observed: from a decrease of Tb below Tc for x=0.01 to an increase of τb for x>0.02. These new experimental results are interpreted in terms of a change in the local charge density of high-Tc oxides associated with the superconducting transition.

Phonon-assisted changes in charge states of deep level defects in germanium

NASA Astrophysics Data System (ADS)

Markevich, A. V.; Litvinov, V. V.; Emtsev, V. V.; Markevich, V. P.; Peaker, A. R.

2006-04-01

Electronic processes associated with changes in the charge states of the vacancy-oxygen center (VO or A center) and vacancy-group-V-impurity atom (P, As, Sb or Bi) pairs (E centers) in irradiated germanium crystals have been studied using deep level transient spectroscopy (DLTS), high-resolution Laplace DLTS and Hall effect measurements. It is found that the electron emission and capture processes related to transitions between the doubly and the singly negatively charged states of the A center and the E centers in Ge are phonon-assisted, i.e., they are accompanied by significant vibrations and re-arrangements of atoms in the vicinity of the defects. Manifestations of the phonon involvements are: (i) temperature-dependent electron capture cross-sections which are well described in the frame of the multi-phonon-assisted capture model; (ii) large changes in entropy related to the ionization of the defects and, associated with these, temperature-dependent positions of energy levels; and (iii) electron emission via phonon-assisted tunneling upon the application of electric field. These effects have been considered in detail for the vacancy-oxygen and the vacancy-donor complexes. On the basis of a combined analysis of the electronic processes a configuration-coordinate diagram of the acceptor states of the A and E centers is plotted. It is found that changes in the entropy of ionization and the energy for electron emission for these traps follow the empirical Meyer-Neldel rule. A model based on multi-phonon-assisted carrier emission from defects is adapted for the explanation of the origin of this rule for the case of electronic processes in Ge.

Energy shift and conduction-to-valence band transition mediated by a time-dependent potential barrier in graphene

NASA Astrophysics Data System (ADS)

Chaves, Andrey; da Costa, D. R.; de Sousa, G. O.; Pereira, J. M.; Farias, G. A.

2015-09-01

We investigate the scattering of a wave packet describing low-energy electrons in graphene by a time-dependent finite-step potential barrier. Our results demonstrate that, after Klein tunneling through the barrier, the electron acquires an extra energy which depends on the rate of change of the barrier height with time. If this rate is negative, the electron loses energy and ends up as a valence band state after leaving the barrier, which effectively behaves as a positively charged quasiparticle.

Photophysical study of some 3-benzoylmethyleneindol-2-ones and estimation of ground and excited states dipole moments from solvatochromic methods using solvent polarity parameters

NASA Astrophysics Data System (ADS)

Saroj, Manju K.; Sharma, Neera; Rastogi, Ramesh C.

2012-03-01

3-Benzoylmethyleneindol-2-ones, isatin based chalcones containing donor and acceptor moieties that exhibit excited-state intramolecular charge transfer, have been studied in different solvents by absorption and emission spectroscopy. The excited state behavior of these compounds is strongly dependent on the nature of substituents and the environment. These compounds show multiple emissions arising from a locally excited state and the two states due to intramolecular processes viz. intramolecular charge transfer (ICT) and excited state intramolecular proton transfer (ESIPT). Excited-state dipole moments have been calculated using Stoke-shifts of LE and ICT states using solvatochromic methods. The higher values of dipole moments obtained lead to support the formation of ICT state as one of the prominent species in the excited states of all 3-benzoylmethyleneindol-2-ones. The correlation of the solvatochromic Stokes-shifts with the microscopic solvent polarity parameter (ETN) was found to be superior to that obtained using bulk solvent polarity functions. The absorption and florescence spectral characteristics have been also investigated as a function of acidity and basicity (Ho/pH) in aqueous phase.

Reformulated space-charge-limited current model and its application to disordered organic systems

NASA Astrophysics Data System (ADS)

Woellner, Cristiano F.; Freire, José A.

2011-02-01

We have reformulated a traditional model used to describe the current-voltage dependence of low mobility materials sandwiched between planar electrodes by using the quasi-electrochemical potential as the fundamental variable instead of the local electric field or the local charge carrier density. This allows the material density-of-states to enter explicitly in the equations and dispenses with the need to assume a particular type of contact. The diffusion current is included and as a consequence the current-voltage dependence obtained covers, with increasing bias, the diffusion limited current, the space-charge limited current, and the injection limited current regimes. The generalized Einstein relation and the field and density dependent mobility are naturally incorporated into the formalism; these two points being of particular relevance for disordered organic semiconductors. The reformulated model can be applied to any material where the carrier density and the mobility may be written as a function of the quasi-electrochemical potential. We applied it to the textbook example of a nondegenerate, constant mobility material and showed how a single dimensionless parameter determines the form of the I(V) curve. We obtained integral expressions for the carrier density and for the mobility as a function of the quasi-electrochemical potential for a Gaussianly disordered organic material and found the general form of the I(V) curve for such materials over the full range of bias, showing how the energetic disorder alone can give rise, in the space-charge limited current regime, to an I∝Vn dependence with an exponent n larger than 2.

Charging and coagulation of radioactive and nonradioactive particles in the atmosphere

DOE PAGES

Kim, Yong-ha; Yiacoumi, Sotira; Nenes, Athanasios; ...

2016-01-01

Charging and coagulation influence one another and impact the particle charge and size distributions in the atmosphere. However, few investigations to date have focused on the coagulation kinetics of atmospheric particles accumulating charge. This study presents three approaches to include mutual effects of charging and coagulation on the microphysical evolution of atmospheric particles such as radioactive particles. The first approach employs ion balance, charge balance, and a bivariate population balance model (PBM) to comprehensively calculate both charge accumulation and coagulation rates of particles. The second approach involves a much simpler description of charging, and uses a monovariate PBM and subsequentmore » effects of charge on particle coagulation. The third approach is further simplified assuming that particles instantaneously reach their steady-state charge distributions. It is found that compared to the other two approaches, the first approach can accurately predict time-dependent changes in the size and charge distributions of particles over a wide size range covering from the free molecule to continuum regimes. The other two approaches can reliably predict both charge accumulation and coagulation rates for particles larger than about 0.04 micrometers and atmospherically relevant conditions. These approaches are applied to investigate coagulation kinetics of particles accumulating charge in a radioactive neutralizer, the urban atmosphere, and an atmospheric system containing radioactive particles. Limitations of the approaches are discussed.« less

The QCD Equation of state and critical end-point estimates at O (μB6)

NASA Astrophysics Data System (ADS)

Sharma, Sayantan; Bielefeld-BNL-CCNU Collaboration

2017-11-01

We present results for the QCD Equation of State at non-zero chemical potentials corresponding to the conserved charges in QCD using Taylor expansion upto sixth order in the baryon number, electric charge and strangeness chemical potentials. The latter two are constrained by the strangeness neutrality and a fixed electric charge to baryon number ratio. In our calculations, we use the Highly Improved Staggered Quarks (HISQ) discretization scheme at physical quark masses and at different values of the lattice spacings to control lattice cut-off effects. Furthermore we calculate the pressure along lines of constant energy density, which serve as proxies for the freeze-out conditions and discuss their dependence on μB, which is necessary for hydrodynamic modelling near freezeout. We also provide an estimate of the radius of convergence of the Taylor series from the 6th order coefficients which provides a new constraint on the location of the critical end-point in the T-μB plane of the QCD phase diagram.

Valence atom with bohmian quantum potential: the golden ratio approach

PubMed Central

2012-01-01

Background The alternative quantum mechanical description of total energy given by Bohmian theory was merged with the concept of the golden ratio and its appearance as the Heisenberg imbalance to provide a new density-based description of the valence atomic state and reactivity charge with the aim of clarifying their features with respect to the so-called DFT ground state and critical charge, respectively. Results The results, based on the so-called double variational algorithm for chemical spaces of reactivity, are fundamental and, among other issues regarding chemical bonding, solve the existing paradox of using a cubic parabola to describe a quadratic charge dependency. Conclusions Overall, the paper provides a qualitative-quantitative explanation of chemical reactivity based on more than half of an electronic pair in bonding, and provide new, more realistic values for the so-called “universal” electronegativity and chemical hardness of atomic systems engaged in reactivity (analogous to the atoms-in-molecules framework). PMID:23146157

The human peripheral subunit-binding domain folds rapidly while overcoming repulsive Coulomb forces

PubMed Central

Arbely, Eyal; Neuweiler, Hannes; Sharpe, Timothy D; Johnson, Christopher M; Fersht, Alan R

2010-01-01

Peripheral subunit binding domains (PSBDs) are integral parts of large multienzyme complexes involved in carbohydrate metabolism. PSBDs facilitate shuttling of prosthetic groups between different catalytic subunits. Their protein surface is characterized by a high density of positive charges required for binding to subunits within the complex. Here, we investigated folding thermodynamics and kinetics of the human PSBD (HSBD) using circular dichroism and tryptophan fluorescence experiments. HSBD was only marginally stable under physiological solvent conditions but folded within microseconds via a barrier-limited apparent two-state transition, analogous to its bacterial homologues. The high positive surface-charge density of HSBD leads to repulsive Coulomb forces that modulate protein stability and folding kinetics, and appear to even induce native-state movement. The electrostatic strain was alleviated at high solution-ionic-strength by Debye-Hückel screening. Differences in ionic-strength dependent characteristics among PSBD homologues could be explained by differences in their surface charge distributions. The findings highlight the trade-off between protein function and stability during protein evolution. PMID:20662005

Bandgap and pseudohelicity effects over conductance in gapped graphene junctures

NASA Astrophysics Data System (ADS)

Navarro-Giraldo, J. A.; Quimbay, C. J.

2018-07-01

We study the conductance in gapped single-layer graphene junctures as a function of bangap, pseudohelicity and charge carriers density. To do it, we first calculate the transmission coefficients of massive charge carries for p–n and n–p–n junctures of gapped single-layer graphene. Next, we calculate the conductance for these two systems using the Landauer formula. Only for the p–n juncture case and non-zero bandgap values, we find the existence of a contribution to the conductance from pseudohelicity inversion states, which is small compared to the contribution from pseudohelicity conservation states. Also, we find for both type of junctures that there exists a window of charge carriers densities values where the conductance is zero (conductance gap), in such a way that the size of this window depends on the squared of the bandgap. We observe that the existence of a bandgap in the system leads to valley mixing and this fact could be useful for the future design of devices based on single-layer graphene.

Analysis of the kinetics of P+ HA- recombination in membrane-embedded wild-type and mutant Rhodobacter sphaeroides reaction centers between 298 and 77 K indicates that the adjacent negatively charged QA ubiquinone modulates the free energy of P+ HA- and may influence the rate of the protein dielectric response.

PubMed

Gibasiewicz, Krzysztof; Pajzderska, Maria; Dobek, Andrzej; Brettel, Klaus; Jones, Michael R

2013-09-26

Time-resolved spectroscopic studies of recombination of the P(+)HA(-) radical pair in photosynthetic reaction centers (RCs) from Rhodobacter sphaeroides give an opportunity to study protein dynamics triggered by light and occurring over the lifetime of P(+)HA(-). The state P(+)HA(-) is formed after the ultrafast light-induced electron transfer from the primary donor pair of bacteriochlorophylls (P) to the acceptor bacteriopheophytin (HA). In order to increase the lifetime of this state, and thus increase the temporal window for the examination of protein dynamics, it is possible to block forward electron transfer from HA(-) to the secondary electron acceptor QA. In this contribution, the dynamics of P(+)HA(-) recombination were compared at a range of temperatures from 77 K to room temperature, electron transfer from HA(-) to QA being blocked either by prereduction of QA or by genetic removal of QA. The observed P(+)HA(-) charge recombination was significantly slower in the QA-deficient RCs, and in both types of complexes, lowering the temperature from RT to 77 K led to a slowing of charge recombination. The effects are explained in the frame of a model in which charge recombination occurs via competing pathways, one of which is thermally activated and includes transient formation of a higher-energy state, P(+)BA(-). An internal electrostatic field supplied by the negative charge on QA increases the free energy levels of the state P(+)HA(-), thus decreasing its energetic distance to the state P(+)BA(-). In addition, the dielectric response of the protein environment to the appearance of the state P(+)HA(-) is accelerated from ∼50-100 ns in the QA-deficient mutant RCs to ∼1-16 ns in WT RCs with a negatively charged QA(-). In both cases, the temperature dependence of the protein dynamics is weak.

Revisiting Cu 63 NMR evidence for charge order in superconducting La 1.885 Sr 0.115 CuO 4

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

Imai, T.; Takahashi, S. K.; Arsenault, A.

Here, the presence of charge and spin stripe order in the La 2CuO 4-based family of superconductors continues to lead to new insight on the unusual ground-state properties of high- T c cuprates. Soon after the discovery of charge stripe order at T charge≃65 K in Nd 3+ co-doped La 1.48Nd 0.4Sr 0.12CuO 4( Tc≃6 K), Hunt et al. demonstrated that La 1.48Nd 0.4Sr 0.12CuO 4 and superconducting La 2–xSr xCuO 4 with x~1/8( Tc≃30 K) share nearly identical NMR anomalies near Tcharge of the former. Their inevitable conclusion that La 1.885Sr 0.115CuO 4 also undergoes charge order at amore » comparable temperature became controversial, because diffraction measurements at the time were unable to detect Bragg peaks associated with charge order. Recent advances in x-ray diffraction techniques finally led to definitive confirmations of the charge order Bragg peaks in La 1.885Sr 0.115CuO 4 with an onset at as high as Tcharge≃80 K. Meanwhile, improved instrumental technology has enabled routine NMR measurements that were not feasible two decades ago. Motivated by these new developments, we revisit the charge order transition of a La 1.885Sr 0.115CuO 4 single crystal based on 63Cu NMR techniques. We demonstrate that 63Cu NMR properties of the nuclear spin I z=–1/2 to +1/2 central transition below Tcharge exhibit unprecedentedly strong dependence on the measurement time scale set by the separation time τ between the 90° and 180° radio-frequency pulses; a new kind of anomalous, very broad winglike 63Cu NMR signals gradually emerge below Tcharge only for extremely short τ≲4μs, while the spectral weight I Normal of the normal NMR signals is progressively wiped out. The NMR linewidth and relaxation rates depend strongly on τ below Tcharge, and their enhancement in the charge ordered state indicates that charge order turns on strong but inhomogeneous growth of Cu spin-spin correlations.« less

Revisiting Cu 63 NMR evidence for charge order in superconducting La 1.885 Sr 0.115 CuO 4

DOE PAGES

Imai, T.; Takahashi, S. K.; Arsenault, A.; ...

2017-12-26

Here, the presence of charge and spin stripe order in the La 2CuO 4-based family of superconductors continues to lead to new insight on the unusual ground-state properties of high- T c cuprates. Soon after the discovery of charge stripe order at T charge≃65 K in Nd 3+ co-doped La 1.48Nd 0.4Sr 0.12CuO 4( Tc≃6 K), Hunt et al. demonstrated that La 1.48Nd 0.4Sr 0.12CuO 4 and superconducting La 2–xSr xCuO 4 with x~1/8( Tc≃30 K) share nearly identical NMR anomalies near Tcharge of the former. Their inevitable conclusion that La 1.885Sr 0.115CuO 4 also undergoes charge order at amore » comparable temperature became controversial, because diffraction measurements at the time were unable to detect Bragg peaks associated with charge order. Recent advances in x-ray diffraction techniques finally led to definitive confirmations of the charge order Bragg peaks in La 1.885Sr 0.115CuO 4 with an onset at as high as Tcharge≃80 K. Meanwhile, improved instrumental technology has enabled routine NMR measurements that were not feasible two decades ago. Motivated by these new developments, we revisit the charge order transition of a La 1.885Sr 0.115CuO 4 single crystal based on 63Cu NMR techniques. We demonstrate that 63Cu NMR properties of the nuclear spin I z=–1/2 to +1/2 central transition below Tcharge exhibit unprecedentedly strong dependence on the measurement time scale set by the separation time τ between the 90° and 180° radio-frequency pulses; a new kind of anomalous, very broad winglike 63Cu NMR signals gradually emerge below Tcharge only for extremely short τ≲4μs, while the spectral weight I Normal of the normal NMR signals is progressively wiped out. The NMR linewidth and relaxation rates depend strongly on τ below Tcharge, and their enhancement in the charge ordered state indicates that charge order turns on strong but inhomogeneous growth of Cu spin-spin correlations.« less

Revisiting 63Cu NMR evidence for charge order in superconducting La1.885Sr0.115CuO4

NASA Astrophysics Data System (ADS)

Imai, T.; Takahashi, S. K.; Arsenault, A.; Acton, A. W.; Lee, D.; He, W.; Lee, Y. S.; Fujita, M.

2017-12-01

The presence of charge and spin stripe order in the La2CuO4 -based family of superconductors continues to lead to new insight on the unusual ground-state properties of high-Tc cuprates. Soon after the discovery of charge stripe order at Tcharge≃65 K in Nd3 + co-doped La1.48Nd0.4Sr0.12CuO4 (Tc≃6 K) [Tranquada et al., Nature (London) 375, 561 (1995), 10.1038/375561a0], Hunt et al. demonstrated that La1.48Nd0.4Sr0.12CuO4 and superconducting La2 -xSrxCuO4 with x ˜1 /8 (Tc≃30 K) share nearly identical NMR anomalies near Tcharge of the former [Phys. Rev. Lett. 82, 4300 (1999), 10.1103/PhysRevLett.82.4300]. Their inevitable conclusion that La1.885Sr0.115CuO4 also undergoes charge order at a comparable temperature became controversial, because diffraction measurements at the time were unable to detect Bragg peaks associated with charge order. Recent advances in x-ray diffraction techniques finally led to definitive confirmations of the charge order Bragg peaks in La1.885Sr0.115CuO4 with an onset at as high as Tcharge≃80 K. Meanwhile, improved instrumental technology has enabled routine NMR measurements that were not feasible two decades ago. Motivated by these new developments, we revisit the charge order transition of a La1.885Sr0.115CuO4 single crystal based on 63Cu NMR techniques. We demonstrate that 63Cu NMR properties of the nuclear spin Iz=-1/2 to +1/2 central transition below Tcharge exhibit unprecedentedly strong dependence on the measurement time scale set by the separation time τ between the 90∘ and 180∘ radio-frequency pulses; a new kind of anomalous, very broad winglike 63Cu NMR signals gradually emerge below Tcharge only for extremely short τ ≲4 μ s , while the spectral weight INormal of the normal NMR signals is progressively wiped out. The NMR linewidth and relaxation rates depend strongly on τ below Tcharge, and their enhancement in the charge ordered state indicates that charge order turns on strong but inhomogeneous growth of Cu spin-spin correlations.

Impact of amorphization on the electronic properties of Zn-Ir-O systems.

PubMed

Muñoz Ramo, David; Bristowe, Paul D

2016-09-01

We analyze the geometry and electronic structure of a series of amorphous Zn-Ir-O systems using classical molecular dynamics followed by density functional theory taking into account two different charge states of Ir (+3 and  +4). The structures obtained consist of a matrix of interconnected metal-oxygen polyhedra, with Zn adopting preferentially a coordination of 4 and Ir a mixture of coordinations between 4 and 6 that depend on the charge state of Ir and its concentration. The amorphous phases display reduced band gaps compared to crystalline ZnIr2O4 and exhibit localized states near the band edges, which harm their transparency and hole mobility. Increasing amounts of Ir in the Ir(4+) phases decrease the band gap further while not altering it significantly in the Ir(3+) phases. The results are consistent with recent transmittance and resistivity measurements.

Hydration states of AFm cement phases

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

Baquerizo, Luis G., E-mail: luis.baquerizoibarra@holcim.com; Matschei, Thomas; Scrivener, Karen L.

2015-07-15

The AFm phase, one of the main products formed during the hydration of Portland and calcium aluminate cement based systems, belongs to the layered double hydrate (LDH) family having positively charged layers and water plus charge-balancing anions in the interlayer. It is known that these phases present different hydration states (i.e. varying water content) depending on the relative humidity (RH), temperature and anion type, which might be linked to volume changes (swelling and shrinkage). Unfortunately the stability conditions of these phases are insufficiently reported. This paper presents novel experimental results on the different hydration states of the most important AFmmore » phases: monocarboaluminate, hemicarboaluminate, strätlingite, hydroxy-AFm and monosulfoaluminate, and the thermodynamic properties associated with changes in their water content during absorption/desorption. This data opens the possibility to model the response of cementitious systems during drying and wetting and to engineer systems more resistant to harsh external conditions.« less

Charged dopants in neutral supercells through substitutional donor (acceptor): nitrogen donor charging of the nitrogen-vacancy center in diamond

NASA Astrophysics Data System (ADS)

Löfgren, Robin; Pawar, Ravinder; Öberg, Sven; Larsson, J. Andreas

2018-02-01

Charged defects are traditionally computed by adding (subtracting) electrons for negative (positive) impurities. When using periodic boundary conditions this results in artificially charged supercells that also require a compensating background charge of the opposite sign, which makes slab supercells problematic because of an arbitrary dependence on the vacuum thickness. In this work, we test the method of using neutral supercells through the use of a substitutional electron donor (acceptor) to describe charged systems. We use density functional theory (DFT) to compare the effects of charging the well-studied NV-center in diamond by a substitutional donor nitrogen. We investigate the influence of the donor-N on the NV-center properties as a function of the distance between them, and find that they converge toward those obtained when adding an electron. We analyze the spin density and conclude that the donor-N has a zero magnetic moment, and thus, will not be seen in electron spin resonance. We validate our DFT energies through comparison to GW simulations. Charging the NV-center with a substitutional donor-N enables accurate calculations of slabs, without the ambiguity of using charged supercells. Implantation of donor-N atoms opens up the possibility to engineer NV-centers with the desired charge state for future ICT and sensor applications.

The small impact of various partial charge distributions in ground and excited state on the computational Stokes shift of 1-methyl-6-oxyquinolinium betaine in diverse water models

NASA Astrophysics Data System (ADS)

Heid, Esther; Harringer, Sophia; Schröder, Christian

2016-10-01

The influence of the partial charge distribution obtained from quantum mechanics of the solute 1-methyl-6-oxyquinolinium betaine in the ground- and first excited state on the time-dependent Stokes shift is studied via molecular dynamics computer simulation. Furthermore, the effect of the employed solvent model — here the non-polarizable SPC, TIP4P and TIP4P/2005 and the polarizable SWM4 water model — on the solvation dynamics of the system is investigated. The use of different functionals and calculation methods influences the partial charge distribution and the magnitude of the dipole moment of the solute, but not the orientation of the dipole moment. Simulations based on the calculated charge distributions show nearly the same relaxation behavior. Approximating the whole solute molecule by a dipole results in the same relaxation behavior, but lower solvation energies, indicating that the time scale of the Stokes shift does not depend on peculiarities of the solute. However, the SPC and TIP4P water models show too fast dynamics which can be ascribed to a too large diffusion coefficient and too low viscosity. The calculated diffusion coefficient and viscosity for the SWM4 and TIP4P/2005 models coincide well with experimental values and the corresponding relaxation behavior is comparable to experimental values. Furthermore we found that for a quantitative description of the Stokes shift of the applied system at least two solvation shells around the solute have to be taken into account.

Origin of the different transport properties of electron and hole polarons in an ambipolar polyselenophene-based conjugated polymer

NASA Astrophysics Data System (ADS)

Chen, Zhuoying; Bird, Matthew; Lemaur, Vincent; Radtke, Guillaume; Cornil, Jérôme; Heeney, Martin; McCulloch, Iain; Sirringhaus, Henning

2011-09-01

Understanding the mechanisms limiting ambipolar transport in conjugated polymer field-effect transistors (FETs) is of both fundamental and practical interest. Here, we present a systematic study comparing hole and electron charge transport in an ambipolar conjugated polymer, semicrystalline poly(3,3''-di-n-decylterselenophene) (PSSS). Starting from a detailed analysis of the device characteristics and temperature/charge-density dependence of the mobility, we interpret the difference between hole and electron transport through both the Vissenberg-Matters and the mobility-edge model. To obtain microscopic insight into the quantum mechanical wave function of the charges at a molecular level, we combine charge modulation spectroscopy (CMS) measuring the charge-induced absorption signatures from positive and negative polarons in these ambipolar FETs with corresponding density functional theory (DFT) calculations. We observe a significantly higher switch-on voltage for electrons than for holes due to deep electron trap states, but also a higher activation energy of the mobility for mobile electrons. The CMS spectra reveal that the electrons that remain mobile and contribute to the FET current have a wave function that is more localized onto a single polymer chain than that of holes, which is extended over several polymer chains. We interpret this as evidence that the transport properties of the mobile electrons in PSSS are still affected by the presence of deep electron traps. The more localized electron state could be due to the mobile electrons interacting with shallow trap states in the vicinity of a chemical, potentially water-related, impurity that might precede the capture of the electron into a deeply trapped state.

ESI-MS of Cucurbituril Complexes Under Negative Polarity.

PubMed

Rodrigues, Maria A A; Mendes, Débora C; Ramamurthy, Vaidhyanathan; Da Silva, José P

2017-11-01

Electrospray ionization mass spectrometry (ESI-MS) is a powerful tool to study host-guest supramolecular interactions. ESI-MS can be used for detailed gas-phase reactivity studies, to clarify the structure, or simply to verify the formation of complexes. Depending on the structure of the host and of the guest, negative and/or positive ESI are used. Here we report the unexpected formation of host-guest complexes between cucurbit[n]urils (n = 7, 8, CB[n]) and amine, styryl pyridine, and styryl pyridine dimer cations, under negative ESI. Non-complexed CB[n] form double charged halide (Br - , Cl - , F - ) adducts. Under negative ESI, halide ions interact with CB[n] outer surface hydrogen atoms. One to one host-guest complexes (1:1) of CB[n] with positive charged guests were also observed as single and double charged ions under negative ESI. The positive charge of guests is neutralized by ion-pairing with halide anions. Depending on the number of positive charges guests retain in the gas phase, one or two additional halide ions are required for neutralization. Complexes 1:2 of CB[8] with styryl pyridines retain two halide ions in the gas phase, one per guest. Styryl pyridine dimers form 1:1 complexes possessing a single extra halide ion and therefore a single positive charge. Negative ESI is sensitive to small structural differences between complexes, distinguishing between 1:2 complexes of styryl pyridine-CB[8] and corresponding 1:1 complexes with the dimer. Negative ESI gives simpler spectra than positive ESI and allows the determination of guest charge state of CB[n] complexes in the gas phase. Graphical Abstract ᅟ.

Delocalization of charge and current in a chiral quasiparticle wave packet

NASA Astrophysics Data System (ADS)

Sarkar, Subhajit

2018-03-01

A chiral quasiparticle wave packet (c-QPWP) is defined as a conventional superposition of chiral quasiparticle states corresponding to an interacting electron system in two dimensions (2D) in the presence of Rashba spin-orbit coupling (RSOC). I investigate its internal structure via studying the charge and the current densities within the first-order perturbation in the electron-electron interaction. It is found that the c-QPWP contains a localized charge which is less than the magnitude of the bare charge and the remaining charge resides at the system boundary. The amount of charge delocalized turns out to be inversely proportional to the degenerate Fermi velocity v0(=√{α2+2 μ /m }) when RSOC (with strength α ) is weak, and therefore externally tunable. For strong RSOC, the magnitudes of both the delocalized charge and the current further strongly depend on the direction of propagation of the wave packet. Both the charge and the current densities consist of an anisotropic r-2 tail away from the center of the wave packet. Possible implications of such delocalizations in real systems corresponding to 2D semiconductor heterostructure are also discussed within the context of particle injection experiments.

High-Rate Charging Induced Intermediate Phases and Structural Changes of Layer-Structured Cathode for Lithium-Ion Batteries

DOE PAGES

Zhou, Yong-Ning; Yue, Ji-Li; Hu, Enyuan; ...

2016-08-08

Using fast time-resolved in situ X-ray diffraction, charge-rate dependent phase transition processes of layer structured cathode material LiNi 1/3Mn 1/3Co 1/3O 2 for lithium-ion batteries are studied. During first charge, intermediate phases emerge at high rates of 10C, 30C, and 60C, but not at low rates of 0.1C and 1C. These intermediate phases can be continuously observed during relaxation after the charging current is switched off. After half-way charging at high rate, sample studied by scanning transmission electron microscopy shows Li-rich and Li-poor phases' coexistence with tetrahedral occupation of Li in Li-poor phase. Also, the high rate induced overpotential ismore » thought to be the driving force for the formation of this intermediate Li-poor phase. The in situ quick X-ray absorption results show that the oxidation of Ni accelerates with increasing charging rate and the Ni 4+ state can be reached at the end of charge with 30C rate. Finally, these results give new insights in the understanding of the layered cathodes during high-rate charging.« less

Self-balancing feature of Lithium-Sulfur batteries

NASA Astrophysics Data System (ADS)

Knap, Vaclav; Stroe, Daniel-Ioan; Christensen, Andreas E.; Propp, Karsten; Fotouhi, Abbas; Auger, Daniel J.; Schaltz, Erik; Teodorescu, Remus

2017-12-01

The Li-S batteries are a prospective battery technology, which despite to its currently remaining drawbacks offers useable performance and interesting features. The polysulfide shuttle mechanism, a characteristic phenomenon for the Li-S batteries, causes a significant self-discharge at higher state-of-charge (SOC) levels, which leads to the energy dissipation of cells with higher charge. In an operation of series-connected Li-S cells, the shuttle mechanism results into a self-balancing effect which is studied here. A model for prediction of the self-balancing effect is proposed in this work and it is validated by experiments. Our results confirm the self-balancing feature of Li-S cells and illustrate their dependence on various conditions such as temperature, charging limits and idling time at high SOC.

Chandra Observations of the Solar System

NASA Astrophysics Data System (ADS)

Lisse, Carey

2014-11-01

Many solar system objects are now known to emit X-rays due to charge-exchange between highly charged solar wind (SW) minor ions and neutrals in their extended atmospheres, including Earth, Venus, Mars, Jupiter, and the heliosphere, with total power outputs on the MW - GW scale. (Currently only upper limits exist for Saturn and Pluto.) Chandra observations of their morphology, spectra, and time dependence provide important information about the neutral atmosphere structure and the SW flux and charge state. Chandra observations of solar x-ray scattering from Earth, Venus, Mars, Jupiter, Saturn, and the Moon have also provided important clues for the scattering material and the solar radiation field at the body. We present here a 15 year summary of Chandra's solar system observations.

Measurements of Ionospheric Density, Temperature, and Spacecraft Charging in a Space Weather Constellation

NASA Astrophysics Data System (ADS)

Balthazor, R. L.; McHarg, M. G.; Wilson, G.

2016-12-01

The Integrated Miniaturized Electrostatic Analyzer (IMESA) is a space weather sensor developed by the United States Air Force Academy and integrated and flown by the DoD's Space Test Program. IMESA records plasma spectrograms from which can be derived plasma density, temperature, and spacecraft frame charging. Results from IMESA currently orbiting on STPSat-3 are presented, showing frame charging effects dependent on a complex function of the number of solar panel cell strings switched in, solar panel current, and plasma density. IMESA will fly on four more satellites launching in the next two calendar years, enabling an undergraduate DoD space weather constellation in Low Earth Orbit that has the ability to significantly improve space weather forecasting capabilities using assimilative forecast models.

A long-range-corrected density functional that performs well for both ground-state properties and time-dependent density functional theory excitation energies, including charge-transfer excited states.

PubMed

Rohrdanz, Mary A; Martins, Katie M; Herbert, John M

2009-02-07

We introduce a hybrid density functional that asymptotically incorporates full Hartree-Fock exchange, based on the long-range-corrected exchange-hole model of Henderson et al. [J. Chem. Phys. 128, 194105 (2008)]. The performance of this functional, for ground-state properties and for vertical excitation energies within time-dependent density functional theory, is systematically evaluated, and optimal values are determined for the range-separation parameter, omega, and for the fraction of short-range Hartree-Fock exchange. We denote the new functional as LRC-omegaPBEh, since it reduces to the standard PBEh hybrid functional (also known as PBE0 or PBE1PBE) for a certain choice of its two parameters. Upon optimization of these parameters against a set of ground- and excited-state benchmarks, the LRC-omegaPBEh functional fulfills three important requirements: (i) It outperforms the PBEh hybrid functional for ground-state atomization energies and reaction barrier heights; (ii) it yields statistical errors comparable to PBEh for valence excitation energies in both small and medium-sized molecules; and (iii) its performance for charge-transfer excitations is comparable to its performance for valence excitations. LRC-omegaPBEh, with the parameters determined herein, is the first density functional that satisfies all three criteria. Notably, short-range Hartree-Fock exchange appears to be necessary in order to obtain accurate ground-state properties and vertical excitation energies using the same value of omega.

Dependence of mobility on shallow localized gap states in single-crystal organic field-effect-transistors

NASA Astrophysics Data System (ADS)

Butko, V. Y.; So, W.; Lang, D. V.; Chi, X.; Lashley, J. C.; Ramirez, A. P.

2009-12-01

In order to optimize the performance of molecular organic electronic devices it is important to study the intermolecular density of states and charge transport mechanisms in the environment of crystalline organic material. Using this approach in Field Effect Transistors (FETs) we show that material purification improves carrier mobility and decreases density of the deep localized electronic state. We also report a general exponential energy dependence of the density of localized states in a vicinity of the mobility edge (Fermi energies up to ∼7 times higher than the thermal energy (kT)) in a variety of the extensively purified molecular organic crystal FETs. This observation and the low activation energy of the order of ∼kT suggest that molecular structural misplacements of the sizes that are comparable with thermal molecular modes rather than impurity deep traps play a role in formation of these shallow states. We find that the charge carrier mobility in the FET nanochannels, μeff, is parameterized by two factors, the free-carrier mobility, μ0, and the ratio of the free carrier density to the total carrier density induced by gate bias. Crystalline FETs fabricated from rubrene, pentacene, and tetracene have a high free-carrier mobility, μ0∼50 cm2/Vs, at 300 K with lower device μeff dominated by localized shallow gap states. This relationship suggests that further improvements in electronic performance could be possible with enhanced device quality.

Resonant Coherent Excitation of Hydrogen-Like Ar Ions to the n =: 3 States

NASA Astrophysics Data System (ADS)

Azuma, T.; Ito, T.; Takabayashi, Y.; Komaki, K.; Yamazaki, Y.; Yamazaki, Y.; Takada, E.; Murakami, T.

We have succeeded in observing resonant coherent excitaion (RCE) of 1s electrons to the n = 3 states in 390 MeV/u hydrogen-like Ar17+ ions planar channeled in a silicon crystal through measurements of the charge-state distribution of ions transmitting the crystal. Furthermore, we directly confirmed RCE to the n = 3 states by observing the enhancement of the de-excitation X-rays, i.e., Kβ X-rays under the resonance condition. The resonance profiles of the charge-state distribution as functions of the incident angle to the crystal, which uniquely relates with the transition energy, have a characteristic structure consisting of several peaks. Compared with the profile of RCE to the n = 2 states, the present profiles show a large peak shift from the j = 1/2 and 3/2 levels in vacuum, and the profiles are much wider than those expected from the Stark-split level structure of the n = 3 manifolds due to the position- (distance from the channel center in the planar channel) dependent strong static field in the crystal.

Electromagnetic pulse-driven spin-dependent currents in semiconductor quantum rings.

PubMed

Zhu, Zhen-Gang; Berakdar, Jamal

2009-04-08

We investigate the non-equilibrium charge and spin-dependent currents in a quantum ring with a Rashba spin-orbit interaction (SOI) driven by two asymmetric picosecond electromagnetic pulses. The equilibrium persistent charge and persistent spin-dependent currents are investigated as well. It is shown that the dynamical charge and the dynamical spin-dependent currents vary smoothly with a static external magnetic flux and the SOI provides a SU(2) effective flux that changes the phases of the dynamic charge and the dynamic spin-dependent currents. The period of the oscillation of the total charge current with the delay time between the pulses is larger in a quantum ring with a larger radius. The parameters of the pulse fields control to a certain extent the total charge and the total spin-dependent currents. The calculations are applicable to nanometre rings fabricated in heterojunctions of III-V and II-VI semiconductors containing several hundreds of electrons.

Energy decomposition analysis for exciplexes using absolutely localized molecular orbitals

NASA Astrophysics Data System (ADS)

Ge, Qinghui; Mao, Yuezhi; Head-Gordon, Martin

2018-02-01

An energy decomposition analysis (EDA) scheme is developed for understanding the intermolecular interaction involving molecules in their excited states. The EDA utilizes absolutely localized molecular orbitals to define intermediate states and is compatible with excited state methods based on linear response theory such as configuration interaction singles and time-dependent density functional theory. The shift in excitation energy when an excited molecule interacts with the environment is decomposed into frozen, polarization, and charge transfer contributions, and the frozen term can be further separated into Pauli repulsion and electrostatics. These terms can be added to their counterparts obtained from the ground state EDA to form a decomposition of the total interaction energy. The EDA scheme is applied to study a variety of systems, including some model systems to demonstrate the correct behavior of all the proposed energy components as well as more realistic systems such as hydrogen-bonding complexes (e.g., formamide-water, pyridine/pyrimidine-water) and halide (F-, Cl-)-water clusters that involve charge-transfer-to-solvent excitations.

Ambipolar surface state thermoelectric power of topological insulator Bi2Se3.

PubMed

Kim, Dohun; Syers, Paul; Butch, Nicholas P; Paglione, Johnpierre; Fuhrer, Michael S

2014-01-01

We measure gate-tuned thermoelectric power of mechanically exfoliated Bi2Se3 thin films in the topological insulator regime. The sign of the thermoelectric power changes across the charge neutrality point as the majority carrier type switches from electron to hole, consistent with the ambipolar electric field effect observed in conductivity and Hall effect measurements. Near the charge neutrality point and at low temperatures, the gate-dependent thermoelectric power follows the semiclassical Mott relation using the expected surface state density of states but is larger than expected at high electron doping, possibly reflecting a large density of states in the bulk gap. The thermoelectric power factor shows significant enhancement near the electron-hole puddle carrier density ∼0.5 × 10(12) cm(-2) per surface at all temperatures. Together with the expected reduction of lattice thermal conductivity in low-dimensional structures, the results demonstrate that nanostructuring and Fermi level tuning of three-dimensional topological insulators can be promising routes to realize efficient thermoelectric devices.

Semiconducting molecular crystals: Bulk in-gap states modified by structural and chemical defects

NASA Astrophysics Data System (ADS)

Haas, S.; Krellner, C.; Goldmann, C.; Pernstich, K. P.; Gundlach, D. J.; Batlogg, B.

2007-03-01

Charge transport in organic molecular crystals is strongly influenced by the density of localized in-gap states (traps). Thus, a profound knowledge of the defect states' origin is essential. Temperature-dependent space-charge limited current (TD-SCLC) spectroscopy was used as a powerful tool to quantitatively study the density of states (DOS) in high-quality rubrene and pentacene single crystals. In particular, changes of the DOS due to intentionally induced chemical and structural defects were monitored. For instance, the controlled exposure of pentacene and rubrene to x-ray radiation results in a broad over-all increase of the DOS. Namely, the ionizing radiation induces a variety of both chemical and structural defects. On the other hand, exposure of rubrene to UV-excited oxygen is reflected in a sharp peak in the DOS, whereas in a similar experiment with pentacene oxygen acts as a dopant, and possible defects are metastable on the time-scale of the measurement, thus leaving the extracted DOS virtually unchanged.

Microfluidic circuit analysis II: implications of ion conservation for microchannels connected in series.

PubMed

Biscombe, Christian J C; Davidson, Malcolm R; Harvie, Dalton J E

2012-01-01

A mathematical framework for analysing electrokinetic flow in microchannel networks is outlined. The model is based on conservation of volume and total charge at network junctions, but in contrast to earlier theories also incorporates conservation of ion charge there. The model is applied to mixed pressure-driven/electro-osmotic flows of binary electrolytes through homogeneous microchannels as well as a 4:1:4 contraction-expansion series network. Under conditions of specified volumetric flow rate and ion currents, non-linear steady-state phenomena may arise: when the direction of the net co-ion flux is opposite to the direction of the net volumetric flow, two different fully developed, steady-state flow solutions may be obtained. Model predictions are compared with two-dimensional computational fluid dynamics (CFD) simulations. For systems where two steady states are realisable, the ultimate steady behaviour is shown to depend in part upon the initial state of the system. Copyright © 2011 Elsevier Inc. All rights reserved.

Entanglement evolution across a conformal interface

NASA Astrophysics Data System (ADS)

Wen, Xueda; Wang, Yuxuan; Ryu, Shinsei

2018-05-01

For two-dimensional conformal field theories (CFTs) in the ground state, it is known that a conformal interface along the entanglement cut can suppress the entanglement entropy from to , where L is the length of the subsystem A, and is the effective central charge which depends on the transmission property of the conformal interface. In this work, by making use of conformal mappings, we show that a conformal interface has the same effect on entanglement evolution in non-equilibrium cases, including global, local and certain inhomogeneous quantum quenches. I.e. a conformal interface suppresses the time evolution of entanglement entropy by effectively replacing the central charge c with , where is exactly the same as that in the ground state case. We confirm this conclusion by a numerical study on a critical fermion chain. Furthermore, based on the quasi-particle picture, we conjecture that this conclusion holds for an arbitrary quantum quench in CFTs, as long as the initial state can be described by a regularized conformal boundary state.

Combined effects of space charge and energetic disorder on photocurrent efficiency loss of field-dependent organic photovoltaic devices

NASA Astrophysics Data System (ADS)

Yoon, Sangcheol; Park, Byoungchoo; Hwang, Inchan

2015-11-01

The loss of photocurrent efficiency by space-charge effects in organic solar cells with energetic disorder was investigated to account for how energetic disorder incorporates space-charge effects, utilizing a drift-diffusion model with field-dependent charge-pair dissociation and suppressed bimolecular recombination. Energetic disorder, which induces the Poole-Frenkel behavior of charge carrier mobility, is known to decrease the mobility of charge carriers and thus reduces photovoltaic performance. We found that even if the mobilities are the same in the absence of space-charge effects, the degree of energetic disorder can be an additional parameter affecting photocurrent efficiency when space-charge effects occur. Introducing the field-dependence parameter that reflects the energetic disorder, the behavior of efficiency loss with energetic disorder can differ depending on which charge carrier is subject to energetic disorder. While the energetic disorder that is applied to higher-mobility charge carriers decreases photocurrent efficiency further, the efficiency loss can be suppressed when energetic disorder is applied to lower-mobility charge carriers.

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

Wang, Li-Fang; Ou, Chin-Ching; Striebel, Kathryn A.

The goal of this research was to measure Mn dissolution from a thin porous spinel LiMn{sub 2}O{sub 4} electrode by rotating ring-disk collection experiments. The amount of Mn dissolution from the spinel LiMn{sub 2}O{sub 4} electrode under various conditions was detected by potential step chronoamperometry. The concentration of dissolved Mn was found to increase with increasing cycle numbers and elevated temperature. The dissolved Mn was not dependent on disk rotation speed, which indicated that the Mn dissolution from the disk was under reaction control. The in situ monitoring of Mn dissolution from the spinel was carried out under various conditions.more » The ring currents exhibited maxima corresponding to the end-of-charge (EOC) and end-of-discharge (EOD), with the largest peak at EOC. The results suggest that the dissolution of Mn from spinel LiMn{sub 2}O{sub 4} occurs during charge/discharge cycling, especially in a charged state (at >4.1 V) and in a discharged state (at <3.1 V). The largest peak at EOC demonstrated that Mn dissolution took place mainly at the top of charge. At elevated temperatures, the ring cathodic currents were larger due to the increase of Mn dissolution rate.« less

Band-like temperature dependence of mobility in a solution-processed organic semiconductor

NASA Astrophysics Data System (ADS)

Sakanoue, Tomo; Sirringhaus, Henning

2010-09-01

The mobility μ of solution-processed organic semiconductorshas improved markedly to room-temperature values of 1-5cm2V-1s-1. In spite of their growing technological importance, the fundamental open question remains whether charges are localized onto individual molecules or exhibit extended-state band conduction like those in inorganic semiconductors. The high bulk mobility of 100cm2V-1s-1 at 10K of some molecular single crystals provides clear evidence that extended-state conduction is possible in van-der-Waals-bonded solids at low temperatures. However, the nature of conduction at room temperature with mobilities close to the Ioffe-Regel limit remains controversial. Here we investigate the origin of an apparent `band-like', negative temperature coefficient of the mobility (dμ/dT<0) in spin-coated films of 6,13-bis(triisopropylsilylethynyl)-pentacene. We use optical spectroscopy of gate-induced charge carriers to show that, at low temperature and small lateral electric field, charges become localized onto individual molecules in shallow trap states, but that a moderate lateral electric field is able to detrap them resulting in highly nonlinear, low-temperature transport. The negative temperature coefficient of the mobility at high fields is not due to extended-state conduction but to localized transport limited by thermal lattice fluctuations.

Band-like temperature dependence of mobility in a solution-processed organic semiconductor.

PubMed

Sakanoue, Tomo; Sirringhaus, Henning

2010-09-01

The mobility mu of solution-processed organic semiconductors has improved markedly to room-temperature values of 1-5 cm(2) V(-1) s(-1). In spite of their growing technological importance, the fundamental open question remains whether charges are localized onto individual molecules or exhibit extended-state band conduction like those in inorganic semiconductors. The high bulk mobility of 100 cm(2) V(-1) s(-1) at 10 K of some molecular single crystals provides clear evidence that extended-state conduction is possible in van-der-Waals-bonded solids at low temperatures. However, the nature of conduction at room temperature with mobilities close to the Ioffe-Regel limit remains controversial. Here we investigate the origin of an apparent 'band-like', negative temperature coefficient of the mobility (dmu/dT<0) in spin-coated films of 6,13-bis(triisopropylsilylethynyl)-pentacene. We use optical spectroscopy of gate-induced charge carriers to show that, at low temperature and small lateral electric field, charges become localized onto individual molecules in shallow trap states, but that a moderate lateral electric field is able to detrap them resulting in highly nonlinear, low-temperature transport. The negative temperature coefficient of the mobility at high fields is not due to extended-state conduction but to localized transport limited by thermal lattice fluctuations.

Spontaneous Charge Separation and Sublimation Processes are Ubiquitous in Nature and in Ionization Processes in Mass Spectrometry

NASA Astrophysics Data System (ADS)

Trimpin, Sarah; Lu, I.-Chung; Rauschenbach, Stephan; Hoang, Khoa; Wang, Beixi; Chubatyi, Nicholas D.; Zhang, Wen-Jing; Inutan, Ellen D.; Pophristic, Milan; Sidorenko, Alexander; McEwen, Charles N.

2018-02-01

Ionization processes have been discovered by which small and large as well as volatile and nonvolatile compounds are converted to gas-phase ions when associated with a matrix and exposed to sub-atmospheric pressure. Here, we discuss experiments further defining these simple and unexpected processes. Charge separation is found to be a common process for small molecule chemicals, solids and liquids, passed through an inlet tube from a higher to a lower pressure region, with and without heat applied. This charge separation process produces positively- and negatively-charged particles with widely different efficiencies depending on the compound and its physical state. Circumstantial evidence is presented suggesting that in the new ionization process, charged particles carry analyte into the gas phase, and desolvation of these particles produce the bare ions similar to electrospray ionization, except that solid particles appear likely to be involved. This mechanistic proposition is in agreement with previous theoretical work related to ion emission from ice.

Charge Carrier Dynamics in Cs2AgBiBr6 Double Perovskite

PubMed Central

2018-01-01

Double perovskites, comprising two different cations, are potential nontoxic alternatives to lead halide perovskites. Here, we characterized thin films and crystals of Cs2AgBiBr6 by time-resolved microwave conductance (TRMC), which probes formation and decay of mobile charges upon pulsed irradiation. Optical excitation of films results in the formation of charges with a yield times mobility product, φΣμ > 1 cm2/Vs. On excitation of millimeter-sized crystals, the TRMC signals show, apart from a fast decay, a long-lived tail. Interestingly, this tail is dominant when exciting close to the bandgap, implying the presence of mobile charges with microsecond lifetimes. From the temperature and intensity dependence of the TRMC signals, we deduce a shallow trap state density of around 1016/cm3 in the bulk of the crystal. Despite this high concentration, trap-assisted recombination of charges in the bulk appears to be slow, which is promising for photovoltaic applications. PMID:29545908

Ferromagnetism in ferroelectric BaTiO3 induced by vacancies: Sensitive dependence on charge state, origin of magnetism, and temperature range of existence

NASA Astrophysics Data System (ADS)

Raeliarijaona, Aldo; Fu, Huaxiang

2017-10-01

Using density-functional calculations we investigate the possibility and underlying mechanism of generating ferromagnetism (FM) in ferroelectric BaTiO3 by native vacancies. For the same vacancy species but different charge states (e.g., VO0 vs VO2 +), our paper reveals a marked difference in magnetic behaviors. For instance, while VO0 is ferromagnetic, VO2 + is not. This sensitive dependence, which has often been overlooked, highlights the critical importance of taking into account different charge states. Furthermore, while oxygen vacancies have been often used in experiments to explain the vacancy-induced FM, our calculation demonstrates that Ti vacancies, in particular VTi3 - and VTi2 - with low formation energies, generate even stronger ferromagnetism in BaTiO3, with a magnetic moment which is 400% larger than that of VO0. Interestingly, this strong FM of VTi can be further enhanced by hole doping. Although both cation vacancies (VTiq) and anion vacancies (VO0) induce FM, their mechanisms differ drastically. FM of anion vacancies originates from the spin-polarized electrons at Ti sites, but FM of cation vacancies stems from the spin-polarized holes at O sites. This paper also sheds light on vacancy-induced FM by discovering that the spin densities of all three considered vacancy species are highly extended in real space, distributed far away from the vacancy. Moreover, we predict that the ferromagnetism caused by VTi3 - is able to survive at high temperatures, which is promising for room-temperature spintronic or multiferroic applications.

SERS of semiconducting nanoparticles (TiO{sub 2} hybrid composites).

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

Musumeci, A.; Gosztola, D.; Schiller, T.

Raman scattering of molecules adsorbed on the surface of TiO{sub 2} nanoparticles was investigated. We find strong enhancement of Raman scattering in hybrid composites that exhibit charge transfer absorption with TiO{sub 2} nanoparticles. An enhancement factor up to {approx}10{sup 3} was observed in the solutions containing TiO{sub 2} nanoparticles and biomolecules, including the important class of neurotransmitters such as dopamine and dopac (3,4-dihydroxy-phenylacetic acid). Only selected vibrations are enhanced, indicating molecular specificity due to distinct binding and orientation of the biomolecules coupled to the TiO{sub 2} surface. All enhanced modes are associated with the asymmetric vibrations of attached molecules thatmore » lower the symmetry of the charge transfer complex. The intensity and the energy of selected vibrations are dependent on the size and shape of nanoparticle support. Moreover, we show that localization of the charge in quantized nanoparticles (2 nm), demonstrated as the blue shift of particle absorption, diminishes SERS enhancement. Importantly, the smallest concentration of adsorbed molecules shows the largest Raman enhancements suggesting the possibility for high sensitivity of this system in the detection of biomolecules that form a charge transfer complex with metal oxide nanoparticles. The wavelength-dependent properties of a hybrid composite suggest a Raman resonant state. Adsorbed molecules that do not show a charge transfer complex show weak enhancements probably due to the dielectric cavity effect.« less

SERS of semiconducting nanoparticles (TIO{sub 2} hybrid composites).

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

Rajh, T.; Musumeci, A.; Gosztola, D.

Raman scattering of molecules adsorbed on the surface of TiO{sub 2} nanoparticles was investigated. We find strong enhancement of Raman scattering in hybrid composites that exhibit charge transfer absorption with TiO{sub 2} nanoparticles. An enhancement factor up to {approx}10{sup 3} was observed in the solutions containing TiO{sub 2} nanoparticles and biomolecules, including the important class of neurotransmitters such as dopamine and dopac (3,4-dihydroxy-phenylacetic acid). Only selected vibrations are enhanced, indicating molecular specificity due to distinct binding and orientation of the biomolecules coupled to the TiO{sub 2} surface. All enhanced modes are associated with the asymmetric vibrations of attached molecules thatmore » lower the symmetry of the charge transfer complex. The intensity and the energy of selected vibrations are dependent on the size and shape of nanoparticle support. Moreover, we show that localization of the charge in quantized nanoparticles (2 nm), demonstrated as the blue shift of particle absorption, diminishes SERS enhancement. Importantly, the smallest concentration of adsorbed molecules shows the largest Raman enhancements suggesting the possibility for high sensitivity of this system in the detection of biomolecules that form a charge transfer complex with metal oxide nanoparticles. The wavelength-dependent properties of a hybrid composite suggest a Raman resonant state. Adsorbed molecules that do not show a charge transfer complex show weak enhancements probably due to the dielectric cavity effect.« less

STM studies of an atomic-scale gate electrode formed by a single charged vacancy in GaAs

NASA Astrophysics Data System (ADS)

Lee, Donghun; Daughton, David; Gupta, Jay

2009-03-01

Electric-field control of spin-spin interactions at the atomic level is desirable for the realization of spintronics and spin-based quantum computation. Here we demonstrate the realization of an atomic-scale gate electrode formed by a single charged vacancy on the GaAs(110) surface[1]. We can position these vacancies with atomic precision using the tip of a home-built, low temperature STM. Tunneling spectroscopy of single Mn acceptors is used to quantify the electrostatic field as a function of distance from the vacancy. Single Mn acceptors are formed by substituting Mn adatoms for Ga atoms in the first layer of the p-GaAs(110) surface[2]. Depending on the distance, the in-gap resonance of single Mn acceptors can shift as much as 200meV. Our data indicate that the electrostatic field decays according to a screened Coulomb potential. The charge state of the vacancy can be switched to neutral, as evidenced by the Mn resonance returning to its unperturbed position. Reversible control of the local electric field as well as charged states of defects in semiconductors can open new insights such as realizing an atomic-scale gate control and studying spin-spin interactions in semiconductors. http://www.physics.ohio-state.edu/sim jgupta [1] D. Lee and J.A. Gupta (in preparation) [2] D. Kitchen et al., Nature 442, 436-439 (2006)

The composition of liquid atmospheric pressure matrix-assisted laser desorption/ionization matrices and its effect on ionization in mass spectrometry.

PubMed

Ryumin, Pavel; Cramer, Rainer

2018-07-12

New liquid atmospheric pressure (AP) matrix-assisted laser desorption/ionization (MALDI) matrices that produce predominantly multiply charged ions have been developed and evaluated with respect to their performance for peptide and protein analysis by mass spectrometry (MS). Both the chromophore and the viscous support liquid in these matrices were optimized for highest MS signal intensity, S/N values and maximum charge state. The best performance in both protein and peptide analysis was achieved employing light diols as matrix support liquids (e.g. ethylene glycol and propylene glycol). Investigating the influence of the chromophore, it was found that 2,5-dihydroxybenzoic acid resulted in a higher analyte ion signal intensity for the analysis of small peptides; however, larger molecules (>17 kDa) were undetectable. For larger molecules, a sample preparation based on α-cyano-4-hydroxycinnammic acid as the chromophore was developed and multiply protonated analytes with charge states of more than 50 were detected. Thus, for the first time it was possible to detect with MALDI MS proteins as large as ∼80 kDa with a high number of charge states, i.e. m/z values below 2000. Systematic investigations of various matrix support liquids have revealed a linear dependency between laser threshold energy and surface tension of the liquid MALDI sample. Copyright © 2018 Elsevier B.V. All rights reserved.

COMPARATIVE ASSESSMENT OF THE COMPOSITION AND CHARGE STATE OF NITROGENASE FeMo-COFACTOR

PubMed Central

Harris, Travis V.; Szilagyi, Robert K.

2011-01-01

A significant limitation in our understanding of the molecular mechanism of biological nitrogen fixation is the uncertain composition of the FeMo-cofactor (FeMo-co) of nitrogenase. In this study we present a systematic, density functional theory-based evaluation of spin coupling schemes, iron oxidation states, ligand protonation states, and interstitial ligand composition using a wide range of experimental criteria. The employed functionals and basis sets were validated with molecular orbital information from X-ray absorption spectroscopic data of relevant iron-sulfur clusters. Independently from the employed level of theory, the electronic structure with the greatest number of antiferromagnetic interactions corresponds to the lowest energy state for a given charge and oxidation state distribution of the iron ions. The relative spin state energies of resting and oxidized FeMo-co already allowed the exclusion of certain iron oxidation state distributions and interstitial ligand compositions. Geometry optimized FeMo-co structures of several models further eliminated additional states and compositions, while reduction potentials indicated a strong preference for the most likely charge state of FeMo-co. Mössbauer and ENDOR parameter calculations were found to be remarkably dependent on the employed training set, density functional and basis set. Overall, we found that a more oxidized [MoIV-2FeII-5FeIII-9S2−-C4−] composition with a hydroxyl-protonated homocitrate ligand satisfies all of the available experimental criteria, and is thus favored over the currently preferred composition of [MoIV-4FeII-3FeIII-9S2−-N3−] from the literature. PMID:21545160

Effect of a spacer on localization of topological states in a Bragg multihelicoidal fiber with a twist defect

NASA Astrophysics Data System (ADS)

Alexeyev, C. N.; Lapin, B. P.; Yavorsky, M. A.

2018-01-01

We have studied the influence of a spacer introduced into a Bragg multihelicoidal fiber with a twist defect on the existence of defect-localized states. We have shown that in the presence of a Gaussian pump the energy of the electromagnetic field stored in topologically charged defect-localized modes essentially depends on the length of the spacer. We have demonstrated that by changing this length on the wavelength scale it is possible to strongly modulate such energy. This property can be used for generation and controlled emission of topologically charged light. We have also shown that if the value of an isotropic spacer’s refractive index deviates from the optimal value defined by the parameters of the multihelicoidal fiber parts the effect of localization disappears.

Ionization states of helium in He-3-rich solar energetic particle events

NASA Technical Reports Server (NTRS)

Klecker, B.; Hovestadt, D.; Moebius, E.; Scholer, M.; Gloeckler, G.; Ipavich, F. M.

1983-01-01

Results of a systematic study of the ionic charge state of helium in the energy range 0.6-1.0 MeV/nucleon for He-3-rich solar energetic particle events during the time period August 1978 to October 1979 are reported. The data have been obtained with the Max-Planck-Institut/University of Maryland experiment on ISEE-3. Whereas for solar energetic particle events with no enrichment of He-3 relative to He-4 surprisingly large abundances of singly ionized helium have been reported recently, He-3-rich solar energetic particle events do not show significant abundances of He-3(+). This result is consistent with current theories explaining large compositional anomalies by mass per charge dependent selective heating of the minor ion species.

Highly Efficient Spin-to-Charge Current Conversion in Strained HgTe Surface States Protected by a HgCdTe Layer

NASA Astrophysics Data System (ADS)

Noel, P.; Thomas, C.; Fu, Y.; Vila, L.; Haas, B.; Jouneau, P.-H.; Gambarelli, S.; Meunier, T.; Ballet, P.; Attané, J. P.

2018-04-01

We report the observation of spin-to-charge current conversion in strained mercury telluride at room temperature, using spin pumping experiments. We show that a HgCdTe barrier can be used to protect the HgTe from direct contact with the ferromagnet, leading to very high conversion rates, with inverse Edelstein lengths up to 2.0 ±0.5 nm . The influence of the HgTe layer thickness on the conversion efficiency is found to differ strongly from what is expected in spin Hall effect systems. These measurements, associated with the temperature dependence of the resistivity, suggest that these high conversion rates are due to the spin momentum locking property of HgTe surface states.

Communication: modeling charge-sign asymmetric solvation free energies with nonlinear boundary conditions.

PubMed

Bardhan, Jaydeep P; Knepley, Matthew G

2014-10-07

We show that charge-sign-dependent asymmetric hydration can be modeled accurately using linear Poisson theory after replacing the standard electric-displacement boundary condition with a simple nonlinear boundary condition. Using a single multiplicative scaling factor to determine atomic radii from molecular dynamics Lennard-Jones parameters, the new model accurately reproduces MD free-energy calculations of hydration asymmetries for: (i) monatomic ions, (ii) titratable amino acids in both their protonated and unprotonated states, and (iii) the Mobley "bracelet" and "rod" test problems [D. L. Mobley, A. E. Barber II, C. J. Fennell, and K. A. Dill, "Charge asymmetries in hydration of polar solutes," J. Phys. Chem. B 112, 2405-2414 (2008)]. Remarkably, the model also justifies the use of linear response expressions for charging free energies. Our boundary-element method implementation demonstrates the ease with which other continuum-electrostatic solvers can be extended to include asymmetry.

Communication: Modeling charge-sign asymmetric solvation free energies with nonlinear boundary conditions

PubMed Central

Bardhan, Jaydeep P.; Knepley, Matthew G.

2014-01-01

We show that charge-sign-dependent asymmetric hydration can be modeled accurately using linear Poisson theory after replacing the standard electric-displacement boundary condition with a simple nonlinear boundary condition. Using a single multiplicative scaling factor to determine atomic radii from molecular dynamics Lennard-Jones parameters, the new model accurately reproduces MD free-energy calculations of hydration asymmetries for: (i) monatomic ions, (ii) titratable amino acids in both their protonated and unprotonated states, and (iii) the Mobley “bracelet” and “rod” test problems [D. L. Mobley, A. E. Barber II, C. J. Fennell, and K. A. Dill, “Charge asymmetries in hydration of polar solutes,” J. Phys. Chem. B 112, 2405–2414 (2008)]. Remarkably, the model also justifies the use of linear response expressions for charging free energies. Our boundary-element method implementation demonstrates the ease with which other continuum-electrostatic solvers can be extended to include asymmetry. PMID:25296776

Model Based Optimal Control, Estimation, and Validation of Lithium-Ion Batteries

NASA Astrophysics Data System (ADS)

Perez, Hector Eduardo

This dissertation focuses on developing and experimentally validating model based control techniques to enhance the operation of lithium ion batteries, safely. An overview of the contributions to address the challenges that arise are provided below. Chapter 1: This chapter provides an introduction to battery fundamentals, models, and control and estimation techniques. Additionally, it provides motivation for the contributions of this dissertation. Chapter 2: This chapter examines reference governor (RG) methods for satisfying state constraints in Li-ion batteries. Mathematically, these constraints are formulated from a first principles electrochemical model. Consequently, the constraints explicitly model specific degradation mechanisms, such as lithium plating, lithium depletion, and overheating. This contrasts with the present paradigm of limiting measured voltage, current, and/or temperature. The critical challenges, however, are that (i) the electrochemical states evolve according to a system of nonlinear partial differential equations, and (ii) the states are not physically measurable. Assuming available state and parameter estimates, this chapter develops RGs for electrochemical battery models. The results demonstrate how electrochemical model state information can be utilized to ensure safe operation, while simultaneously enhancing energy capacity, power, and charge speeds in Li-ion batteries. Chapter 3: Complex multi-partial differential equation (PDE) electrochemical battery models are characterized by parameters that are often difficult to measure or identify. This parametric uncertainty influences the state estimates of electrochemical model-based observers for applications such as state-of-charge (SOC) estimation. This chapter develops two sensitivity-based interval observers that map bounded parameter uncertainty to state estimation intervals, within the context of electrochemical PDE models and SOC estimation. Theoretically, this chapter extends the notion of interval observers to PDE models using a sensitivity-based approach. Practically, this chapter quantifies the sensitivity of battery state estimates to parameter variations, enabling robust battery management schemes. The effectiveness of the proposed sensitivity-based interval observers is verified via a numerical study for the range of uncertain parameters. Chapter 4: This chapter seeks to derive insight on battery charging control using electrochemistry models. Directly using full order complex multi-partial differential equation (PDE) electrochemical battery models is difficult and sometimes impossible to implement. This chapter develops an approach for obtaining optimal charge control schemes, while ensuring safety through constraint satisfaction. An optimal charge control problem is mathematically formulated via a coupled reduced order electrochemical-thermal model which conserves key electrochemical and thermal state information. The Legendre-Gauss-Radau (LGR) pseudo-spectral method with adaptive multi-mesh-interval collocation is employed to solve the resulting nonlinear multi-state optimal control problem. Minimum time charge protocols are analyzed in detail subject to solid and electrolyte phase concentration constraints, as well as temperature constraints. The optimization scheme is examined using different input current bounds, and an insight on battery design for fast charging is provided. Experimental results are provided to compare the tradeoffs between an electrochemical-thermal model based optimal charge protocol and a traditional charge protocol. Chapter 5: Fast and safe charging protocols are crucial for enhancing the practicality of batteries, especially for mobile applications such as smartphones and electric vehicles. This chapter proposes an innovative approach to devising optimally health-conscious fast-safe charge protocols. A multi-objective optimal control problem is mathematically formulated via a coupled electro-thermal-aging battery model, where electrical and aging sub-models depend upon the core temperature captured by a two-state thermal sub-model. The Legendre-Gauss-Radau (LGR) pseudo-spectral method with adaptive multi-mesh-interval collocation is employed to solve the resulting highly nonlinear six-state optimal control problem. Charge time and health degradation are therefore optimally traded off, subject to both electrical and thermal constraints. Minimum-time, minimum-aging, and balanced charge scenarios are examined in detail. Sensitivities to the upper voltage bound, ambient temperature, and cooling convection resistance are investigated as well. Experimental results are provided to compare the tradeoffs between a balanced and traditional charge protocol. Chapter 6: This chapter provides concluding remarks on the findings of this dissertation and a discussion of future work.

Unemployment Insurance Fund Insolvency and Debt in Michigan.

ERIC Educational Resources Information Center

Blaustein, Saul J.

Without changes in Michigan's unemployment insurance law, the state's unemployment insurance debt will probably reach $3.8 billion by the end of 1985. Currently, Michigan's employers pay unemployment insurance tax rates that vary from 1 to 9 percent, depending upon the amount of benefits charged against their accounts. Beginning with the federal…

Jurisdictional Control: The Regulation of Nurses' Aides.

ERIC Educational Resources Information Center

Reinhard, Susan C.

1988-01-01

The future of health care depends on a more unified nursing hierarchy. It makes sense to place the regulation of nurses' aides within the jurisdiction of the state nursing board, the agency charged with providing safe nursing care. Strengthening nursing's jurisdictional control will not only improve the quality of care, it will increase the…

Characterization and dynamic charge dependent modeling of conducting polymer trilayer bending

NASA Astrophysics Data System (ADS)

Farajollahi, Meisam; Sassani, Farrokh; Naserifar, Naser; Fannir, Adelyne; Plesse, Cédric; Nguyen, Giao T. M.; Vidal, Frédéric; Madden, John D. W.

2016-11-01

Trilayer bending actuators are charge driven devices that have the ability to function in air and provide large mechanical amplification. The electronic and mechanical properties of these actuators are known to be functions of their charge state making prediction of their responses more difficult when they operate over their full range of deformation. In this work, a combination of state space representation and a two-dimensional RC transmission line model are used to implement a nonlinear time variant model for conducting polymer-based trilayer actuators. Electrical conductivity and Young’s modulus of electromechanically active PEDOT conducting polymer containing films as a function of applied voltage were measured and incorporated into the model. A 16% drop in Young’s modulus and 24 times increase in conductivity are observed by oxidizing the PEDOT. A closed form formulation for radius of curvature of trilayer actuators considering asymmetric and location dependent Young’s modulus and conductivity in the conducting polymer layers is derived and implemented in the model. The nonlinear model shows the capability to predict the radius of curvature as a function of time and position with reasonable consistency (within 4%). The formulation is useful for general trilayer configurations to calculate the radius of curvature as a function of time. The proposed electrochemical modeling approach may also be useful for modeling energy storage devices.

Photoinduced charge separation in a colloidal system of exfoliated layered semiconductor controlled by coexisting aluminosilicate clay.

PubMed

Nakato, Teruyuki; Yamada, Yoshimi; Miyamoto, Nobuyoshi

2009-02-05

We investigated photoinduced charge separation occurring in a multicomponent colloidal system composed of oxide nanosheets of photocatalytically active niobate and photochemically inert clay and electron accepting methylviologen dications (MV2+). The inorganic nanosheets were obtained by exfoliation of layered hexaniobate and hectorite clay. The niobate and clay nanosheets were spatially separated in the colloidally dispersed state, and the MV2+ molecules were selectively adsorbed on the clay platelets. UV irradiation of the colloids led to electron transfer from the niobate nanosheets to the MV2+ molecules adsorbed on clay. The photoinduced electron transfer produced methylviologen radical cations (MV*+), which was characterized by high yield and long lifetime. The yield and stability of the MV*+ species were found to depend strongly on the clay content of the colloid: from a few mol % to approximately 70 mol % of the yield and several tens of minutes to more than 40 h of the lifetime. The contents of the niobate nanosheets and MV2+ molecules and the aging of the colloid also affected the photoinduced charge separation. In the absence of MV2+ molecules in the colloid, UV irradiation induced electron accumulation in the niobate nanosheets. The stability of the electron-accumulated state also depended on the clay content. The variation in the photochemical behavior is discussed in relation to the viscosity of the colloid.

Observations of Heavy Ions in the Magnetosphere

NASA Astrophysics Data System (ADS)

Kistler, L. M.

2017-12-01

There are two sources for the hot ions in the magnetosphere: the solar wind and the ionosphere. The solar wind is predominantly protons, with about 4% He++ and less than 1% other high charge state heavy ions. The ionospheric outflow is also predominantly H+, but can contain a significant fraction of heavy ions including O+, N+, He+, O++, and molecular ions (NO+, N2+, O2+). The ionospheric outflow composition varies significantly both with geomagnetic activity and with solar EUV. The variability in the contribution of the two sources, the variability in the ionospheric source itself, and the transport paths of the different species are all important in determining the ion composition at a given location in the magnetosphere. In addition to the source variations, loss processes within the magnetosphere can be mass dependent, changing the composition. In particular, charge exchange is strongly species dependent, and can lead to heavy ion dominance at some energies in the inner magnetosphere. In this talk we will review the current state of our understanding of the composition of the magnetosphere and the processes that determine it.

Generation Dependent Ultrafast Charge Separation and Recombination in a Pyrene-Viologen Family of Dendrons.

PubMed

Gong, Zheng; Bao, Jianhua; Nagai, Keiji; Iyoda, Tomokazu; Kawauchi, Takehiro; Piotrowiak, Piotr

2016-05-12

The ability of a dendritic network to intercept electrons and extend the lifetime of a short-lived photoinduced charge separated (CS) state was investigated in a homologous family of methyl viologen (MV(2+)) dendrons spanning four generations, G0 through G3. The CS state in the parent pyrene-methylene-viologen G0 system with a single acceptor exhibits an extremely short lifetime of τ = 0.72 ps. The expansion of the viologen network introduces slower components to the recombination kinetics by allowing the injected electron to migrate further away from the donor. The long-lived fraction of the population increases monotonically in the order G3 > G2 > G1 > G0, while the respective recombination rates decrease. In the highest generation of the dendron ∼14% of the CS state population experiences a 10-fold or greater lifetime extension. Long range tunneling across multiple viologen units and sequential site-to-site hopping both contribute to the overall effect. The large excess energy deposited in the apical viologen upon charge separation and the presence of an extended network of low lying π-orbitals likely facilitate shuttling the electron further down the dendron.

Anions in Electrothermal Supercharging of Proteins with Electrospray Ionization Follow a Reverse Hofmeister Series

PubMed Central

2015-01-01

The effects of different anions on the extent of electrothermal supercharging of proteins from aqueous ammonium and sodium salt solutions were investigated. Sulfate and hydrogen phosphate are the most effective anions at producing high charge state protein ions from buffered aqueous solution, whereas iodide and perchlorate are ineffective with electrothermal supercharging. The propensity for these anions to produce high charge state protein ions follows the following trend: sulfate > hydrogen phosphate > thiocyanate > bicarbonate > chloride > formate ≈ bromide > acetate > iodide > perchlorate. This trend correlates with the reverse Hofmeister series over a wide range of salt concentrations (1 mM to 2 M) and with several physical properties, including solvent surface tension, anion viscosity B-coefficient, and anion surface/bulk partitioning coefficient, all of which are related to the Hofmeister series. The effectiveness of electrothermal supercharging does not depend on bubble formation, either from thermal degradation of the buffer or from coalescence of dissolved gas. These results provide evidence that the effect of different ions in the formation of high charge state ions by electrothermal supercharging is largely a result of Hofmeister effects on protein stability leading to protein unfolding in the heated ESI droplet. PMID:24410546

Thermal dissociation of ions limits the degree of the gas-phase H/D exchange at the atmospheric pressure.

PubMed

Kostyukevich, Y; Kononikhin, A; Popov, I; Nikolaev, E

2017-04-01

We present the application of the extended desolvating capillaries for increasing the degree of the gas-phase hydrogen/deuterium exchange reaction at atmospheric pressure. The use of the extended capillaries results in the increase of the time that ions spend in the high pressure region, what leads to the significant improvement of the efficiency of the reaction. For the small protein ubiquitin, it was observed that for the same temperature, the number of exchanges increases with the decrease of the charge state so that the lowest charge state can exchange twice the number of hydrogen than the highest one. With the increase of the temperature, the difference decreases, and eventually, the number of exchanges equalizes for all charge states. The value of this temperature and the corresponding number of exchanges depend on the geometric parameters of the capillary. Further increase of the temperature leads to the thermal dissociation of the protein ion. The observed b/y fragments are identical to those produced by collision-induced dissociation performed in the ion trap. Copyright © 2017 John Wiley & Sons, Ltd. Copyright © 2017 John Wiley & Sons, Ltd.

Tunneling spectroscopy of close-spaced dangling-bond pairs in Si(001):H

PubMed Central

Engelund, Mads; Zuzak, Rafał; Godlewski, Szymon; Kolmer, Marek; Frederiksen, Thomas; García-Lekue, Aran; Sánchez-Portal, Daniel; Szymonski, Marek

2015-01-01

We present a combined experimental and theoretical study of the electronic properties of close-spaced dangling-bond (DB) pairs in a hydrogen-passivated Si(001):H p-doped surface. Two types of DB pairs are considered, called “cross” and “line” structures. Our scanning tunneling spectroscopy (STS) data show that, although the spectra taken over different DBs in each pair exhibit a remarkable resemblance, they appear shifted by a constant energy that depends on the DB-pair type. This spontaneous asymmetry persists after repeated STS measurements. By comparison with density functional theory (DFT) calculations, we demonstrate that the magnitude of this shift and the relative position of the STS peaks can be explained by distinct charge states for each DB in the pair. We also explain how the charge state is modified by the presence of the scanning tunneling microscopy (STM) tip and the applied bias. Our results indicate that, using the STM tip, it is possible to control the charge state of individual DBs in complex structures, even if they are in close proximity. This observation might have important consequences for the design of electronic circuits and logic gates based on DBs in passivated silicon surfaces. PMID:26404520

Secondary Electron Emission From Solar Cell Coverslides And Its Effect On Absolute Vehicle Charging

NASA Astrophysics Data System (ADS)

Ferguson, Dale C.

2011-10-01

It has often been stated that earthed conductive solar cell coverslides are the best way to prevent electrostatic discharges on space solar arrays in GEO. While it is true that such coverslides will prevent differential charging on the solar arrays, it will be shown through NASCAP- 2k simulations that the secondary electron emission of such coverslides is very important for absolute vehicle charging. In particular, carbon nanotube coatings, due to the extremely low secondary electron emission from carbon, may exacerbate absolute vehicle charging. However, if they are earthed, because of their conductivity they may minimize differential charging and the possibility of arcing elsewhere on the spacecraft. Such results may also be true for insulative coverslides if spacecraft thermal blankets are made of materials with high secondary electron emission. Finally, photoemission from coverslides is investigated, with regard to anti-reflection coatings. Surfaces which reflect UV can have low photoemission, while those that absorb may have higher photoemission rates. Thus, anti-reflection coatings may lead to higher absolute spacecraft charging rates. NASCAP-2k simulations will be used to investigate these dependences for realistic spacecraft.

Molecular layers of ZnPc and FePc on Au(111) surface: Charge transfer and chemical interaction

NASA Astrophysics Data System (ADS)

Ahmadi, Sareh; Shariati, M. Nina; Yu, Shun; Göthelid, Mats

2012-08-01

We have studied zinc phthalocyanine (ZnPc) and iron phthalocyanine (FePc) thick films and monolayers on Au(111) using photoelectron spectroscopy and x-ray absorption spectroscopy. Both molecules are adsorbed flat on the surface at monolayer. ZnPc keeps this orientation in all investigated coverages, whereas FePc molecules stand up in the thick film. The stronger inter-molecular interaction of FePc molecules leads to change of orientation, as well as higher conductivity in FePc layer in comparison with ZnPc, which is reflected in thickness-dependent differences in core-level shifts. Work function changes indicate that both molecules donate charge to Au; through the π-system. However, the Fe3d derived lowest unoccupied molecular orbital receives charge from the substrate when forming an interface state at the Fermi level. Thus, the central atom plays an important role in mediating the charge, but the charge transfer as a whole is a balance between the two different charge transfer channels; π-system and the central atom.

Probing and Exploiting the Interplay between Nuclear and Electronic Motion in Charge Transfer Processes.

PubMed

Delor, Milan; Sazanovich, Igor V; Towrie, Michael; Weinstein, Julia A

2015-04-21

The Born-Oppenheimer approximation refers to the assumption that the nuclear and electronic wave functions describing a molecular system evolve and can be determined independently. It is now well-known that this approximation often breaks down and that nuclear-electronic (vibronic) coupling contributes greatly to the ultrafast photophysics and photochemistry observed in many systems ranging from simple molecules to biological organisms. In order to probe vibronic coupling in a time-dependent manner, one must use spectroscopic tools capable of correlating the motions of electrons and nuclei on an ultrafast time scale. Recent developments in nonlinear multidimensional electronic and vibrational spectroscopies allow monitoring both electronic and structural factors with unprecedented time and spatial resolution. In this Account, we present recent studies from our group that make use of different variants of frequency-domain transient two-dimensional infrared (T-2DIR) spectroscopy, a pulse sequence combining electronic and vibrational excitations in the form of a UV-visible pump, a narrowband (12 cm(-1)) IR pump, and a broadband (400 cm(-1)) IR probe. In the first example, T-2DIR is used to directly compare vibrational dynamics in the ground and relaxed electronic excited states of Re(Cl)(CO)3(4,4'-diethylester-2,2'-bipyridine) and Ru(4,4'-diethylester-2,2'-bipyridine)2(NCS)2, prototypical charge transfer complexes used in photocatalytic CO2 reduction and electron injection in dye-sensitized solar cells. The experiments show that intramolecular vibrational redistribution (IVR) and vibrational energy transfer (VET) are up to an order of magnitude faster in the triplet charge transfer excited state than in the ground state. These results show the influence of electronic arrangement on vibrational coupling patterns, with direct implications for vibronic coupling mechanisms in charge transfer excited states. In the second example, we show unambiguously that electronic and vibrational movement are coupled in a donor-bridge-acceptor complex based on a Pt(II) trans-acetylide design motif. Time-resolved IR (TRIR) spectroscopy reveals that the rate of electron transfer (ET) is highly dependent on the amount of excess energy localized on the bridge following electronic excitation. Using an adaptation of T-2DIR, we are able to selectively perturb bridge-localized vibrational modes during charge separation, resulting in the donor-acceptor charge separation pathway being completely switched off, with all excess energy redirected toward the formation of a long-lived intraligand triplet state. A series of control experiments reveal that this effect is mode specific: it is only when the high-frequency bridging C≡C stretching mode is pumped that radical changes in photoproduct yields are observed. These experiments therefore suggest that one may perturb electronic movement by stimulating structural motion along the reaction coordinate using IR light. These studies add to a growing body of evidence suggesting that controlling the pathways and efficiency of charge transfer may be achieved through synthetic and perturbative approaches aiming to modulate vibronic coupling. Achieving such control would represent a breakthrough for charge transfer-based applications such as solar energy conversion and molecular electronics.

Electronic Absorption Spectra of Neutral Perylene (C20H12), Terrylene (C30H16), and Quaterrylene (C40H20) and their Positive and Negative Ions: Ne Matrix-Isolation Spectroscopy and Time Dependent Density Functional Theory Calculations

NASA Technical Reports Server (NTRS)

Halasinski, Thomas M.; Weisman, Jennifer L.; Lee, Timothy J.; Salama, Farid; Head-Gordon, Martin; Kwak, Dochan (Technical Monitor)

2002-01-01

We present a full experimental and theoretical study of an interesting series of polycyclic aromatic hydrocarbons, the oligorylenes. The absorption spectra of perylene, terrylene and quaterrylene in neutral, cationic and anionic charge states are obtained by matrix-isolation spectroscopy in Ne. The experimental spectra are dominated by a bright state that red shifts with growing molecular size. Excitation energies and state symmetry assignments are supported by calculations using time dependent density functional theory methods. These calculations also provide new insight into the observed trends in oscillator strength and excitation energy for the bright states: the oscillator strength per unit mass of carbon increases along the series.

State-Resolved Metal Nanoparticle Dynamics Viewed through the Combined Lenses of Ultrafast and Magneto-optical Spectroscopies.

PubMed

Zhao, Tian; Herbert, Patrick J; Zheng, Hongjun; Knappenberger, Kenneth L

2018-06-19

Electronic carrier dynamics play pivotal roles in the functional properties of nanomaterials. For colloidal metals, the mechanisms and influences of these dynamics are structure dependent. The coherent carrier dynamics of collective plasmon modes for nanoparticles (approximately 2 nm and larger) determine optical amplification factors that are important to applied spectroscopy techniques. In the nanocluster domain (sub-2 nm), carrier coupling to vibrational modes affects photoluminescence yields. The performance of photocatalytic materials featuring both nanoparticles and nanoclusters also depends on the relaxation dynamics of nonequilibrium charge carriers. The challenges for developing comprehensive descriptions of carrier dynamics spanning both domains are multifold. Plasmon coherences are short-lived, persisting for only tens of femtoseconds. Nanoclusters exhibit discrete carrier dynamics that can persist for microseconds in some cases. On this time scale, many state-dependent processes, including vibrational relaxation, charge transfer, and spin conversion, affect carrier dynamics in ways that are nonscalable but, rather, structure specific. Hence, state-resolved spectroscopy methods are needed for understanding carrier dynamics in the nanocluster domain. Based on these considerations, a detailed understanding of structure-dependent carrier dynamics across length scales requires an appropriate combination of spectroscopic methods. Plasmon mode-specific dynamics can be obtained through ultrafast correlated light and electron microscopy (UCLEM), which pairs interferometric nonlinear optical (INLO) with electron imaging methods. INLO yields nanostructure spectral resonance responses, which capture the system's homogeneous line width and coherence dynamics. State-resolved nanocluster dynamics can be obtained by pairing ultrafast with magnetic-optical spectroscopy methods. In particular, variable-temperature variable-field (VTVH) spectroscopies allow quantification of transient, excited states, providing quantification of important parameters such as spin and orbital angular momenta as well as the energy gaps that separate electronic fine structure states. Ultrafast two-dimensional electronic spectroscopy (2DES) can be used to understand how these details influence state-to-state carrier dynamics. In combination, VTVH and 2DES methods can provide chemists with detailed information regarding the structure-dependent and state-specific flow of energy through metal nanoclusters. In this Account, we highlight recent advances toward understanding structure-dependent carrier dynamics for metals spanning the sub-nanometer to tens of nanometers length scale. We demonstrate the use of UCLEM methods for arresting interband scattering effects. For sub-nanometer thiol-protected nanoclusters, we discuss the effectiveness of VTVH for distinguishing state-specific radiative recombination originating from a gold core versus organometallic protecting layers. This state specificity is refined further using femtosecond 2DES and two-color methods to isolate so-called superatom state dynamics and vibrationally mediated spin-conversion and emission processes. Finally, we discuss prospects for merging VTVH and 2DES methods into a single platform.

Constraining the magnitude of the Chiral Magnetic Effect with Event Shape Engineering in Pb–Pb collisions at s NN = 2.76  TeV

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

Acharya, S.; Adam, J.; Adamová, D.

In ultrarelativistic heavy-ion collisions, the event-by-event variation of the elliptic flow v 2 reflects fluctuations in the shape of the initial state of the system. This allows to select events with the same centrality but different initial geometry. This selection technique, Event Shape Engineering, has been used in the analysis of charge-dependent two- and three-particle correlations in Pb–Pb collisions atmore » $$\\sqrt{s}$$$_ {NN}$$=2.76 TeV. The two-particle correlator 〈cos⁡(φ α -φ β)〉 calculated for different combinations of charges α and β is almost independent of v 2 (for a given centrality), while the three-particle correlator 〈cos⁡(φ α +φ β -2Ψ 2)〉 scales almost linearly both with the event v 2 and charged-particle pseudorapidity density. The charge dependence of the three-particle correlator is often interpreted as evidence for the Chiral Magnetic Effect (CME), a parity violating effect of the strong interaction. However, its measured dependence on v 2 points to a large non-CME contribution to the correlator. Finally, comparing the results with Monte Carlo calculations including a magnetic field due to the spectators, the upper limit of the CME signal contribution to the three-particle correlator in the 10–50% centrality interval is found to be 26–33% at 95% confidence level.« less

Constraining the magnitude of the Chiral Magnetic Effect with Event Shape Engineering in Pb–Pb collisions at s NN = 2.76  TeV

DOE PAGES

Acharya, S.; Adam, J.; Adamová, D.; ...

2017-12-12

In ultrarelativistic heavy-ion collisions, the event-by-event variation of the elliptic flow v 2 reflects fluctuations in the shape of the initial state of the system. This allows to select events with the same centrality but different initial geometry. This selection technique, Event Shape Engineering, has been used in the analysis of charge-dependent two- and three-particle correlations in Pb–Pb collisions atmore » $$\\sqrt{s}$$$_ {NN}$$=2.76 TeV. The two-particle correlator 〈cos⁡(φ α -φ β)〉 calculated for different combinations of charges α and β is almost independent of v 2 (for a given centrality), while the three-particle correlator 〈cos⁡(φ α +φ β -2Ψ 2)〉 scales almost linearly both with the event v 2 and charged-particle pseudorapidity density. The charge dependence of the three-particle correlator is often interpreted as evidence for the Chiral Magnetic Effect (CME), a parity violating effect of the strong interaction. However, its measured dependence on v 2 points to a large non-CME contribution to the correlator. Finally, comparing the results with Monte Carlo calculations including a magnetic field due to the spectators, the upper limit of the CME signal contribution to the three-particle correlator in the 10–50% centrality interval is found to be 26–33% at 95% confidence level.« less

Sodium dopants in helium clusters: Structure, equilibrium and submersion kinetics

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

Calvo, F.

Alkali impurities bind to helium nanodroplets very differently depending on their size and charge state, large neutral or charged dopants being wetted by the droplet whereas small neutral impurities prefer to reside aside. Using various computational modeling tools such as quantum Monte Carlo and path-integral molecular dynamics simulations, we have revisited some aspects of the physical chemistry of helium droplets interacting with sodium impurities, including the onset of snowball formation in presence of many-body polarization forces, the transition from non-wetted to wetted behavior in larger sodium clusters, and the kinetics of submersion of small dopants after sudden ionization.

On the Violence of High Explosive Reactions

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

Tarver, C M; Chidester, S K

High explosive reactions can be caused by three general energy deposition processes: impact ignition by frictional and/or shear heating; bulk thermal heating; and shock compression. The violence of the subsequent reaction varies from benign slow combustion to catastrophic detonation of the entire charge. The degree of violence depends on many variables, including the rate of energy delivery, the physical and chemical properties of the explosive, and the strength of the confinement surrounding the explosive charge. The current state of experimental and computer modeling research on the violence of impact, thermal, and shock-induced reactions is reviewed.

Temperature Dependence of Magnetically Active Charge Excitations in Magnetite across the Verwey Transition

NASA Astrophysics Data System (ADS)

Taguchi, M.; Chainani, A.; Ueda, S.; Matsunami, M.; Ishida, Y.; Eguchi, R.; Tsuda, S.; Takata, Y.; Yabashi, M.; Tamasaku, K.; Nishino, Y.; Ishikawa, T.; Daimon, H.; Todo, S.; Tanaka, H.; Oura, M.; Senba, Y.; Ohashi, H.; Shin, S.

2015-12-01

We study the electronic structure of bulk single crystals and epitaxial films of Fe3 O4 . Fe 2 p core level spectra show clear differences between hard x-ray (HAX) and soft x-ray photoemission spectroscopy (PES). The bulk-sensitive spectra exhibit temperature (T ) dependence across the Verwey transition, which is missing in the surface-sensitive spectra. By using an extended impurity Anderson full-multiplet model—and in contrast to an earlier peak assignment—we show that the two distinct Fe species (A and B site) and the charge modulation at the B site are responsible for the newly found double peaks in the main peak above TV and its T -dependent evolution. The Fe 2 p HAXPES spectra show a clear magnetic circular dichroism (MCD) in the metallic phase of magnetized 100-nm-thick films. The model calculations also reproduce the MCD and identify the contributions from magnetically distinct A and B sites. Valence band HAXPES shows a finite density of states at EF for the polaronic half metal with a remnant order above TV and a clear gap formation below TV. The results indicate that the Verwey transition is driven by changes in the strongly correlated and magnetically active B -site electronic states, consistent with resistivity and optical spectra.

Supramolecular control of the spin-dependent dynamics of long-lived charge-separated states at the micellar interface as studied by magnetic field effect.

PubMed

Miura, Tomoaki

2013-05-30

Spin selectivity in long-lived charge separation at the micellar interface is studied using the magnetic field effect (MFE). An amphiphilic viologen is complexed with a nonionic surfactant to form a supramolecular acceptor cage, of which the size is controlled by the acceptor concentration, as confirmed by dynamic light scattering measurement. Photoinduced electron transfer (ET) from a guest polyaromatic molecule to the viologen moiety is observed spin-dependently with time-resolved fluorescence (trFL) and transient absorption (TA). A negative MFE on the radical yield is successfully observed, which indicates generation of singlet-born long-lived radical pair that is realized by supramolecular control of the donor-acceptor (D-A) distances. The dominance of the singlet-precursor MFE is sensitive to the acceptor concentration, which presumably affects the D-A distance as well as the cage size. However, theoretical analysis of the MFE gives large recombination rates of ca. 10(8) s(-1), which indicate the contribution of spin-allowed recombination of the pseudocontact radical pair generated by still active in-cage diffusion. Dependence of the viologen concentration and alkyl chain length on the recombination and escape dynamics is discussed in terms of precursor spin states and the microenvironments in the cage.

Comprehensive investigation of the excited-state dynamics of push-pull triphenylamine dyes as models for photonic applications.

PubMed

Ishow, Eléna; Clavier, Gilles; Miomandre, Fabien; Rebarz, Mateusz; Buntinx, Guy; Poizat, Olivier

2013-09-07

A series of emitting push-pull triarylamine derivatives, models of their widely used homologues in photonics and organic electronics, was investigated by steady-state and time-resolved spectroscopy. Their structural originality stems from the sole change of the electron-withdrawing substituent X (-H: 1, -CN: 2, -NO2: 3, -CHC(CN)2: 4), giving rise to efficient emission tuning from blue to red upon increasing the X electron-withdrawing character. All compounds are highly fluorescent in alkanes. The more polar compounds 2-4 undergo considerable Stokes shift and emission quenching in polar solvents. Femtosecond transient absorption data allowed us to identify the nature of the emissive state which varies as a function of the compound and surrounding polarity. A long-lived ππ* excited state with weak charge transfer character was found for 1. This excited state evolves into a long-lived ICT state with red-shifted emission for 2 in polar solvents. For 3 and 4, the ICT state is directly populated in all solvents. Long-lived and emissive in n-hexane, it relaxes in toluene to a new ICT' conformation with stronger charge transfer character and enhanced Stokes shift. In more polar THF, ethanol, and nitrile solvents, ICT relaxes to a dark excited state ICT'' with viscosity-dependent kinetics (<10 ps). The ICT'' state lifetime drops with increasing solvent polarity (150 ps for 3 in THF, 8.5 ps in butyronitrile, 1.9 ps in acetonitrile), denoting an efficient radiationless deactivation to the ground state (back charge transfer). This result reveals a very small S0-S1 energy gap at the relaxed ICT'' geometry, with a possible close-lying S0-S1 conical intersection, which suggests that the ICT → ICT'' process results from a structural change involving a large-amplitude molecular distortion. This fast structural change can account for the strong fluorescence quenching observed for 3 and 4 in polar solvents. Finally, the magnitude of intersystem crossing between the singlet and triplet excited states largely depends on the electron-deficient X unit and the solvent itself. These observations help one conclude on the prevailing role played by the electron-withdrawing groups and the surrounding polarity in the photophysical performances of triphenylamine derivatives, largely employed in numerous emissive solid-state devices.

Charge-transfer channel in quantum dot-graphene hybrid materials

NASA Astrophysics Data System (ADS)

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.

Hospitalisation charges for fibromyalgia in the United States, 1999-2007.

PubMed

Haviland, Mark G; Banta, Jim E; Przekop, Peter

2012-01-01

To estimate fibromyalgia (FM) hospitalisation costs (i.e. charges) for patients in the United States from 1999 to 2007; to determine factors associated with variation in costs of FM and non-FM hospitalisations; and to investigate hospital procedures associated with FM hospitalisations. Data were from the Nationwide Inpatient Sample, a large database of hospitalisations in the U.S. Over the study period, an estimated 63,772 patients - two-thirds women, one-third men - had been hospitalised for FM (FM criterion was the International Classification of Diseases, 9th Revision, Clinical Modification diagnosis code 729.1, Myositis and Myalgia, unspecified). Demographics and hospital characteristics were described with frequencies and mean inflation-adjusted charges. Two multivariable linear regressions (one for FM and a second for non-FM patients), with Consumer Price Index (CPI)-adjusted charges (hospital and related services category) in thousands of dollars as the dependent variable, were performed, excluding cases with masked or missing data. Procedures were categorised with a standard classification scheme. Survey-adjusted total CPI-adjusted charges over the study period were estimated to be approximately $1.0 billion. Hospital procedures and Charlson-Deyo Index (co-morbidity severity) scores were the strongest predictors of charges in bivariate and multivariate analyses (for both FM and non-FM patients). The majority of procedures for FM patients were related to musculoskeletal, gastrointestinal, or cardiovascular systems. Most FM patients, however, did not have any procedure or a life-threatening co-morbid illness. Over the nine-year period, hospital charges for FM were substantial. Studies of how to reduce or avoid these costs in the treatment of FM need to be undertaken.

Charge-transfer channel in quantum dot-graphene hybrid materials.

PubMed

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

2018-04-06

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 Cd 13 Se 13 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.

Point-Defect Nature of the Ultraviolet Absorption Band in AlN

NASA Astrophysics Data System (ADS)

Alden, D.; Harris, J. S.; Bryan, Z.; Baker, J. N.; Reddy, P.; Mita, S.; Callsen, G.; Hoffmann, A.; Irving, D. L.; Collazo, R.; Sitar, Z.

2018-05-01

We present an approach where point defects and defect complexes are identified using power-dependent photoluminescence excitation spectroscopy, impurity data from SIMS, and density-functional-theory (DFT)-based calculations accounting for the total charge balance in the crystal. Employing the capabilities of such an experimental computational approach, in this work, the ultraviolet-C absorption band at 4.7 eV, as well as the 2.7- and 3.9-eV luminescence bands in AlN single crystals grown via physical vapor transport (PVT) are studied in detail. Photoluminescence excitation spectroscopy measurements demonstrate the relationship between the defect luminescent bands centered at 3.9 and 2.7 eV to the commonly observed absorption band centered at 4.7 eV. Accordingly, the thermodynamic transition energy for the absorption band at 4.7 eV and the luminescence band at 3.9 eV is estimated at 4.2 eV, in agreement with the thermodynamic transition energy for the CN- point defect. Finally, the 2.7-eV PL band is the result of a donor-acceptor pair transition between the VN and CN point defects since nitrogen vacancies are predicted to be present in the crystal in concentrations similar to carbon-employing charge-balance-constrained DFT calculations. Power-dependent photoluminescence measurements reveal the presence of the deep donor state with a thermodynamic transition energy of 5.0 eV, which we hypothesize to be nitrogen vacancies in agreement with predictions based on theory. The charge state, concentration, and type of impurities in the crystal are calculated considering a fixed amount of impurities and using a DFT-based defect solver, which considers their respective formation energies and the total charge balance in the crystal. The presented results show that nitrogen vacancies are the most likely candidate for the deep donor state involved in the donor-acceptor pair transition with peak emission at 2.7 eV for the conditions relevant to PVT growth.

Coupled sensitizer-catalyst dyads: electron-transfer reactions in a perylene-polyoxometalate conjugate.

PubMed

Odobel, Fabrice; Séverac, Marjorie; Pellegrin, Yann; Blart, Errol; Fosse, Céline; Cannizzo, Caroline; Mayer, Cédric R; Elliott, Kristopher J; Harriman, Anthony

2009-01-01

Ultrafast discharge of a single-electron capacitor: A variety of intramolecular electron-transfer reactions are apparent for polyoxometalates functionalized with covalently attached perylene monoimide chromophores, but these are restricted to single-electron events. (et=electron transfer, cr=charge recombination, csr=charge-shift reaction, PER=perylene, POM=polyoxometalate).A new strategy is introduced that permits covalent attachment of an organic chromophore to a polyoxometalate (POM) cluster. Two examples are reported that differ according to the nature of the anchoring group and the flexibility of the linker. Both POMs are functionalized with perylene monoimide units, which function as photon collectors and form a relatively long-lived charge-transfer state under illumination. They are reduced to a stable pi-radical anion by electrolysis or to a protonated dianion under photolysis in the presence of aqueous triethanolamine. The presence of the POM opens up an intramolecular electron-transfer route by which the charge-transfer state reduces the POM. The rate of this process depends on the molecular conformation and appears to involve through-space interactions. Prior reduction of the POM leads to efficient fluorescence quenching, again due to intramolecular electron transfer. In most cases, it is difficult to resolve the electron-transfer products because of relatively fast reverse charge shift that occurs within a closed conformer. Although the POM can store multiple electrons, it has not proved possible to use these systems as molecular-scale capacitors because of efficient electron transfer from the one-electron-reduced POM to the excited singlet state of the perylene monoimide.

Ground-State Charge-Density Distribution in a Crystal of the Luminescent ortho-Phenylenediboronic Acid Complex with 8-Hydroxyquinoline.

PubMed

Jarzembska, Katarzyna N; Kamiński, Radosław; Durka, Krzysztof; Woźniak, Krzysztof

2018-05-10

This contribution is devoted to the first electron density studies of a luminescent oxyquinolinato boron complex in the solid state. ortho-Phenylenediboronic acid mixed with 8-hydroxyquinoline in dioxane forms high-quality single crystals via slow solvent evaporation, which allows successful high resolution data collection (sin θ/λ = 1.2 Å -1 ) and charge density distribution modeling. Particular attention has been paid to the boron-oxygen fragment connecting the two parts of the complex, and to the solvent species exhibiting anharmonic thermal motion. The experiment and theory compared rather well in terms of atomic charges and volumes, except for the boron centers. Boron atoms, as expected, constitute the most electron-deficient species in the complex molecule, whereas the neighboring oxygen and carbon atoms are the most significantly negatively charged ones. This part of the molecule appears to be very much involved in the charge transfer occurring between the acid fragment and oxyquinoline moiety leading to the observed fluorescence, as supported by the time-dependent density functional theory (TDDFT) results and the generated transition density maps. TDDFT calculations indicated that p-type atomic orbitals contributing to the HOMO-1, HOMO, and LUMO play the major role in the lowest energy transitions, and enabled further comparison with the charge density features, which is discussed in details. Furthermore, the results confirmed the known fact the Q ligand character is most important for the spectroscopic properties of this class of complexes.

Interplay between hopping and band transport in high-mobility disordered semiconductors at large carrier concentrations: The case of the amorphous oxide InGaZnO

NASA Astrophysics Data System (ADS)

Fishchuk, I. I.; Kadashchuk, A.; Bhoolokam, A.; de Jamblinne de Meux, A.; Pourtois, G.; Gavrilyuk, M. M.; Köhler, A.; Bässler, H.; Heremans, P.; Genoe, J.

2016-05-01

We suggest an analytic theory based on the effective medium approximation (EMA) which is able to describe charge-carrier transport in a disordered semiconductor with a significant degree of degeneration realized at high carrier concentrations, especially relevant in some thin-film transistors (TFTs), when the Fermi level is very close to the conduction-band edge. The EMA model is based on special averaging of the Fermi-Dirac carrier distributions using a suitably normalized cumulative density-of-state distribution that includes both delocalized states and the localized states. The principal advantage of the present model is its ability to describe universally effective drift and Hall mobility in heterogeneous materials as a function of disorder, temperature, and carrier concentration within the same theoretical formalism. It also bridges a gap between hopping and bandlike transport in an energetically heterogeneous system. The key assumption of the model is that the charge carriers move through delocalized states and that, in addition to the tail of the localized states, the disorder can give rise to spatial energy variation of the transport-band edge being described by a Gaussian distribution. It can explain a puzzling observation of activated and carrier-concentration-dependent Hall mobility in a disordered system featuring an ideal Hall effect. The present model has been successfully applied to describe experimental results on the charge transport measured in an amorphous oxide semiconductor, In-Ga-Zn-O (a-IGZO). In particular, the model reproduces well both the conventional Meyer-Neldel (MN) compensation behavior for the charge-carrier mobility and inverse-MN effect for the conductivity observed in the same a-IGZO TFT. The model was further supported by ab initio calculations revealing that the amorphization of IGZO gives rise to variation of the conduction-band edge rather than to the creation of localized states. The obtained changes agree with the one we used to describe the charge transport. We found that the band-edge variation dominates the charge transport in high-quality a-IGZO TFTs in the above-threshold voltage region, whereas the localized states need not to be invoked to account for the experimental results in this material.

Charge carrier localization effects on the quantum efficiency and operating temperature range of InAs{sub x}P{sub 1−x}/InP quantum well detectors

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

Vashisht, Geetanjali, E-mail: geetanjali@rrcat.gov.in; Dixit, V. K., E-mail: dixit@rrcat.gov.in; Porwal, S.

2016-03-07

The effect of charge carrier localization resulting in “S-shaped” temperature dependence of the photoluminescence peak energy of InAs{sub x}P{sub 1−x}/InP quantum wells (QWs) is distinctly revealed by the temperature dependent surface photo voltage (SPV) and photoconductivity (PC) processes. It is observed that the escape efficiency of carriers from QWs depends on the localization energy, where the carriers are unable to contribute in SPV/PC signal below a critical temperature. Below the critical temperature, carriers are strongly trapped in the localized states and are therefore unable to escape from the QW. Further, the critical temperature increases with the magnitude of localization energymore » of carriers. Carrier localization thus plays a pivotal role in defining the operating temperature range of InAs{sub x}P{sub 1−x}/InP QW detectors.« less

Charge and spin control of ultrafast electron and hole dynamics in single CdSe/ZnSe quantum dots

NASA Astrophysics Data System (ADS)

Hinz, C.; Gumbsheimer, P.; Traum, C.; Holtkemper, M.; Bauer, B.; Haase, J.; Mahapatra, S.; Frey, A.; Brunner, K.; Reiter, D. E.; Kuhn, T.; Seletskiy, D. V.; Leitenstorfer, A.

2018-01-01

We study the dynamics of photoexcited electrons and holes in single negatively charged CdSe/ZnSe quantum dots with two-color femtosecond pump-probe spectroscopy. An initial characterization of the energy level structure is performed at low temperatures and magnetic fields of up to 5 T. Emission and absorption resonances are assigned to specific transitions between few-fermion states by a theoretical model based on a configuration interaction approach. To analyze the dynamics of individual charge carriers, we initialize the quantum system into excited trion states with defined energy and spin. Subsequently, the time-dependent occupation of the trion ground state is monitored by spectrally resolved differential transmission measurements. We observe subpicosecond dynamics for a hole excited to the D shell. The energy dependence of this D -to-S shell intraband transition is investigated in quantum dots of varying size. Excitation of an electron-hole pair in the respective p shells leads to the formation of singlet and triplet spin configurations. Relaxation of the p -shell singlet is observed to occur on a time scale of a few picoseconds. Pumping of p -shell triplet transitions opens up two pathways with distinctly different scattering times. These processes are shown to be governed by the mixing of singlet and triplet states due to exchange interactions enabling simultaneous electron and hole spin flips. To isolate the relaxation channels, we align the spin of the residual electron by a magnetic field and employ laser pulses of defined helicity. This step provides ultrafast preparation of a fully inverted trion ground state of the quantum dot with near unity probability, enabling deterministic addition of a single photon to the probe pulse. Therefore our experiments represent a significant step towards using single quantum emitters with well-controled inversion to manipulate the photon statistics of ultrafast light pulses.

Electronic Properties of Suspended Few-Layer Graphene Membranes

NASA Astrophysics Data System (ADS)

Myhro, Kevin Scott

Graphene, the two-dimensional (2D) honeycomb lattice of sp2-hybrized carbon atoms, has emerged as a "wonder" material with unique properties, such as its linear energy dispersion with massless Dirac fermions, so-called half-integer quantum Hall (QH) effect, unparalleled tensile strength, and high optical transparency and thermal conductivity. Its few-layer counterparts have similar mechanical but remarkably different electrical properties, including layer- and stacking-dependent band structures, massive charge carriers, and energy gaps that may arise from single particle effect as well as electronic interactions. This dissertation reports my six year study of dual-gated suspended few-layer graphene (FLG) field effect transistor (FET) devices. In particular, we focus on their electronic transport properties at low temperature as a function of out-of-plane electric field E⊥ and interlayer potential U⊥, charge carrier density n, temperature T, and out-of-plane (B ⊥) and parallel (B∥) magnetic fields. A number of broken symmetry states in the absence and presence of external fields are observed in rhombohedral-stacked bilayer- (BLG), trilayer- (r-TLG), and tetralayer graphene (r-4LG). We also study the morphological deformation of suspended graphene membranes under electrostatic and thermal manipulation, which is relevant for analyzing low temperature transport data. In particular, in BLG, r-TLG and r-4LG, we observe intrinsic insulating states in the absence of external fields, with energy gaps of 2, 40, and 80 meV, respectively. We attribute this increasing gap size with number of layers N to enhanced electronic-interactions near the charge neutrality point, due to the layer-dependent energy dispersions kN in r-FLG, which give rise to increasingly diverging density of states and interaction strength with increasing N, at least up to four layers. Our observations of the spontaneous insulating state in r-FLG are consistent with a layer antiferromagnetic state with broken time reversal symmetry, where the top and bottom layers are oppositely spin polarized.

Ground water in Pavant Valley

USGS Publications Warehouse

Dennis, P. E.; Maxey, G.B.; Thomas, H.E.

1946-01-01

The users of wells for irrigation in Pavant Valley, particularly in the Flowell district, have long been cognizant of their utter dependency upon ground water for livelihood, and were among the first in the State to make an organized effort to conserve supplies by prevention of waste. Since passage of the State ground-water law in 1935, the State Engineer has not approved applications for new wells in the areas of most concentrated development, and has deferred adjudication of existing water rights until adequate data concerning the ground-water resources become available. The investigation of ground-water resources in Pavant Valley was suggested by the State Engineer and constitutes one of a series that are being made in the important groundwater basins of Utah by the Federal Geological Survey in cooperation with the State Engineer. The investigation was under the general supervision of Oscar E. Meinzer, geologist in charge of the ground-water division of the Federal Geological Survey. H. E. Thomas, in charge of groundwater investigations in Utah, returned from military service overseas in time to assist in the completion of the manuscript, and edited the report.

Dense simple plasmas as high-temperature liquid simple metals

NASA Technical Reports Server (NTRS)

Perrot, F.

1990-01-01

The thermodynamic properties of dense plasmas considered as high-temperature liquid metals are studied. An attempt is made to show that the neutral pseudoatom picture of liquid simple metals may be extended for describing plasmas in ranges of densities and temperatures where their electronic structure remains 'simple'. The primary features of the model when applied to plasmas include the temperature-dependent self-consistent calculation of the electron charge density and the determination of a density and temperature-dependent ionization state.

Multilevel non-volatile data storage utilizing common current hysteresis of networked single walled carbon nanotubes

NASA Astrophysics Data System (ADS)

Hwang, Ihn; Wang, Wei; Hwang, Sun Kak; Cho, Sung Hwan; Kim, Kang Lib; Jeong, Beomjin; Huh, June; Park, Cheolmin

2016-05-01

The characteristic source-drain current hysteresis frequently observed in field-effect transistors with networked single walled carbon-nanotube (NSWNT) channels is problematic for the reliable switching and sensing performance of devices. But the two distinct current states of the hysteresis curve at a zero gate voltage can be useful for memory applications. In this work, we demonstrate a novel non-volatile transistor memory with solution-processed NSWNTs which are suitable for multilevel data programming and reading. A polymer passivation layer with a small amount of water employed on the top of the NSWNT channel serves as an efficient gate voltage dependent charge trapping and de-trapping site. A systematic investigation evidences that the water mixed in a polymer passivation solution is critical for reliable non-volatile memory operation. The optimized device is air-stable and temperature-resistive up to 80 °C and exhibits excellent non-volatile memory performance with an on/off current ratio greater than 104, a switching time less than 100 ms, data retention longer than 4000 s, and write/read endurance over 100 cycles. Furthermore, the gate voltage dependent charge injection mediated by water in the passivation layer allowed for multilevel operation of our memory in which 4 distinct current states were programmed repetitively and preserved over a long time period.The characteristic source-drain current hysteresis frequently observed in field-effect transistors with networked single walled carbon-nanotube (NSWNT) channels is problematic for the reliable switching and sensing performance of devices. But the two distinct current states of the hysteresis curve at a zero gate voltage can be useful for memory applications. In this work, we demonstrate a novel non-volatile transistor memory with solution-processed NSWNTs which are suitable for multilevel data programming and reading. A polymer passivation layer with a small amount of water employed on the top of the NSWNT channel serves as an efficient gate voltage dependent charge trapping and de-trapping site. A systematic investigation evidences that the water mixed in a polymer passivation solution is critical for reliable non-volatile memory operation. The optimized device is air-stable and temperature-resistive up to 80 °C and exhibits excellent non-volatile memory performance with an on/off current ratio greater than 104, a switching time less than 100 ms, data retention longer than 4000 s, and write/read endurance over 100 cycles. Furthermore, the gate voltage dependent charge injection mediated by water in the passivation layer allowed for multilevel operation of our memory in which 4 distinct current states were programmed repetitively and preserved over a long time period. Electronic supplementary information (ESI) available. See DOI: 10.1039/c6nr00505e

A study of the energy dependence of the underlying event in proton-antiproton collisions

DOE PAGES

Aaltonen, T.

2015-11-23

We study charged particle production (p T > 0.5 GeV/c, |η| < 0.8) in proton-antiproton collisions at 300 GeV, 900 GeV, and 1.96 TeV. We use the direction of the charged particle with the largest transverse momentum in each event to define three regions of η-Φspace; “toward”, “away”, and “transverse”. Furthermore, the average number and the average scalar p T sum of charged particles in the transverse region are sensitive to the modeling of the “underlying event”. The transverse region is divided into a MAX and MIN transverse region, which helps separate the “hard component” (initial and final-state radiation) frommore » the “beam-beam remnant” and multiple parton interaction components of the scattering. We found that the center-of-mass energy dependence of the various components of the event are studied in detail. The data presented here can be used to constrain and improve QCD Monte Carlo models, resulting in more precise predictions at the LHC energies of 13 and 14 TeV.« less

Quasi-Particle Relaxation and Quantum Femtosecond Magnetism in Non-Equilibrium Phases of Insulating Manganites

NASA Astrophysics Data System (ADS)

Perakis, Ilias; Kapetanakis, Myron; Lingos, Panagiotis; Barmparis, George; Patz, A.; Li, T.; Wang, Jigang

We study the role of spin quantum fluctuations driven by photoelectrons during 100fs photo-excitation of colossal magneto-resistive manganites in anti-ferromagnetic (AFM) charge-ordered insulating states with Jahn-Teller distortions. Our mean-field calculation of composite fermion excitations demonstrates that spin fluctuations reduce the energy gap by quasi-instantaneously deforming the AFM background, thus opening a conductive electronic pathway via FM correlation. We obtain two quasi-particle bands with distinct spin-charge dynamics and dependence on lattice distortions. To connect with fs-resolved spectroscopy experiments, we note the emergence of fs magnetization in the low-temperature magneto-optical signal, with threshold dependence on laser intensity characteristic of a photo-induced phase transition. Simultaneously, the differential reflectivity shows bi-exponential relaxation, with fs component, small at low intensity, exceeding ps component above threshold for fs AFM-to-FM switching. This suggests the emergence of a non-equilibrium metallic FM phase prior to establishment of a new lattice structure, linked with quantum magnetism via spin/charge/lattice couplings for weak magnetic fields.

Steric hindrance inhibits excited-state relaxation and lowers the extent of intramolecular charge transfer in two-photon absorbing dyes.

PubMed

Stewart, David J; Dalton, Matthew J; Long, Stephanie L; Kannan, Ramamurthi; Yu, Zhenning; Cooper, Thomas M; Haley, Joy E; Tan, Loon-Seng

2016-02-21

The two-photon absorbing dye AF240 [1, (7-benzothiazol-2-yl-9,9-diethylfluoren-2-yl)diphenylamine] is modified by adding bulky alkyl groups to the diphenylamino moiety. Three new compounds are synthesized which have ethyl groups in both ortho positions of each phenyl ring (2), t-butyl groups in one ortho position of each phenyl ring (3), and t-butyl groups in the para position of each phenyl ring (4). The dyes are examined in several aprotic solvents with varying polarity to observe the effects of the sterically hindering bulky groups on the ground and excited-state photophysical properties. While the ground state shows minimal solvent dependence, there is significant dependence on the fluorescence quantum yield and lifetime, as well as the excited-state energy levels. This effect is caused by the formation of an intramolecular charge-transfer (ICT) state, which is observed in the solvents more polar than n-hexane and supported by TD-DFT calculations. Electronic effects of ortho or para alkyl substitution should be similar, yet drastic differences are observed. A red shift in the fluorescence maximum is observed in 4 relative to 1, yet a blue shift occurs in 2 and 3 because the substituents at the sterically sensitive ortho-positions inhibit excited-state geometric relaxation and result in less ICT character than 1. Coupled with theoretical calculations, the data support a planar ICT (PICT) excited state where the diphenylamino nitrogen in an sp(2)-like geometry is integral with the plane containing the fluorene and benzothiazole moieties. Ultrafast transient absorption experiments show that ICT occurs rapidly (<150 fs) followed by geometric and solvent relaxation in ∼ 1-4 ps to form the PICT or solvent-stabilized ICT (SSICT) state. This relaxation is not observed in non-polar n-hexane because the solvent dependent ICT state energy lies higher than the locally-excited (LE) state. Finally, formation of a triplet state (T1) is only efficiently observed in n-hexane for all four dyes.

Emission switching of 4,6-diphenylpyrimidones: solvent and solid state effects.

PubMed

Adjaye-Mensah, Edward; Gonzalez, Walter G; Bussé, David R; Captain, Burjor; Miksovska, Jaroslava; Wilson, James N

2012-08-30

The photophysics of 1-ethyl-4,6-bis(4-methoxyphenyl)-2(1H)-pyrimidone (1) and 1-ethyl-4,6-bis(4-(dimethylamino)phenyl)-2(1H)-pyrimidone (2) were investigated to determine the mechanisms of emission switching in response to protonation. UV-vis and steady state emission spectroscopy of the protonated and unprotonated forms across a range of solvents reveal the polarity dependence of the vertical excitation energies. Emission lifetimes and quantum yields show the solvent dependency of the excited states. Emission enhancements were observed in polyethylene glycol solutions and in the solid state (both thin film and single crystal), demonstrating the role of intramolecular rotation in thermal relaxation of the excited states. TD-DFT calculations provide insights into the excited state geometries and the role of intramolecular charge transfer. The collected data show that emission of diphenylpyrimidones can be modulated by four factors, including the identity of the electron-donating auxochrome, protonation state, solvent polarity, and viscosity.

a Time-Dependent Many-Electron Approach to Atomic and Molecular Interactions

NASA Astrophysics Data System (ADS)

Runge, Keith

A new methodology is developed for the description of electronic rearrangement in atomic and molecular collisions. Using the eikonal representation of the total wavefunction, time -dependent equations are derived for the electronic densities within the time-dependent Hartree-Fock approximation. An averaged effective potential which ensures time reversal invariance is used to describe the effect of the fast electronic transitions on the slower nuclear motions. Electron translation factors (ETF) are introduced to eliminate spurious asymptotic couplings, and a local ETF is incorporated into a basis of traveling atomic orbitals. A reference density is used to describe local electronic relaxation and to account for the time propagation of fast and slow motions, and is shown to lead to an efficient integration scheme. Expressions for time-dependent electronic populations and polarization parameters are given. Electronic integrals over Gaussians including ETFs are derived to extend electronic state calculations to dynamical phenomena. Results of the method are in good agreement with experimental data for charge transfer integral cross sections over a projectile energy range of three orders of magnitude in the proton-Hydrogen atom system. The more demanding calculations of integral alignment, state-to-state integral cross sections, and differential cross sections are found to agree well with experimental data provided care is taken to include ETFs in the calculation of electronic integrals and to choose the appropriate effective potential. The method is found to be in good agreement with experimental data for the calculation of charge transfer integral cross sections and state-to-state integral cross sections in the one-electron heteronuclear Helium(2+)-Hydrogen atom system and in the two-electron system, Hydrogen atom-Hydrogen atom. Time-dependent electronic populations are seen to oscillate rapidly in the midst of collision event. In particular, multiple exchanges of the electron are seen to occur in the proton-Hydrogen atom system at low collision energies. The concepts and results derived from the approach provide new insight into the dynamics of nuclear screening and electronic rearrangement in atomic collisions.

Electrical conductivity and dielectric properties of TlInS2 single crystals

NASA Astrophysics Data System (ADS)

El-Nahass, M. M.; Youssef, S. B.; Ali, H. A. M.; Hassan, A.

2011-07-01

TlInS2 single crystals were grown by using Bridgman-Stockbauer technique. Measurements of DC conductivity were carried out in parallel (σ//) and perpendicular (σ⊥) directions to the c-axis over a temperature range from 303 to 463 K. The anisotropic behaviour of the electrical conductivity was also detected. AC conductivity and dielectric measurements were studied as a function of both frequency (102-106 Hz) and temperature (297-375 K). The frequency dependence of the AC conductivity revealed that σac(ω) obeys the universal law: σac(ω) = Aωs. The mechanism of the ac charge transport across the layers of TlInS2 single crystals was referred to the hopping over localized states near the Fermi level in the frequency range >3.5 × 103 Hz. The temperature dependence of σac(ω) for TlInS2 showed that σac is thermally activated process. Both of ɛ1 and ɛ2 decrease by increasing frequency and increase by increasing temperature. Some parameters were calculated as: the density of localized states near the Fermi level NF = 1.5 × 1020 eV-1 cm-3, the average time of charge carrier hoping between localized states τ = 3.79 μs and the average hopping distance R = 6.07 nm.

Free volume dependent fluorescence property of PMMA composite: Positron annihilation studies

NASA Astrophysics Data System (ADS)

Ravindrachary, V.; Praveena, S. D.; Bhajantri, R. F.; Ismayil, Crasta, Vincent

2013-02-01

The free volume related fluorescence properties of chalcone chromophore [1-(4-methylphenyl)-3-(4-N, N, dimethylaminophenyl)-2-propen-1-one doped Poly(methyl methacrylate) have been studied using fluorescence spectroscopy and Positron Annihilation lifetime spectroscopy techniques. The fluorescence spectra show that the fluorescence behavior depends on the free volume dependent polymer microstructure and varies with dopant concentration with in the composite. The origin and variation of fluorescence is understood by twisted internal charge transfer state as well as free volume. The Positron annihilation study shows that the free volume related microstructure of the composite is vary with doping level.

Thermally induced charge current through long molecules

NASA Astrophysics Data System (ADS)

Zimbovskaya, Natalya A.; Nitzan, Abraham

2018-01-01

In this work, we theoretically study steady state thermoelectric transport through a single-molecule junction with a long chain-like bridge. Electron transmission through the system is computed using a tight-binding model for the bridge. We analyze dependences of thermocurrent on the bridge length in unbiased and biased systems operating within and beyond the linear response regime. It is shown that the length-dependent thermocurrent is controlled by the lineshape of electron transmission in the interval corresponding to the HOMO/LUMO transport channel. Also, it is demonstrated that electron interactions with molecular vibrations may significantly affect the length-dependent thermocurrent.

Theoretical study of dynamic electron-spin-polarization via the doublet-quartet quantum-mixed state and time-resolved ESR spectra of the quartet high-spin state.

PubMed

Teki, Yoshio; Matsumoto, Takafumi

2011-04-07

The mechanism of the unique dynamic electron polarization of the quartet (S = 3/2) high-spin state via a doublet-quartet quantum-mixed state and detail theoretical calculations of the population transfer are reported. By the photo-induced electron transfer, the quantum-mixed charge-separate state is generated in acceptor-donor-radical triad (A-D-R). This mechanism explains well the unique dynamic electron polarization of the quartet state of A-D-R. The generation of the selectively populated quantum-mixed state and its transfer to the strongly coupled pure quartet and doublet states have been treated both by a perturbation approach and by exact numerical calculations. The analytical solutions show that generation of the quantum-mixed states with the selective populations after de-coherence and/or accompanying the (complete) dephasing during the charge-recombination are essential for the unique dynamic electron polarization. Thus, the elimination of the quantum coherence (loss of the quantum information) is the key process for the population transfer from the quantum-mixed state to the quartet state. The generation of high-field polarization on the strongly coupled quartet state by the charge-recombination process can be explained by a polarization transfer from the quantum-mixed charge-separate state. Typical time-resolved ESR patterns of the quantum-mixed state and of the strongly coupled quartet state are simulated based on the generation mechanism of the dynamic electron polarization. The dependence of the spectral pattern of the quartet high-spin state has been clarified for the fine-structure tensor and the exchange interaction of the quantum-mixed state. The spectral pattern of the quartet state is not sensitive towards the fine-structure tensor of the quantum-mixed state, because this tensor contributes only as a perturbation in the population transfer to the spin-sublevels of the quartet state. Based on the stochastic Liouville equation, it is also discussed why the selective population in the quantum-mixed state is generated for the "finite field" spin-sublevels. The numerical calculations of the elimination of the quantum coherence (de-coherence and/or dephasing) are demonstrated. A new possibility of the enhanced intersystem crossing pathway in solution is also proposed.

Study of ordered hadron chains with the ATLAS detector

NASA Astrophysics Data System (ADS)

Aaboud, M.; Aad, G.; Abbott, B.; Abdinov, O.; Abeloos, B.; Abidi, S. H.; Abouzeid, O. S.; Abraham, N. L.; Abramowicz, H.; Abreu, H.; Abreu, R.; Abulaiti, Y.; Acharya, B. S.; Adachi, S.; Adamczyk, L.; Adelman, J.; Adersberger, M.; Adye, T.; Affolder, A. A.; Afik, Y.; Agatonovic-Jovin, T.; Agheorghiesei, C.; Aguilar-Saavedra, J. A.; Ahlen, S. P.; Ahmadov, F.; Aielli, G.; Akatsuka, S.; Akerstedt, H.; Åkesson, T. P. A.; Akilli, E.; Akimov, A. V.; Alberghi, G. L.; Albert, J.; Albicocco, P.; Alconada Verzini, M. J.; Alderweireldt, S. C.; Aleksa, M.; Aleksandrov, I. N.; Alexa, C.; Alexander, G.; Alexopoulos, T.; Alhroob, M.; Ali, B.; Aliev, M.; Alimonti, G.; Alison, J.; Alkire, S. P.; Allbrooke, B. M. M.; Allen, B. W.; Allport, P. P.; Aloisio, A.; Alonso, A.; Alonso, F.; Alpigiani, C.; Alshehri, A. A.; Alstaty, M. I.; Alvarez Gonzalez, B.; Álvarez Piqueras, D.; Alviggi, M. G.; Amadio, B. T.; Amaral Coutinho, Y.; Amelung, C.; Amidei, D.; Amor Dos Santos, S. P.; Amoroso, S.; Amundsen, G.; Anastopoulos, C.; Ancu, L. S.; Andari, N.; Andeen, T.; Anders, C. F.; Anders, J. K.; Anderson, K. J.; Andreazza, A.; Andrei, V.; Angelidakis, S.; Angelozzi, I.; Angerami, A.; Anisenkov, A. V.; Anjos, N.; Annovi, A.; Antel, C.; Antonelli, M.; Antonov, A.; Antrim, D. J.; Anulli, F.; Aoki, M.; Aperio Bella, L.; Arabidze, G.; Arai, Y.; Araque, J. P.; Araujo Ferraz, V.; Arce, A. T. H.; Ardell, R. E.; Arduh, F. A.; Arguin, J.-F.; Argyropoulos, S.; Arik, M.; Armbruster, A. J.; Armitage, L. J.; Arnaez, O.; Arnold, H.; Arratia, M.; Arslan, O.; Artamonov, A.; Artoni, G.; Artz, S.; Asai, S.; Asbah, N.; Ashkenazi, A.; Asquith, L.; Assamagan, K.; Astalos, R.; Atkinson, M.; Atlay, N. B.; Augsten, K.; Avolio, G.; Axen, B.; Ayoub, M. K.; Azuelos, G.; Baas, A. E.; Baca, M. J.; Bachacou, H.; Bachas, K.; Backes, M.; Bagnaia, P.; Bahmani, M.; Bahrasemani, H.; Baines, J. T.; Bajic, M.; Baker, O. K.; Baldin, E. M.; Balek, P.; Balli, F.; Balunas, W. K.; Banas, E.; Bandyopadhyay, A.; Banerjee, Sw.; Bannoura, A. A. E.; Barak, L.; Barberio, E. L.; Barberis, D.; Barbero, M.; Barillari, T.; Barisits, M.-S.; Barkeloo, J. T.; Barklow, T.; Barlow, N.; Barnes, S. L.; Barnett, B. M.; Barnett, R. M.; Barnovska-Blenessy, Z.; Baroncelli, A.; Barone, G.; Barr, A. J.; Barranco Navarro, L.; Barreiro, F.; Barreiro Guimarães da Costa, J.; Bartoldus, R.; Barton, A. E.; Bartos, P.; Basalaev, A.; Bassalat, A.; Bates, R. L.; Batista, S. J.; Batley, J. R.; Battaglia, M.; Bauce, M.; Bauer, F.; Bawa, H. S.; Beacham, J. B.; Beattie, M. D.; Beau, T.; Beauchemin, P. H.; Bechtle, P.; Beck, H. P.; Beck, H. C.; Becker, K.; Becker, M.; Becot, C.; Beddall, A. J.; Beddall, A.; Bednyakov, V. A.; Bedognetti, M.; Bee, C. P.; Beermann, T. A.; Begalli, M.; Begel, M.; Behr, J. K.; Bell, A. S.; Bella, G.; Bellagamba, L.; Bellerive, A.; Bellomo, M.; Belotskiy, K.; Beltramello, O.; Belyaev, N. L.; Benary, O.; Benchekroun, D.; Bender, M.; Bendtz, K.; Benekos, N.; Benhammou, Y.; Benhar Noccioli, E.; Benitez, J.; Benjamin, D. P.; Benoit, M.; Bensinger, J. R.; Bentvelsen, S.; Beresford, L.; Beretta, M.; Berge, D.; Bergeaas Kuutmann, E.; Berger, N.; Beringer, J.; Berlendis, S.; Bernard, N. R.; Bernardi, G.; Bernius, C.; Bernlochner, F. U.; Berry, T.; Berta, P.; Bertella, C.; Bertoli, G.; Bertolucci, F.; Bertram, I. A.; Bertsche, C.; Bertsche, D.; Besjes, G. J.; Bessidskaia Bylund, O.; Bessner, M.; Besson, N.; Betancourt, C.; Bethani, A.; Bethke, S.; Bevan, A. J.; Beyer, J.; Bianchi, R. M.; Biebel, O.; Biedermann, D.; Bielski, R.; Bierwagen, K.; Biesuz, N. V.; Biglietti, M.; Billoud, T. R. V.; Bilokon, H.; Bindi, M.; Bingul, A.; Bini, C.; Biondi, S.; Bisanz, T.; Bittrich, C.; Bjergaard, D. M.; Black, J. E.; Black, K. M.; Blair, R. E.; Blazek, T.; Bloch, I.; Blocker, C.; Blue, A.; Blum, W.; Blumenschein, U.; Blunier, S.; Bobbink, G. J.; Bobrovnikov, V. S.; Bocchetta, S. S.; Bocci, A.; Bock, C.; Boehler, M.; Boerner, D.; Bogavac, D.; Bogdanchikov, A. G.; Bohm, C.; Boisvert, V.; Bokan, P.; Bold, T.; Boldyrev, A. S.; Bolz, A. E.; Bomben, M.; Bona, M.; Boonekamp, M.; Borisov, A.; Borissov, G.; Bortfeldt, J.; Bortoletto, D.; Bortolotto, V.; Boscherini, D.; Bosman, M.; Bossio Sola, J. D.; Boudreau, J.; Bouffard, J.; Bouhova-Thacker, E. V.; Boumediene, D.; Bourdarios, C.; Boutle, S. K.; Boveia, A.; Boyd, J.; Boyko, I. R.; Bracinik, J.; Brandt, A.; Brandt, G.; Brandt, O.; Bratzler, U.; Brau, B.; Brau, J. E.; Breaden Madden, W. D.; Brendlinger, K.; Brennan, A. J.; Brenner, L.; Brenner, R.; Bressler, S.; Briglin, D. L.; Bristow, T. M.; Britton, D.; Britzger, D.; Brochu, F. M.; Brock, I.; Brock, R.; Brooijmans, G.; Brooks, T.; Brooks, W. K.; Brosamer, J.; Brost, E.; Broughton, J. H.; Bruckman de Renstrom, P. A.; Bruncko, D.; Bruni, A.; Bruni, G.; Bruni, L. S.; Brunt, Bh; Bruschi, M.; Bruscino, N.; Bryant, P.; Bryngemark, L.; Buanes, T.; Buat, Q.; Buchholz, P.; Buckley, A. G.; Budagov, I. A.; Buehrer, F.; Bugge, M. K.; Bulekov, O.; Bullock, D.; Burch, T. J.; Burdin, S.; Burgard, C. D.; Burger, A. M.; Burghgrave, B.; Burka, K.; Burke, S.; Burmeister, I.; Burr, J. T. P.; Busato, E.; Büscher, D.; Büscher, V.; Bussey, P.; Butler, J. M.; Buttar, C. M.; Butterworth, J. M.; Butti, P.; Buttinger, W.; Buzatu, A.; Buzykaev, A. R.; Cabrera Urbán, S.; Caforio, D.; Cairo, V. M.; Cakir, O.; Calace, N.; Calafiura, P.; Calandri, A.; Calderini, G.; Calfayan, P.; Callea, G.; Caloba, L. P.; Calvente Lopez, S.; Calvet, D.; Calvet, S.; Calvet, T. P.; Camacho Toro, R.; Camarda, S.; Camarri, P.; Cameron, D.; Caminal Armadans, R.; Camincher, C.; Campana, S.; Campanelli, M.; Camplani, A.; Campoverde, A.; Canale, V.; Cano Bret, M.; Cantero, J.; Cao, T.; Capeans Garrido, M. D. M.; Caprini, I.; Caprini, M.; Capua, M.; Carbone, R. M.; Cardarelli, R.; Cardillo, F.; Carli, I.; Carli, T.; Carlino, G.; Carlson, B. T.; Carminati, L.; Carney, R. M. D.; Caron, S.; Carquin, E.; Carrá, S.; Carrillo-Montoya, G. D.; Casadei, D.; Casado, M. P.; Casolino, M.; Casper, D. W.; Castelijn, R.; Castillo Gimenez, V.; Castro, N. F.; Catinaccio, A.; Catmore, J. R.; Cattai, A.; Caudron, J.; Cavaliere, V.; Cavallaro, E.; Cavalli, D.; Cavalli-Sforza, M.; Cavasinni, V.; Celebi, E.; Ceradini, F.; Cerda Alberich, L.; Cerqueira, A. S.; Cerri, A.; Cerrito, L.; Cerutti, F.; Cervelli, A.; Cetin, S. A.; Chafaq, A.; Chakraborty, D.; Chan, S. K.; Chan, W. S.; Chan, Y. L.; Chang, P.; Chapman, J. D.; Charlton, D. G.; Chau, C. C.; Chavez Barajas, C. A.; Che, S.; Cheatham, S.; Chegwidden, A.; Chekanov, S.; Chekulaev, S. V.; Chelkov, G. A.; Chelstowska, M. A.; Chen, C.; Chen, H.; Chen, J.; Chen, S.; Chen, S.; Chen, X.; Chen, Y.; Cheng, H. C.; Cheng, H. J.; Cheplakov, A.; Cheremushkina, E.; Cherkaoui El Moursli, R.; Cheu, E.; Cheung, K.; Chevalier, L.; Chiarella, V.; Chiarelli, G.; Chiodini, G.; Chisholm, A. S.; Chitan, A.; Chiu, Y. H.; Chizhov, M. V.; Choi, K.; Chomont, A. R.; Chouridou, S.; Chow, Y. S.; Christodoulou, V.; Chu, M. C.; Chudoba, J.; Chuinard, A. J.; Chwastowski, J. J.; Chytka, L.; Ciftci, A. K.; Cinca, D.; Cindro, V.; Cioara, I. A.; Ciocca, C.; Ciocio, A.; Cirotto, F.; Citron, Z. H.; Citterio, M.; Ciubancan, M.; Clark, A.; Clark, B. L.; Clark, M. R.; Clark, P. J.; Clarke, R. N.; Clement, C.; Coadou, Y.; Cobal, M.; Coccaro, A.; Cochran, J.; Colasurdo, L.; Cole, B.; Colijn, A. P.; Collot, J.; Colombo, T.; Conde Muiño, P.; Coniavitis, E.; Connell, S. H.; Connelly, I. A.; Constantinescu, S.; Conti, G.; Conventi, F.; Cooke, M.; Cooper-Sarkar, A. M.; Cormier, F.; Cormier, K. J. R.; Corradi, M.; Corriveau, F.; Cortes-Gonzalez, A.; Cortiana, G.; Costa, G.; Costa, M. J.; Costanzo, D.; Cottin, G.; Cowan, G.; Cox, B. E.; Cranmer, K.; Crawley, S. J.; Creager, R. A.; Cree, G.; Crépé-Renaudin, S.; Crescioli, F.; Cribbs, W. A.; Cristinziani, M.; Croft, V.; Crosetti, G.; Cueto, A.; Cuhadar Donszelmann, T.; Cukierman, A. R.; Cummings, J.; Curatolo, M.; Cúth, J.; Czekierda, S.; Czodrowski, P.; D'Amen, G.; D'Auria, S.; D'Eramo, L.; D'Onofrio, M.; da Cunha Sargedas de Sousa, M. J.; da Via, C.; Dabrowski, W.; Dado, T.; Dai, T.; Dale, O.; Dallaire, F.; Dallapiccola, C.; Dam, M.; Dandoy, J. R.; Daneri, M. F.; Dang, N. P.; Daniells, A. C.; Dann, N. S.; Danninger, M.; Dano Hoffmann, M.; Dao, V.; Darbo, G.; Darmora, S.; Dassoulas, J.; Dattagupta, A.; Daubney, T.; Davey, W.; David, C.; Davidek, T.; Davis, D. R.; Davison, P.; Dawe, E.; Dawson, I.; de, K.; de Asmundis, R.; de Benedetti, A.; de Castro, S.; de Cecco, S.; de Groot, N.; de Jong, P.; de la Torre, H.; de Lorenzi, F.; de Maria, A.; de Pedis, D.; de Salvo, A.; de Sanctis, U.; de Santo, A.; de Vasconcelos Corga, K.; de Vivie de Regie, J. B.; Debbe, R.; Debenedetti, C.; Dedovich, D. V.; Dehghanian, N.; Deigaard, I.; Del Gaudio, M.; Del Peso, J.; Delgove, D.; Deliot, F.; Delitzsch, C. M.; Dell'Acqua, A.; Dell'Asta, L.; Dell'Orso, M.; Della Pietra, M.; Della Volpe, D.; Delmastro, M.; Delporte, C.; Delsart, P. A.; Demarco, D. A.; Demers, S.; Demichev, M.; Demilly, A.; Denisov, S. P.; Denysiuk, D.; Derendarz, D.; Derkaoui, J. E.; Derue, F.; Dervan, P.; Desch, K.; Deterre, C.; Dette, K.; Devesa, M. R.; Deviveiros, P. O.; Dewhurst, A.; Dhaliwal, S.; di Bello, F. A.; di Ciaccio, A.; di Ciaccio, L.; di Clemente, W. K.; di Donato, C.; di Girolamo, A.; di Girolamo, B.; di Micco, B.; di Nardo, R.; di Petrillo, K. F.; di Simone, A.; di Sipio, R.; di Valentino, D.; Diaconu, C.; Diamond, M.; Dias, F. A.; Diaz, M. A.; Diehl, E. B.; Dietrich, J.; Díez Cornell, S.; Dimitrievska, A.; Dingfelder, J.; Dita, P.; Dita, S.; Dittus, F.; Djama, F.; Djobava, T.; Djuvsland, J. I.; Do Vale, M. A. 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S.; Osculati, B.; Ospanov, R.; Otero Y Garzon, G.; Otono, H.; Ouchrif, M.; Ould-Saada, F.; Ouraou, A.; Oussoren, K. P.; Ouyang, Q.; Owen, M.; Owen, R. E.; Ozcan, V. E.; Ozturk, N.; Pachal, K.; Pacheco Pages, A.; Pacheco Rodriguez, L.; Padilla Aranda, C.; Pagan Griso, S.; Paganini, M.; Paige, F.; Palacino, G.; Palazzo, S.; Palestini, S.; Palka, M.; Pallin, D.; Panagiotopoulou, E. St.; Panagoulias, I.; Pandini, C. E.; Panduro Vazquez, J. G.; Pani, P.; Panitkin, S.; Pantea, D.; Paolozzi, L.; Papadopoulou, Th. D.; Papageorgiou, K.; Paramonov, A.; Paredes Hernandez, D.; Parker, A. J.; Parker, M. A.; Parker, K. A.; Parodi, F.; Parsons, J. A.; Parzefall, U.; Pascuzzi, V. R.; Pasner, J. M.; Pasqualucci, E.; Passaggio, S.; Pastore, Fr.; Pataraia, S.; Pater, J. R.; Pauly, T.; Pearson, B.; Pedraza Lopez, S.; Pedro, R.; Peleganchuk, S. V.; Penc, O.; Peng, C.; Peng, H.; Penwell, J.; Peralva, B. S.; Perego, M. M.; Perepelitsa, D. V.; Peri, F.; Perini, L.; Pernegger, H.; Perrella, S.; Peschke, R.; Peshekhonov, V. D.; Peters, K.; Peters, R. F. Y.; Petersen, B. A.; Petersen, T. C.; Petit, E.; Petridis, A.; Petridou, C.; Petroff, P.; Petrolo, E.; Petrov, M.; Petrucci, F.; Pettersson, N. E.; Peyaud, A.; Pezoa, R.; Phillips, F. H.; Phillips, P. W.; Piacquadio, G.; Pianori, E.; Picazio, A.; Piccaro, E.; Pickering, M. A.; Piegaia, R.; Pilcher, J. E.; Pilkington, A. D.; Pin, A. W. J.; Pinamonti, M.; Pinfold, J. L.; Pirumov, H.; Pitt, M.; Plazak, L.; Pleier, M.-A.; Pleskot, V.; Plotnikova, E.; Pluth, D.; Podberezko, P.; Poettgen, R.; Poggi, R.; Poggioli, L.; Pogrebnyak, I.; Pohl, D.; Polesello, G.; Poley, A.; Policicchio, A.; Polifka, R.; Polini, A.; Pollard, C. S.; Polychronakos, V.; Pommès, K.; Ponomarenko, D.; Pontecorvo, L.; Popeneciu, G. A.; Pospisil, S.; Potamianos, K.; Potrap, I. N.; Potter, C. J.; Poulsen, T.; Poveda, J.; Pozo Astigarraga, M. 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M.; Stroynowski, R.; Strubig, A.; Stucci, S. A.; Stugu, B.; Styles, N. A.; Su, D.; Su, J.; Suchek, S.; Sugaya, Y.; Suk, M.; Sulin, V. V.; Sultan, Dms; Sultansoy, S.; Sumida, T.; Sun, S.; Sun, X.; Suruliz, K.; Suster, C. J. E.; Sutton, M. R.; Suzuki, S.; Svatos, M.; Swiatlowski, M.; Swift, S. P.; Sykora, I.; Sykora, T.; Ta, D.; Tackmann, K.; Taenzer, J.; Taffard, A.; Tafirout, R.; Tahirovic, E.; Taiblum, N.; Takai, H.; Takashima, R.; Takasugi, E. H.; Takeshita, T.; Takubo, Y.; Talby, M.; Talyshev, A. A.; Tanaka, J.; Tanaka, M.; Tanaka, R.; Tanaka, S.; Tanioka, R.; Tannenwald, B. B.; Tapia Araya, S.; Tapprogge, S.; Tarem, S.; Tartarelli, G. F.; Tas, P.; Tasevsky, M.; Tashiro, T.; Tassi, E.; Tavares Delgado, A.; Tayalati, Y.; Taylor, A. C.; Taylor, A. J.; Taylor, G. N.; Taylor, P. T. E.; Taylor, W.; Teixeira-Dias, P.; Temple, D.; Ten Kate, H.; Teng, P. K.; Teoh, J. J.; Tepel, F.; Terada, S.; Terashi, K.; Terron, J.; Terzo, S.; Testa, M.; Teuscher, R. J.; Theveneaux-Pelzer, T.; Thiele, F.; Thomas, J. P.; Thomas-Wilsker, J.; Thompson, P. D.; Thompson, A. S.; Thomsen, L. A.; Thomson, E.; Tibbetts, M. J.; Ticse Torres, R. E.; Tikhomirov, V. O.; Tikhonov, Yu. A.; Timoshenko, S.; Tipton, P.; Tisserant, S.; Todome, K.; Todorova-Nova, S.; Todt, S.; Tojo, J.; Tokár, S.; Tokushuku, K.; Tolley, E.; Tomlinson, L.; Tomoto, M.; Tompkins, L.; Toms, K.; Tong, B.; Tornambe, P.; Torrence, E.; Torres, H.; Torró Pastor, E.; Toth, J.; Touchard, F.; Tovey, D. R.; Treado, C. J.; Trefzger, T.; Tresoldi, F.; Tricoli, A.; Trigger, I. M.; Trincaz-Duvoid, S.; Tripiana, M. F.; Trischuk, W.; Trocmé, B.; Trofymov, A.; Troncon, C.; Trottier-McDonald, M.; Trovatelli, M.; Truong, L.; Trzebinski, M.; Trzupek, A.; Tsang, K. W.; Tseng, J. C.-L.; Tsiareshka, P. V.; Tsipolitis, G.; Tsirintanis, N.; Tsiskaridze, S.; Tsiskaridze, V.; Tskhadadze, E. G.; Tsui, K. M.; Tsukerman, I. I.; Tsulaia, V.; Tsuno, S.; Tsybychev, D.; Tu, Y.; Tudorache, A.; Tudorache, V.; Tulbure, T. T.; Tuna, A. N.; Tupputi, S. A.; Turchikhin, S.; Turgeman, D.; Turk Cakir, I.; Turra, R.; Tuts, P. M.; Ucchielli, G.; Ueda, I.; Ughetto, M.; Ukegawa, F.; Unal, G.; Undrus, A.; Unel, G.; Ungaro, F. C.; Unno, Y.; Unverdorben, C.; Urban, J.; Urquijo, P.; Urrejola, P.; Usai, G.; Usui, J.; Vacavant, L.; Vacek, V.; Vachon, B.; Vadla, K. O. H.; Vaidya, A.; Valderanis, C.; Valdes Santurio, E.; Valente, M.; Valentinetti, S.; Valero, A.; Valéry, L.; Valkar, S.; Vallier, A.; Valls Ferrer, J. A.; van den Wollenberg, W.; van der Graaf, H.; van Gemmeren, P.; van Nieuwkoop, J.; van Vulpen, I.; van Woerden, M. C.; Vanadia, M.; Vandelli, W.; Vaniachine, A.; Vankov, P.; Vardanyan, G.; Vari, R.; Varnes, E. W.; Varni, C.; Varol, T.; Varouchas, D.; Vartapetian, A.; Varvell, K. E.; Vasquez, J. G.; Vasquez, G. A.; Vazeille, F.; Vazquez Schroeder, T.; Veatch, J.; Veeraraghavan, V.; Veloce, L. M.; Veloso, F.; Veneziano, S.; Ventura, A.; Venturi, M.; Venturi, N.; Venturini, A.; Vercesi, V.; Verducci, M.; Verkerke, W.; Vermeulen, A. T.; Vermeulen, J. C.; Vetterli, M. C.; Viaux Maira, N.; Viazlo, O.; Vichou, I.; Vickey, T.; Vickey Boeriu, O. E.; Viehhauser, G. H. A.; Viel, S.; Vigani, L.; Villa, M.; Villaplana Perez, M.; Vilucchi, E.; Vincter, M. G.; Vinogradov, V. B.; Vishwakarma, A.; Vittori, C.; Vivarelli, I.; Vlachos, S.; Vogel, M.; Vokac, P.; Volpi, G.; von der Schmitt, H.; von Toerne, E.; Vorobel, V.; Vorobev, K.; Vos, M.; Voss, R.; Vossebeld, J. H.; Vranjes, N.; Vranjes Milosavljevic, M.; Vrba, V.; Vreeswijk, M.; Vuillermet, R.; Vukotic, I.; Wagner, P.; Wagner, W.; Wagner-Kuhr, J.; Wahlberg, H.; Wahrmund, S.; Walder, J.; Walker, R.; Walkowiak, W.; Wallangen, V.; Wang, C.; Wang, C.; Wang, F.; Wang, H.; Wang, H.; Wang, J.; Wang, J.; Wang, Q.; Wang, R.; Wang, S. M.; Wang, T.; Wang, W.; Wang, W.; Wang, Z.; Wanotayaroj, C.; Warburton, A.; Ward, C. P.; Wardrope, D. R.; Washbrook, A.; Watkins, P. M.; Watson, A. T.; Watson, M. F.; Watts, G.; Watts, S.; Waugh, B. M.; Webb, A. F.; Webb, S.; Weber, M. S.; Weber, S. W.; Weber, S. A.; Webster, J. S.; Weidberg, A. R.; Weinert, B.; Weingarten, J.; Weirich, M.; Weiser, C.; Weits, H.; Wells, P. S.; Wenaus, T.; Wengler, T.; Wenig, S.; Wermes, N.; Werner, M. D.; Werner, P.; Wessels, M.; Weston, T. D.; Whalen, K.; Whallon, N. L.; Wharton, A. M.; White, A. S.; White, A.; White, M. J.; White, R.; Whiteson, D.; Whitmore, B. W.; Wickens, F. J.; Wiedenmann, W.; Wielers, M.; Wiglesworth, C.; Wiik-Fuchs, L. A. M.; Wildauer, A.; Wilk, F.; Wilkens, H. G.; Williams, H. H.; Williams, S.; Willis, C.; Willocq, S.; Wilson, J. A.; Wingerter-Seez, I.; Winkels, E.; Winklmeier, F.; Winston, O. J.; Winter, B. T.; Wittgen, M.; Wobisch, M.; Wolf, T. M. H.; Wolff, R.; Wolter, M. W.; Wolters, H.; Wong, V. W. S.; Worm, S. D.; Wosiek, B. K.; Wotschack, J.; Wozniak, K. W.; Wu, M.; Wu, S. L.; Wu, X.; Wu, Y.; Wyatt, T. R.; Wynne, B. M.; Xella, S.; Xi, Z.; Xia, L.; Xu, D.; Xu, L.; Xu, T.; Yabsley, B.; Yacoob, S.; Yamaguchi, D.; Yamaguchi, Y.; Yamamoto, A.; Yamamoto, S.; Yamanaka, T.; Yamane, F.; Yamatani, M.; Yamazaki, Y.; Yan, Z.; Yang, H.; Yang, H.; Yang, Y.; Yang, Z.; Yao, W.-M.; Yap, Y. C.; Yasu, Y.; Yatsenko, E.; Yau Wong, K. H.; Ye, J.; Ye, S.; Yeletskikh, I.; Yigitbasi, E.; Yildirim, E.; Yorita, K.; Yoshihara, K.; Young, C.; Young, C. J. S.; Yu, J.; Yu, J.; Yuen, S. P. Y.; Yusuff, I.; Zabinski, B.; Zacharis, G.; Zaidan, R.; Zaitsev, A. M.; Zakharchuk, N.; Zalieckas, J.; Zaman, A.; Zambito, S.; Zanzi, D.; Zeitnitz, C.; Zemaityte, G.; Zemla, A.; Zeng, J. C.; Zeng, Q.; Zenin, O.; Ženiš, T.; Zerwas, D.; Zhang, D.; Zhang, F.; Zhang, G.; Zhang, H.; Zhang, J.; Zhang, L.; Zhang, L.; Zhang, M.; Zhang, P.; Zhang, R.; Zhang, R.; Zhang, X.; Zhang, Y.; Zhang, Z.; Zhao, X.; Zhao, Y.; Zhao, Z.; Zhemchugov, A.; Zhou, B.; Zhou, C.; Zhou, L.; Zhou, M.; Zhou, M.; Zhou, N.; Zhu, C. G.; Zhu, H.; Zhu, J.; Zhu, Y.; Zhuang, X.; Zhukov, K.; Zibell, A.; Zieminska, D.; Zimine, N. I.; Zimmermann, C.; Zimmermann, S.; Zinonos, Z.; Zinser, M.; Ziolkowski, M.; Živković, L.; Zobernig, G.; Zoccoli, A.; Zou, R.; Zur Nedden, M.; Zwalinski, L.; Atlas Collaboration

2017-11-01

The analysis of the momentum difference between charged hadrons in high-energy proton-proton collisions is performed in order to study coherent particle production. The observed correlation pattern agrees with a model of a helical QCD string fragmenting into a chain of ground-state hadrons. A threshold momentum difference in the production of adjacent pairs of charged hadrons is observed, in agreement with model predictions. The presence of low-mass hadron chains also explains the emergence of charge-combination-dependent two-particle correlations commonly attributed to Bose-Einstein interference. The data sample consists of 190 μ b-1 of minimum-bias events collected with proton-proton collisions at a center-of-mass energy √{s }=7 TeV in the early low-luminosity data taking with the ATLAS detector at the LHC.

Redox reactions with empirical potentials: atomistic battery discharge simulations.

PubMed

Dapp, Wolf B; Müser, Martin H

2013-08-14

Batteries are pivotal components in overcoming some of today's greatest technological challenges. Yet to date there is no self-consistent atomistic description of a complete battery. We take first steps toward modeling of a battery as a whole microscopically. Our focus lies on phenomena occurring at the electrode-electrolyte interface which are not easily studied with other methods. We use the redox split-charge equilibration (redoxSQE) method that assigns a discrete ionization state to each atom. Along with exchanging partial charges across bonds, atoms can swap integer charges. With redoxSQE we study the discharge behavior of a nano-battery, and demonstrate that this reproduces the generic properties of a macroscopic battery qualitatively. Examples are the dependence of the battery's capacity on temperature and discharge rate, as well as performance degradation upon recharge.

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

Aaboud, M.; Aad, G.; Abbott, B.

The analysis of the momentum difference between charged hadrons in high-energy proton-proton collisions is performed in order to study coherent particle production. The observed correlation pattern agrees with a model of a helical QCD string fragmenting into a chain of ground-state hadrons. A threshold momentum difference in the production of adjacent pairs of charged hadrons is observed, in agreement with model predictions. The presence of low-mass hadron chains also explains the emergence of charge-combination-dependent two-particle correlations commonly attributed to Bose-Einstein interference. Here, the data sample consists of 190 μb –1 of minimum-bias events collected with proton-proton collisions at a center-of-massmore » energy √s=7 TeV in the early low-luminosity data taking with the ATLAS detector at the LHC.« less

12 CFR 7.4001 - Charging interest at rates permitted competing institutions; charging interest to corporate...

Code of Federal Regulations, 2011 CFR

2011-01-01

... bank may lawfully charge the highest rate permitted to be charged by a state-licensed small loan... small loan companies. (c) Effect on state definitions of interest. The Federal definition of the term... the law of that state. If state law permits different interest charges on specified classes of loans...

12 CFR 7.4001 - Charging interest at rates permitted competing institutions; charging interest to corporate...

Code of Federal Regulations, 2014 CFR

2014-01-01

... bank may lawfully charge the highest rate permitted to be charged by a state-licensed small loan... small loan companies. (c) Effect on state definitions of interest. The Federal definition of the term... the law of that state. If state law permits different interest charges on specified classes of loans...

12 CFR 7.4001 - Charging interest at rates permitted competing institutions; charging interest to corporate...

Code of Federal Regulations, 2013 CFR

2013-01-01

... bank may lawfully charge the highest rate permitted to be charged by a state-licensed small loan... small loan companies. (c) Effect on state definitions of interest. The Federal definition of the term... the law of that state. If state law permits different interest charges on specified classes of loans...

12 CFR 7.4001 - Charging interest at rates permitted competing institutions; charging interest to corporate...

Code of Federal Regulations, 2012 CFR

2012-01-01

... bank may lawfully charge the highest rate permitted to be charged by a state-licensed small loan... small loan companies. (c) Effect on state definitions of interest. The Federal definition of the term... the law of that state. If state law permits different interest charges on specified classes of loans...

Measurements of Lunar Dust Charging Properties by Electron Impact

NASA Technical Reports Server (NTRS)

Abbas, Mian M.; Tankosic, Dragana; Craven, Paul D.; Schneider, Todd A.; Vaughn, Jason A.; LeClair, Andre; Spann, James F.; Norwood, Joseph K.

2009-01-01

Dust grains in the lunar environment are believed to be electrostatically charged predominantly by photoelectric emissions resulting from solar UV radiation on the dayside, and on the nightside by interaction with electrons in the solar wind plasma. In the high vacuum environment on the lunar surface with virtually no atmosphere, the positive and negative charge states of micron/submicron dust grains lead to some unusual physical and dynamical dust phenomena. Knowledge of the electrostatic charging properties of dust grains in the lunar environment is required for addressing their hazardous effect on the humans and mechanical systems. It is well recognized that the charging properties of individual small micron size dust grains are substantially different from the measurements on bulk materials. In this paper we present the results of measurements on charging of individual Apollo 11 and Apollo 17 dust grains by exposing them to mono-energetic electron beams in the 10-100 eV energy range. The charging/discharging rates of positively and negatively charged particles of approx. 0.1 to 5 micron radii are discussed in terms of the sticking efficiencies and secondary electron yields. The secondary electron emission process is found to be a complex and effective charging/discharging mechanism for incident electron energies as low as 10-25 eV, with a strong dependence on particle size. Implications of the laboratory measurements on the nature of dust grain charging in the lunar environment are discussed.

In situ measurement of surface potential developed on MgO thin film surface under ion irradiation using ion scattering spectroscopy

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

Nagatomi, T.; Kuwayama, T.; Takai, Y.

2009-11-15

The application of ion scattering spectroscopy (ISS) to the in situ measurement of the surface potential developed on an insulator surface under positive ion irradiation was investigated. The ISS spectra measured for a MgO film of 600 nm thickness on a Si substrate by the irradiation of 950 eV He{sup +} ions revealed that the surface is positively charged by approximately 180 V. For accurate measurement of the surface potential, a correction to take into account the angular deflection of primary ions induced by the high surface potential is required. The dependence of the surface potential on the sample temperaturemore » revealed that no charging is induced above 700 deg. C, indicating that accumulated charges can be removed by heating to 700 deg. C. From the measurement of the ion-induced secondary electron yield using a collector electrode located in front of the sample surface, the surface potential and ion-induced secondary electron yield were found to be strongly affected by the experimental setup. Secondary electrons produced by the impact of slow positive secondary ions, the maximum energy of which corresponds to the surface potential, play an important role when the bias voltage applied to the collector electrode is positively high for the present experimental setup. The surface potential developed on the surface of MgO films of 600 and 200 nm thickness was measured in situ, revealing that the amount of accumulated charges and the time required to attain the steady state of charging are slightly dependent on the beam current of primary ions and strongly dependent on the thickness of the MgO film. The present results confirmed that the application of ISS has high potential for investigating charging phenomena and the secondary electron emission from insulator surfaces under positive ion irradiation.« less

Lectures on Quantum Mechanics

NASA Astrophysics Data System (ADS)

Weinberg, Steven

2015-09-01

Preface; Notation; 1. Historical introduction; 2. Particle states in a central potential; 3. General principles of quantum mechanics; 4. Spin; 5. Approximations for energy eigenstates; 6. Approximations for time-dependent problems; 7. Potential scattering; 8. General scattering theory; 9. The canonical formalism; 10. Charged particles in electromagnetic fields; 11. The quantum theory of radiation; 12. Entanglement; Author index; Subject index.

Charge state manipulation of qubits in diamond

PubMed Central

Grotz, Bernhard; Hauf, Moritz V.; Dankerl, Markus; Naydenov, Boris; Pezzagna, Sébastien; Meijer, Jan; Jelezko, Fedor; Wrachtrup, Jörg; Stutzmann, Martin; Reinhard, Friedemann; Garrido, Jose A.

2012-01-01

The nitrogen-vacancy (NV) centre in diamond is a promising candidate for a solid-state qubit. However, its charge state is known to be unstable, discharging from the qubit state NV− into the neutral state NV0 under various circumstances. Here we demonstrate that the charge state can be controlled by an electrolytic gate electrode. This way, single centres can be switched from an unknown non-fluorescent state into the neutral charge state NV0, and the population of an ensemble of centres can be shifted from NV0 to NV−. Numerical simulations confirm the manipulation of the charge state to be induced by the gate-controlled shift of the Fermi level at the diamond surface. This result opens the way to a dynamic control of transitions between charge states and to explore hitherto inaccessible states, such as NV+. PMID:22395620

Charge state distribution of 86Kr in hydrogen and helium gas charge strippers at 2.7 MeV /nucleon

NASA Astrophysics Data System (ADS)

Kuboki, H.; Okuno, H.; Hasebe, H.; Fukunishi, N.; Ikezawa, E.; Imao, H.; Kamigaito, O.; Kase, M.

2014-12-01

The charge state distributions of krypton (86Kr) with an energy of 2.7 MeV /nucleon were measured using hydrogen (H2 ) and helium (He) gas charge strippers. A differential pumping system was constructed to confine H2 and He gases to a thickness sufficient for the charge state distributions to attain equilibrium. The mean charge states of 86Kr in H2 and He gases attained equilibrium at 25.1 and 23.2, respectively, whereas the mean charge state in N2 gas at equilibrium was estimated to be less than 20. The charge distributions are successfully reproduced by the cross sections of ionization and electron capture processes optimized by a fitting procedure.

First Principles Modeling and Interpretation of Ionization-Triggered Charge Migration in Molecules

NASA Astrophysics Data System (ADS)

Bruner, Adam; Hernandez, Sam; Mauger, Francois; Abanador, Paul; Gaarde, Mette; Schafer, Ken; Lopata, Ken

Modeling attosecond coherent charge migration in molecules is important for understanding initial steps of photochemistry and light harvesting processes. Ionization triggered hole migration can be difficult to characterize and interpret as the dynamics can be convoluted with excited states. Here, we introduce a real-time time-dependent density functional theory (RT-TDDFT) approach for modeling such dynamics from first principles. To isolate the specific hole dynamics from excited states, Fourier transform analysis and orbital occupations are used to provide a spatial hole representation in the frequency domain. These techniques are applied to hole transfer across a thiophene dimer as well as core-hole triggered valence motion in nitrosobenzene. This work was supported by U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award No. DE-SC0012462.

Quantification of the memory imprint effect for a charged particle environment

NASA Technical Reports Server (NTRS)

Bhuva, B. L.; Johnson, R. L., Jr.; Gyurcsik, R. S.; Kerns, S. E.; Fernald, K. W.

1987-01-01

The effects of total accumulated dose on the single-event vulnerability of NMOS resistive-load SRAMs are investigated. The bias-dependent shifts in device parameters can imprint the memory state present during exposure or erase the imprinted state. Analysis of these effects is presented along with an analytic model developed for the quantification of these effects. The results indicate that the imprint effect is dominated by the difference in the threshold voltage of the n-channel devices.

Up-Conversion Intersystem Crossing Rates in Organic Emitters for Thermally Activated Delayed Fluorescence: Impact of the Nature of Singlet vs Triplet Excited States.

PubMed

Samanta, Pralok K; Kim, Dongwook; Coropceanu, Veaceslav; Brédas, Jean-Luc

2017-03-22

The rates for up-conversion intersystem crossing (UISC) from the T 1 state to the S 1 state are calculated for a series of organic emitters with an emphasis on thermally activated delayed fluorescence (TADF) materials. Both the spin-orbit coupling and the energy difference between the S 1 and T 1 states (ΔE ST ) are evaluated, at the density functional theory (DFT) and time-dependent DFT levels. The calculated UISC rates and ΔE ST values are found to be in good agreement with available experimental data. Our results underline that small ΔE ST values and sizable spin-orbit coupling matrix elements have to be simultaneously realized in order to facilitate UISC and ultimately TADF. Importantly, the spatial separation of the highest occupied and lowest unoccupied molecular orbitals of the emitter, a widely accepted strategy for the design of TADF molecules, does not necessarily lead to a sufficient reduction in ΔE ST ; in fact, either a significant charge-transfer (CT) contribution to the T 1 state or a minimal energy difference between the local-excitation and charge-transfer triplet states is required to achieve a small ΔE ST . Also, having S 1 and T 1 states of a different nature is found to strongly enhance spin-orbit coupling, which is consistent with the El-Sayed rule for ISC rates. Overall, our results indicate that having either similar energies for the local-excitation and charge-transfer triplet states or the right balance between a substantial CT contribution to T 1 and somewhat different natures of the S 1 and T 1 states, paves the way toward UISC enhancement and thus TADF efficiency improvement.

Level Anticrossing of Impurity States in Semiconductor Nanocrystals

PubMed Central

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

2014-01-01

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

Diabatization for Time-Dependent Density Functional Theory: Exciton Transfers and Related Conical Intersections.

PubMed

Tamura, Hiroyuki

2016-11-23

Intermolecular exciton transfers and related conical intersections are analyzed by diabatization for time-dependent density functional theory. The diabatic states are expressed as a linear combination of the adiabatic states so as to emulate the well-defined reference states. The singlet exciton coupling calculated by the diabatization scheme includes contributions from the Coulomb (Förster) and electron exchange (Dexter) couplings. For triplet exciton transfers, the Dexter coupling, charge transfer integral, and diabatic potentials of stacked molecules are calculated for analyzing direct and superexchange pathways. We discuss some topologies of molecular aggregates that induce conical intersections on the vanishing points of the exciton coupling, namely boundary of H- and J-aggregates and T-shape aggregates, as well as canceled exciton coupling to the bright state of H-aggregate, i.e., selective exciton transfer to the dark state. The diabatization scheme automatically accounts for the Berry phase by fixing the signs of reference states while scanning the coordinates.

STATIC QUARK ANTI-QUARK FREE AND INTERNAL ENERGY IN 2-FLAVOR QCD AND BOUND STATES IN THE QGP.

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

ZANTOW, F.; KACZMAREK, O.

2005-07-25

We present results on heavy quark free energies in 2-flavour QCD. The temperature dependence of the interaction between static quark anti-quark pairs will be analyzed in terms of temperature dependent screening radii, which give a first estimate on the medium modification of (heavy quark) bound states in the quark gluon plasma. Comparing those radii to the (zero temperature) mean squared charge radii of chasmonium states indicates that the J/{Psi} may survive the phase transition as a bound state, while {chi}{sub c} and {Psi}{prime} are expected to show significant thermal modifications at temperatures close to the transition. Furthermore we will analyzemore » the relation between heavy quark free energies, entropy contributions and internal energy and discuss their relation to potential models used to analyze the melting of heavy quark bound states above the deconfinement temperature. Results of different groups and various potential models for bound states in the deconfined phase of QCD are compared.« less

Charge trapping phenomena of tetraethylorthosilicate thin film containing Si nanocrystals synthesized by solid-state reaction.

PubMed

Lau, H W; Tan, O K; Liu, Y; Trigg, D A; Chen, T P

2006-08-28

In this work, we report on the fabrication of tetraethylorthosilicate (TEOS) thin dielectric film containing silicon nanocrystals (Si nc), synthesized by solid-state reaction, in a capacitor structure. A metal-insulator-semi-conductor (MIS) capacitor, with 28 nm thick Si nc in a TEOS thin film, has been fabricated. For this MIS, both electron and hole trapping in the Si nc are possible, depending on the polarity of the bias voltage. A V(FB) shift greater than 1 V can be experienced by a bias voltage of 16 V applied to the metal electrode for 1 s. Though there is no top control oxide, the discharge time for 10% of charges can be up to 4480 s when it is biased at 16 V for 1 s. It is further demonstrated that charging and discharging mechanisms are due to the Si nc rather than the TEOS oxide defects. This form of Si nc in a TEOS thin film capacitor provides the possibility of memory applications at low cost.

Four-qubit systems and dyonic black Hole-Black branes in superstring theory

NASA Astrophysics Data System (ADS)

Belhaj, A.; Bensed, M.; Benslimane, Z.; Sedra, M. B.; Segui, A.

Using dyonic solutions in the type IIA superstring theory on Calabi-Yau (CY) manifolds, we reconsider the study of black objects and quantum information theory using string/string duality in six dimensions. Concretely, we relate four-qubits with a stringy quaternionic moduli space of type IIA compactification associated with a dyonic black solution formed by black holes (BHs) and black 2-branes (B2B) carrying eight electric charges and eight magnetic charges. This connection is made by associating the cohomology classes of the heterotic superstring on T4 to four-qubit states. These states are interpreted in terms of such dyonic charges resulting from the quaternionic symmetric space SO(4,4) SO(4)×SO(4) corresponding to a N = 4 sigma model superpotential in two dimensions. The superpotential is considered as a functional depending on four quaternionic fields mapped to a class of Clifford algebras denoted as Cl0,4. A link between such an algebra and the cohomology classes of T4 in heterotic superstring theory is also given.

The Effect of Oxidation and Charge/Discharge rates on Li Plating in All-Solid-State Batteries

NASA Astrophysics Data System (ADS)

Yulaev, Alexander; Oleshko, Vladimir; Talin, A. Alec; Leite, Marina S.; Kolmakov, Andrei

All-solid-state Li-ion batteries (SSLIBs) is currently an extensive area of research due to their promising specific power and energy density properties. Moreover, SSLIBs significantly mitigate the safety risks of the thermal runaway that may occur in liquid electrolyte batteries. We fabricated a model SSLIB, which consists of LiCoO2 cathode layer, LiPON as an electrolyte, and a model ultra-thin carbon anode. Using in operando scanning electron microscopy in conjunction with electrochemical measurements, we found that depending on ambient oxidizing conditions and charging rate, the morphology of plated lithium alternates between quasi-1D and 3D microstructures. In addition, we were able to use an electron beam as a virtual nano-electrode to selectively control the nucleation rate and Li growth structure during the SSLIB charging with high spatial resolution. Finally, we determined the conditions when lithium may be oxidized even during battery cycling under UHV conditions, leading to significant capacity losses. We foresee that our work will provide deeper insights into a safe SSLIB performance under real world operating conditions.

Nanowires formed by the co-assembly of a negatively charged low-molecular weight gelator and a zwitterionic polythiophene.

PubMed

Li, Feng; Palaniswamy, Ganesan; de Jong, Menno R; Aslund, Andreas; Konradsson, Peter; Marcelis, Antonius T M; Sudhölter, Ernst J R; Stuart, Martien A Cohen; Leermakers, Frans A M

2010-06-21

Conjugated organic nanowires have been prepared by co-assembling a carboxylate containing low-molecular weight gelator (LMWG) and an amino acid substituted polythiophene derivative (PTT). Upon introducing the zwitterionic polyelectrolyte PTT to a basic molecular solution of the organogelator, the negative charges on the LMWG are compensated by the positive charges of the PTT. As a result, nanowires form through co-assembly. These nanowires are visualized by both transmission electron microscopy (TEM) and atomic force microscopy (AFM). Depending on the concentration and ratio of the components these nanowires can be micrometers long. These measurements further suggest that the aggregates adopt a helical conformation. The morphology of these nanowires are studied with fluorescent confocal laser scanning microscopy (CLSM). The interactions between LMWG and PTT are characterized by steady-state and time-resolved fluorescence spectroscopy studies. The steady-state spectra indicate that the backbone of the PTT adopts a more planar and more aggregated conformation when interacting with LMWG. The time- resolved fluorescence decay studies confirm this interpretation.

3D Localized Trions in Monolayer WSe2 in a Charge Tunable van der Waals Heterostructure.

PubMed

Chakraborty, Chitraleema; Qiu, Liangyu; Konthasinghe, Kumarasiri; Mukherjee, Arunabh; Dhara, Sajal; Vamivakas, Nick

2018-05-09

Monolayer transition metal dichalcogenides (TMDCs) have recently emerged as a host material for localized optically active quantum emitters that generate single photons. (1-5) Here, we investigate fully localized excitons and trions from such TMDC quantum emitters embedded in a van der Waals heterostructure. We use direct electrostatic doping through the vertical heterostructure device assembly to generate quantum confined trions. Distinct spectral jumps as a function of applied voltage bias, and excitation power-dependent charging, demonstrate the observation of the two different excitonic complexes. We also observe a reduction of the intervalley electron-hole exchange interaction in the confined trion due to the addition of an extra electron, which is manifested by a decrease in its fine structure splitting. We further confirm this decrease of exchange interaction for the case of the charged states by a comparative study of the circular polarization resolved photoluminescence from individual excitonic states. The valley polarization selection rules inherited by the localized trions will provide a pathway toward realizing a localized spin-valley-photon interface.

Deuterium kinetic isotope effects on the dissociation of a protein-fatty acid complex in the gas phase.

PubMed

Liu, Lan; Michelsen, Klaus; Kitova, Elena N; Schnier, Paul D; Brown, Alex; Klassen, John S

2012-04-04

Deuterium kinetic isotope effects (KIEs) are reported for the first time for the dissociation of a protein-ligand complex in the gas phase. Temperature-dependent rate constants were measured for the loss of neutral ligand from the deprotonated ions of the 1:1 complex of bovine β-lactoglobulin (Lg) and palmitic acid (PA), (Lg + PA)(n-) → Lg(n-) + PA, at the 6- and 7- charge states. At 25 °C, partial or complete deuteration of the acyl chain of PA results in a measurable inverse KIE for both charge states. The magnitude of the KIEs is temperature dependent, and Arrhenius analysis of the rate constants reveals that deuteration of PA results in a decrease in activation energy. In contrast, there is no measurable deuterium KIE for the dissociation of the (Lg + PA) complex in aqueous solution at pH 8. Deuterium KIEs were calculated using conventional transition-state theory with an assumption of a late dissociative transition state (TS), in which the ligand is free of the binding pocket. The vibrational frequencies of deuterated and non-deuterated PA in the gas phase and in various solvents (n-hexane, 1-chlorohexane, acetone, and water) were established computationally. The KIEs calculated from the corresponding differences in zero-point energies account qualitatively for the observation of an inverse KIE but do not account for the magnitude of the KIEs nor their temperature dependence. It is proposed that the dissociation of the (Lg + PA) complex in aqueous solution also proceeds through a late TS in which the acyl chain is extensively hydrated such that there is no significant differential change in the vibrational frequencies along the reaction coordinate and, consequently, no significant KIE.

Charge Mediated Compaction and Rearrangement of Gas-Phase Proteins: A Case Study Considering Two Proteins at Opposing Ends of the Structure-Disorder Continuum

NASA Astrophysics Data System (ADS)

Jhingree, Jacquelyn R.; Bellina, Bruno; Pacholarz, Kamila J.; Barran, Perdita E.

2017-07-01

Charge reduction in the gas phase provides a direct means of manipulating protein charge state, and when coupled to ion mobility mass spectrometry (IM-MS), it is possible to monitor the effect of charge on protein conformation in the absence of solution. Use of the electron transfer reagent 1,3-dicyanobenzene, coupled with IM-MS, allows us to monitor the effect of charge reduction on the conformation of two proteins deliberately chosen from opposite sides of the order to disorder continuum: bovine pancreatic trypsin inhibitor (BPTI) and beta casein. The ordered BPTI presents compact conformers for each of three charge states accompanied by narrow collision cross-section distributions (TWCCSDN2→He). Upon reduction of BPTI, irrespective of precursor charge state, the TWCCSN2→He decreases to a similar distribution as found for the nESI generated ion of identical charge. The behavior of beta casein upon charge reduction is more complex. It presents over a wide charge state range (9-28), and intermediate charge states (13-18) have broad TWCCSDN2→He with multiple conformations, where both compaction and rearrangement are seen. Further, we see that the TWCCSDN2→He of the latter charge states are even affected by the presence of radical anions. Overall, we conclude that the flexible nature of some proteins result in broad conformational distributions comprised of many families, even for single charge states, and the barrier between different states can be easily overcome by an alteration of the net charge.

Ultrafast dynamics of isolated model photoactive yellow protein chromophores: "Chemical perturbation theory" in the laboratory.

PubMed

Vengris, Mikas; Larsen, Delmar S; van der Horst, Michael A; Larsen, Olaf F A; Hellingwerf, Klaas J; van Grondelle, Rienk

2005-03-10

Pump-probe and pump-dump probe experiments have been performed on several isolated model chromophores of the photoactive yellow protein (PYP). The observed transient absorption spectra are discussed in terms of the spectral signatures ascribed to solvation, excited-state twisting, and vibrational relaxation. It is observed that the protonation state has a profound effect on the excited-state lifetime of p-coumaric acid. Pigments with ester groups on the coumaryl tail end and charged phenolic moieties show dynamics that are significantly different from those of other pigments. Here, an unrelaxed ground-state intermediate could be observed in pump-probe signals. A similar intermediate could be identified in the sinapinic acid and in isomerization-locked chromophores by means of pump-dump probe spectroscopy; however, in these compounds it is less pronounced and could be due to ground-state solvation and/or vibrational relaxation. Because of strong protonation-state dependencies and the effect of electron donor groups, it is argued that charge redistribution upon excitation determines the twisting reaction pathway, possibly through interaction with the environment. It is suggested that the same pathway may be responsible for the initiation of the photocycle in native PYP.

Controlling photophysics of styrylnaphthalimides through TICT, fluorescence and E,Z-photoisomerization interplay.

PubMed

Panchenko, Pavel A; Arkhipova, Antonina N; Fedorova, Olga A; Fedorov, Yuri V; Zakharko, Marina A; Arkhipov, Dmitry E; Jonusauskas, Gediminas

2017-01-04

The photophysical properties of naphthalimide dyes NI1-3 with electron releasing 4-methoxy- (NI1), 3,4-dimethoxystyryl- (NI2) and dimethylaminostyryl (NI3) groups are examined in a variety of protic and aprotic solvents. All compounds demonstrate positive solvatochromism in the steady-state absorption and fluorescence spectra. The analysis of the dependence of the Stokes shift on the polarity of the solvent using the Lippert-Mataga equation allowed us to determine the change in the dipole moment upon excitation. The obtained data correspond to the formation of highly polar charge transfer states. Based on the transient absorption spectra and time-resolved fluorescence measurements, the presence of two different emissive states was definitely proved. The primarily formed planar Local Excited (LE) state dominates in non-polar solvents like cyclohexane and toluene where it relaxes mostly through fluorescence and E,Z-isomerisation pathways. In polar solvents, an alternative relaxation channel emerges that consists of twisting around single bond between styryl and naphthalimide fragments, which leads to the formation of a Twisted Intramolecular Charge Transfer (TICT) state. The factors affecting the fluorescence of TICT states are discussed. The observed spectral effects are rationalized using quantum-chemical calculations, X-ray data and NMR spectroscopy.

Double core-hole emissivity of transient aluminum plasmas produced in the interaction with ultra-intense x-ray laser pulse

NASA Astrophysics Data System (ADS)

Gao, Cheng; Zeng, Jiaolong; Yuan, Jianmin

2015-11-01

Emissivity of single core-hole (SCH) and double core-hole (DCH) states of aluminum plasmas produced in the interaction with ultra-intense x-ray laser pulse interaction are investigated systematically by solving the time-dependent rate equation implemented in the detailed level accounting approximation. We first demonstrated the plasma density effects on level populations and charge state distribution. Compared with recent experiments, it is shown that the plasma density effects play important roles in the evolution dynamics. Then we systematically investigated the emissivity of the transient aluminum plasmas produced by the x-ray laser pulses with a few photon energies above the threshold photon energy to create DCH states. For the laser photon energy where there are resonant absorptions (RA), 1s-np transitions with both full 1s and SCH 1s states play important roles in time evolution of the population and DCH emission spectroscopy. The significant RA effects are illustrated in detail for x-ray pulses, which creates the 1s-2p resonant absorption from the SCH states of Al VII. With the increase of the photon energy, the emissions from lower charge states become larger.

Role of macromolecular crowding and salt ions on the structural-fluctuation of a highly compact configuration of carbonmonoxycytochrome c.

PubMed

Kumar, Rajesh; Sharma, Deepak; Jain, Rishu; Kumar, Sandeep; Kumar, Rajesh

2015-12-01

Carbonmonoxycytochrome c refolds to a native-like compact state (NCO-state), where the non-native Fe(2+)-CO interaction persists. Structural and molecular properties extracted from CD, fluorescence and NMR experiments reveal that the NCO-state shows the generic properties of molten globules. Slow thermal-dissociation of CO transforms the NCO-state to native-state (N-state), where the native Fe(2+)-M80 bond recovers. To determine the role of crowding agents and salt ions on the structural-fluctuation of NCO, the kinetic and thermodynamic parameters for CO-dissociation from NCO (NCO→N+CO) were measured at varying concentrations of crowding agents (dextran 70, dextran 40, ficoll 70) and salt ions (anion: ClO4(-), I(-), Br(-), NO3(-), Cl(-); cation: NH4(+), K(+), Na(+)). As [crowding agent] or [ion] is increased, the rate coefficient of CO-dissociation (kdiss) decreases exponentially. Furthermore, the extent of decrease in kdiss is found to be dependent on (i) size, charge density and charge dispersion of the ion, and (ii) size, shape, and viscosity of the crowding agent. Copyright © 2015 Elsevier B.V. All rights reserved.

Excited-State Conformational/Electronic Responses of Saddle-Shaped N,N'-Disubstituted-Dihydrodibenzo[a,c]phenazines: Wide-Tuning Emission from Red to Deep Blue and White Light Combination.

PubMed

Zhang, Zhiyun; Wu, Yu-Sin; Tang, Kuo-Chun; Chen, Chi-Lin; Ho, Jr-Wei; Su, Jianhua; Tian, He; Chou, Pi-Tai

2015-07-08

A tailored strategy is utilized to modify 5,10-dimethylphenazine (DMP) to donor-acceptor type N,N'-disubstituted-dihydrodibenzo[a,c]phenazines. The representative compounds DMAC (N,N'-dimethyl), DPAC (N,N'-diphenyl), and FlPAC (N-phenyl-N'-fluorenyl) reveal significant nonplanar distortions (i.e., a saddle shape) and remarkably large Stokes-shifted emission independent of the solvent polarity. For DPAC and FlPAC with higher steric hindrance on the N,N'-substituents, normal Stokes-shifted emission also appears, for which the peak wavelength reveals solvent-polarity dependence. These unique photophysical behaviors are rationalized by electronic configuration coupled conformation changes en route to the geometry planarization in the excited state. This proposed mechanism is different from the symmetry rule imposed to explain the anomalously long-wavelength emission for DMP and is firmly supported by polarity-, viscosity-, and temperature-dependent steady-state and nanosecond time-resolved spectroscopy. Together with femtosecond early dynamics and computational simulation of the reaction energy surfaces, the results lead us to establish a sequential, three-step kinetics. Upon electronic excitation of N,N'-disubstituted-dihydrodibenzo[a,c]phenazines, intramolecular charge-transfer takes place, followed by the combination of polarization stabilization and skeletal motion toward the planarization, i.e., elongation of the π-delocalization over the benzo[a,c]phenazines moiety. Along the planarization, DPAC and FlPAC encounter steric hindrance raised by the N,N'-disubstitutes, resulting in a local minimum state, i.e., the intermediate. The combination of initial charge-transfer state, intermediate, and the final planarization state renders the full spectrum of interest and significance in their anomalous photophysics. Depending on rigidity, the N,N'-disubstituted-dihydrodibenzo[a,c]phenazines exhibit multiple emissions, which can be widely tuned from red to deep blue and even to white light generation upon optimization of the surrounding media.

Determination of trap distributions from current characteristics of pentacene field-effect transistors with surface modified gate oxide

NASA Astrophysics Data System (ADS)

Scheinert, Susanne; Pernstich, Kurt P.; Batlogg, Bertram; Paasch, Gernot

2007-11-01

It has been demonstrated [K. P. Pernstich, S. Haas, D. Oberhoff, C. Goldmann, D. J. Gundlach, B. Batlogg, A. N. Rashid, and G. Schitter, J. Appl. Phys. 96, 6431 (2004)] that a controllable shift of the threshold voltage in pentacene thin film transistors is caused by the use of organosilanes with different functional groups forming a self-assembled monolayer (SAM) on the gate oxide. The observed broadening of the subthreshold region indicates that the SAM creates additional trap states. Indeed, it is well known that traps strongly influence the behavior of organic field-effect transistors (OFETs). Therefore, the so-called "amorphous silicon (a-Si) model" has been suggested to be an appropriate model to describe OFETs. The main specifics of this model are transport of carriers above a mobility edge obeying Boltzmann statistics and exponentially distributed tail states and deep trap states. Here, approximate trap distributions are determined by adjusting two-dimensional numerical simulations to the experimental data. It follows from a systematic variation of parameters describing the trap distributions that the existence of both donorlike and acceptorlike trap distributions near the valence band, respectively, and a fixed negative interface charge have to be assumed. For two typical devices with different organosilanes the electrical characteristics can be described well with a donorlike bulk trap distribution, an acceptorlike interface distribution, and/or a fixed negative interface charge. As expected, the density of the fixed or trapped interface charge depends strongly on the surface treatment of the dielectric. There are some limitations in determining the trap distributions caused by either slow time-dependent processes resulting in differences between transfer and output characteristics, or in the uncertainty of the effective mobility.

Air Force Ni-H2 cell test program: State of Charge test

NASA Technical Reports Server (NTRS)

Moore, Bruce; Smellie, Douglas

1995-01-01

Nickel-Hydrogen cells are being cycled under a LEO (low earth orbit) test regime to examine the benefits of operating the cells at lower States of Charge (SOC) than typically used. A group of four cells are cycled using a voltage limiting charge regime that limits the State of Charge that the cells are allowed to reach. The test cells are then compared to identical cells being cycled at or near 100% State of Charge using a constant current charge regime.

Alternative Fuels Data Center: Louisiana State University: The State's

Science.gov Websites

First Workplace Charging Challenge Partner Louisiana State University: The State's First State University: The State's First Workplace Charging Challenge Partner on Facebook Tweet about Alternative Fuels Data Center: Louisiana State University: The State's First Workplace Charging Challenge

100 years of the physics of diodes

NASA Astrophysics Data System (ADS)

Zhang, Peng; Valfells, Ágúst; Ang, L. K.; Luginsland, J. W.; Lau, Y. Y.

2017-03-01

The Child-Langmuir Law (CL), discovered a century ago, gives the maximum current that can be transported across a planar diode in the steady state. As a quintessential example of the impact of space charge shielding near a charged surface, it is central to the studies of high current diodes, such as high power microwave sources, vacuum microelectronics, electron and ion sources, and high current drivers used in high energy density physics experiments. CL remains a touchstone of fundamental sheath physics, including contemporary studies of nanoscale quantum diodes and nano gap based plasmonic devices. Its solid state analog is the Mott-Gurney law, governing the maximum charge injection in solids, such as organic materials and other dielectrics, which is important to energy devices, such as solar cells and light emitting diodes. This paper reviews the important advances in the physics of diodes since the discovery of CL, including virtual cathode formation and extension of CL to multiple dimensions, to the quantum regime, and to ultrafast processes. We review the influence of magnetic fields, multiple species in bipolar flow, electromagnetic and time dependent effects in both short pulse and high frequency THz limits, and single electron regimes. Transitions from various emission mechanisms (thermionic-, field-, and photoemission) to the space charge limited state (CL) will be addressed, especially highlighting the important simulation and experimental developments in selected contemporary areas of study. We stress the fundamental physical links between the physics of beams to limiting currents in other areas, such as low temperature plasmas, laser plasmas, and space propulsion.

Low temperature specific heat of charge ordered Pr_1-xCa_xMnO_3

NASA Astrophysics Data System (ADS)

Smolyaninova, V. N.; Biswas, Amlan; Zhang, X.; Greene, R. L.

2000-03-01

Mixed-valent perovskite manganese oxides at certain doping levels develope a real space ordering of Mn^3+ and Mn^4+ at low temperatures^1, which can be destroyed (``melted'') by the application of a modest magnetic field.^2 To better understand the low-temperature ground state and the physics of the ``melted'' charge-ordered state, the specific heat, resistivity and magnetization of charge-ordered Pr_1-xCa_xMnO3 were measured with and without magnetic field for single crystal and ceramic samples of different x. A large excess specific heat of nonmagnetic origin was found, similar to that found in La_0.5Ca_0.5MnO3 ^3. Significant changes in the specific heat associated with the ``melting'' of the charge ordering were observed in applied magnetic fields up to 9 T. Possible explanations for this anomalous specific heat and its magnetic field dependence will be discussed . ^*This work is supported in part by NSF MRSEC Grant at the University of Maryland. ^1S. Mori, C. H. Chen and S-W. Cheong, Nature 392, 473 (1998). ^2Y. Tomioka et al., Phys. Rev. Lett. 74, 5108 (1995). ^3V. N. Smolyaninova, K. Ghosh and R. L. Greene, Phys. Rev. B 58, R14 725 (1998).

Quantum and classical dissipation of charged particles

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

Ibarra-Sierra, V.G.; Anzaldo-Meneses, A.; Cardoso, J.L.

2013-08-15

A Hamiltonian approach is presented to study the two dimensional motion of damped electric charges in time dependent electromagnetic fields. The classical and the corresponding quantum mechanical problems are solved for particular cases using canonical transformations applied to Hamiltonians for a particle with variable mass. Green’s function is constructed and, from it, the motion of a Gaussian wave packet is studied in detail. -- Highlights: •Hamiltonian of a damped charged particle in time dependent electromagnetic fields. •Exact Green’s function of a charged particle in time dependent electromagnetic fields. •Time evolution of a Gaussian wave packet of a damped charged particle.more » •Classical and quantum dynamics of a damped electric charge.« less

Azimuthal angle dependence of the charge imbalance from charge conservation effects

NASA Astrophysics Data System (ADS)

BoŻek, Piotr

2018-03-01

The experimental search for the chiral magnetic effect in heavy-ion collisions is based on charge-dependent correlations between emitted particles. Recently, a sensitive observable comparing event-by-event distributions of the charge splitting projected on the directions along and perpendicular to the direction of the elliptic flow has been proposed. The results of a (3 + 1)-dimensional hydrodynamic model show that the preliminary experimental data of the STAR Collaboration can be explained as due to background effects, such as resonance decays and local charge conservation in the particle production. A related observable based on the third-order harmonic flow is proposed to further investigate such background effects in charge-dependent correlations.

Resonant inelastic x-ray scattering study of charge excitations in superconducting and nonsuperconducting PrFeAsO₁₋ y

DOE PAGES

Jarrige, I.; Nomura, T.; Ishii, K.; ...

2012-09-05

We report the first observation by momentum-resolved resonant inelastic x-ray scattering of charge excitations in an iron-based superconductor and its parent compound, PrFeAsO₀.₇ and PrFeAsO, respectively, with two main results. First, using calculations based on a 16-band dp model, we show that the energy of the lowest-lying excitations, identified as dd interband transitions of dominant xz,yz orbital character, exhibits a dramatic dependence on electron correlation. This enables us to estimate the Coulomb repulsion U and Hund's coupling J, and to highlight the role played by J in these peculiar orbital-dependent electron correlation effects. Second, we show that short-range antiferromagnetic correlations,more » which are a prerequisite to the occurrence of these excitations at the Γ point, are still present in the superconducting state.« less

Effects of charge inhomogeneities on elementary excitations in La 2-xSr xCuO₄

DOE PAGES

Park, S. R.; Hamann, A.; Pintschovius, L.; ...

2011-12-12

Purely local experimental probes of many copper oxide superconductors show that their electronic states are inhomogeneous in real space. For example, scanning tunneling spectroscopic imaging shows strong variations in real space, and according to nuclear quadrupole resonance (NQR) studies, the charge distribution in the bulk varies on the nanoscale. However, the analysis of the experimental results utilizing spatially averaged probes often ignores this fact. We have performed a detailed investigation of the doping dependence of the energy and linewidth of the zone-boundary Cu-O bond-stretching vibration in La 2-xSr xCuO₄ by inelastic neutron scattering. Both our results as well as previouslymore » reported angle-dependent momentum widths of the electronic spectral function detected by angle-resolved photoemission can be reproduced by including the same distribution of local environments extracted from the NQR analysis.« less

Using resonant x-ray scattering to determine how structure controls the charge generation process in PCPDTBT:PC70BM solar cells

NASA Astrophysics Data System (ADS)

Pope, Michael; Waldrip, Matthew; Ferron, Thomas; Collins, Brian

Increased solar power conversion efficiencies to 12% in bulk heterojunction organic photovoltaics (OPVs) continue to brighten their prospects as an economically viable source of solar energy. It is known that OPV performance can be enhanced through processing additives that change the nanostructure. We track these critical structure-property relationships in the OPV system PCPDTBT:PC70BM while varying the amount of DIO additive. Resonant Soft X-ray Scattering reveals domain purity, domain size, and molecular orientation to highlight the system's complex dependence on DIO concentration. We will show the effect the resulting structure has on charge generation and recombination via in-situ transient and steady state optoelectronic measurements. By measuring structure, excited state dynamics and device performance all on the same sample enables direct relationships to be measured. We show that the appropriate balance of crystallinity, domain size and domain purity are important for optimized excited state dynamics and device performance.

Charge density wave order in 1D mirror twin boundaries of single-layer MoSe 2

DOE PAGES

Barja, Sara; Wickenburg, Sebastian; Liu, Zhen-Fei; ...

2016-04-18

Here, We provide direct evidence for the existence of isolated, one-dimensional charge density waves at mirror twin boundaries (MTBs) of single-layer semiconducting MoSe 2. Such MTBs have been previously observed by transmission electron microscopy and have been predicted to be metallic in MoSe 2 and MoS 2. Our low-temperature scanning tunnelling microscopy/spectroscopy measurements revealed a substantial bandgap of 100 meV opening at the Fermi energy in the otherwise metallic one-dimensional structures. We found a periodic modulation in the density of states along the MTB, with a wavelength of approximately three lattice constants. In addition to mapping the energy-dependent densitymore » of states, we determined the atomic structure and bonding of the MTB through simultaneous high-resolution non-contact atomic force microscopy. Density functional theory calculations based on the observed structure reproduced both the gap opening and the spatially resolved density of states.« less

Spin-valley locking in the normal state of a transition-metal dichalcogenide superconductor.

PubMed

Bawden, L; Cooil, S P; Mazzola, F; Riley, J M; Collins-McIntyre, L J; Sunko, V; Hunvik, K W B; Leandersson, M; Polley, C M; Balasubramanian, T; Kim, T K; Hoesch, M; Wells, J W; Balakrishnan, G; Bahramy, M S; King, P D C

2016-05-23

Metallic transition-metal dichalcogenides (TMDCs) are benchmark systems for studying and controlling intertwined electronic orders in solids, with superconductivity developing from a charge-density wave state. The interplay between such phases is thought to play a critical role in the unconventional superconductivity of cuprates, Fe-based and heavy-fermion systems, yet even for the more moderately-correlated TMDCs, their nature and origins have proved controversial. Here, we study a prototypical example, 2H-NbSe2, by spin- and angle-resolved photoemission and first-principles theory. We find that the normal state, from which its hallmark collective phases emerge, is characterized by quasiparticles whose spin is locked to their valley pseudospin. This results from a combination of strong spin-orbit interactions and local inversion symmetry breaking, while interlayer coupling further drives a rich three-dimensional momentum dependence of the underlying Fermi-surface spin texture. These findings necessitate a re-investigation of the nature of charge order and superconducting pairing in NbSe2 and related TMDCs.

Direct observation of anisotropic small-hole polarons in an orthorhombic structure of BiV O4 films

NASA Astrophysics Data System (ADS)

Chaudhuri, A.; Mandal, L.; Chi, X.; Yang, M.; Scott, M. C.; Motapothula, M.; Yu, X. J.; Yang, P.; Shao-Horn, Y.; Venkatesan, T.; Wee, A. T. S.; Rusydi, A.

2018-05-01

Here, we report an anisotropic small-hole polaron in an orthorhombic structure of BiV O4 films grown by pulsed-laser deposition on yttrium-doped zirconium oxide substrate. The polaronic state and electronic structure of BiV O4 films are revealed using a combination of polarization-dependent x-ray absorption spectroscopy at V L3 ,2 edges, spectroscopic ellipsometry, x-ray photoemission spectroscopies, and high-resolution x-ray diffraction with the support of first-principles calculations. We find that in the orthorhombic phase, which is slightly different from the conventional pucherite structure, the unoccupied V 3d orbitals and charge inhomogeneities lead to an anisotropic small-hole polaron state. Our result shows the importance of the interplay of charge and lattice for the formation of a hole polaronic state, which has a significant impact in the electrical conductivity of BiV O4 , hence its potential use as a photoanode for water splitting.

Kinetic mechanism for reversible structural transition in MoTe2 induced by excess charge carriers

NASA Astrophysics Data System (ADS)

Rubel, O.

2018-06-01

Kinetic of a reversible structural transition between insulating (2H) and metallic (1T ') phases in a monolayer MoTe2 due to an electrostatic doping is studied using first-principle calculations. The driving force for the structural transition is the energy gained by transferring excess electrons from the bottom of the conduction band to lower energy gapless states in the metallic phase as have been noticed in earlier studies. The corresponding structural transformation involves dissociation of Mo-Te bonds (one per formula unit), which results in a kinetic energy barrier of 0.83 eV. The transformation involves a consecutive movement of atoms similar to a domain wall motion. The presence of excess charge carriers modifies not only the total energy of the initial and final states, but also lowers an energy of the transition state. An experimentally observed hysteresis in the switching process can be attributed to changes in the kinetic energy barrier due to its dependence on the excess carrier density.

Valley dependent g-factor anisotropy in Silicon quantum dots

NASA Astrophysics Data System (ADS)

Ferdous, Rifat; Kawakami, Erika; Scarlino, Pasquale; Nowak, Michal; Klimeck, Gerhard; Friesen, Mark; Coppersmith, Susan N.; Eriksson, Mark A.; Vandersypen, Lieven M. K.; Rahman, Rajib

Silicon (Si) quantum dots (QD) provide a promising platform for a spin based quantum computer, because of the exceptionally long spin coherence times in Si and the existing industrial infrastructure. Due to the presence of an interface and a vertical electric field, the two lowest energy states of a Si QD are primarily composed of two conduction band valleys. Confinement by the interface and the E-field not only affect the charge properties of these states, but also their spin properties through the spin-orbit interaction (SO), which differs significantly from the SO in bulk Si. Recent experiments have found that the g-factors of these states are different and dependent on the direction of the B-field. Using an atomistic tight-binding model, we investigate the electric and magnetic field dependence of the electron g-factor of the valley states in a Si QD. We find that the g-factors are valley dependent and show 180-degree periodicity as a function of an in-plane magnetic field orientation. However, atomic scale roughness can strongly affect the anisotropic g-factors. Our study helps to reconcile disparate experimental observations and to achieve better external control over electron spins in Si QD, by electric and magnetic fields.

The influence of carrier dynamics on double-state lasing in quantum dot lasers at variable temperature

NASA Astrophysics Data System (ADS)

Korenev, V. V.; Savelyev, A. V.; Zhukov, A. E.; Omelchenko, A. V.; Maximov, M. V.

2014-12-01

It is shown in analytical form that the carrier capture from the matrix as well as carrier dynamics in quantum dots plays an important role in double-state lasing phenomenon. In particular, the de-synchronization of hole and electron captures allows one to describe recently observed quenching of ground-state lasing, which takes place in quantum dot lasers operating in double-state lasing regime at high injection. From the other side, the detailed analysis of charge carrier dynamics in the single quantum dot enables one to describe the observed light-current characteristics and key temperature dependences.

Influence of gap states on the nonresonant second hyperpolarizabilities of conjugated organic polymers

NASA Technical Reports Server (NTRS)

Beratan, David N.

1989-01-01

The presence of conjugation and substitution defects introduces gap states in finite polyenes that are shown to influence the size and sign of the second molecular hyperpolarizability (SMH). Using a one-electron tight-binding model, the dependence of SMH on the defect-state occupancy and energy in finite polyenes is calculated. Defects can cause a significant decrease or enhancement of SMH by impeding charge delocalization or by creating partly filled bands (mimicking the one-band limit), respectively. Concomitant sign changes in SMH are predicted. Calculation results suggest strategies for designing molecules that can be either photochemically or electrochemically switched between states with considerably different SMHs.

Photoemission perspective on pseudogap, superconducting fluctuations, and charge order in cuprates: a review of recent progress

NASA Astrophysics Data System (ADS)

Vishik, I. M.

2018-06-01

In the course of seeking the microscopic mechanism of superconductivity in cuprate high temperature superconductors, the pseudogap phase— the very abnormal ‘normal’ state on the hole-doped side— has proven to be as big of a quandary as superconductivity itself. Angle-resolved photoemission spectroscopy (ARPES) is a powerful tool for assessing the momentum-dependent phenomenology of the pseudogap, and recent technological developments have permitted a more detailed understanding. This report reviews recent progress in understanding the relationship between superconductivity and the pseudogap, the Fermi arc phenomena, and the relationship between charge order and pseudogap from the perspective of ARPES measurements.

Random Telegraph Signal Amplitudes in Sub 100 nm (Decanano) MOSFETs: A 3D 'Atomistic' Simulation Study

NASA Technical Reports Server (NTRS)

Asenov, Asen; Balasubramaniam, R.; Brown, A. R.; Davies, J. H.; Saini, Subhash

2000-01-01

In this paper we use 3D simulations to study the amplitudes of random telegraph signals (RTS) associated with the trapping of a single carrier in interface states in the channel of sub 100 nm (decanano) MOSFETs. Both simulations using continuous doping charge and random discrete dopants in the active region of the MOSFETs are presented. We have studied the dependence of the RTS amplitudes on the position of the trapped charge in the channel and on the device design parameters. We have observed a significant increase in the maximum RTS amplitude when discrete random dopants are employed in the simulations.

NiO: correlated band structure of a charge-transfer insulator.

PubMed

Kunes, J; Anisimov, V I; Skornyakov, S L; Lukoyanov, A V; Vollhardt, D

2007-10-12

The band structure of the prototypical charge-transfer insulator NiO is computed by using a combination of an ab initio band structure method and the dynamical mean-field theory with a quantum Monte-Carlo impurity solver. Employing a Hamiltonian which includes both Ni d and O p orbitals we find excellent agreement with the energy bands determined from angle-resolved photoemission spectroscopy. This brings an important progress in a long-standing problem of solid-state theory. Most notably we obtain the low-energy Zhang-Rice bands with strongly k-dependent orbital character discussed previously in the context of low-energy model theories.

Theoretical characterization and design of small molecule donor material containing naphthodithiophene central unit for efficient organic solar cells.

PubMed

Duan, Yu-Ai; Geng, Yun; Li, Hai-Bin; Jin, Jun-Ling; Wu, Yong; Su, Zhong-Min

2013-07-15

To seek for high-performance small molecule donor materials used in heterojunction solar cell, six acceptor-donor-acceptor small molecules based on naphtho[2,3-b:6,7-b']dithiophene (NDT) units with different acceptor units were designed and characterized using density functional theory and time-dependent density functional theory. Their geometries, electronic structures, photophysical, and charge transport properties have been scrutinized comparing with the reported donor material NDT(TDPP)2 (TDPP  =  thiophene-capped diketopyrrolopyrrole). The open circuit voltage (V(oc)), energetic driving force(ΔE(L-L)), and exciton binding energy (E(b)) were also provided to give an elementary understanding on their cell performance. The results reveal that the frontier molecular orbitals of 3-7 match well with the acceptor material PC61 BM, and compounds 3-5 were found to exhibit the comparable performances to 1 and show promising potential in organic solar cells. In particular, comparing with 1, system 7 with naphthobisthiadiazole acceptor unit displays broader absorption spectrum, higher V(oc), lower E(b), and similar carrier mobility. An in-depth insight into the nature of the involved excited states based on transition density matrix and charge density difference indicates that all S1 states are mainly intramolecular charge transfer states with the charge transfer from central NDT unit to bilateral acceptor units, and also imply that the exciton of 7 can be dissociated easily due to its large extent of the charge transfer. In a word, 7 maybe superior to 1 and may act as a promising donor candidate for organic solar cell. Copyright © 2013 Wiley Periodicals, Inc.

The voltage sensor of excitation–contraction coupling in mammals: Inactivation and interaction with Ca2+

PubMed Central

2017-01-01

In skeletal muscle, the four-helix voltage-sensing modules (VSMs) of CaV1.1 calcium channels simultaneously gate two Ca2+ pathways: the CaV1.1 pore itself and the RyR1 calcium release channel in the sarcoplasmic reticulum. Here, to gain insight into the mechanism by which VSMs gate RyR1, we quantify intramembrane charge movement associated with VSM activation (sensing current) and gated Ca2+ release flux in single muscle cells of mice and rats. As found for most four-helix VSMs, upon sustained depolarization, rodent VSMs lose the ability to activate Ca2+ release channels opening; their properties change from a functionally capable mode, in which the mobile sensor charge is called charge 1, to an inactivated mode, charge 2, with a voltage dependence shifted toward more negative voltages. We find that charge 2 is promoted and Ca2+ release inactivated when resting, well-polarized muscle cells are exposed to low extracellular [Ca2+] and that the opposite occurs in high [Ca2+]. It follows that murine VSMs are partly inactivated at rest, which establishes the reduced availability of voltage sensing as a pathogenic mechanism in disorders of calcemia. We additionally find that the degree of resting inactivation is significantly different in two mouse strains, which underscores the variability of voltage sensor properties and their vulnerability to environmental conditions. Our studies reveal that the resting and activated states of VSMs are equally favored by extracellular Ca2+. Promotion by an extracellular species of two states of the VSM that differ in the conformation of the activation gate requires the existence of a second gate, inactivation, topologically extracellular and therefore accessible from outside regardless of the activation state. PMID:29021148

New effects of a long-lived negatively charged massive particle on big bang nucleosynthesis

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

Kusakabe, Motohiko; Kim, K. S.; Cheoun, Myung-Ki

Primordial {sup 7}Li abundance inferred from observations of metal-poor stars is a factor of about 3 lower than the theoretical value of standard big bang nucleosynthesis (BBN) model. One of the solutions to the Li problem is {sup 7}Be destruction during the BBN epoch caused by a long-lived negatively charged massive particle, X{sup −}. The particle can bind to nuclei, and X-bound nuclei (X-nuclei) can experience new reactions. The radiative X{sup −} capture by {sup 7}Be nuclei followed by proton capture of the bound state of {sup 7}Be and X{sup −} ({sup 7}Be{sub x}) is a possible {sup 7}Be destructionmore » reaction. Since the primordial abundance of {sup 7}Li originates mainly from {sup 7}Li produced via the electron capture of {sup 7}Be after BBN, the {sup 7}Be destruction provides a solution to the {sup 7}Li problem. We suggest a new route of {sup 7}Be{sub x} formation, that is the {sup 7}Be charge exchange at the reaction of {sup 7}Be{sup 3+} ion and X{sup −}. The formation rate depends on the ionization fraction of {sup 7}Be{sup 3+} ion, the charge exchange cross section of {sup 7}Be{sup 3+}, and the probability that excited states {sup 7}Be{sub x}* produced at the charge exchange are converted to the ground state. We find that this reaction can be equally important as or more important than ordinary radiative recombination of {sup 7}Be and X{sup −}. The effect of this new route is shown in a nuclear reaction network calculation.« less

Simulating the thermodynamics of charging in weak polyelectrolytes: the Debye-Hückel limit

NASA Astrophysics Data System (ADS)

Rathee, Vikramjit S.; Sikora, Benjamin J.; Sidky, Hythem; Whitmer, Jonathan K.

2018-01-01

The coil-globule transition in weak (annealed) polyelectrolytes involves a subtle balance of pH, charge strength, and solvation forces. In this work, we utilize a coarse-grained hybrid grand-canonical Monte Carlo and molecular dynamics approach to explore the swelling behavior of weak linear and star polyelectrolytes under different ionic screening conditions and pH. Importantly, we are able to quantify topology-dependent effects in charging which arise at the core of star polymers. Our results are suggestive of suppression of charging in star weak polyelectrolytes in comparison to linear weak polyelectrolytes. Furthermore, we characterize the coil-globule transition in linear and star weak polyelectrolyte through expanded ensemble density-of-states simulations which suggest a change from a first order to second order phase transition moving from linear to star polyelectrolytes. Lastly, we characterize the inhomogeneous charging across the weak star polyelectrolyte through observed shifts in {{Δ }}{{{pK}}}{{o}}, and compare with experimental work. We discuss these results in relation to surfaces functionalized by weak polyelectrolyte brushes and weak polyelectrolyte-based drug delivery applications.

Charged Residues at the First Transmembrane Region Contribute to the Voltage Dependence of the Slow Gate of Connexins.

PubMed

Pinto, Bernardo I; García, Isaac E; Pupo, Amaury; Retamal, Mauricio A; Martínez, Agustín D; Latorre, Ramón; González, Carlos

2016-07-22

Connexins (Cxs) are a family of membrane-spanning proteins that form gap junction channels and hemichannels. Connexin-based channels exhibit two distinct voltage-dependent gating mechanisms termed slow and fast gating. Residues located at the C terminus of the first transmembrane segment (TM-1) are important structural components of the slow gate. Here, we determined the role of the charged residues at the end of TM-1 in voltage sensing in Cx26, Cx46, and Cx50. Conductance/voltage curves obtained from tail currents together with kinetics analysis reveal that the fast and slow gates of Cx26 involves the movement of two and four charges across the electric field, respectively. Primary sequence alignment of different Cxs shows the presence of well conserved glutamate residues in the C terminus of TM-1; only Cx26 contains a lysine in that position (lysine 41). Neutralization of lysine 41 in Cx26 increases the voltage dependence of the slow gate. Swapping of lysine 41 with glutamate 42 maintains the voltage dependence. In Cx46, neutralization of negative charges or addition of a positive charge in the Cx26 equivalent region reduced the slow gate voltage dependence. In Cx50, the addition of a glutamate in the same region decreased the voltage dependence, and the neutralization of a negative charge increased it. These results indicate that the charges at the end of TM-1 are part of the slow gate voltage sensor in Cxs. The fact that Cx42, which has no charge in this region, still presents voltage-dependent slow gating suggests that charges still unidentified also contribute to the slow gate voltage sensitivity. © 2016 by The American Society for Biochemistry and Molecular Biology, Inc.

Charged Residues at the First Transmembrane Region Contribute to the Voltage Dependence of the Slow Gate of Connexins*

PubMed Central

Pinto, Bernardo I.; García, Isaac E.; Pupo, Amaury; Retamal, Mauricio A.; Martínez, Agustín D.; Latorre, Ramón; González, Carlos

2016-01-01

Connexins (Cxs) are a family of membrane-spanning proteins that form gap junction channels and hemichannels. Connexin-based channels exhibit two distinct voltage-dependent gating mechanisms termed slow and fast gating. Residues located at the C terminus of the first transmembrane segment (TM-1) are important structural components of the slow gate. Here, we determined the role of the charged residues at the end of TM-1 in voltage sensing in Cx26, Cx46, and Cx50. Conductance/voltage curves obtained from tail currents together with kinetics analysis reveal that the fast and slow gates of Cx26 involves the movement of two and four charges across the electric field, respectively. Primary sequence alignment of different Cxs shows the presence of well conserved glutamate residues in the C terminus of TM-1; only Cx26 contains a lysine in that position (lysine 41). Neutralization of lysine 41 in Cx26 increases the voltage dependence of the slow gate. Swapping of lysine 41 with glutamate 42 maintains the voltage dependence. In Cx46, neutralization of negative charges or addition of a positive charge in the Cx26 equivalent region reduced the slow gate voltage dependence. In Cx50, the addition of a glutamate in the same region decreased the voltage dependence, and the neutralization of a negative charge increased it. These results indicate that the charges at the end of TM-1 are part of the slow gate voltage sensor in Cxs. The fact that Cx42, which has no charge in this region, still presents voltage-dependent slow gating suggests that charges still unidentified also contribute to the slow gate voltage sensitivity. PMID:27143357

Hidden crossing theory of charge exchange in H+ + He+(1 s) collisions in vicinity of maximum of cross section

NASA Astrophysics Data System (ADS)

Grozdanov, Tasko P.; Solov'ev, Evgeni A.

2018-04-01

Within the framework of dynamical adiabatic approach the hidden crossing theory of inelastic transitions is applied to charge exchange in H+ + He+(1 s) collisions in the wide range of center of mass collision energies E cm = (1.6 -70) keV. The good agreement with experiment and molecular close coupling calculations is obtained. At low energies our 4-state results are closest to the experiment and correctly reproduce the shoulder in energy dependence of the cross section around E cm = 6 keV. The 2-state results correctly predict the position of the maximum of the cross section at E cm ≈ 40 keV, whereas 4-state results fail to correctly describe the region around the maximum. The reason for this is the fact that adiabatic approximation for a given two-state hidden crossing is applicable for values of the Schtueckelberg parameter >1. But with increase of principal quantum number N the Schtueckelberg parameter decreases as N -3. That is why the 4-state approach involving higher excited states fails at smaller collision energies E cm ≈ 15 keV, while the 2-state approximation which involves low lying states can be extended to higher collision energies.

Cu doped diamond: Effect of charge state and defect aggregation on spin interactions in a 3d transition metal doped wide band-gap semiconductor

NASA Astrophysics Data System (ADS)

Benecha, E. M.; Lombardi, E. B.

2018-05-01

We present a first principles study of Cu in diamond using DFT+U electronic structure methods, by carefully considering the impact of co-doping, charge state, and Fermi level position on its stability, lattice location, spin states, and electronic properties. We show that the energetic stability and spin states of Cu are strongly dependent on the Fermi level position and the type of diamond co-doping, with Cu being energetically more favorable in n-type or p-type co-doped diamond compared to intrinsic diamond. Since Cu has been predicted to order magnetically in a number of other wide band-gap semiconductors, we have also evaluated this possibility for Cu doped diamond. We show that while Cu exhibits strong spin interactions at specific interatomic separations in diamond, a detailed consideration of the impact of Fermi level position and Cu aggregation precludes magnetic ordering, with Cu forming non-magnetic, antiferromagnetic, or paramagnetic clusters. These results have important implications in the understanding of the properties of transition metal dopants in diamond for device applications.

Exploring the effect of hole localization on the charge-phonon dynamics of hole doped delafossite

NASA Astrophysics Data System (ADS)

Mazumder, Nilesh; Mandal, Prasanta; Roy, Rajarshi; Ghorai, Uttam Kumar; Saha, Subhajit; Chattopadhyay, Kalyan Kumar

2017-09-01

For weak or moderate doping, electrical measurement is not suitable for detecting changes in the charge localization inside a semiconductor. Here, to investigate the nature of charge-phonon coupling in the presence of gradually delocalized holes within a weak doping regime (~1016 cm-3), we examine the temperature dependent Raman spectra (303-817 K) of prototype hole doped delafossite CuC{{r}1-x}M{{g}x}{{O}2-y}{{S}y} (x  =  0/0.03, y  =  0/0.01). For both {{E}g} and {{A}1g} phonons, negative lineshape asymmetry and relative thermal hardening are distinctly observed upon SO× and (MgCr\\bullet+SO×) doping. Using Allen formalism, charge density of states at the Fermi level per spin and molecule, and charge delocalization associated to a - b plane, are estimated to increase appreciably upon codoping compared to the c -axis. We delineate the interdependence between charge-phonon coupling constant (λ ) and anharmonic phonon lifetime ({τanh} ), and deduce that excitation of delocalized holes weakly coupled with phonons of larger {τanh} is the governing feature of observed Fano asymmetry (q ) reversal.

Fabrication of Gate-tunable Graphene Devices for Scanning Tunneling Microscopy Studies with Coulomb Impurities

PubMed Central

Jung, Han Sae; Tsai, Hsin-Zon; Wong, Dillon; Germany, Chad; Kahn, Salman; Kim, Youngkyou; Aikawa, Andrew S.; Desai, Dhruv K.; Rodgers, Griffin F.; Bradley, Aaron J.; Velasco, Jairo; Watanabe, Kenji; Taniguchi, Takashi; Wang, Feng; Zettl, Alex; Crommie, Michael F.

2015-01-01

Owing to its relativistic low-energy charge carriers, the interaction between graphene and various impurities leads to a wealth of new physics and degrees of freedom to control electronic devices. In particular, the behavior of graphene’s charge carriers in response to potentials from charged Coulomb impurities is predicted to differ significantly from that of most materials. Scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS) can provide detailed information on both the spatial and energy dependence of graphene's electronic structure in the presence of a charged impurity. The design of a hybrid impurity-graphene device, fabricated using controlled deposition of impurities onto a back-gated graphene surface, has enabled several novel methods for controllably tuning graphene’s electronic properties.1-8 Electrostatic gating enables control of the charge carrier density in graphene and the ability to reversibly tune the charge2 and/or molecular5 states of an impurity. This paper outlines the process of fabricating a gate-tunable graphene device decorated with individual Coulomb impurities for combined STM/STS studies.2-5 These studies provide valuable insights into the underlying physics, as well as signposts for designing hybrid graphene devices. PMID:26273961